Advanced Materials - 2023 - Shi - Carbon Dots For Electroluminescent Light Emitting Diodes Recent Progress and Future

REVIEW
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Carbon Dots for Electroluminescent Light-Emitting Diodes:

Recent Progress and Future Prospects
Yuxin Shi, Wen Su, Fanglong Yuan,* Ting Yuan, Xianzhi Song, Yuyi Han, Shuyan Wei,
Yang Zhang, Yunchao Li, Xiaohong Li, and Louzhen Fan*
have been extensively explored. To date,

Carbon dots (CDs), as emerging carbon nanomaterials, have been regarded as all-inorganic LEDs, such as gallium nitride
promising alternatives for electroluminescent light-emitting diodes (LEDs) (GaN)-based electroluminescent LEDs,
owing to their distinct characteristics, such as low toxicity, tuneable have been widely used in daily life since
photoluminescence, and good photostability. In the last few years, despite their introduction in the 1960s. However,
they can hardly be integrated with other
remarkable progress achieved in CD-based LEDs, their device performance is
semiconductor technologies into flexible
still inferior to that of well-developed organic, heavy-metal-based QDs, and devices.[3] In addition, organic LEDs have
perovskite LEDs. To better exploit LED applications and boost device already been partially commercialized
performance, in this review, a comprehensive overview of currently explored due to their high device performance and
CDs is presented, focusing on their key optical characteristics, which are long operational lifetime.[4] Considering
their weak molecular interactions, organic
closely related to the structural design of CDs from their carbon core to
materials are also promising for use in
surface modifications, and to macroscopic structural engineering, including flexible devices.[5] Nevertheless, organic
the embedding of CDs in the matrix or spatial arrangement of CDs. The emitters generally suffer from broad
design of CD-based LEDs for display and lighting applications based on the full-width at half-maximum (FWHM,
fluorescence, phosphorescence, and delayed fluorescence emission of CDs is > 40 nm) of the emission spectra, com-
also highlighted. Finally, it is concluded with a discussion regarding the key plex synthesis methods, and complicated
device manufacturing with high costs,
challenges and plausible prospects in this field. It is hoped that this review
which greatly limit their wide commer-
inspires more extensive research on CDs from a new perspective and cial applications.[6–10] In this case, heavy
promotes practical applications of CD-based LEDs in multiple directions of metal-based quantum dots (QDs) and
current and future research. perovskites, which feature solution pro-
cessability, size/composition-dependent
bright and tuneable photoluminescence
(PL) emission, and narrow FWHMs less
1. Introduction than 40 nm, have been developed as promising candidates for
LEDs.[11–19] However, the severe toxicity of heavy metals in con-
The advent of the information age is motivating the rapid de- ventional QDs and perovskites greatly limits their practical ap-
velopment of electroluminescent light-emitting diodes (LEDs), plications. Therefore, the development of a new generation of
which are considered as the most promising next-generation environmentally friendly and low toxic light-emitting materials
display and lighting technologies.[1,2] The active emission ma- with excellent optical and electrical properties is highly desired
terials in electroluminescent LEDs, serving as the key com- for next-generation high-performance full-color display and light-
ponents for the conversion of electric current into photons, ing technologies.
In the last few years, due to their high photostability, tune-
Y. Shi, F. Yuan, T. Yuan, X. Song, Y. Han, S. Wei, Y. Zhang, Y. Li, X. Li, L. Fan able PL emission, low toxicity and solution-processability,[20–24]
Key Laboratory of Theoretical & Computational Photochemistry of carbon dots (CDs) have attracted tremendous attention for opto-
Ministry of Education electronic devices, especially for electroluminescent LEDs.[25–35]
College of Chemistry
Beijing Normal University
The optical properties of CDs are generally determined by their
Beijing 100875, China specific quantum-confined, chemical, and surface structures,
E-mail: flyuan@bnu.edu.cn; lzfan@bnu.edu.cn which enable various degrees of tunability and precise design in
W. Su CDs.[36–43] In general, the structural design of CDs is mainly clas-
CAS Center for Excellence in Nanoscience sified as the design of the carbon core and surface modification
National Center for Nanoscience and Technology and macroscopic structural engineering, including the embed-
Beijing 100190, China
ding of CDs in the matrix or the spatial arrangement of CDs.
The ORCID identification number(s) for the author(s) of this article First, the arrangement of the benzene ring that determines the
can be found under https://doi.org/10.1002/adma.202210699 edge morphology, such as zigzag and armchair, and heteroge-
DOI: 10.1002/adma.202210699 neous elemental doping are usually combined to modulate the
Adv. Mater. 2023, 35, 2210699 2210699 (1 of 19) © 2023 Wiley-VCH GmbH
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intrinsic structure of the internal carbon core.[44–49] The structure

of the carbon core is closely related to the typical particle size and
shape of CDs and even the PL centers and exciton capture cen-
ters. Moreover, the structural functionalization of CDs, typically
including the chemical bonding of functional groups, organic
small molecules, and polymers, is also crucial to tune the opti-
cal and photophysical properties of CDs, such as the energy lev-
els, exciton recombination and electron–phonon coupling, thus
inducing tuneable PL, improved PL quantum yield (PLQY) and
the controlled FWHM of CDs.[47–52] Interestingly, macroscopic
structural regulation by embedding CDs in the matrix and spa-
tial arrangement for those packed with multiple dots, such as as-
sembly and aggregation induced by surface interactions of hydro-
gen bonding, metal coordination, electrostatics or 𝜋-𝜋 conjuga-
tion, can be tailored to program different chemical and physical
functions of CDs.[53–57] This can not only restrict the interference
of the external environment and intramolecular vibrations and
rotations but also controllably endow CDs with unique optical
properties, especially triplet state-related optical properties such
as room temperature phosphorescence (RTP) and delayed fluo-
rescence (DF).[58–61] These features provide a solid foundation for
Figure 1. Schematic illustration of the topical areas of this review, focus-
the exploration of the optical and photophysical properties and ing on the optical properties and recent trends in electroluminescent LED
mechanisms of CDs and further indicate the considerable poten- applications of CDs.
tial applications of CDs in electroluminescent LEDs.[62–66]
Since the first report of CD-based electroluminescent LEDs
in 2011,[67] remarkable progress has been made in this field to
date, benefiting from the elaborate structural design of CDs with addition, the prospects of CDs with fluorescence emission, RTP
unique optical properties. For instance, red fluorescent carbon and DF emission for electroluminescent LED applications are
quantum dots (CQDs) with a high PLQY up to 86% have been also discussed (Figure 1). Finally, to realize high-quality CDs with
synthesized, and a maximum luminance (Lmax ) up to 5909 cd m−2 improved optical and electrical properties for high-performance
has been achieved for the corresponding warm white LEDs.[68] electroluminescent LEDs suitable for future practical applica-
Furthermore, by engineering the rigid triangular structure of the tions, we conclude with a discussion regarding the key challenges
carbon core, multicolor fluorescent CDs with narrow FWHMs and plausible future prospects in this field. We hope that this re-
of 30 nm have also been successfully prepared for the fabrica- view will help readers not only grasp the progress of research on
tion of high color purity narrow-bandwidth emission electrolumi- the optical characteristics of CDs and their LED applications but
nescent LEDs.[69] Moreover, deep-blue LEDs based on CDs with also appreciate the remaining challenges and problems. We be-
a PLQY of 70% ± 10% showed an external quantum efficiency lieve that the future of CDs and their LED applications is bright,
(EQE) of 4%, which is the maximum EQE value achieved based and we anticipate that this field will continue to grow on multiple
on the fluorescence emission of CDs.[70] Recently, to break the fronts, with continued impacts occurring for both fundamental
EQE limit of 5% for LEDs based on the fluorescence emission of research and applications.
CDs, the triplet excitons of CDs have been successfully utilized
in electroluminescent LEDs with EQEs greater than 5% by elab-
orately designing a framework structure to regulate the energy 2. Optical Characteristics of CDs
levels of CDs.[71] Despite the remarkable progress achieved, com-
pared with well-developed organic LEDs and conventional heavy- Literally, CDs are typically a class of 0D carbon nanoparticles,
metal-containing QDs and perovskite LEDs, CD-based electrolu- which are less than 10 nm across with an obvious crystal lat-
minescent LEDs still exhibit inferior device performance, includ- tice parameter of ≈0.34 and ≈0.21 nm corresponding to the (002)
ing low luminance, broad FWHM, low EQE, and severe energy and (100) interlayer spacing of graphite and graphene.[72–74] The
losses of triplet excitons, which thus hinders their further practi- optical properties of CDs can not only be tailored by controlling
cal applications. the size, shape, and heteroatom doping but also be influenced by
Currently, there are many reviews published focusing on the numerous different functional groups, such as epoxy, carbonyl,
synthesis of CDs and their versatile potential applications. How- hydroxyl, and carboxyl groups, on their surfaces and edges.[75,76]
ever, there are limited review articles focusing on CD-based elec- Therefore, CDs generally exhibit unique optical properties, such
troluminescent LEDs. In this review, to further better exploit as highly tuneable PL emission from deep ultraviolet to near-
the LED applications of CDs and boost the device performance, infrared, improved PLQY, controlled FWHM, and exceptional
we discuss the recent frontiers in the optical characteristics of triplet state-related RTP and DF emissions, stemming from the
CDs based on structural design from a broad range of perspec- remarkable quantum confinement effect, surface effect, edge ef-
tives, including tuneable PL emission, improved PLQY, con- fect, and readiness for functionalization with various organic or
trolled FWHM, and triplet state-related RTP and DF emission. In polymeric species.
Figure 2. a) Calculated emission wavelength using the time-dependent DFT method in vacuum as a function of the diameter of CDs and b) as a
function of the coverage of functional groups. Reproduced with permission.[47] Copyright 2014, Royal Society of Chemistry. c) The optimized ground
state calculated at the DFT level, and d) HOMO and LUMO orbital distribution for the series of CDs at an optimized ground state. e) Calculated vertical
transition energies for the triplet state [EVA (S1 )] at the ground state geometry and spin-orbit coupling matrix element (SOCME) values in accordance
with the extent of oxidation. Reproduced with permission.[81] Copyright 2020, Wiley-VCH. f) Optimized geometric structure of pristine and various C–N
configurations of CDs, i.e., pyridinic-N, pyrrolic-N and graphitic-N CDs, as well as pyrrolic-N-rich CDs in varying pyrrolic-N concentrations from 1.4% to
10%. g) Calculated UV‒Vis absorption spectra. Reproduced with permission.[82] Copyright 2022, Springer Nature.
2.1. Tuneable PL Emission low to red, respectively.[46] Accordingly, theoretical calculations

demonstrated that with increasing size from 0.46 to 2.31 nm,
From the perspective of photophysics and practical applications, a redshift in the fluorescence emission peaks is observed with
one of the most fascinating features of CDs is their tuneable tuneable emission wavelengths ranging from deep UV to near
PL emission. Considering the energy level splitting due to the infrared (Figure 2a).[47] The observed linear and steep size de-
size of the sp2 -conjugated domain being smaller than the exci- pendence indicated that by varying the diameters, the emission
ton Bohr radius, the bandgap emission depends on the size of of CDs can cover the entire visible spectrum region. It has also
the sp2 -conjugated domains of CDs.[37–43] For instance, we first been shown that CDs with dominant zigzag edges have a smaller
obtained bright tuneable multicolor bandgap fluorescent CQDs bandgap than similarly sized CDs with dominant armchair edges
with particle sizes ranging from 1.95 nm to 6.68 nm, correspond- because of localized states on zigzag edges. Therefore, zigzag
ing to different PL emissions from blue to green and from yel- edges of CDs will narrow the bandgap with red-shifted emission.
Furthermore, these studies also demonstrated that although dif- tional groups prepared under harsh reaction conditions, free
ferent functional groups show a strong influence on the highest excitons are easily trapped and quenched at defect sites.[83,84]
occupied molecular orbital (HOMO) and the lowest unoccupied Therefore, numerous excitons are depleted as heat rather than
molecular orbital (LUMO) of CDs with intact sp2 carbon cores, emitted from core states or surface states, which fundamentally
the differences between energy gaps that determine the emission limits the fabrication of high-performance CD-based electrolu-
wavelengths of CDs vary little. minescent LEDs. Therefore, engineering a high-quality carbon
However, for CDs that usually possess many defects inside or core with high crystallinity can greatly suppress energy losses
at the edges of the carbon core, the tuning of PL emission is and improve the optical properties of CDs. For instance, almost
completely different.[77,78] For instance, CDs synthesized by top- defect-free narrow-bandwidth emission triangular CQDs (NBE-
down methods, such as acid-oxidation exfoliation and laser ab- T-CQDs) have been successfully synthesized. The well-resolved
lation, have been revealed to show a large number of surface de- lattice fringes at 0.21 nm observed from high-resolution trans-
fects from sp3 and sp2 hybridized carbons and functional groups, mission electron microscopy (HRTEM) images correspond to the
thus leading to excitation-dependent PL emission.[79,80] More- (100) interlayer spacing of graphene, which indicates the high
over, Figure 2b further shows that the oxidized functional groups crystallinity of CDs that results in a high PLQY of up to 72%.[69]
at the edge of CDs and vacancy defects play a crucial role in reg- The PLQY of CDs is also influenced by surface and edge
ulating the energy levels and bandgap energies of CDs, which effects.[85,86] For example, oxygen-containing functional groups
could result in large redshifts of the emission peaks of CDs, rang- have been demonstrated to serve as nonradiative recombina-
ing from green emission to red emission. tion centers, which could induce fast charge trapping and de-
The different singlet–triplet energy splitting of CDs can also be crease the 𝜋 electron cloud density of CDs, thus leading to a re-
controlled by different ratios of functional groups, thus leading duced PLQY. Therefore, PLQY can be significantly improved by
to a change in the fluorescence emission to triplet state-related surface modification or passivation by functional groups, such
RTP and DF emission of CDs. For example, by varying the de- as amino, carboxyl, alkyl, and polymeric molecules. For exam-
gree of oxidation, the increased ratio of oxygenated carbon to sp2 ple, our group synthesized bright red-emissive electron-donating
carbon in CDs can induce the tuning of long-lived afterglow from group passivated CQDs (R-EGP-CQDs) with a PLQY as high
RTP to thermally activated DF (TADF).[81] Density functional the- as 86.0%.[68] Theoretical studies demonstrated that the rigid 𝜋-
ory (DFT) calculations further revealed that a large number of conjugated skeleton structure is the origin of red emission, and
oxygen-containing functional groups on the edge sites of CDs can the passivation of N,N-dimethyl, N,N-diethyl, and N,N-dipropyl
induce geometry distortion of CDs (Figure 2c). This will lead to plays a key role in inducing the charge transfer excited state in
a larger electron redistribution, thus resulting in a small energy the 𝜋-conjugated structure, thus achieving the record high PLQY
gap due to the small spatial orbital overlap between the HOMO for red fluorescent CDs to date.
and LUMO energy levels (Figure 2d). The high extent of oxidation In addition, due to the large 𝜋-conjugated carbon plane,
in CDs strongly supports the energetic stabilization of the sin- CDs show a strong tendency to form sandwich-shaped H-
glet state and effective electronic transition between singlet and aggregates. In this case, the PLQY is significantly reduced due
triplet states (Figure 2e). Moreover, controlling the C–N configu- to the severe aggregation-caused quenching (ACQ) effect, espe-
rations and concentrations are promising strategies to tailor the cially for solid-state CDs with strong intermolecular 𝜋−𝜋 stack-
optical properties of CDs. The role of nitrogen in forming various ing. Different from ACQ induced by strong intermolecular in-
C–N configurations, i.e., pyridinic-N, pyrrolic-N, and graphitic-N, teractions, aggregation-induced emission (AIE), depending on
and their concentrations were studied based on thermotical cal- the molecular structures and intermolecular packing, generally
culations (Figure 2f). The calculated UV‒vis absorption spectra possesses twisted-propeller-shaped molecular structures.[87–89]
revealed that, compared with other configurations, the spectrum These unique structures greatly boost the PL emission without
of pyrrolic-N CDs shows an additional minor peak centered at significant displacement in the aggregated state. The design of
525 nm, which is similar to that of as-synthesized N-rich CDs AIE CDs with fascinating structures and functionalities, such as
with the tail up to the first NIR window range, and the inten- the modification of functional groups and assembly, the restric-
sity varies with the concentration of nitrogen from 1.4% to 10% tion of intramolecular motions and structure rigidification, has
(Figure 2g).[82] Generally, functional groups with strong electron been reported in various studies. Moreover, since AIE is practi-
withdrawing (e.g., nitryl, cyanide) and electron donating proper- cally useful for solid-state emission, CDs with AIE used as the
ties (e.g., alkyl, amino) have a greater impact on the distribution active layer may lead to hitherto impossible technological inno-
of electron clouds than other functional groups, which are closely vations in the development of electroluminescent LEDs. There-
related to the overlap and shift of different energy level orbitals. fore, a macroscopic spatial arrangement can be carried out to pre-
vent the formation of aggregated states of CDs.[90–92] For exam-
ple, boric acid edge-functionalized CDs with crystalline graphite
2.2. Improved PLQYs structures were synthesized, which showed a high PLQY of up
to 90% in a polystyrene matrix.[93] By elaborately controlling in-
PLQY is one of the most important optical parameters for light- terlayer 𝜋–𝜋 stacking and hydrogen bonding, CDs, as versatile
emitting materials. Generally, a low PLQY means severe nonra- building blocks, can be self-assembled to form 2D nanosheets.
diative energy losses. The PLQY of most synthesized CDs is very Due to the coexistence of CD–CD and CD–solvent interactions,
low (typically < 20%) due to the existence of abundant edge and the CDs in different polar solutions can be self-assembled in dif-
surface defects. For example, for CDs with numerous sp3 and ferent ways, thus leading to different PLQYs with tuneable PL
sp2 hybridized carbons and dangling chemical bonds or func- emission. Compared with green‒yellow PL dominated by the
Figure 3. a) Synthesis route of the NBE-T-CQDs by solvothermal treatment and the typical aberration-corrected high-angle annular dark-field scanning
TEM images of B-, G-, Y-, and R-NBE-T-CQDs. Scale bar, 2 nm. b) Photographs of the NBE-T-CQD ethanol solution under daylight and fluorescence
images under UV light (excited at 365 nm). c) Normalized UV‒vis absorption and PL spectra of B-, G-, Y-, and R-NBE-T-CQDs. Reproduced with
permission.[69] Copyright 2018, Springer Nature. d) Schematic illustration of the synthetic strategy of HCP-DB-CDs. e) Absorption and f) PL of HCP-
DB-CDs. Reproduced with permission.[70] Copyright 2020, Springer Nature. g) Schematic illustration of the preparation of CPDs. h) Absorption spectra
and i) PL emission spectra. Reproduced with permission.[55] Copyright 2020, Wiley-VCH.
monomer states in nonpolar solvents, long-wavelength emission explored by choosing different precursors and various synthe-
with high PLQY in CDs could be realized due to the assembled sis methods, which heralds the potential of high color purity
2D nanosheets of CDs in less polar solvents. However, the emis- CD-based LEDs that could compete with the conventional well-
sion of CDs will be significantly quenched by the assembled fi- developed heavy metal-based QD LEDs available today.
brous morphology with enhanced 𝜋–𝜋 stacking in a strongly po- First, the design of the carbon core is expected to be the most
lar solvent. Nevertheless, limited by the incomplete exploration intuitive and effective approach to achieve a narrow FWHM, in
of CDs, developing facile and efficient approaches for structural which the specific precursors can precisely control the nucleation
control to achieve high-quality CDs with full-color emission and and growth process of CDs. Significantly, by selecting a three-
near-unity PLQY remains a major challenge. fold symmetric phloroglucinol to engineer a uniquely shaped
carbon core, highly crystalline NBE-T-CQDs with a special tri-
angular structure were first synthesized (Figure 3a). The strong
2.3. Full Width at Half-Maximum and narrow excitonic absorption peaks of the NBE-T-CQDs cor-
respond well to the PL emission spectra with a narrow FWHM
2.3.1. Narrow FWHM for Displays of 29 nm, which for the first time subverts the traditional view
that only broadband emission spectra can be achieved in CDs
To realize a wide color gamut for display technology, a nar- (Figure 3b,c).[69] It has been revealed that CDs with a triangu-
row FWHM of the electroluminescence (EL) spectra of LEDs lar structure (T-CDs) show more uniformly distributed electron
with high color purity light emission is highly desired. Typically, cloud density across the whole molecular structure than CDs
electroluminescent LEDs that can meet the requirements for with a square-like structure (S-CDs), thus resulting in dramati-
ultrahigh-definition display applications should possess FWHMs cally reduced electron–phonon coupling. Therefore, in terms of
as narrow as 20 nm. Remarkable progress has been achieved optical properties, the FWHM of the PL spectra of T-CDs is much
in the preparation of efficient CDs and the fabrication of smaller than that of S-CDs.
monochrome CD-based electroluminescent LEDs. However, due In view of surface defects and different kinds of functional
to multiple surface defects and PL centers, most of the reported groups, the emission spectra of CDs usually show a large FWHM
CDs show broadband emission spectra with a large FWHM of of more than 80 nm.[94,95] Chemical modification has been
more than 80 nm, which severely restricts the CDs for ultrahigh- demonstrated as an effective strategy to suppress molecular vi-
definition display applications. To realize high color purity light bration and distortion to achieve narrow-linewidth emission. For
emission, a series of CDs with narrow FWHMs have been widely instance, high color purity deep-blue CDs (HCP-DB-CDs) have
been successfully synthesized (Figure 3d), which displayed a nar- and 1,3-di-9-carbazolylbenzene (mCP) with blue emission or by
row FWHM of 35 nm and a color coordinate of (0.15, 0.05) combining different CDs with three primary blue, green, and red
closely approaching the Rec. 2020 specification (0.131, 0.046) emission. For example, we synthesized red emissive CQDs (R-
for blue emitters (Figure 3e,f).[70] Theoretical calculations indi- CQDs) with a high QY of 53% and prepared red/green/blue tri-
cated that, compared with oxygen-containing functional groups color CQD phosphors by dispersing R-CQDs and our previously
(especially the carboxyl group and epoxy group) with a strong reported B-CQDs and G-CQDs into a highly transparent poly-
polarization effect, passivating the surface defects of CDs with mer matrix of polyvinylpyrrolidone. By varying the mass ratios
nitrogen-containing functional groups (amino group) can effec- of these phosphors, warm WLEDs were fabricated with a record
tively increase the degree of wavefunction delocalization to stabi- color rendering index (CRI) of 97.[98] Moreover, without the use
lize bandgap fluctuation, thus resulting in PL emission spectra of a polymer matrix, red/green/blue solid-state bandgap fluores-
with a narrow FWHM. Moreover, the influencing factors on the cent carbon quantum rings (R/G/B-SBF-CQRs) centered at 474,
FWHM have also been investigated with DFT calculations. The 530, and 630 nm, respectively, have also been successfully synthe-
results revealed that the FWHM is influenced by the position of sized (Figure 4a). The repulsion of the adjacent –CN groups in the
hydroxyl groups. Investigations of molecules with different lig- three primary color SBF-CQRs can overcome the notorious ACQ
ands (–Br, –OH, –COOH, –NH2 ) have confirmed that larger lig- for solid-state lighting with improved QYs reaching 30–46%. By
ands lead to a redshift of the absorption peak and an enlarged integrating R/G/B-SBF-CQRs phosphors into a 405 nm near-UV
FWHM of the emission spectra.[94] Therefore, for CDs with lig- LED chip without using a polymer matrix, the fabricated WLEDs
ands, reducing the steric hindrance of the ligand and achieving exhibited favorable warm white light emission with a low corre-
better symmetry are expected to achieve a narrow FWHM. These lated color temperature (CCT) of 3576 K, a high CRI of 96.6 and a
results demonstrate that chemical modification plays a signifi- high luminous efficiency of 48.7 lm W−1 (Figure 4b).[57] Although
cant role in regulating the optical properties of CDs, thus pro- white light emission consisting of different emissions from mul-
viding guidelines for the elaborate design of functional groups to tiple components shows a simple operation process, there are a
realize high color purity CDs with narrow FWHM in the future. series of challenges that hinder its further practical applications,
In addition, carbonized polymer dots (CPDs), as an emerging such as the change in white light emission during the device op-
type of CD, have also received extensive attention due to their eration process due to the different stabilities of different com-
unique hybrid structures consisting of the typical incompletely ponents, the overlap of the absorption and PL emission spectra
carbonized carbon cores and the shell of polymer chains.[96,97] between different components, and severe energy losses during
These CPDs can not only shed insight into new polymer prop- electron–photon conversion.
erties of CDs but also offer a new route for investigating the Another way to generate white light is to use single-component
structure–property relationship of CDs. For example, highly effi- CDs that cover a wide range of the visible spectrum.[99,100] Mo-
cient deep-red CPDs have been synthesized by using taxus leaves tivated by the advantages of low power consumption, no phase
as the starting materials (Figure 3g). The deep-red CPDs showed separation, and high reliability, this method has also attracted
excitation-independent emission peaking at ≈673 nm with a nar- increased attention for WLED applications. For instance, solid-
row FWHM of ≈20 nm (Figure 3h,i).[55] Detailed structural char- state white emissive CDs have been realized, which exhibited
acterizations revealed that CPDs were composed of carbon cores an ultrabroadband emission spectrum peaking at 550 nm with
and the shells of polymer chains with unique polymer character- an extremely large FWHM of over 200 nm covering the en-
istics. The optical properties of CPDs were demonstrated to be tire visible spectral window from 400 to 750 nm.[101] The hy-
related to the 𝜋-conjugated system formed by N heterocycles and drogen bonding between CDs induced by amine and carbonyl
aromatic rings, which was responsible for the deep-red emission groups at the edge of CDs can overcome self-quenching and
with narrow FWHM. However, it should be noted that the exact increase the aggregation size of CDs, which further broadens
structural compositions and luminescence mechanisms of CPDs the emission spectra and shifts the aggregation-induced emis-
are still under development, and more in-depth investigations are sion band to the red spectral region. Interestingly, in addition
needed to better control the precise synthesis and optical proper- to fluorescence emission, the utilization of triplet-related emis-
ties of CDs. sion is also a new approach to realize white light emission by
broadening the emission spectra of CDs. Due to the abundant
nonconjugated functional groups and incompletely carbonized
2.3.2. Broad FWHM for Lighting carbon cores, CPDs possess molecular state-related emission
centers, which contribute to the generation of multiple hybrid or-
In lighting technologies, white LEDs (WLEDs) typically exhibit a bitals and energy level structures for electron transitions. There-
sun-like broadband spectrum with a continuous emission wave- fore, CPDs generally possess a small energy gap that is benefi-
length ranging from 380 to 780 nm. Currently, most of the cial for accelerating ISC processes, which is expected to achieve
reported CDs show broadband emission spectra with a large triplet emission. Moreover, the supramolecular crosslinked net-
FWHM of more than 80 nm. Therefore, CDs are promising for work structure in the aggregated state is vital for the RTP and
the fabrication of WLEDs. To date, there are two general strate- DF of CDs by restricting the nonradiative transition of the triplet
gies to realize CD-based WLEDs. The first strategy is the combi- excitons. For example, single-component CDs with fluorescence-
nation of multiple components with different emission colors to phosphorescence dual emission have been successfully reported,
realize white light emission.[56] White light emission is expected which enables single-component white light emission by the
to be achieved by dispersing CDs with yellow or orange emis- elaborate combination of blue fluorescence emission and yel-
sion into host materials such as poly(N-vinyl carbazole) (PVK) low phosphorescence emission.[102] Meanwhile, by strategically
Figure 4. a) Schematic illustration of carbon quantum rings and b) their normalized emission spectra. Reproduced with permission.[57] Copyright 2021,
Wiley-VCH. c) Schematic diagram and growth mechanism of CPDs and d) phosphorescence spectra of the CPDs measured at 298 and 77 K upon
excitation at 375 nm. Reproduced with permission.[103] Copyright 2020, Wiley-VCH.
designing covalently crosslinked polymer frameworks with heavy maximum value of 5% based on the fluorescence emission, but it
doping of N and P, white light emission based on CPDs was can exceed 20% by the utilization of triplet excitons, thus greatly
also observed (Figure 4c). The realization of hybrid fluorescence– breaking the statistical limit of device performance based on flu-
phosphorescence emission indicates that the rational structural orescent CDs.
design of CPDs is of great significance for the modulation of op- Recently, continuous efforts have been made toward formulat-
tical properties, indicating a new direction for the further devel- ing rational rules for designing bright RTP and DF. Generally, the
opment of CD-based WLEDs (Figure 4d).[103] typical RTP of organic emitters can be systematically designed
through different strategies, such as heavy-atom doping,[106–109]
functional group modification,[71,102,110] organic aggregates,[111]
2.4. Triplet State-Related RTP and DF and matrix-assisted stabilization of triplet excited states.[112,113]
These approaches can not only effectively stabilize the triplet en-
Different from the fluorescence emission originating from the ergy level to suppress unfavorable nonradiative relaxation but
exciton transition with the same spin multiplicity between the also strengthen the spin–orbital coupling to induce strong in-
singlet state (S1 ) and ground state (S0 ), RTP and DF are closely tersystem crossing (ISC) transitions from S1 to T1 . For instance,
related to the triplet state (T1 ). The strong exciton binding en- compared with amino groups, anchoring carbonyl groups at the
ergy and complex excited state structure of organic optoelec- edge of the large conjugated structure can promote ISC and in-
tronic materials determine the radiative transition process.[104] duce intermolecular electronic coupling (Figure 5a). Therefore, a
Typically, due to the differences in spin multiplicity, under elec- yellow phosphorescence emission with an overall PLQY of 25%
trical excitation, 75% of the triplet excitons are depleted as heat was successfully achieved (Figure 5b).[102] Furthermore, the ra-
rather than light, and only 25% of the singlet excitons are used tional design of the CD organic framework structure (CDOF) is
for fluorescence emission. Theoretically, the maximum EQE demonstrated as an efficient strategy to stabilize triplet emission
(EQEmax) of CD-based electroluminescent LEDs can be estimated (Figure 5c), thus leading to a red phosphorescence emission with
as follows[105] an overall high PLQY of 42.3% (Figure 5d).[71] Theoretical calcula-
tions and experiments demonstrated that the side chains around
( )
EQEmax = 𝜂out × IQE = 𝜂out × 𝛾 × 𝜂S∕T × 𝜙PLQY (1) CDs can significantly stabilize the triplet energy level of CDs, re-
duce the energy gap between S0 and T1 and increase the spin–
where 𝜂 out is the light out-coupling efficiency (typically ≈ 0.2), 𝛾 is orbital coupling between S1 and T1 .
the balanced charge of injected holes and electrons (theoretically Different from RTP, a small energy gap between T1 and S1
= 1), 𝜂 S/T is the singlet exciton (25%) and triplet exciton (≈75%), (theoretically, ∆EST < 0.30 eV), which can facilitate reverse ISC
and ΦPLQY is the PLQY of conventional fluorescent materials (the (RISC) from T1 to S1, is the first prerequisite for designing
maximum value is 100%). Therefore, the EQEmax can only reach a efficient TADF emitters. When the energy levels between T1
Figure 5. a) Energy-level diagrams of the relevant photophysical process and b) prompt (red line) and delayed (blue line) PL spectra excited at 380 nm.
Reproduced with permission.[102] Copyright 2019, Royal Society of Chemistry. c) Schematic illustration of CDOFs and d) UV−vis absorption spectra
and PL spectra of DMF solution, powder, and film of CDOFs under ambient conditions. Reproduced with permission.[71] Copyright 2021, American
Chemical Society. e) Proposed in situ formation process of the photoluminescent CDs@AlPO-5 composite. f) The steady-state PL spectrum (deep blue
line) and delayed PL spectrum (olive line) of CDs@AlPO-5 excited at 370 nm and 77 K. g) Temperature-dependent transient PL decay. Reproduced
with permission.[59] Copyright 2017, American Association for the Advancement of Science. h) Proposed Jablonski diagram for the triplet population
via two-channel ISC from the localized sp2 carbon subdomain and carbonyl groups at edge sites (C and O). i) Afterglow decay curves and j) average
afterglow lifetime of CDs. Reproduced with permission.[81] Copyright 2020, Wiley-VCH.
and S1 are close, that is, the ∆EST is small, the endothermic channel ISC between RTP and TADF provides a new approach to
RISC process can be overcome by the thermal motions of the engineer singlet–triplet splitting in CDs.
molecule atoms. As a result, triplet excitons that generally ex- Self-assembly provides a powerful approach for sophisticated
perience nonradiative losses due to the spin-forbidden transi- regulation of molecular interactions to bring highly ordered
tion can be converted to singlet excitons via RISC, leading to stacking between monomers via noncovalent intermolecular in-
TADF emission. For instance, by confining CDs in zeolitic matri- teractions, such as hydrogen bonding, 𝜋–𝜋 stacking, and elec-
ces (CDs@AlPO-5) (Figure 5e), highly efficient TADF emission trostatic interactions. It is easy to obtain aggregates with various
was achieved (Figure 5f).[59] The nanoconfined space of zeolites morphologies from the nanoscale to micron level and even from
can efficiently suppress the nonradiative relaxation of CDs de- 0D to 3D, which can effectively regulate the triplet state to pro-
rived from intramolecular vibrations and rotations, thus stabi- mote RTP and DF emission. Moreover, coassembly by the com-
lizing the triplet state to promote the RISC process. However, bination of CDs with various matrices is another way to regulate
CDs@AlPO-5 showed ultralong lifetimes up to 350 ms at am- the RTP and DF emission of CDs. Several strategies have been
bient temperature and atmosphere, which inevitably led to the developed to enhance triplet emission, such as the introduction
accumulation of uncompensated charges and associated carrier of halogen atoms and carbonyl groups, host–guest doping meth-
losses under electric excitation (Figure 5g). Significantly, control- ods, crystal engineering, and H-aggregation. These macroscopic
lable singlet–triplet energy splitting of CDs from RTP to TADF compounds with stable configurations can create a minimized
has been successfully achieved by varying the degree of oxidation microenvironment for molecular vibrational dissipation to pro-
of CDs, which is consistent with the ratio of oxygenated carbon mote the ISC process, suppress the nonradiative relaxation decay
and carbonyl groups at edge sites (Figure 5h).[81] The transient of the excited triplet state and protect the CDs against quench-
afterglow decay curves and the average lifetimes of CDs further ing by water and oxygen. Moreover, there are many other struc-
revealed the unique afterglow characteristics of RTP and TADF, tural characteristics that can endow CDs with various interest-
in which the coexistence of decay components for both promot- ing and unique properties, such as high solubility in organic sol-
ing fluorescence and afterglow demonstrated the overlap of RTP vents, good optical–thermal stability, easy functionalization, con-
and TADF (Figure 5i,j). The controllable transition from the two- trollable electron and hole injections and high charge transport
Figure 6. Illustrations of the typical structure of CDs functionalized with different groups or organic materials (left) and electroluminescent LEDs (right).
properties.[114–117] These features set a solid foundation for the best performance of CD-based electroluminescent LEDs at that
applications of CDs in electroluminescent LEDs. time in which CDs were directly used as the active emission layer.
Nevertheless, the devices showed a large FWHM of more than
80 nm in the emission spectra with inferior color purity, thus
3. Electroluminescent LEDs Based on CDs significantly hindering their ultrahigh-definition display applica-
Benefiting from their unique optical properties, CDs as active tions.
emission materials in electroluminescent LEDs have been ex- To improve the color purity, CDs with narrow FWHM
tensively investigated, and remarkable progress has already been were synthesized and successfully used in electroluminescent
made.[118–123] The optical properties of CDs and the device con- LEDs.[124] For instance, via surface passivation with aniline
figuration are crucial for device performance (Figure 6). Here, derivatives, multicolor CDs with narrow-bandwidth emission
we mainly focus on the discussion of the singlet state-related flu- were synthesized.[125] The aniline derivatives showed no visible
orescence emission and triplet state-related RTP and DF of CDs PL themselves, but they could induce the formation of uniform,
for electroluminescent LEDs. proper energy gaps by conjugating with CDs, leading to high
color tunability and color purity. Green, orange, and red electro-
luminescent LEDs based on the functionalized CDs displayed
3.1. Electroluminescent LEDs Based on Fluorescence Emission high color purity with a narrow FWHM of 20–50 nm, an Lmax
of 390 cd m−2 , an EQEmax of 1.28% and a maximum current ef-
3.1.1. Display Applications ficiency of 3.47 cd A−1 (Figure 7a). To further improve the de-
vice performance, by engineering the rigid triangular structure
The optical properties of conventional CDs are usually domi- of the carbon core, efficient CDs with a narrow bandwidth of
nated by surface defects or molecular states, which gives rise 30 nm and a high PLQY of 54–72% were synthesized for elec-
to fundamental limitations to the effectiveness of carrier injec- troluminescent LEDs.[69] By blending CDs with the host material
tion for electroluminescent LED applications. Therefore, it is im- PVK to avoid aggregation-induced quenching, unprecedented
portant to employ highly crystalline CDs with bandgap emis- high color purity narrow-bandwidth EL emission was realized.
sion instead of surface defect-related emission for electrolumi- The multicolor LEDs based on the NBE-T-CQDs displayed nar-
nescent LED applications. Notably, monochrome electrolumines- row FWHMs of 30–39 nm and high device performance with
cent LEDs based on the stable fluorescence emission of CDs from Lmax of 1882–4762 cd m−2 and current efficiency of 1.22–5.11 cd
blue to red were successfully fabricated. It should be emphasized A−1 . These results overturn the traditional view that CD-based
that CDs were directly used as active emission layers without a LEDs can only exhibit broadband emission and poor color purity
hole transport layer in the conventional simple device structure, with FWHM commonly exceeding 80 nm, indicating the great
which indicates that the injected electrons and holes undergo ra- potential of high color purity CDs as an alternative candidate
diative recombination in the CD active emission layer.[46] The to conventional well-developed QDs and perovskites for display
Lmax reached 136 cd m−2 for blue LEDs, which represented the applications (Figure 7b). The elaborate structural design of CDs
Figure 7. a) EL spectra and photographs of the corresponding CD-based LEDs. Reproduced with permission.[125] Copyright 2016, Springer Nature. b)
EL spectra of the B-, G-, Y-, and R-LEDs at different bias voltages (insets are the operation photographs of the B-, G-, Y-, and R-LEDs with the logo of
BNU). Reproduced with permission.[69] Copyright 2018, Springer Nature. c) Device structure, d) energy level diagram, e) EL spectra, and f) EQE–current
density of HCP-DB-CD-based LEDs. Reproduced with permission.[70] Copyright 2019, Springer Nature.
opens a new door for the synthesis of highly efficient CDs with and electroluminescent WLEDs. In phosphor-converted WLEDs,
narrow FWHM and their development in next-generation high- there are two general strategies to realize WLEDs.[126–129] The first
performance CD-based display technology. strategy to generate white light emission is the combination of a
Device structure optimization with balanced injection and ra- blue GaN LED chip and synthesized CDs with yellow or orange
diative recombination of electrons and holes is crucial to the per- emission that partially absorb blue EL from the LED chip. Al-
formance improvement of LEDs. Through the optimization of though the operational process is simple, WLEDs always show a
the hole transport layer of devices (Figure 7c,d), deep-blue LEDs low CRI due to incomplete spectral coverage in the whole visible
peaking at 440 nm based on highly efficient CDs were realized region, especially in the cyan and red emission regions. More-
(Figure 7e). The deep-blue LEDs displayed high device perfor- over, the blue light retinal injury arising from a strong blue spike
mance with an Lmax of 5240 cd m−2 , one order of magnitude of 450–500 nm in the white-light spectrum prevents this technol-
higher than that of previously reported blue CD-based LEDs. ogy from widespread studies and applications. Ideally, the sec-
More importantly, the EQE of the deep-blue LEDs reached 4%, ond strategy is a suitable combination of red/green/blue tricolor
which is the record value achieved to date for fluorescent CD- phosphors with broadband emission spectra excited by the UV
based LEDs, also exceeding that of Cd2+ /Pb2+ -based deep-blue LED chips, thus yielding a combined white emission covering the
LEDs (Figure 7f).[70] These results indicate that both the elabo- whole visible region. This strategy can significantly improve CRI
rate designed device structures and excellent optical properties and chromatic stability and reduce the light toxicity of the blue
of CDs are crucial to the improved LED performance. LED chip to the eyes. For instance, by combining highly efficient
three primary blue, green, and red emissive CD phosphors, UV-
pumped warm WLEDs were achieved for the first time.[98] The
3.1.2. Lighting Applications warm WLEDs showed good color chromatics and device stability
and a high CRI of 97, which is higher than that of conventional
Currently, the fabrication of CD-based WLEDs can be classi- semiconductor QD-based WLEDs. Considering their low toxic-
fied into two categories, including phosphor-converted WLEDs ity, good photothermal stability, high PLQYs and low costs, the
Figure 8. a) EL spectra using CD-blended PVK as emissive layers and luminance–current–voltage characteristics of WLEDs. Reproduced with
permission.[131] Copyright 2015, Springer Nature. b) Luminance–current–voltage characteristic, current efficiency versus current density, EL spectra
and color coordinates of the WLEDs. Reproduced with permission.[46] Copyright 2017, Wiley-VCH. c) The device configuration and energy level diagram.
d) EL spectra, corresponding color coordinates, current–voltage–luminance and current efficiency of WLEDs. Reproduced with permission.[68] Copyright
2019, Wiley-VCH.
fabrication of phosphor-converted WLEDs has been widely sion color coordinates of (0.30, 0.33). The Lmax reached as high
demonstrated for solid-state lighting; however, they still suffer as approximately 2050 cd m−2 with a corresponding current ef-
from a series of issues, such as severe phase separation, serious ficiency of 1.1 cd A−1 , which is even comparable to that of semi-
secondary energy losses during electron–photon conversion, and conductor QD-based WLEDs (Figure 8b).[46]
a complex device structure. Currently, due to the short-wavelength emission of most re-
Different from the phosphor-converted WLEDs in which the ported CDs, the corresponding CD-based electroluminescent
phosphors are excited by short-wavelength light from LED chips, WLEDs usually exhibit CCTs of over 5000 K, which is not suit-
electroluminescent WLEDs rely on direct charge carrier injec- able for indoor lighting and other occasions that require warm
tion into the light-emitting layer without energy losses, indicat- white light. Therefore, to control the Commission Internationale
ing the full use of the CDs to achieve white light emission with de L’Eclairage (CIE) and CCT, warm WLEDs were fabricated
improved efficiency.[130] To date, remarkable progress has been by blending PVK with different red R-EGP-CQDs centered at
made in CD-based electroluminescent WLEDs for lighting. For 637, 642, and 645 nm (Figure 8c). The warm WLEDs exhib-
example, WLEDs based on CDs with green emission peaking at ited corresponding CIE color coordinates and CCTs of (0.379,
500 nm dispersed into the host material PVK were demonstrated 0.314)/3365 K, (0.383, 0.311)/3168 K, and (0.388, 0.309)/2987 K,
(Figure 8a).[131] By using a simple device structure to eliminate respectively, as well as high device performance with Lmax as high
the influence of light emission from other functional layers, the as ≈5248–5909 cd m−2 and current efficiency of 3.65–3.85 cd A−1
origin of EL was revealed. Experimental results and computer (Figure 8d).[68] Although electroluminescent WLEDs can be eas-
simulations demonstrated that the hybridized CD-PVK complex ily prepared by adjusting the emission wavelength of CDs, the
state was formed to achieve controllable white emission. The complicated synthesis methods, poor charge transport properties
light-emitting mechanism and energy transfer between CDs and and thermal stability of CDs restrict their further applications.
the host material PVK has also been revealed. However, the de- Therefore, it is urgent to develop simple and facile methods to
vice performance of the WLEDs is relatively poor (Lmax is 1 cd prepare efficient CDs with long-wavelength emission or single-
m−2 at 11 V) compared with that of reported semiconductor QD- component white light emission with a broad spectral range for
based WLEDs. To further improve the performance of WLEDs, the development of electroluminescent WLEDs.
bright multicolor bandgap fluorescent CDs blended with PVK However, unlike conventional QDs and perovskite material-
have been used as the active emission layers to fabricate high- based LEDs, which show theoretical EQEs of more than 20% due
performance electroluminescent WLEDs with ideal white emis- to the negligible energy gap of ∆EST , the EQE of LEDs based on
Figure 9. a) Energy level diagram, b) EL spectra of the LEDs at different bias voltages (inset is the operation photograph of the LEDs with the logo of
BNU), c) color coordinates, and d) EQE−voltage characteristics of LEDs. Reproduced with permission.[71] Copyright 2021, American Chemical Society.
CDs with fluorescence emission can only reach 5% under elec- cations. In addition, CDs with RTP and DF emission also suffer
trical excitation. For instance, electroluminescent LEDs based on from unstable triplet excited states, low PLQYs, and the unbal-
blue fluorescent CDs with a PLQY of up to 70% ± 10% exhibited anced charge recombination of injected holes and electrons when
a high Lmax of 5240 cd m−2 but only showed a maximum EQE applied in LEDs. Therefore, the fabrication of high-performance
of 4%.[70] The inferior efficiency of the devices due to the energy LEDs based on the RTP and DF emission of CDs still faces
losses of triplet excitons in fluorescent CDs seriously hinders the tremendous challenges. Furthermore, the long lifetime of RTP
further development of high-performance next-generation LEDs. emission at the scale of the millisecond level leads to the accumu-
Electroluminescent LEDs based on CDs with RTP and DF proper- lation and losses of uncompensated charges, which inevitably re-
ties acting as active emission layers can achieve theoretical high sults in severe efficiency roll-off.[132,133] Therefore, the ideal CDs
EQEs of more than 20%, breaking the limitation of device per- with RTP and DF for electroluminescent devices should show
formance based on fluorescence emission. Therefore, future re- the characteristics of high PLQY, solution processability, excel-
search should focus on developing CDs with RTP and DF prop- lent charge transport properties and short carrier lifetimes. Re-
erties for electroluminescent LEDs with improved device perfor- cently, by using CDOFs with an overall PLQY of 42.3% and a
mance. short lifetime of 795.4 μs as the active emission layer (Figure
9a), electroluminescent LEDs combining blue fluorescence emis-
sion (≈25% singlet excitons) and red phosphorescence emission
3.2. Electroluminescent LEDs Based on Triplet State-Related (≈75% triplet excitons) were first realized (Figure 9b).[71] The CD-
Emission OFs displayed high and well-matched electron and hole mobili-
ties of 1.26 × 10−3 and 3.15 × 10−3 cm2 V−1 s−1 , respectively, and
Although remarkable progress has been achieved in electrolu- the hole mobility was 2 to 3 orders of magnitude higher than
minescent LEDs based on the fluorescence emission of CDs in those of previously reported CDs.[134] The distinct optical prop-
terms of brightness and FWHM, the limitation of 5% EQE greatly erties and excellent charge carrier transport properties of CDOFs
restricts the further development of CD-based LEDs. Therefore, lead to high device performance with an Lmax of 1818 cd m−2 and
significant efforts have been devoted to the development of elec- color coordinate of (0.64, 0.30) (Figure 9c). More significantly, a
troluminescent LEDs based on triplet state-related emission, record EQE of up to 5.6% of the devices directly indicates that
which can significantly boost the EQE of devices. However, the triplet excitons of CDs are successfully utilized for light emis-
RTP and DF emission of CDs are usually realized by embedding sion for the first time in electroluminescent LEDs, breaking the
CDs in a crystal or polymer matrix, which could result in the poor 5% EQE limitation of LEDs fabricated based on the fluorescence
solution processability of CDs/matrix composites for LED appli- emission of CDs (Figure 9d).
Considering the energy level splitting and exciton transitions

induced by vibrational coupling between the ground and excited
states, the reported triplet state-related emission of CDs usu-
ally exhibits a broadband emission spectrum (FWHM of 80–
100 nm).[135] This will result in significantly increased operat-
ing costs and poor color purity that are not conducive to satis-
fying the device performance requirements for practical display
applications. Therefore, it is very important to develop highly effi-
cient RTP and DF with narrow FWHM and high PLQY, especially
those capable of achieving high color purity defined by the CIE
harmonized broadcast standards and high perceived brightness
under the same power consumption.
4. Summary and Outlook

Due to their low toxicity, tuneable photoluminescence, good pho-
tostability and solution processability, CDs have been consid-
ered one of the most promising light-emitting candidates for
next-generation display and lighting technologies. In this review,
we mainly summarize the unique optical properties, structural Figure 10. Schematic illustration of the summary and outlook of this re-
view.
design of CDs, and recent advances of CD-based electrolumi-
nescent LEDs. However, compared with well-developed emit-
ters such as organic materials, heavy-metal-based QDs and per- great diversity of chemical reactions, such as amide reactions
ovskites as well as their exceptional device performance, there are and aldol reactions, which impart the development of multifunc-
still many challenges in CDs and their practical applications in tional CD-based materials with suitable optical/electronic prop-
electroluminescent LEDs that have yet to be addressed, in terms erties and different structures. However, the surface defects and
of the unclear structure and large-scale preparation of highly ef- edge defects, such as the position, number and structure of func-
ficient CDs, relatively poor RTP and TADF properties due to the tional groups and elements on CDs, still cannot be precisely de-
lack of a deep understanding of the structure–property relation- termined. Moreover, the uneven size distribution of CDs and a
ship of CDs, immature chiral CDs with circularly polarized light large number of reaction mixtures, such as unreacted precursors,
emission for 3D display applications, low device performance intermediates, and side products, further seriously limit the es-
compared with perovskite-, QD-, and organic-LEDs, and the lack tablishment of the structure–property relationship (Figure 10).
of in-depth theoretical research for the prediction of the structure Notably, free radical reactions that experience continuous pro-
and properties of CDs. Therefore, in this section, we discuss the duction of free radicals are an important methodology for explor-
current challenges and unresolved issues in CDs and their LED ing the synthesis of CDs with well-defined structures in the fu-
applications, as well as future prospective research directions in ture. This can not only provide specific reaction sites for target re-
this field (Figure 10). actions but also enhance the extraordinary impetus of precursors
to participate in chemical reactions, thus achieving large-scale
4.1. Large-Scale Synthesis of CDs with Precise and Well-Defined synthesis and precise structural control.[136,137] To date, many free
Structures radical additives, such as peroxides, azo compounds, and metal-
centered radicals, have been used to promote chemical reactions,
Generally, CDs are synthesized by one-pot methods, including and remarkable progress has been made.[138] As evidenced by the
top-down and bottom-up methods. Therefore, the precursors and most recent achievements in contemporary CD functionalization
synthetic conditions are of increasing importance for the ar- chemistry, the synthesis of CDs via radical reactions is a topic of
rangement of benzene rings, the doping of heterogeneous el- considerable ongoing research interest.[139–141] However, limited
ements, the modification of functional groups, and even the by the free radical species, reaction conditions and characteristic
shape, size and spatial arrangement of CDs. However, most stud- tools, the detailed reaction mechanism is still not clear, mainly
ies have only focused on a particular set of CDs prepared with including the reactivity of radicals of various chemical natures
similar precursors, leading to apparent optical mechanism con- with respect to CDs, the tendency of free radicals to add multi-
troversies and structural limitations. Moreover, there is still a lack ple times and rapidly to samples, and the structural pattern that
of deep understanding of how operating conditions can be trans- results in the growth process of CDs. Therefore, apart from the
lated into versatile methodologies toward tailorable properties. research advancements mentioned above, further investigations
Along this background, versatile and high-precision synthesis are needed in the future.
methods are urgently needed for a comprehensive analysis of the
optical/electronic properties of CDs with well-defined structures.
In addition, pre- and post-modification are also effective meth- 4.2. Improved RTP and DF Emission Properties
ods to engineer tuneable and tailored CDs. Considering the facile
preparation process and low-cost production, the surface passi- Continuous progress has been made in designing complex struc-
vation and functionalization of CDs can be realized through a tures of CDs to accomplish improved RTP and DF properties.[142]
The strategies for engineering CDs with unique structures to opening up new opportunities and possibilities for the fabrica-
achieve specific RTP and DF properties mainly include 1) the tion of high-performance CPL LEDs promising for 3D display
functionalization of CDs at the atomic level (i.e., elemental dop- applications.[150,151] Compared with conventional display technol-
ing, internal vacancy, edge growth) and molecular level (i.e., func- ogy, 3D displays show a stronger and more realistic sense of
tional groups and small molecules) and 2) embedding CDs in a depth, better pixel resolution and faster response speed. These
well-matched matrix to form heterojunction nanostructures or 3D displays have been highly praised by consumers because
molecular aggregates and assemblies based on spatial arrange- of the immersive visual effect of 3D entertainment. Since left-
ments. The rational design of the representative structure for and right-circularly polarized light emission from LEDs can be
each CD that was created preliminarily revealed the structure- switched by spin reversal, chiral materials play a significant role
RTP and DF property relationship. The successful utilization in binocular vision for stereoscopic imaging, thus displaying
of CDs based on RTP and DF in improving the device perfor- great potential in 3D displays.[152,153]
mance of electroluminescent LEDs has also been demonstrated To date, although different kinds of CPL materials, such
recently.[143–145] as chiral transition-metal complexes, polymers, small organic
However, research on CDs with RTP and DF is still at its early molecules and perovskites, have been developed, they still suf-
stage, and conclusive evidence and convincing explanations are fer from various issues, such as high cost, toxicity and low device
still absent for identifying the relationship between the lumines- performance.[149,154–155] Chiral CDs as emerging emitters have at-
cence mechanisms and structure of CDs. Although different ex- tracted extensive attention due to their advantages of high photo-
planations of the triplet-related emission of CDs have been re- stability, low toxicity and solution-processability.[156–158] Affected
ported, such as surface state, quantum confinement, and molecu- by their atomic geometry and spatial structure, atomically precise
lar state, it is difficult to clearly distinguish these influence factors chiral CDs can be broadly sorted into three categories based on
from each other. Therefore, it is still challenging to effectively reg- the different origins of chirality: 1) chiral carbon cores; 2) asym-
ulate the optical properties of RTP and DF, such as improved QY, metric arrangement of surface structures, including chiral func-
tuneable emission wavelength and carrier lifetime. In addition, tional groups and chiral small molecules; and 3) embedded in
the structural variability of CDs and inherent diversity of excited chiral crystals or polymer matrices. Theoretically, this sorting has
states also result in difficulty in accurately evaluating the whole established the basic research system and unfolded the full po-
picture of the optical properties of CDs.[146] Therefore, establish- tential of synthesis processes. However, the boundaries between
ing the structure–property relationship remains a complex and these categories are blurred, and a unifying picture describing
difficult task, mainly due to the lack of precise characterization chirality at the nanoscale is still lacking. The precise relationship
methods for the structure of CDs (Figure 10). between the structure and related chiral optical properties, sepa-
Recently, atomic-level high-resolution electron microscopy ration and purification, and structural characterization of chiral
methods, such as scanning tunnelling microscopy and atomic CDs are still in preliminary stages. To date, most of the reported
force microscopy, that can resolve single nanoparticles beyond CPL materials still cannot meet the real application requirements
the diffraction limit have been considered nanomanipulation because of the low PLQY and dissymmetry factor values in the
tools to precisely position nanometric or molecular objects on range of 10−5 to 10−2 . Further work is urgently needed to design
various surfaces.[147] Great progress has been made in visualizing and synthesize chiral CDs with improved and tuneable CPL prop-
the morphology and microstructure of CDs, as well as the critical erties for electroluminescent LEDs (Figure 10).
steps in the synthesis process, which offers outstanding possibili-
ties in the fabrication and investigation of complex nanostructure
architectures.[148] To date, research in the field of nanomanipula- 4.4. Film Processing and Device Structural Optimization
tion has provided various experimental procedures, all with the
purpose of ensuring both a high success rate and accuracy of ex- Compared with rough, discontinuous, and severely heteroge-
periments. Some techniques even include external stimuli such neous thin films, the precise processing of the morphology
as temperature, electric fields, or the use of automatic manip- (uniformity, coverage, roughness) and microstructure (aggre-
ulation sequences. However, there are still a series of problems, gate size/distribution, texture) of thin films can significantly af-
including high operating costs, complicated operating processes, fect the optoelectronic properties of films for high-performance
and harsh experimental conditions, that still need to be overcome devices.[159] Various thin-film processing technologies, such as
in this area, and future advances should be built on the inter- solution spin-coating, printing, and blade coating, have been uti-
disciplinary integration of materials, optical imaging and spec- lized for the preparation of the active emission layer for electro-
troscopy. luminescent LEDs. Different from powder processing and vac-
uum evaporation, in which vapor is transported to a substrate to
form thin films, due to its simple operation process and low cost,
4.3. Chiral CDs with Circularly Polarized Light Emission for 3D spin-coating is compatible with widely available nanosized CDs
Display that are easily carbonized at high temperatures.[160,161] However,
during film processing, the film morphology and microstruc-
As one of the most fundamental characteristics of nature, chi- ture are completely different under different conditions, espe-
rality plays an important role in different fields ranging from cially considering that CDs experience molecular rearrangement,
physics to astronomy, chemistry, and biology.[149] Introducing aggregation and assembly that are quite different from the dis-
chirality in semiconductors has recently been demonstrated as an persed monomolecular structure in solution states. The com-
effective strategy to achieve circularly polarized emission (CPL), monly used processing techniques are still immature for CD
materials whose optical properties are closely related to molec- erties but not yet well-defined structures.[167–169] With the aid of a
ular interactions and spatial arrangements (Figure 10). In addi- large amount of experimental data, a close relationship between
tion, CDs with good solubility in common organic solvents, such their structural design and the unique properties of emerging
as chloroform and chlorobenzene, are critical when forming an CDs is expected to be established, which is crucial for the ex-
active layer with good film processability, which determines their ploration of high PLQY, controlled FWHM, and triplet-related
applicability in electroluminescent LEDs. Considering that con- emission. Furthermore, building models to select the host ma-
jugated polymers generally exhibit improved solubility in com- terials and transport layers with well-matched energy levels and
mon organic solvents, modifying alkyl side chains or functional complementary luminescence of CDs is another difficult task to
groups around CDs by selecting precursors or post modifications realize efficient devices. Therefore, further application of ML to
is expected to improve the solubility of CDs. Due to the large investigations of CDs is to be considered as a new application
sp2 -conjugated domains, CDs often show strong light emission to support both in silico and experimental work and becoming
as isolated molecules but exhibit low QY at high concentrations more available to scientists with easy-to-use tools and accessible
and are even completely quenched in the solid state. Therefore, accumulative databases (Figure 10).
ACQ is largely responsible for the lack of fluorescence and triplet However, to date, computational studies of large and complex
emission in molecular solids, as changes in the excited-state elec- systems only rely on extremely simplified CD models, and there
tronic structures of the aggregates lead to an increased tendency are no consistent and reliable methods to solve these problems.
for nonradiative decay. Most of the existing ML methods are computer-oriented and still
Device structure optimization is also important for perfor- in the theoretical stage, which is far from traditional experiments
mance improvement in the future.[162,163] The optimization of in practical research. Therefore, long-term continuous accumu-
carrier transport layers is necessary for balancing the electron lation and correction with the assistance of a large number of
and hole injection and recombination as well as suppressing the experimental results are needed in the future.
energy loss between the interfacial transitions. Moreover, the im-
provement of device performance largely depends on the well-
matched energy levels between the active emission material and Acknowledgements
host material, as well as between the active emission layer and Y.S. and W.S. contributed equally to this work. This work was sup-
other transport layers for boosting charge carrier injection and ported by the National Natural Science Foundation of China (22172008,
transportation, which imposes severe constraints on device archi- 21872010), the National Key Research and Development Program of China
tecture and functionality. Therefore, more efforts should focus on (2019YFE0112200), and the Fundamental Research Funds for the Cen-
understanding the link between the chemical structure of CDs tral Universities (2020NTST11), China Postdoctoral Science Foundation
(2021M690803).
and the corresponding material/film/device properties and ex-
ploring new formulations for CD-based electroluminescent LED
applications. Conflict of Interest
The authors declare no conflict of interest.
4.5. Deep/Machine Learning-Assisted Synthesis of CDs with
Unique Structures and Properties
Keywords
Machine learning (ML) and artificial intelligence allow a machine carbon dots, display and lighting, light-emitting diodes, optical character-
to learn representative data by training without having the recog- istics, structural design
nition method explicitly programmed into it, thus realizing the
summary of laws, prediction of structural models, and optimiza- Received: November 17, 2022
Revised: February 21, 2023
tion of experimental processes.[164,165] Especially in recent years,
Published online: July 23, 2023
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Yuxin Shi received her Master’s degree in Physical Chemistry from Beijing Normal University (BNU)
in 2021. She is now a Ph.D. student with research interests focused on the controllable synthesis of
carbon nanomaterials with fluorescence, phosphorescence, thermally activated delayed fluorescence
for LED applications.
Wen Su received her Ph.D. degree in Physical Chemistry from BNU in 2020. She is currently a postdoc-
toral fellow at the National Center for Nanoscience and Technology (NCNST), Chinese Academy of
Sciences (CAS). Her research interest is focused on the design and synthesis of functional nanomate-
rials for luminescence, imaging, and nanomedicine.
Fanglong Yuan obtained his Ph.D. degree at BNU in 2018, and carried out his postdoctoral research
at Linköping University, and University of Toronto. Now he is a full professor at College of Chemistry,
BNU. His research interest is focused on the organic/inorganic functional materials chemistry, light-
emitting materials, optical, and photophysical properties, and optoelectronic devices.
Louzhen Fan is now a chemistry professor in the College of Chemistry, Beijing Normal University.
She received her Ph.D. in physical chemistry in 1998 under the supervision of Prof. Daoben Zhu and
Prof. Yongfang Li from Institute of Chemistry, Chinese Academy of Sciences, Beijing. Her research
interests are focused on the synthesis of novel carbon and metal nanomaterials and their applications
in biology and energy.

Advanced Materials - 2023 - Shi - Carbon Dots For Electroluminescent Light Emitting Diodes Recent Progress and Future

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Carbon Dots for Electroluminescent Light-Emitting Diodes:

have been extensively explored. To date,

intrinsic structure of the internal carbon core.[44–49] The structure

2.1. Tuneable PL Emission low to red, respectively.[46] Accordingly, theoretical calculations

Considering the energy level splitting and exciton transitions

4. Summary and Outlook

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