REVIEW
Power Conversion Efficiency
Optical Design in Perovskite Solar Cells
Kaimo Deng and Liang Li*
Organic–inorganic hybrid perovskite solar cells (PSCs) have undergone an
unprecedented development in the past few years and their power conversion
efficiency (PCE) has reached over 23%. The conversion from light to
electricity in the photovoltaic device has an intimate connection with the light
absorption and charge dynamics. To further improve the PCE, it is necessary
to optimize the device architecture and maximize the light absorption of the
active materials, so that more photoexcited carriers can be generated and
collected. The optical properties can also affect the device stability, especially
for the long-term exposure under UV light. Herein, recent progress of optical
designs in PSCs toward better device performance and wider applications are
summarized. The design strategies from the perspective of optical properties
may further boost the development of PSCs.
1. Introduction
Solar cells based on organic–inorganic hybrid perovskite have
become one of the most efficient photovoltaic devices, and
recent years have witnessed the rapid increase of power con-
version efficiency (PCE) from about 3% to over 23%, which can
rival the commercial silicon solar cells.[1–14] The high PCE of
perovskite solar cells (PSCs) is due to the excellent optoelec-
tronic properties of the organic–inorganic hybrid perovskite,
the crystal structure of which is shown in Figure  1a, such as
a large absorption coefficient, a long carrier diffusion length,
and a high tolerance toward the bulky defects.[15–17] The archi-
tectures of PSCs include a regular type (n-i-p) and an inverted
type (p-i-n), in which the perovskite materials serve as the
light absorber with an intrinsic semiconductor property and
the sandwiching semiconductors function as charge selec-
tive layers. According to the morphology of the n-type charge
selective layer, the regular type device can be categorized into
mesoporous or planar structured device with porous scaffold
or compact layer, as shown in Figure 1b,c, respectively.[18–20]
The inverted PSCs are generally constructed with a planar
structure in Figure 1d. Great efforts have been devoted to the
Dr. K. Deng, Prof. L. Li
School of Physical Science and Technology
Center for Energy Conversion Materials & Physics (CECMP)
Jiangsu Key Laboratory of Thin Films
Soochow University
Suzhou 215006, P. R. China
E-mail: lli@suda.edu.cn
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/smtd.201900150.
DOI: 10.1002/smtd.201900150
Small Methods 2019, 1900150 1900150  (1 of 19)
www.small-methods.com
fast development of PSCs from the per-
spective of architecture optimization, func-
tional material design,[21–28] and interface
engineering,[29–37] through which the
charge dynamics within the device can be
optimized with an efficient charge trans-
port and suppressed charge recombina-
tion. Moreover, the perovskite film can be
fabricated through solution processing,
and the high quality thin film can compete
with well-known photovoltaic materials
such as silicon and GaAs that is processed
by high temperature method or vacuum
technology, in many vital material prop-
erties for photovoltaic application.[10,38]
These outstanding optoelectronic proper-
ties make it an ideal choice for the next-
generation photovoltaic devices and the application prospect of
PSCs attracts extensive attention from worldwide researchers.
The involved optical property of the PSCs also has a huge
connection to the device performance since it affects the light
absorption and photocarrier generation, which largely deter-
mines the final photocurrent and output power.[5,39,40] The
composition and bandgap of perovskite can also be tuned
to realize a full coverage of light absorption in the visible
wavelength range. The perovskite with a direct energy band
ensures a superior light absorption ability, and the required
thickness of the light active materials can be reduced to con-
struct a thin film device.[41–44] A highly efficient light man-
agement is expected for PSCs. Wang et al.[45] calculated
the light distribution for the planar PSCs with a 350-nm
thick CH3NH3PbI3 (MAPbI3) perovskite film as the light
absorber. It is unexpected that only 65% of the incident light
can be absorbed by the perovskite film and the remaining
loss occurs mainly due to the light escape from the device
(15%) and the light reflection at the glass surface (4%). To
get a better PCE, it is necessary to optimize the device archi-
tecture and maximize the light harvesting of the PSCs.
The optical property also has a great impact on the
device stability due to the UV light with high-energy photons
in the incident solar spectra,[46,47] especially when TiO2 is used
within the PSCs. An intended optical design that enables
the device with a transparent or colorful property may help
expand the application of PSCs. Thus, the optical design for
PSCs should not be ignored, and the optimized optical proper-
ties will further boost the device performance. To the best of
our knowledge, there have been many impressive advances of
optical designs in PSCs as presented by the schematic drawing
in Figure 1e. In this review, we first summarize the advanced
light trapping technique that is applied on the glass surface,
conductive transparent substrate, electron transport layer
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.small-methods.com

(ETL), and hole transport layer (HTL). The light trapping is

mainly ascribed to the morphology-related light–matter inter- Kaimo Deng received his
action such as light scattering, diffraction, and photonic effect. B.S. degree in applied
Then, we focus on the perovskite materials with bandgap engi- physics and Ph.D. degree
neering and embedded periodic nanostructures, and the dis- in condensed matter physics
cussion about the assisted light absorption through plasmonic from the University of
effect, tandem device, and upconversion. We also pay extra Science and Technology
attention to the effort that improves the UV stability of PSCs in of China. Since 2015, he
terms of the UV down-shifting layer and interface engineering. is an associate professor
In the end, exciting progress about new-concept devices such in the School of Physical
as transparent and colorful PSCs is briefly introduced. Science and Technology,
Soochow University, China.
His research interests lie
in the field of optoelectronic and solar energy harvesting
2. Light Trapping
materials, especially with a focus on nanostructure-based
2.1. Antireflection devices.

For typical PSCs, the incident light enters the device through
the glass side of transparent conductive substrates. At the Liang Li received his
flat air/glass interface, light reflection is inevitable due to a Ph.D. degree from the
different diffraction index of the glass and air. According to Institute of Solid State
the classical electromagnetic theory, the reflection ratio is Physics, Chinese Academy
determined by the diffraction index and the incident angle. of Sciences, in 2006.
To reduce the reflection, an interface modification layer is From 2007 to 2012, he
required. For crystalline silicon solar cells, light-trapping strat- worked in the National
egies include the pyramid structure and the antireflection thin University of Singapore
film. As for the PSCs, the refraction index of the antireflection (NUS), Singapore; National
layer should be well chosen since it has a close relationship Institute of Advanced
with the light reflection, and the surface morphology is also Industrial Science and
quite important due to the possible multi-reflection.[47,48] The Technology (AIST), Japan;
antireflection layer should also have a negligible absorption to National Institute of Materials Science (NIMS), Japan;
maximize the light transmittance. and the University of Western Ontario (UWO), Canada.
Fan et al.[49] reported a nanocone array antireflection layer that Since August 2012, he is a full professor in Soochow
is attached on the front side of the glass substrate to improve the University, China. His research group focuses mainly on
transmittance for PSCs, as shown in Figure 2a,b. The nanocone energy conversion materials for solar cells, photodetectors,
array is made of polydimethylsiloxane (PDMS), which is a com- and electrochemical batteries.
mercial transparent polymer with a refraction index lower than

Figure 1.  a) Crystal structure of perovskite. Architectures of PSCs: b) mesoporous regular type, c) planar regular type, and d) planar inverted type.
Reproduced with permission.[15] Copyright 2015, Wiley-VCH. e) A schematic drawing that shows the optical designs in PSCs.

Small Methods 2019, 1900150 1900150  (2 of 19) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.small-methods.com

Figure 2.  a) Schematic structure of PSCs with antireflection layer. b) SEM image of PDMS nanocone array. c) J–V curve, and d) EQE spectra of PSCs
with or without antireflection layer. Reproduced with permission.[49] Copyright 2015, American Chemical Society. SEM images of e) etched silicon
and f) PDMS antireflection layer. g) Optical properties of PDMS antireflection layer. Reproduced with permission.[50] Copyright 2015, The Royal Society
of Chemistry.

that of glass. The nanocone morphology is duplicated from the
anodized Al foil. They also investigated the influence of the aspect
ratios of the nancones on the antireflection property by using
different Al templates. With the optimized nanocones, the PCE of
the PSCs can be enhanced from 10.6% to 11.7%. The improvement
is mainly due to the increased short-circuit current density (Jsc)
(Figure 2c), which has resulted from the antireflection effect, as
can be confirmed from the external quantum efficiency spectra
shown in Figure 2d. In addition to the antireflection property, the
nanocone PDMS layer also possesses a self-cleaning property due
to the excellent hydrophobicity. Dudem et al.[50] used an inverted
micro-pyramidal structured PDMS antireflection layer to enhance
the device performance. The antireflection layer is fabricated
with micro-pyramidal structured silicon as the template, which is
obtained through etching the flat silicon substrate with chemical
solution (Figure 2e,f). Introducing the antireflection layer on the
glass leads to an enhanced average light transmittance of 94.9%,
compared to 90.1% for the bare glass (Figure 2g). Using MAPbI3
as the light absorber, the reference PSCs deliver a PCE of 17.17%
and it is boosted to 17.71% with the PDMS antireflection layer.
The main reason for the improved performance is the increased
Jsc, which is consistent with the enhanced light transmittance.
The device with the PDMS antireflection film has a slower reduc-
tion rate in PCE as the title angle increases under the light illu-
mination, while the PCE of the reference device without PDMS
layer steeply decreases as the tilted angle increases. This can be
explained by the enhanced light absorption in the active layer due
to the increased light scattering. Jost and coworkers[51] developed a
light management foil using UV-cured lacquer, and Zheng et al.[52]
fabricated a haze PDMS layer with a textured surface morphology
that is replicated from the epidermal texture of rose petals. Both
the antireflection layers can reduce the light reflection at the glass
side of the conductive substrate and increase the light transmit-
tance, thereby improving the Jsc of the PSCs.
Except for the organic polymers, inorganic materials can
also be applied as the antireflection layer. Huang et al.[53] mini-
mized the light loss at the air/glass interface by employing
a SiO2 nanosphere–based antireflection coating. The SiO2
nanospheres are spin-coated on the glass surface, and the
microstructure and thickness of the deposited layer can be
tuned by the spin-coating speed. A maximum light transmit-
tance of 96.1% at 550 nm can be achieved for the optimized
SiO2 antireflection coating, leading to an improved PCE from
14.81% to 15.82% for MAPbI3-based PSCs.
2.2. Transparent Conductive Substrate
The most widely used transparent conductive substances are
fluorine-doped tin oxide (FTO) and tin-doped In2O3 (ITO). The
compact and flat conductive layer is deposited on the glass
substrate with a thickness of several hundred nanometers.
Incident light can pass through the transparent conductive sub-
strate without much change in the direction of propagation.
To increase the light scattering and the optical light path, the
conductive substrate can be modified.

Small Methods 2019, 1900150 1900150  (3 of 19) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
Figure 3. SEM images of a) pristine and b) etched FTO. c) Absorption spectra of perovskite deposited on different substrate. Reproduced with
permission.[54] Copyright 2017, Wiley-VCH. d) Top view and e) cross-sectional SEM images of SnO2:Sb nanorod array. f) Transmittance spectra.
Reproduced with permission.[56] Copyright 2018, Wiley-VCH.
Yu et al.[54] reported the use of hierarchically porous FTO
substrate for PSCs. An electrochemical etching is employed
to modify the substrate surface to create the porous structure,
as shown in Figure  3a,b. Compared with the flat conductive
substrate, the porous structure has a pronounced light scat-
tering due to the coarse surface, as shown in Figure 3c. In
addition, the porous morphology provides an increased con-
tact area between the perovskite active material and the elec-
tron collecting layer, which facilitates the charge transport and
suppress the charge recombination. With the porous conduc-
tive substrate, a remarkable PCE of 19.22% with a low hyster-
esis index can be realized. In a recent report, Chan et al.[55]
used patterned FTO substrates with a 2D photonic structure
for PSCs. They employ ion etching with a monosphere layer
as the physical mask to pattern the FTO-conductive layer. The
patterned FTO substrate has an enhanced light scattering, and
the corresponding device has better light harvesting and PCE.
In addition to the widely used conductive substrates, alu-
minum-doped ZnO and antimony-doped tin oxide (ATO) are
also well-known inorganic transparent conductive materials.
Our group reported the growth of ATO nanorod array on FTO
substrate as a conductive mesoporous layer for PSCs.[56] The
nanorod array is vertical to the substrate surface with an average
thickness of 310 nm and diameter of 70 nm (Figure 3d,e).
The FTO substrate with well-aligned ATO nanorod array can
achieve a light transmittance up to 90% (Figure 3f), which is
higher than that of the bare FTO substrate. The increased light
transmittance can lead to the enhanced light absorption of the
active materials. The size of the nanorod array that is com-
parable to the visible light wavelength can increase the light
scattering, which can also contribute to the light harvesting.
Using the ATO nanorod array as the conductive layer, the PCE
of the PSCs can be boosted from 17.8% to 20.1% with MAPbI3
as the active layer.
Small Methods 2019, 1900150 1900150  (4 of 19)
www.small-methods.com
2.3. ETL
2.3.1. Ordered Structure
The ETL has a vital influence on the performance of the
device. One role of the ETL in the PSCs is to extract the elec-
trons from the active material and simultaneously block the
holes, while the other role is to transport the collected charges
into the electrode. A suitable ETL should have a high charge
mobility, an excellent chemical stability, and a suitable energy
alignment to match the light active layer. The most widely used
ETL are n-type metal oxide semiconductors such as TiO2,[20]
SnO2,[57] and ZnO,[58] and organic semiconductors including
PCBM and C60[59] are also frequently used for the p-i-n devices.
Thanks to the development of synthetic strategies, the mor-
phology of metal oxide semiconductor can be rationally tuned.
The record PSCs employ the compact/nanoparticle TiO2 com-
posite layer as the ETL, in which the compact layer effectively
blocks the holes, and the nanoparticle scaffold with a sufficient
contact area benefits an efficient charge extraction. However,
the small size of the nanoparticles that is down to dozens of
nanometers induces a poor light scattering ability, and the inci-
dent light almost passes through the ETL without changing the
direction. To increase the light scattering, the inorganic ETL
with a size that is comparable to the light wavelength can be
used, which may render the ETL to serve as the third role (light
scattering centers) in PSCs. Table 1 summarizes representative
PSCs using the inorganic n-type ETL with a size that is close to
the light wavelength.[60–79]
TiO2 is the most widely studied n-type metal oxide semi-
conductor for PSCs. Except for the nanoparticle TiO2 scaffold
for the mesoporous structured devices, TiO2 nanostructures
with a 1D or 3D morphology also attract extensive attention.
Park et al.[60] first reported the PSCs based on rutile TiO2
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.small-methods.com

Table 1.  Summary of PSCs based on ordered ETL nanostructures.

ETL Device architecture ETL thickness [nm] PCE [%] Reference

TiO2 nanorod FTO/compact-TiO2/nanorod TiO2/MAPbI3/Spiro-MeOTAD/Au 560 9.4 [60]
TiO2 nanorod FTO/compact-TiO2/nanorod TiO2/MAPbI3-xClx/Spiro-MeOTAD/Au 500–550 10.5 [61]
TiO2 nanorod FTO/compact-TiO2/nanorod TiO2/MAPbI3/Spiro-MeOTAD/Au 180 18.22 [62]
TiO2 nanorod FTO/nanorod TiO2/MAPbI3-xClx /Spiro-MeOTAD/Au 350–400 19.02 [63]
TiO2 nanorod FTO/nanorod TiO2/FAMAPbIBr /Spiro-MeOTAD/Au 180 19.11 [64]
TiO2 nanocone FTO/compact-TiO2/TiO2 nanocone/MAPbI3/Spiro-MeOTAD/Au 1100 11.7 [65]
TiO2 nanocone FTO/TiO2 nanocone/MAPbI3/Spiro-MeOTAD/Au 460 11.41 [66]
TiO2 nanotube Ti/TiO2 nanotube/MAPbI3/carbon nanotube 300 8.31 [67]
TiO2 nanotube FTO/TiO2 nanotube/MAPbI3 /Spiro-MeOTAD/Au 400–450 14.8 [68]
TiO2 nanotube FTO/compact-TiO2/TiO2 nanotube/MAPbI3/Spiro-MeOTAD/Ag 250 13.8 [69]
3D TiO2 FTO/3D TiO2/MAPbI3/spiro-MeOTAD/Ag 600 9.0 [70]
3D TiO2 FTO/3D TiO2/MAPbI3/spiro-MeOTAD/Ag 600 15.20 [71]
3D TiO2 FTO/3D TiO2/MAPbI3/spiro-MeOTAD/Au 460 13.17 [72]
3D TiO2 FTO/3D TiO2/MAPbI3-xClx/Spiro-OMeTAD/Au 540 10.5 [73]
ZnO nanorod FTO/compact-ZnO/ZnO nanorod/MAPbI3/Spiro-MeOTAD/Ag 1000 5.0 [74]
ZnO nanorod FTO/compact-ZnO/ZnO nanorod/MAPbI3/Spiro-MeOTAD/Au 1000 11.13 [75]
Mg-ZnO nanorod FTO/compact-ZnO/ZnO nanorod/MAPbI3/Spiro-MeOTAD/Au — 15.3 [76]
N-ZnO nanorod FTO/compact-ZnO/ZnO nanorod/MAPbI3/Spiro-MeOTAD/Ag 1070 16.12 [77]
ZnO nanorod FTO/compact-ZnO/ZnO nanorod/MAPbI3/Spiro-MeOTAD/Au 870 17.29 [78]
In-ZnO nanopillar FTO/compact-ZnO/ZnO nanopillar/MAPbI3/Spiro-MeOTAD/Ag 450 18.24 [79]

nanorods with a length of around 600 nm. The rutile nanorods
are grown on the FTO substrate through a hydrothermal reac-
tion, and the length can be controlled by the reaction time.
They find that the photovoltaic parameters of the device largely
depend on the length of the nanorods, which has a direct con-
nection with the light absorption, charge extraction, and trans-
port. The well crystallized nanorods with a highly ordered struc-
ture are believed to facilitate the charge transport by providing a
direct pathway for the collected electrons to reach the electrode.
Jose and coworkers[61] demonstrated the successful fabrica-
tion of a PSC module by using solution-grown TiO2 nanorods
as the ETL. The nanorod-based module shows an improved
stability compared with devices based on a compact TiO2 layer or
nanoparticle TiO2 scaffold, which is due to the superior phase
stability of the perovskite active layer when contacting with
TiO2 nanorod scaffold. To increase the contact area between the
perovskite and ETL, Nazeeruddin et al.[67] reported the anatase
TiO2 nanotube array–based PSCs and a PCE of 14.8% can be
reached. The nanotube array is prepared by electrochemical
anodizing of Ti-coated FTO substrate, and nanotubes with
a length ranging from 400 to 450 nm and a pore diameter of
55 to 85 nm can be finally obtained. Wong et al.[68] designed
novel flexible PSCs based on TiO2 nanotube. Conductive carbon
nanotube is deposited on top of the perovskite layer, which
serve as a dual function of a hole collector and transparent
electrode for the incident light. In order to further improve the
light harvesting and charge transport, Wang et al.[70] designed a
3D TiO2 nanowire architecture as the ETL for PSCs. They find
that the performance of the device has a large dependence on
the length of the TiO2 nanowire. As the length increases, the
Jsc increases while the open-circuit voltage (Voc) and fill factor
(FF) decreases. The optimized device based on the hierarchical
nanostructure achieves a higher PCE than the 1D nanostruc-
tured ETL, which is mainly ascribed to the unique morphology
that provides a pronounced light scattering and efficient charge
transport.
ZnO is another frequently used n-type semiconductor
as ETL for PSCs. The morphology can be easily modulated
through solution processing technique such as chemical bath
deposition. ZnO-based nanorod arrays have also been studied
as ETL for efficient PSCs. Compared with TiO2, ZnO has a
higher charge mobility and conductivity, which can efficiently
transport the collected electrons. ZnO nanorod arrays have a
pronounced light scattering, and the electronic property such
as the energy band and Fermi level affects the charge extrac-
tion and transport. Amassian et al.[77] reported the growth of
nitrogen-doped ZnO nanorod with an enhanced electron
mobility and reduced work function. The corresponding PSCs
exhibit a hysteresis-free and scan-independent property with an
impressive PCE of 16.1%. By doping the ZnO nanopillar with
iodion, Zheng et al.[79] successfully manipulates the work func-
tion and electron extraction ability, promoting the PCE of PSCs
up to 18.24%.
2.3.2. Photonic Effect
Nanostructure with a periodic size that is comparable to the
light wavelength is an alternative choice to increase the light
scattering and harvesting. The efficient PSCs typically have a

Small Methods 2019, 1900150 1900150  (5 of 19) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.small-methods.com

total thickness of <1 µm and the thickness of the mesoporous
TiO2 scaffold is in the range from 200 to 300 nm. The nano­
structure-embedded ETL should be well designed to enhance
the light scattering. Park et al.[80] reported moth-eye patterned
TiO2 mesoporous scaffold with a periodic 2D hexagonal sym-
metry to enhance the light harvesting of PSCs. They first
fabricated a moth-eye 500-nm-dorm patterned silicon master,
and a UV-curable polymer (PFPE) is used to replicate the
moth-eye structure with a negative copy of the silicon master.
Finally, PDMS solution is cast onto the PFPE mold to get the
PDMS template with the same morphology of silicon master.
To form the moth-eye patterned TiO2 mesoporous scaffold,
the spin-coated TiO2 wet layer is stamped with the flexible
PDMS template and the morphology of the TiO2 layer, as
shown in Figure  4a, is cast into the negative copy of the sil-
icon master. Compared with the flat mesoporous TiO2 layer,
the moth-eye patterned TiO2 has a reduced light reflection,
and the deposited perovskite has an enhanced light absorp-
tion in the longer wavelength due to the light scattering. The
improved light harvesting yields a higher Jsc and PCE for the
moth-eye TiO2–based PSCs than that of the flat TiO2. Moon
et al.[81] introduced a 2D photonic structure into the TiO2
mesoporous scaffold (Figure 4b). They use a polystyrene (PS)
sphere monolayer as the physical mask during the ion etching
to pattern the TiO2 scaffold. The 2D photonic TiO2 scaffold
can result in a higher light absorption ability and Jsc for PSCs.
In a recent report, we introduced a grating pattern into the
TiO2 scaffold (Figure 4c) as the ETL,[82] and the patterned ETL
with a strong light scattering ability and enhanced light trans-
mittance could successfully improve the light absorption in
the PSCs.
The inverse opal structure that consists of ordered arrays
of voids with a continuous refraction index alternation is
also widely studied for light–material interaction. Snaith
et al.[83] reported the use of a highly ordered SiO2 honey-
comb structure to guide the growth of perovskite with a
controlled domain size and thickness. They first spin-coat
the PS spheres onto the FTO/compact TiO2 substrate and
then infiltrate the voids with oxide precursor solution. Then
a high-temperature annealing removes the PS spheres, and
the porous honeycomb structure with a photonic property
can be formed (Figure 4d). The corresponding PSCs can pos-
sess enhanced Voc and FF compared to the reference device
without the honeycomb structure. Yang and coworkers[84]
demonstrated the inverse opal-like TiO2 structure as effi-
cient ETL for PSCs by spin-coating of Ti-precursor and PS
spheres mixed solution, in which the PS spheres function as
sacrificial templates. A heat treatment leads to the simulta-
neous formation of the bottom compact layer and the upper
inverse opal structure (Figure 4e). The inverse opal structure
improves the light transmittance both in the ultraviolet and
the visible light range compared with the P25 nanoparticle

Figure 4.  a) SEM image of the moth-eye patterned TiO2 nanoparticle scaffold. Reproduced with permission.[80] Copyright 2016, Wiley-VCH. b) SEM
image of 2D photonic structured TiO2 nanoparticle scaffold. Reproduced with permission.[81] Copyright 2018, Elsevier. c) SEM image of grating
patterned TiO2 scaffold. d) SEM images of porous SiO2 honeycomb structure (magnified inset SEM image, scale bar: 1 µm). Reproduced with
permission.[83] Copyright 2015, American Chemical Society. e) SEM image of TiO2 inverse opal structure. Reproduced with permission.[84] Copyright
2015, Wiley-VCH.

Small Methods 2019, 1900150 1900150  (6 of 19) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
ETL, which is the main cause for the enhanced PCE of the
corresponding device. Moon et al.[85] studied the effect of the
thickness of the inverse opal TiO2 structure on the perfor-
mance of the PSCs. By controlling the thickness in the range
of 200–800 nm, they found that a 600-nm thick ETL with suf-
ficient light harvesting can induce the best performance and
a very low hysteresis index can be achieved for the forward
and reverse scan.
The periodic nanostructure can also be integrated into the
organic ETL for better light harvesting. Tang et al.[86] reported
the use of moth-eye nanostructure patterned PCBM as the ETL
for the p-i-n type PSCs through a nanoimprint process with
prepatterned PDMS molds. Compared to the reference device
with a flat PCBM layer, the device with moth-eye patterned
PCBM layer exhibits a remarkable enhancement in the light
harvesting and thereby an increased Jsc.
2.4. HTL
The perovskite light absorber has a smaller absorption coef-
ficient in the longer wavelength range, and thereby a part
of the long-wavelength light can be transmitted through the
perovskite film without being absorbed. This is one of the
reasons for the low light response in the long-wavelength
range for most of the PSCs, especially for devices without
a light trapping design. In fact, the morphology-modulated
induced light management can also be realized in the HTL,
in addition to the charge selective property.[87] Xu and cow-
orkers[88] reported the Spiro-OMeTAD/P3HT mixed com-
posite as the HTL. The molecule/polymer composite HTL
with a periodic microstructure can be formed through self-
assembly during the deposition, which promotes the light
absorption and Jsc of the PSCs. In the inverted PSCs, Hong
et al.[89] employed nanoporous nickel oxide that is prepared
by a co-precipitation method as the HTL and a PCE of 19.1%
could be obtained.
Figure 5.  Energy band diagram for typical organic–inorganic hybrid perovskite. Reproduced with permission.[24] Copyright 2015, Wiley-VCH.
Small Methods 2019, 1900150
www.small-methods.com
3. Active Material Design
3.1. Bandgap Engineering
As building blocks in optoelectronic devices such as solar cells
and photodetectors, the light absorption ability of the perovskite
has a direct connection to the device performance. The perov-
skite family with a direct bandgap for the optoelectronic appli-
cation typically shows a large absorption coefficient. The light
absorption range is determined by the bandgap of the semicon-
ductor. Photons with energy that is larger than the bandgap can
be absorbed while a sub-bandgap photon cannot excite an elec-
tron from the valence band to the conductance band. To maxi-
mize the energy harvesting from the solar light, the bandgap of
the perovskite should be well chosen to balance the light absorp-
tion range and the output power of the final device. According
to the energy-band theory, the bandgap is related to the crystal
structure. The perovskite materials share the same crystal
structure with calcium titanium oxide, known as the perovskite
structure. The cubic crystal structure with a general formula of
ABX3 can accommodate many cations and anions. Elements
can remain stable in the perovskite structure if the tolerance
factor that is defined by the diameters of the embedded ions
is in the range of 0.75–1.0. The A-site on the corners of the lat-
tice can be an alkaline-earth metal ion, rare-earth ion or organic
group, while the B-site on the center of the lattice is usually
occupied by transition metal elements. The size and electron-
egativity of the embedded ions largely affect the bandgap.
Figure  5 depicts the energy band of representative perovskite
materials for optoelectronic application.[24] The first perovskite
material (MAPbI3) that is applied in PSCs has a bandgap of
1.55 eV and a corresponding absorption edge around 780 nm.[1]
Replacing I with Br leads to an increased bandgap of 2.3 eV for
MAPbBr3, while the MA organic group can be completely sub-
stituted by HC(=NH)NH2 (FA), an organic group with a larger
size, resulting in a lower bandgap of 1.5 eV for FAPbI3. The
A-site can also be occupied by mixed FA and MA with a tunable
1900150  (7 of 19) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.small-methods.com

ratio and bandgap. The record PSCs with a PCE over 23% is
based on the mixed cation perovskite.[13] Inorganic perovskite
materials with an increased stability[90,91] such as CsPbI3 and
CsPbBr3 have also been developed and applied in solar cells,
photodetectors, as well as light emitting diodes. The B-site Pb
ions can be totally or partly replaced by Sn to get a Pb-free solar
cells or reduced Pb content in the perovskite,[92,93] which is
attracting extra attention for environment-friendly devices.
3.2. Morphology Manipulation
The morphology of the perovskite materials can also affect the
light absorption. The perovskite layer in typical PSCs has a flat
surface and the light scattering effect at the interface is quite
limited. For a compact MAPbI3 active layer, an obvious reduc-
tion in absorption can be identified for the light wavelength
that exceeds 500 nm compared with the strong light absorption
at short-wavelength range. For other photovoltaic devices such
as dye-sensitized solar cells, the insufficient light absorption is
generally remedied by using internal light scattering centers
with a diameter that is comparable to the light wavelength. In
consideration of the limited thickness of PSCs, adding an extra
light scattering layer seems to be impractical.
An alternative solution is tuning the morphology of the
perovskite active layer itself to improve the optoelectronic
property. Cheng et al.[94] developed a gas-assisted fabrication
technique to grow a surface-textured perovskite film. During
the spin-coating of perovskite precursor solution, a stream
of nitrogen gas is used to quickly remove the solvent and the
annealed perovskite film has a dense bottom layer with a tex-
tured surface. The textured perovskite film has improved light
harvesting for the light wavelength over 500 nm than the planar
one, and the charge extraction efficiency can be enhanced at
the perovskite/HTL interface similar to the porous TiO2 scaf-
fold/perovskite interface. Compared with randomly distributed
scattering centers, periodic nanostructure are more desirable
for device performance considering the light management.
Chen et al.[95] reported a 2D inverse opal–structured perovskite
film as the active material for PSCs. They fabricated the 2D
inverse opal structure with a different void size through a PS-
sphere template method. A PS sphere monolayer on the sub-
strate is infiltrated with a perovskite precursor solution and
heat treatment followed to promote the perovskite crystalliza-
tion. The substrate is finally immersed in toluene to selectively
remove the PS spheres, leaving the perovskite film with a 2D
inverse opal structure, as shown in Figure 6a–c. A bandgap shift
and sparkling visible colors can be found for the inverse opal
structure compared to the nonstructured perovskite film. The
device based on the 2D inverse opal perovskite film achieves a
colorful feature and satisfactory PCE.
The ordered perovskite nanostructure can also be obtained
through an imprinting process. Song et al.[96] reported a
microscale whispering-gallery embedded perovskite film with
improved light trapping for PSCs. To introduce the desired sur-
face morphology, the silicon mold is placed on the perovskite

Figure 6.  SEM and AFM images of 2D inverse opal-structured perovskite based on PS spheres with different diameters: a) 500, b) 1000, c) 2000 nm.
Reproduced with permission.[95] Copyright 2016, American Chemical Society. d) AFM images and profile line of perovskite with whispering-gallery
morphology. Reproduced with permission.[96] Copyright 2018, Elsevier. e) AFM images and profile line of perovskite with grating pattern. Reproduced
with permission.[97] Copyright 2018, Wiley-VCH.

Small Methods 2019, 1900150 1900150  (8 of 19) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
film that is in an intermediate state, and vertical pressure is
applied during the heat treatment. The imprinted perovskite
film with a periodic morphology (Figure 6d) has better
crystallization and reduced defects compared with the non-
imprinted film. They also developed an optical disk imprinted
perovskite film for PSCs.[97] In contrast to silicon mold that is
prepared through an expensive and complex process, the com-
mercial optical disk with the morphology of closely packed
tracks is much cheaper. The resultant perovskite film achieves
a patterned surface with regularly spaced lines, (Figure 6e)
and the grating-like nanostructure has a grating effect that dif-
fracts the incident light into different directions. Both the whis-
pering-gallery and grating-embedded PSCs not only exhibit
improved light harvesting but also facilitate the charge extrac-
tion with increased contact area between the HTL and the
perovskite layer, thus delivering an enhanced PCE compared to
reference devices without a surface morphology modification.
The deficient light absorption in the long-wavelength range
can be in principle solved by using a thick perovskite film.
However, the perovskite film with an increased thickness will
be usually accompanied by more defects and a serious charge
recombination in the bulk, which may lead to a substantial loss
in Voc and FF. It is necessary to synthesize a thick perovskite
film with reduced defects. Zhou and coworkers[98] reported an
additive-induced chemical reduction of intrinsic defects in the
perovskite film. They find that the introduction of methylamine
into the precursor solution can avoid the precursor stoichiom-
etry deviation during the film growth, and high-quality perov-
skite films can be fabricated with significantly reduced intrinsic
defects. The planar PSCs based on a 650-nm thick perovskite
film can deliver a PCE of 20.02% with enhanced light har-
vesting in the long-wavelength range as confirmed by the EQE
spectra. Chen and coworkers[99] developed a hot casting method
at a low temperature of 70 °C to produce a thick perovskite film
over 800 nm. They use a mixed solvent precursor and a con-
secutive spin-coating process to control the growth of the perov-
skite film with large grains and a vertical crystal orientation.
The device performance is insensitive toward the thickness of
the perovskite film, and a stabilized PCE of 19% is achieved
with a p-i-n device structure.
4. Assisted Light Absorption
4.1. Plasmonic Effect
Noble metal nanostructures have been applied in PSCs with
an enhanced light absorption through the localized sur-
face plasmon resonance. The involved mechanisms for the
improved light absorption can be different.[100–103] The collec-
tive oscillation of electrons in response to the optical excitation
within the metal nanostructure can redistribute the electric
field near the surface area, and the increased local electric field
can enhance the light absorption cross section of the active
materials. Besides, the metal nanostructure with a large size
that is comparable to the light wavelength can exhibit strong
light scattering and increase the optical path length, which
is also beneficial to the light absorption. The last role of the
metal nanostructure is directly serving as a light sensitizer.
Small Methods 2019, 1900150 1900150  (9 of 19)
www.small-methods.com
The captured photon energy excites the electrons and the hot
electron can be injected into the electron acceptor.
Silver nanostructures can be easily synthesized with dif-
ferent shapes and sizes through a wet chemical procedure,
which attracts great interest from the academic community.
They are considered as ideal choices for large-scale production
with a low cost. However, the chemical and thermal instability
restrict the application in photovoltaic device that requires a
high temperature annealing such as dye sensitized solar cells.
Snaith et al.[104] reported the spherical core–shell Ag@TiO2-
incorporated PSCs with improved Jsc and PCE. To increase the
stability of the as-synthesized Ag nanoparticle, they coat the
silver core with a uniform TiO2 shell, as shown in Figure  7a.
The core–shell Ag@TiO2 exhibits almost the same character-
istic plasmonic resonance around 400 nm with the bare silver
nanoparticle as confirmed by the absorption spectra. The
coated 2-nm thick shell can not only increase the stability of
the silver core but also reduce the charge recombination and
the corrosion by the halide element in the perovskite layer. The
core–shell nanostructure that is annealed at 150 °C can main-
tain the plasmonic absorption peak, which is compatible with
the mesoporous Al2O3-based PSCs that are processed through
a low temperature procedure. The Ag@TiO2 nanoparticles are
introduced into the Al2O3 layer, and the device with the plas-
monic nanoparticles obtains an enhanced PCE compared with
the control device, and the main cause for the improved PCE
is the increase of Jsc, as shown in Figure 7b,c, which is ascribed
to the plasmonic effect and the photon recycling.
Gold nanostructure has also been widely applied in thin-film
solar cells. Spherical metal nanoparticle typically has a narrow
plasmonic excitation band at 380 nm for Ag and 530 nm for
Au,[100,104] which overlaps with the high absorption wavelength
range for the perovskite layer. Thus, the plasmonic effect of the
spherical metal nanoparticles on the enhanced light absorp-
tion for the perovskite active materials is quite limited. In
contrast, a metal nanorod exhibits two plasmonic bands from
the longitudinal and transverse resonance mode, and the reso-
nance band position can be tuned by changing the aspect ratio
of the nanorod. Lei and coworkers[105] developed a wet chem-
istry synthesis of core–shell Au@Ag nanocuboids for PSCs.
The nanocuboids possess a strong and wide-range resonance
band that covers the wavelength range from 300 to 800 nm.
The simulated electric field profile for the Au@Ag nanocuboids
with a different shell thickness is provided in Figure 7d,e dem-
onstrating a pronounced plasmonic effect at the surface area.
In addition to the plasmonic absorption enhancement, the
hybrid nanostructure can introduce an increased light scat-
tering within the device, leading to a 20.8% enhancement in
PCE compared with reference devices. Wang et al.[106] incor-
porated core–shell Au@SiO2 nanorods into the inverted PSCs
with Al2O3 as the scaffold and Br-containing perovskite as the
active materials. The device with the nanorods can yield a sig-
nificantly increased Jsc and PCE due to the plasmonic effect.
The gold nanoparticles can also improve the performance of
PSCs through the hot electron injection to the charge collective
layer. Sun et al.[107] studied the TiOx-Au nanoparticle composites
for PSCs, and the enhanced device performance is related to
the plasmon-induced hot carrier injection, which can result in a
higher built-in potential and Voc.
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.small-methods.com

Figure 7.  a) TEM images of core-shell Ag@TiO2 nanoparticles. b) J–V curves and c) IPCE spectra of PSCs with or without Ag@TiO2. Reproduced with
permission.[104] Copyright 2015, Wiley-VCH. Simulated electric field profile of Au@Ag nanocuboids: d) longitudinal, e) transverse resonance mode.
Reproduced with permission.[105] Copyright 2017, Elsevier.

4.2. Tandem Absorption Layer
One major factor that limits the PCE of single p-n junction solar
cells is the spectral mismatch. Photons with energy lower than
the bandgap of the light absorber cannot be absorbed, while a
photon with energy that is larger than the bandgap can only
generate one electron–hole pair and the extra energy will be lost
as heat. It is desirable to make better use of the solar light and
expand the light absorption range by combining two kinds of
light absorbers with a different bandgap, such as a combination
of the perovskite and light-absorbing polymer or fullerene.[108]
Tandem solar cells consist of two junctions with a different
bandgap, so that the top junction with a larger bandgap can
absorb the higher-energy photons, and photons with lower
energies will transmit and be absorbed by the bottom junc-
tion.[109,110] The two-junction design can enable the tandem
device to harvest a wider range of the solar spectra and mini-
mize the energy loss due to the spectral mismatch. Figure  8a
shows the schematic of two basic structures of the tandem
solar cells.[111] The two terminal device is fabricated by depos-
iting each layer in sequence onto a single substrate and the two
single-junction are connected together through a monolithic
integration. In four-terminal tandem solar cells, each device
has their own electrodes, and the device with a high bandgap is
mechanically stacked on top of the device with a low bandgap.
The bandgap of the perovskite materials can be rationally tuned
by changing the element composition, and the perovskite film
can be prepared via solution processing at a low temperature,
both of which make it a suitable candidate as building blocks
for tandem solar cells.
All-perovskite tandem solar cells have unique advantages
such as low costs and easy processing. To achieve a high PCE,
the bandgap of the rear and front solar cells should be carefully
chosen. Mixed cation hybrid halide perovskite with an appro-
priate bandgap is an ideal candidate for the front cell. However,
the Pb-based perovskite can hardly satisfy the requirement of
the rear cell, which typically needs a low bandgap less than
1.48 eV, as predicted by the calculation. As mentioned in a pre-
vious section, introducing Sn into the perovskite materials as the
B-site cation can reduce the bandgap. Snaith and coworkers[111]
reported the use of tin-containing perovskites with a bandgap
of 1.2 eV for the rear cell in combination with a 1.8 eV perov-
skite front cell to construct a tandem device. They develop a
precursor-phase anti-solvent immersion method to deposit a
uniform layer of mixed tin–lead perovskite. Figure 8b,c shows
the device structure and the J–V curves of the tandem solar
cells. The two-terminal tandem device can deliver a PCE of 17%
and 13.8% for a small and large active area (1 cm2), respectively,

Small Methods 2019, 1900150 1900150  (10 of 19) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
Figure 8. a) Schematic of tandem solar cells with two-terminal or four-terminal structure. b) Cross-sectional SEM images and c) J–V curves of
two-terminal tandem perovskite-perovskite solar cells. Reproduced with permission.[111] Copyright 2016, AAAS.
with a high Voc of 1.65 V. Yan et al.[112] reported a low bandgap
(1.25 eV) mixed tin–lead perovskite with large grains and a long
carrier lifetime, and a high PCE of 17.6% can be achieved for
the low-bandgap mixed Sn-Pb single-junction solar cells. Com-
bining a front cell with a 1.58 eV bandgap, the all-perovskite
four-terminal tandem device results in a champion PCE of
21.2%. By simultaneously optimizing the front and rear cells,
Yen et al.[113] successfully developed an efficient two-terminal
tandem PSCs (1.2 and 1.8 eV) with a reduced Voc loss. A PCE
of 18.5% can be realized for the tandem device with a high
Voc of 1.98 V and negligible J–V hysteresis. It is noted that the
Sn-containing perovskite typically shows a poor stability due to
the oxidation of Sn2+ into the more stable state of Sn4+, which
remains to be solved.
The tandem photovoltaic device that integrates commercial
solar cells with PSCs is considered as a promising approach
to further reduce the cost per kilowatt by improving the device
performance.[109] Silicon solar cells dominate the photovoltaic
market due to the mature industry and high PCE. The bandgap
of silicon is around 1.1 eV, which can be used as the rear solar
cell that absorbs low-energy photons. Mailoa et al.[114] for the
first time demonstrated a silicon–perovskite tandem device,
which is a landmark for the fast development of tandem solar
cells based on silicon and perovskite. They employ a tunnel
junction to establish a charge neutrality by electron and hole
tunneling. In spite of the low quality of perovskite and silicon
Small Methods 2019, 1900150 1900150  (11 of 19)
www.small-methods.com
solar cells, the PCE of the tandem device can still reach 13.7%
with a Voc of 1.65 V. To improve the performance of the front
PSCs, Snaith et al.[115] developed a 1.74 eV perovskite by var-
ying the halide composition and using mixed FA-Cs as the
A-site cations. The perovskite material is highly crystallized
and exhibits an excellent photostability. Single-junction solar
cells based on perovskite can obtain a Voc of 1.2 V and a PCE of
over 17% for the small area device, which is a promising can-
didate to combine with efficient silicon solar cells. Integrating
commercial crystalline silicon solar cells with highly efficient
PSCs is a feasible method to increase the PCE of tandem solar
cells. Wu et al.[116] designed a perovskite/silicon tandem solar
cell based on a mesoscopic perovskite solar cell and a crystal-
line silicon solar cell with a high temperature tolerance, which
leads to a steady state PCE of 22.5% with a Voc of 1.75 V. The
interfacial optimization is necessary to minimize the charge
recombination and construct an effective electrical connection
between the subcells with a high optical transparency. In a
recent report, McGehee et al.[117] fabricated two-terminal perov-
skite/silicon tandem solar cells with a PCE of 23.6% featuring
an infrared-tuned silicon heterojunction with Cs-FA mixed
cation perovskite. The device structure and performance are
presented in Figure  9. They innovatively introduce a zinc tin
oxide and SnO2 bilayer as a window layer, which can result in a
reduced parasitic absorption, enhanced stability toward thermal
and environmental conditions, efficient charge extraction,
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
Figure 9. a) Schematic of perovskite–silicon tandem solar cells. b) Optical image of the rear side of silicon solar cells before silver deposition.
c–e) Cross-sectional SEM images. f) J–V curves and g) EQE spectra of tandem solar cells. Reproduced with permission.[117] Copyright 2017,
Nature Publishing Group.
and protective properties to prevent the damage of vulnerable
active layers during the subsequent sputtering process for the
electrode deposition.
Perovskite-Cu(In,Ga)(S,Se)2 (CIGS) tandem device is another
type of tandem solar cell which receives extensive attention. The
record PCE of CIGS solar cells has reached 22.6%, and it is one
of the commercial photovoltaic devices that can compete with the
market-dominating silicon solar cells.[109] In contrast to silicon
with an indirect bandgap, CIGS is a direct bandgap semicon-
ductor with a typical bandgap that is similar to silicon, and the
high absorption coefficient renders a 2-µm thick CIGS to absorb
most of the incident light. CIGS–perovskite tandem solar cells
share the same structure with the silicon–perovskite counterpart,
which consists of a wide-bandgap perovskite solar cell upon a low-
bandgap CIGS solar cell, and the two subcells can be assembled
together by a two-terminal or four-terminal connection.[118,119]
To fabricate highly efficient tandem solar cells, the mechanically
stacked subcells in a four-terminal tandem device should employ
a transparent electrode for the front cell, while the two-terminal
tandem device requires a compatible processing for each depos-
ited layer and optimized interface with reduced defects and
excellent stability. Yang and coworkers[120] recently reported the
interface engineering of the CIGS surface and HTL between the
subcells, and a PCE of 22.43% can be obtained in a two-terminal
perovskite–CIGS tandem device, which is approaching the record
PCE of single-junction CIGS solar cells.
Small Methods 2019, 1900150 1900150  (12 of 19)
www.small-methods.com
4.3. Upconversion
For the single-junction PSCs, the light absorption range is
determined by the bandgap of the perovskite active layer. The
solar spectra cover a wide range of wavelength from UV to
infrared. However, typical PSCs can only absorb light in the
UV–visible range and the sub-bandgap photons will transmit
without being absorbed. Thus, a large part of the solar energy
in the infrared region cannot be used, which comprises about
40% of the total incident solar energy. Upconversion provides
a viable approach to decrease the energy loss by converting
near-infrared photons into high-energy photons, which can be
harvested and contribute an extra Jsc. The upconversion process
has also been employed in silicon solar cells and dye-sensitized
solar cells. Rare earth ion–doped inorganic matrix (NaYF4: Yb3+,
Er3+) is one of the most studied system to realize the upconver-
sion, where the Yb3+ ion serves as a light sensitizer and the Er3+
ion is the light emitting center. Fluorine-based lattice accounts
for the most efficient upconversion system, since it has a low
phonon energy and an excellent stability which can minimize
the non-radiative recombination and enhance the upconversion
efficiency. It can be easily tailored into a nanoscale size down to
several nanometers with a wet chemical procedure. Lin et al.[121]
reported the use of surface ligand–modified NaYF4:Yb3+, Er3+
nanoparticles as mesoporous scaffold for PSCs and demon-
strated the near-infrared light response within the device due
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
to the near-infrared to visible light upconversion. Song et al.[122]
introduced a fluoride-based upconversion layer on the back side
of the PSCs through pulsed laser deposition and observed an
increased Jsc due to the upconversion. However, the upconver-
sion efficiency is quite limited even for the best upconversion
system, and the upconversion luminescence generally can only
be realized under high-power excitation such as laser irradia-
tion. A conversion range with a wide wavelength coverage is
more preferred than a single-wavelength conversion to better
use the infrared light.
5. UV Light Stability
The long-term stability of PSCs under working conditions needs
to be addressed before its wide application. As for the active
material itself, the mixed cation hybrid halide perovskite that is
used in the high-efficiency device may undergo a phase separa-
tion under continuous light exposure, which can degrade the
device performance by introducing extra recombination centers
and reducing the Voc. The perovskite materials are vulnerable to
environmental conditions such as moisture and UV light. Mois-
ture can directly react with the perovskite materials and push
the dynamic equilibrium toward the decomposition direction,
which is the main cause for the fast performance degradation
of PSCs under ambient conditions. UV light with high-energy
photons has a negative influence on the structural and elec-
tric property of the organic functional layer, thus reducing the
lifetime. Especially for TiO2-based state-of-art device, UV light
exposure may lead to the formation of oxygen vacancies and
defects, and the UV-related photocatalytic property of TiO2 can
accelerate the decomposition of perovskite materials.[44,46] In a
practical application, the damage effect of UV light should be
reduced as much as possible.
5.1. Down-Shifting
The most common method to reduce the negative effect of UV
light is to use a cutoff filter that excludes the entering of UV
light into PSCs, which is frequently placed above the device
under prolonged illumination. However, the UV light accounts
for a considerable part of the solar spectra and removing UV
light from the incident light will affect the photocurrent gen-
eration. To remedy the loss of photocurrent, a down-shifting
layer that converts the UV light into visible light that can be
still absorbed by the active materials may replace the UV filter.
The light conversion layer should be transparent to the incident
light beyond the UV range. Rare earth–containing fluorescent
materials can emit light with fixed wavelengths under a broad
band light excitation and they also exhibit excellent stability.
Khan et al.[123] first introduced a rare earth down-shifting layer
into PSCs. They choose YVO4:Eu3+, a traditional red phosphor,
to convert the UV light. The UV light is mainly absorbed by
the vanadate, and the rare earth Eu3+ ions serve as the activator
for 612 nm light emission. The nanoparticle layer in front of
the PSCs renders the device with improved light harvesting
and stability under a long-term illumination test. The rare
earth coordination complex is another well-known luminescent
Small Methods 2019, 1900150 1900150  (13 of 19)
www.small-methods.com
compound, and one of its advantages over inorganic phosphors
is the good compatibility with polymer to form a compact and
transparent thin film, which is of great importance for the
down-shifting layer. Dai et al.[124] reported the Eu-containing
complex embedded PVP matrix film that converts the UV light
for PSCs. Song et al.[122] investigated a high quantum yield Eu
complex with a formula of Eu(TTA)2(Phen)MAA as the down-
shifting layer for PSCs. The functional group TTA is respon-
sible for the broadband light absorption in the UV range.
The captured energy is transferred from the TTA to the light
emitting centers (Eu3+), and the energy is released through
the electronic transition within f-f configuration in the form of
photons.
Fluorescent dye molecules with a high quantum efficiency
are also competitive alternatives for the spectral modifica-
tion. Hagfeldt and coworkers[125] reported a luminescent
down-shifting layer that integrates a commercial fluorescent
dye (Lumogen F Violet 570, BASF) with UV-curable mixed
polymer for PSCs as schematically presented in Figure  10a.
The organic dye can efficiently absorb light in the UV range
in which the PSCs have a poor light response and the emis-
sion spectra covers a broad range from 400 to 550 nm as
shown in Figure 10b, which matches well with the absorption
of the perovskite materials. The J–V curves and IPCE spectra in
Figure 10c,d indicate that the device with the conversion layer
has a higher Jsc and PCE, which is ascribed to the better light
harvesting in the UV range. The long-term stability test under
a continuous UV light exposure indicates that the device with a
UV–visible conversion layer has an improved UV stability in an
inert atmosphere compared with the control device.
5.2. Interface Engineering
Upon UV light illumination, the photo-excited holes in the
mesoporous TiO2 can react with oxygen that is absorbed at
oxygen vacancies and lead to the formation of deep traps,
which can enhance the charge recombination. To reduce the
UV light–induced performance degradation for TiO2-based
PSCs, it is necessary to passivate the photocatalytic property
of TiO2. Ito et al.[126] introduced a Sb2S3 surface blocking layer
between TiO2 and perovskite to investigate its effect on device
stability. The inserted Sb2S3 layer with a suitable energy band
position can not only improve the photovoltaic performance by
reducing the charge recombination in TiO2 but also promote
the stability of unencapsulated device against light exposure.
Yong et al.[127] coated a uniform CdS layer onto the TiO2 sur-
face through a simple solution processing for PSCs. CdS is a
widely used inorganic sensitizer for quantum dot solar cells,
and it can successfully passivate the surface state of TiO2 and
enhance the device stability toward light. In a recent report,
Snaith and coworkers[128] modified the TiO2 surface with CsBr,
which can lower the pin-hole density and the work function of
TiO2. They find that the UV-induced perovskite degradation can
be largely inhibited with the existence of CsBr at the interface
as shown in Figure 11a. The interfacial modifier can simultane-
ously reduce the photocatalytic effect of TiO2 and the defects at
the TiO2/perovskite interface, both of which favor the improved
PCE and UV stability as shown in Figure 11b,c.
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.small-methods.com

Figure 10.  a) Schematic of the luminescent down-shifting layer on top of PSCs. b) Fluorescent property of the dye molecules. Inset shows the optical
image of the solar cells with the down-shifting layer under light exposure. c) J–V curves and d) IPCE spectra of PSCs with or without the down-shifting
layer. Reproduced with permission.[125] Copyright 2016, AAAS.

Despite the passivation strategy that is applied at the TiO2 first used a Al2O3 nanoparticle layer as a mesoporous scaffold
surface, the UV stability of TiO2-based device needs further opti- for PSCs. The device structure is almost identical to conven-
mization, which inspires the research community to replace the tional device except for the mesoporous scaffold as shown in
TiO2 scaffold with an alternative counterpart. Snaith et al.[129] Figure 11d,e. Al2O3 is a wide bandgap insulator and it only

Figure 11.  a) Schematic structure, b) EQE, and c) stability of the PSCs with or without interface modification of CsBr. Reproduced with permission.[128]
Copyright 2016, The Royal Society of Chemistry. Mesoporous structured PSCs with d) TiO2 and e) Al2O3 scaffold. f) Aging test of PSCs based on
mesoporous Al2O3. Reproduced with permission.[129] Copyright 2013, Nature Publishing Group.

Small Methods 2019, 1900150 1900150  (14 of 19) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
serves as the scaffold for the perovskite deposition. The replace-
ment of the TiO2 scaffold with Al2O3 will not reduce the device
performance, and the long-term stability of the Al2O3-based
device is largely improved, which can maintain a stable photo-
current over 1000 h under continuous light exposure without
using a UV cutoff filter, as shown in Figure 11f.
6. New-Concept Photovoltaic Device
6.1. Transparent Device
The metal electrode such as Ag or Au with a typical thickness of
100 nm is commonly used in PSCs. The thick metal electrode
blocks the light transmittance, and it is the main restriction for
the fabrication of transparent PSCs. The iodide and bromide
perovskite with MA as the A-site cation can strongly absorb light
in the visible range. If a transparent conductive electrode can
replace the opaque metal electrode, semi-transparent devices
can be obtained.[130,131] To maintain the device performance, the
transparent electrode should exhibit high conductivity and good
compatibility to the perovskite film processing with solvent or
high temperature.
Cheng and coworkers[132] fabricated a MoO3-Au-MoO3-
stacked transparent electrode. The MoO3 is chosen for its excel-
lent hole injection property and a suitable nucleation surface
for the deposition of Au, which is proved to favor the formation
of transparent electrode by eliminating the surface plasmonic
effect. The stacked electrode contains a ultra-thin Au layer with
a thickness of 10 nm and it exhibits an enhanced transparency
compared to pure metal film. To totally remove the metal in the
electrode, Mathews and coworkers[133] first demonstrated the
metal electrode-free PSCs by using a carbon nanotube network
as the transparent electrode as shown in Figure  12a,b. Due to
the excellent conductivity, carbon nanotube has been applied in
Figure 12.  a) Optical image of carbon nanotube film. b) Schematic and c) J–V curves of semitransparent PSCs. Reproduced with permission.[133]
Copyright 2016, American Chemical Society. d) Absorption spectra of perovskite. e) Schematic drawing of the transparent PSCs. f) Optical images
showing the excellent transparency of the device. Reproduced with permission.[136] Copyright 2018, Cell Press.
Small Methods 2019, 1900150 1900150  (15 of 19)
www.small-methods.com
many types of solar cells and it can also function as the charge-
selective contact for PSCs with a proper energy band position.
The carbon nanotube–based device achieves a semitransparent
property, and the device can work efficiently under light illu-
mination from each electrode side as confirmed by the J–V
curve shown in Figure 12c. Graphene is another highly con-
ductive and transparent representative in the fullerene family.
Yan et al.[134] constructed semitransparent PSCs by using multi-
layer stacked graphene as the transparent electrode. The gra-
phene electrode is fabricated by chemical vapor deposition and
then transferred on plastic substrate. Finally, it is laminated on
the perovskite under a low temperature and pressure. Zheng
et al.[135] reported the fabrication of semitransparent PSCs
through a low temperature and solution processed method.
They employed the transparent conducting polymer poly(3,4-et
hylenedioxythiophene):polystyrene sulfonate (PEDOT: PSS)
as both the cathode and anode for the device, and an impres-
sive PCE of 13.9% could be achieved. Flexible semitransparent
devices based on plastic substrates such as polyethylene tereph-
thalate and polyimide were also demonstrated.
To construct a transparent device, the perovskite mate-
rials with a strong visible absorption should be replaced. Lunt
et al.[136] recently reported transparent PSCs based on MAPbCl3,
which selectively absorbs light in the UV range of 400–440 nm,
as shown in Figure 12d. Due to the fast crystallization rate of
the inorganic perovskite and the low solubility of precursor in
common solvents, it is difficult to obtain high-quality perovskite
film. They develop a vacuum-assisted solution deposition com-
bined with a methylamine gas treatment to prepare a compact
and transparent perovskite film. The transparent device has an
inverted structure (Figure 12e) with a bottom electrode of ITO
and a top transparent electrode that consists of Ag and Alq3,
in which Alq3 is deposited to enhance the transparency. The
light harvesting ability of the transparent device can be evalu-
ated from the optical properties and quantum efficiency, which
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.small-methods.com

offers a theoretical PCE of 7% and visible transparency over
99%. The highly transparent property of the PSCs, as shown in
Figure 12f, holds great promise in smart windows and multi-
junction tandem solar cells.
6.2. Colorful Device
The colorful PSCs have a good application prospect in photovol-
taic integrated buildings and aesthetic appealing designs.[137–140]
To create the desired color, bandgap engineering of the perov-
skite film and the nanostructure related optical property are
generally used. For example, a different molar ratio of I and
Br can change the color of perovskite with MA as the A-site
cation from yellow to red. However, a large bandgap can lead to
a decreased PCE due to the reduced light absorption range. A
strict rule to develop colorful PSCs is not at the expense of PCE
and thus the morphology-induced color is a better choice.
Snaith et al.[141] reported the realization of colorful PSCs
through a tunable structural color of the photonic structure
within the device. Instead of pure TiO2 mesoporous scaffold,
they alternatively deposited mesoporous TiO2 nanoparticle layer
and SiO2 nanoparticle layer on the FTO substrate to obtain a
composite multilayer with a periodic high and low refractive
index. Figure 13a,b shows the scheme and cross-sectional SEM
image of PSCs with an embedded photonic structure. To prevent
the infiltration of TiO2 into the porous SiO2 scaffold, it is filled
with polymer which can be removed during the high tempera-
ture annealing. The high refractive index contrast between the
porous SiO2 and TiO2 layer makes sure that the photonic struc-
tural color can still be preserved after the perovskite infiltra-
tion, as shown in Figure 13c. Zhou et al.[142] designed colorful
PSCs by using the PEDOT:PSS as the electrode. The colorful
property results from the light interference with the polymer
electrode, which selectively reflects the incident light to gen-
erate the structural color. Figure 13d,e shows the device archi-
tecture and digital images of the PSCs. The top electrode is
deposited by transfer printing, and the thickness can be con-
trolled by the spin-coating speed and numbers of the depos-
ited layers. The color that the device displays has a direct rela-
tionship with the thickness of the polymer electrode, and the
refractive index of the bottom HTL can also affect the reflected
light wavelength.
7. Conclusion and Outlook
There have been great achievements in the past few years in
exploring the unique properties of the organic–inorganic
hybrid perovskite and boosting the performance of PSCs. In
this review, we have summarized the frequently used optical
designs for PSCs to optimize the optoelectronic conversion

Figure 13.  a) Schematic drawing and b) cross-sectional SEM image of PSCs. c) Different colors induced by the tunable photonic structure. Reproduced
with permission.[141] Copyright 2016, American Chemical Society. d) Diagram of the PSCs showing the selective reflection of incident light. e) Optical
images of the colorful PSCs. Reproduced with permission.[142] Copyright 2016, American Chemical Society.

Small Methods 2019, 1900150 1900150  (16 of 19) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
and construct devices with specific applications. The contin-
uous effort that is devoted to this exciting field from worldwide
researchers will bring about more impressive innovations and
advances, and we are optimistic about the further development
of PSCs in PCE, stability, and eco-friendly issues. In consid-
eration of the optical properties–related designs, there is still
great potential for further improvement in device performance.
First of all, the light-trapping techniques with more efficient
light management and the perovskite materials with a higher
absorption coefficient may increase the light harvesting and the
photocurrent. The reduced thickness of light absorber may lead
to the realization of a ultra-thin device. Second, more efficient
light conversion materials may effectively convert the UV light
into visible light and address the UV stability of the device.
Third, the development of the transparent electrode and inter-
face engineering will enable the tandem device that integrates
the PSCs and commercial solar cells with an expanded light
absorption range and continuously increased PCE, which repre-
sents one of the major topics in future research. The designing
strategies from the perspective of optical properties toward
better device performance and stability may contribute a lot for
the future application of PSCs.
Acknowledgements
This research was supported by the National Natural Science Foundation
of China (51772197, 51422206, 51372159), 1000 Youth Talents Plan, Key
University Science Research Project of Jiangsu Province (17KJA430013),
333 High-level Talents Cultivation Project of Jiangsu Province, and Six
Talents Peak Project of Jiangsu Province, and funded by the Priority
Academic Program Development of Jiangsu Higher Education
Institutions (PAPD).
Conflict of Interest
The authors declare no conflict of interest.
Keywords
optical design, perovskite solar cells, power conversion efficiency, UV
stability
Received: February 23, 2019
Revised: March 13, 2019
Published online:
[1] A. Kojima, K. Teshima, Y. Shirai, T. Miyasaka, J. Am. Chem. Soc.
2009, 131, 6050.
[2] M. Lee, J. Teuscher, T. Miyasaka, T. Murakami, H. Snaith, Science
2012, 338, 643.
[3] J. Burschka, N. Pellet, S. Moon, R. H. Baker, P. Gao,
M. Nazeeruddin, M. Grätzel, Nature 2013, 499, 316.
[4] M. Liu, M. Johnston, H. Snaith, Nature 2013, 501, 395.
[5] N. Jeon, J. Noh, Y. Kim, W. Yang, S. Ryu, S. Seok, Nat. Mater. 2014,
13, 897.
[6] H. Zhou, Q. Chen, G. Li, S. Luo, T. Song, H. Duan, Z. Hong,
J. You, Y. Liu, Y. Yang, Science 2014, 345, 542.
Small Methods 2019, 1900150 1900150  (17 of 19)
www.small-methods.com
[7] Q. Dong, Y. Fang, Y. Shao, P. Mulligan, J. Qiu, L. Cao, J. Huang,
Science 2015, 347, 967.
[8] W. Yang, J. Noh, N. J. Jeon, Y. Kim, S. Ryu, J. Seo, S. Seok, Science
2015, 348, 1234.
[9] M. Saliba, T. Matsui, K. Domanski, J. Seo, A. Ummadisingu,
S. Zakeeruddin, J. Correa-Baena, W. Tress, A. Abate, A. Hagfeldt,
M. Grätzel, Science 2016, 354, 206.
[10] X. Li, D. Bi, C. Yi, J. Décoppet, J. Luo, S. Zakeeruddin, A. Hagfeldt,
M. Grätzel, Science 2016, 353, 58.
[11] Q. Jiang, L. Zhang, H. Wang, X. Yang, J. Meng, H. Liu, Z. Yin,
J. Wu, X. Zhang, J. You, Nat. Energy 2017, 2, 16177.
[12] H. Tan, A. Jain, O. Voznyy, X. Lan, F. Arquer, J. Fan,
R. Quintero-Bermudez, M. Yuan, B. Zhang, Y. Zhao, F. Fan, P. Li,
L. Quan, Y. Zhao, Z. Lu, Z. Yang, S. Hoogland, E. Sargent, Science
2017, 355, 722.
[13] N. Jeon, H. Na, E. Jung, T. Yang, Y. Lee, G. Kim, H. Shin, S. Seok,
J. Lee, J. Seo, Nat. Energy 2018, 3, 682.
[14] D. Luo, W. Yang, Z. Wang, A. Sadhanala, Q. Hu, R. Su, R. Shivanna,
G. Trindade, J. Watts, Z. Xu, T. Liu, K. Chen, F. Ye, P. Wu, L. Zhao,
J. Wu, Y. Tu, Y. Zhang, X. Yang, W. Zhang, R. Friend, Q. Gong,
H. Snaith, R. Zhu, Science 2018, 360, 1442.
[15] T. Leijtens, G. Eperon, N. Noel, S. Habisreutinger, A. Petrozza,
H. Snaith, Adv. Energy Mater. 2015, 5, 1500963.
[16] J. Huang, Y. Yuan, Y. Shao, Y. Yan, Nat. Rev. 2017, 2, 17042.
[17] M. Petrus, J. Schlipf, C. Li, T. Gujar, N. Giesbrecht,
P. Müller-Buschbaum, M. Thelakkat, T. Bein, S. Hüttner,
P. Docampo, Adv. Energy Mater. 2017, 7, 1700264.
[18] H. Snaith, J. Phys. Chem. Lett. 2013, 4, 3623.
[19] S. Stranks, H. Snaith, Nat. Nanotechnol. 2015, 10, 391.
[20] G. Yang, H. Tao, P. Qin, W. Ke, G. Fang, J. Mater. Chem. A 2016,
4, 3970.
[21] J. Im, I. Jang, N. Pellet, M. Grätzel, N. Park, Nat. Nanotechnol.
2014, 9, 927.
[22] M. Xiao, F. Huang, W. Huang, Y. Dkhissi, Y. Zhu, J. Etheridge,
A. Gray-Weale, U. Bach, Y. Cheng, L. Spiccia, Angew. Chem. 2014,
126, 10056.
[23] N. Jeon, J. Noh, W. Yang, Y. Kim, S. Ryu, J. Seo, S. Seok, Nature
2015, 517, 476.
[24] H. Jung, N. Park, Small 2015, 11, 10.
[25] T. Liu, Q. Hu, J. Wu, K. Chen, L. Zhao, F. Liu, C. Wang, H. Lu,
S. Jia, T. Russell, R. Zhu, Q. Gong, Adv. Energy Mater. 2016, 6,
1501890.
[26] F. Huang, A. Pascoe, W. Wu, Z. Ku, Y. Peng, J. Zhong, R. Caruso,
Y. Cheng, Adv. Mater. 2017, 29, 1601715.
[27] H. Chen, Adv. Funct. Mater. 2017, 27, 1605654.
[28] G. Xu, R. Xue, W. Chen, J. Zhang, M. Zhang, H. Chen, C. Cui,
H. Li, Y. Li, Y. Li, Adv. Energy Mater. 2018, 8, 1703054.
[29] J. Chen, N. Park, Adv. Mater. 2018, 1803019.
[30] Z. Yang, J. Dou, M. Wang, Sol. RRL 2018, 2, 1800177.
[31] W. Ke, C. Xiao, C. Wang, B. Saparov, H. Duan, D. Zhao, Z. Xiao,
P. Schulz, S. Harvey, W. Liao, W. Meng, Y. Yu, A. Cimaroli, C. Jiang,
K. Zhu, M. Al-Jassim, G. Fang, D. Mitzi, Y. Yan, Adv. Mater. 2016,
28, 5214.
[32] J. Peng, Y. Wu, W. Ye, D. Jacobs, H. Shen, X. Fu, Y. Wan, T. Duong,
N. Wu, C. Barugkin, H. Nguyen, D. Zhong, J. Li, T. Lu, Y. Liu,
M. Lockrey, K. Weber, K. Catchpole, T. White, Energy Environ. Sci.
2017, 10, 1792.
[33] Q. Wang, Q. Dong, T. Li, A. Gruverman, J. Huang, Adv. Mater.
2016, 28, 6734.
[34] T. Bu, J. Li, F. Zheng, W. Chen, X. Wen, Z. Ku, Y. Peng, J. Zhong,
Y. Cheng, F. Huang, Nat. Commun. 2018, 9, 4609.
[35] X. Zheng, B. Chen, J. Dai, Y. Fang, Y. Bai, Y. Lin, H. Wei, X. Zeng,
J. Huang, Nat. Energy 2017, 2, 17102.
[36] M. Abdi-Jalebi, Z. Andaji-Garmaroudi, S. Cacovich, C. Stavrakas,
B. Philippe, J. Richter, M. Alsari, E. Booker, E. Hutter, A. Pearson,
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
S. Lilliu, T. Savenije, H. Rensmo, G. Divitini, C. Ducati, R. Friend,
S. Stranks, Nature 2018, 555, 497.
[37] C. Ran, J. Xu, W. Gao, C. Huang, S. Dou, Chem. Soc. Rev. 2018, 47,
4581.
[38] J. Correa-Baena, M. Saliba, T. Buonassisi, M. Grätzel, A. Abate,
W. Tress, A. Hagfeldt, Science 2017, 358, 739.
[39] D. Bi, C. Yi, J. Luo, J. Décoppet, F. Zhang, S. Zakeeruddin, X. Li,
A. Hagfeldt, M. Grätzel, Nat. Energy 2016, 1, 16142.
[40] X. Xiao, C. Bao, Y. Fang, J. Dai, B. Ecker, C. Wang, Y. Lin, S. Tang,
Y. Liu, Y. Deng, X. Zheng, Y. Gao, X. Zeng, J. Huang, Adv. Mater.
2018, 30, 1705176.
[41] J. Heo, D. Song, S. Im, Adv. Mater. 2014, 26, 8179.
[42] Y. Zhao, K. Zhu, J. Am. Chem. Soc. 2014, 136, 12241.
[43] C. Wang, C. Xiao, Y. Yu, D. Zhao, R. Awni, C. Grice, K. Ghimire,
I. Constantinou, W. Liao, A. Cimaroli, P. Liu, J. Chen, N. Podraza,
C. Jiang, M. Al-Jassim, X. Zhao, Y. Yan, Adv. Energy Mater. 2017, 7,
1700414.
[44] G. Niu, X. Guo, L. Wang, J. Mater. Chem. A 2015, 3, 8970.
[45] D. Wang, H. Cui, G. Hou, Z. Zhu, Q. Yan, G. Su, Sci. Rep. 2016, 6,
18922.
[46] T. Berhe, W. Su, C. Chen, C. Pan, J. Cheng, H. Chen, M. Tsai,
L. Chen, A. Dubale, B. Hwang, Energy Environ. Sci. 2016, 9, 323.
[47] H. Zhou, J. Xu, X. Liu, H. Zhang, D. Wang, Z. Chen, D. Zhang,
T. Fan, Adv. Funct. Mater. 2018, 28, 1705309.
[48] R. Ginting, E. Jeon, J. Kim, W. Jin, J. Kang, ACS Appl. Mater. Interfaces
2018, 10, 31291.
[49] M. Tavakoli, K. Tsui, Q. Zhang, J. He, Y. Yao, D. Li, Z. Fan,
ACS Nano 2015, 9, 10287.
[50] B. Dudem, J. Heo, J. Leem, J. Yu, S. Im, J. Mater. Chem. A 2016,
4, 7573.
[51] M. Jost, S. Albrecht, L. Kegelmann, C. Wolff, F. Lang, B. Lipovsek,
J. Krc, L. Korte, D. Neher, B. Rech, M. Topic, ACS Photonics 2017,
4, 1232.
[52] K. Li, Y. Zhang, H. Zhen, H. Wang, S. Liu, F. Yan, Z. Zheng,
J. Mater. Chem. A 2017, 5, 969.
[53] Q. Luo, X. Deng, C. Zhang, M. Yu, X. Zhou, Z. Wang, X. Chen,
S. Huang, Sol. Energy 2018, 169, 128.
[54] H. Yu, J. Lee, J. Yun, K. Lee, J. Ryu, J. Lee, D. Hwang, Se. Kim,
J. Jang, Adv. Energy Mater. 2017, 7, 1700749.
[55] C. Chan, C. Lin, M. Liu, K. Lee, Z. Ji, B. Huang, Adv. Mater. Interfaces
2018, 5, 1801118.
[56] H. Sun, K. Deng, Y. Zhu, M. Liao, J. Xiong, Y. Li, L. Li, Adv. Mater.
2018, 30, 1801935.
[57] Q. Jiang, X. Zhang, J. You, Small 2018, 14, 1801154.
[58] P. Zhang, J. Wu, T. Zhang, Y. Wang, D. Liu, H. Chen, L. Ji, C. Liu,
W. Ahmad, Z. Chen, S. Li, Adv. Mater. 2018, 30, 1703737.
[59] J. Hou, O. Inganäs, R. Friend, F. Gao, Nat. Mater. 2018, 17,
119.
[60] H. Kim, J. Lee, N. Yantara, P. Boix, S. Kulkarni, S. Mhaisalkar,
M. Grätzel, N. Park, Nano Lett. 2013, 13, 2412.
[61] A. Fakharuddin, F. Giacomo, A. Palma, F. Matteocci, I. Ahmed,
S. Razza, A. Epifanio, S. Licoccia, J. Ismail, A. Carlo, T. Brown,
R. Jose, ACS Nano 2015, 9, 8420.
[62] X. Li, S. Dai, P. Zhu, L. Deng, S. Xie, Q. Cui, H. Chen, N. Wang,
H. Lin, ACS Appl. Mater. Interfaces 2016, 8, 21358.
[63] C. Liu, R. Zhu, A. Ng, Z. Ren, S. Cheung, L. Du, S. So, J. Zapien,
A. Djurisic, D. Phillips, C. Surya, J. Mater. Chem. A 2017, 5, 15970.
[64] Q. Cui, X. Zhao, H. Lin, L. Yang, H. Chen, Y. Zhang, X. Li,
Nanoscale 2017, 9, 18897.
[65] D. Zhong, B. Cai, X. Wang, Z. Yang, Y. Xing, S. Miao, W. Zhang,
C. Li, Nano Energy 2015, 11, 409.
[66] G. Peng, J. Wu, S. Wu, X. Xu, J. Ellis, G. Xu, A. Stard, D. Gao,
J. Mater. Chem. A 2016, 4, 1520.
[67] P. Qin, M. Paulose, M. Dar, T. Moehl, N. Arora, P. Gao,
O. Varghese, M. Grätzel, M. Nazeeruddin, Small 2015, 11, 5533.
Small Methods 2019, 1900150 1900150  (18 of 19)
www.small-methods.com
[68] X. Wang, Z. Li, W. Xu, S. Kulkarni, S. Batabyal, S. Zhang, A. Cao,
L. Wong, Nano Energy 2015, 11, 728.
[69] X. Gao, J. Li, S. Gollon, M. Qiu, D. Guan, X. Guo, J. Chen, C. Yuan,
Phys. Chem. Chem. Phys. 2017, 19, 4956.
[70] Y. Yu, J. Li, D. Geng, J. Wang, L. Zhang, T. Andrew, M. Arnold,
X. Wang, ACS Nano 2015, 9, 564.
[71] K. Mahmood, B. Swain, A. Amassian, Adv. Mater. 2015, 27, 2859.
[72] S. Lin, Y. Su, H. Cho, P. Kung, W. Liao, J. Wu, J. Mater. Chem. A
2016, 4, 1119.
[73] O. Jaramillo-Quintero, M. Fuente, R. Sanchez, I. Recalde,
E. Juarez-Perez, M. Rincón, I. Mora-Seró, Nanoscale 2016, 8, 6271.
[74] D. Bi, G. Boschloo, S. Schwarzmuller, L. Yang, E. Johansson,
A. Hagfeldt, Nanoscale 2013, 5, 11686.
[75] D. Son, J. Im, H. Kim, N. Park, J. Phys. Chem. C 2014, 118, 16567.
[76] J. Dong, J. Shi, D. Li, Y. Luo, Q. Meng, Appl. Phys. Lett. 2015, 107,
073507.
[77] K. Mahmood, B. Swain, A. Amassian, Adv. Energy Mater. 2015, 5,
1500568.
[78] S. Li, P. Zhang, H. Chen, Y. Wang, D. Liu, J. Wu, H. Sarvari,
Z. Chen, J. Power Sources 2017, 342, 990.
[79] Y. Zheng, E. Zhao, F. Meng, X. Lai, X. Dong, J. Wu, X. Tao, J. Mater.
Chem. A 2017, 5, 12416.
[80] S. Kang, S. Jang, J. Lee, J. Yoon, D. Yoo, J. Lee, M. Choi, N. Park,
Small 2016, 12, 2443.
[81] D. Choia, S. Nama, K. Jungb, J. Moon, Nano Energy 2019, 56, 365.
[82] K. Deng, Z. Liu, M. Wang, L. Li, Adv. Funct. Mater. 2019, 1900830.
[83] M. T. Horantner, W. Zhang, M. Saliba, K. Wojciechowski,
H. J. Snaith, Energy Environ. Sci. 2015, 8, 2041.
[84] X. Chen, S. Yang, Y. Zheng, Y. Chen, Y. Hou, X. Yang, H. Yang,
Adv. Sci. 2015, 2, 1500105.
[85] S. Ha, J. Heo, S. Im, J. Moon, J. Mater. Chem. A 2017, 5, 1972.
[86] J. Wei, R. Xu, Y. Li, C. Li, J. Chen, X. Zhao, Z. Xie, C. Lee, W. Zhang,
J. Tang, Adv. Energy Mater. 2017, 7, 1700492.
[87] Z. Yu, L. Sun, Small Methods 2018, 2, 1700280.
[88] M. Long, Z. Chen, T. Zhang, Y. Xiao, X. Zeng, J. Chen, K. Yan, J. Xu,
Nanoscale 2016, 8, 6290.
[89] S. Mali, H. Kim, H. Kim, S. Shim, C. Hong, Mater. Today 2018, 21,
483.
[90] Y. Wang, T. Zhang, M. Kan, Y. Zhao, J. Am. Chem. Soc. 2018, 140,
12345.
[91] J. Duan, Y. Zhao, B. He, Q. Tang, Angew. Chem., Int. Ed. 2018, 57,
3787.
[92] W. Ke, C. Stoumpos, I. Spanopoulos, L. Mao, M. Chen,
M. Wasielewski, M. Kanatzidis, J. Am. Chem. Soc. 2017, 139,
14800.
[93] S. Shao, Y. Cui, H. Duim, X. Qiu, J. Dong, G. Brink, G. Portale,
R. Chiechi, S. Zhang, J. Hou, M. Loi, Adv. Mater. 2018, 30,
1803703.
[94] A. Pascoe, S. Meyer, W. Huang, W. Li, I. Benesperi, N. Duffy,
L. Spiccia, U. Bach, Y. Cheng, Adv. Funct. Mater. 2016, 26,
1278.
[95] K. Meng, S. Gao, L. Wu, G. Wang, X. Liu, G. Chen, Z. Liu, G. Chen,
Nano Lett. 2016, 16, 4166.
[96] Y. Wang, M. Li, X. Zhou, P. Li, X. Hu, Y. Song, Nano Energy 2018,
51, 556.
[97] Y. Wang, P. Wang, X. Zhou, C. Li, H. Li, X. Hu, F. Li, X. Liu, M. Li,
Y. Song, Adv. Energy Mater. 2018, 8, 1702960.
[98] Z. Liu, J. Hu, H. Jiao, L. Li, G. Zheng, Y. Chen, Y. Huang, Q. Zhang,
C. Shen, Q. Chen, H. Zhou, Adv. Mater. 2017, 29, 1606774.
[99] J. Chen, L. Zuo, Y. Zhang, X. Lian, W. Fu, J. Yan, J. Li, G. Wu, C. Li,
H. Chen, Adv. Energy Mater. 2018, 8, 1800438.
[100] W. Zhang, M. Saliba, S. Stranks, Y. Sun, X. Shi, U. Wiesner,
H. Snaith, Nano Lett. 2013, 13, 4505.
[101] D. Lee, W. Kim, B. Cha, J. Kwon, S. Kim, M. Kim, J. Kim, D. Wang,
J. Park, ACS Appl. Mater. Interfaces 2016, 8, 449.
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
[102] S. Carretero-Palacios, A. Jimenez-Solano, H. Míguez, ACS Energy
Lett. 2016, 1, 323.
[103] N. Pathak, N. Chander, V. Komarala, R. Sharma, Plasmonics 2017,
12, 237.
[104] M. Saliba, W. Zhang, V. Burlakov, S. Stranks, Y. Sun, J. Ball,
M. Johnston, A. Goriely, U. Wiesner, H. Snaith, Adv. Funct. Mater.
2015, 25, 5038.
[105] N. Fu, Z. Bao, Y. Zhang, G. Zhang, S. Ke, P. Lin, J. Dai, H. Huang,
D. Lei, Nano Energy 2017, 41, 654.
[106] J. Cui, C. Chen, J. Han, K. Cao, W. Zhang, Y. Shen, M. Wang,
Adv. Sci. 2016, 3, 1500312.
[107] Z. Yuan, Z. Wu, S. Bai, Z. Xia, W. Xu, T. Song, H. Wu, L. Xu, J. Si,
Y. Jin, B. Sun, Adv. Energy Mater. 2015, 5, 1500038.
[108] A. Abrusci, S. Stranks, P. Docampo, H. Yip, A. Jen, H. Snaith,
Nano Lett. 2013, 13, 3124.
[109] J. Lee, Y. Hsieh, N. Marco, S. Bae, Q. Han, Y. Yang, J. Phys. Chem. Lett.
2017, 8, 1999.
[110] B. Chen, X. Zheng, Y. Bai, N. Padture, J. Huang, Adv. Energy Mater.
2017, 7, 1602400.
[111] G. Eperon, T. Leijtens, K. Bush, R. Prasanna, T. Green, J. Wang,
D. McMeekin, G. Volonakis, R. Milot, R. May, A. Palmstrom,
D. Slotcavage, R. Belisle, J. Patel, E. Parrott, R. Sutton, W. Ma,
F. Moghadam, B. Conings, A. Babayigit, H. Boyen, S. Bent, F. Giustino,
L. Herz, M. Johnston, M. McGehee, H. Snaith, Science 2016, 354, 861.
[112] D. Zhao, Y. Yu, C. Wang, W. Liao, N. Shrestha, C. Grice,
A. Cimaroli, L. Guan, R. Ellingson, K. Zhu, X. Zhao, R. Xiong,
Y. Yan, Nat. Energy 2017, 2, 17018.
[113] A. Rajagopal, Z. Yang, S. Jo, I. Braly, P. Liang, H. Hillhouse, A. Jen,
Adv. Mater. 2017, 29, 1702140.
[114] J. Mailoa, C. Bailie, E. Johlin, E. Hoke, A. Akey, W. Nguyen,
M. McGehee, T. Buonassisi, Appl. Phys. Lett. 2015, 106, 121105.
[115] D. McMeekin, G. Sadoughi, W. Rehman, G. Eperon, M. Saliba,
M. Hörantner, A. Haghighirad, N. Sakai, L. Korte, B. Rech,
M. Johnston, L. Herz, H. Snaith, Science 2016, 351, 151.
[116] Y. Wu, D. Yan, J. Peng, T. Duong, Y. Wan, S. Phang, H. Shen,
N. Wu, C. Barugkin, X. Fu, S. Surve, D. Grant, D. Walter, T. White,
K. Catchpole, K. Weber, Energy Environ. Sci. 2017, 10, 2472.
[117] K. Bush, A. Palmstrom, Z. Yu, M. Boccard, R. Cheacharoen,
J. Mailoa, D. McMeekin, R. Hoye, C. Bailie, T. Leijtens, I. Peters,
M. Minichetti, N. Rolston, R. Prasanna, S. Sofia, D. Harwood,
W. Ma, F. Moghadam, H. Snaith, T. Buonassisi, Z. Holman,
S. Bent, M. McGehee, Nat. Energy 2017, 2, 17009.
[118] T. Todorov, T. Gershon, O. Gunawan, Y. Lee, C. Sturdevant,
L. Chang, S. Guha, Adv. Energy Mater. 2015, 5, 1500799.
[119] A. Guchhait, H. Dewi, S. Leow, H. Wang, G. Han, F. Suhaimi,
S. Mhaisalkar, L. Wong, N. Mathews, ACS Energy Lett. 2017, 2, 807.
Small Methods 2019, 1900150 1900150  (19 of 19)
www.small-methods.com
[120] Q. Han, Y. Hsieh, L. Meng, J. Wu, P. Sun, E. Yao, S. Chang, S. Bae,
T. Kato, V. Bermudez, Y. Yang, Science 2018, 361, 904.
[121] M. He, X. Pang, X. Liu, B. Jiang, Y. He, H. Snaith, Z. Lin,
Angew. Chem., Int. Ed. 2016, 55, 4280.
[122] H. Li, C. Chen, J. Jin, W. Bi, B. Zhang, X. Chen, L. Xu, D. Liu,
Q. Dai, H. Song, Nano Energy 2018, 50, 699.
[123] N. Chander, A. Khan, P. Chandrasekhar, E. Thouti, S. Swami,
V. Dutta, V. Komarala, Appl. Phys. Lett. 2014, 105, 033904.
[124] L. Jiang, W. Chen, J. Zheng, L. Zhu, L. Mo, Z. Li, L. Hu, T. Hayat,
A. Alsaedi, C. Zhang, S. Dai, ACS Appl. Mater. Interfaces 2017, 9,
26958.
[125] F. Bella, G. Griffini, J. Correa-Baena, G. Saracco, M. Grätzel,
A. Hagfeldt, S. Turri, C. Gerbaldi, Science 2016, 354, 203.
[126] S. Ito, S. Tanaka, K. Manabe, H. Nishino, J. Phys. Chem. C 2014,
118, 16995.
[127] I. Hwang, M. Baek, K. Yong, ACS Appl. Mater. Interfaces 2015, 7,
27863.
[128] W. Li, W. Zhang, S. Reenen, R. Sutton, J. Fan, A. Haghighirad,
M. Johnston, L. Wang, H. Snaith, Energy Environ. Sci. 2016, 9,
490.
[129] T. Leijtens, G. Eperon, S. Pathak, A. Abate, M. Lee, H. Snaith,
Nat. Commun. 2013, 4, 2885.
[130] C. Chang, K. Lee, W. Huang, H. Siao, Y. Chang, Chem. Mater.
2015, 27, 5122.
[131] W. Chen, J. Zhang, G. Xu, R. Xue, Y. Li, Y. Zhou, J. Hou, Y. Li,
Adv. Mater. 2018, 30, 1800855.
[132] E. Gaspera, Y. Peng, Q. Hou, L. Spiccia, U. Bach, J. Jasieniak,
Y. Cheng, Nano Energy 2015, 13, 249.
[133] Z. Li, S. Kulkarni, P. Boix, E. Shi, A. Cao, K. Fu, S. Batabyal,
J. Zhang, Q. Xiong, L. Wong, N. Mathews, S. Mhaisalkar,
ACS Nano 2014, 8, 6797.
[134] P. You, Z. Liu, Q. Tai, S. Liu, F. Yan, Adv. Mater. 2015, 27, 3632.
[135] Y. Zhang, Z. Wu, P. Li, L. Ono, Y. Qi, J. Zhou, H. Shen, C. Surya,
Z. Zheng, Adv. Energy Mater. 2018, 8, 1701569.
[136] D. Liu, C. Yang, R. Lunt, Joule 2018, 2, 1827.
[137] G. Eperon, V. Burlakov, A. Goriely, H. Snaith, ACS Nano 2014, 8,
591.
[138] Y. Deng, Q. Wang, Y. Yuan, J. Huang, Mater. Horiz. 2015, 2, 578.
[139] C. Quiroz, C. Bronnbauer, I. Levchuk, Y. Hou, C. Brabec,
K. Forberich, ACS Nano 2016, 10, 5104.
[140] D. Liu, L. Wang, Q. Cui, L. Guo, Adv. Sci. 2018, 5, 1800836.
[141] W. Zhang, M. Anaya, G. Lozano, M. Calvo, M. Johnston,
H. Míguez, H. Snaith, Nano Lett. 2015, 15, 1698.
[142] Y. Jiang, B. Luo, F. Jiang, F. Jiang, C. Fuentes-Hernandez, T. Liu,
L. Mao, S. Xiong, Z. Li, T. Wang, B. Kippelen, Y. Zhou, Nano Lett.
2016, 16, 7829.
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim