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Chang-Wen Chen, Hao-Wei Kang, Sheng-Yi Hsiao, Po-Fan Yang, Kai-Ming Chiang,
and Hao-Wu Lin*
Organometal halide perovskites (CH3NH3PbI3xClx and
CH3NH3PbI3) have recently attracted tremendous attention as
promising materials for solar energy conversion. The pioneer
devices demonstrated a power conversion efficiency (PCE) of
4%, as reported by Miyasaka and co-workers in 2009.[1] The
PCEs soon evolved to exceed 12% in a few years both in mesosuperstructure-type and planar-type cells.[212] The planar-type
device architecture is particularly interesting due to the simple
cell configuration and possible low-temperature fabrication on
flexible substrates. However, unlike meso-superstructure-type
devices, in which perovskite can be scaffolded by mesoporous
matrices, incomplete and non-uniform coverage of perovskite
films was usually observed in planar-type perovskite solar cells
and has been regarded as the major factor resulting in decreased
device performance.[1315] Many efforts have been made to control the morphology of perovskite thin films including optimization of the annealing time and temperature,[13,16] selection
of the under-layer material and thickness,[4,11,1719] and the use
of alternative deposition methods such as two-step deposition
and vacuum sublimation.[9,10,18,20] Among these methods, the
vacuum thermal co-evaporation of CH3NH3I and PbCl2 (or
PbI2) and the resulting perovskite thin films exhibited the most
homogeneous morphology and the highest thin-film coverage,
leading to a high performance of 1215% PCE.[6,8] Despite the
promising results, however, to date, only limited reports have
utilized this vacuum sublimation technique to fabricate perovskite layers.[6,8] The main reason could be due to the small
molecular weight of CH3NH3I, which results in a random diffusion of molecules inside the vacuum chamber and causes
difficulty with the monitoring and control of the CH3NH3I deposition rate using quartz microbalance sensors.[6,8]
In this paper, we demonstrate a novel method of perovskite
thin-film deposition via a layer-by-layer sequential vacuum sublimation. The process is relatively simpler than the co-evaporation technique; however, surprisingly, very uniform perovskite
thin films with high coverage can be produced. By incorporating these perovskite thin films with a poly(3,4-ethylenediox
ythiophene):poly(styrene sulfonate) (PEDOT:PSS) hole transporting layer and thermal evaporated C60/Bathophenanthroline (Bphen) electron transporting layers (ETLs), the cells with
C.-W. Chang, H.-W. Kang, S.-Y. Hsiao, P.-F. Yang,
K.-M. Chiang, Prof. H.-W. Lin
Department of Materials Science and Engineering
National Tsing Hua University
Hsinchu 30013, Taiwan
E-mail: hwlin@mx.nthu.edu.tw

DOI: 10.1002/adma.201402461

Adv. Mater. 2014, 26, 66476652

a simple device structure attain efficiencies as high as 15.4%

under simulated 1-Sun illumination. Because the devices are
free of high-temperature-prepared metal oxide layers and the
substrates are maintained under 100 C throughout the fabrication, the deposition method is suitable for a wide variety of
rigid and flexible applications.
The procedure of layer-by-layer sequential vacuum deposition is illustrated in Scheme 1. A simple one-material-at-a-time
deposition was used. First, PbCl2 films were thermally sublimed onto PEDOT:PSS-coated indium tin oxide (ITO) glass.
The surface morphology of the vacuum-deposited PbCl2 was
investigated by atomic force microscopy (AFM) and scanning
electron microscopy (SEM). The PbCl2 films were extremely
smooth with a root mean square roughness (Rrms) of 7.8 nm. As
illustrated in Figure 1a and Figure S1 in the Supporting Information, a nanocrystalline structure with 100 to 200 nm domain
sizes and full surface coverage can be observed. CH3NH3I was
then sublimed onto the PbCl2 layers. Upon CH3NH3I deposition, PbCl2 reacted with CH3NH3I in situ and formed perovskite thin films (CH3NH3PbI3xClx). The color of the thin film
gradually changed from transparent to a dark reddish-brown
appearance, as shown in Figure 1b. The thickness of the perovskite thin film was observed to be proportional to the thickness
of the PbCl2 layer with a ratio of ca. 2.9:1. A post-annealing process at 100 C in vacuum was applied for a short period (several
minutes) to fully crystallize the perovskite film and remove the
residual CH3NH3I on the surface.
The prepared perovskite layers were further capped with
layer-by-layer vacuum deposition of C60/Bphen ETLs and a
Ca/Ag cathode to complete the devices.[21] Note that we not
only utilized a simple device structure but also low-cost pristine organic compounds (C60, Bphen) to demonstrate their
commercial potential. All the layers (PbCl2, C60, Bphen, Ca,
and Ag) were fabricated with constant deposition rates, which
were monitored by quartz microbalance sensors, except for
CH3NH3I layer. The small-molecular-weight CH3NH3I makes
it difficult to accumulate the material onto the sensor head, and
random pulsation of the deposition rate was observed. This
observation partially explains the difficulty of controlling codeposition of PbCl2 (PbI2) and CH3NH3I to form a perovskite
film. Consequently, the CH3NH3I layers were deposited with a
constant source temperature of 85 C. Figure S2 in the Supporting Information shows the currentvoltage (JV) characteristics of perovskite solar cells of different PbCl2 thicknesses.
The samples were maintained at room temperature during the
entire vacuum sublimation process. It is clear that only the
devices with PbCl2 of less than 25 nm exhibit reasonable photovoltaic behavior. This result indicates that the reaction interface
area of PbCl2 and CH3NH3I is limited by the smooth surface of

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Efficient and Uniform Planar-Type Perovskite Solar Cells by

Simple Sequential Vacuum Deposition

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crystalline morphologies in these films.

The sample with the substrate temperature of 65 C exhibits a large domain size
of ca. 1 m, which is 10 times larger than
the crystal domain size of the seed PbCl2
layer. Two distinct layer structures are
also observed in the cross-sectional SEM
image. Only the upper part of the PbCl2
thin film reacted with CH3NH3I to form
the perovskite film, and the lower part of ca.
50 nm PbCl2 did not fully convert to the
highly crystalline perovskite. More intriguing
is that when the perovskite thin films were
prepared at the 75 C substrate temperature,
the crystalline structure fused together, and
fuzzy domain boundaries were observed.
The tilt-angle SEM image clearly illustrates
the long-range fusion of the perovskite
crystal domains all over the film (Figure 2g)
and Figure S4 in the Supporting InformaScheme 1. Schematic illustration of perovskite solar cells fabricated by sequential layer-by-layer tion). When the perovskite films were fabvacuum deposition.
ricated at a substrate temperature of 85 C,
vivid crystal domains reappeared but with
much smaller domain sizes of ca. 200 nm.
The films were further characterized by X-ray diffraction (XRD)
the vacuum-sublimed PbCl2 layer, leading to a reaction penetra(Figure 3a). For the sample with a substrate temperature of
tion depth equal to or less than 25 nm.
65 C, CH3NH3PbI3xClx signals were observed, while the
Intriguingly, we observed that the reaction penetration depth
can be extended by simply increasing the substrate temperature
signal intensities were weak. In addition, the pattern contains
while evaporating the CH3NH3I layer. Figure 2 and Figure S3
a small diffraction peak at approximately 15.7, which indicates the presence of CH3NH3PbCl3 (the CH3NH3PbCl3 (110)
in the Supporting Information show the morphology of perovskite thin films prepared from 150 nm PbCl2 seed layers at
diffraction peak).[8] However, for the substrate temperature of
higher substrate temperatures (6585 C). Similar to the vac75 C, a highly oriented pure orthorhombic CH3NH3PbI3xClx
uum-deposited PbCl2, full surface coverage can be observed in
crystal was obtained. Four clear diffraction signals are identified at 14.35, 28.70, 43.45 and 59.05, which can be assigned
all the perovskite films prepared at different substrate temperato the 110, 220, 330, and 440 peaks, respectively.[8] Interesting,
tures. All the films have smooth surfaces with Rrms values of
24.1 nm, 22.7 nm and 23.3 nm for substrate temperatures of
if the films were sublimed at a higher temperature (85 C),
65 C, 75 C and 85 C, respectively. The surface roughness is
regardless of the highly crystallized appearance observed in
much lower than that of the previously reported solution proSEM images, the crystallization was not as pure as the films
cessed films.[22] The smooth perovskite thin films can be attribwith substrate temperatures of 75 C. This finding could due
to the violent reaction of CH3NH3I and PbCl2 at the 85 C hot
uted to the ultra-smooth starting PbCl2 layer. Notably, even
with the same low surface roughness and full surface coverage
sample surface, which may impair the crystal quality, which is
characteristics in all the perovskite thin films prepared
not observed in the surface morphology but is clearly exhibat various substrate temperatures, we observe divergent
ited in the XRD patterns. The absorption spectra of these films

Figure 1. a) AFM image (30 m by 30 m) of the vacuum-deposited PbCl2 thin film. b) Photographs of the vacuum deposited PbCl2 (left) and perovskite
(right) thin films.

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promising photovoltaic performance by

incorporating the 75 C perovskite thin films
in the devices.
Figure 4 shows the JV characteristics of
150 nm PbCl2 (430 nm perovskite) devices.
The fabrication condition was kept the same
as for the above-mentioned cells. The only
control variables were the substrate temperature when the CH3NH3I layer deposition was
performed. The highest-performing device
was, as expected, fabricated at a 75 C substrate temperature. The cell delivered a shortcircuit current density (Jsc) of 20.9 mA/cm2,
an open-circuit voltage (Voc) of 1.02 V and a
high fill factor (FF) of 72.2%, leading to a very
high PCE of 15.4%. The efficiency is among
one of the highest PCE values reported in
vacuum-deposited perovskite solar cells,
which is particularly remarkable given the
simple layer-by-layer sequential fabrication
and the complete omission of costly organic
compounds and high-temperature processes.
The sample with the substrate temperature
of 65 C exhibits a kink in the JV curve and
a lower Jsc of 14.4 mA/cm2, which is caused
by the incompletely converted PbCl2 film
near the PEDOT:PSS interface. In contrast,
the device with the substrate temperature
of 85 C device exhibits kink-free characteristics but the lowest Jsc of 9.0 mA/cm2
and PCE of 4.5%. This result is quite surprising because the film exhibits similar
absorbance as the 75 C substrate temperature films. The poor crystallization could be
the main reason for the low efficiency. The
external quantum efficiency (EQE) spectrum of the 75 C sample exhibits a high
value of 80% across the entire 450 to 750 nm
wavelength range, indicating full absorption and efficient carrier extraction in the
430 nm-thick perovskite film. The smaller
EQE value of 6070% observed at ca. 400 nm
is due to the combination effect of the higher
Figure 2. ac) Cross-sectional and df) top view SEM images of the perovskite thin films reflection of the glass/air interface and the
fabricated at substrate temperatures of 65 C (a,d); 75 C (b,e); and 85 C (c,f). g) Tilt-angle higher absorption of ITO and PEDOT:PSS
SEM image of the perovskite thin film fabricated at 75 C substrate temperature (magnifica- at this wavelength. The integrated EQE over
tion: 4500).
AM 1.5G solar photon flux estimates a Jsc
of 20.3 mA/cm2, which is consistent with
the measured value obtained from solar simulators. Negliare presented in Figure 3b. The 430 nm-thick 75 C and 85 C
gible hysteresis of the JV characteristics was observed for
samples exhibit a similar high absorption in the entire ultrathe reverse and forward scan directions (see Figure S5, Supviolet to 750 nm wavelength range with absorbance values as
porting Information).[2327] The Jsc of cells with and without a
high as 0.745. The extremely high absorbance of >4 in the
blue to green wavelength range indicates a pinhole-free film
mask has been examined, and the difference was always less
quality. The 65 C thin film exhibits a much lower absorption,
than 3% (see Figure S6, Supporting Information). The high
which again confirms the incomplete formation of the perovsperformance of champion devices can be attributed to the
kite layer. With the combination of encouraging characteristics
continuous low-contamination vacuum deposition process
including full surface coverage, a large grain size, long-range
throughout the device fabrication, the good crystallinity, and
continuous and homogeneous thin-film morphology and a
the unusual continuous, homogeneous, and pinhole-free perhigh level of crystallization phase purity, one can anticipate
ovskite thin films.

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8x10

6x10

4x10
2x10

* (110)

(220)

4
2

85 C
o

65 C

10

20

30

20

30

40

2 ()

50

60

75 C

60

(b)

-4
-8
-12
-16
o

65 C
o
75 C
o
85 C

-20
-24

100

65 C
o
75 C
o
85 C

0.0

0.2

0.4

600

700

1.2

40

800

Figure 3. a) XRD patterns and b) absorbance spectra of ITO/

PEDOT:PSS/perovskite (430 nm) thin films fabricated at various substrate temperatures.

To further demonstrate the reproducibility of the sequential

vacuum deposition technique, 12 separate devices from 3 different batches were fabricated and measured using the optimized fabrication conditions (75 C substrate temperature,
430 nm perovskite). Figure S7 in the Supporting Information
and Table 1 show the histogram and the average performance,
respectively. All the parameters including Voc, Jsc, and FF were
highly reproducible with low variation. Impressive 3.5%, 2.1%,
5.7% and 5.9% relative standard deviations were observed for
Voc, Jsc, FF and PCE, respectively. The average PCE of ca. 14%
is also encouraging, which is only slightly lower than the best
PCE = 15.4% cell. The promising results demonstrate the great
advantage of this fabrication method in solar module production, of which sub-cells are series and parallel connected. Preliminary device stability results are shown in Figure S8 in the
Supporting Information. An encapsulated device was stored in
the dark and in ambient air at room temperature. The device
showed a good stability over three months and the PCE value
still remained at 86% of its initial efficiency.
Compared with previous vacuum co-deposition fabrications of perovskite layer,[6,8,28] both the sequential layer-by-layer

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1.0

60

500

0.8

(b)

65 C
o
75 C
o
85 C

20

400

0.6

80

EQE (%)

Wavelength (nm)

6650

70

(a)

Voltage (V)

Absorbance

50

(440)

(330)

40

2 ()

10

Current Density (mA/cm )

1x10

Intensity (Counts)

(a)

Intensity (counts)

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400

500

600

700

800

Wavelength (nm)
Figure 4. a) JV characteristics of perovskite solar cells fabricated at
6585 C substrate temperatures measured under 1 sun AM 1.5G illumination (solid lines) and in the dark (dashed lines). b) The corresponding
EQE spectra of the devices.

deposition method proposed in this study and co-deposition

of lead halide and methylammonium halide lead to pinhole-free perovskite films. However, the sequential vacuum
deposition approach possesses three distinct advantages:
i) It creates perovskite films with a much larger crystal domain
size (micrometer grain size versus tens of nanometers in the
co-deposition method), which may result in better carriertransport and carrier-diffusion properties; ii) the sequential
Table 1. Performance of solar cells in this work.
VOC
[V]

JSC
[mA/cm2]

FF
[%]

PCE
[%]

65 C

0.93

14.4

45.4

6.1

75 C (highest)a)

1.02

20.9

72.2

15.4

75 C (average s.d.)b)
85 C

0.98 0.03
1.13

20.8 0.4 68.6 0.04

9.0

44.6

13.9 0.82
4.5

a)The

highest performing device; b)The average and standard deviation (s.d.) of the
12 cells from 3 different batches processed at the 75 C substrate temperature.

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Experimental Section
Device and Thin-Film Preparation: The devices were prepared on
cleaned ITO substrates by spin coating a PEDOT:PSS (Clevios AI 4083)
thin film. Then, the substrates were loaded into a high vacuum chamber
(base pressure < 1 106 Torr) to evaporate PbCl2, CH3NH3I, C60,
Bphen, Ca, Ag thin films layer-by-layer. The substrates were kept at room
temperature, and all the layers (PbCl2, C60, Bphen, Ca, and Ag) were
fabricated with constant deposition rates except the CH3NH3I layer. The
substrates were controlled at specific temperatures (room temperature,
65 C, 75 C and 85 C), while the CH3NH3I layers were deposited with
a constant source temperature of 85 C. The devices were configured as:
glass substrate/ITO (145 nm)/PEDOT:PSS (30 nm)/CH3NH3PbI3xClx/
C60 (100 nm)/Bphen (6 nm)/Ca (1 nm)/Ag (120 nm). The devices were
encapsulated using a UV-cured sealant (Everwide Chemical Co., Epowide
EX) and a cover glass under an anhydrous nitrogen atmosphere after
fabrication and subsequently characterized in air.
Characterization: Perovskite thin films for SEM, AFM, XRD and
absorption measurements were prepared using the same fabrication
conditions as for the solar cells with layer structures configured as: glass
substrate/ITO (145 nm)/PEDOT:PSS (30 nm)/CH3NH3PbI3xClx. The
SEM images were obtained using a Japan Electron Optics Laboratory
Co., Ltd. (JEOL) JSM-7000F scanning electron microscope. The AFM
images were acquired using a Bruker Dimension Icon atomic force
microscope. The X-ray diffraction was performed using a Rigaku TTRAX
III instrument with Cu K radiation. The absorption spectra were

Adv. Mater. 2014, 26, 66476652

acquired using a SHIMADZU UV-2600 UVvis spectrophotometer. The

current density versus voltage (JV) characteristics of the devices were
measured using a Keithley SourceMeter 2636A in the dark and under
AM 1.5G simulated solar illumination with an intensity of 100 mW/cm2
(1 sun, calibrated by a NREL-traceable KG5 filtered silicon reference
cell). The ITO anode and the metal cathode were arranged in a cross-bar
geometry and the device area was determined by the overlap of the ITO
and the metal electrodes. Accurate device areas (ca. 0.05 cm2) were
measured device-by-device using a calibrated optical microscope. The
EQE spectra were acquired by illuminating a chopped monochromatic
light with a continuous-wave bias white light (from halogen lamp) on
the solar cells. The monochromatic light intensities were measured with
a NIST-traceable power meter (Ophir). The photocurrent signals were
then extracted using the lock-in technique using a current preamplifier
(Stanford Research System) followed by a lock-in amplifier (AMETEK).

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vacuum deposition method can be analogous to a two-step

solution process:[10,18,29] both sequential vacuum evaporation
and the two-step solution process decouple the disposition
of the reagent salts and offer an enhanced control over the
perovskite morphology by individual manipulation of the lead
halide and methylammonium halide deposition parameters;
iii) the sublimation temperature of CH3NH3I in high vacuum
(75 C) is much lower than that of lead halides, C60, organic
carrier transporting layers, and metals (all >250 C). Sequential layer-by-layer vacuum deposition offers the possibility of
dedicated chambers for each layer, which can minimize the
contamination issue of CH3NH3I resublimation when higherevaporation-temperature materials are evaporated.
In conclusion, we have developed a novel sequential layerby-layer vacuum sublimation method to fabricate planar-type
organometal halide perovskite solar cells. A clear fabricationcondition-morphology-device-performance correlation was
observed. The sublimed PbCl2 converted to perovskite in situ
upon CH3NH3I deposition, resulting in a uniform thin film
with unusual large-scale homogeneous crystalline structures
at an optimized substrate temperature. By sandwiching these
vacuum-deposited perovskite films between the anode and
vacuum sublimed electron-transporting layers and the cathode,
the simple device architecture delivered a remarkable performance of Voc = 1.02 V, Jsc = 20.89 mA/cm2, FF = 72.2% and
PCE as high as 15.4%. The cells also exhibited a promising
reproducibility with an average PCE of ca. 14% and a relative
standard deviation as small as 6%. We envision that the integration of a simplified device structure, simple layer-by-layer
fabrication, a low-contamination and highly homogeneous sub100 C vacuum process, low-cost raw materials and the compatibility of a matured mass-production infrastructure will make
this particular method a promising technology that brings perovskite solar cells a large step closer to commercial production.

Supporting Information
Supporting Information is available from the Wiley Online Library or
from the author.

Acknowledgements
The authors would like to acknowledge the financial support from
the Ministry of Science and Technology of Taiwan (1022221-E-007
125-MY3, 1012112-M-007017-MY3, 1022633-M-007002, 103-3113E-007-004) and the Low Carbon Energy Research Center, National Tsing
Hua University.
Received: June 3, 2014
Revised: July 18, 2014
Published online: September 1, 2014

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