Flexible Perovskite Solar Cells

Machine Translated by Google
Review
Flexible Perovskite Solar Cells
Hyun Suk Jung,1, * Gill Sang Han,1 Nam-Gyu Park,2, * and Min Jae Ko3, *
Since the first report on solid-state perovskite solar cells (PSCs) with 9.7% effi ciency and Context & Scale
500-h long-term stability in 2012, PSCs have achieved an amazing power-conversion In a short time of 7 years,
efficiency (PCE) of 24.2%, exceeding the PCEs of multi-crys talline Si (22.3%), thin-film perovskite solar cells (PSCs) have
crystalline Si (21.2%), copper indium gallium selenide (22.6%), and CdTe-based thin-film achieved an amazing power
SCs (22.1%), and are suitable for transform ing into flexible solar cells based on plastic conversion efficiency (PCE) of
substrates. The light weight and flex ibility of flexible-PSCs (F-PSCs) allows their use in 24.2%, which exceeds the PCEs of
niche applications such as portable electric chargers, electronic textiles, large-scale multi-crystalline Si (22.3%), thin film
industrial roofing, and power sources for unmanned aerial vehicles (UAVs). However, the F- crystalline Si (21.2%), copper indium
PSCs always exhibit inferior efficiency compared to rigid PSCs, i.e., champion-cell ef gallium selenide (22.6%), and CdTe-
ficiency of F-PSCs is 19.11%, which is apparently lower than that of rigid cells. based thin-film SCs (22.1%).
Also, the world-best module efficiency for rigid perovskite module is 17.18% (30 cm2 )
higher than that for flexible perovskite module efficiency, 15.22% (30 cm2 ). Moreover, the Owing to low process
F-PSCs have not shown better long-term stability in comparison with rigid PSCs. In this temperature, mechanical
review paper, we investigate fundamental challenges of F-PSCs regarding relatively low durability, and the potential for the
efficiency and stability and demonstrate the recent efforts to overcome big hurdles. Also, solution-based roll-to-roll
current attempts for the commercialization of F-PSCs are introduced. (R2R) process, the PSC has a
strong potential of being utilized in
the form of flexible solar cell
Introduction based on a plastic substrate. This

flexible-PSC (F-PSC) is expected to
In photovoltaic history, there has been no solar cell like the perovskite solar cell (PSC),
be used in niche applications such
which has achieved an amazing power conversion efficiency (PCE) of 24.2% in such a
as portable electric chargers,
short time of 7 years. This efficiency exceeds the PCEs of multi-crystalline Si (22.3%), thin-
electronic textiles, large-scale
film crystalline Si (21.2%), copper indium gallium selenide (22.6%), and CdTe-based thin-
industrial roofing, and power sources
film SCs (22.1%), owing to the excellent optical, electrical, and chemical properties of
for unmanned aerial
perovskite materials.1,2 In 2012, the study on adopting the perovskite materials in a solid-
vehicles (UAVs).
state sensitized cell reported the achievement of 9.7% PCE,3 which triggered the efficiency
race in PSCs. In 2019, more than 12,000 research papers cumulatively and many
However, the champion-cell
commercial companies, including Oxford PV, Dyesol, and Frontier Energy Solutions, are
efficiency of the F-PSC is 19.11%,
developing their own technol ogies for the commercialization of perovskite solar modules.
which is apparently lower than that
of the rigid cell (24.2%). Also, the
world-best perovskite module
The cost-effective material,4 low formation energy,5 mechanical durability,6 and potential
efficiency on a rigid substrate is
for a solution-based roll-to-roll (R2R) process make the PSC suitable for realizing a flexible
17.1%, outstripping the efficiency of
thin-film solar cell that employs a plastic substrate such as poly ethylene terephthalate
flexible perovskite module (11.7%).
(PET). Furthermore, the flexible PSC (F-PSC) using plastic substrate would produce the
Moreover, the F-PSCs have not
most competitive power per weight among the solar cells (Figure 1A).7 Therefore, F-PSCs
shown superior long term stability to
can be used in niche applications such as portable electric chargers, electronic textiles,
rigid cells. To commercialize the F-
large-scale industrial roofing, and power sources for unmanned aerial vehicles (UAVs).
PSC, the efficiency needs to be
comparable to the glass-based rigid
PSC as well as the long-term stability.
In contrast with rigid PSC based on glass substrate, the charge transport layer, espe cially
the electron transport layer (ETL), like TiO2, ZnO, and SnO2, should be formed at a low
temperature of below 150 C in plastic-based F-PSCs, which is a non-trivial
1850 Joule 3, 1850–1880, August 21, 2019 ª 2019 Elsevier Inc.

challenge to achieving high efficiency. Since the F-PSC is potentially used in bend able or foldable
In this review paper, we
electronic devices, robust bending durability is another important issue. In this regard, there has been
investigate the fundamental
remarkable progress in developing F-PSCs with high efficiency as well as with bending durability.
challenges of F-PSCs such as the optical
transmittance of flexible substrates and
electrical
In 2014, the F-PSC with a meaningful efficiency of 10.2% was exploited by using ZnO nanocolloids
conductivity of flexible
ETL (5 nm).8 The high-density and uniform ZnO layer was successfully prepared without a sintering
transparent conducting oxides, uniform
process. In 2015, Kim et al.6 realized a high PCE of 12.2% flexible cell by fabricating a TiO2 ETL using
coating technology with a large area on
plasma-enhanced atomic layer deposition (PEALD). They performed the bending durability test of F-
flexible substrates, the high moisture
PSC for the first time and characterized the excellent bending durability of perovskite materials. Park
permeability of plastic flexible substrates,
et al.9 also proved the super-flexibility of F-PSCs by demonstrating the complete shape recovery of
and super flexibility. We also introduce
the device under repeated crumpling condition without signifi cant mechanical damage. The PCE was
recent efforts for overcoming the
maintained up to 60% of initial value even after 50 cycles of complete crumpling (Figures 1B and 1C).
aforementioned issues as well as for
Another breakthrough was achieved by exploiting the inverted structured F-PSC, which adopted an
facilitating the commercialization of F-
organic charge transport layer.10 Owing to the use of PEDOT:PSS as an organic hole-trans port layer
PSCs. As a perspective, we suggest the
(HTL), the maximum processing temperature for manufacturing flexible PSS was 90 C. Stretchable
future direction of research and
and ultra-lightweight F-PSC with the inverted structure was successfully fabricated, implying that the F-
development of F-PSCs such as the
PSC could be applied to power avia tion models.7 The photovoltaic performance of ultrathin F-PSC
module technology involving assembling
was displayed as a function of compression condition (Figure 1D).
multiple subcells and the flexible tandem
devices
including flexible PSC/CIGS or flexible

Recently, there have been many review papers introducing recent progress in F-PSCs.11–16 In
PSC/organic photovoltaics (OPVs).
contrast with the previously published review papers, this review paper pays attention to the key
scientific challenges underlying the inherently low PCEs in F-PSCs compared to PSCs employing rigid
substrates. So far, champion cell efficiency of the flexible cell is 19.11%,17 which is apparently lower
than that of the rigid cell, 24.2%. Also, the world-best efficiency for rigid perovskite module is 17.1%,
which is fairly higher compared to flexible perovskite module,18 11.7% and 15.2% for the area of 703
and 30 cm2 , respectively, as displayed in Fig ure 1E.19–21 Moreover, the F-PSCs have not shown
good long-term stability in com parison with rigid cells. Theperformance
fundamentalofreason
F-PSCsforisthe inferior
related to the
difference in chemical and physical properties of substrate materials that are glass and plastic. In
particular, the restrictive process temperature for plastic substrate hinders the fabrication of highly
conductive transparent con ducting oxide (TCO) and recombination-free charge transport layer, which
makes it difficult to achieve high efficiency. Also, the optical transmittance of plastic sub strate is lower
than that of the glass substrate, which is another reason for inferior photovoltaic performance for F-
PSC. The PET is permeable to oxygen and water molecules, and is not able to perfectly block the
attack from oxygen and water, un like glass materials.22,23
In this review paper, we investigate the fundamental challenges of F-PSCs regarding relatively low
1School of Advanced Materials Science and
efficiency and stability compared to glass substrate-based PSCs and demonstrate the recent attempts
Engineering, Sungkyunkwan University, Suwon
to overcome big hurdles. Moreover, this paper deals with the efforts that have been made to facilitate 16419, Republic of Korea 2School of Chemical
the commercialization of Engineering, Sungkyunkwan University, Suwon
F-PSC. 16419, Republic of Korea 3Department of Chemical
Engineering, Hanyang University, Seoul 04763,
Republic of Korea *Correspondence:
Fundamental Challenges in Flexible Perovskite Solar Cells Challenge in
hsjung1@skku.edu (H.S.J.), npark@skku.edu (N.-
Substrate Materials for the Flexible Solar Cells First, a general review of G.P.), mjko@hanyang.ac.kr (M.J.K.) https://doi.org/
the substrate materials for flexible solar cells is provided.24 Flexible substrates are among the most 10.1016/j.joule.2019.07.023
important components required to realize
Joule 3, 1850-1880, August 21, 2019 1851

Figure 1. The Superiority of F-PSCs and Progress of PCE in F-PSCs/Module

(A) Comparison of power-per-weight for the various solar cells. Reprinted with permission from Kaltenbrunner et al.7 Copyright 2015 Springer Nature.
(B) Shape recoverable F-PSCs after random crumpling followed by thermal treatment.
(C) Photovoltaic performance before and after crumpling test. Reprinted with permission from Park et al.9 Copyright 2015 John Wiley and Sons.
7
(D) Stretchable F-PSCs and their current-voltage characteristics as a function of compression. Reprinted with permission from Kaltenbrunner et al.
Copyright 2015 Springer Nature.
(E) Progress of PCEs in rigid-type cells and F-PSCs for unit cell and module.2,17–19,21
high-performance flexible electronics. Many performances strongly depend on sub

strate characteristics. Here, several requirements for the flexible substrates of
photo voltaic devices are listed, as follows. (1) Optical properties: because solar
cells are light-absorbing devices, the substrate should optically transmit as much
light as possible, especially more than 90% transmission in the visible-light region.
(2) Barrier properties: most electronic devices are vulnerable to oxygen or moisture,
which leads to significant degradation of performance. The substrate should act as
a bar rier layer to avoid the penetration of oxygen and water vapor for long-term
stable performance. (3) Higher conductivity: charge-collecting layers, such as
TCOs, are usually deposited on the substrate to function as transparent conductive
electrodes (TCEs) consisting of the TCO and substrate. The sheet resistance of
TCEs is closely related to the photovoltaic performance, especially the fill factor
and photocurrent density of solar cells. (4) Chemical properties: the substrates are
exposed to a wide range of process chemicals such as gas and solvents during
fabrication, and hence must be stable to these chemicals. PET and polyethylene
naphthalate (PEN) films, which are widely used polymeric substrates, show good
resistance to various sol vents. (5) Mechanical properties: flexible substrates should
comply with deformable transformation under severe stress and strain and effectively release stress without
1852 Joules 3, 1850-1880, August 21, 2019

losing their original functions. In addition, dimensional stability, that is, the ability of
materials to maintain its original dimensions while being used or processed, should
be ensured. (6) Thermal and thermomechanical properties: two parameters, i.e.,
the thermal transition temperature and the coefficient of thermal expansion (CTE),
have to be considered. The softening temperature of substrate materials, especially
the so-called glass transition temperature (Tg) for the polymer, must be compatible
with the maximum processing temperature (Tmax) that films can be subjected to.
The substrates would be expanded or contracted during temperature change. Sig
nificant mismatch of thermal properties between the neighboring layers would exert
additional stress on the lattice, resulting in the creation of strain and cracking during
heating and cooling processes. The limit of tolerable thermal mismatch is expressed
by jDCTE,DTj %0:1% 0:3%, where DCTE and DT are the difference in CTE between
the base substrate and the neighboring layers that are subsequently deposited, and
the temperature excursion during processing, respectively. (7) Surface roughness:
rough surface of the substrate could not assure the conformal coating of layers and
avoidance of electrical short circuiting in the device. When the roughness is very
large, additional planarization processes are necessary like polishing and coating
for the steel-based substrates and polymer, respectively, which would in crease the
processing cost.
Three types of materials, i.e., ultrathin flexible glass, metal foils, and polymers, are
available for the substrate of flexible photovoltaics. Glass substrates with a thickness
of several hundred mm become flexible. The flexible glass can meet most of the
stan dards for the requirements of the flexible substrate, described above. The
strong temperature tolerance of up to over 600 C, good dimensional stability, low
CTE of 10 6
/ C, andheavy
fragility, perfect gas barrier
weight, properties
and high are very
cost would attractive.
be big concerns, However,
as compared
to other candidate materials. By contrast, thin metal foils such as stainless steel and
Ti retain very good mechanical properties and resistance to process chemicals;
however, the impermeability of light would limit its application to the substrate of
flexible solar cells. Polymer substrate would be ideal in terms of flexibility, light
weight, low cost, and R2R processability. However, there are many drawbacks such
as low heat resistance, high CTE, and poor gas barrier properties for oxygen and
moisture.
In particular, because of the low Tg and high CTE of the polymer substrate,
shrinkage or expansion of polymer substrate would occur with temperature change.
Therefore, the whole fabrication processes should be completely redesigned and
compared to the processes capable of high-temperature heat treatments. In addition,
according to the tolerance thermal mismatch rule explained above, even a small
mismatch would cause cracked or strained TCO or device. Therefore, the process
windows for a polymer-based solar device become very narrow. In addition,
regarding the barrier properties of polymer substrates, most of the polymer
substrates do not satisfactorily meet the demanding requirements for oxygen and
moisture protec tion. As a result, the extra encapsulations are highly necessary for
the long-term stable operation of F-PSCs. Additionally, it is desirable that the
functions that are antireflection (AR) and ultraviolet (UV) proof (AR+UV-proof) are
added to the encap sulating layer for further light absorption and long-term stability, respectively.
Optical Transmittance of Flexible Substrates and Electrical Conductivity of Flexible

Transparent Conducting Oxides In this regard, this discussion focuses on polymer-
substrate-based F-PSCs, because polymer substrates would be ideal platforms for
the realization of all flexible elec tronics. A number of polymers could be applied to
materials for flexible substrates.
Biaxially oriented PET and PEN films, using heat-setting for the crystallization and
Joules 3, 1850-1880, August 21, 2019 1853

Table 1. Property Parameters for Polymer Substrate
Substrate PEN PET PI PC
Tg (C) 120–155 70–110 155–270 145
Tm ( C) 269 115–258 250–452 115–160
Density (g/cm3 ) 1.36 1.39 1.35–1.43 1.20–1.22
Modulus (MPa) 0.1–0.5 3 103 2–4.1 3 103 2.5 3 103 2.0–2.6 3 103
Work temp. ( C)
–
50–150 <400 40–130
CTE (ppm/C) 20 15–33 8–20 75
Water absorption (%) 0.3–0.4 0.4–0.6 1.3–3.0 0.16–0.35
Solvent resistance good good good poor
Dimensional stability good good fair fair
Tm: melting temperature
stabilization of the films, are widely used as conventional and commercially available
polymer substrates, despite several drawbacks, such as low heat resistance and
dimensional instability during processing. Polycarbonate (PC) and polyethersulfone
(PES) are optically more transparent and have a relatively high Tg compared with PET
and PEN, but they lack process chemical resistance and have poor gas barrier prop
erties. Polyimide (PI) exhibits excellent thermal properties but is not optically clear,
which is critical for a substrate material of light-absorbing devices, although color less
PI has been recently developed. Table 1 compares the properties of flexible
polymer substrates.25
For use as TCEs, TCOs are subsequently deposited on the flexible substrates. As
base materials of TCOs, indium oxide (In2O3), tin oxide (SnO2), and zinc oxide
(ZnO) are typically used. By doping specific metal ions to those, the transparency
and conductivity noticeably increase because of the extrinsic doping effects. Among
the TCOs, indium tin oxide or tin-doped indium oxide (ITO) and fluorine-doped tin
oxide (FTO) are commercially and widely used in optoelectronic devices.
The deposition process of TCO on polymer substrates such as PET and PEN is
limited because of thermal sensitivities of polymers. The flexible TCEs with higher
optical transmittance and conductivity are basic essentials for the high performance
of F-PSC. However, typically, the overall performance of plastic-based F-PSC would
be inferior to that of rigid glass-based PSCs due to the lower optical transmittance
and lower electrical conductivity of polymer-based TCE.
The optical transmittance of substrates is very critical for PCE because photoactive
materials should absorb as much light as possible. Polymeric materials inherently
absorb ultraviolet and even visible light to some extent, due to the electronic tran sition
of the chromophore in polymers, leading to the light-harvesting loss for the
photoactive materials. Zhao et al.26 demonstrate that the flexible ITO/PET sub strates
show relatively lower transmittance in the visible range, compared to ITO/
glass, due to the lower transparency of the polymer (Figure 2A).
The optical properties of F-PSCs are also affected by those of TCOs that are gener ally
transparent in visible and infrared regions due to the large bandgap (Eg) of over
3.0 eV. The transmission window defined by the two imposed boundaries (lg and lp)
is also observed. The lg at the short wavelength of UV regions is related to photon
absorption with energy larger than Eg. The second transmission edge (lp) is referred
to as the plasma wavelength, where the frequency of the light is the same as the
1854 Joules 3, 1850-1880, August 21, 2019

Figure 2. The Optical and Electrical Properties of TCOs

(A) Comparison of the optical transmittance of ITO (100 nm), PET (125 um), and ITO (130 nm) and glass. Reprinted with permission from Zhao et al.26
Copyright 2014 Royal Society of Chemistry.
(B) The wavelength dependence of optical transmittance of TCO.27
(C) The temperature dependence of sheet resistance of TCE. Reprinted with permission from Zardetto et al.29 Copyright 2011 John Wiley and Sons.
frequency of the collective oscillation of electrons in materials. The lp is generally

detected at the longer wavelength around the near-infrared region. For wavelengths
larger than lp, the transmittance steeply decreases as the reflectance caused by the
plasma resonance of the electrons becomes dominant.27 The two absorption edges
(lg and lp) are shifted to a shorter wavelength as the carrier concentration of TCOs
increases, as shown in Figure 2B. Since the carrier concentration affects both the
electrical and the optical properties of TCOs, optimization of carrier concentration
is necessary. Ideally, TCO should have large transmission windows with higher elec
tric conductivity.
The ITO is the most widely used TCO for polymer substrates, due to the better trans
mittance and lower sheet resistance than others. It is generally known that the elec
trical properties of ITO strongly depend on the film composition and deposition
parameters such as sputtering power, oxygen pressure, film thickness, and substrate
deposition temperature.28 Zardetto et al.29 reported that the sheet resistance of
PET/ITO increases at over 180 C and the sheet resistance of PEN/ITO increases at
235 C. However, this would not be an issue for the polymer substrates in which a
low-temperature process is essential. On the other hand, the conductivity of plas tic-
based TCE employing ITO is typically lower than that of a glass-based one,
due to the relatively lower carrier concentration of ITO films on polymers. The micro
structure of ITO without high-temperature thermal treatments is generally amor phous
or partially crystalline, leading to poor electrical properties.
For the fabrication of ITO-based glass, ITO is dc-magnetron sputtered at glass sub
strates while the substrate is maintained at approximately 300 C–400 C, or sput tered
on the cold substrate, followed by annealing at 200 C. Such a heat treatment
would result in a high degree of the crystalline or partially crystalline microstructure
of ITO. Meanwhile, the conduction electrons are created because oxygen defi ciencies
could donate a maximum of two unbound electrons by removing oxygen
from the cluster, which is beneficial for better electrical conductivity. Besides,
dopant S4+ would replace In3+ by extrinsic doping during sputtering, further produc
ing one more electron in the conduction band of In2O3 x. Both the oxygen vacancies
and tin dopants in substitutional lattice positions would simultaneously contribute to
electrical conductivity. On the other hand, such contributions as doping and crystal
effects would not be expected in the ITO deposited at room-temperature process ing
limited by the polymer substrate. Bellingham et al.30 reported that the higher
Joules 3, 1850-1880, August 21, 2019 1855

resistivity of the amorphous or less crystalline ITO films would be a consequence of the
inability to activate the impurity dopant, i.e., limited diffusion of Sn4+ from inter stitial
locations and grain boundaries into an In3+ site, caused by the low deposition temperature.
In this case, the conductivity solely depends on oxygen vacancies.
Furthermore, the electron transports in the amorphous or less crystalline ITO films would
not be as effective as those in the ordered crystalline structure, due to the relatively large
amount of defects and charge traps. Figure 2C exhibits the sheet resistance of PET/ITO
and glass/ITO. The sheet resistances of PEN/ITO and PET/ITO significantly increase after
thermal treatment at 200 C and 240 C, respectively.29
As described previously, the morphological, electrical, and optical properties of ITO films
change depending on the deposition condition and types of substrates. How ever, except
for the ITO crystalline quality and preferred orientation, no significant difference in chemical
composition or chemistry according to the process tempera ture was reported.31–36 Lee
investigated the relationship between microstructure of ITO and electron scattering
mechanisms at the various process conditions.33 For the less crystalline ITO, the grain
boundary scattering was dominant while ITO with a high crystallinity was governed by the
ionized-impurity scattering mechanism due to the higher carrier concentration.
Deposition of thicker TCO on plastic substrates is another strategy to compensate for the
low conductivity. However, because the absorption of TCO films rises strongly with
increasing thickness, there are some limitations to meet both the desired properties
together.
Recently, F-PSCs have been fabricated using various transparent electrodes, such as
metal-based materials (nanowires, grids, and networks), conducting polymers, car bon-
based materials (carbon nanotube and graphene), and oxide–metal–oxide mul
tilayers.37,38 Table 2 summarizes the transmittance and sheet resistance of various
flexible PCEs for the F-PSCs reported.
Challenges in Uniform Coating Technology with a Large Area on Flexible

Substrates
With the dramatic boosting of the certified efficiency of up to 24% for rigid glass based
PSCs,2 there has been much interest and effort for the enlargement of the de vice area
and upscaling. A few reviews of research on the processing and upscaling of PSC modules
have recently been reported.48–52 High-quality perovskite films with a small area (25
cm2 ) can be fabricated using a simple solution method, such as spin coating. However,
despite a few reports on the fabrication of large-area PSCs using spin coating, it is
generally accepted that there are limitations to the extension of the process to large-area
modules (25 cm2 or larger), because it is difficult to control the morphology and kinetics of
perovskite crystals over a large area without pinholes.
However, in terms of cost and productivity, flexible solar devices are more promising than
rigid glass ones. For the commercialization of F-PSCs, it is important to develop a process
to make mass production with an R2R process possible. The printing and coating methods
can be divided into contact and noncontact methods depending on whether the coating
materials are in direct contact with the coating plate (Fig ure 3). Screen printing,
flexography, gravure printing, and soft lithography belong to the contact methods that have
been widely used recently in printed electronics.
Recently, Cruz et al.25 reported the relationship between process parameters and printing
quality for the fabrication of printed electronics on polymer substrates.
1856 Joules 3, 1850-1880, August 21, 2019

Table 2. Transmittance and Sheet Resistance of Various Flexible Substrates for the F-PSCs
Substrates Electrodes Transmittance (%) Sheet Structure of PSCs PCE (%) Ref.
Resistance
(U/cm2 )
PET AZO/Ag/AZO 81 7.5 PET/AZO/Ag/AZO/PEDOT: PSS/PolyTPD/MAPbI3/PCBM/Au 7 10
Ti Foil Ag (8 nm)
– –
Ti foil/TiO2 BL/MP-TiO2/ MAPbI3/Spiro/Ag 0.77 39
Ti Foil Ag (12 nm)

– –
Ti Foil Ag (16 nm)

– –
Ti Foil Ag (20 nm)

– –
Ti Foil CNTs 60–80 –
Ti foil/TiO2 NTs+MAPbI3/CNTs+Spiro 8.31 40
You
Ag (1 nm) +ITO> 80 107.14 Ti/TiO2 BL/TiO2+MAPbI3/ Spiro/Ag+ITO 11.01 41
PET PEDOT: PSS + EG> 60 28 PET / PEDOT: PSS (PH1000) + EG / PEDOT: PSS (VPAI 4083) / 4.9 42
MAPbI3/PCBM/TiOx/Al
This willow glass 81.5 31.3 MgF2/Willow glass/ITO/SnO2/ FAMACs/Spiro/MoOx/Al 17.3 43
Willow glass AZO 85.8 17.8 MgF2/Willow glass/ITO/SnO2/ FAMACs/Spiro/MoOx/Al 12.2 43
Willow glass IZO 76.4 11.6 MgF2/Willow glass/ITO/SnO2/ FAMACs/Spiro/MoOx/Al 18.1 43
PET AuCl3 GR >80 75 Al / PCBM / MAPbI3 / PEDOT: PSS / AuCl3-GR / APTES / PET 17.9 37
DOG AZO/AgNW/ 88.6 at 550 nm 11.86 Au/Spiro/MAPbI3/ZnO/AZO/AgNW/AZO 11.23 44

AZO
PEN graphene ~97 552.0 PEN/Graphene/MoO3/PEDOT:PSS/MAPbI3/C60/BCP/LiF/Al 16.8 45
PET ITO 70 15 PET/ITO/PEDOT: PSS (VPAI 4083)/MAPbI3/PCBM/TiOx/Al 4.3 42
Glass ITO 80 8 Glass/ITO/PEDOT: PSS (VPAI 4083)/MAPbI3/PCBM/TiOx/Al 9 42
Glass ITO – –
Glass/ITO/PEDOT: PSS/MAPbI3/PCBM/Al 11.5 46
PET ITO – –
PET/ITO/PEDOT: PSS/MAPbI3/PCBM/Al 9.2 46
PET PEDOT: PSS – –

PET / PEDOT: PSS / CH3NH3PbI3-xClx / PTCDI / Cr2O3 / Cr / Au 12 47
Cellulose MoOx/Au/MoOx 62.5 (top 9 paper/Au/SnO2/meso-TiO 2/CH3NH3PbI3/Spiro-OMeTAD/ 2.7 38
paper electrode) MoOx/Au/MoOx
They proposed that the coating quality on the substrates mainly depends on the sur face
wettability, spreadability, and adhesion. In particular, when polymer substrates
are used, the low surface energy of polymer substrates gives rise to poor coating or
printing quality, requiring additional surface treatment before processing. Such
additional processes generally increase the cycle time and production costs. The
coating quality generally depends on the surface tension of the bottom layer. There fore, a
deep understanding of the relationship between process parameters and
printing quality is required for the fabrication of high-performance F-PSCs with large
areas. Conformal coating or printing without pinholes on floppy substrates is crucial
to the performance of F-PSCs. In particular, the control of the crystallization kinetics
of the perovskite layer should be uniformly controlled over a large area during sol vent
evaporation. Moreover, the profiles of plastic substrates as supporting layers
generally remain intact, even after multiple coatings of upper layers. Therefore,
the planarization for uniform coating is important. In addition, accumulated internal
stress or strain is generated when the mechanical and thermal shocks are applied to
the films, leading to delamination or debonding. This is more severe for large-area
devices.
High Moisture Permeability of Plastic Flexible Substrates

Although the light absorption ability of organic-inorganic hybrid perovskite is excel lent, the
ionic nature of perovskite crystals makes them inherently vulnerable to
moisture as well as oxygen, resulting in the degradation and phase transition
of the perovskite. To avoid such deterioration, the substrate requires complete
Joules 3, 1850-1880, August 21, 2019 1857

Figure 3. Schematic Illustration of Contact (Upper Three Figures) and Noncontact (Lower Three
Figures) Methods for Perovskite Layer Coating on a Flexible Substrate
protection from the intrusion of moisture. By contrast, glass substrates can block the
penetration of moisture through the substrates. However, F-PSCs with polymer sub
strates have severe stability problems because of the much higher water vapor trans
mission rate (WVTR) or oxygen transmission rate (OTR) of polymeric substrates.
The WVTR and OTR of polymer materials are generally approximately 1–10 g/(m2
day) and about 1–10 mL/(m2 day), requiring additional lamination or encapsulation
6
to achieve those values in the range of 10 .
The reasons for the poor barrier stability and higher gas permeability are related to
the morphology of polymers in the films. The microstructure of polymers can be
divided into a crystalline part and an amorphous structure, depending on whether
the arrangements of the polymers are regular or irregular. PET and PEN, which are
widely used as substrates, are semi-crystalline polymers in which crystalline and
amorphous are mixed, thus easing penetration of gas or moisture molecules. How
ever, inorganic materials, such as glass SiO2, are regularly arranged in an atomic
arrangement. As a result, such a dense structure of inorganic materials effectively
suppresses the penetration of the molecules, such as moisture or oxygen. The fac
tors affecting the moisture permeability are (1) film thickness, (2) film density, and
(3) crystallinity.53 Gas molecules diffuse through the nanoscale or micron-scale
pores, called ‘‘free volume,’’ in the polymers. There are three stages of penetration
of gas molecules: (1) polymer adsorption of penetrating molecules, (2) diffusion due
to the difference in concentration of the molecules inside and outside the polymer,
and (3) desorption from the polymer film. These three series of steps are continuous,
especially water molecules penetrating the interior. The thermal motion of polymer
segments facilitates this penetration. Considering these sequential steps, the thicker
the polymer substrate, the longer the diffusion distance of the molecules becomes,
resulting in lower moisture permeability. However, because the gas transmittance
decreases as the thickness increases, it is important to select an appropriate thick
ness of polymer substrate because of the trade-off relationship with optical transmit
tance. Additionally, as the density of the film increases, the size of the free volume
pore becomes smaller, so diffusion becomes difficult, and the moisture permeability
becomes lower. Finally, the free volume occupies the amorphous region rather than
the crystalline portion, so the moisture permeability decreases as the crystalline part
1858 Joules 3, 1850-1880, August 21, 2019

increases. Naturally, as the amorphous area increases, the free volume and moisture
permeability increase.
To relieve concerns about the stability issue, flexible film packaging employing a gas-
barrier encapsulating function should be developed for F-PSCs. The encapsu lating
package includes flexible front/back sheets, flexible encapsulant, edge seal, and
electrical joints. A typical configuration of flexible packaging for F-PSCs is a transparent
front sheet/encapsulant/F-PSC/encapsulant/back sheet.54 In addition to the gas-
barrier property, the materials embedded in barrier films should exhibit a relatively
higher dielectric constant, optical transparency, thermal and UV stabilities, good
adhesion, chemical inertness, processability, and me chanical strength with scratch
resistance. Organic encapsulating materials are a good candidate to meet most of the
requirements above, except gas barrier properties. Recently, organic-inorganic
multilayer films have been commonly used to obtain better barrier properties.55 For
further performance development of barrier film, the encapsulation and packaging
technology developed in organic 6 g/(m2 day) would pro light-emitting diodes (OLEDs)
of 10 6 g/(m2 day) than vide deep insight, because OLEDs require that requires
a higheraWVTR
WVTRof
10 solar cells.
Challenges in Super Flexibility

The excellent mechanical properties of organic-inorganic hybrid perovskite mate rials
make the possibility of flexible solar cells promising. Ko et al.9 reported the mechanical
properties of all layers of organic-inorganic hybrid F-PSCs using nanoin dentation and
theoretical analyses. The Young’s modulus (E) of the hybrid perovskite layer was
noticeably lower (approximately one-tenth) than that of metal-oxide-based perovskite,
thus leading to the higher flexibility of the device. The finite-element analysis
demonstrated that significantly small plastic strain was generated over a small region
within the F-PSCs under bending. In terms of microstructure, such exceptional flexibility
is thought to originate from the weak van der Waals bonding between perovskite
+
caused by extended alkyl chains (R) in R- layers, as well as a within the perovskite
+
NH3 hydrogen/ionic bonding of NH3sheets. On the other hand, Jing Feng reported the
elastic and anisotropic properties of CH3NH3BX3 (B = Sn, PB; X = Br, I),56 suggesting
that the elastic properties are not determined by the interaction among organic and
inorganic ions, but by the type and strength of the metal–halogen (B–X) bond. The
ratio of the bulk modulus (B) to the shear modulus (G), or B/G would be a good index
for the evaluation of the ductile ability of mate rials. The hybrid perovskite materials
have a relatively lower shear modulus, implying a larger B/G with high ductility, which
would be desirable as the absorbing layer of flexible solar cells. In addition, the Poisson
ratio (n) is another parameter to deter mine the softness of materials. Taking into the
consideration that n values for hybrid organic-inorganic perovskites and ductile solids
are greater than 0.3 and 0.26, respectively, it is conjectured that the hybrid perovskite
would be adequately soft as a photon absorber on the polymer substrates. Further
studies on the molecular origin of super-flexibility of perovskite materials are necessary.
For the evaluation of flexibility, bending tests are widely used for flexible electronics.
During bending, the outer and inner surfaces experience tensile and compression
stress, respectively. The plane inside the device, where no uniaxial stress is applied
by balancing the tensile and compression stress, is defined as a neutral plane. If the
neutral plane is located at the most fragile layer, the mechanical durability is sus
tained. On the other hand, the relationship between the film strain and the radius of
bending curvature is expressed by e = d/2r, where e, d, and r are the strain, device
Joules 3, 1850-1880, August 21, 2019 1859

thickness, and radius of curvature (bending radius), respectively. According to this

relation, the thinner devices could ensure the bending stability, because a relatively
smaller strain would be applied to the devices. In this regard, the hybrid perovskites
would be ideal photo-absorbing materials because of the high absorption coeffi cient
and intrinsic soft character, enabling thinner devices. However, ITOs coated on
polymer substrates do not have high bending durability compared with perov skite
because of the ITO’s small Poisson ratio and large modulus. Thus, during repeated
bending tests, cracks occur in the ITO layer, inducing degradations in the perovskite
layer. Therefore, for the realization of super F-PSCs, strategies to uti lize new TCO
materials with a ductile nature should be introduced.
Recent Efforts on Improving Performance of Flexible Perovskite Solar Cells

Because of the restriction on process temperature for fabricating transparent con
ducting oxide, ETL and HTL, and perovskite absorber, the PCE of flexible cells is
not that much higher than those of glass-based rigid cells because of high series
resistance and facilitated recombination of charges that are inherent issues for F-
PSCs. Also, the employment of brittle TCOs like ITO and aluminum-doped ZnO
(AZO) may not enable enough flexibility to PSCs. In this section, recent efforts on
improving flexibility as well as enhancing charge collection for high efficiency and
flexibility are discussed.
The Exploitation of New Flexible TCO Substrates

ITO or FTO has been abundantly utilized in both rigid and F-PSCs. However, from
the viewpoint of cost-effectiveness, photovoltaic performance, and flexibility, these
TCO materials may not be the best way to achieve a goal. Efforts have been made
to replace these TCO materials with new compositional TCO materials. Kim et al.57
ex ploited new TCO materials that are composed of W-doped ITO (IWO) for F-PSC.
These IWO materials, prepared by plasma arc ion plating method, were analyzed
to possess high mobility (61.7 cm2 /Vs) and high transmittance of 96% at 550 nm.
Also, work function for IWO was 4.85 eV, much higher than that for ITO (4.65 eV).
This high work function may enhance Voc. To overcome the brittleness of TCO,
AZO/Ag/AZO, that is, double-sandwich structure, was provided. This new type of
TCO showed fairly low sheet resistance of 7.5 U/sq and the resultant flexible cell
maintained 98.5% of initial PCE after 50 cycles of bending test at 2.75 cm radius of
curvature.10 So far, comparative studies of photovoltaic performance of PSCs,
depending on various TCO materials, have not been reported, which is of great
importance to decide the right TCO materials for F-PSCs. Dou et al.43 performed a
comparative study regarding the influence of TCO materials on the photovoltaic
performance of PSCs (Figure 4). They demonstrated that the F-PSCs employing
the In-doped ZnO (IZO) achieved the highest efficiency of 18.1% due to the high
Voc and FF. The other TCO materials, such as ITO and AZO, showed rela tively
inferior PSC. Especially, the AZO materials showed the lowest PCE of 12.2% due
to the chemical reaction between AZO and perovskite layer, verified by analyzing
surface stoichiometry and change in photoluminescence spectra of perov skite
materials.43
Although ITO films have the same composition, the photovoltaic performance of F-
PSCs may be different depending on the fabrication method of ITO. Kim et al.58
compared the cell performance containing ITO films prepared by (1) ion-plated pro
cess and (2) sputtering process. The ion-planted ITO film showed better electrical
and optical properties such as sheet resistance and optical transmittance in compar
ison with the ITO films prepared by a sputtering process. The resultant PCE of PSC
based on ion-planted ITO was measured to be 15.4%, which implies that the
1860 Joules 3, 1850-1880, August 21, 2019

Figure 4. The Influence of TCO Materials on the Photovoltaic Performance of F-PSCs (A)
Schematic representation of device architecture for the F-PSCs, where different transparent conducting oxide (TCO), AZO (aluminum-doped zinc oxide),
ITO (tin-doped indium oxide), and amorphous IZO (indium-zinc oxide) were investigated. X-ray diffraction (XRD) patterns and transmittance of AZO, ITO,
and IZO are shown on the left. Current density-voltage (J–V) characteristics (reverse scans) under 100 mW/cm2 AM1.5G for champion
Cs0.04MA0.16FA0.80Pb1.04I2.6Br0.48 perovskite devices with (B) willow glass-AZO, (C) willow glass-ITO, and (D) willow glass-IZO. Reprinted with
permission from Dou et al.43 Copyright 2017 American Chemical Society.
photovoltaic performance of F-PSC may change according to the electrical and op

tical quality of TCO, which may be determined by preparation method.58
Metal foils have been one of the promising candidates as a flexible electrode owing
to high flexibility, high electrical conductivity, and a wide process temperature win
dow. In particular, Ti metal foils have been abundantly utilized as a flexible substrate
due to easy formation of TiO2 ETL. An attempt to replace Ti with cheap Cu foil has
been made.59 Cu foil is capable of simply forming CuI HTL. Although many efforts
have been made, it is challenging to achieve a high efficiency due to the inherent
op tical reflectivity of metal, however. Many studies have focused on the exploitation
of top electrodes that possess a high conductivity and high optical transmittance.
Ag metal film has been well utilized as a translucent top electrode. Since the
translucent Ag metal itself does not show high electrical conductivity as well as high
optical trans mittance, the modification of Ag film has been proposed.39,41,60 For
example, Ag nanowire electrodes showed the improved PCE of 7.45% compared
to the PCE of bare Ag electrode cells (6.15%). The F-PSCs employing 13 nm thick
Ag layer coated with amorphous ITO (a-ITO) exhibited 11.01%. Another Ni mesh
metal grid was utilized to replace Ag materials.61 In this study, a transparent
conductive adhesive (TCA) was adopted to reduce interfacial resistance between the metal grid and
Joules 3, 1850-1880, August 21, 2019 1861

Figure 5. Metal-Polymer Hybrid Transparent Flexible Electrode

(A) Image of the large-area flexible PET substrate with embedded Ag-mesh (FEAM) substrate.
(B) Diagram for the hybrid electrode (PET–Ag-mesh–PH1000).
(C) The structure of the FEAMs substrate with detail parameters.
(D) J–V curves in reverse and forward scan measured under 100 mW/cm2 AM 1.5G illumination and
dark for the champion flexible PET–Ag-mesh–PH1000–PEDOT:PSS–MAPbI3–PCBM–Al solar cell:
inset shows photograph of corresponding ultra-thin F-PSCs. Reprinted with permission from Li
et al.67 Copyright 2016 Springer Nature.
hole-conducting layer, which yielded 10.3% of PCE. Carbon-based nanomaterials

such as carbon nanotube (CNT) and graphene are other good candidates for trans
parent top electrode materials in Ti foil-based F-PSCs.40,62 Especially, the anodized
Ti-metal-based PSC employing a graphene top electrode exhibited a PCE of 15%.62
Instead of metal-foil substrate, flexible CNT or graphene materials that are directly
deposited on plastic substrates may be one of the alternatives to brittle TCO
materials.63 Liu et al.64 adopted a graphene layer instead of TCO and achieved a
su per-light flexible solar cell with a power density of 5.07 W/g. Efficiency of graphene
based F-PSCs has been significantly improved by combining with PEDOT:PSS layer
and incorporating dopants such as AuCl3 and MoO3 into graphene.37,45 The F-PSC
containing AuCl3-doped graphene layer with PEDOT:PSS showed a high PCE of
17.4%.37 CNTs have been also utilized as flexible transparent electrode materials.
Although the photovoltaic performance of CNT-based cells is inferior to that of gra
phene-based cells, the superior mechanical stability and large-scale fabrication pos
sibility make it appropriate for commercialization of F-PSC.65
Silver nanowire (Ag NW) or mesh has been well investigated as transparent elec
trode materials in F-PSCs owing to high figure of merit, relatively good chemical sta
bility, and bending durability. These materials are usually combined together with
PEDOT:PSS to enhance the electrical conductivity of the transparent electrode.
The Ag NWs/PEDOT:PSS electrode-based cell exhibited 11% PCE and the efficiency
was retained after 10,000 cycles of bending test under 5 mm of a radius of curva
ture.66 Moreover, to overcome the difference in work function between Ag and
PEDOT:PSS, polymer or graphene oxide (GO) interlayers were inserted.67,68 The
PCE of Ag-mesh/PH10000/PEDOT:PSS based cell was 14% achieved by Li et al.67
(Figure 5). This cell retained 95.4% of initial PCE after 5,000 bending cycles under
radius curvature of 5 mm.
1862 Joules 3, 1850-1880, August 21, 2019

Advanced Electron Transport and Hole Transport Layer for Flexible Cells
In n-i-p structure flexible cell, low-temperature formation of an ETL such as ZnO,
TiO2, and SnO2 layer on plastic-based TCO substrate is challenging. To overcome
inferior electron-transport properties of low-temperature-treated ETL, interface
modification method with C60 or graphene and new composition oxide ETL has
been exploited. Also, various carbon-based materials have been used as ETL layers.
ZnO compared with TiO2 is relatively suitable for the low-temperature process.69
Also, ZnO possesses better electrical conductivity and carrier lifetime in comparison
with TiO2, which led to a high PCE of 15.6% in F-PSCs.69
TiO2 ETLs have been well studied in F-PSCs. There have been mostly two ways to
form TiO2 ETL in a flexible plastic substrate. First, low-temperature deposition using
vacuum-based thin-film deposition systems such as the evaporator, sputter, and
atomic layer deposition (ALD); second, deposition of well-crystallized TiO2 colloidal
particles and subsequent treatment such as UV treatment or low-temperature an
nealing treatment.70–72
The RF-sputtering method for deposition of TiO2 layer has been well known. Usually,
amorphous TiO2 layer can be obtained using the low-temperature sputtering method.
Yang et al.73 compared carrier transport, recombination, and lifetime char acteristics
of both amorphous and anatase TiO2 layer. Fermi level of amorphous TiO2 was
4.15 eV, slightly lower than that of anatase TiO2 ( 4.01 eV). This leads to superior
electron-transport property of an amorphous layer, achieving a PCE of 15.07% for F-
PSC.73 The PEALD method is favorable for precise control of thickness and reducing
oxygen vacancies in TiO2 ETL. Kim et al.6 realized F-PSC with a PCE of 12.2% by
fabricating TiO2 ETL with the aid of low-temperature PEALD process, as shown in
Figure 6. The charge transport properties of TiO2 ETL prepared by PEALD are
enhanced by interface modification with PCBM, which yields 17.7% PCE.74
Moreover, Giacomo et al.72 were able to fabricate F-PSC modules by combining
TiO2 ETL prepared by PEALD and mesoscopic TiO2 layer. TiO2 layer can be depos
ited by electron-beam evaporation and the resultant cell efficiency was reported to
be 13.5%.75
Highly crystalline anatase nanoparticles may be directly deposited as ETL. However,

the ligand or residual organics attached on the surface of TiO2 would be detrimental
to electron transport in the ETL. Therefore, further low-temperature treatment or UV
treatment is needed to achieve a high PCE. So far, UV treatment is more efficient in
removing organics and attaching each TiO2 particles than low-temperature treat
ment (150 C).70,71 The flexible cell employing the low-temperature UV-treated
Nb:TiO2 ETL exhibited 16.01% PCE due to the enhanced electron transport.
Since the stability and hysteresis issues of TiO2 materials, SnO2 has been conceived
as another alternative to ETL materials due to its enhanced charge transport prop
erty.76 Usually, SnO2 layer has been prepared by a solution coating method that
contains precursor solution coating and subsequent heat treatment. However, this
heat-treatment process is not suitable for obtaining SnO2 with good crystal quality in
plastic-based flexible cells due to limited heat-treatment temperature. Plasma
treatment may be a good method to overcome the temperature issue. N2 plasma
treatment broke alkoxy and hydroxy group to form Sn-O bonding at a low temper
ature, as shown in Figure 7. The resultant PCE of F-PSC was 18.1%.77 The employ
ment of highly crystalline SnO2 colloids is another way to achieve high efficiency.
Park et al.78 synthesized highly crystalline and dispersed SnO2 colloids. This SnO2
Joules 3, 1850-1880, August 21, 2019 1863

Figure 6. Amorphous TiO2 ETL for F-PSCs Using PEALD at the Low-Temperature Process (A)
The structure and best performing device of F-PSCs on ITO–PEN, with a TiO2 ETL by using
PEALD. Cross-sectional SEM image of the inorganic-organic halide perovskite planar heterojunction
flexible solar cell and schematic of the flexible device structure. J–V curve measured under the
simulated solar light for the best performing PEN–ITO–TiOx–CH3NH3PbI3-x)Clx–spiro MeOTAD–Ag
flexible device. Reprinted with permission from Kim et al.6 Copyright 2015 Royal Society of Chemistry.
(B) F-PSCs with hybrid double ETL (PCBM and TiO2 prepared by PEALD). A cross-sectional TEM
image of the as-prepared a-TiO2–PCBM ETL.-based PSCs. A schematic representation and J–V
curve of an a-TiO2–PCBM ETL-based PSC on the ITO-PEN substrate. Reprinted with permission
from Kim et al.74 Copyright 2018 John Wiley and Sons.
colloid ETL exhibited excellent charge-transport property, which enabled a PCE of 17.7%.
PEALD-synthesized ETL shows also the excellent photovoltaic performance with a PCE of
18.36%.21 In addition, the low-temperature-processed EDTA (ethylene diamine tetraacetic
acid)-complexed SnO2-based F-PSC achieved a PCE over 18.4%.79 To enhance the
charge-transport property of SnO2 ETL, doping metal ions or mixing graphene oxide have
been attempted.80,81
New composition ETLs have been exploited to enhance charge transport as well as to
reduce the hysteresis phenomenon in F-PSC. Zn2SnO4 (ZSO) is a good example,
82 The PCE of ZSO-based F-PSCs
possessing better optical transmittance than SnO2. has been improved by tailoring particle
size and stacking structure, which leads to yielding 16.5% PCE.83 Also, the combination
of PCBM with ZSO was reported to facilitate electron transport in F-PSC.84 Nb-doped WOx
(W(Nb)Ox) was used as ETL. By controlling the thickness of W(Nb)Ox, PCE and hysteresis
properties were improved.85 Recently, fairly interesting ETL material that is nanocrystalline
titanium metal-organic frameworks (nTi-MOF) was proposed. The addition of PCBM
increased the electrical conductivity and enhanced the charge injection properties of nTi-
MOF. The flexible cell employing nTi-MOF/PCBM demonstrated a PCE of 17.43%.86
Large bandgap materials such as Nb2O5 and Al2O3 were utilized as ETLs. The elec tron
transport from the perovskite layer to TCO was enabled by quantum tunneling effect.87,88
However, the inherent high series resistance is still challenging to achieve high efficiency.
As an alternative, electrically conductive organic materials, including the modified C60 and
PCBM, have been utilized as ETLs. Stearyl dimethyl benzyl ammonium chloride (SDBAC)-
doped [6,6]-phenyl-C61-butyric acid methyl ester (PC61BM) was used as ETL wherein
SDBAC enhanced the conductivity and therefore
1864 Joules 3, 1850-1880, August 21, 2019

Figure 7. New Composition ETLs

(A) Schematic representation of the SnO2 thin-film fabrication methodology using a modified sol–gel technique by employing low-power RF N2 plasma
exposure. Cross sectional SEM image of PET–ITO–SnO2–m-Al2O3– ((FA0.83MA0.17)0.95Cs0.05PbI2.5Br0.5) –spiro-OMeTAD–Au flexible device and
architecture schematic of F-PSC. Reprinted with permission from Subbiah et al.77 Copyright 2018 American Chemical Society.
(B) A uniform SnO2 QD thin film by using ligand-capped ultrafine SnO2 quantum dots. Reprinted with permission from Park et al.78 Copyright 2018
American Chemical Society.
(C) Schematic of the synthetic protocol for nTi-MOF. The successive linked TiO2 clusters with BDC molecules create small nanocrystals. Device structure
of a F-PSC incorporating nTi-MOF/PCBM. The best performing J-V curve of the flexible nTi-MOF–PCBM PSCs. Reprinted with permission from Ryu et al.86
Copyright 2018 American Chemical Society.
enhanced the PCE to 11.8%. The polyallylamine-coupled C60 showed an excellent

charge extraction and the increased Voc owing to work function shift, thereby real
izing a highly efficient F-PSC with a PCE of 15.2%.89 Yang et al.90 used solid-state
ionic liquids (ss-IL) for ETL. The large bandgap, anti-reflection, high electron
mobility, and proper work function for ss-IL ETL enabled a high efficiency of 16.09%.
Moreover, the ss-IL ETL reduced the electron trap-state density of the perovskite
layer, leading to effectively suppressed hysteresis.
In p-i-n structure, HTL has been actively studied because HTL requires high optical
transmittance, bending durability, hole injection, and hole-transport properties in p-i-
n F-PSC. In this regard, PEDOT:PSS have been proposed as suitable HTL mate
rials.47 However, the relatively poor charge transport in the out of plane direction
due to its lamellar structure, the potential energy loss at the interface between
PEDOT:PSS and perovskite layer due to low work function, and corrosion capability
to the adjacent layers due to its acidity are critical issues.91 Therefore, new organic
HTL materials such as 1,4-bis(4-sulfonatobutoxy)benzene and thiophene moieties
(PhNa-1T) and (N-(4-(9H-carbazol-9-yl)phenyl)-7-(4-(bis(4-methoxyphenyl)amino)
phenyl)-N-(7-(4-(bis(4-methoxyphenyl)amino)phenyl)-9,9-dioctyl-9H-fluoren-2-yl)-
9,9-dioctyl-9H-fluoren-2-amine (CzPAF-TPA)) have been exploited.91,92 For
example, the F-PSC using PhNa-1T as HTL showed significantly higher 14.7% PCE in comparison
Joules 3, 1850-1880, August 21, 2019 1865

with the PEDOT:PSS-based one (8.4%), which was ascribed to the decreased potential
energy loss at the interface between perovskite and HTL as well as to efficient hole
injection.91
Since the organic HTLs exhibit relatively low stability compared with inorganic HTLs,
research on developing new HTLs has been shifted to exploit new inorganic HTLs.
In particular, NiOx materials have received a great deal of attention due to the well-
aligned band structure with perovskite layer, good optical transparency, and electron
blocking capability.91 The NiOx HTLs have been deposited by vacuum thin-film
fabrication tools such as ALD, RF-sputtering, and evaporation.93–95 How ever, in F-
PSC for potential roll to roll process, low-temperature solution coating has been under
active research.96–98 Najafi et al.98 achieved 16.6% PCE in F-PSC, which exhibited
fairly good stability. Over 85% of the maximum stabilized output ef ficiency was retained
after 1,000 h aging employing a thin MAPbI3 perovskite.98 Also, NiOx derivatives have
been studied to improve photovoltaic perfor mance.99–101 Cu-doped NiOx (Cu:NiOx)
HTL-based F-PSC demonstrated 17.16% because of the improved charge injection
and the improved surface morphology.100 Noticeably, the hybrid HTL composed of
PEDOT:PSS–NiOx made it possible to achieve 18.0% PCE in F-PSC.101 Cu-based
HTL materials such as CuyCrzO2 and CuSCN have been introduced.102,103 However,
these materials are fairly challenging due to the problem of formation of CuI coming
from inter-diffusion of Cu and In ions.102,103
In p-i-n structure, n-type ETL needs efficient electron extraction, full coverage on the
perovskite layer, no damage on perovskite layer during the coating process, and no
chemical reaction between ETL and perovskite under operating conditions.104 In this
regard, fullerene-based ETL such as PCBM has been the most popular in p-i-n struc
tured PSC. However, the wettability of PCBM on the perovskite layer is not better than
polymer-based ETL, which may induce the deterioration of long-term stability related
to insufficient coverage of PCBM. Therefore, polymeric ETLs, including the naphthalene
diimide (NDI)-based polymer with strong electron withdrawing dicyanothiophene
(P(NDI2DT-TTCN)) and triphenylamine (TPA)-(3-cyano-4,5,5-tri methyl-2(5H)-
furanylidene)malononitrile (3CN), have been developed in F-PSC.
Representatively, the flexible cell employing the P(NDI2DT-TTCN) as ETL achieved
17.0% PCE with good long-term stability owing to the improved charge extraction
ability. Also, the mechanical durability of this material was better than PCBM.104
High-Quality Perovskite Film for Flexible Cells

The formation of high-quality perovskite film with large grain size, low trap density, high
coverage, and high crystallinity, etc., is one of the major challenges for high-ef ficiency
F-PSCs on the plastic substrate. In general, perovskite film exhibits poor film quality
on the flexible substrate, because of the low surface energy, poor wettability, and
wrinkle of the plastic substrate. Therefore, it is necessary to develop a suitable
perovskite precursor for the same perovskite film quality on a flexible substrate,
compared with high-quality perovskite film on a rigid substrate. Bi et al.105 investi
gated the various ratios of FAI:MABr concentration in perovskite precursors, the
optimized composition of which exhibits the long recombination lifetime, small trap
state density, and pin-hole-free film, resulting in 18.1% of PCE in F-PSCs.
One of the strategies for high-quality perovskite film is to add the additives in the
perovskite precursor. H2O is critical to controlling the crystallization rate and grain
size, which achieved the 13.11% PCE (Figure 8A).106 Moreover, the dual additives of
DIO and H2O in perovskite precursors can induce gradient evaporation during
1866 Joules 3, 1850-1880, August 21, 2019

Figure 8. Additive Induced High-Quality Perovskite Film (A)

Schematic illustration of the different morphology development for CH3NH3PbI3 xClx films with and
without H2O additive. Reprinted with permission from Du et al.106 Copyright 2017 American Chemical
Society.
(B) Illustration of the F-PSC structure and J–V curves of F-PSCs under both reverse and forward scan
directions using MAPbI3–DS (dimethyl sulfide) as the absorber layer. Reprinted with permission from
Feng et al.107 Copyright 2018 John Wiley and Sons.
(C) Cross-sectional SEM image and J-V curves of a F-PSC with the Rb1K4CsFAMA absorber.
Reprinted with permission from Cao et al.17 Copyright 2019 Royal Society of Chemistry.
the drying and heat process. This leads to high-quality perovskite film with large
grain and uniformity, achieving a PCE of 18.0% for F-PSC.101 A dimethyl sulfide
(DS) additive has been successfully developed as it chelates with Pb2+ to form an
in termediate complex and slows down the crystallization rate of perovskite film.
The resultant PCE of F-PSC was 18.4% with good mechanical tolerance (Figure
8B).107 Recently, a quintuple-cation perovskite film containing Rb+, K+, Cs+, FA+,
and MA+ was proposed to reduce the trap density in the perovskite film, which a
cham pion PCE for F-PSC of 19.11% was achieved with less hysteresis (Figure 8C).17
Ultra-Flexible Perovskite Solar Cells

F-PSCs can be potentially used as a flexible power source for mobile devices as
well as a portable outdoor electricity generator. For example, the recent advent of
fold able smartphones is expected to open a new era of flexible electronics. In
foldable devices, there are two types of folding modes: in-folding and out-folding. In-
folding mode requires an extremely small bending radius of curvature like 2 mm,
which is fairly challenging in foldable devices composed of inorganic electrical components.
Also, many F-PSCs contain inorganic materials including TCO, ETLs, and HTL that
are not favorable for reliable flexibility. The F-PSC adopting PEN/Sn-doped indium
oxide (ITO) showed 1,000 times bending durability at the radius of curvature of 10
mm. However, at the radius of curvature of 4 mm, the cell performance signifi cantly
deteriorated because of the fracture of ITO layer (Figure 9).6
Efforts have been made to improve the bending reliability of F-PSCs by replacing
or modifying inorganic TCO and substrate materials. Nanostructured ITO demon
strated the improved flexibility of PSCs. The inverted nanocone ITO showed
Joules 3, 1850-1880, August 21, 2019 1867

Figure 9. Highly Bending and Durable F-PSCs

(A) Normalized PCE measured after bending the substrate within a specified radius of 400 mm to 1
mm and normalized PCE as a function of bending cycles with different radii of 400 nm, 10 nm, and 4
mm. The real images attached on the human neck, wrist, and finger corresponding to 400 nm, 10 nm
and 4 nm bending radii, respectively (inset within upper figure). Real images taken during the bending
tests (inset within lower figure). Reprinted with permission from Kim et al.6 Copyright 2015 Royal
Society of Chemistry.
(B) Device structure of Gr-Mo/PEN based F-PSC and Normalized PCEs as a Function of Bending
Cycles at a Fixed Bending Radius of 4 mm for the Gr-Mo–PEN and ITO–PEN devices. The inset
photograph shows the Gr-Mo–PEN device bent at a bending radius. Reprinted with permission from
Yoon et al.45 Copyright 2017 Royal Society of Chemistry.
improved bending durability compared with the planar ITO based cell. The F-PSC
employing inverted cone retained 95% of the initial PCE after 200 cycles of bending
test under a 6 mm radius of curvature, which was ascribed to strain relaxing effect of
nanocone structure.108
Metal nanowires possess excellent flexibility, which enables to replace the relatively
brittle TCO. However, the roughness and adhesion issues remain. These issues have
been resolved by combining an oxide layer or hybrid layer.109,110 The composite of
crystalline ITO metal nanowire-GFRHybrimers is one of the representative examples.
The flexible cell containing this nanocomposite showed excellent bending dura bility.
Under 2.5 mm radius of curvature, this cell showed 20% degradation to initial PCE
after 500 cycles of bending test.110
The PEDOT:PSS system has been frequently utilized for realizing ultra-F-PSCs owing
to its flexible nature of the polymer. The F-PSCs employing PEDOT:PSS materials do
not possess any cracks from the fracture of PEDOT:PSS in contrast with ITO materials
under a severe bending condition such as a 4 mm radius of curvature.111 The F-PSCs
1868 Joules 3, 1850-1880, August 21, 2019

based on highly conductive nitric acid treated PEDOT:PSS with 50 nm thickness ex

hibited 90% of the initial efficiency after 1,000 cycles of bending test under 5 mm of
the radius of curvature.112 Combination of Ag mesh and PEDOT:PSS enhances the
electrical conductivity of the transparent electrode, which results in a PCE of 14%.67
Moreover, this flexible cell exhibits excellent bending durability, retaining over 95.4%
of its initial PCE value even after 5,000 fully bending cycles under 5 mm radius of
curvature.
Carbon nanomaterials such as CNT and graphene have shown excellent flexibility
with proper electrical conductivity compared with TCO. All-carbon-electrode-based F-
PSC employing graphene as the transparent bottom electrode and CNT as the top
electrode retains 84% of the initial PCE after 2,000 cycles of the bending test under
a 4 mm radius of curvature.63 MoO3-decorated graphene-based F-PSC demonstrates
super flexibility, i.e., only 10% degradation in PCE is observed after 1,000 cycles of
the bending test at a radius of curvature = 2 mm. Moreover, this cell achieved 16.8%
PCE, which exhibits the great potential for the highly efficient foldable photovoltaic cell.45
The flexibility of PSC has been improved by adopting a new type of flexible substrates
with conducting layers such as Ti plate–TiO2 substrate.113 The highly bendable PSC
containing TiO2 nanolayer-coated Ti plates does not show any degra dation in PCE
after 1,000 cycles bending test at 4 mm radius of curvature, which is explained in
terms of high crystallinity with low oxygen vacancy that improves bending durability.113
Toward Commercialization
Owing to abundant cheap precursor materials and low-cost processes, the perov
skite solar module has been believed to be economically viable, which will enable it
to be a leader in the future photovoltaic market. The manufacturing costs for the
perovskite solar module has been expected to be one-third of those based on bulk
silicon PV technologies.12 Moreover, the levelized cost of the electricity (LCOE) for
perovskite solar modules could reach 6 US cents/KWh, comparable to the LCOE for
the fossil fuels once the module efficiency and lifetime exceeded 12% and 15 years,
respectively.
High efficiency and bending durability for F-PSCs provide prolific application
opportunities. These flexible solar cells have the capability of being installed on the
curved surface, which is suitable for building integrated photovoltaics (BIPV).
Moreover, lightweight with high efficiency enables to achieve a high-power density of
2 W/g,67 which makes them possible to be utilized as a power source in high-alti
tude unmanned aerial vehicles (HAUAVs). To commercialize this F-PSC, however,
several issues remain: (1) developing uniformly large-area coating technology (Table
3), (2) ensuring long-term stability by encapsulation technology, and (3) ex ploiting
emerging unique flexible cells for special applications need to be solved.
Uniform and Large Area Coating Technologies for Flexible Modules

Spin coating method has been adopted in the fabrication of small-sized cells, which
is not suitable for obtaining uniform ETL, HTL, and perovskite light-absorbing layers
due to deflection of large size flexible substrate. Rather, the flexible substrate makes
it easy to realize mass production based on R2R process. In R2R, slot-die coating
method has been utilized to fabricate large size F-PSC owing to facile mass produc
tion of thin films with uniform thickness. Research on slot-die R2R coating has
focused on optimizing some process parameters to (1) improve the uniformity of each
ETL, HTL, and Perovskite layer; (2) control crystallization kinetics of perovskite;
Joules 3, 1850-1880, August 21, 2019 1869

Table 3. The Uniform and Large-Area Coating Methods for Perovskite Modules, and Comparison of Device Structure, Substrate Type, Active Area,
and Performance of Perovskite Modules
Scalable Coating Substrate Device Structure Active Jsc Voc (V) Fill PCE (%) Ref.
Coating Layer Method Type Area (cm2 ) (mA/cm2 ) Factor (%)
Perovskite doctor-blade rigid glass/FTO/TiO2/perovskite/spiro 10.1 4.29 4.11 58.14 10.26 119
doctor-blade rigid glass / FTO / TiO2 / perovskite / P3HT glass / 100 0.83 9.61 53.79 4.30 119
doctor-blade rigid ITO / PTAA / perovskite / 33 1.19 18.1 71.3 15.3 120
fullerene (C60)/bathocuproine (BCP)
doctor-blade rigid glass / ITO / PTAA / perovskite / 57.2 1.26 17.04 67.5 14.6 120
fullerene (C60)/bathocuproine (BCP)
bar rigid glass/FTO/TiO2/ perovskite 24.97 2.72 8.66 72.6 17.1 18
(double-layered)/P3HT
drop casting rigid glass/FTO/TiO2/ZrO2- perovskite/ 31 4.9 3.72 57.5 10.46 121
carbon
drop casting rigid glass/FTO/TiO2/ZrO2- perovskite/ 70 1.772 9.63 62.9 10.74 121
carbon
drop casting rigid glass/FTO/TiO2/ZrO2- perovskite/ 49 2 9.3 56 10.4 122

carbon
soft-cover rigid glass/FTO/TiO2/ perovskite/spiro 36.1 1.97 10.5 75.7 15.7 123
deposition
spray rigid glass/FTO/TiO2/ perovskite/PTAA glass/ITO/ 40 2.10 10.5 70.16 15.5 124
lock-die rigid TiO2/perovskite/spiro 168.75 0.692 21.2 67.9 10 125
spin rigid glass/ITO/TiO2/perovskite/spiro 4 19.9 0.91 75 13.6 126
spin rigid glass/ITO/PEDOT/perovskite/PCBM 60 1.9 8.1 57 8.7 127
spin rigid glass/ITO/PEDOT/perovskite/PCBM 40 2.0 10.1 63.7 12.9 128
spin rigid glass / ITO / PTAA / PFN / perovskite / 9.06 16.86 3.27 73 14.1 129
PCBM / PFN / Ag
ETL or HTL ALD + screen flexible PET/ITO/ALD-TiO2/TiO2 scaffold/ 7.92 5.2 3.39 71 3.1 72
printing perovskite/spiro-OMeTAD/Au
RF-sputtering + flexible AZO/LiF/C60/Perovskite/spiro 10.2 2.1 7.3 67.5 10.5 130
evaporation OMETAD/Au
lock-die flexible PET/ITO/SnO2/perovskite/spiro 16.09 3.28 6.727 69 15.22 20

OMETAD/Au
spin flexible PEN/ITO/MFGO/perovskite/ 10 4.34 3.76 49.1 8.1 131
PC61BM / BCP / Ag
spin flexible PET/ITO/SnO2/meso-TiO2/ 12 3.12 5.014 55.9 8.8 132
perovskite/spiro-OMeTAD/Au
spin flexible PET/ITO/SnO2/perovskite/spiro 10 6.479 3.075 62 12.31 133

OMETAD/Au
spin rigid glass/FTO/SnO2/perovskite/spiro 25 1.98 11.2 69.0 15.3 134

OMETAD/Au
spin rigid glass/FTO/SnO2/perovskite/spiro 100 1.02 20.2 0.68 14.03 134

OMETAD/Au
and (3) enhance the PCE of the flexible device (Figure 10).114 However, the research
on manufacturing F-PSC using the slot-die method is at an early stage. This research
is still ongoing for achieving the exploitation of commercially viable F-PSCs. Since
slot-die coating of organic materials such as PEDOT:PSS and spiro-OMETAD is rela
tively favorable compared with inorganic ETL and perovskite materials, efforts have
been made to fabricate uniform ETLs or perovskite layers.20,114–116
Bu et al.20 developed a strategy to form high quality SnO2 ETLs using the slot-die
coating method. By modifying the SnO2 surface with KOH, the surface defects at
the interface between SnO2 and perovskite layer were significantly reduced owing
1870 Joules 3, 1850-1880, August 21, 2019

Figure 10. Photographic Images of the R2R-Coated Perovskite Layer and an Example of the
Manufactured Flexible Devices
Reprinted with permission from Galagan et al.114 Copyright 2018 John Wiley and Sons.
to the formation of KBr, which resulted in improving efficiency and reducing hyster
esis on F-PSCs. The efficiency of flexible perovskite module with a size of 5 3 6 cm2
was 15.22%.
PEDOT:PSS as HTL in the p-i-n structure was coated using a slot-die R2R process.
To improve film coverage and morphology of the perovskite layer, 3-aminopropanoic
acid was adopted as a self-assembled monolayer containing a carboxyl group.
This carboxyl group was found to act as nuclei for crystallization of perovskite, which
resulted in a much smoother perovskite surface morphology together with a PCE
enhancement.116
The feasibility of upscaling F-PSC to a width of 30 cm based on slot-die R2R coating

was demonstrated by Galagan et al.114 They performed R2R deposition of ETL and
perovskite layers at the web speed of 3–5 m/min with nontoxic solvents, which
showed a potential for future R2R manufacturing and commercialization of F-PSCs.
Beside the slot-die R2R coating method, solution-shearing and spray-coating

methods have been introduced. Crystal nucleation and growth in large-area MAPbI3
thin films was confined by using solution shearing, which yielded near single-crystal
line perovskite microarrays with a high degree of controlled macroscopic alignment
and crystal orientation and consequently exhibited significant improvements in op
tical and optoelectronic properties.117
Also, TiO2 ETL and perovskite layers with high uniformity, crystallinity, and surface
coverage were obtained by using an ultrasonic spray-coating (USC) method.118 The
TiO2 ETL deposited by USC was cured by high-density pulsed beam of infrared light,
realizing F-PSCs with a PCE of 8.1% that are robust under mechanical
stress.
Recent Encapsulation Technologies for Long-Term Stability

Although remarkable advances in the efficiency of F-PSC have been achieved, the
toxicity of the water-soluble lead compound and the poor stability are big chal lenges
for commercialization. Encapsulation technology is able to block the emis sion of
lead as well as extend lifetime of PSC by prohibiting exposure to ambient air
containing moisture and oxygen.
Joules 3, 1850-1880, August 21, 2019 1871

Weerasinghe et al.135 demonstrated that encapsulation of PSC devices using

high-quality flexible barrier materials and simple encapsulation architectures can
significantly improve long-term stability under ambient storage conditions.
Also, the Ca film tests revealed that the ingress of moisture and oxygen
through the adhesive layers and around electrical wire contacts is a significant life
time-limiting factor, which highlights the importance of developing new encapsula tion
architectures.
The combination of polyurethane resin encapsulation and Cr2O3–Cr interlayer

demonstrated the improved air stability of ultra-thin F-PSCs. Especially, the employ
ment of a chromium oxide–chromium interlayer was found to effectively protect the
metal top contacts from reactions with the perovskite, which was beneficial for ex
tending the long-term stability.7
Functional encapsulating materials possessing their own unique properties have

been introduced. Nanocone PDMS, which possesses antireflection and water-repel
lent functions, was attached to the front side of the flexible substrate. These
nanocone PDMS encapsulation materials contributed to improving the optical trans
mittance as well as to achieving the water-repelling effect (Figure 11A).136 The multi
layer encapsulating film consisting of ultra hydrophobic and relatively hydrophilic
layers significantly enhanced the stability of PSCs under very humid condi
tions.137,138 The ultra-hydrophobic film containing poly(methyl methacrylate)
(PMMA), polyurethane (PU), and SiO2 nanoparticles in contact with environments
served to repel water in humid environments and prevent water permeation into
the vulnerable perovskite layer, as shown in Figure 11B.138 The moderately hydro
philic PMMA layer acted as a desiccant to extract residual water from the perovskite
layer itself during the solar cell operation. The dual function of the coating film re
tained the PCE of PSCs at 17.3% for 180 min when exposed to over 95% humidity.
Emerging Flexible Photovoltaics for Pioneering a New Market

The exploitation of new concept F-PSCs can extend applicability to various devices
or systems, which facilitate opening and cornering an emerging photovoltaic mar ket.
Since the manufacturing process of PSCs is relatively simple and cost effective
compared with other photovoltaic cells, the realization of new concept solar cells us
ing perovskite absorber is viable.
The F-PSC is capable of achieving high power-per-weight if the ultra-thin and light
plastic substrate is employed. Kaltenbrunner et al.7 used 1.4 mm PET film as sub
strate and achieved a power-per-weight of 23 W/g, which is a fairly outstanding
result because the power-per-weight of silicon solar cells is 1 W/g (Figure 12A). Po
tential future applications are power sources for UAV for environmental and indus trial
monitoring, rescue and emergency response, and tactical security applica tions.7 On
the other hand, Lucarelli et al.139 reported the F-PSC that exhibits a
PCE of 10.8% and 12.1% at low luminance of 200 lx and 400 lx, respectively. In
typical office and building environments, indoor lighting could supply enough en ergy
to drive low-power sensors equipped with F-PSC, implying another potential
application of F-PSC.
Once the F-PSC uses biocompatible textiles (Figure 12B),140 wire-shaped sub
strates,141 or cellulose papers38 instead of conventional plastic substrates, this cell
can be used as reliable power sources for wearable electronics. The PSC was simply
stacked onto a textile by using an elastomer with a good adhesive property. The PCE
of textile-based F-PSC was 15% with improved ambient stability and washable
1872 Joules 3, 1850-1880, August 21, 2019

Figure 11. Strategies for Resisting Water in Humid Environments (A)

Schematic structure of the PSC device with nanocone PDMS film attached on the top and SEM image
of PDMS nanocone with 1 mm pitch and 1 mm depth. Inset image is a drop of water on the surface of
the nanocone PDMS layer, with AR 1.0 showing a large contact angle of 155 . Reprinted with
permission from Tavakoli et al.136 Copyright 2015 American Chemical Society.
(B) SEM image for the cross-section of the PMMA-PU-SiO2–PMMA-PU double-layer coated PSCs. A
change in PCE of the PSCs coated with the PMMA-PU-SiO2–PMMA-PU double layer in the ambient
conditions of 100% humidity for 180 min. Schematic illustration of the passivation effect of the PMMA-
PU-SiO2–PMMA-PU double layer. Reprinted with permission from Yoo et al.138 Copyright 2017
Springer Nature.
capability owing to the encapsulation effect of the elastomer and demonstrating the
promising potential for the wearable device applications.140 Recently, Castro-Her
mosa et al.38 reported the F-PSC fabricated on a paper substrate that exhibits a
maximum PCE of 2.7% by adopting a top semitransparent electrode. Semitrans parent
F-PSC possesses a wide variety of potential applications such as solar glass for
buildings and solar curtains for upholstery, to wearable electronics and fashion (Figure
12C).112 The semitransparent F-PSC without TCO was realized by utilizing highly
conductive n-PEDOT:PSS as both the bottom and top transparent electrodes.
The n-PEDOT:PSS was stacked onto Spiro-OMeTAD by using a stamp-transfer pro
cess with PDMS. The resultant PCE was measured as 10.3% and maintained more
than 90% of the initial value after 1,000 cycles of bending test at a radius of curvature
of 5 mm.112
Recently, self-healing F-PSC based on self-repairing of electrical pathways in me

chanically damaged metals has been exploited (Figure 12D).142 The composite of
core-shell-structured liquid metal microcapsules (LMCs) synthesized via in situ
Joules 3, 1850-1880, August 21, 2019 1873

Figure 12. Niche Applications of F-PSCs

(A) Power sources for UAV. Reprinted with permission from Kaltenbrunner et al.7 Copyright 2015
Springer Nature.
(B) The biocompatible textile-based F-PSCs. Reprinted with permission from Lam et al.140
Copyright 2017 Royal Society of Chemistry.
(C) Semi-transparent PSCs by using stamp-transfer process with PDMS. Reprinted with permission
from Zhang et al.112 Copyright 2018 John Wiley and Sons.
(D) A solar-powered smart watch embedded with self-healing conductors. Reprinted with
permission from Chu et al.142 Copyright 2018 John Wiley and Sons.
polymerizations of urea-formaldehyde onto liquid metal colloids passivated the

metal top electrode. Once the LMC passivation film was ruptured by cutting or
pressing, the LMC released and transported liquid metal to damaged sites, which
led to recovering the broken electrical pathway. The average recovery ratio of the
PCEs was revealed to be 99% after recovering the damaged sites, which demon
strates the great potential of self-repairing devices beneficial to mechanical issues
related to the repeated deformation.142
Perspectives
For the successful realization of flexible, foldable, and stretchable electronics for
future portable devices, it is essential to develop a power supplying system that in
tegrates all of them including the storage system together. Flexible solar cells are
expected to offer those functions. Among them, F-PSCs have the advantages of
both the high power of inorganic solar cells as well as the flexibility and light weight
of organic solar cells, making them ideal power-generating systems. In this paper,
we have summarized the fundamental challenges and recent efforts for the develop
ment of F-PSCs. As discussed, the reported PCEs of F-PSCs do not exceed those
of the conventional rigid PSCs, mainly due to the limitations in processing and
material selection. Nevertheless, the advantages over rigid PSCs are very clear, such as the
1874 Joules 3, 1850-1880, August 21, 2019

Figure 13. Schematic of F-PSC Module with Monolithic Interconnection P1,

P2, and P3 stand for first, second, and third laser scribing process. PET and c-TiO2 represent
poly(ethylene terephthalate) and compact-TiO2. ITO, c-TiO2, and spiro-MeOTAD can be replaced by
different TCO, oxide, and hole-transporting materials. Au can be also replaced by cheaper and more
efficient metal electrode materials.
light weight and versatility of applications due to the customized and integrated
devices.
In this part, we emphasize the module technology for the future developments of F-
PSCs. Although several papers have been published on the fabrication of large
sized F-PSCs using printing technology, their direct application to actual operating
devices has not been achieved. For the practical application of F-PSCs as power
sup plying devices for soft and conformal electronics such as those employed for
the internet of things (IoT) devices and sensors, the module technology, which
involves assembling multiple subcells, should be developed for boosting the power
to levels that would meet the minimum input powers of related electronics and
power storage systems. For this purpose, many subcells are generally interconnected
in a mono lithic form or a grid-type structure; the former is generally thought to be
more proper for F-PSCs due to the overall coating process and compatibility of the
layer mate rials.51 Through series interconnection, the parasitic resistive loss
originating from the series and shunt resistances could be reduced when the solar cells are enlarged.
Recently, there have been only a few reports on the F-PSC module.20,51,132,143
Bu et al.20 introduced a facile interface passivation strategy with potassium
treatment for the SnO2 ETL and demonstrated the fabrication of an F-PSC module
with a PCE of 15.22% and large size (5 3 6 cm2 ) using the slot-die printing method.
The po tassium treatments induced hysteresis-free, stable, and high PCE by
facilitating the growth of perovskite grains. Li et al.132 demonstrated a sequential
deposition method for the formation of pinhole-free CH3NH3PbI3 perovskite thin
films for the fabrication of F-PSC modules (active area of 16 cm2 ) with PCE over 8%.
Three scribing processes, referred to as P1, P2, and P3 scribing steps, are essential
for the fabrication of the monolithic interconnected module.51 As depicted in Fig
ure 13, the P1, P2, and P3 processes represent the isolation of the TCO between
cells, selective removal of the ETL/perovskite layer/HTL for the connection from the
top contact of the unit cells to the bottom TCO, and isolation of the top metal
electrode between neighboring cells, respectively. The patterned area for P1, P2,
and P3 belong to the dead area where power cannot be produced in the solar-cell
module. Conventionally, nanosecond lasers or mechanical scribing tools are widely
used for the P1, P2, and P3 processes. Rakocevic et al.144 compared mechanical
and laser patterning technologies for the fabrication of glass-based PSC module.
They found that the mechanical scribing is a reliable and relatively cost-effective
patterning technique, whereas the laser ablation can provide greater variability with
respect to substrates and layer materials. Further study is necessary to compare
the scribing technologies for the plastic-based F-PSC. Recently, Dagar et al.132
Joules 3, 1850-1880, August 21, 2019 1875

reported an F-PSC module with a 12 cm2 active area patterned with a laser that
exhibits a PCE of 8.8%. This F-PSC module was designed using three scribing steps
(P1, P2, and P3 scribing steps) based on an efficient, fully laser scribing procedure.
For the F-PSCs, especially on ITO-polymers, patterned lines are not as thin, sharp,
and clean as those for the glass-based PSCs, implying that the high performance of
unit cells in F-PSCs might not be reproducible in modules with a large area. There
fore, the scribing adaptability, as well as the high performances and large area pro
cessability, should be considered together.
Recently, intensive and extensive studies have been conducted on perovskite-based

tandem solar cells, and a PCE of 28.0% was achieved for the PSC/silicon tandem
cells.2 Owing to the considerable interest in PSC-based tandem devices, we predict
that flexible tandem devices such as flexible PSC/CIGS or flexible PSC/organic pho
tovoltaics (OPV) could be realized as future generation devices if new architectures,
materials, and processes are developed.
ACKNOWLEDGMENTS
This work was supported by the National Research Foundation of Korea (NRF)
grants funded by the Ministry of Science and ICT: NRF-2012M3A6A7054861, NRF
2014M3A6A7060583, NRF-2012M3A6A7054856, and NRF-2017R1A2B3010927
(Global Frontier R&D Program on Center for Multiscale Energy System);
NRF-2016M3D1A1027663 and NRF-2016M3D1A1027664 (Future Materials
Discovery Program); NRF-2018R1A2B2006708 (Research Program); and NRF
2015M1A2A2053004 and NRF-2015M1A2A2056827 (Climate Change Manage
ment Program).
AUTHOR CONTRIBUTIONS
H.S.J., M.J.K., and N.-G.P. perceived scientific challenges and recent efforts as the
flexible perovskite solar cell topics in this review article and wrote the manuscript.
G.S.H. revised the manuscript, collected permissions, and corrected typos.
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1880 Joules 3, 1850-1880, August 21, 2019

Flexible Perovskite Solar Cells

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Flexible Perovskite Solar Cells

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Introduction based on a plastic substrate. This

1850 Joule 3, 1850–1880, August 21, 2019 ª 2019 Elsevier Inc.

including flexible PSC/CIGS or flexible

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Figure 1. The Superiority of F-PSCs and Progress of PCE in F-PSCs/Module

high-performance flexible electronics. Many performances strongly depend on sub

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Optical Transmittance of Flexible Substrates and Electrical Conductivity of Flexible

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Table 1. Property Parameters for Polymer Substrate

Substrate PEN PET PI PC

Tg (C) 120–155 70–110 155–270 145

Tm ( C) 269 115–258 250–452 115–160

Density (g/cm3 ) 1.36 1.39 1.35–1.43 1.20–1.22

CTE (ppm/C) 20 15–33 8–20 75

Water absorption (%) 0.3–0.4 0.4–0.6 1.3–3.0 0.16–0.35

Solvent resistance good good good poor

Dimensional stability good good fair fair

Tm: melting temperature

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Figure 2. The Optical and Electrical Properties of TCOs

frequency of the collective oscillation of electrons in materials. The lp is generally

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Challenges in Uniform Coating Technology with a Large Area on Flexible

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PET AZO/Ag/AZO 81 7.5 PET/AZO/Ag/AZO/PEDOT: PSS/PolyTPD/MAPbI3/PCBM/Au 7 10

Ti foil/TiO2 BL/MP-TiO2/ MAPbI3/Spiro/Ag 0.77 39

Ti Foil Ag (12 nm)

Ti foil/TiO2 BL/MP-TiO2/ MAPbI3/Spiro/Ag 6.15 39

Ti Foil Ag (16 nm)

Ti foil/TiO2 BL/MP-TiO2/ MAPbI3/Spiro/Ag 3.85 39

Ti Foil Ag (20 nm)

Ti foil/TiO2 BL/MP-TiO2/ MAPbI3/Spiro/Ag 2.99 39

Ti Foil CNTs 60–80 –

Ti foil/TiO2 NTs+MAPbI3/CNTs+Spiro 8.31 40

This willow glass 81.5 31.3 MgF2/Willow glass/ITO/SnO2/ FAMACs/Spiro/MoOx/Al 17.3 43

Willow glass AZO 85.8 17.8 MgF2/Willow glass/ITO/SnO2/ FAMACs/Spiro/MoOx/Al 12.2 43

Willow glass IZO 76.4 11.6 MgF2/Willow glass/ITO/SnO2/ FAMACs/Spiro/MoOx/Al 18.1 43

DOG AZO/AgNW/ 88.6 at 550 nm 11.86 Au/Spiro/MAPbI3/ZnO/AZO/AgNW/AZO 11.23 44

PEN graphene ~97 552.0 PEN/Graphene/MoO3/PEDOT:PSS/MAPbI3/C60/BCP/LiF/Al 16.8 45

PET ITO 70 15 PET/ITO/PEDOT: PSS (VPAI 4083)/MAPbI3/PCBM/TiOx/Al 4.3 42

Glass ITO 80 8 Glass/ITO/PEDOT: PSS (VPAI 4083)/MAPbI3/PCBM/TiOx/Al 9 42

PET PEDOT: PSS – –

Cellulose MoOx/Au/MoOx 62.5 (top 9 paper/Au/SnO2/meso-TiO 2/CH3NH3PbI3/Spiro-OMeTAD/ 2.7 38

paper electrode) MoOx/Au/MoOx

High Moisture Permeability of Plastic Flexible Substrates

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Challenges in Super Flexibility

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thickness, and radius of curvature (bending radius), respectively. According to this

Recent Efforts on Improving Performance of Flexible Perovskite Solar Cells

The Exploitation of New Flexible TCO Substrates

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photovoltaic performance of F-PSC may change according to the electrical and op

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Figure 5. Metal-Polymer Hybrid Transparent Flexible Electrode

hole-conducting layer, which yielded 10.3% of PCE. Carbon-based nanomaterials

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Highly crystalline anatase nanoparticles may be directly deposited as ETL. However,

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Figure 7. New Composition ETLs