Full-Color Realization of Micro-LED Displays: Nanomaterials

nanomaterials
Review
Full-Color Realization of Micro-LED Displays
Yifan Wu, Jianshe Ma, Ping Su * , Lijun Zhang and Bizhong Xia
Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China;
wuyf19@mails.tsinghua.edu.cn (Y.W.); ma.jianshe@sz.tsinghua.edu.cn (J.M.);
zhanglj18@mails.tsinghua.edu.cn (L.Z.); xiabz@sz.tsinghua.edu.cn (B.X.)
* Correspondence: su.ping@sz.tsinghua.edu.cn

Received: 25 October 2020; Accepted: 7 December 2020; Published: 10 December 2020
Abstract: Emerging technologies, such as smart wearable devices, augmented reality (AR)/virtual
reality (VR) displays, and naked-eye 3D projection, have gradually entered our lives, accompanied
by an urgent market demand for high-end display technologies. Ultra-high-resolution displays,
flexible displays, and transparent displays are all important types of future display technology,
and traditional display technology cannot meet the relevant requirements. Micro-light-emitting
diodes (micro-LEDs), which have the advantages of a high contrast, a short response time, a wide
color gamut, low power consumption, and a long life, are expected to replace traditional liquid-crystal
displays (LCD) and organic light-emitting diodes (OLED) screens and become the leaders in the next
generation of display technology. However, there are two major obstacles to moving micro-LEDs
from the laboratory to the commercial market. One is improving the yield rate and reducing the cost
of the mass transfer of micro-LEDs, and the other is realizing a full-color display using micro-LED
chips. This review will outline the three main methods for applying current micro-LED full-color
displays, red, green, and blue (RGB) three-color micro-LED transfer technology, color conversion
technology, and single-chip multi-color growth technology, to summarize present-day micro-LED
full-color display technologies and help guide the follow-up research.
Keywords: micro-LED; full-color display; mass transfer; color conversion; monolithic growth
1. Introduction
Augmented reality (AR) and virtual reality (VR) technologies are developing rapidly with the
maturity of artificial intelligence and image recognition technology. Among them, near-eye displays
(NEDs) and head-mounted displays (HMDs) are key devices for AR/VR products. At present,
mainstream near-eye displays are mostly liquid-crystal displays (LCDs) and organic light-emitting
diodes (OLEDs) [1]. However, LCDs have a slow response speed, poor conversion efficiency, and low
color saturation and are gradually being replaced by OLED displays that have the advantages of
self-luminescence, wide viewing angles, high contrast, low power consumption, and fast response
speeds. In addition, the excellent flexibility and transparency of OLEDs also provides a broad space
for emerging electronic products, such as curved displays, smart watches, and folding displays [2].
However, due to the characteristics of OLED’s organic light-emitting materials, defects, such as
their rapid aging, short life span, and low color purity, have been gradually exposed [3]. Therefore,
both LCD and OLED technologies have technical limitations and cannot perfectly adapt to the display
performance of AR/VR. Mini-LEDs and micro-LEDs, which inherited the characteristics of inorganic
LEDs and have micron-level dimensions, have become popular as the next generation of display
technology. Micro-LED technology was first proposed by a research team at Texas Tech University in
2000 [3]. The pixel pitch limit to distinguish Mini-LEDs and micro-LEDs is 100 µm, and those smaller
than 100 µm are defined as micro-LEDs [4]. With the advancement of the manufacturing process,
Nanomaterials 2020, 10, 2482; doi:10.3390/nano10122482 www.mdpi.com/journal/nanomaterials

Nanomaterials 2020, 10, 2482 2 of 33
the pixel size and pixel pitch of micro-LEDs have gradually decreased from 100 µm. In terms of
functionality, Mini-LEDs are mainly used as backlight displays [5,6], while micro-LEDs [7], which have
the advantages of a high contrast, a high response speed, a wide color gamut, low power consumption,
and a long life, are considered to be an ideal display technology for AR/VR. Table 1 provides a
comparison of micro-LED with other display technologies.
Table 1. Performance comparison of micro-light-emitting diodes (micro-LEDs) with liquid-crystal

displays (LCD) and organic light-emitting diodes (OLED).
Display Technology LCD OLED Micro-LED

Luminous mode Backlight module Self-luminous Self-luminous
Luminous efficiency Low Medium High
Brightness (cd/sqm) 3000 1000 10,000
Contrast 5000:1 10,000:1 1,000,000:1
Life (hours) 60 K 20–30 K 80–100 K
Color rendering 75% NTSC 124% NTSC 140% NTSC
Response time Millisecond level Microsecond level Nanosecond level
Energy consumption High About 60–85% of LCD About 30–40% of LCD
Pixels per inch (PPI) 800 500 >2000
NTSC—National Television Standards Committee.
The world’s first micro-LED display was launched by Sony at the 2012 Consumer Electronics
Show (CES) exhibition and was called crystal light-emitting diodes (CLED). This display has a size
of 55 inches, with unprecedented picture color, response speed, and high contrast. In the following
years, Sony officially launched this technology to the market, successfully opening the door to the
commercialization of micro-LED display technology. In 2018, Samsung showed off the world’s first
spliced 146–inch micro-LED TV, “the Wall”; X-Celeprint also demonstrated their 5.1–inch micro-LED
full-color display, and LG introduced a 175–inch micro-LED display in the same year. In 2020,
many micro-LED companies, such as Jade Bird Display, Lumiode, Plessey, PlayNitride, etc., have begun
to gradually launch their own products, and Vuzix is expected to launch its first micro-LED glasses
next year. PlayNiride also plans to build its second micro-LED production line, which will increase its
productivity by 2–3 times. It can thus be seen that micro-LED has gradually stepped onto the stage of
the display field.
In addition, micro-LEDs also have great potential in neural photosensitization [8,9], microscopic
imaging [10], flexible display backlighting [5,11], biological detection [12], cochlear implants [13],
and visible light communication (VLC) [14–17]. However, despite such excellent performance,
micro-LED display face many difficulties in their commercial mass production. The two main technical
problems of this technology are the mass transfer of LED chips [18] and the production of a full-color
display [19]. For inorganic LEDs, the size of the grown wafer is limited, usually to 4 inches or
8 inches [20]. Therefore, to realize a large-area micro-LED display, it is necessary to transfer the LED
array grown on the wafer to a circuit substrate that can drive it to illuminate. This process requires
the support of mass transfer technology. The mass transfer technologies applied to micro-LEDs
mainly include pick and place technology, self-assembly technology, and selective release and transfer
technology, each of which has its own advantages and limitations; moreover, the accuracy and yield
have a great influence on the performance of the display. A 4K full-color TV includes (3840 × 2160 × 3)
pixels. If the mass transfer technology used can guarantee a 99.99% yield, 2488 pixels may still be
damaged. This will undoubtedly increase the difficulty and cost of later maintenance. Therefore,
the yield and cost of the massive transfer limit the development of micro-LED technology to a certain extent.
Another difficulty of micro-LED displays is the realization of full color. Many teams have reported
on the development of micro-LEDs [3,21–28], but these studies only briefly describe the realization of a
full-color micro-LED solution. This review will introduce in detail the three main methods for achieving
a full-color micro-LED: (1) integrating red, green, and blue (RGB) micro-LED chips through transfer
and bonding, (2) adding a color conversion layer on a mono-color or bi-color array, and (3) directly
growing multi-color
Nanomaterials micro-LEDs
2020, 10, x FOR on the same substrate.
PEER REVIEW 3 of 33
2.
2. Chip
Chip Transfer
Transfer and
and Bonding
Bonding
The
The most
most direct
direct solution
solution to
to achieve
achieve aa full-color
full-color micro-LED
micro-LED isis to
to epitaxially
epitaxially grow
grow RGB
RGB micro-LED
micro-LED
chips on GaN and GaAs wafers. Then, through large-area and high-precision transfer
chips on GaN and GaAs wafers. Then, through large-area and high-precision transfer technology, technology,
the
the three-color micro-LEDs are bonded onto the same drive substrate to form an RGB
three-color micro-LEDs are bonded onto the same drive substrate to form an RGB micro-LED display micro-LED
display array. Independent
array. Independent addressing
addressing and Pulse
and Pulse widthwidth modulation
modulation (PWM)
(PWM) technologycan
technology can control
control the
the
brightness
brightness and
and grayscale
grayscale of
of each
each RGB
RGB pixel,
pixel,which
whichcancanrealize
realizeaafull-color
full-colorofofthe
themicro-LED
micro-LEDdisplay.
display.
2.1. Horisontally and Vertically Stacked Micro-LED Structures

2.1. Horisontally and Vertically Stacked Micro-LED Structures
There are two main arrangement structures for obtaining a full-color micro-LED array in this
There are two main arrangement structures for obtaining a full-color micro-LED array in this
way: a horizontal arrangement structure and a vertical stack structure. In 2016, Deng et al. used
way: a horizontal arrangement structure and a vertical stack structure. In 2016, Deng et al. used chips
chips on board (COB) technology to integrate RGB three-color micro-LEDs on a transparent quartz
on board (COB) technology to integrate RGB three-color micro-LEDs on a transparent quartz
substrate (LEDoTS) with addressable pixels to form a color display [29]. The display substrate area
substrate (LEDoTS) with addressable pixels to form a color display [29]. The display substrate area
was 5 × 5 mm22 , and the resolution was 5 × 5 × 3. The side length of each RGB pixel was 1 mm, and the
was 5 × 5 mm , and the resolution was 5 × 5 × 3. The side length of each RGB pixel was 1 mm, and the
emission wavelengths of the RGB three-color LEDs were 450 nm, 565 nm, and 630 nm, respectively.
emission wavelengths of the RGB three-color LEDs were 450 nm, 565 nm, and 630 nm, respectively.
The planar structure is shown in Figure 1a. Field-programmable gate array (FPGA), as the main control
The planar structure is shown in Figure 1a. Field-programmable gate array (FPGA), as the main
unit of a LEDoTS color display, controls the cathode constant current driver and the anode scan driver
control unit of a LEDoTS color display, controls the cathode constant current driver and the anode
through dynamic scanning and PWM modulation to realize the independent addressing and dimming
scan driver through dynamic scanning and PWM modulation to realize the independent addressing
of each RGB sub-pixel. Its working principle is shown in Figure 1b. In 2017, the authors used the same
and dimming of each RGB sub-pixel. Its working principle is shown in Figure 1b. In 2017, the authors
technology to develop a smaller 8 × 8 × 4 R-G-B-IR micro-LED array [30]. The dimensions of the blue,
used the same technology to develop a smaller 8 × 8 × 4 R-G-B-IR micro-LED array [30]. The
green, red, and infrared LEDs were 230 µm × 385 µm, 210 µm × 210 µm, 225 µm × 225 µm, and 285 µm
dimensions of the blue, green, red, and infrared LEDs were 230 μm × 385 μm, 210 μm × 210 μm, 225
× 285 µm, respectively. The peak wavelengths of the emission spectrum were 460 nm, 572 nm, 630 nm,
μm × 225 μm, and 285 μm × 285 μm, respectively. The peak wavelengths of the emission spectrum
and
were850
460nm,
nm,and
572the maximum
nm, 630 nm, andhalf-wavelength wasmaximum
850 nm, and the less than 30 nm.
half-wavelength was less than 30 nm.
Figure 1.1.(a)
Figure (a)Horizontally
Horizontallyarranged
arranged red,
red, green,
green, and,and,
blueblue
(RGB)(RGB) three-color
three-color light-emitting
light-emitting diodesdiodes
(LED)
(LED)plane
pixel pixelstructure;
plane structure; (b) horizontally
(b) horizontally arranged
arranged RGB RGB micro-LED
micro-LED array workingarray working
principle. principle.
Reproduced
Reproduced
from from
[29], with [29], withfrom
permission permission
Institutefrom Instituteand
of Electrical of Electrical
Electronicsand Electronics
Engineers, Engineers, 2016.
2016.
Vertically
Verticallystacked
stackedLED
LEDstructures
structures have
havebeen
beenstudied
studiedfor for
a long period
a long of time
period [31,32].
of time For micro-LED
[31,32]. For micro-
displays with high
LED displays with resolution on a limited
high resolution substrate,
on a limited the area
substrate, theof theof
area substrate occupied
the substrate by each
occupied by RGB
each
pixel
RGB of the of
pixel vertically stackedstacked
the vertically RGB micro-LED array is reduced
RGB micro-LED array is by 2/3 compared
reduced to the horizontal
by 2/3 compared to the
arrangement structure. In
horizontal arrangement 2017, Kang
structure. et al.Kang
In 2017, proposed
et al. aproposed
color-tunable display composed
a color-tunable of blue and
display composed of
green passive
blue and greenmatrix micro-LED
passive matrix arrays
micro-LEDstacked vertically
arrays stacked[33].vertically
This display
[33].array
This can independently
display array can
address each pixel,
independently and, each
address by modulating
pixel, and,theby PWM duty cycles
modulating the PWMof theduty
bluecycles
or green micro-LED
of the blue or drive
green
voltages, the light-emitting wavelengths of each pixel can be changed from 450 nm
micro-LED drive voltages, the light-emitting wavelengths of each pixel can be changed from 450 nm to 540 nm, as shown
in
to Figure
540 nm, 2a.as shown in Figure 2a.
The
The preparation
preparation of of this
this array
array is
is shown
shown in in Figure
Figure 2b.2b. Blue
Blue and
and green
green micro-LEDs
micro-LEDs are are grown
grown on on
double-side-polished
double-side-polished(DSP) (DSP)sapphire.
sapphire. After that,
After the the
that, entire wafer
entire is decomposed
wafer is decomposedinto individual pixels
into individual
pixels with sizes of 75 μm × 75 μm by inductively coupled plasma (ICP) etching, and each pixel chip
is bonded onto the receiving substrate through mass transfer technology. Each sub-pixel is connected
with a metal cross line, and the column line and the row line are electrically isolated. The green
passive matrix in the lower layer needs to be slightly larger than the blue passive matrix in the upper
layer (their dimensions are 0.8 × 0.8 cm2 and 1.2 × 1.2 cm2, respectively). Finally, after accurately
with sizes of 75 µm × 75 µm by inductively coupled plasma (ICP) etching, and each pixel chip is
bonded onto the receiving substrate through mass transfer technology. Each sub-pixel is connected
with a metal cross line, and the column line and the row line are electrically isolated. The green
passive matrix in the lower layer needs to be slightly larger than the blue passive matrix in the upper
Nanomaterials 2020, 10, x FOR PEER REVIEW 4 of 33
layer (their dimensions are 0.8 × 0.8 cm2 and 1.2 × 1.2 cm2 , respectively). Finally, after accurately
aligning
aligning each
each pixel
pixel ofof the
the two
two arrays,
arrays, thethe photoresist
photoresist isis used
used for for bonding
bonding under
under aa temperature
temperature of of
250 ◦ C and a pressure of 1 kg/cm22. The device has a transmittance of 63% and four modes: (1) green
250 °C and a pressure of 1 kg/cm . The device has a transmittance of 63% and four modes: (1) green
independent
independentlight lightemission,
emission,(2) (2)blue
blueindependent
independentlight lightemission,
emission,(3) (3)blue
blueandandgreen
greenlight
lightemission
emissionin in
different positions, and (4) blue and green light emission in the same pixel
different positions, and (4) blue and green light emission in the same pixel position superimposed. position superimposed.
The
Theresults
resultsofofthetheoptical
opticalperformance
performance tests of these
tests of thesefourfour
modes
modes are shown
are shownin Figure 2c. When
in Figure only blue
2c. When only
light
blue is emitted,
light the peak
is emitted, of its of
the peak electroluminescence
its electroluminescence (EL) spectrum
(EL) spectrumis at aiswavelength of 450ofnm,
at a wavelength 450and,
nm,
when only green light is emitted, the peak of its EL spectrum is at a wavelength
and, when only green light is emitted, the peak of its EL spectrum is at a wavelength of 540 nm. Each of 540 nm. Each pixel
of the device
pixel can be addressed
of the device independently,
can be addressed and the light
independently, and ofthedifferent
light ofwavelengths can be emitted
different wavelengths can at
be
different
emitted at pixels at thepixels
different same time.
at theItsame
is also possible
time. to adjust
It is also the PWM
possible duty
to adjust thecycle
PWM at the
dutysame pixel
cycle to
at the
change
same pixelthe emission
to changewavelength
the emission from 450 nm tofrom
wavelength 540 nm.450 However,
nm to 540 the nm.performance
However, the ofperformance
such verticallyof
stacked LEDs is severely
such vertically stacked limited
LEDs is by severely
the light absorption
limited by and thepoorlightthermal conductivity
absorption and poor of adjacent
thermal
narrow-band
conductivity gap quantum
of adjacent wells (QWs).
narrow-band gap quantum wells (QWs).
Figure2.2. (a)
Figure (a) Electroluminescence
Electroluminescence (EL)
(EL) spectra
spectra measured
measured byby changing
changing the
the Pulse
Pulsewidth
widthmodulation
modulation
(PWM)
(PWM) duty ratios of the green sub-pixels and blue sub-pixels, and microscope images at
duty ratios of the green sub-pixels and blue sub-pixels, and microscope images atthe
thesame
same
pixel positions of the micro-LED array under different PWM duty ratios; (b) manufacturing
pixel positions of the micro-LED array under different PWM duty ratios; (b) manufacturing steps of steps
of vertically stacked passive matrix micro-LED arrays; (c) four emission modes of vertically stacked
vertically stacked passive matrix micro-LED arrays; (c) four emission modes of vertically stacked
passive matrix micro-LED arrays. Reproduced from [33], The Optical Society, 2017.
passive matrix micro-LED arrays. Reproduced from [33], The Optical Society, 2017.
In 2020, Ostendo introduced a multi-color addressable micro-LED display—the Quantum Photonic

In 2020, Ostendo introduced a multi-color addressable micro-LED display—the Quantum
Imager (QPI), with a vertical structure to produce a full-color micro-LED display [34]. The pixel pitch
Photonic Imager (QPI), with a vertical structure to produce a full-color micro-LED display [34]. The
of the RGB three-color micro-LED chips are less than 10 µm, where the blue and green layers are based
pixel pitch of the RGB three-color micro-LED chips are less than 10 μm, where the blue and green
on GaN, as well as the red layers are based on AlInGaP. The RGB three-color single chips are stacked
layers are based on GaN, as well as the red layers are based on AlInGaP. The RGB three-color single
on the same substrate (from top to bottom: red, green, and blue) through wafer-wafer fusion bonding
chips are stacked on the same substrate (from top to bottom: red, green, and blue) through wafer-
techniques, and the RGB light emitting shares the same optical aperture. The micro-LED RGB array is
wafer fusion bonding techniques, and the RGB light emitting shares the same optical aperture. The
controlled by the underlying silicon Complementary Metal Oxide Semiconductor (CMOS) substrate,
micro-LED RGB array is controlled by the underlying silicon Complementary Metal Oxide
which can provide digital control logic and power for each pixel RGB micro-LED. Through PWM
Semiconductor (CMOS) substrate, which can provide digital control logic and power for each pixel
modulation, color correction, luminance correction, and uniformity correction, electrical and optical
RGB micro-LED. Through PWM modulation, color correction, luminance correction, and uniformity
information are transmitted in multiple bonding interfaces of the stack structure so that the multicolor
correction, electrical and optical information are transmitted in multiple bonding interfaces of the
emissions and displays of a single vertical structure chip can be realized. The vertical structure of
stack structure so that the multicolor emissions and displays of a single vertical structure chip can be
the micro-LED RGB array first needs RGB three-color micro-LED chips to be separately epitaxially
realized. The vertical structure of the micro-LED RGB array first needs RGB three-color micro-LED
grown to prepare wafers of the same size with a pitch of 5–10 µm. The three processed wafers are then
chips to be separately epitaxially grown to prepare wafers of the same size with a pitch of 5–10 μm.
sequentially bonded to the same drive substrate, and the alignment accuracy between the bonded
The three processed wafers are then sequentially bonded to the same drive substrate, and the
alignment accuracy between the bonded wafers is better than 1 μm each time. Afterward, the
substrate and part of the P- or N-doped layer are removed by laser lift-off technology or grinding and
wet etching technology (depending on the growth substrate). Finally, the RGB three-color wafers are
bonded by wafer–wafer fusion technology. A QPI display has the advantages of full color, high
resolution, high brightness, high contrast, and low power consumption, and its vertical structure
wafers is better than 1 µm each time. Afterward, the substrate and part of the P- or N-doped layer are
removed by laser lift-off technology or grinding and wet etching technology (depending on the growth
substrate). Finally, the RGB three-color wafers are bonded by wafer–wafer fusion technology. A QPI
display has the advantages of full color, high resolution, high brightness, high contrast, and low power
consumption, and its vertical structure enables it to achieve higher pixel density on small size displays,
which is very suitable for wearable AR/VR devices.
At present, RGB micro-LED chips can be accurately and efficiently transferred from one substrate
to another through multiple transfer methods, such as elastomer stamp technology, laser induction
technology, fluid transportation technology, electrostatic transfer technology, and roll-to-roll
(roll-to-panel) technology. In the following, we briefly describe these methods for micro-LED mass
transfer and analyze their theory, features, and application scope.
2.2. Elastomer Stamp Transfer

Elastomer stamp transfer technology can transfer a large number of microstructures from one
substrate to another at high speed [35–38]. Rogers’ team initially used elastomer stamps for large-scale
transfer printing [11]. This technology closely contacts the micro devices on the donor substrate with
an elastomer stamp array matching the pitch of the micro devices on the donor substrate. Through the
van der Waals force between the elastomer stamp and the latter, the micro device is picked up
and transferred to the receptor substrate. The picking and placing of the elastomer stamp on the
microstructure are determined by the peeling speed after the two contact each other. By pulling the
stamp away from the donor substrate at a sufficiently high peeling speed (usually faster than 10 cm/s),
the elastomer stamp can generate strong adhesive force to adhere the microstructure to the surface
of the stamp and remove the target device from the donor substrate. When the peeling speed of the
stamp is less than 1 mm/s, the microstructure will be separated from the stamp and remain on the
receptor substrate instead of being adsorbed by the stamp.
In 2005, Lee et al. proposed two elastomer stamp transfer methods that can realize the selective
transfer of thin film transistors (TFT) to rigid or flexible substrates [39]. The transfer processes of
these two methods are shown in Figure 3. The first method uses polydimethylsiloxane (PDMS) as an
elastomer stamp, which comes into contact with the micro-silicon structure on the silicon-on-insulator
(SOI). Due to the strong automatic adhesion of the PDMS, the Si microstructure in the corresponding
area of the protruding PDMS part will be selectively detached from the SOI surface. After that,
the PDMS part comes into contact with a polyethylene terephthalate (PET) receiving plate coated with
polyurethane (PU), and then ultraviolet/ultraviolet ozone (UV/UVO) exposure is performed on the
PET side to fully cure the PU and strengthen its bond with the Si microstructure. Lastly, the PDMS is
peeled off, and the microstructures are bonded. The second method is to use decal-transfer lithography
(DTL) technology based on method one, using a flat, unmolded PDMS plate for selective transfer.
The adhesion strength of the plate is enhanced by photochemical treatment. Afterward, selective
masking and an UVO treatment are performed on the surface of the PDMS plate. By exposing the
plate, the PDMS coating with changed photochemical properties comes into contact with the SOI wafer
and is heated to 70 ◦ C for 30 min. Finally, the PDMS is stripped from the SOI, thereby selectively
transferring the Si microstructure from the SOI wafer to the plate with the PDMS.
The elastomer stamp has excellent flexibility and stickiness, allowing it to make large-area physical
contact on the surface of an incompletely flat substrate and transfer fragile, thin, and micro-scale
devices without damaging the devices. Therefore, elastomer stamp transfer technology can transfer
micro-LED chips from one substrate to another in a cost-effective manner. Moreover, the substrate of
the stamp is usually a rigid material (such as glass), which can make it difficult to bend in the lateral
dimension and reduce lateral deformation, thereby obtaining good transfer yield and accuracy. In 2017,
Radauscher et al. used elastomer stamp technology to manufacture active and passive color micro-LED
arrays and proved that this method has a high transfer yield greater than 99.99% [11]. In 2019, Kim et al.
found that elastomer stamp transfer technology controls the adhesion force of the stamp by changing
two methods are shown in Figure 3. The first method uses polydimethylsiloxane (PDMS) as an
elastomer stamp, which comes into contact with the micro-silicon structure on the silicon-on-
insulator (SOI). Due to the strong automatic adhesion of the PDMS, the Si microstructure in the
corresponding area of the protruding PDMS part will be selectively detached from the SOI surface.
After that, the PDMS part comes into contact with a polyethylene terephthalate (PET) receiving plate
coated with polyurethane (PU), and then ultraviolet/ultraviolet ozone (UV/UVO) exposure is
performed on the PET side to fully cure the PU and strengthen its bond with the Si microstructure.
the contact
Lastly, force is
the PDMS or peeled
peelingoff,
speed
and ofthethe polymer stamp
microstructures arebut has a The
bonded. problem of method
second repeatability [40].
is to use
Therefore, the authors chose to use a magnetorheological elastomer as the stamp
decal-transfer lithography (DTL) technology based on method one, using a flat, unmolded PDMS and controlled the
adsorption
plate force bytransfer.
for selective changing theadhesion
The magneticstrength
field nearofthe
thestamp
plateduring the transfer.
is enhanced This method
by photochemical
successfully
treatment. optimized
Afterward, the elastomer
selective maskingstamp
and an transfer technology.
UVO treatment are In 2020, Lu on
performed et the
al. optimized the
surface of the
micro-LED elastomer stamp transfer technology using the support vector machine
PDMS plate. By exposing the plate, the PDMS coating with changed photochemical properties comes (SVM) model [41].
Thecontact
into results showed
with thethatSOI the SVM
wafer andmodel and atolarge
is heated 70 °Cnumber of transfer
for 30 min. Finally,signal feature
the PDMS is databases offer
stripped from
85%SOI,
the classification predictiontransferring
thereby selectively accuracy forthethe Si
elastomer stamp transfer
microstructure from the process, which
SOI wafer tocan
thesignificantly
plate with
improve
the PDMS.the transfer efficiency of elastomer stamp transfer technology.
Figure3.
Figure (a) The transfer
3. (a) transferprinting
printingstep using
step polydimethylsiloxane
using (PDMS)
polydimethylsiloxane and and
(PDMS) (b) the
(b)elastomer stamp
the elastomer
transfer step using decal-transfer lithography (DTL) technology. Reproduced from [39], with permission
stamp transfer step using decal-transfer lithography (DTL) technology. Reproduced from [39], with
from John Wiley
permission and Sons,
from John Wiley2005.
and Sons, 2005.
2.3. Laser-Induced Transfer

Laser-induced forward transfer (LIFT) is a high-resolution single-step direct printing technology.
LIFT can achieve surface micro-patterning or the partial deposition of solid or liquid materials
and is widely used in selective printing of electronic devices, such as organic TFT, OLED,
Micro-Electro-Mechanical System (MEMS), and sensors [42,43]. The steps for transferring solid-state
pixels are shown in Figure 4a. The transfer of solid-state pixels is done to irradiate a thin layer
of absorbing material deposited on a transparent substrate with a pulsed laser. After irradiation,
light–matter interactions occur at the interface between the substrate and the absorbing material,
causing the local pressure of the irradiated area to increase rapidly. In this way, a small pixel on
the absorbing material film is separated from the donor substrate and deposited on the opposite
receiving substrate. Because the size and shape of the emitted material are controlled by the size
and shape of the incident laser spot, LIFT can not only deposit typically sized devices but can also
transfer microstructures.
In 2013, on the basis of LIFT technology, Uniqarta introduced Massively Parallel Laser-Enabled
Transfer (MPLET) technology to realize the large-scale transfer of a micro-LED [44]. MPLET technology
is based on the single-beam laser transmission process, and its working principle is shown in Figure 4b.
The micro-LEDs are deposited on a glass substrate plated with a dynamic release layer (DRL). When an
ultraviolet (UV) beam irradiates a certain area of the substrate, bubbles will be generated between the
substrate and the DRL layer. Under the force of bubble expansion and gravity, the micro devices will
be transferred to the receiving substrate with a pitch of 10–300 µm. After that, the MPLET technology
uses a diffractive optical element to diffract a single laser beam into multiple sub-beams, the number of
which depends on the laser power, as shown in Figure 4c. Each sub-beam corresponds to the transfer
of a micro-LED. In this way, the micro-LEDs can be transferred in batches under one irradiation,
which greatly shortens the process of single beam scanning transmission. At present, the transfer
speed of MPLET technology for large panels can reach 100 M units/hour, and the transfer speed of
Nanomaterials
small panels2020,
can10, x FOR PEER
exceed 500 MREVIEW
units/hour, with a transfer accuracy of ±34 µm. 7 of 33
Figure 4. (a)(a)Principle
Principleof laser-induced forward transfer technology. Reproduced from from
[43], with
Figure 4. (a) Principle of of laser-induced
laser-induced forward
forward transfer
transfer technology.
technology. Reproduced
Reproduced [43],
from [43], with
permission
with from
permission Elsevier, 2016; (b) principle of massively parallel laser transmission technology
permission fromfrom Elsevier,
Elsevier, 2016;
2016; (b)(b) principle
principle of ofmassively
massivelyparallel
parallellaser
laser transmission
transmission technology
launched by
launched by Uniqarta
Uniqarta and
and (c)
(c) Massively
Massively Parallel
Parallel Laser-Enabled Transfer (MPLET)
(MPLET) technology thatthat
Massively Parallel Laser-Enabled Transfer
Transfer (MPLET) technology
technology
uses diffractive
uses diffractive optical
diffractive optical elements
optical elements to transmit
elementstototransmit multiple
transmitmultiple
multiple pixels in
pixels parallel. Reproduced
in parallel. from
Reproduced [44], with
pixels in parallel. Reproduced from from [44],
[44], with
permission
with fromfrom
permission John John
Wiley and Sons,
Wiley and 2018.2018.
Sons,
permission from John Wiley and Sons, 2018.
2.4. Fluidically Self-Assembled Transfer

2.4. Fluidically Self-Assembled TransferTransfer
Fluidically Self-Assembled (FSA) technology can freely assemble microstructures on a substrate
Fluidically Self-Assembled (FSA) technology can freely assemble microstructures on a substrate
in aa large area with a simple operation and offers a small interconnection parasitic effect compared to
in a large area
large area with
with aa simple
simple operation
operation andand offers
offers aa small
small interconnection
interconnection parasitic
parasitic effect
effect compared
compared
other
to transfer methods. In 1994, Yeh et al. realized the transfer of trapezoidal GaAs LED devices from
to other transfer methods. In 1994, Yeh et al. realized the transfer of trapezoidal GaAs LED devices
other transfer methods. In 1994, Yeh et al. realized the transfer of trapezoidal GaAs LED devices
afrom
growth wafer wafer to an Si substrate via FSA [45,46], the processprocessof which is shown shown
in Figure 5a. To use
from aa growth
growth wafer to to an
an SiSi substrate
substrate via
via FSA
FSA [45,46],
[45,46], thethe process of of which
which is is shown in in Figure
Figure 5a.
5a.
FSA
To technology to transfer microstructures, the first step is tostep
use is
photolithography to etch antoinverted
To use FSA technology to transfer microstructures, the first step is to use photolithography to etch an
use FSA technology to transfer microstructures, the first to use photolithography etch an
trapezoidal
inverted hole with a certain inclination inclination
on the silicon substrate and then deposit an Al-Cr-Sn contact
inverted trapezoidal
trapezoidal holehole with
with aa certain
certain inclination on on the
the silicon
silicon substrate
substrate andand then
then deposit
deposit an an Al-
Al-
layer
Cr-Sn on the hole bottom as a receiving substrate forsubstrate
the chip transfer. Then, trapezoidal LED chips
Cr-Sn contact
contact layer
layer onon the
the hole
hole bottom
bottom asas aa receiving
receiving substrate for for the
the chip
chip transfer.
transfer. Then,
Then, trapezoidal
trapezoidal
are
LED grown on the GaAs wafer via molecular beam epitaxy (MBE), and a Cr-Ni barrier layer and Au
LED chips are grown on the GaAs wafer via molecular beam epitaxy (MBE), and a Cr-Ni barrier layer
chips are grown on the GaAs wafer via molecular beam epitaxy (MBE), and a Cr-Ni barrier layer
contact
and layer arelayer
depositeddeposited
on the n-doped GaAs layer for subsequent bonding with the Siwith substrate.
and AuAu contact
contact layer are are deposited on on the
the n-doped
n-doped GaAsGaAs layerlayer forfor subsequent
subsequent bonding
bonding with the the Si
Si
Afterwards,
substrate. the disperseddispersed
micro-LED devices flow through through
the Si substrate via the ethanol carrier
substrate. Afterwards,
Afterwards, the the dispersed micro-LED
micro-LED devicesdevices flowflow through the the Si
Si substrate
substrate viavia the
the ethanol
ethanol
liquid.
carrier Because the substrate has inverted trapezoidal holes, holes, under the action of gravity and fluid
carrier liquid.
liquid. Because
Because thethe substrate
substrate has
has inverted
inverted trapezoidal
trapezoidal holes, under under thethe action
action ofof gravity
gravity andand
vibration,
fluid the micro-LED devices in the carrier liquid can be accurately captured. After theAfter Au layersAu of
fluid vibration,
vibration, the the micro-LED
micro-LED devices
devices inin the
the carrier
carrier liquid
liquid can can be
be accurately
accurately captured.
captured. After the the Au
the LED
layers of come
the intocome
LED contact
intowith the Al-Cr-Sn
contact with the layers
Al-Cr-Snon the bottom
layers on of the
the Si substrate’s
bottom of the Si holes, by heating
substrate’s holes,
layers of the LED come into contact with the Al-Cr-Sn layers on the bottom of the Si substrate’s holes,
the
by substrate, the temperaturetemperature
of Sn becomes Sn higher than its melting point, allowing the allowing
Sn to diffuse
by heating
heating the the substrate,
substrate, thethe temperature of of Sn becomes
becomes higherhigher thanthan itsits melting
melting point,
point, allowing the the
to
Sn the diffuse
Au and form an alloy with the Au. Finally, throughFinally,
cooling, the bottom of the micro-LEDs and
Sn to
to diffuse to to the
the Au
Au and
and form
form anan alloy
alloy with
with the
the Au.
Au. Finally, throughthrough cooling,
cooling, the the bottom
bottom of of the
the
the Si substrate base
micro-LEDs aresubstrate
solidified to complete the bonding.
micro-LEDs and and the
the Si
Si substrate basebase are
are solidified
solidified to to complete
complete the the bonding.
bonding.
Figure 5. (a)(a)The
Figure 5. Theloading
loading process
process of of fluid
fluid self-assembly
self-assembly technology.
technology. Reproduced
Reproduced from from [45],
[45], with
Figure
with 5. (a) Thefrom
permission loading process
Institute of fluidand
of Electrical self-assembly
Electronicstechnology. Reproduced
Engineers, 1994; fromdiagram
(b) Principle [45], with
of
permission from Institute of Electrical and Electronics Engineers, 1994; (b) Principle diagram of
permission from
electrostatic Institute
transfer of Electrical
technology [47]. and Electronics Engineers, 1994; (b) Principle diagram of
electrostatic transfer technology [47].
electrostatic transfer technology [47].
In
In 2007,
2007, Ehsan
Ehsan Saeedi
Saeedi et
et al.
al. used
used FSA
FSA technology
technology to
to transfer
transfer micro-LEDs
micro-LEDs grown
grown onon AlGaAs
AlGaAs
substrates
substrates to
to flexible
flexible substrates
substrates [48].
[48]. In
In their
their latest
latest experiment,
experiment, the
the authors
authors were
were able
able to
to achieve
achieve aa
yield
yield of
of 65%
65% byby placing
placing the
the LED
LED atat the
the correct
correct binding
binding site
site through
through FSA
FSA technology.
technology. The
The main
main
In 2007, Ehsan Saeedi et al. used FSA technology to transfer micro-LEDs grown on AlGaAs
substrates to flexible substrates [48]. In their latest experiment, the authors were able to achieve a yield
of 65% by placing the LED at the correct binding site through FSA technology. The main problems in
reducing the yield are solder changes of the metal contact on the LED and the rapid degradation of
solder on the contact pad in an acidic environment.
Although FSA technology can place scattered microstructures on the receiving substrate compactly
and on a large scale, this technology also has many defects in the integration process. FSA technology
has imposed strict requirements for the carrier solution and bonding material when transferring
micro devices, which will limit its application scope to a certain extent. Moreover, due to the
manufacturing process of the microstructure and the material properties of the substrate, the transferred
microstructure may not match the holes of the receiving substrate. In addition, determining how
to bond more effectively after the microstructure enters the hole represents another area for FSA’s
subsequent optimization.
2.5. Electrostatic Transfer

Electrostatic transfer technology was proposed by the LuxVue company in 2012, who successfully
fabricated a micro device array using the electrostatic transfer method. The working principle of this
method is shown in Figure 5b [47]. By applying a voltage to a silicon electrostatic head, the electrostatic
transfer head array picks up the micro device array from the carrier substrate via a charged adsorption
force. After that, the receiving substrate is brought into contact with the micro device array, and the
control voltage of the electrostatic transfer head is removed, thereby releasing the micro device array
onto the receiving substrate. The advantage of the electrostatic transfer technology is that it can
selectively transfer individual components or parts of components, and the pitch of the transfer
electrostatic head array and the pitch of the micro-LED on the receiving substrate need not be the same,
so the transfer is very flexible. However, the voltage applied to the transfer head during electrostatic
induction can produce a charging phenomenon, which may damage the micro-LEDs.
2.6. Roll-to-Roll or Roll-to-Panel Imprinting Transfer

Roll-to-roll (R2R) or roll-to-panel (R2P) imprinting technology can realize low-cost,
high-throughput, and high-efficiency micro-device imprinting or patterning on flexible substrates
or rigid substrates [49–51]. The whole system includes two embossing rollers and a conveyor belt
supported by the two rollers, which can ensure that the system has a larger curing surface and a
constant curing pressure, thereby speeding up the transfer of micro devices. In 2013, Korea institute
of machinery & materials developed an R2R transmission system that can control the contact load
in real time and transfer In-Ga-Zn-O (IGZO) TFTs from rigid substrates to flexible substrates [50].
The R2R transfer speed can be maintained at 1 mm/s and can effectively prevent the device from
breaking due to fluctuations in the load contact during the transfer process of the film structure.
In 2017, KIMM demonstrated an R2R transfer printing process suitable for micro-LEDs and successfully
fabricated an active matrix micro-LED flexible display driven by TFT [51]. The whole embossing
process is divided into three stages, as shown in Figure 6. First, the Si-TFT array is transferred from the
silicon-on-insulator (SOI) growth wafer to the transition substrate through the first R2R. Then, in the
second R2R, the micro-LED is transferred from the GaAs substrate to the transition substrate. Finally,
after the two are bonded, both are transferred from the transition substrate to the flexible substrate
through the third R2R to integrate the active matrix light emitting diode (AMLED) display.
The entire transfer process is performed by an automatic R2R transfer device with an overlay
alignment function, and the transfer rate of the Si-TFT and micro-LED is close to 99.9%. By using two
microscopes for precise position matching, the entire system can maintain a precise alignment of up to
3 µm. However, the maximum mechanical stretch ability of the flexible display prepared by this system
can only reach 40%, and, when the TFT is measured on a soft stretchable substrate, the hard probe can
easily tear the electrode, which will cause its electrical performance to decrease. These defects can be
further improved by using optimized interconnected structures or reduced pixel sizes.
Figure6.6.Schematic
Figure Schematicdiagram
diagramofofthe
thesteps
stepsfor
forassembling
assemblingaaflexible
flexibleAMLED
AMLEDdisplay
displayusing
usingthree-roll
three-roll
transfertechnology.
transfer technology.Reproduced
Reproducedfrom
from[51],
[51],with
withpermission
permissionfrom
fromJohn
JohnWiley
Wileyand
and Sons,
Sons, 2017.
2017.
2.7. Summary
The entire transfer process is performed by an automatic R2R transfer device with an overlay
alignment function,
In summary, andtransfer
Mass the transfer rate of has
technology the Si-TFT and micro-LED
great limitations in bothis equipment
close to 99.9%.
andBy using two
technology.
microscopes for precise position matching, the entire system can maintain a precise
As the size of micro-LEDs decreases, the accuracy of the transfer equipment, the matching degree alignment of up
to 3 μm. However, the maximum mechanical stretch ability of the flexible display
of the transfer head, and the high cost of equipment investment make the mass transfer technology prepared by this
system can
difficult only reach
to improve. The40%, and, whencapacity,
production the TFT yield,
is measured
bad dies on detection
a soft stretchable substrate, the
and maintenance willhard
all
probe can easily tear the electrode, which will cause its electrical performance to decrease.
affect the transfer cost. To prepare a 4K full-color micro-LED display, the resolution is 3840 × 2160, These
defects
and eachcan bemust
pixel further
be improved
composedby of using optimized
three RGB colors.interconnected structures
Therefore, 22,550,400 or reduced
micro-LED pixel
chips needsizes.
to
be correctly transferred and bonded to the driving substrate, which is very demanding for current
2.7. Summary
mass transfer technology. Fluid self-assembly technology is suitable for low cost and large spacing
micro-LED. However,
In summary, Mass until its low
transfer transfer efficiency
technology has greatand unstable
limitations inbonding methodsand
both equipment are technology.
improved,
FSA cansize
As the onlyofstay in lab. Indecreases,
micro-LEDs contrast, elastomer
the accuracy stamp transfer
of the transfertechnology,
equipment, with
theits unique degree
matching soft andof
sticky characteristics, can efficiently transfer micro-devices to rigid or
the transfer head, and the high cost of equipment investment make the mass transfer technology flexible substrates. Therefore, it is
the most commonly used mass transfer technology at present. Both laser-induced
difficult to improve. The production capacity, yield, bad dies detection and maintenance will all affect transfer technology
and
the electrostatic
transfer cost.transfer
To prepare technology have good
a 4K full-color repeatability,
micro-LED display, which greatly reduces
the resolution is 3840the transfer
× 2160, andcost.
each
Poor repeatability is a weak point of stamp transfer technology that
pixel must be composed of three RGB colors. Therefore, 22,550,400 micro-LED chips need to be cannot be ignored. And the high
precision
correctlyof LIFT makes
transferred and it bonded
even more prominent
to the in the facewhich
driving substrate, of ultra-small spacing micro-LED
is very demanding for current arrays.
mass
The advantage
transfer of R2RFluid
technology. technology lies in its
self-assembly large throughput.
technology is suitable Forforthe
lowfuture production
cost and of large-size
large spacing micro-
micro-LED
LED. However, displays,
until itsits
advantages
low transfer are efficiency
obvious. Various transferbonding
and unstable technologies
methodsare trying to efficiently
are improved, FSA
and
canaccurately
only stay intransfer
lab. Inmicro-LEDs from thestamp
contrast, elastomer growth wafer to
transfer the drive substrate.
technology, Table 2soft
with its unique summarizes
and sticky
and compares the
characteristics, canmainstream technologies
efficiently transfer currentlytoused
micro-devices rigidfor the mass
or flexible transfer of
substrates. micro-devices.
Therefore, it is the
By comparison, we are concerned that elastomer stamp transfer technology
most commonly used mass transfer technology at present. Both laser-induced transfer technology is still the main transfer
method for the future
and electrostatic microtechnology
transfer and small devices.
have good Replacing the conventional
repeatability, which greatly stamp transfer
reduces thehead withcost.
transfer an
electromagnetic head or other flexible head to improve its repeatability has
Poor repeatability is a weak point of stamp transfer technology that cannot be ignored. And the high been proven to be a feasible
solution,
precisionwhich improves
of LIFT makes it the reliability
even of the stamp
more prominent transfer
in the face of technology
ultra-small and reduces
spacing its transfer
micro-LED cost.
arrays.
However, manufacturers
The advantage still need to
of R2R technology choose
lies in its the appropriate
large throughput. transfer
For the technology accordingoftolarge-size
future production the cost
performance and application
micro-LED displays, scenarios.
its advantages are obvious. Various transfer technologies are trying to efficiently
and accurately transfer micro-LEDs from the growth wafer to the drive substrate. Table 2 summarizes
and compares the mainstream technologies currently used for the mass transfer of micro-devices. By
comparison, we are concerned that elastomer stamp transfer technology is still the main transfer
method for the future micro and small devices. Replacing the conventional stamp transfer head with
an electromagnetic head or other flexible head to improve its repeatability has been proven to be a
feasible solution, which improves the reliability of the stamp transfer technology and reduces its
transfer cost. However, manufacturers still need to choose the appropriate transfer technology
according to the cost performance and application scenarios.
Table 2. Comparison of various mass transfer technologies.
Mass
Nanomaterials
Transfer
Transfer 2020, 10, 2482 Advantage Disadvantage10 of 33
Performance
Method
Softnessofand
Table 2. Comparison stickiness
various of elastomer
mass transfer technologies.
Elastomer Transfer yield stamp ensure that it can transfer the
Mass Transfer Method Transfer Performance Advantage Poor Disadvantage
repeatability.
stamp in 99.99% microstructures in an economical and
Softness and stickiness of elastomer stamp
efficient way.
ensure that it can transfer the
Elastomer stamp Transfer yield in 99.99% Poor repeatability.
High resolution and impurities
microstructures will and The transfer
in an economical stability is
Laser-induced ≤500 million efficient way.
not be introduced on the substrate affected by the laser
transfer units/hour
surface.and impurities will not be The transfer
High resolution source. stability is
Laser-induced transfer ≤500 million units/hour affected by the
Transfer yield Easy to operate, introduced
smallonparasitic
the substrate surface. Low transfer efficiency
effects laser source.
FSA transfer
in 65% and
Easy low cost.
to operate, small parasitic effects and andtransfer
Low accuracy.
efficiency
FSA transfer Transfer yield in 65%
low cost. and accuracy.
Electrostatic phenomena
Electrostatic ~1 Electrostatic
can damage phenomena
Electrostatic transfer ~1 million/hourFlexible andFlexible
goodand repeatability.
good repeatability.
can damage
transfer million/hour microdevices;
microdevices; small
small
transferarea.
transfer area.
R2R (R2P) Transfer yieldyield inLow

Transfer cost, highLow
~99.9%
cost, high throughput
throughput and high and It can
It can damage larger
damage larger
R2R (R2P) high efficiency. microdevices.
in ~99.9% efficiency. microdevices.
In
In addition,
addition,since
sincethe
thegrowth
growthmaterials
materials of of
blue andand
blue green LEDs
green are based
LEDs on GaN,
are based but the
on GaN, red
but LEDs
the red
are based on GaAs or GaP. Therefore, different growth materials lead to different performance
LEDs are based on GaAs or GaP. Therefore, different growth materials lead to different performance of RGB
micro-LEDs in terms ofintemperature,
of RGB micro-LEDs lifetime and driving
terms of temperature, lifetimevoltage. Using unprocessed
and driving voltage. Using general-purpose
unprocessed
drivers will cause the output current of the driver circuit to have a certain deviation
general-purpose drivers will cause the output current of the driver circuit to have a certain from the theoretical
deviation
current, which will yield color differences in the micro-LED display. To ensure the
from the theoretical current, which will yield color differences in the micro-LED display. To ensure uniformity of the
full-color micro-LED display, specific driving conditions need to be established for that
the uniformity of the full-color micro-LED display, specific driving conditions need to be established display, which
makes
for thatthedisplay,
integration
which process
makestoothe
complicated.
integrationTherefore,
process before the breakthrough
too complicated. of mass
Therefore, transfer
before the
technology, the use of the same material or substrates to grow RGB three-color micro-LEDs
breakthrough of mass transfer technology, the use of the same material or substrates to grow RGB would be
the best solution to achieve full-color displays.
three-color micro-LEDs would be the best solution to achieve full-color displays.
3. Color Conversion Technology
3. Color Conversion Technology
Color conversion technology is a method that can realize a full-color micro-LED display without
Color conversion technology is a method that can realize a full-color micro-LED display without
a mass transfer and is utilized in two main ways. One is to use a UV or blue micro-LED array as the
a mass transfer and is utilized in two main ways. One is to use a UV or blue micro-LED array as the
excitation light source and place colored phosphors, quantum dots (QDs), or other light-emitting nano
excitation light source and place colored phosphors, quantum dots (QDs), or other light-emitting
organic materials onto an RGB color conversion layer covering the micro-LED light source to achieve
nano organic materials onto an RGB color conversion layer covering the micro-LED light source to
multi-wavelength light emissions, as shown in Figure 7. If the UV micro-LED is the light source, it is
achieve multi-wavelength light emissions, as shown in Figure 7. If the UV micro-LED is the light
necessary to use three conversion materials to produce the RGB three-color conversion layers; if the
source, it is necessary to use three conversion materials to produce the RGB three-color conversion
excitation light source is a blue LED, only the corresponding red and green conversion layers are
layers; if the excitation light source is a blue LED, only the corresponding red and green conversion
needed to realize the full-color display of the micro-LED.
layers are needed to realize the full-color display of the micro-LED.
Schematic diagram
Figure 7. Schematic diagram of color conversion technology.
An
An alternative
alternative method
methodofofimplementing
implementinga full-color
a full-colordisplay
displayis to
is first convert
to first the blue
convert micro-LED
the blue micro-
into
LED white lightlight
into white and and
thenthen
cover the the
cover RGBRGB filter onon
filter thethe
white light
white lightsource
sourcetotoobtain
obtainthe
theRGB
RGB tricolor
tricolor
sub-light
sub-light source. This method
source. This method doesdoes not
not need
need to to distinguish
distinguish between
between the the RGB
RGB pixels
pixels of
of the
the micro-LED
micro-LED
array
array but only needs to prepare the corresponding RGB pixel filters, making the preparation simple
but only needs to prepare the corresponding RGB pixel filters, making the preparation simple
and low-cost. In 2019, Xu et al. proposed a full-color LED micro-display system
and low-cost. In 2019, Xu et al. proposed a full-color LED micro-display system based on time based on time division
multiplexing with dynamic
division multiplexing color filters
with dynamic [52].
color The[52].
filters wholeThesystem
wholeissystem
composed of a micro-LED
is composed display
of a micro-LED
module, a color conversion
display module, layer, a microcontroller
a color conversion unit (MCU),
layer, a microcontroller unit and
(MCU),a dynamic color filter
and a dynamic module,
color filter
as shown in Figure 8a. The area of the micro-LED display module is 7 mm × 11 mm, the resolution is
920 × 480, and the pixel pitch is 12.8 µm; when constructed, this module can emit 450 nm blue light.
The color conversion layer with a thickness of less than 3 µm is composed of QDs, which are coated on
module, as2020,
Nanomaterials shown in Figure
10, 2482 8a. The area of the micro-LED display module is 7 mm × 11 mm, 11 ofthe
33
resolution is 920 × 480, and the pixel pitch is 12.8 μm; when constructed, this module can emit 450
nm blue light. The color conversion layer with a thickness of less than 3 μm is composed of QDs,
the micro-LED
which are coatedarray to convert
on the bluearray
micro-LED light to
into white blue
convert light.light
The into
corewhite
component of this
light. The coresystem is the
component
dynamic color filter, which consists of four-color blocks of red, green, blue, and colorless.
of this system is the dynamic color filter, which consists of four-color blocks of red, green, blue, and By rotating
the color filter,
colorless. the MCU
By rotating theoutputs a gray-scale
color filter, the MCU image of thea corresponding
outputs gray-scale image channel
of theaccording to the
corresponding
duty ratio of the different colors, thus displaying the color image using a time-division
channel according to the duty ratio of the different colors, thus displaying the color image using a multiplexing
method. The working
time-division process
multiplexing is shown
method. The in Figure process
working 8b. However,
is shownthein
filter absorbs
Figure 2/3 of thethe
8b. However, emitted
filter
light,
absorbs which greatly
2/3 of reduces
the emitted the which
light, luminous efficiency
greatly reducesof the
the luminous
micro-LEDefficiency
array, soofthe
thefirst method
micro-LED
with
array,separate
so the light
first conversion
method with materials is more
separate light suitable
conversionfor the development
materials is more of color conversion
suitable for the
micro-LED
development displays.
of color conversion micro-LED displays.
Figure 8.8. (a)

Figure (a)Dynamic
Dynamiccolor filter
color full-color
filter LEDLED
full-color micro-display systemsystem
micro-display structure based on
structure time on
based division
time
multiplexing and (b) the working process of the system. Reproduced from [52], with permission from
division multiplexing and (b) the working process of the system. Reproduced from [52], with
John Wiley and Sons, 2019.
permission from John Wiley and Sons, 2019.
The material of the color conversion layer is generally phosphors or QDs. The phosphor is
The material of the color conversion layer is generally phosphors or QDs. The phosphor is
composed of some wide band gap materials (such as oxides, nitrides, and sulfides) and a small
composed of some wide band gap materials (such as oxides, nitrides, and sulfides) and a small
number of doping ions (transition metals or rare earth compounds). Although phosphors have
number of doping ions (transition metals or rare earth compounds). Although phosphors have
mature preparation technology, high thermal and chemical stability, and a good quantum yield [53],
mature preparation technology, high thermal and chemical stability, and a good quantum yield [53],
their particle size is in the micron level, making them difficult to uniformly coat on micro-LED pixels at
their particle size is in the micron level, making them difficult to uniformly coat on micro-LED pixels
the same size level, which will affect the color conversion efficiency and uniformity of the micro-LED
at the same size level, which will affect the color conversion efficiency and uniformity of the micro-
display. In contrast, the rapidly developed QDs of recent years have a nanometer size, a narrow
LED display. In contrast, the rapidly developed QDs of recent years have a nanometer size, a narrow
emission spectrum, a wide absorption spectrum, higher luminous efficiency, etc. Therefore, QDs are
emission spectrum, a wide absorption spectrum, higher luminous efficiency, etc. Therefore, QDs are
more suitable for full-color micro-LED displays. This section will introduce the methods used for
more suitable for full-color micro-LED displays. This section will introduce the methods used for
achieving full-color micro-LED displays through the phosphor color conversion layer, the QD color
achieving full-color micro-LED displays through the phosphor color conversion layer, the QD color
conversion layer, and other color conversion technologies over the past ten years.
conversion layer, and other color conversion technologies over the past ten years.
3.1. Phosphor Color Conversion LEDs
3.1. Phosphor Color Conversion LEDs
Phosphors have the advantages of a high and stable quantum yield, high thermal stability,
Phosphors
and high chemical have the advantages
stability (humidityofresistance),
a high andso stable
theyquantum
are often yield, high
used for UVthermal
LEDs or stability, and
blue LEDs
high chemical stability (humidity resistance), so they are often used for
to synthesize white light through down conversion [54]. Commonly used phosphors include yellow UV LEDs or blue LEDs to
synthesize yttrium
emission: white light throughgarnet
aluminum down(YAG):
conversion
Ce3+ [54].
, red Commonly
emission: Ca usedSrphosphors2+ include yellow 2+
1-x x S: Eu , Sr2 Si5 N8 : Eu ,
emission: yttrium
3+ aluminum garnet (YAG): Ce 3+, red emission: Ca1-xSrxS: Eu2+, Sr2Si5N8: Eu2+, CaSiN2:
CaSiN2 : Ce , green emission: SrGa2 S4 : Eu , SrSi2 O2 N2 : Eu , blue emission: LiCaPO4 :Eu2+ ,
2+ 2+
Ce3+(PO
Sr , green emission:
2+ SrGa2S4: Eu2+, SrSi2O2N2: Eu2+, blue emission: LiCaPO4:Eu2+, Sr5(PO4)3Cl: Eu2+, etc.
5 4 )3 Cl: Eu , etc. [53]. Converting blue micro-LEDs into white light via yellow phosphor and
[53]. Converting
then dividing each blue
RGB micro-LEDs into white
sub-pixel with a colorlight
filtervia yellow
is one phosphor
method used toand then dividing
realize each
a full-color RGB
display.
sub-pixel with a color filter is one method used to realize a full-color display. However,
However, as mentioned above, the color filter will absorb most of the emitted light, and the scattering on as mentioned
above,
the colorthe color
filter filter
will will absorb
produce most
crosstalk of the each
between emitted light, and
sub-pixel. the scattering
Therefore, preparingon the
the color filter will
RGB phosphor
produce
as a color crosstalk
conversion between
layer and each sub-pixel.
coating Therefore,
the phosphor preparing
on each the isRGB
light pixel phosphor
a more efficientas a color
method.
conversion layer and coating the phosphor on each light pixel is a more efficient
In 2011, Zhao et al. used phosphors to manufacture the first full-color active LED array displaysmethod.
on silicon (LEDoS) [55,56]. These displays used a 380 nm UV LED array to excite red, green, and blue
In 2011, Zhao et al. used phosphors to manufacture the first full-color active LED array displays
on silicon (LEDoS) [55,56]. These displays used a 380 nm UV LED array to excite red, green, and blue
phosphors
phosphors to to achieve
achieve aafull-color
full-colordisplay.
display.This
This type
type of of
LEDLED array
array hashas a resolution
a resolution of 8 of × 8 aand
× 88and a
pixel
pixel pitch of 550 µm. Each color pixel is composed of two green, one red, and
pitch of 550 μm. Each color pixel is composed of two green, one red, and one blue sub-pixels, asone blue sub-pixels,
as shown
shown in in Figure
Figure 9a.9a.The
The colorconversion
color conversionlayer
layerisismade
madeby bydeep
deep reactive-ion
reactive-ion etching
etching (DRIE)
(DRIE) onon aa
single
single crystal silicon wafer. Then, phosphors with a separate emission wavelength are dropped into
crystal silicon wafer. Then, phosphors with a separate emission wavelength are dropped into
the
the corresponding
corresponding etching
etching holes
holes on
on the
the color
color conversion
conversion layer.
layer. After
After the
the phosphor
phosphor isis cured,
cured, the
the color
color
conversion
conversion layer
layer can
can bebe excited
excited by
by the
the UV
UV LED
LED array
array toto achieve
achieve aa full-color
full-color display,
display, asas shown
shown inin
Figure 9b.
Figure 9b.
Figure 9.
Figure 9. (a) Single color pixel composition;
composition; (b) Full-color display using UV LED to excite the RGB
RGB
phosphor. Reproduced
phosphor. Reproduced from
from [55],
[55], with
with permission
permissionfrom
fromJohn
JohnWiley
Wileyand
andSons,
Sons,2012.
2012.
However,
However, for for micro-LEDs
micro-LEDs with with sizes
sizes below
below 100 μm, oversized
100 µm, oversized phosphors
phosphors cannot
cannot bebe used
used to to
prepare a uniform color conversion layer that conforms to the micro-LED display
prepare a uniform color conversion layer that conforms to the micro-LED display pixels. The size of pixels. The size of
the
the phosphor
phosphor willwill vary
vary according
according to to the
the preparation
preparation process. Table 33 shows
process. Table shows the
the various
various processes
processes for for
preparing
preparing thethe phosphor
phosphor and and the
the size
size of
of the
the phosphor
phosphor that
that can
can be
be obtained
obtained under
under thisthis process.
process. ItIt can
can
be
be concluded
concluded thatthat by
by using
using advanced
advanced synthesis technology, nano-sized
synthesis technology, phosphors can
nano-sized phosphors can be
be prepared.
prepared.
However,
However,although
althoughsmaller-sized
smaller-sizedphosphors
phosphors areare
beneficial to improve
beneficial to improvethe color uniformity
the color of theof
uniformity color
the
conversion layer, their
color conversion layer,luminous efficiency
their luminous is proportional
efficiency to their size,
is proportional which
to their size,also means
which alsothat the light
means that
efficiency of the color
the light efficiency conversion
of the layer prepared
color conversion from small-sized
layer prepared phosphors
from small-sized will be reduced.
phosphors In 2013,
will be reduced.
Chen et al.
In 2013, Chenfound that
et al. mixing
found thatlarge-sized and small-sized
mixing large-sized phosphors
and small-sized together can
phosphors greatly
together canimprove
greatly
the color uniformity of mixed phosphors at the expense of a small amount
improve the color uniformity of mixed phosphors at the expense of a small amount of light efficiencyof light efficiency [57].
The authors mixed 4 µm small-sized phosphor particles and 22 µm large-sized
[57]. The authors mixed 4 μm small-sized phosphor particles and 22 μm large-sized phosphor phosphor particles in a
ratio of 3:2
particles into obtain
a ratio ofthe
3:2 best performance
to obtain the best with 91.6% angular
performance color angular
with 91.6% uniformity and
color 95.7% normalized
uniformity and 95.7%
light efficiency. Therefore, this method can effectively improve the uniformity
normalized light efficiency. Therefore, this method can effectively improve the uniformity and and luminous efficiency
of phosphor
luminous LEDs. of phosphor LEDs.
efficiency
Table 3.
Table Overview of
3. Overview of the
the phosphor
phosphor particle
particle sizes
sizes obtained
obtained by
by different
different preparation
preparation processes
processes[58].
[58].
Preparation
Preparation Solid State
Solid State Sol gel/ Spray
Process Reaction Sol gel/ PechiniCo-Precipitation
Pechini Co-Precipitation Hydrothermal
Hydrothermal Combustion
Combustion Spray Pyrolysis
Process Reaction Pyrolysis
size
size >5 μm
>5 µm 10 nm–2
10 nm–2
µm μm 10 nm–1
10 nm–1
µm μm 10 nm–1 µm μm 500500
10 nm–1 nm–2 µm μm 100100
nm–2 nm–2
nm–2
µmμm
Nevertheless, as
Nevertheless, as the
the sizes
sizes of
of micro-LED
micro-LED pixels
pixels shrink,
shrink, the
the relatively
relatively large
large sizes
sizes of
of the
the phosphors
phosphors
will limit the color uniformity. Although this color uniformity can be improved by preparing a smallera
will limit the color uniformity. Although this color uniformity can be improved by preparing
smaller
size size phosphor
phosphor or mixingorphosphors,
mixing phosphors,
quantum quantum
efficiencyefficiency will stillwith
will still decrease decrease
size. with size. This
This reduction
reduction will eventually affect the display of the micro-LED. Therefore, it is necessary
will eventually affect the display of the micro-LED. Therefore, it is necessary to find a conversion to find a
conversion material with a smaller size and a higher conversion efficiency to replace the
material with a smaller size and a higher conversion efficiency to replace the phosphor, for which QDs phosphor,
for the
are which
bestQDs are the best candidates.
candidates.
3.2. Quantum
3.2. Quantum Dot Color Conversion
Dot Color Conversion LEDs
LEDs
QDs are
QDs are aa new
new type
type of
of semiconductor
semiconductor nanomaterial
nanomaterial that
that have
have the
the advantages
advantages of
of aa nanometer
nanometer
size, a high quantum yield, a broad absorption spectrum, and a narrow emission spectrum.
size, a high quantum yield, a broad absorption spectrum, and a narrow emission spectrum. When When
the
the
QDsQDs areare excited
excited by electricity
by electricity or light,
or light, theythey
can canemitemit
lightlight
withwith different
different wavelengths
wavelengths relatedrelated to
to their
their
size,size,
shape,shape,
andand composition.
composition. In In this
this way,
way, thetheemission
emissionwavelength
wavelengthcan can be be adjusted
adjusted by by changing
changing
these
these parameters, which can be used to realize a full-color display with micro-LEDs [59–65].QDs
parameters, which can be used to realize a full-color display with micro-LEDs [59–65]. QDsare are
usually
usuallyII-VI II-VIgroup
groupcompounds,
compounds, III-V
III-Vgroupgroup compounds,
compounds, or I-III-VI
or I-III-VIcompounds,
compounds, such such
as CdSe, InP,
as CdSe,
and
InP,CuInS
and CuInS2 [66]. The deposition methods of QDs mainly include spin coating [67], aerosol printing
2 [66]. The deposition methods of QDs mainly include spin coating [67], aerosol
technology [68], photolithography
printing technology [68], photolithography technologytechnology
[69], inkjet[69],printing
inkjet[70,71],
printing and the pulse
[70,71], and spraying
the pulse
method
spraying [72]. In addition,
method [72]. Insince QDs have
addition, sinceaQDs shorter havelight-emitting life, they have
a shorter light-emitting a faster
life, modulation
they have a faster
response
modulation response speed, and their narrow emission linewidth gives them have a good colorwhich
speed, and their narrow emission linewidth gives them have a good color purity, purity,
provides the possibility
which provides of wavelength
the possibility of wavelengthdivisiondivision
multiplexing for visible
multiplexing for light
visible communication.
light communication. Thus,
QD-converted
Thus, QD-converted full-color micro-LEDs
full-color are not are
micro-LEDs onlynot used
onlyforused
displays but alsobut
for displays widely
also applied in visible
widely applied in
light communication [73–75].
visible light communication [73–75].
InIn2015,
2015,HanHanet etal.
al. prepared
preparedaafull-color
full-colordisplay
displayininwhichwhichthe theRGB RGBQDs QDsconversion
conversionlayer layerwas was
excited
excitedby byaaUV UVmicro-LED
micro-LEDarray array[71].[71].ThisThismicro-LED
micro-LED display
display array
array had
had a resolution
a resolution of of
128128 × 128,
× 128,a
pixel size of 35 μm, and a pixel pitch of 40 μm. RGB three-color QDs
a pixel size of 35 µm, and a pixel pitch of 40 µm. RGB three-color QDs are composed of CdSe/ZnS and are composed of CdSe/ZnS and
CdS,
CdS, which
which can can emit
emitlight
lightwith
withwavelengths
wavelengths of of450450
nm,nm,520 520
nm, nm,
and 630andnm,630respectively,
nm, respectively, when
when excited
excited by 365 nm ultraviolet light. The QDs are sprayed on the micro-LED
by 365 nm ultraviolet light. The QDs are sprayed on the micro-LED array by aerosol inkjet printing array by aerosol inkjet
printing technology, the process of which is shown in Figure
technology, the process of which is shown in Figure 10a. First, the QD solution at a concentration10a. First, the QD solution at of
a
concentration
about 5 mg/mL of is
about 5 mg/mL
atomized and is atomizedinand
entrained the entrained in the
air flow jetted byairtheflow
print jetted
head; bythen,
the print head;
the process
then,
parameters of aerosol inkjet printing are adjusted to obtain a spray linewidth of 35 µm. ForofQDs
the process parameters of aerosol inkjet printing are adjusted to obtain a spray linewidth 35
μm. For QDs
of different of different
sizes, to ensuresizes, to ensure of
the uniformity thespraying,
uniformity theof spraying,
spraying needsthe tospraying
be performedneeds to underbe
performed under different flow rates of gas, which means that the
different flow rates of gas, which means that the larger QD is, the faster the gas flow rate must be. larger QD is, the faster the gas
flow
Afterrate mustQDs
the RGB be. are
After the RGB
sprayed ontoQDs are sprayed
the micro-LED arrayontoin the micro-LED
sequence, array inBragg
a distributed sequence,
reflector a
distributed Bragg reflector
(DBR) is deposited on the top(DBR) is deposited
to reflect on the top
the ultraviolet lighttothat
reflect
leakedthe ultraviolet
back to thelight colorthat leaked
conversion
back to the
layer for reuse.color conversion layer for reuse.
The
Theoptical
optical performance
performance of of this
thisQD-based
QD-basedmicro-LED micro-LEDdisplay display is is shown
shown in in Figure
Figure 10b–d.
10b–d. Figure
Figure 10b
10b shows
shows the reflectance
the reflectance spectrum
spectrum of theofDBR the structure
DBR structure placedplaced
on top on topmicro-LED
of the of the micro-LED
array. This array. This
structure
structure has a reflectivity
has a reflectivity of 90% atof395 90% nm,at 395
as wellnm, as as awell as a reflectivity
reflectivity of only 10% of only 10%nm
at 450 at 450
(B), nm520(B),nm520 (G),
nm
and(G),
630and nm630 (R).nm (R). Therefore,
Therefore, the leaked the leaked
UV light UVcanlight
be can be effectively
effectively recovered, recovered,
and other and light
othercan lightbe
can be emitted. Figure 10c demonstrates that the QD micro-LED display
emitted. Figure 10c demonstrates that the QD micro-LED display with a DBR structure can effectively with a DBR structure can
effectively
inhibit theinhibit
leakage theofleakage of ultraviolet
ultraviolet light andthe
light and increase increase
luminous the luminous
intensity by intensity
194% (B), by 194%
173%(B), (G),
173% (G), and
and 183% (R). 183%
Figure(R).10dFigure
provides10daprovides
comparison a comparison
between thebetween
QD micro-LEDthe QD display
micro-LED and display
the Nationaland
the National
Television Television
Standards Standards
Committee Committee
(NTSC) (NTSC)Commission
International InternationalonCommission
Illuminationon Illumination
(CIE) 1976 color
(CIE) 1976 color space chromaticity diagram. The QD micro-LED
space chromaticity diagram. The QD micro-LED display has a wider color gamut, which is 1.52 display has a wider color gamut,
times
which
that ofisNTSC.
1.52 times that of NTSC.
Figure10.
Figure (a)Quantum
10.(a) Quantumdots
dots(QDs)
(QDs)printing
printingprocess;
process;(b)
(b)distributed
distributedBragg
Braggreflector
reflector(DBR)
(DBR)reflection
reflection
spectrum; (c) emission spectrum with and without a DBR structure; (d) the NTSC CIE 1976 color
spectrum; (c) emission spectrum with and without a DBR structure; (d) the NTSC CIE 1976 color space space
chromadiagram.
chroma diagram.Reproduced
Reproducedfrom
from[71],
[71],The
TheOptical
OpticalSociety,
Society,2012.
2012.
As the size of the micro-LED decreases, the optical crosstalk between each sub-pixel will seriously
As the size of the micro-LED decreases, the optical crosstalk between each sub-pixel will
affect the contrast, color purity, and saturation of the display. To reduce the optical crosstalk between
seriously affect the contrast, color purity, and saturation of the display. To reduce the optical crosstalk
the sub-pixels in the QD micro-LED display, Kuo et al. used photolithography and photoresist (PR)
between the sub-pixels in the QD micro-LED display, Kuo et al. used photolithography and
photoresist (PR) to prepare an anti-crosstalk window mold in 2017. The structure of this window

to prepare an anti-crosstalk window mold in 2017. The structure of this window mold is shown
in Figure
mold 11a [76]
is shown and is11a
in Figure composed
[76] andof is acomposed
window forof aQD injection
window and injection
for QD a barrierand
walla for reducing
barrier wall
for reducing crosstalk. The window size is the same as the sub-pixel size of the micro-LED array. Theis
crosstalk. The window size is the same as the sub-pixel size of the micro-LED array. The barrier wall
silver-plated
barrier wall isto silver-plated
prevent emission light leakage.
to prevent Figure
emission 11b,c
light are theFigure
leakage. fluorescence microscope
11b,c are images of
the fluorescence
the QD micro-LED array with the anti-crosstalk mold and without the crosstalk
microscope images of the QD micro-LED array with the anti-crosstalk mold and without the crosstalkmold, respectively.
Here, there
mold, is no clear
respectively. isolation
Here, therebetween eachisolation
is no clear sub-pixelbetween
in the QDeachmicro-LED array
sub-pixel in without
the QD the crosstalk
micro-LED
prevention mold. The blue QDs overlap with the red and green QDs, and the crosstalk
array without the crosstalk prevention mold. The blue QDs overlap with the red and green QDs, degree is about
and
32.8%. In contrast, the QD micro-LED array with anti-crosstalk molds has a clear
the crosstalk degree is about 32.8%. In contrast, the QD micro-LED array with anti-crosstalk molds boundary, and the
crosstalk degree is almost zero, which effectively reduces the optical crosstalk between
has a clear boundary, and the crosstalk degree is almost zero, which effectively reduces the optical each sub-pixel
in the QDbetween
crosstalk micro-LED eachdisplay.
sub-pixel in the QD micro-LED display.
Figure11.
Figure (a)QD
11. (a) QD micro-LED
micro-LED array with the the anti-crosstalk
anti-crosstalkmold;
mold;(b)
(b)fluorescence
fluorescencemicroscope
microscopeimage
imageof
the
of QD
the micro-LED
QD micro-LED array
arraywithout the
without thecrosstalk prevention
crosstalk prevention mold;
mold;(c)(c)
fluorescence
fluorescence microscope
microscopeimage
imageof
the
of QD
the micro-LED
QD micro-LEDarray with
array thethe
with anti-crosstalk mold.
anti-crosstalk Reproduced
mold. fromfrom
Reproduced [76],[76],
Photonics Research,
Photonics 2017.
Research,
2017.
Another problem for QD micro-LED displays is the stability and quantum yield of QDs. The dry
QD conversion
Another problem layer suffers
for QDfrom a low quantum
micro-LED displaysyield,is theplotting
stabilitydifficulties,
and quantum andyield
an unstable
of QDs.structure,
The dry
QD conversion layer suffers from a low quantum yield, plotting difficulties, and an unstabletostructure,
which will increase with the thickness of the dry QD film [77,78]. Therefore, it is necessary mix QDs
with other
which will substances
increase with andthe then distribute
thickness of the
themixture
dry QDinto filmLED molds
[77,78]. or place the
Therefore, it ismixture
necessary ontotoLEDs
mix
to manufacture QD-LEDs [66]. In 2018, Zhou et al. used a microwave
QDs with other substances and then distribute the mixture into LED molds or place the mixture onto assisted heating method to mix
QDs and
LEDs sodium silicate
to manufacture aqueous[66].
QD-LEDs solution within
In 2018, Zhou 30 et
s. al.
Theusedquantum yield of the
a microwave prepared
assisted QD method
heating solution
(69%) was more than twice that of the original QD solution (33%)
to mix QDs and sodium silicate aqueous solution within 30 s. The quantum yield of the prepared QD [75]. In 2020, Ho et al. prepared
an RGB color
solution (69%)conversion
was more film than using
twice salt-sealed
that of theQD [79]. The
original QD salt layer(33%)
solution covering [75].theInQD 2020,successfully
Ho et al.
protectedan
prepared theRGBQD fromcoloroxygen,
conversion moisture, heat, salt-sealed
film using and other external
QD [79].environments,
The salt layerthereby covering prolonging
the QD
the reliability and service life of the QD-LED. The photoresist hybrid
successfully protected the QD from oxygen, moisture, heat, and other external environments, thereby QD provided a method for
patterning multi-color QD arrays. This method can not only control
prolonging the reliability and service life of the QD-LED. The photoresist hybrid QD provided a the thickness and size of the QD
conversion
method for layer but also
patterning retain the QD
multi-color characteristics
arrays. This ofmethod
photolithography
can not only technology,
control the thereby providing
thickness and
a cost-effective solution for the development of high-resolution, large-area
size of the QD conversion layer but also retain the characteristics of photolithography technology, micro-LED displays [80].
In 2020,providing
thereby Chen et al.a prepared
cost-effectivean RGB full-color
solution for themicro-LED
development arrayofusing a photoresistlarge-area
high-resolution, color conversion
micro-
layer mixed with QD [81]. The experiments show that QDs fused
LED displays [80]. In 2020, Chen et al. prepared an RGB full-color micro-LED array using a with photoresist can reach a quantum
yield of 60–70%,
photoresist color and the optical
conversion layerdensity
mixed ofwith
red andQDgreen mixed
[81]. The QDs can reach
experiments show 1.5that
andQDs 0.8, respectively.
fused with
In addition
photoresist to using
can reach high-quality
a quantum yieldQDs or micro-LED
of 60–70%, and the excitation light sources,
optical density of redoptimization
and green mixed of the
structures can also improve
QDs can reach 1.5 and 0.8, respectively. the light efficiency of QD micro-LEDs. Chen et al. prepared a monolithic
RGBInQD micro-LEDs
addition to usingwith black matrix
high-quality QDs photoresist
or micro-LED spacers, hybridlight
excitation Bragg reflector
sources, (HBR) structures,
optimization of the
and distributed
structures can alsoBraggimprovereflector
the light(DBR) structures.
efficiency of QDThese structures
micro-LEDs. Chen areet shown
al. preparedin Figure 12a [82].
a monolithic
The QD
RGB average transmittance
micro-LEDs with blackof the blackphotoresist
matrix matrix photoresist
spacers, hybridin the Bragg
visiblereflector
light band (HBR) is only 0.56%.
structures,
Spin-coating
and distributed thisBragg
photoresist
reflectoron (DBR)
the sidewall of each
structures. RGB structures
These sub-pixel not areonly
shown prevents
in Figurecrosstalk between
12a [82]. The
pixels but
average also blocks the
transmittance leakage
of the blackof blue light,
matrix therebyinincreasing
photoresist the visiblethe contrast
light band is ratio
only of 0.56%.
the RGB QD
Spin-
micro-LED from 11 to 22. To further improve the color purity and
coating this photoresist on the sidewall of each RGB sub-pixel not only prevents crosstalk between light output intensity of red and
green but
pixels light, a distributed
also blocks the Braggleakage reflector
of blue(DBR) with high
light, thereby reflectivity
increasing theunder
contrastblueratio
lightofwasthe fabricated
RGB QD
micro-LED from 11 to 22. To further improve the color purity and light output intensity of redand
on top of the QD micro-LED along with a hybrid Bragg reflector (HBR) composed of a DBR anda
silver-plated
green layer at the Bragg
light, a distributed bottom. This structure
reflector (DBR) with can reflect the blue light
high reflectivity underleaking
blue back
light towas thefabricated
QD color
on top of the QD micro-LED along with a hybrid Bragg reflector (HBR) composed of a DBR and a
silver-plated layer at the bottom. This structure can reflect the blue light leaking back to the QD color
conversion layer, allowing the red and green QDs to be excited by more blue light. According to the

conversion layer, allowing the red and green QDs to be excited by more blue light. According to the
authors’ tests,
tests, compared
comparedtotoQD QDmicro-LED
micro-LEDwithoutwithout HBR,HBR, thethe
redred
and green
and greenoutput
outputintensity
intensityof the
of QD
the
micro-LED
QD micro-LEDwith with
HBR was
HBRincreased by about
was increased by 23%.
aboutMoreover, the red and
23%. Moreover, the green
red and outputgreenintensities
output
of the QD of
intensities micro-LED with bothwith
the QD micro-LED HBRboth and HBR
DBR and increased by aboutby
DBR increased more
about 27% compared
more to the QD
27% compared to
micro-LED with HBR only.
the QD micro-LED with HBR only.
Gou et al. proposed
proposed aa funnel
funneltube
tubearray
arrayforforaamicro-LED
micro-LEDdisplay displayforforcolor
colorconversion,
conversion, as asshown
shown in
Figure
in 12b12b
Figure [83,84]. The
[83,84]. simulation
The simulation showed
showed that thethe
that inner
innerwall of of
wall thethe
funnel
funnel tube
tubestructure
structure is made
is madeof
absorptive
of absorptive or reflective material,
or reflective andand
material, eacheach
sub-light
sub-light source is completely
source is completely isolated by the
isolated byfunnel tube
the funnel
structure,
tube whichwhich
structure, can effectively reducereduce
can effectively color crosstalk between
color crosstalk pixels. In
between addition,
pixels. as the cone
In addition, as theangle of
cone
the funnel
angle of thetube becomes
funnel tube smaller,
becomesthe luminous
smaller, theefficiency
luminousofefficiency
the micro-LED
of the ismicro-LED
gradually increased
is gradually by
up to threebytimes
increased up tothat without
three times the
thatfunnel
without tubethestructure.
funnel tube Therefore,
structure. this structurethis
Therefore, canstructure
improve can the
environmental
improve contrast of the
the environmental QD micro-LED.
contrast of the QD micro-LED.
In 2020, Kang et al. applied
applied aa nanoporous
nanoporous (NP) (NP) GaN GaN structure
structure to the QD color conversionconversion of a
micro-LED display [85,86]. Compared
Compared to ordinary QD films, the GaN GaN NP NP structure
structure has high high structural
structural
stability and improves the light absorption
stability absorption rate of QD through its unique type of multiple light
The preparation
scattering. The preparation process
process of of the
the GaN
GaN NP NP structure
structure conversion
conversion layer
layer isis shown
shown in inFigure
Figure12c.12c.
The NP GaN conversion layer with a pitch of 40 µm μm and an area of 36 36 × × 36 µmμm22 was
was prepared by
conventional photolithography
conventional photolithography and and chlorine-based
chlorine-based inductively
inductively coupled
coupled plasma
plasmaetching
etching technology,
technology,
followed by loading the red and green QDs into
followed into thethe corresponding
corresponding NP NP GaNGaN holes.
holes. To To prevent
between the
crosstalk between the RGB
RGB sub-pixels,
sub-pixels, aa Ni/Al
Ni/Al layer
layer was was deposited
deposited on on the
the sidewalls
sidewalls of of the
the NPNP GaN.
GaN.
The experiments
experiments show showthat
thatthe
thegreen
greenand andred
redQDsQDs filling thethe
filling GaNGaN NPNPstructure
structurecan can
achieve
achieveabout 96%
about
and 100%
96% lightlight
and 100% conversion efficiency
conversion under
efficiency the excitation
under the excitationof 370ofnm 370blue
nm light.
blue light.
Figure 12.
Figure (a) Monolithic
12. (a) Monolithic RGB
RGB QDQD micro-LED
micro-LED with
with aa black
black matrix
matrix photoresist
photoresist spacer,
spacer, hybrid Bragg
hybrid Bragg
reflector (HBR) and DBR structure. Reproduced from [82], with permission from Institute of
reflector (HBR) and DBR structure. Reproduced from [82], with permission from Institute of ElectricalElectrical
and Electronics
and ElectronicsEngineers, 2018;
Engineers, (b) RGB
2018; QD micro-LED
(b) RGB with a funnel
QD micro-LED with tube array structure.
a funnel tube arrayReproduced
structure.
from [84], with permission from John Wiley and Sons, 2019; (c) GaN nanoporous
Reproduced from [84], with permission from John Wiley and Sons, 2019; (c) GaN nanoporous (NP) structure
(NP)
conversion layer preparation process. Reprinted with permission from [85]. Copyright (2020)
structure conversion layer preparation process. Reprinted with permission from [85]. Copyright (2020)American
Chemical Society.
American Chemical Society.
3.3. Other Color Conversion Technologies
3.3. Other Color Conversion Technologies
In addition to using phosphors or QD conversion layers to achieve full-color micro-LED displays
In addition to using phosphors or QD conversion layers to achieve full-color micro-LED displays
with micro-LEDs, other conversion materials and external conversion structures can also be used.
with micro-LEDs, other conversion materials and external conversion structures can also be used.
Liu et al. proposed a micro-LED full-color projection system on silicon (LEDoS) in 2013, which is
Liu et al. proposed a micro-LED full-color projection system on silicon (LEDoS) in 2013, which is
called a 3-LEDoS projector [87,88]. In this system, the RGB three-color micro-LED array on the silicon
called a 3-LEDoS projector [87,88]. In this system, the RGB three-color micro-LED array on the silicon
is mounted onto a trichroic prism, as shown in Figure 13a–c. Each monochromatic micro-LED array
is mounted onto a trichroic prism, as shown in Figure 13a–c. Each monochromatic micro-LED array
on the silicon is bonded to an addressable active silicon substrate via flip chip technology with a
on the silicon is bonded to an addressable active silicon substrate via flip chip technology with a
resolution of 30 × 30 and a pixel pitch of 140 µm. The monochromatic emission wavelengths of the
resolution of 30 × 30 and a pixel pitch of 140 μm. The monochromatic emission wavelengths of the
RGB three-color micro-LED array are 630 nm (R), 535 nm (G), and 445 nm (B), respectively.
RGB three-color micro-LED array are 630 nm (R), 535 nm (G), and 445 nm (B), respectively.
Figure 13. (a)

(a)Triangular
Triangularprism
prism projection source with an RGB three-color micro-LED array on silicon
Figure
Figure 13.
13. (a) Triangular prism projection
projection source
source with
with anan RGB
RGB three-color
three-color micro-LED
micro-LED array
array on
on silicon
silicon
(3-LEDoS);
(3-LEDoS); (b) 3-LEDoS
(b) 3-LEDoS projector
projectorprototype and
prototype and(c) schematic
(c) diagram
schematic diagramof the
of optical
the architecture;
optical (d)
architecture;
(3-LEDoS); (b) 3-LEDoS projector prototype and (c) schematic diagram of the optical architecture; (d)
The
(d) image projected on the wallwall
by thethe
3-LEDoS. Reproduced from
from[87],
[87],with
withpermission from
TheThe image
image projected
projected ononthethe
wall bybythe 3-LEDoS.
3-LEDoS. Reproduced
Reproduced from [87], with permission
permission from
from
Institute
InstituteofofElectrical
Electricaland
and Electronics
Electronics Engineers,
Engineers,2013.
2013.
Institute of Electrical and Electronics Engineers, 2013.
Theimage
The imagesignals
signals areare transmitted
transmitted to the
to the three
three arrayarray drives
drives through
through the external
the external control control unit,
unit, and
The image signals are transmitted to the three array drives through the external control unit, and
and a full-color image can then be projected using a trichroic prism, as shown
a full-color image can then be projected using a trichroic prism, as shown in Figure 13d. The team in Figure 13d. The team
a full-color image can then be projected using a trichroic prism, as shown in Figure 13d. The team
subsequentlymanufactured
subsequently manufacturedaahigher higherquality
qualityLEDoS
LEDoSchip chipwith
withaaresolution
resolutionofof100 100××100100and andaapixel
pixel
subsequently manufactured a higher quality LEDoS chip with a resolution of 100 × 100 and a pixel
pitchof
pitch of50
50μm.
µm.In In2018,
2018,Zhang
Zhangetetal.al.prepared
preparedultra-high-brightness
ultra-high-brightnessmicro-LED
micro-LEDdisplay displaypanels
panelswith
with
pitch of 50 μm. In 2018, Zhang et al. prepared ultra-high-brightness micro-LED display panels with
display resolutions of 640 × 480 and pixel pitches of 20 µm through the monolithic
display resolutions of 640 × 480 and pixel pitches of 20 μm through the monolithic hybrid integration hybrid integration
display resolutions of 640 × 480 and pixel pitches of 20 μm through the monolithic hybrid integration
technologyofofBeida
technology BeidaJade JadeBird
BirdCo.,
Co.,Ltd.
Ltd.[89].
[89].The
Thecolor
colorcombination
combinationprismprismintegrates
integratesthe thelight
lightemitted
emitted
technology of Beida Jade Bird Co., Ltd. [89]. The color combination prism integrates the light emitted
bybythe
thered,
red,green,
green,andandbluebluemonochromatic
monochromaticmicro-LED
micro-LEDdisplay
displaypanels
panels toto form
form aa full-color
full-color image.
image.
by the red, green, and blue monochromatic micro-LED display panels to form a full-color image.
InIn2014,
2014,Joao
Joaoetetal. al. used
usedliquid
liquidcapillary
capillaryforce
forcetototransfer
transferaamicron-sized
micron-sizedZnCdSe/ZnCdMgSe
ZnCdSe/ZnCdMgSe
In 2014, Joao et al. used liquid capillary force to transfer a micron-sized ZnCdSe/ZnCdMgSe
multiplequantum
multiple quantumwell well(MQW)
(MQW)color colorconversion
conversionfilm filmtotoaamicro-LED
micro-LEDwith withan anemission
emissionwavelength
wavelength
multiple quantum well (MQW) color conversion film to a micro-LED with an emission wavelength
of 450 nm and prepared a hybrid micro-LED that can emit 540 nm
of 450 nm and prepared a hybrid micro-LED that can emit 540 nm light waves [90]. The II-VI light waves [90]. The II-VIMQW
MQW
of 450 nm and prepared a hybrid micro-LED that can emit 540 nm light waves [90]. The II-VI MQW
colorconversion
color conversionfilm filmisisgrown
grownon onananInP
InPsubstrate,
substrate,andandthe
theInGaAs
InGaAsgrowth
growthbuffer
bufferlayer
layerisisproduced
produced
color conversion film is grown on an InP substrate, and the InGaAs growth buffer layer is produced
viaMBE.
via MBE.ThisThislayer
layerisiscomposed
composedofofnine nineZnCdSe
ZnCdSeQWs QWswithwithCdMgZnSe
CdMgZnSebarriers,
barriers,and anditsitsthickness
thicknessisis
via MBE. This layer is composed of nine ZnCdSe QWs with CdMgZnSe barriers, and its thickness is
lessthan
less than2.5
2.5μm.
µm.Its Itsstructure
structureisisshown
shownininFigure
Figure14a14aandandisisbonded
bondedtotothe thesapphire
sapphiresubstrate
substrateofofthethe
less than 2.5 μm. Its structure is shown in Figure 14a and is bonded to the sapphire substrate of the
micro-LEDvia
micro-LED vialiquid
liquidcapillary
capillaryforce.
force.The
Theluminous
luminouseffect
effectunder
underthetheexcitation
excitationof ofaa450
450nmnmlight
lightsource
source
micro-LED via liquid capillary force. The luminous effect under the excitation of a 450 nm light source
isisshown
shownininFigure
Figure14b. 14b. ByBy changing
changing thethe materials
materials of this
of this MQW MQW conversion
conversion filmfilm structure,
structure, suchsuch as
as III-
is shown in Figure 14b. By changing the materials of this MQW conversion film structure, such as III-
VIII-V AlGaInP
AlGaInP (yellow
(yellow to red)
to red) andand InGaN
InGaN (green),
(green), thisthis structure
structure can
can bebe extended
extended totoother
otherwavelengths,
wavelengths,
V AlGaInP (yellow to red) and InGaN (green), this structure can be extended to other wavelengths,
allowingaafull-color
allowing full-colordisplay
displayto tobe
berealized
realizedusing
usingmicro-LEDs.
micro-LEDs.
allowing a full-color display to be realized using micro-LEDs.
Figure 14. (a) II-VI multiple quantum well (MQW) structure design, (b) top view micrograph of the
Figure 14. (a) II-VI multiple quantum well (MQW) structure design, (b) top view micrograph of the
Figure 14.
mixing (a) II-VI
device multiple
and the quantum
effect of well
II-VI film (MQW)
when structure
excited design,
by a blue (b) top view from
LED. Reproduced micrograph of the
[90], Institute
mixing device and the effect of II-VI film when excited by a blue LED. Reproduced from [90], Institute
mixing
of device
Physics, 2015.and the effect of II-VI film when excited by a blue LED. Reproduced from [90], Institute
of Physics, 2015.
of Physics, 2015.
The deposition of QDs will face problems, such as low printing efficiency, the inability to pattern,
The
the coffeedeposition ofand
ring effect, QDsa will
roughface problems,
and uneven such as low
thickness ofprinting
the efficiency,
QD color the inability
conversion to pattern,
layer. Techniques,
The deposition of QDs will face problems, such as low printing efficiency, the inability to pattern,
the coffee
such ring
as spin effect,
coating, and a rough and uneven thickness of the QD color conversion layer. Techniques,
the coffee ring effect,fog
andcoating,
a roughandandspray printing,
uneven cannot
thickness efficiently
of the QD color and controllably
conversion deposit
layer. QDs or
Techniques,
such as spinon
phosphors coating,
each fog coating,
sub-pixel. and spray
Therefore, a printing,
stable, lowcannot
cost, efficiently
high and controllably
resolution, uniform, anddeposit QDs
patternable
such as spin coating, fog coating, and spray printing, cannot efficiently and controllably deposit QDs
or phosphors
deposition on each
technology sub-pixel. Therefore, a stable, low cost, high resolution, uniform, and
or phosphors on eachis sub-pixel.
required. In 2020, Kima etstable,
Therefore, al. proposed
low cost,to deposit a color conversion
high resolution, uniform,layer
and
patternable deposition technology is required. In 2020, Kim et al. proposed to deposit a color
patternable deposition technology is required. In 2020, Kim et al. proposed to deposit a color
conversion layer made of a mixture of light-cured acrylic and nano-organic color conversion
conversion layer made of a mixture of light-cured acrylic and nano-organic color conversion

made of a mixture of light-cured acrylic and nano-organic color conversion materials onto a blue
micro-LED
materials through
onto a blue traditional
micro-LED photolithography
through traditionaltechnology to achieve
photolithography a full-color
technology displaya full-
to achieve [91].
Through
color traditional
display photolithography
[91]. Through traditionaltechnology, the conversion
photolithography material
technology, the was accurately
conversion deposited
material was
onto each sub-pixel,
accurately depositedand ontothe position,
each size,and
sub-pixel, thickness, and patterning
the position, of the and
size, thickness, colorpatterning
conversion oflayer was
the color
able to be controlled. The structure of the color conversion device array based on
conversion layer was able to be controlled. The structure of the color conversion device array based blue micro-LEDs
is shown in Figure 15. × The 2 , the resolution is 100 × 100,
on blue micro-LEDs is The
shownchipinsize is 1015.
Figure 10 mmchip size is 10 × 10 mm2, the and the is
resolution size
100of× each
100,
2
sub-pixel
and the size of ×each
is 60 100 sub-pixel
µm withisa 60 pixel pitch
× 100 μmof 300 µm.
2 with Here,
a pixel pitchgreen andμm.
of 300 red Here,
perylene
green imides
and redare
mixed with
perylene organic
imides areinsulator
mixed with materials,
organicacrylic resinmaterials,
insulator solutions,acrylic
and photoactive compounds
resin solutions, containing
and photoactive
a positive tone
compounds of diazonaphthoquinone
containing to form a color conversion
a positive tone of diazonaphthoquinone to formlayer
a colorthat is deposited
conversion layeronto
that
a blue micro-LED array via traditional photolithography technology. In addition,
is deposited onto a blue micro-LED array via traditional photolithography technology. In addition, to avoid color
crosstalk
to between
avoid color each sub-pixel,
crosstalk between eacha black matrix isaalso
sub-pixel, black deposited
matrix isbetween the bluebetween
also deposited micro-LED thechips
blue
using photolithography.
micro-LED chips using photolithography.
15. Schematic
Figure 15.
Figure Schematicdiagram of aoffull-color
diagram micro-LED
a full-color based on
micro-LED light-curing
based color-changing
on light-curing materials.
color-changing
Reproduced
materials. from [91], MDPI,
Reproduced 2020.
from [91], MDPI, 2020.
The team studied the thickness, transmittance, conversion efficiency, and mixing rate of the color
The team studied the thickness, transmittance, conversion efficiency, and mixing rate of the color
conversion layer and concluded that the transmittance of the color conversion layer was almost 100%
conversion layer and concluded that the transmittance of the color conversion layer was almost 100%
in the visible light range. Under the excitation of 365 nm blue light, the green and red conversion
in the visible light range. Under the excitation of 365 nm blue light, the green and red conversion
materials absorbed the blue light and emitted the light at 550 nm and 620 nm, respectively. Finally,
materials absorbed the blue light and emitted the light at 550 nm and 620 nm, respectively. Finally,
by comparing the different mixing ratios of the acrylic and nano-organic color conversion materials,
by comparing the different mixing ratios of the acrylic and nano-organic color conversion materials,
the best conversion efficiency of the green and red conversion materials was determined to be obtained
the best conversion efficiency of the green and red conversion materials was determined to be
with 0.6% organic color conversion materials (the conversion efficiency of the green and red mixtures
obtained with 0.6% organic color conversion materials (the conversion efficiency of the green and red
was 47% and 35%, respectively).
mixtures was 47% and 35%, respectively).
3.4. Summary
3.4. Summary
In summary, color conversion technology is an effective solution to achieve full-color micro-LEDs.
In summary, color conversion technology is an effective solution to achieve full-color micro-
It does not require complex mass transfer technology to bond the RGB three-color LED chips to the
LEDs. It does not require complex mass transfer technology to bond the RGB three-color LED chips
same substrate to achieve full-color micro-LEDs. Thus, the chip defect rates caused by mass transfer
to the same substrate to achieve full-color micro-LEDs. Thus, the chip defect rates caused by mass
technology and the uneven color and brightness caused by RGB LED chips of different materials can
transfer technology and the uneven color and brightness caused by RGB LED chips of different
be avoided.
materials can be avoided.
Phosphor is a mature color conversion substance used for solid-state lighting. However, as the
Phosphor is a mature color conversion substance used for solid-state lighting. However, as the
sizes of micro-LED chips gradually shrink, defects caused by the small size of phosphors lead to
sizes of micro-LED chips gradually shrink, defects caused by the small size of phosphors lead to
degradation of light efficiency, wide emission spectra, and uneven color distribution, making them
degradation of light efficiency, wide emission spectra, and uneven color distribution, making them
difficult to be considered a high-quality choice for micro-LED color displays in the future. Due to
difficult to be considered a high-quality choice for micro-LED color displays in the future. Due to
their nanometer size, high quantum yield, wide absorption spectrum, and narrow emission spectrum,
their nanometer size, high quantum yield, wide absorption spectrum, and narrow emission spectrum,
quantum dots give the QD color conversion layer an adjustable wavelength, high color accuracy,
quantum dots give the QD color conversion layer an adjustable wavelength, high color accuracy,
high color saturation, and high color uniformity. Such excellent performance makes QDs the best
high color saturation, and high color uniformity. Such excellent performance makes QDs the best
choice to replace phosphors in the next generation of micro-display color conversion.
choice to replace phosphors in the next generation of micro-display color conversion.
Color purity shows the ability of the display to restore the nature origin colors, and it is an
important indicator in evaluating the displays. An LCD illuminated by the backlight, so, its color
Color purity shows the ability of the display to restore the nature origin colors, and it is an
important indicator in evaluating the displays. An LCD illuminated by the backlight, so, its color
purity is affected by the spectral composition of the backlight and the RGB color filter. An OLED
realizes spontaneous light through the design of organic molecular structure, so it has a wider color
gamut and higher color purity than LCD. However, due to the low lifespan of OLEDs, their various
properties will become unstable over time, including the color purity. A full-color micro-LED display
based on QD relies on the narrow and continuous emission spectrum of QDs, and the stability,
long life and strong energy saving of the LED itself. So, it has unparalleled color expression ability.
According to the Recommendation BT.2020 published by The International Telecommunication Union
Radiocommunication Sector (ITU-R), QD micro-LED displays are in the leading position with their
83% color purity, while OLED displays can only reach 75% at most.
However, QDs are not perfect, as the conversion efficiency and stability of QDs remain severely
limited. On the one hand, these limitations come from the lack of mature spraying technology for
QDs. On the other hand, the synthesis quality of QD materials cannot be guaranteed. The current QD
spraying process has low efficiency and uneven spray thickness, and the QD layers cannot be patterned.
And due to its nature, QD is often metastable when mixed with other solutions, which will result in
low conversion efficiency. The conversion efficiency of QDs will affect the power consumption and
life of QD displays. Although some external structures can be used to increase the external quantum
efficiency (EQE) of QD micro-LEDs and hybrid QDs to increase their yields, QDs with high conversion
efficiency also need to be further studied. Any QD material will be extremely sensitive to external
conditions, such as light, heat, oxygen, and moisture. This instability will cause the degradation of the
QD materials, which will quench the luminescence of the micro-LEDs. The stability of QDs will directly
affect the reliability and life of color micro-LED displays, so determining how to improve the stability
of QD materials is the research focus of color-transfer micro-LED displays. Fortunately, existing studies
have shown that QD stability can be improved by methods, such as ion doping, engineering the design
of the QD ligand surface, and encapsulation of the QDs with polymers or oxide materials. Finally, QD
contain heavy metal elements that are harmful to the human body and have a certain level of toxicity.
Thus, the next step of research needs to prepare high-quality QDs without heavy metals or find other
high-quality color conversion materials.
4. Monolithic Multi-Color Growth Technology

As described above, a full-color micro-LED display can be achieved through mass transfer and
color conversion technology. However, as the sizes of the micro-LED chips shrink, and the demand
for display resolution increases, the costs and difficulties of transfer and bonding technology will
undoubtedly increase. Although color transfer technology can avoid these problems and realize
full-color micro-LEDs, the color conversion layer faces the problems of low external quantum efficiency,
a short lifetime, poor reliability, and complicated preparation. Therefore, realizing the growth of
multi-color LEDs on a single wafer is the ultimate solution for realizing full-color micro-LEDs.
Theoretically, InGaN/GaN MQWs LEDs can change the wavelengths of monochromatic LEDs by
modulating the indium (In) content in the MQW. The higher the In content is, the longer the emission
wavelength will be. However, as the In content increases, the internal quantum efficiency (IQE) of
the LED will drop rapidly, especially when the wavelength is larger than 520 nm, which also means
that high-efficiency green and red LEDs cannot be generated using traditional InGaN/GaN MQWs.
This decrease in IQE is mainly caused by surface defects in the MQW, the internal polarization’s electric
field and poor miscibility between InN and GaN [92]. Excessive In content will significantly aggravate
the lattice and thermal mismatch between the GaN barrier and the InGaN well, resulting in increased
strain in this light-emitting heterostructure and producing defects at the surface interface, such as
dislocations, related V-defects, different point defects, etc. These defects are likely to become the center
of non-radiative recombination, which will increase the probability of non-radiative recombination,
thereby reducing the IQE of the LED. In addition, due to the low thermodynamic stability of InGaN
with a high In content, phase separation in this layer will reduce the chemical uniformity of the MQW,
which will lead
Nanomaterials 2020,to 10,the degradation
x FOR PEER REVIEW of the MQW active region. Another factor affecting the low quantum 19 of 33
efficiency of long-wavelength LEDs is the piezoelectric polarization electric field caused by lattice
mismatches
in and the[93].
nitride materials spontaneous polarization
MQW containing too electric
much Infieldwillinhave
nitride materials
a large internal [93]. MQW containing
polarization electric
too much In will have a large internal polarization electric field, which will
field, which will separate the electron-hole wave function in the MQW, thereby reducing the effective separate the electron-hole
wave functionradiation
luminescence in the MQW, thereby reducing
recombination rate. Thisthe effective
is also known luminescence
as the quantum radiation
confined recombination
Stark Effect
rate. This
(QCSE) is In
[94]. also knownthe
addition, as low
the quantum
quantum confined
efficiencyStark Effect (QCSE) LEDs
of long-wavelength [94]. Inmay addition, the low
also be affected
quantum
by the Auger efficiency of long-wavelength
recombination [95], carrier LEDs may also asymmetry
(electron/hole) be affected by the
[96], andAuger recombination
carrier leakage from[95], the
carrier region
active (electron/hole) asymmetry the
[97]. Considering [96],challenges
and carrierinleakage from the active of
the implementation region [97]. Considering
long-wave InGaN-based the
challenges
LEDs, in the usually
red LEDs implementation of long-wave
use GaP/GaAs as theirInGaN-based
growth substrate.LEDs,However,
red LEDs usually
studies usehaveGaP/GaAs
shown that as
theirand
IQE growth EQEsubstrate.
will also However, studies haveas
decrease significantly shown thatsize
the chip IQEdecreases
and EQE will[98].also decrease significantly
as theInchip
the size
past decreases
ten years,[98].
although multi-color micro-LEDs grown on the same substrate using the
In the
standard past ten years,
approaches have although multi-color
not been prepared, themicro-LEDs
emergence of grown
someon the same substrate
technologies has madeusing the
this type
of growthapproaches
standard possible. For haveexample,
not been a growth
prepared, buffer layer couldofbesome
the emergence usedtechnologies
to alleviate the has lattice
made andthis
thermal mismatch
type of growth between
possible. ForGaN and InGaN,
example, a growthallowing threecould
buffer layer kindsbe ofused
RGBto micro-LEDs
alleviate the tolattice
be grown
and
on the substrate.
thermal mismatch Moreover,
between GaN nanowires or nanoring
and InGaN, allowing structures couldofbeRGB
three kinds prepared on GaN
micro-LEDs totobeachieve
grown
micro-LEDs
on the substrate. with Moreover,
a tunable wavelength.
nanowires orInnanoring
addition,structures
the wavelength
could be ofprepared
a single-chipon GaN LEDtocould
achievebe
tuned through
micro-LEDs witha multi-active QW structure.
a tunable wavelength. In This section
addition, thewill introduceof
wavelength thea LED technologies
single-chip LED couldthat are
be
expected
tuned through to realize single-chipQW
a multi-active multi-color
structure.light
Thisemissions
section willandintroduce
provide research
the LED directions
technologies forthat
the
future realization
are expected of thesingle-chip
to realize single-chipmulti-color
growth of light
RGB emissions
multi-colorand micro-LED chips. directions for the
provide research
future realization of the single-chip growth of RGB multi-color micro-LED chips.
4.1. Growth Buffer Technology
4.1. Growth Buffer Technology
To grow RGB three-color LEDs on the same substrate, it is necessary to use epitaxial QW
To grow
structures withRGB three-color
different LEDs onFor
In content. the green
same substrate, it is necessary
and red LEDs, the largeto use epitaxialinQW
In content thestructures
QW will
with different
inevitably cause Inan content.
excessive Forlattice
greenmismatch
and red LEDs,
between thethelarge
GaN Inbarrier
contentlayers
in theandQW thewill
InGaNinevitably
wells,
cause an excessive lattice mismatch between the GaN barrier layers
which will affect the performance of the LEDs. Studies have shown that the maximum In content and the InGaN wells, which will
in
affect the performance of the LEDs. Studies have shown that the maximum
traditional InGaN/GaN QW structure is limited to 25% [99]. Therefore, it is necessary to find a suitable In content in traditional
InGaN/GaN
growth buffer QW structure
layer is limited
as a seed to 25%
layer to grow[99]. Therefore, it iswith
heterostructures necessary to find a suitable
high crystallinity, growth
as shown in
buffer layer
Figure 16. as a seed layer to grow heterostructures with high crystallinity, as shown in Figure 16.
Figure 16.
Figure Multicolor LED
16. Multicolor LED structure
structure with
with aa growth
growth buffer
buffer layer.
layer.
Using its TM technology, Soitec developed a truly relaxed InGaN pseudo-substrate

Using its Smart
Smart Cut
CutTM technology, Soitec developed a truly relaxed InGaN pseudo-substrate
(InGaNOS).
(InGaNOS). The InGaNOS layer is deposited between
The InGaNOS layer is deposited between thethe GaN substrate and
GaN substrate and thethe InGaN
InGaN MQWMQW active
active
layer. This
layer. Thisarrangement
arrangementcan canalleviate
alleviatethe
the compressive
compressive strain
strain between
between thethe layers,
layers, thereby
thereby reducing
reducing the
the lattice mismatch and internal polarization electric field between the GaN
lattice mismatch and internal polarization electric field between the GaN and InGaN with high and InGaN with high
In
In content that exhibit high In doping capacity [100,101]. In 2017, Even et al. tested the
content that exhibit high In doping capacity [100,101]. In 2017, Even et al. tested the performance of performance of
three InGaNOS types with different in-plane lattice constants under three various
three InGaNOS types with different in-plane lattice constants under three various growth conditions growth conditions
(3.190
(3.190 Å,
Å, 3.200
3.200 Å,Å, and
and 3.205
3.205 Å),
Å), and
and the
the results
results are
are shown
shown in in Figure
Figure 1717 [102]. The test
[102]. The test results
results show
show
that the
that the InGaN
InGaN structure
structure grown
grown onon the
the InGaNOS
InGaNOS substrate
substrate can
can achieve
achieve emissions
emissions fromfrom blue
blue to
to amber
amber
(482 nm to 617 nm), and the IQE values measured at 536 nm and 566 nm
(482 nm to 617 nm), and the IQE values measured at 536 nm and 566 nm are 31% and 10%,are 31% and 10%, respectively.
Therefore,
respectively. InGaNOS technology
Therefore, InGaNOS cantechnology
effectively can
grow LEDs of different
effectively grow LEDs colorsof on the same
different substrate.
colors on the
same substrate.
Figure
Figure 17. (a–c) are
17. (a–c) are the
the PL
PL (photoluminescence)
(photoluminescence) spectras
spectras at
at 300
300 K
K of
of the
the blue,
blue, green,
green, and
and amber
amber InGaN
InGaN
heterostructures
heterostructures grown in InGaNOS under three growth conditions. The insets in the right
grown in InGaNOS under three growth conditions. The insets in the lower lowercorner
right
are emission
corner diagramsdiagrams
are emission of the InGaNOS
of thesamples
InGaNOS under laser excitation,
samples under laser where (a) blue luminescence
excitation, where (a) blue is
observed for InGaNOS
luminescence is observed a =InGaNOS
withfor 3.190 Å grown
with aat=a3.190
growth temperature
Å grown and rate
at a growth
◦
of 750 C and
temperature and0.1rate
lm/h,
of
respectively; (b) green luminescence is observed for InGaNOS with a = 3.200 Å grown
750 °C and 0.1 lm/h, respectively; (b) green luminescence is observed for InGaNOS with a = 3.200 Å at a growth
temperature and rate of 730 ◦ C and 0.1 lm/h, respectively; (c) amber luminescence is observed for
grown at a growth temperature and rate of 730 °C and 0.1 lm/h, respectively; (c) amber luminescence
InGaNOS with a = 3.205 Å grown at a growth temperature and rate of 720 ◦ C and 0.3 lm/h, respectively.
is observed for InGaNOS with a = 3.205 Å grown at a growth temperature and rate of 720 °C and 0.3
Reproduced from [102], with permission from American Institute of Physics, 2017.
lm/h, respectively. Reproduced from [102], with permission from American Institute of Physics, 2017.
In 2020, Dussaigne et al. experimentally proved that the deposition of an InGaN/GaN superlattice
In 2020, Dussaigne et al. experimentally proved that the deposition of an InGaN/GaN
structure on an InGaNOS pseudo-substrate has the potential to fill surface V defects and further
superlattice structure on an InGaNOS pseudo-substrate has the potential to fill surface V defects and
improve the crystal quality on InGaNOS [103]. The team used this structure to prepare a red-emitting
further improve the crystal quality on InGaNOS [103]. The team used this structure to prepare a red-
MQW on InGaNOS and measured its center wavelength at 624 nm with an IQE of 6.5% estimated from
emitting MQW on InGaNOS and measured its center wavelength at 624 nm with an IQE of 6.5%
the ratio of the PL intensities measured at 20 and 290 K.
estimated from the ratio of the PL intensities measured at 20 and 290 K.
InGaNOS pseudo-substrate technology can successfully overcome the internal strain of the
InGaNOS pseudo-substrate technology can successfully overcome the internal strain of the
GaN/InGaN LED structure, allowing the amount of In doping to exceed its own limits and emit longer
GaN/InGaN LED structure, allowing the amount of In doping to exceed its own limits and emit
wavelength light. With selective area growth technology (SAG), this technology has the potential to
longer wavelength light. With selective area growth technology (SAG), this technology has the
grow RGB micro-LEDs on the same substrate.
potential to grow RGB micro-LEDs on the same substrate.
4.2. Monolithic Wavelength Tunable MQW Micro-LEDs
4.2. Monolithic Wavelength Tunable MQW Micro-LEDs
The light wavelength emitted by an LED is mainly controlled by the structure and composition
of theThe lightquantum
LED’s wavelength well.emitted by angrowing
Therefore, LED is mainly controlled
a QW structure by the structure
containing multiple and composition
active regions
of the LED’s quantum well. Therefore, growing a QW structure containing
on the same substrate and injecting carriers into different active layers of the LED structure multiple active regions
in a
on the same substrate and injecting carriers into different active layers
controllable manner under external conditions is another method to realize a single-chip LED that of the LED structure in a
controllable manner
emits multi-wavelength light. under external conditions is another method to realize a single-chip LED that
emitsInmulti-wavelength
2010, Damilano et light.
al. proposed a blue LED structure grown on top of InGaN/GaN MQWs,
In 2010, Damilano
which can convert the emission et al. proposed
wavelengtha blue
fromLED structure
blue grown on[104,105].
to yellow-green top of InGaN/GaN MQWs,
The LED structure
which
has twocan convert
active the emission
regions. wavelength
The first active region from blue blue
generates to yellow-green
light through [104,105]. The LED
EL and then structure
stimulates the
has two active regions. The first active region generates blue light through
PL of the MQW layer, thereby realizing the conversion of blue light to yellow-green light; this region’sEL and then stimulates
the PL structure
overall of the MQW layer,inthereby
is shown realizing
the left half the 18a.
of Figure conversion of blue light toLED
This dual-active-layer yellow-green light;
structure uses this
metal
region’schemical
organic overall structure is shown(MOCVD)
vapor deposition in the left half of Figure
technology to18a.
grow This dual-active-layer
a 6.6 µm thick undoped LEDGaNstructure
layer
uses metal organic chemical vapor deposition (MOCVD) technology to
on a c-plane sapphire substrate. Then, 20 periods of InGaN (3.1 nm)/GaN (20 nm) MQW are depositedgrow a 6.6 μm thick undoped
GaNused
and layerason thea green-yellow
c-plane sapphire lightsubstrate.
conversion Then,
layer.20Finally,
periods of InGaN
a blue LED is (3.1 nm)/GaN
grown on MQW (20 nm) MQW
as a pump
are deposited
light source. The andluminous
used as the green-yellow
color of the LEDlight conversion
depends on thelayer. Finally,ofathe
absorption blue LED light
pump is grown
source on
MQW as a pump light source. The luminous color of the LED depends on
by the yellow-green light conversion layer, which is the IQE of the yellow-green light conversion the absorption of the pump
light source
layer. by the yellow-green
The experimental results show light
thatconversion layer,ofwhich
the absorption is the
the light IQE of the
conversion layeryellow-green
changes withlight the
conversion
pump layer. The
light source, experimental
which means that the results show
shorter thethat
pump thewavelength
absorption is, of the
thestronger
light conversion layer
the absorption
changes of
capacity withthe the
lightpump light source,
conversion which
layer will means
be, and that the
the closer theshorter
emission thewavelength
pump wavelength
of the LED is,will
the
strongertothe
become absorption capacity
yellow-green. The rightof theoflight
half Figureconversion
18a showslayer will be, and the
the luminescence closer
of the the when
device emissionthe
wavelength of the LED will become to
pump light source wavelength changes from 405 nm to 450 nm.yellow-green. The right half of Figure 18a shows the
luminescence of the device when the pump light source wavelength changes
In 2012, Dawson’s team demonstrated a micro-LED array made of an InGaN epitaxial structure from 405 nm to 450 nm.
with In 2012,InDawson’s
a high content up team demonstrated
to 0.4 a micro-LED
[106]. The micro-LED array
array made
in this of anhad
study InGaN epitaxialofstructure
a resolution 16 × 16,
with a high In content up to 0.4 [106]. The micro-LED array in this study had a resolution of 16 × 16,
and the pixel diameter and center spacing were 72 μm and 100 μm, respectively. The authors used a
flip-chip design to bond the micro-LED on a CMOS substrate and achieved a programmable dynamic

and the pixel diameter and center spacing were 72 µm and 100 µm, respectively. The authors used a
image display
flip-chip design through
to bonda the
computer
micro-LED and
on aa CMOS
field-programmable gate array
substrate and achieved (FPGA). The
a programmable epitaxial
dynamic
imageof
structure display
this LED through a computer
includes and athick
a 1.5 μm field-programmable
GaN buffer layer, gate aarray
4 μm (FPGA). The epitaxial
thick n-doped GaN structure
layer, five-
of this LED includes a 1.5 µm thick GaN buffer layer, a 4 µm thick n-doped
period In0.18Ga0.82N (3 nm)/GaN (10 nm) MQWs (secondary active layer) emitted at 460 nm, five- GaN layer, five-period
In0.18
period InGa
0.4Ga
NN(3(2.5
0.820.6 nm)/GaN
nm)/GaN (10 nm)
(12 nm) MQWsMQWs (secondary active
(the main layer)
active emitted
layer) at 460atnm,
emitted 600five-period
nm, and a 210
In0.4 Ga0.6 N (2.5 nm)/GaN (12 nm) MQWs (the main active layer) emitted at 600 nm, and a 210 nm thick
nm thick p-GaN layer, as shown in Figure 18b. The secondary active layer with low In content is used
p-GaN layer, as shown in Figure 18b. The secondary active layer with low In content is used as a
as a carrier storage layer, and a pre-strain relaxation layer is used to improve the radiation efficiency
carrier storage layer, and a pre-strain relaxation layer is used to improve the radiation efficiency of the
of the main active layer. By adjusting the injection current of the micro-LED, the emission wavelength
main active layer. By adjusting the injection current of the micro-LED, the emission wavelength of the
of the
LEDLED cancanbe be changed
changed fromfrom
red red to green,
to green, as shown
as shown in theinupper
the upper
part ofpart of Figure
Figure 18c.
18c. This This
blue blue
shift of shift
of the
thewavelength
wavelengthisiscaused caused by the screening
by the screeningand andband-filling
band-filling effects
effects of QCSE
of QCSE on non-polar
on non-polar quantum
quantum
wells. In addition,
wells. In addition, to ensure
to ensurethat
thatthe
thepixels
pixelsofof different colorshave
different colors haveuniform
uniform brightness,
brightness, the duty
the duty cyclecycle
of the driving voltage can be changed to modulate the average brightness of each pixel, as shown
of the driving voltage can be changed to modulate the average brightness of each pixel, as shown in in
the lower
the lower partpart of Figure
of Figure 18c.
18c.
Figure 18. (a) The blue LED structure grown on top of InGaN / GaN multiple QWs with light emission
Figure 18. (a) The blue LED structure grown on top of InGaN / GaN multiple QWs with light emission
under different wavelength pump light sources proposed by Damiano et al. Reproduced from [104],
under different wavelength pump light sources proposed by Damiano et al. Reproduced from [104],
with permission from American Institute of Physics, 2010; The dual active area micro-LED structure
withproposed
permission from
by the American
Dawson team Institute of In
with a high Physics, 2010; The
mole fraction dual
up to active
0.4 (b), andarea micro-LED
its (c) EL spectrum structure
in
proposed by the Dawson
using different injectionteam with
currents a high
and In mole fraction
the brightness change ofupthe
toLED
0.4 (b),
underand its (c) EL
different dutyspectrum
cycles in
usingofdifferent injection
the driving voltagecurrents and the from
(c). Reproduced brightness change
[106], with of the LED
permission fromunder different
Institute duty cycles
of Electrical and of
the driving voltage
Electronics (c). 2012.
Engineers, Reproduced from [106], with permission from Institute of Electrical and
Electronics Engineers, 2012.
The multi-active area epitaxial structure micro-LED proposed by Dawson’s team can achieve red
light emissions at 0.5 mA with an output power of 0.93 W, green light emissions at 80 mA with 0.5% duty
The multi-active area epitaxial structure micro-LED proposed by Dawson’s team can achieve
and 1.03 W output power, and yellow light emissions at 18 mA with a duty cycle of 2% and an output
red light emissions at 0.5 mA with an output power of 0.93 W, green light emissions at 80 mA with
power of 0.97 W, which surpasses the limitations of monolithic InGaN-based LED multi-color displays.
0.5%However,
duty andbecause
1.03 Wthe output power, and yellow light emissions at 18 mA with a duty cycle of 2%
driving circuit for this structure is too complicated to realize the independent
and control
an output power of 0.97 W,
of each pixel, this technologywhichis surpasses the limitations
currently unable to achieve of monolithic
a full-color InGaN-based
micro-LED display,LED
multi-color
and the IQEdisplays.
and colorHowever,
adjustmentbecause thethe
range of driving circuittofor
device needs this structure
be further optimized. is too complicated
In 2016, Chen’s to
realize
teamthe independent
inserted a carriercontrol
blockingoflayer
each(ICBL)
pixel,between
this technology
multiple QWsis currently
in different unable
active to achieve
regions a full-
[107].
colorThe
micro-LED
experiments display,
showedand thatthe IQE
ICBL canand color
guide mostadjustment range
of the carriers (holesof and
the electrons)
device needs to be
into the further
target
QW where
optimized. they recombine,
In 2016, Chen’s team thereby generating
inserted lightblocking
a carrier of a specific
layerwavelength
(ICBL) betweenunder the injectionQWs
multiple of in
different controlled currents. This structure effectively controls the carrier injection
different active regions [107]. The experiments showed that ICBL can guide most of the carriers (holes distribution of the
and entire active into
electrons) region andtarget
the can beQWusedwhere
to improve
theythe luminous efficiency
recombine, thereby and wavelength
generating range
light of ofa the
specific
multi-active QW structure of LED with an adjustable wavelength.
wavelength under the injection of different controlled currents. This structure effectively controls the
carrier injection distribution of the entire active region and can be used to improve the luminous
efficiency and wavelength range of the multi-active QW structure of LED with an adjustable
wavelength.
4.3. Monolithic Wavelength Tunable Nanowire LED

The size of a nanowire LED array is at the micron or even submicron level. By horizontally
arranging an RGB LED array composed of this nanowire structure, multi-color emissions can be
4.3. Monolithic Wavelength Tunable Nanowire LED

The size of a nanowire LED array is at the micron or even submicron level. By horizontally
arranging an RGB LED array composed of this nanowire structure, multi-color emissions can be
easily generated. Therefore, nanowire LEDs have been widely studied for their possible use in
full-color displays [108–111]. Compared with conventional InGaN/GaN quantum-well LEDs, nanowire
heterostructures have many obvious advantages, including greatly reducing the dislocation density and
polarization field in the active region of the device, improving the light extraction efficiency, and offering
good compatibility with low-cost, large-area silicon substrates [112–115]. Such nanostructures include
dot-in-a-wire nanowires, core/shell nanowires, and nano-column structures. The emission wavelength
can be modulated by changing the composition, diameter, and injection current of the nanowires.
In 2011, Hong et al. prepared a core/shell GaN nanowire array. By applying different external
voltages, the emission wavelength of the nanowire LED can be continuously modulated from red to
blue [116]. The core/shell GaN nanowire structure is grown on an n+ -GaN/Al2 O3 (0001) substrate
with a SiO2 growth mask layer that has some submicron hole patterns. The average length, diameter,
and adjacent spacing of each nanowire structure are 520 nm, 220 nm, and 550 nm, respectively. All of
these parameters can be controlled by changing the lithography design and growth parameters.
After the GaN nanorod arrays are grown, nano Inx Ga1−x N/GaN MQWs are is epitaxially grown on the
entire surface of each GaN nanorod array via selective metal organic vapor phase epitaxy (MOVPE)
technology. Subsequently, p-type-doped GaN with Mg is coated on the outside of the MQW to form a
capping film. The structure and preparation process are shown in Figure 19a. The emission wavelength
of the core/shell GaN nanowire LED is controlled by an external voltage, just like a multi-active QW
LED. The lower part of Figure 19a shows a series of EL images under various bias voltages. It can be
seen that, with an increase in bias voltage, the color of the emitted light gradually changes from red
toNanomaterials
blue. 2020, 10, x FOR PEER REVIEW 23 of 33
Figure 19. (a) Shell/core nanowire LED structure and EL images driven by different external
Figure 19. (a) Shell/core nanowire LED structure and EL images driven by different external voltages.
voltages. Reproduced from [116], with permission from John Wiley and Sons, 2011; (b) InGaN/GaN
Reproduced from [116], with permission from John Wiley and Sons, 2011; (b) InGaN/GaN dot-in-a-
dot-in-a-wire LED structure. Reproduced from [117], with permission from Institute of Physics, 2011.
wire LED structure. Reproduced from [117], with permission from Institute of Physics, 2011. All rights
All rights reserved.
reserved.
In the same year, Nguyen et al. proposed a nanowire LED containing QDs (dot-in-a-wire).
In 2020, Liu et al. prepared nanowire LED arrays with sizes as small as 150 nm through selective
By changing the composition or size of the QDs in the nanowire structure, efficient emissions can be
area growth (SAG) technology [119,120]. The authors used radio frequency plasma-assisted
achieved over almost the entire visible wavelength range [117,118]. InGaN/GaN dot-in-a-wire LEDs
molecular beam epitaxy (PA-MBE) and a Ti mask to selectively grow nanowire arrays of different
are grown directly on Si (111) substrates, and the device heterostructure is composed of a 0.4 µm GaN:Si
diameters on a sapphire substrate. The nanowire structure consisted of a 0.44 μm n-GaN layer, a 6-
layer, an InGaN/GaN active layer, and a 0.2 µm GaN:Mg layer. This structure is shown in Figure 19b.
period InGaN/GaN quantum disk, and a 0.15 μm p-GaN layer, as shown in Figure 20a. The emission
There are multiple InGaN/GaN QDs with a diameter of about 3 nm in the active area, and the core of
wavelength of a nanowire is related to the diameter of the nanowire. As the diameter decreases, the
each QD is InGaN, which is then covered by GaN. The different emission wavelengths are produced
emission wavelength moves closer to a red color. This is due to the lateral diffusion of In atoms during
the growth of the nanowires. Small diameter nanowires can limit this diffusion, thereby increasing
the contribution of In component incorporation. Therefore, by changing the diameter of the nanowire,
the emission wavelength of the nanowire LED can be modulated, as shown in Figure 20b. In addition,
by increasing the effective area (changing the diameter and length of the nanowire structure), the
light extraction efficiency of the device can be significantly improved. This method also offers a
by changes to the In composition in the InGaN/GaN QD layer. During the growth process of the active
region of QDs, by using a relatively low substrate temperature or a high In/Ga flux ratio, a high In
composition nanowire structure (up to about 50%) can be achieved, thereby achieving orange/red
emissions. The active area of this nanowire structure is in the middle of the nanowire, far away from
the growth interface. Therefore, the effect of the strain caused by lattice mismatches on the active region
is reduced, and the formation of dislocations is also minimized. In addition, using relatively small
(about 3 nm) InGaN QDs can significantly increase the IQE of the LED. Compared with conventional
plane InGaN/GaN QW LEDs, due to their efficient lateral stress relaxation, InGaN/GaN dot-in-a-wire
Figure 19. (a) Shell/core nanowire LED structure and EL images driven by different external voltages.
nanowire LEDs still offer high efficiency in high current density injection. In addition, they also
Reproduced from [116], with permission from John Wiley and Sons, 2011; (b) InGaN/GaN dot-in-a-
have excellent volt–ampere characteristics, in which cascade resistance (approximately 20–50 Ω) and
wire LED structure. Reproduced from [117], with permission from Institute of Physics, 2011. All rights
leakage currents are very small under a relatively large reverse bias (Under the reverse voltage of −4 V,
reserved.
the leakage voltage is about 0 A).
In
In 2020,
2020, Liu
Liu et
et al. prepared nanowire
al. prepared nanowire LEDLED arrays
arrays with
with sizes
sizes as small as
as small as 150
150 nm
nm through
through selective
selective
area growth (SAG) technology [119,120]. The authors used radio frequency
area growth (SAG) technology [119,120]. The authors used radio frequency plasma-assisted plasma-assisted molecular
beam epitaxy
molecular beam(PA-MBE)
epitaxyand a Ti mask
(PA-MBE) to aselectively
and Ti mask to grow nanowire
selectively arrays
grow of different
nanowire diameters
arrays on a
of different
sapphire
diameterssubstrate. The nanowire
on a sapphire substrate. structure consisted
The nanowire of a 0.44consisted
structure µm n-GaN of layer,
a 0.44aμm6-period
n-GaN InGaN/GaN
layer, a 6-
quantum disk, and a 0.15 µm p-GaN layer, as shown in Figure 20a. The
period InGaN/GaN quantum disk, and a 0.15 μm p-GaN layer, as shown in Figure 20a. The emission emission wavelength of
awavelength
nanowire is related to the diameter of the nanowire. As the diameter decreases,
of a nanowire is related to the diameter of the nanowire. As the diameter decreases, the the emission
wavelength moves closer
emission wavelength moves to closer
a red to
color.
a redThis is This
color. due istodue
the to
lateral diffusion
the lateral of In of
diffusion atoms during
In atoms the
during
growth of the nanowires. Small diameter nanowires can limit this diffusion,
the growth of the nanowires. Small diameter nanowires can limit this diffusion, thereby increasing thereby increasing the
contribution of In
the contribution ofcomponent
In component incorporation.
incorporation. Therefore,
Therefore, byby changing
changingthe thediameter
diameterof ofthe
thenanowire,
nanowire,
the emission wavelength of the nanowire LED can be modulated, as shown in
the emission wavelength of the nanowire LED can be modulated, as shown in Figure 20b. In addition, Figure 20b. In addition,
by increasing the effective area (changing the diameter and length of the nanowire
by increasing the effective area (changing the diameter and length of the nanowire structure), structure), the light
the
extraction efficiency
light extraction of the device
efficiency of the can be significantly
device improved.improved.
can be significantly This method Thisalso offers aalso
method controllable
offers a
emission cone
controllable angle, which
emission has great
cone angle, potential
which in micro-LED
has great potential infull-color
micro-LED displays.
full-color displays.
20. (a)
Figure 20. (a)AAnanowire
nanowirestructure with
structure withdifferent diameters
different and and
diameters (b) its normalized
(b) EL spectrum
its normalized under
EL spectrum
different diameters.
under different Reproduced
diameters. from [120],
Reproduced fromwith permission
[120], from Nano
with permission fromLetters, 2016. 2016.
Nano Letters,
Nanowire
Nanowire LEDs
LEDs have
have the
the growth-dependent
growth-dependent characteristics
characteristics depending
depending on on achieving
achieving tunable
tunable
emission wavelength. By selectively growing nanowire structures with different growth parameters
emission wavelength. By selectively growing nanowire structures with different growth parameters on
the same substrate to form a nanowire LED array, a full-color display can be realized. Compared
on the same substrate to form a nanowire LED array, a full-color display can be realized. Compared with
the conventional InGaN/GaN QW structure, nanowires offer effective stress relaxation to obtain efficient
quantum efficiency, due to their small contact areas and active regions far from the interface, which can
reduce the polarization electric field and dislocation density inside the active region. In addition,
with the conventional

Nanomaterials 2020, 10, 2482 InGaN/GaN QW structure, nanowires offer effective stress relaxation to 24
obtain
of 33
efficient quantum efficiency, due to their small contact areas and active regions far from the interface,
which can reduce the polarization electric field and dislocation density inside the active region. In
because
addition,ofbecause
the extremely small sizesmall
of the extremely and resistance of nanowires,
size and resistance they offerthey
of nanowires, a good current
offer a goodinjection
current
level and heat dissipation.
injection level and heat dissipation.
4.4. Monolithic Integrated Nano-Ring Micro-LED Array
4.4. Monolithic Integrated Nano-Ring Micro-LED Array
In 2018, Sung et al. implemented the conversion of the emission wavelength from green to blue by
In 2018, Sung et al. implemented the conversion of the emission wavelength from green to blue
preparing a nano-ring (NR) structure on a green LED. After that, the authors added red QDs to the blue
by preparing a nano-ring (NR) structure on a green LED. After that, the authors added red QDs to
nanoring to prepare a monolithic RGB micro-LED array [121]. The entire monolithic RGB micro-LED
the blue nanoring to prepare a monolithic RGB micro-LED array [121]. The entire monolithic RGB
device consists of three parts: a normally grown green LED, a blue LED with a nano-ring structure,
micro-LED device consists of three parts: a normally grown green LED, a blue LED with a nano-ring
and a red LED coated with red QDs on the blue LED, as shown in Figure 21a–c. Nano-ring LEDs can
structure, and a red LED coated with red QDs on the blue LED, as shown in Figure 21a–c. Nano-ring
achieve a tunable emission wavelength by changing the width of the nano-ring wall. Due to the lattice
LEDs can achieve a tunable emission wavelength by changing the width of the nano-ring wall. Due
mismatch between InGaN and GaN, there is a large strain inside the active region, which generates an
to the lattice mismatch between InGaN and GaN, there is a large strain inside the active region, which
excessive piezoelectric polarization electric field. This will reduce the overlap of the wave functions of
generates an excessive piezoelectric polarization electric field. This will reduce the overlap of the
holes and electrons, so that the PL emission peak of the green nanoring will be significantly blue-shifted.
wave functions of holes and electrons, so that the PL emission peak of the green nanoring will be
Through the experimental verification in Ref. [122], it is found that the strain in the active region is
significantly blue-shifted. Through the experimental verification in Ref. [122], it is found that the
related to the wall thickness of the nanoring. Therefore, by reducing the width of the nanoring wall,
strain in the active region is related to the wall thickness of the nanoring. Therefore, by reducing the
the blue shift of the emission wavelength of the green nanoring can be achieved. The outer and inner
width of the nanoring wall, the blue shift of the emission wavelength of the green nanoring can be
diameters of the NR prepared by the authors were 900 nm and 700 nm, respectively. The normalized
achieved. The outer and inner diameters of the NR prepared by the authors were 900 nm and 700 nm,
EL spectrum of the three-color RGB NR-QD-micro-LED is shown in Figure 21d. The peak wavelengths
respectively. The normalized EL spectrum of the three-color RGB NR-QD-micro-LED is shown in
of RGB are 630 nm, 525 nm, and 467 nm, and the peak EQE of the green and blue sub-pixels are 16%
Figure 21d. The peak wavelengths of RGB are 630 nm, 525 nm, and 467 nm, and the peak EQE of the
and 15%, respectively.
green and blue sub-pixels are 16% and 15%, respectively.
Figure 21. (a) Structure of the nano-ring (NR)-QD-micro-LED; (b,c) are the SEM images of the RGB
Figure 21. (a) Structure of the nano-ring (NR)-QD-micro-LED; (b,c) are the SEM images of the RGB
pixel array and the nanostructure, respectively; (d) is the RGB NR-QD-micro-LED normalized EL
pixel array and the nanostructure, respectively; (d) is the RGB NR-QD-micro-LED normalized EL
spectrum. Reproduced from [121], with permission from Photonics Research, 2017.
spectrum. Reproduced from [121], with permission from Photonics Research, 2017.
To further improve the performance of the micro-LED, the authors used atomic layer deposition
To further improve the performance of the micro-LED, the authors used atomic layer deposition
(ALD) to deposit a 1 nm thick Al2 O3 layer on the sidewall of the nanoring structure. Doing so effectively
(ALD) to deposit a 1 nm thick Al2O3 layer on the sidewall of the nanoring structure. Doing so
reduced the total internal reflection caused by the inner wall of the nano-ring and the non-radiative
effectively reduced the total internal reflection caused by the inner wall of the nano-ring and the non-
recombination caused by the surface defects of the side wall, which increased the photoluminescence
radiative recombination caused by the surface defects of the side wall, which increased the
intensity of the nano-ring LED by 143.7%. This process also enabled the QDs to be adjacently coupled
photoluminescence intensity of the nano-ring LED by 143.7%. This process also enabled the QDs to
with QWMs through non-radiative resonance energy transfer (NRET), thereby improving the color
be adjacently coupled with QWMs through non-radiative resonance energy transfer (NRET), thereby
conversion efficiency of the QDs. Finally, the authors added a distributed Bragg reflector to the red
improving the color conversion efficiency of the QDs. Finally, the authors added a distributed Bragg
sub-pixel to increase the reuse of blue photons.
reflector to the red sub-pixel to increase the reuse of blue photons.
Thus, the red light produced by this method is generated by QD, which will certainly affect the
Thus, the red light produced by this method is generated by QD, which will certainly affect the
luminous efficiency of the device. However, this wavelength-tunable nanostructure provides a method
luminous efficiency of the device. However, this wavelength-tunable nanostructure provides a
for growing blue and green LEDs on a single substrate, which reduces the cost and complexity of
preparing micro-LED full-color displays.
4.5. Summary
In summary, due to the differences in the growth substrate and composition of LEDs with different
emission wavelengths, there is an extremely low miscibility between them. The consequences of this
low miscibility are mainly manifested as low quantum efficiency, excessively broad emission spectrum,
blue shift of the central emission wavelength, high lateral resistance, and low stability. In addition,
the existing growth process is another factor limiting the emergence of single-substrate multi-color
LEDs. Since LEDs of different compositions need to be grown at different temperatures or gases, it is
also a difficult point to grow one type of LED without destroying other types of LEDs. Furthermore,
stable and precise fine-pitch masks are also necessary for growing multi-color micro-LEDs on the
substrate. A lot of research has been devoted to the preparation of multi-color LEDs that can grow
monolithically. These growth technologies can greatly reduce the cost and difficulty of micro-LEDs
and have great significance to realize the full-color display of micro-LEDs in the future.
Growing a buffer layer is a feasible solution. By depositing a growth buffer layer between the
growth substrate and the active layer, the lattice mismatch between them can be relieved, and the
crystallinity of the heterojunction can be improved, allowing LED structures with different In contents
to be grown on the same substrate. However, the IQE of the green and red sub-pixels will be
much lower than that of the blue sub-pixel, which will affect the uniformity of the full-color display.
Therefore, improving the luminous efficiency of long-wavelength LEDs is an important step for
the realization of single-substrate multi-color micro-LEDs in the future. Many strategies have been
proposed to effectively improve the performance of long-wavelength LEDs, such as using non-polar or
semi-polar growth substrates, to relieve the spontaneous polarization electric field inside the LED [123],
using different MQW structures to reduce the piezoelectric polarization caused by the strain [124,125],
using a quaternary AlGaInN alloy as a barrier, and mutually compensating for the piezoelectric
polarization electric field and the spontaneous polarization electric field by adjusting the composition
of Al and In [126].
Multi-active area QW LEDs can recombine carriers in different active areas by changing the
injection current, thereby emitting lights of different wavelengths. However, excessive In doping will
increase the strain in the InGaN / GaN QWs, which will generate a strong internal electric field that
forces the separation of the electron-hole wave function and reduces the quantum efficiency of the
device. Therefore, the light-emitting wavelength range of the multi-active QW LED cannot cover the
entire visible light band. In addition, since the multi-active area LED modulates the light-emitting
wavelength via the injecting current, designing a drive circuit that can independently control each
pixel is key to applying this technology in displays.
The emergence of nanowire-structured LEDs provides another direction for the monolithic growth
of multicolor LEDs. However, the structural preparation conditions of LEDs are harsh, and, due to
the lack of effective lateral restrictions, the IQEs of such devices may be severely limited by the
non-radiative recombination of carriers caused by defects on the surfaces of the nanowires. In addition,
as the In content in the nanowire structure increases, the emission wavelength will become difficult
to control. Therefore, if nanowire LED displays are to move out of the laboratory in the future,
their growth conditions must be controllable, and their growth distribution must be uniform.
Multicolor micro-LED monolithic growth technology is still in its exploratory period, but there
is no doubt that this technology has great potential. For displays, it is difficult for multi-active
QW LEDs to achieve independent control of each sub-pixel, making it impossible to achieve local
dimming. Therefore, this technology is more suitable for visible light communications with different
wavelengths. Nano-structured LEDs are complex to prepare, and mass production will increase costs.
Therefore, although growing multi-color micro-LEDs on the same substrate can greatly reduce the
frequency of mass transfers, thereby reducing the cost of transfer and the rate of defective chips.
Nano-structured micro-LED displays still need more preparation time before they can appear on the
market. But once the multi-color micro-LED arrays are epitaxial, the RGB pixel pitch is fixed, so the
multi-color micro-LED arrays cannot be applied to drive substrates of different sizes. And once a pixel
is damaged, a single chip cannot be replaced, which also makes subsequent maintenance difficult.
However, monolithic integrated multi-color micro-LEDs have appeared on the market. In October
2019, the micro-LED company Plessey successfully grew blue and green native micro-LEDs on the
same wafer, and, in December of the same year, Plessey realized the growth of efficient red micro-LEDs
on InGaN, which showed the possibility to grow RGB three-color micro-LEDs on the same wafer.
Multi-color LEDs grown on a buffer layer may be the focus of monolithic multi-color LEDs in the future.
5. Conclusions
Ultimately, this article reviewed the various technologies and solutions proposed over the past
ten years for micro-LEDs to achieve full color and summarized the characteristics and defects of these
various technologies. Integrating micro-LEDs of different colors and materials onto the same driving
substrate through transfer and bonding technology is the main method for preparing micro-LED
full-color displays for the market. This article outlined the use of full-color micro-LED displays
prepared by this method and introduced the mass transfer technology used in micro-LED chips.
However, with the improvement of the mass transfer yield index and the demand for high-resolution
high-end displays, it is difficult for current mass transfer technology to achieve high-efficiency and
high-precision transmission, which has aggravated the production costs and maintenance costs of
micro-LED displays and stagnated their marketization. Therefore, before the transfer yields and costs
of mass transfer technologies are improved, full-color micro-LED displays with color conversion layers
will dominate the entire market.
Color conversion technology has developed rapidly in recent years. With this technology, LEDs
of various colors do not need to be grown on different wafers, as well as to carry out transfer bonding.
One only needs to prepare a color conversion medium in a color conversion layer and use blue or
UV LED for pump excitation to achieve multi-color light emission. QDs are the most popular color
conversion medium, and their preparation process is gradually mature. For example, Sharp used QDs
to prepare a 1053 pixels per inch (PPI) full-color micro-LED display prototype. However, the conversion
efficiency of this color conversion material is not perfect, and it is easily degraded by various external
factors during light excitation. These defects are the key research directions for using color conversion
technology to realize micro-LED displays in the future.
Growing RGB three-color LEDs on the same wafer or substrate is currently somewhat impractical,
but this is the ultimate goal for micro-LED full-color displays. At the end of this article, the potential LED
technologies for growing different colors directly on a single chip were introduced. These technologies
have unlimited potential and can overcome the limitations of transfer technology and color conversion
technology. Among them, nanowire LEDs offer good strain relaxation due to their special structures,
giving them great prospects in multi-wavelength emissions. However, their harsh growth conditions
and processes make them suitable only for the laboratory; there is still work needed before we can
grow multi-color LEDs directly on the same wafer.
In the past ten years, micro-LED technology has developed rapidly, but full-color displays using
micro-LEDs are still in their infancy. However, their development is optimistic. Display technology
plays an extremely important role in today’s society. Various emerging products have accompanied an
endless demand for high-resolution, high-contrast, and high-efficiency micro-LED displays. Since Apple
acquired Luxvue in 2014 and began to develop micro-LEDs, major electronics giants have successively
entered the market. This is a good sign because the introduction of the market provides many
possibilities for the development of micro-LEDs. More and more universities and enterprises have
begun to participate in the research and preparation of micro-LEDs. We consider that the purpose
of mass transfer technology research is to improve the efficiency and accuracy of transfer, which is
the only way to reduce the cost of micro-LED displays. And developing the full-color display of
micro-LED is the key to applying micro-LED to the display field. We believe that the two mountains of
micro-LED display in the next decade will be crossed, and micro-LED will lead the field by virtue of
its outstanding performance in energy consumption, color, resolution, and life. From small displays,
such as smart watches, head-mounted displays, and smart glasses, to micro-LED TVs, smart phones,
and projectors, micro-LED technology has quietly arrived as the next generation of display technology.
Author Contributions: Conceptualization, writing, review and supervision J.M., investigation, writing and
editing Y.W., writing, review and supervision P.S., writing, review L.Z., writing, review B.X. All authors have read
and agreed to the published version of the manuscript.
Funding: This research was funded by the Basic Research Program of Shenzhen, grant number
(JCYJ20170412171744267) and the Shenzhen general research fund (JCYJ20190813172405231).
Conflicts of Interest: The authors declare no conflict of interest.
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Full-Color Realization of Micro-LED Displays: Nanomaterials

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Nanomaterials 2020, 10, 2482; doi:10.3390/nano10122482 www.mdpi.com/journal/nanomaterials

Table 1. Performance comparison of micro-light-emitting diodes (micro-LEDs) with liquid-crystal

Display Technology LCD OLED Micro-LED

2.1. Horisontally and Vertically Stacked Micro-LED Structures

In 2020, Ostendo introduced a multi-color addressable micro-LED display—the Quantum Photonic

2.2. Elastomer Stamp Transfer

2.3. Laser-Induced Transfer

2.4. Fluidically Self-Assembled Transfer

2.5. Electrostatic Transfer

2.6. Roll-to-Roll or Roll-to-Panel Imprinting Transfer

Table 2. Comparison of various mass transfer technologies.

R2R (R2P) Transfer yieldyield inLow

Figure 8.8. (a)

Nanomaterials 2020, 10, x FOR PEER REVIEW 14 of 33

Nanomaterials 2020, 10, x FOR PEER REVIEW 15 of 33

Figure 13. (a)

Nanomaterials 2020, 10, x FOR PEER REVIEW 17 of 33

4. Monolithic Multi-Color Growth Technology

Using its TM technology, Soitec developed a truly relaxed InGaN pseudo-substrate

Nanomaterials 2020, 10, x FOR PEER REVIEW 21 of 33

4.3. Monolithic Wavelength Tunable Nanowire LED

4.3. Monolithic Wavelength Tunable Nanowire LED

with the conventional

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