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Efficient Charge Transfer and Fine-Tuned Energy Level
Alignment in a THF-Processed Fullerene-Free Organic Solar
Cell with 11.3% Efficiency
Zhong Zheng, Omar M. Awartani, Bhoj Gautam, Delong Liu, Yunpeng Qin, Wanning Li,
Alexander Bataller, Kenan Gundogdu,* Harald Ade,* and Jianhui Hou*
In polymer solar cells (PSCs) with bulk heterojunction (BHJ)[1]
structured active layers, fullerene- or non-fullerene-based
organic semiconductors can be used as electron acceptors to
generate a photocurrent with polymeric donors.[2,3] Great efforts
have been devoted to improve the power conversion efficiency
(PCE) of PSCs for decades.[1,4–6] Up to now, systematic investiga-
tions relating to the working mechanism and device engineering
have been performed mostly in fullerene-based PSCs.[7–9] In
recent years, with the rapid progress in the synthesis and use of
new non-fullerene-based acceptor materials, non-fullerene PSCs
have also showed great potential in achieving outstanding pho-
tovoltaic performance.[10–12] However, compared with fullerene-
based PSCs, detailed studies of the working mechanism (e.g.,
hole transfer dynamics) and processing methods related to
highly efficient non-fullerene PSCs are still lacking.
As is well known, the open circuit voltage (Voc) of a PSC is
dominated by the gap between the lowest unoccupied molec-
ular orbital (LUMO) level of the acceptor and the highest
occupied molecular orbital (HOMO) level of the donor,[13]
and the Voc can be improved by lowering the HOMO level
of the donor.[5,14,15] On the other hand, limited by the large
Coulombic attraction between the holes and electrons in exci-
tons, the molecular energy level alignments of the donor and
acceptor need to be fine-tuned.[13,16] Generally, for fullerene-
based PSCs, the HOMO and LUMO of the donor should be
higher than those of the acceptor and the ΔLUMO (difference
between LUMO levels of the donor and acceptor) and ΔHOMO
(difference between HOMO levels of the donor and acceptor)
should not be smaller than 0.2–0.3 eV.[13,16,17] In fact, these
requirements for the molecular energy level alignments have
Dr. Z. Zheng, D. Liu, Y. Qin, W. Li, Prof. J. Hou
Beijing National Laboratory for Molecular Sciences
Institute of Chemistry
Chinese Academy of Sciences
Beijing 100190, China
E-mail: hjhzlz@iccas.ac.cn
Dr. Z. Zheng, D. Liu, W. Li, Prof. J. Hou
University of Chinese Academy of Sciences
Beijing 100049, P. R. China
Dr. O. M. Awartani, Dr. B. Gautam, Dr. A. Bataller,
Prof. K. Gundogdu, Prof. H. Ade
Department of Physics and ORaCEL
North Carolina State University
Raleigh, NC 27695, USA
E-mail: kgundog@ncsu.edu; harald_ade@ncsu.edu
DOI: 10.1002/adma.201604241
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generally limited further improvement of Voc of fullerene-
based PSCs. For example, although Voc over 1 V could be real-
ized in fullerene-based PSCs, these devices often de­monstrated
relatively low short circuit current density (Jsc) and fill factor
(FF) due to the unfavorable molecular energy level align-
ments.[18,19] According to recent studies, over 10% PCE has
been achieved by utilizing the solar light within 800 nm (Eg
> 1.55 eV) in fullerene-based PSCs, but the Voc values are all
lower than 0.84 V.[6,20,21] Owing to the rapid progress of non-
fullerene acceptors for PSCs,[22,23] efficient non-fullerene-
based PSCs were successfully fabricated.[10,11,24] These results
demonstrate that non-fullerene-based PSCs are promising for
realizing high Voc[22,25–27] and also indicate that the require-
ments for molecular energy level alignment in non-fullerene
PSCs might be different from those in fullerene-based PSCs,
but this interesting topic has not yet been studied systemati-
cally. Specifically, prior studies on fullerene devices focused on
electron (ΔLUMO) transfer dynamics only, yet hole (ΔHOMO)
transfer dynamics is also very important for non-fullerene
acceptors due to their high optical absorption and substantial
contribution to the Jsc.
Here, we employed three custom-synthesized conjugated
polymers[28] named PBQ-0F, PBQ-QF, and PBQ-4F as donor
materials that are each blended with a non-fullerene acceptor
named ITIC[10] yielding a series of non-fullerene-based PSCs
(see Figure 1a,c). These three polymers possess similar
optical band gaps but different molecular energy levels. As
de­monstrated in Figure 1, both the HOMO and LUMO levels of
the polymers are tuned upon fluorination. As a result, blending
these polymers with ITIC, three non-fullerene-based active
layers with different molecular energy level alignments were
achieved. In detail, the ΔHOMO values for PBQ-0F:ITIC, PBQ-
QF:ITIC, and PBQ-4F:ITIC blends are 0.35, 0.19, and 0.04 eV
and the ΔLUMO values are 0.46, 0.32, and 0.24 eV, respectively.
Our results indicate that when these polymers are blended with
ITIC, we obtain systematically different device performances as
shown in Table 1. This is mainly due to the differences in Voc,
but Jsc and FF also contribute to the variation in PCE. There-
fore, these three BHJ blends offer a very useful model system to
investigate the correlations between the molecular energy level
alignments, performance, and device physics of non-fullerene-
based PSCs. Our results show that despite a small ΔHOMO of
0.04 eV in the blend of PBQ-4F:ITIC, efficient ultrafast charge
transfer (CT) occurs and the corresponding device exhibits low
germinate and bimolecular recombination, resulting in high
PCE over 11.3%.
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Figure 1.  a) Molecular structures of PBQ-0F, PBQ-QF, and PBQ-4F. b) Energy level schematic of PBQ-0F, PBQ-QF, PBQ-4F, and ITIC. c) Molecular
structure of ITIC.

In order to concisely demonstrate the molecular energy We found that the three polymers and ITIC could be easily
level alignments in the three BHJ blends and discern possible dissolved in many types of organic solvents such as chloro-
batch–to–batch variations, we measured the absorption spectra form, tetrahydrofuran (THF), toluene, and chlorobenzene,
by UV–Vis absorption spectroscopy and the HOMO levels of which indicates that any of these solvents could be used as
the three polymers and ITIC using electrochemical cyclic the primary processing solvent for making the active layers.
voltammetry(CV).[10,28,29] The optical band gaps of the polymers Since THF is a low toxicity solvent and also is biodegradable,
and ITIC are listed in Table S1 (Supporting Information). As the use of THF will not cause accumulative pollution to the
shown in Figure S1a (Supporting Information), the absorption environment. Therefore, THF was used as the processing sol-
edges (λedge) of the PBQ-0F, PBQ-QF, PBQ-4F, and ITIC are vent to make devices with an ITO/ZnO/BHJ/MoO3/Al archi-
729, 721, 693, and 790 nm, corresponding to the optical energy tecture. The PCEs of the devices are 2.02%, 3.97%, and 5.11%
gaps (Eg) of 1.70, 1.72, 1.79, and 1.57 eV, respectively. For the for PBQ-0F:ITIC, PBQ-QF-ITIC, and PBQ-4F:ITIC, respec-
polymer films, the fluorination is helpful for improving their tively (see Figure S3 and Table S4, Supporting Information).
extinction coefficient, and as a result, for the blend films, the Then, the photovoltaic performance of the devices was further
absorbance around 700 nm can be slightly improved, which optimized by selecting an appropriate solvent additive. We
may be beneficial to improve the external quantum efficiency found that for the three BHJ blends in this work, isopropanol
(EQE) and therefore higher Jsc. As shown in Figure S1b and (IPA), with a similar boiling point to THF, works very well
Table S1 (Supporting Information), the HOMO levels of the for optimizing photovoltaic performance of the devices. By
polymers and ITIC are calculated from the onset oxidation carefully screening the volume ratios of IPA (see Figure S3
potentials, and their LUMO levels were derived by subtracting and Table S4, Supporting Information), we found that the
their Eg from the HOMO values. In addition to CV measure- optimal photovoltaic performance can be obtained by using
ments, we also used ultraviolet photoelectron spectroscopy a 95:5, v/v mixture of THF:IPA. For example, the Jsc and FF
(UPS) to cross-validate the HOMO level values obtained from were improved simultaneously for the PBQ-4F:ITIC devices
CV measurements as shown in Figure S2 (Supporting Infor- after adopting 5% of IPA, and as a result, a PCE of 11.34 %
mation). While the absolute energy level values from the CV with Voc = 0.95 V, Jsc = 17.87 mA cm−2, and FF = 66.80% was
and UPS measurements are somewhat different, the trend is obtained. As shown in atomic force microscopy (AFM) and
similar. Therefore, as shown in Figure 1b, for PBQ-0F:ITIC, transmission electron microscopy (TEM) measurements
PBQ-QF:ITIC, and PBQ-4F:ITIC, the ΔHOMO values are 0.35, (Figure S4, Supporting Information), phase separation in the
0.19, and 0.04 eV, and the ΔLUMO values are 0.46, 0.32, and PBQ-4F:ITIC blend film can be slightly enhanced by adding
0.24 eV, respectively. 5% IPA.
As shown in Figure 2a and Table 1, the Voc of the devices
Table 1. Summary of parameters extracted from J–V and EQE charac- is directly proportional to the gap between the donor’s HOMO
teristics of PBQ-0F:ITIC, PBQ-QF:ITIC, and PBQ-4F:ITIC-based devices. and the acceptor’s LUMO.[5,28] It is worth noting that the PBQ-
4F:ITIC device shows a high Voc of 0.95 V, which is an out-
Voc Jsc FF PCE Jsca) (calculated) standing value for a PSC with an effective Eg < 1.6 eV, and as
[V] [mA cm−2] [%] [%] [mA cm−2] shown in Figure 2b,c, the EQE reaches over 70% in the spectral
PBQ-0F:ITICb) 0.69 16.16 59.91 6.68 16.47 range from 550 to 700 nm. The comparisons among the optical
PBQ-QF:ITICb) 0.83 17.16 62.49 8.90 17.24 density and EQE curves (see Figure 2b,c) indicate that the
PBQ-4F:ITICb) 0.95 17.87 66.80 11.34 17.73
increased extinction coefficients of the polymers by the fluorina-
tion effect play an important role in improving the EQE as well
PBQ-4F:ITICc) 0.95 18.20 65.01 11.24 17.54
as the Jsc of the devices. The current density values obtained
d)
PBQ-4F:ITIC 0.95 17.83 65.35 11.07 17.31 from integrating the EQE curves and the standard solar spec-
a)The J calculated from EQE data of optimized devices; b)Device is fabricated in a trum are shown in Figure 2b, these values are consisted with
sc
glove box filled with nitrogen; c)Device architecture: ITO/PEDOT:PSS/PBQ-4F:ITIC/ the Jsc data obtained from the current density–voltage (J–V)
PFN-Br/Al; d)Device is fabricated in ambient air. measurements, indicating the measurements are reliable.

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Figure 2.  a) Current density–voltage characteristics (J–V characteristics) and b) EQE characteristics of devices based on PBQ-0F:ITIC, PBQ-QF:ITIC,
and PBQ-4F:ITIC. J–V characteristics were operated under standard AM 1.5G solar illumination. c) Absorptions of PBQ-0F:ITIC, PBQ-QF:ITIC, and
PBQ-4F:ITIC blend films with thicknesses of 100 ± 3 nm.
The high PCE of the PBQ-4F:ITIC-based PSCs can be
easily reproduced with a small statistical spread. As shown in
Figure S5 and Table S3 (Supporting Information), the average
PCE of the 50 cells fabricated from one batch are 11.03 ± 0.16%.
We also used a normal architecture of ITO/PEDOT:PSS/active
layer/PFN-Br[30]/Al to make the device. As shown in Figure S1
(Supporting Information), by employing such a device struc-
ture, the best PCE reached 11.24%. Moreover, we fabricated
inverted devices under ambient atmosphere and found that
the photovoltaic performance of the PBQ-4F:ITIC-based PSCs
could be reproduced, for example, the best device yields a PCE
of 11.07%.
To better understand the observed differences, as shown in
Figure S9 and Table S5 (Supporting Information), hole and
electron mobilities of the three blend films were measured
using the space–charge–limited–current (SCLC) method.[31]
The hole mobility of PBQ-4F:ITIC was 1.0 × 10−3 cm2 V−1 s−1,
which was higher than PBQ-0F:ITIC (7.8 × 10−4 cm2 V−1 s−1)
and PBQ-QF:ITIC (8.6 × 10−4 cm2 V−1 s−1). On the other hand,
the electron mobility of PBQ-4F was 1.0 × 10−3 cm2 V−1 s−1,
which was higher than PBQ-0F:ITIC (8.2 × 10−4 cm2 V−1 s−1)
and PBQ-QF:ITIC (8.3 × 10−4 cm2 V−1 s−1).
In order to characterize the molecular packing and texture
of the samples, grazing incidence wide-angle X-ray scattering
(GIWAXS)[32] measurements were carried out. All samples
were prepared under the same conditions used in device fab-
rication. As shown in Figure S6a–c (Supporting Information),
the three neat polymers exhibit very similar scattering profiles
with preferential face-on packing and similar peak location for
laminar (100) and π–π (010) stacking of qxy = ≈0.27 Å−1 and
qz = ≈1.75 Å−1, respectively, which correspond to a d-spacing
of ≈23 and ≈3.5 Å, respectively. The 2D GIWAXS data set for
the neat ITIC film exhibits, a relatively isotropic stacking in the
(100) and the (010) directions (Figure S6d, Supporting Infor-
mation), with a weak face-on packing orientation. After being
blended with ITIC, the chain packing features of the blends
are similar to those of the neat polymers (Figure 3a–c). The
out–of–plane (OOP) integrated π–π intensity for the PBQ-
QF:ITIC and the PBQ-4F:ITIC is 30% and 45% larger than
the PBQ-0F:ITIC intensity, respectively. FF and Jsc are plotted
against this parameter in Figure 3d and exhibit good correla-
tions. For peak fitting details and lineouts consult Figure S7a–d
(Supporting Information). The (010) peak intensity is indicative
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of the ordered polymer population with a preferential face-on
stacking orientation. Such orientation is often beneficial for
efficient charge transport and collection out of the device.[33]
Therefore, PBQ-4F:ITIC has the most beneficial packing and
texture, consistent with its high performance.
To further investigate the morphology of the different blends,
they were characterized with resonant soft X-ray scattering
(R-SoXS) at several different photon energies between 270 and
290 eV to quantify the in–plane composition variations over
length scales ranging from ≈10 to ≈1000 nm (Figure S8a, Sup-
porting Information).[34,35] The fitting results of the 284.2 eV
data with two log-normal distributions (Figure S8b–d, Sup-
porting Information) show that PBQ-0F:ITIC, PBQ-QF:ITIC,
and PBQ-4F:ITIC reveal relatively similar characteristic domain
spacings of 16, 12, and 15 nm, respectively, from the dominant
peak at high q. The domain size is approximately equal to ½
of the characteristic domain spacing, resulting in domain sizes
of 8.0, 6.0, and 7.5 nm, respectively. A minor low q peak with
10% of the scattering intensity yields spacings of 67, 49, and
59 nm, respectively (Table S6, Supporting Information). This
reveals that the smallest domains dominate the morphology in
all three blends. While characteristic spacings have been pre-
viously correlated to photocurrent,[36] the domain spacing for
the three blends here does not show large and systematic vari-
ation. Furthermore, the spacing is very small and corresponds
to domain sizes smaller than a typical exciton diffusion length.
Therefore, the variations observed are not expected to have a
significant influence on the relative device performance. More-
over, following established procedure, the relative average com-
position variations, which relate to domain purities, are deter-
mined to be 1.0, 0.93, and 0.93 for PBQ-0F:ITIC, PBQ-QF:ITIC,
and PBQ-4F:ITIC, respectively. Although, previously related to
FF,[10] the composition variations are small and inconsistent
and do not play a major role in determining the FF of our three
devices. This indicates that, morphologically, the OOP π–π
intensity is the likely dominant factor impacting FF and Jsc,
controlling the hole mobility in the films and thus charge crea-
tion and extraction.
In order to relate the underlying photophysics to device per-
formance, we performed femtosecond transient absorption
spectroscopy (TAS). In these measurements, the pump excita-
tion was tuned to 1.7 eV (730 nm) to selectively excite the ITIC
acceptor (Figure S1a, Supporting Information). The resulting
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Figure 3.  2D GIWAXS data sets for blend films. a) PBQ-0F:ITIC, b) PBQ-QF:ITIC, and c) PBQ-4F:ITIC. d) Thickness and background-normalized
out–of–plane line cut profiles for the (010) peak for all three blends. e) Photovoltaic device performance parameters, (i) Jsc and (ii) FF, versus out–
of–plane (010), that is, π–π stacking, peak area for each of the device blends from fits that include a function for the amorphous background (see the
Supporting Information).

polaron and exciton dynamics are measured using a broad-
band probe pulse in the near IR region. Since initial excitons
are only created in the acceptor domains, the resulting polaron
dynamics directly report the hole transfer from the acceptor to
the donor. The photoinduced absorption (PIA) signature of the
hole polaron in the polymer and the singlet exciton PIA feature
in the ITIC are, however, located in the same spectral region
(1.0–1.5 eV) centered ≈1.28 eV (Figure S10, Supporting Infor-
mation). Although there is significant spectral overlap, it is pos-
sible to differentiate these two species as they have significantly
different lifetimes. ITIC excitons have a lifetime of only about
8 ps, whereas polarons survive for longer than 5 ns (the longest
time window available in the experiment).[37,38] Figure 4a shows
the time evolution of the 1.28 eV PIA signal in both neat ITIC
and the blends with selective ITIC excitation at 1.7 eV. These
transients reflect exciton recombination in the ITIC and the
charge generation and relaxation dynamics in the polymer.
The early decay is nearly the same in all samples, indicating
it is mostly dominated by exciton depletion dynamics, which
is the same in all three blends. Although it is not possible to
completely isolate the early polaron dynamics, the subtrac-
tion of the ITIC transient from that of the blends (Figure 4b)
provides a good approximation. This resulting time evolution
of the polaron exhibits a similar rise in all three blends with
characteristic times for PBQ-0F:ITIC, PBQ-QF:ITIC, and PBQ-
4F:ITIC of 16.6, 19.3, and 19.6 ps, respectively. This indicates
that all three blends are similarly efficient for hole transfer
from acceptor to donor polymer.
In contrast to the charge creation, the decay dynamics of the
three blends are different. The characteristic decay times are
16.4, 14.4, and 8.03 ns for PBQ-0F:ITIC, PBQ-QF:ITIC, and
PBQ-4F:ITIC, respectively. In a biased device, high mobility
leads to efficient extraction of charges, which reduces the bimo-
lecular recombination rate. In contrast, without bias, more
mobile holes can more rapidly find an electron to recombine.
The fast decay of the polaron population in the PBQ-4F:ITIC
is thus likely due to a high local mobility of charges (charges
are not extracted in our measurement) and controlled by bimo-
lecular recombination. This is, in general, consistent with
the observed mobilities, WAXS, and FF, although the TAS is
dominated by local mobilities, whereas the devices are likely
impacted mostly by the global mobility as measured in SCLC.
Importantly, even though the ΔHOMO is only 0.04 eV in
PBQ-4F:ITIC, the ultrafast TAS measurements show that
hole transfer is efficient and is comparable with the polymer
blends with high ΔHOMO, that is, 0.35 eV for PBQ-0F:ITIC

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Figure 4.  Time evolution of a) ITIC, PBQ-0F:ITIC, PBQ-QF:ITIC, and PBQ-4F:ITIC films monitored at 1.28 eV and b) hole transfer dynamics for three
blends. Excitation energy is 1.7 eV.
and 0.19 eV for PBQ-QF:ITIC. Our results indicate that charge
generation can be very efficient in the polymer:non-fullerene
blends even with very low ΔHOMO. We suggest a reasonable
mechanism for the interesting phenomenon as following. For
the blend of a polymer donor and a fullerene acceptor, the
ultrafast charge transfer occurs due to the π-orbital overlap-
ping between the donor and the acceptor which is also known
as the formation of charge transfer state, and the driving force
for the ultrafast charge transfer originates from the variation in
the π-electron densities of the donor and the acceptor. However,
according to the chemical structure of ITIC, we can see that
the di-cyano-substituted end groups have strong electron with-
drawing effect and these end groups are also not surrounded by
non-conjugated segments, so when these end groups approach
the electron-enriched backbone of the polymer donor, the
strong dipole effect of the end groups may facilitate the charge
transfer process and also prevent the bimolecular recombina-
tion. However, determination of the energetic disorder and the
energy of the CT state by photothermal deflection spectroscopy
or sensitive EQE/electroluminescence measurements are nec-
essary to fully understand why PBQ-4F:ITIC blends exhibit effi-
cient charge generation even with such a small energy offset
(0.04 eV). Such complex characterization is outside the scope
of this work.
In conclusion, we investigated a series of non-fullerene-based
PSCs based on the non-fullerene acceptor ITIC and three con-
jugated donor polymers with similar chemical structures but
varied molecular energy levels. The results show that although
the HOMO level of PBQ-4F is only 0.04 eV higher than that
of ITIC, the device based on PBQ-4F:ITIC can still yield high
EQE over the whole spectral response range, implying that
the excitons generated in both the donor and acceptor can be
efficiently separated into free charges and then collected by
the electrodes. This nearly identical charge generation was
explicitly verified with TAS for the formation of free holes. We
surmise that such small offset without detrimental impact is
likely related to the tendency of ITIC and other small molecular
acceptors to form CT states with lower energetic disorder than
fullerene devices,[39,40] although explicit systematic studies are
required to fully elucidate the underlying cause. Moreover, our
results show that the polymer with more fluorine tends to form
stronger inter-chain π–π interaction when it is blended with
ITIC, which is helpful for efficient charge transport. As a result,
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COMMUNICATION
due to the combination of morphology control and electronic
structure tuning, the PBQ-4F:ITIC-based PSCs that were fabri-
cated by an environmental friendly solvent mixture yield a high
PCE of 11.34% with a high Voc of 0.95 V.
Supporting Information
Supporting Information is available from the Wiley Online Library or
from the author.
Acknowledgements
The authors acknowledge the financial support from the National
Natural Science Foundation of China (Nos. 91333204 and 21325419)
and the Strategic Priority Research Program of the Chinese Academy of
Sciences (XDB12030200). The X-ray characterization by O.M.A. and H.A.
at North Carolina State University (NCSU) was supported by a UNC-GA
Research Opportunity Initiative grant. Transient absorption spectroscopy
work at NCSU (B.G., A.B., and K.G.) was supported by the Office of
Naval Research (ONR) Grant No. N000141310526 P00002. A. Hunt,
J. Carpenter, C. Zhu, E. Schaible, M. Brady, and C. Wang are
acknowledged for assisting with the measurements and maintaining the
instruments. Z.Z., O.M.A. and B.G. equally contributed to this work.
Received: August 8, 2016
Revised: October 13, 2016
Published online:
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