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Fast P3HT Exciton Dissociation and Absorption
Enhancement of Organic Solar Cells by
PEG-Functionalized Graphene Quantum Dots
Travis G. Novak, Jungmo Kim, Sung Ho Song, Gwang Hoon Jun, Hyojung Kim,
Mun Seok Jeong, and Seokwoo Jeon*
In recent years, organic photovoltaic (OPV) devices have
attracted much research attention due to their potential
for low-cost, flexible, and environmentally friendly solar
power.[1–3] Although significant progress has been made, a
fundamental issue is the trade-off between optical density
and charge transport. To this end, various active-layer addi-
tives have been researched, including metal nanoparticles,[4]
inorganic semiconducting quantum dots,[5] and carbon
nanotubes.[6] However, these devices have significant draw-
backs, such as increased fabrication complexity, toxicity, and
expensive raw materials.
As an alternative, graphene quantum dots (GQDs) pro-
vide tunable energy gaps, good chemical stability, and easy
dispersion in a wide variety of organic solvents,[7–9] making
them potentially attractive in organic solar applications. Pre-
vious research has demonstrated the potential of using GQDs
as an active layer material in OPV.[10–13] The positive effects of
functional groups have also been studied to improve the inter-
action between graphene and other organic layers.[10,13–15]
Although GQDs have been shown to increase solar
efficiency, for designs where GQDs are blended with other
donor/acceptor materials, the mechanism of enhancement
is still unclear. Proposed effects include decreased series
resistance, increased active layer absorption, improved mor-
phology, and optical scattering by GQDs.[11–13] Although
these descriptions hold merit and are not necessarily mutually
exclusive, there is still insufficient explanation regarding the
role of GQDs in OPV. Most notably, an absorption increase
is consistently reported in longer wavelength regions, where
GQDs in this size range are almost entirely transparent.
Therefore, to form a more comprehensive explanation, an
investigation into the relationship between GQD-induced
charge-transfer kinetics and P3HT absorption is needed.
T. G. Novak, J. Kim, Dr. S. H. Song, G. H. Jun, Prof. S. Jeon
Department of Materials Science and Engineering
Korea Advanced Institute of Science and Technology
Daejeon 305-701, South Korea
E-mail: jeon39@kaist.ac.kr
H. Kim, Prof. M. S. Jeong
Department of Energy Science
Sungkyunkwan University
2066, Seobu-ro, Jangan-gu, Suwon, Gyeonggi-do 440-746, South Korea
DOI: 10.1002/smll.201503108
small 2015, © 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
DOI: 10.1002/smll.201503108
Organic Solar Cells
To better elucidate the effects of GQDs, we pre-
pared high-quality GQDs through graphite intercalation
compounds (GICs). Although several other methods exist
to make high-quality GQDs, including unzipping C60 mole-
cules,[16] hydrothermal cutting,[17] and electron beam litho-
graphy,[18] these methods are complex and unsuitable for
mass-production. Because of this, research into GQD-OPV
designs has generally focused on GQD production from
reduced graphene oxide (rGO), which is economical and
scalable, but leaves numerous oxygenous groups and defects
even after reduction. As an alternative, production from
GICs is a simple, scalable, and environmentally friendly
method for producing high-quality GQDs with high yield
(<60%) and fewer in-plane defects.[19,20] Because of its higher
quality, graphene produced through intercalation compounds
has been shown to be superior to rGO in various applications.
In this work, we have produced improved P3HT:PCBM
solar cells through the addition of GQDs functionalized with
various molecular weights of polyethylene glycol (PEG).
Functionalization with low molecular weight PEG was shown
to significantly improve the GQD interaction with the active
layer, resulting in improved PCE over both reference cells
and cells produced with pristine GQDs. The mechanism of
enhancement was shown to be faster P3HT exciton dissocia-
tion in GQD-containing cells, which results in an absorption
improvement in the visible range due to fewer bound charges
remaining in P3HT. This was proven through production of
P3HT and PCBM thin films and subsequent analysis with
UV–vis and TA-spectroscopy.
Figure 1a shows a drawing of the PEG-functionalized
GQDs. The PEG chain likely attaches to the GQD via amine
bond. Three different molecular weights of PEG functionali-
zation were studied: 200, 1000, and 3000, and were designated
200PEG-GQD, 1000PEG-GQD, and 3000PEG-GQD. A
TEM image of the 200PEG-GQDs is seen in Figure 1b. Like
the pristine GQDs, the functionalized GQDs have a tight
size distribution, with no change in lateral size observed after
functionalization. In addition, the crystallinity can clearly be
seen in the inset image, with the measured lattice param-
eter. AFM scans show that while 200PEG-GQDs appear
similar to pristine GQDs (Figure 1c), functionalization with
longer chains (Figure S1, Supporting Information) signifi-
cantly increases GQD height. This thickness increase may
be a product of chain wrapping around the GQD or some
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Figure 1. Morphology of PEG-GQDs. a) Drawing of GQD with various lengths of PEG chains drawn to scale. b) TEM image of 200PEG-GQDs with insets
showing the lattice parameter measurement and diffraction pattern. c) AFM image showing 200PEG-GQDs and inset line scan indicating heights.

functionalization in the basal plane. The functionalization
of GQDs improves their distribution in chlorobenzene, and
potentially improves charge transfer between the GQDs and
P3HT.
Figure 2a illustrates the FTIR spectra after functionali-
zation. By overlaying, we see that the C-C peak (1524 cm–1)
is not altered and the C–O band at (1724 cm–1) is minimal,
proving the low oxidation state of the dots. The C–O–C bond,
not seen in pristine GQDs, appears prominently after func-
tionalization and increases with increasing chain length. The
Raman spectra in Figure 2b show a slight shift of both D and
G peaks for all PEG-functionalized GQDs. This G-peak shift
is often characteristic of n-doping in graphene,[21,22] indi-
cating that PEG may have electron-donating properties when

Figure 2. Characterization of PEG-GQDs. a) FT-IR spectra showing C-O-C bond increase with increasing MW of PEG. b) Raman peaks with shift after
functionalization. c) UV–vis absorption in DI-water, with inset showing π–π* shoulder peak at 260 nm. d) PL properties at 325 nm excitation.

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Table 1. Full solar performance parameters. Six devices were tested for
each design

Jsc Voc Fill factor [%] Efficiency

Reference 12.0 ± 0.3 0.52 ± 0.01 48.1 ± 0.6 3.00 ± 0.08
GQD 13.4 ± 1.0 0.46 ± 0.02 39.7 ± 2.0 2.45 ± 0.42
200PEG-GQD 13.8 ± 0.5 0.55 ± 0.01 54.2 ± 0.9 4.10 ± 0.04
1000PEG-GQD 12.2 ± 0.4 0.50 ± 0.01 48.5 ± 2.3 2.98 ± 0.17
3000PEG-GQD 8.2 ± 0.9 0.30 ± 0.02 27.6 ± 4.0 0.81 ± 0.11

proves that the absorption increase in the active layer is not

due to absorption at the GQDs or the functional groups. In
addition, the PL intensity of GQDs is found to not corre-
late with absorption either, indicating that emission from the
Figure 3. Device performance. Current density–voltage (J–V) properties
of devices with various types of GQDs and comparison to the reference GQDs and subsequent reabsorption in the active layer (down-
cells. Inset shows the basic device design. conversion) is not the dominant mechanism either. We also
note that the absorption above 650 nm appears to be slightly
functionalized. As seen in Figure 2c, the absorption spectrum reduced after GQD addition. In the case of metal nano-
is only slightly modified by functionalization, and all GQDs particles, where optical field effects play a dominant role in
have minimal absorption in the visible range. However, the absorption increase, the enhancement is seen throughout
the PL of the GQDs (Figure 2d) in solution is significantly the spectrum.[4] Therefore, it is clear that the absorption effect
increased by functionalization, with the PL intensity of GQDs is not simply a product of optical scattering.
increasing with PEG chain length. We have previously con-
firmed that this extrinsic PL emission in the long wavelengths
is a product of charge-transfer to the edges of GQDs.[19]
Figure 3a shows the IV curves of the produced devices
and an inset showing the device layers. At least six cells were
produced for each design, and the full device parameters
are summarized in Table 1. To ascertain the effect of func-
tional groups, the GQD concentration was held constant at
0.025 mg mL−1. The addition of pristine GQDs is not shown
to improve overall efficiency, as the short circuit current (Jsc)
increases but fill factor (FF) and open circuit voltage (Voc)
are degraded. Similar behavior was previously reported
with unmodified rGO flakes.[21] Because pristine GQDs pro-
duced through this method have minimal oxidation and edge
functional groups, it is likely that very few edge sites exist
to facilitate exciton dissociation from organic layers. Other
works have shown that various edge functional groups can be
beneficial for extracting bound charges from P3HT, and thus
solar performance.[10,14,15]
For functionalized GQDs, increasing PEG chain length is
shown to significantly degrade performance, and a clear trend
is seen with Jsc and Voc. This may be due to chain wrapping of
the longer PEG chains around the GQD, or PEG interfering
with donor/acceptor domain formation. Peak performance
was achieved with the shortest chain (200 MW), and the
PCE of the best device was 4.24%, compared to 3.05% for
the best reference cell. The devices also showed outstanding
consistency, with all six cells of this design showing a PCE
>4%. The improvement mostly originates from an increase in
Jsc and FF, although some Voc increase may be attributable to
decreased recombination.
Figure 4a shows that absorption of the films generally
improves in the visible range with the addition of GQDs.
However, we note that the effect is not consistent throughout Figure 4. Active layer absorption. UV–vis on P3HT:PCBM thin films with
the spectrum, and that the range of improvement appears a) various types of GQDs added and b) normalized absorption peaks
where GQDs were shown to be transparent in solution. This showing a redshift with functionalization decreasing chain length.

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By normalizing peaks in the visible range, it can be seen [25]

that the visible peaks slightly redshift (Figure 4b) a result
that has been previously reported in P3HT:PCBM blends
containing GQDs and in CNTs.[6,11] This has been attrib-
uted to increased electron delocalization in the P3HT chain.
In addition, the shoulder peaks at 550 and 600 nm become
more prominent in GQDs with short chain PEG. Previous
work involving GQD or CNT addition has demonstrated that
the absorption improvement in longer wavelength regions
correlates with improved EQE in approximately the same
spectral ranges.[12,23,24] We assert that shorter PEG chains
induce faster exciton dissociation from P3HT, leading to a
stronger electronic effect in the active layer and progressively
better absorption in this region.
To elucidate the effects of the functionalized GQDs, we
prepared thin films based on the constituent active layer
materials and analyzed the absorption spectra. By doing this,
we can rule out more complex effects such as P3HT-PCBM
domain alignments, charge-transfer excitons, and potential
interactions with other OPV layers. Figure 5a shows that the
GQDs have no significant effect on the PCBM thin film, and
the blend shows minimal absorption in the longer wavelength
(>450 nm) regions. This also indicates that the absorption of
GQDs in the film is minimal, an intuitive result given the
extremely low loading-level and insignificant absorption by
GQDs in the visible region. By contrast, addition of GQDs
into P3HT thin films dramatically increases the absorptivity
(Figure 5b), but there is no observed redshift in the peaks.
This is because the addition of PCBM or other acceptor mol-
ecules has been known to blueshift the absorption peak in
P3HT. In the P3HT:PCBM blend, the absorption peak is
≈475 nm, so additional absorption in the 510 nm range results
in a redshift. However, in pristine P3HT, no shift occurs
because the absorption peak is already located in this range.
The stark difference between the GQD effects on P3HT
and PCBM indicates a unique electronic interaction rather
than a simple mechanism such as scattering or absorption at
the GQDs, providing further evidence of our proposed fast
exciton dissociation mechanism.
To better illustrate the role of GQDs in P3HT thin films,
we normalized the absorption spectra relative to pristine
P3HT by subtracting the absorption values of the GQD-
P3HT blend from that of the pristine P3HT film. As seen
in Figure 5c, the absorption improvement peaks at 509 nm.
This peak corresponds to 0–2 transition, and is observed in
transient absorption spectroscopy as being particularly sen-
sitive to charge kinetics.[25–27] An additional shoulder can be
seen for the 0–1 transition at ≈550 nm, and the very promi-
nent shoulder at ≈600 nm corresponds to the 0–0 transition.
The absorption in this range (<620 nm) is characteristic of
the ground state bleach (GSB), where excitons in the bound
state prevent additional absorption from incoming photons.
In cells with GQDs, we propose that this effect is lessened
due to improved exciton dissociation. With fewer excitons
remaining in the bound state, more electrons are available in
the ground state to absorb the incoming photon, and there-
fore the absorption in this range is increased.
In pristine P3HT, the corollary photo-induced absorption
(PIA) effect is widely reported to begin at 620 nm and
peak at 660 nm.[26–28] If exciton dissociation is faster in

Figure 5. Evidence for fast exciton dissociation. UV–vis absorption of a) PCBM and b) P3HT thin films with 2000PEG-GQDs added. c) Absorption of
the 200PEG-GQD+P3HT thin film subtracted from P3HT. The regions seen in transient absorption spectroscopy are indicated with shoulder peaks
corresponding to P3HT modes labeled. d) Transient absorption decay with probe at 600 nm and extracted time constants. Inset is an illustration
of the electron diffusion path based on the LUMO energy levels.

4 www.small-journal.com © 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim small 2015,
DOI: 10.1002/smll.201503108
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GQD-containing P3HT thin films, the absorption in this
region is expected to be less than that of pristine P3HT. As
seen in Figure 5c, the peak is found in the expected range,
and the PIA region boundaries are near the reported range
as well. Beyond 725 nm, the relative absorption again
becomes positive, which may be a product of stimulated
emission (SE) effect observed in this region.[26,29] This cor-
relation between absorption and exciton dissociation directly
explains the observed trends in both our results and in pre-
vious works. In P3HT-based blends, many papers have shown
these same improvements in long-wavelength regions, but
have also observed a subtle decrease in absorption beginning
at ≈620 nm.[6,11] Because fewer bound states will decrease
absorption in this region, our proposed mechanism perfectly
explains this trend.
To confirm this mechanism, we performed transient
absorption spectroscopy with a 470 nm pump pulse and a
probe set at 600 nm, corresponding to the 0–0 mode. As seen
in the normalized profiles (Figure 5d), the decay for P3HT
blended with 200PEG-GQD is clearly faster. By fitting the
profile, slow and fast decay constants were revealed. 200PEG-
GQD addition had a particularly dramatic effect on the slow
decay constant, which was reduced by over half (26.10 to
12.25 ps) in comparison to pristine P3HT. The inset shows
the band diagram for the solar cells. For PEG-functionalized
GQDs, we determined the LUMO to be ≈3.3 eV by cyclic
voltammetry (Figure S2, Supporting Information). This level
is in line with many previously reported values for GQDs,
which range from 3.2 to 3.6 eV,[10,30,31] and it sits between
the LUMO levels of P3HT and PCBM. The graphene-P3HT
interface is known to promote fast electron exchange,[32]
so the rapid transfer of bound electrons from the LUMO
of P3HT to the GQD is likely the mechanism by which the
exciton dissociates.
Additional evidence of exciton effects of GQDs is seen
in the supporting information. Owing to the previously dis-
cussed charge transport mechanisms, the GQDs function-
alized with 200PEG dissociate excitons most efficiently,
and the normalized features because less pronounced with
pristine GQDs or 3000PEG-GQDs (Figure S3, Supporting
Information). Overall, the near perfect alignment of rela-
tive absorption features to those seen in transient absorption
spectroscopy and faster decay profiles are powerful evidence
for faster exciton decay in GQD-P3HT blends. Furthermore,
we note that the GSB has already been shown to play a large
role in P3HT absorption,[33] and it is known that tailoring
the charge transfer kinetics of P3HT-based devices can sig-
nificantly impact overall solar efficiency.[34,35] Therefore, we
can confidently attribute the absorption increase in the active
layer to this electronic effect.
We also investigated potential morphological changes to
the active layer by performing AFM analysis on P3HT:PCBM
thin films (Figure S4, Supporting Information). We observe
no clear trend in surface roughness depending on GQD type,
and all films are reasonably smooth and uniform. However,
the phase images show that while both the reference film
and 200PEG-GQD films have smooth and continuous phase
separation, the films produced with longer chain PEG-func-
tionalization show larger and more clump-like domains. This
small 2015, © 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
DOI: 10.1002/smll.201503108
poor phase separation may explain why the 3000PEG-GQD
cells perform poorly despite strong absorption in the visible
region.
In conclusion, we reported a 36% improvement in effi-
ciency of P3HT:PCBM solar cells through insertion of
PEG-functionalized graphene quantum dots. We revealed
a significant improvement in active layer absorption, and
attributed the increase to faster P3HT exciton dissociation
through use of UV–vis analysis and TA-spectroscopy. This
result has important implications for not only future GQD-
OPV designs, but also for other active layer additives.
Experimental Section
Fabrication of PEG-Functionalized Graphene Quantum Dots:
GQDs were fabricated through GICs by a previously reported
method.[19] In a typical reaction, 30 mg of graphite powder was
mixed with 450 mg of sodium potassium tartrate and reacted in a
glovebox for 24 h at 250 °C. The resulting GIC was then dispersed
in water and filtered to produce small GQDs (>5 nm) of 1–3 layers.
Dialysis was then used to remove any remaining salt.
Functionalization of GQDs with PEG: The aqueous solution of
GQDs was mixed with PEG-bisamine of various molecular weights
in a ratio of 2 mg PEG per mL of solution. The mixture was reacted
at 120 °C with stirring for 72 h to ensure full functionalization. After
cooling, the dialysis process was repeated to remove any unfunc-
tionalized PEG. The water was then evaporated and the GQDs were
redispersed in chlorobenzene.
GQD Characterization: TEM images were obtained by drying
GQD solutions on a carbon grid. For Raman spectra, the GQD solu-
tions were dried onto a SiO2 substrate and measured. Both UV–vis
absorption and PL measurements were conducted in DI water at a
solution concentration of ≈0.5 mg mL–1.
Fabrication of OPV Cells with GQDs: Indium tin oxide (ITO)-
coated glass was cleaned with 2-propanol and a mixture of
NH3 and H2O2. Air plasma treatment was then used to enhance the
wetting between ITO and poly(3,4-ethylenedioxythiophene):poly-
(styrenesulfonate) (PEDOT:PSS) purchased from Sigma Aldrich.
PEDOT:PSS was spin-coated onto ITO at 4000 rpm for 1 min and
then baked at 150 °C for 15 min. P3HT and PCBM were dissolved
and stirred in 1 mL of chlorobenzene for 12 h. For samples con-
taining GQDs, the PCBM solution was mixed with 100 μL of GQDs
in chlorobenzene. The blend of GQDs, P3HT, and PCBM was spin-
coated onto the PEDOT:PSS at 300 rpm for 1 min then 1000 rpm
for 10 s in a glove box filled with N2 gas. An Al electrode was ther-
mally evaporated onto the device in a vacuum (pressure: 10-7 Torr).
Finally, the device was annealed at 150 °C for 5 min.
Characterization: The photovoltaic properties of the OPV cell
were characterized under 1-sun output power, using a xenon lamp
with an air mass global filter (AM 1.5). A silicon reference solar cell
certified by the National Renewable Energy Laboratory (NREL) was
used to calibrate the light and confirm the measurement condi-
tions. Current–voltage (I–V) measurements were performed using
an electrochemical analyzer (CompactStat, Ivium Technologies).
The entire test is repeated for the six devices for each set of fabri-
cation conditions.
Transient Absorption Spectroscopy: TA-spectroscopy was
performed with a Ti:Sapphire laser using a 1-kHz repetition rate,
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 communications
0.1 μJ excitation energy, and 470 nm pump wavelength. The probe
was set at the ground-state (600 nm) and decay kinetics were
extracted using a biexponential function fitting.
Supporting Information
Supporting Information is available from the Wiley Online Library
or from the author.
Acknowledgements
This work was supported by the Center for Advanced Soft-Elec-
tronics funded by the Ministry of Science, ICT and Future Planning
as Global Frontier Project (Grant No. CASE-2013M3A6A5073173),
the nanomaterial technology development program through
the national research foundation of Korea (NRF) funded by
the Ministry of Science, ICT and future planning (Grant No.
2012M3A7B4049807), and the GRC project of KAIST Institute for
the NanoCentury.
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Received: October 14, 2015
Revised: November 25, 2015
Published online:
small 2015,
DOI: 10.1002/smll.201503108