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Highly Transparent Organic Solar Cells with All‐Near‐Infrared Photoactive

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Article in Small Methods · July 2019

DOI: 10.1002/smtd.201900424

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Communication
Transparent Solar Cells [Link]

Highly Transparent Organic Solar Cells with All-Near-

Infrared Photoactive Materials
Yuanpeng Xie, Ruoxi Xia, Tengfei Li, Linglong Ye, Xiaowei Zhan, Hin-Lap Yip,*
and Yanming Sun*

technologies that can be integrated with

Transparent organic photovoltaics are identified as important components buildings as windows, roofs, walls, etc.[4]
for building-integrated photovoltaics and smart window technologies. In In addition to maintaining an attractive
this work, highly transparent organic solar cells (T-OSCs) based on all-near- appearance of buildings, T-OSCs can gen-
infrared (NIR) harvesting materials (optical bandgap, E gopt < 1.4 eV) are first erate electricity directly from sunlight, pro-
viding additional values for power supply
fabricated. Both donor and acceptor materials used in T-OSCs exhibit great
to the building. Several important param-
transparency in the visible region. After combining MoO3/Ag or MoO3/Ag/ eters, such as visible light transmittance
MoO3 transparent electrode, T-OSCs show excellent visible light transmit- (VLT), power conversion efficiency (PCE),
tance (VLT) of 52–61.5% with power conversion efficiencies of 3.5–4.2%. As and color-rendering index (CRI), are used
far as it is known, this all-NIR active layer represents the most visible trans- to evaluate the performance of T-OSCs.[5]
VLT also named luminosity, which is the
parent donor–acceptor combination in OSCs. In addition to high VLT, T-OSCs
brightness of an object as perceived by a
have great aesthetic value, good color-rendering index (CRI > 90), and high human eyes. It can be calculated by inte-
light energy utilization properties. This work highlights great potential of NIR grating the transmission spectrum against
photoactive materials for T-OSCs. the photopic response of human eyes,[6]
and can be expressed as

Organic photovoltaic device is a viable way to relieve the growing

energy stress by directly converting solar energy into electric VLT =
∫ T ( λ )P ( λ )S ( λ ) d λ (1)
energy.[1] Transparent nature is an outstanding technological ∫ P ( λ )S ( λ ) d λ
strength for organic materials compared to silicon and inor-
ganic semiconductor materials.[2,3] Transparent organic solar where λ is the visible region wavelength, T is the transmission,
cells (T-OSCs) have been identified as important components P is the human eye photopic response (380–780 nm), and S is
for building-integrated photovoltaics (BIPVs) and smart window the light flux of AM 1.5G. To date, fullerene acceptor–based
semitransparent organic solar cells show VLTs of 20–30%
and PCEs of 4–8%.[7–16] Since the emergence of nonfullerene
Y. Xie, L. Ye, Prof. Y. Sun
Heeger Beijing Research and Development Center acceptors (NFAs), higher VTLs of 30–40% and higher PCEs of
School of Chemistry 8–10% have been achieved.[17–38] It should be noted that T-OSCs
Beihang University with VLTs below 50% may fulfill only certain applications that
Beijing 100191, P. R. China require low transparencies, and therefore it is highly desirable
E-mail: sunym@[Link]
to develop new T-OSCs with high transparencies to broaden
R. Xia, Prof. H.-L. Yip
Department State Key Laboratory of Luminescent Materials and Devices their applications.[39] The low VLT of both fullerene- and NFA-
School of Materials Science and Engineering based transparent devices is mainly ascribed to the low visible
South China University of Technology transmittance of photoactive layer and strong visible absorption
Guangzhou 510640, P. R. China of transparent electrode.[40]
E-mail: msangusyip@[Link]
Theoretical calculations have predicted that highly trans-
T. Li, Prof. X. Zhan
parent (VLT > 60%) and highly efficient (PCE > 10%) could be
Department of Materials Science and Engineering
College of Engineering simultaneously realized in one OSC by developing active layers
Peking University that can selectively harvest the near-ultraviolet (NUV) and near-
Beijing 100871, P. R. China infrared (NIR) light.[41,42] For example, Loo and co-workers
Prof. H.-L. Yip reported a highly transparent (≈70%) device with ultrawide
Innovation Center for Printed Photovoltaics bandgap donors and acceptor that can selectively harvest near-
South China Institute of Collaborative Innovation
Dongguan 523808, P. R. China UV light. A PCE of ≈1.4% was obtained because of the low
distribution (≈2%) of sun energy in the near-UV region.[43,44]
The ORCID identification number(s) for the author(s) of this article In contrast, all-NIR photoactive materials can maintain high
can be found under [Link]
visible transparency, while simultaneously utilizing NIR
DOI: 10.1002/smtd.201900424 solar irradiation to achieve high efficiency. Unfortunately, the

Small Methods 2019, 3, 1900424 1900424 (1 of 6) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
[Link] [Link]

Figure 1. a) Chemical structures of PDTP-DFBT and FOIC. b) AM 1.5G curve, human eyes response curve, and normalized UV–vis absorption spectra
of PDTP-DFBT and FOIC neat films. c) Photograph of PDTP-DFBT:FOIC active layer film on ITO glass. d) Inverted device structure with top MoO3 as
an optical management layer.

T-OSCs based on all-NIR materials (E gopt < 1.4 eV) have not been films exhibit E gopt of 1.38 and 1.32 eV, respectively. Both of them
reported yet. have weak absorption in the visible region (400–700 nm) and
Herein, ultralow bandgap donor PDTP-DFBT[45] (E gopt = 1.38 eV) strong signature in the NIR region (>700 nm). AM 1.5G solar
and ultralow bandgap NFA FOIC[46] (E gopt = 1.32 eV) were used spectrum is composed of UV region, visible region, and NIR
to fabricate highly transparent OSCs for the first time. The region. 51% of solar energy is located at the NIR region, which
basic device architecture for the T-OSC is indium tin oxide is large than 47% of the visible spectrum and 2% of the UV
(ITO)/ZnO/bulk heterojunction (BHJ)/MoO3 (3 nm)/Ag (10 nm), spectrum. Human eyes’ response curve shows narrow dis-
which delivered a VLT of 52.0% and a maximum PCE of 4.2%. tribution in the range of 380–780 nm with maximum weight
In such a device, the thin MoO3 functioned served as a hole- at 550 nm. The transmittance around 550 nm makes more
extraction layer and the thin Ag film served as the top transparent contributions to luminosity, while light with a wavelength
electrode. To further improve the transmittance without causing shorter than 400 nm or longer than 700 nm has less influ-
a significant reduction in efficiency, an extra optical management ence. These results indicate that NIR-absorbing materials have
layer MoO3 was deposited on top of the Ag transparent electrode great potential to produce T-OSCs with both good transparency
to optimize the optical property of the T-OSCs.[47–49] Optical simu- and efficiency. Figure S1 (Supporting Information) showed
lation suggests that the VLT could reach a maximum value when the transmittance spectra of ITO glass and PDTP-DFBT:FOIC
the thickness of top MoO3 is 35 nm. Guided by optical simulation, active layer on ITO glass. ITO glass shows a luminosity of
a 35 nm MoO3 optical layer was applied to the T-OSC, and the 90.8%. Active layer/ITO glass exhibited a maximum transmit-
resultant device exhibited a more clear-looking appearance with tance of 82% at 470 nm, with an impressive luminosity value of
a higher VLT of 61.5% and a decent PCE of 3.5%. Our results 73.6%. Figure 1c illustrates the picture of a 3 cm × 3 cm active
manifest that all-NIR photoactive materials have outstanding layer on ITO glass. Clear and bright background indicates
achievement in visible light transmittance, PCE, and aesthetic good performance of PDTP-DFBT:FOIC for T-OSC. As shown
value, which represent the bright future of T-OSCs. in Figure 1d, inverted device structure of ITO (110 nm)/ZnO
Chemical structures of PDTP-DFBT and FOIC are shown in (20 nm)/PDTP-DFBT:FOIC (75 nm)/MoO3 (3 nm)/Ag (10 nm)
Figure 1a. As shown in Figure 1b, PDTP-DFBT and FOIC neat was used to fabricate T-OSC. Top MoO3 was introduced as an

Small Methods 2019, 3, 1900424 1900424 (2 of 6) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
[Link] [Link]

Figure 2. a) Simulated luminosity and simulated current density with different thickness of top MoO3. The simulated current density is obtained under
a maximum EQE of 100%. b) Simulated transmittance curves without and with 35 nm top MoO3. Simulated optical electric field |E|2 distribution of the
T-OSCs c) without top MoO3 and d) with 35 nm top MoO3. The light intensities of e) λ = 550 nm and f) λ = 800 nm in different positions.

optical management layer to further enhance optical transmit- significantly improved in the range of 400–700 nm with a
tance of the transparent devices. maximum transmittance of 73.8% at 470 nm. As simulated in
Optical simulation is a powerful method for guiding the Figure 2c,d, optical electric field |E|2 distribution reflects the light
optimal device architecture.[50] To predict the optimal thickness intensity at different positions with the device. The green light is
of top MoO3, the device luminosity with different top MoO3 greatly contributed to luminosity, attributing to the sensitivity of
thickness is simulated in Figure 2a. Transparent device without human eyes to green light, while NIR light is helpful for photon-
top MoO3 shows a decent luminosity of 47%, while transparent to-charge conversion in PDTP-DFBT:FOIC blend. Hence, the
device with 35 nm top MoO3 shows a maximum luminosity of light intensities of λ = 550 nm and λ = 800 nm in different
65%. Current density (Jsc) of the devices with different top MoO3 positions are investigated in Figure 2e,f. The transparent device
thickness is also calculated. The calculated Jsc for devices with based on 35 nm top MoO3 shows a lower intensity of 550 nm
35 nm top MoO3 is 83% that of the device without top MoO3. within the active layer compared to the reference transparent
Detailed simulated transmission spectra for transparent devices device, which ultimately leads to high transmittance. For 800 nm
without and with 35 nm top MoO3 are shown in Figure 2b. light, the transparent device with 35 nm top MoO3 is similar to
For device with 35 nm top MoO3, the transmittance has been the reference transparent device, which can ensure relatively

Small Methods 2019, 3, 1900424 1900424 (3 of 6) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
[Link] [Link]

Figure 3. a) Current–voltage (J–V) curves. b) EQE curves and c) transmittance of transparent OSCs without and with 35 nm top MoO3. d) Comparison
of our results with representative VLT (>50%) and PCE values reported in the literature for transparent solar cells.

high current density. These results indicate that the transparent external quantum efficiency (EQE) spectrum of the T-OSCs. The
device with 35 nm top MoO3 has excellent property both in VTL integrated Jsc based on 0 and 35 nm top MoO3 are 10.60 and
and PCE. 8.48 mA cm−2, respectively, which are well consistent with the
Inspired by the optical simulation, the current density– J–V results. Figure 3c demonstrates the transmission spectrum
voltage (J–V) curves of T-OSCs without and with 35 nm top of T-OSCs. The control transparent devices display a prominent
MoO3 are illustrated in Figure 3a and the detailed device luminosity of 52.0% with a maximum transmittance of 55.4%
parameters are listed in Table 1. For the opaque device, a best at 540 nm. As expected, after evaporating 35 nm top MoO3, the
PCE of 6.1% is obtained with a short-circuit current density transmittance showed remarkable upshift from 460 to 900 nm,
(Jsc) of 14.61 mA cm−2, an open-circuit voltage (Voc) of 0.716 V, yielding an impressive luminosity of 61.5% with a maximum
and a fill factor (FF) of 58.0% (see Figure S2 in the Supporting transmission of 65.3% at 550 nm. This helps us to understand
Information). The low FF is possibly attributed to unbalanced the significantly dropped Jsc of the T-OSCs after incorporating
hole and electron mobilities (Figure S2c, Supporting Informa- 35 nm top MoO3. To our best knowledge, a PCE of 3.5% with a
tion). T-OSCs based on 0 nm top MoO3 show a maximum PCE luminosity of 61.5% is among the champion values for transparent
of 4.2% with Jsc = 11.00 mA cm−2, Voc = 0.710 V, and FF = 53.9%. solar cells (Figure 3d). The quantum utilization efficiency
After incorporating 35 nm top MoO3, an optimal PCE of (EQE + T) is used to describe the light energy utilization in semi-
3.5% is obtained with Jsc = 8.80 mA cm−2, Voc = 0.748 V, and transparent devices,[41,50] which is defined as the sum of external
FF = 53.0%. It is noted that the relative Jsc of 80% in comparison quantum efficiency and the transmittance. As shown in Figure S3
with the reference transparent device is very close to the (Supporting Information), the reference T-OSC delivers an average
theoretical calculating value of 83%. When the simulated light EQE + T value of 70% (from 400 to 700 nm) with a maximum
illuminating from the top side, the T-OSCs with 0 and 35 nm value of 78.8% at 550 nm. In contrast, the T-OSC with 35 nm
top MoO3 show best PCEs of 2.5% and 2.2% (see Table S1 in top MoO3 shows an average EQE + T value of 72.6% with a
the Supporting Information), respectively. Figure 3b shows the maximum value of 82.5%, which suggests that higher visible

Table 1. The detailed parameters of T-OSCs without and with 35 nm top MoO3.

Top MoO3 [nm] Jsc [mA cm−2] Voc [V] FF [%] PCEa) [%] VLT [%] CRI
0 10.90 ± 0.20 0.710 ± 0.002 52.0 ± 0.5 4.2(4.0) 52.0 90.9
35 8.61 ± 0.20 0.744 ± 0.004 51.3 ± 0.2 3.5(3.3) 61.5 91.2

a)The
statistical results obtained from over ten devices.

Small Methods 2019, 3, 1900424 1900424 (4 of 6) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
[Link] [Link]

Figure 4. a) Color coordinates of transparent devices without and with 35 nm top MoO3 on a CIE 1931xyY chromaticity diagram. Photographs taken
through T-OSCs b) without top MoO3 and c) with 35 nm top MoO3.

light utilization efficiency of light energy can be achieved using Our results reveal that a combination of using all-NIR light-har-
top MoO3 optical management layer. More importantly, all the vesting materials and appropriate optical management could
EQE + T values are far below 100% that verified good authen- produce highly transparent OSCs. A high efficiency is expected
ticity of our results. when employing new NIR photoactive materials.
Aesthetic essential factor and human color perception also
are very important for T-OSCs. The color coordinates (x, y),
CRI, and correlative color temperature (CCT) are used to eval- Supporting Information
uate human visual color perception, which can be calculated Supporting Information is available from the Wiley Online Library or
from the transmission spectrum of T-OSCs. The color coor- from the author.
dinates and CRI represent the relationship between incident
light and the transmitted light of T-OSCs, while the CCT is the
temperature compared to a blackbody radiator. The color coor- Acknowledgements
dinates of T-OSCs without and with 35 nm top MoO3 in the
Y.X. and R.X. contributed equally to this work. This work was financially
CIE 1931 chromaticity diagram are illustrated in Figure 4a. The supported by the National Natural Science Foundation of China (NSFC)
control transparent device and the optimal transparent device (Grant Nos. 21734001, 21674007, 91633301, and 21761132001) and the
showed CIE color coordinates of (0.3274, 0.3593) and (0.3444, Ministry of Science and Technology (Grant No. 2017YF0206600).
0.3746), CCT of 5700 K and 5080 K with excellent CRI of 90.9
and 91.2, respectively. The great color rendering property of
T-OSCs is further verified by digital photographs of T-OSCs. As Conflict of Interest
shown in Figure 4b,c, the flowers behind the T-OSCs can be The authors declare no conflict of interest.
clearly seen with good color consistency. These results demon-
strate appealing color appearance of our T-OSCs.
In summary, highly transparent organic solar cells are devel- Keywords
oped using a new strategy involving an ultranarrow polymer
donor and an ultranarrow nonfullerene acceptor. This new all-near-infrared, efficiency, transparent organic solar cells, visible light
transmittance
combination can selectively allow most of the visible light to
transmit through the device to ensure high luminosity, but can Received: June 5, 2019
also harvest NIR light to achieve high efficiency. When a 10 nm Revised: June 20, 2019
Ag film is used as the top transparent electrode, the T-OSC gave Published online: July 25, 2019
a visible light transmittance of 52% with a PCE of 4.2%. Guided
by optical simulation, an optimal optical film of MoO3 with
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Small Methods 2019, 3, 1900424 1900424 (6 of 6) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Copyright WILEY-VCH Verlag GmbH & Co. KGaA, 69469 Weinheim, Germany, 2019.

Supporting Information
for Small Methods, DOI: 10.1002/smtd.201900424

Highly Transparent Organic Solar Cells with All-Near-

Infrared Photoactive Materials
Yuanpeng Xie, Ruoxi Xia, Tengfei Li, Linglong Ye, Xiaowei
Zhan, Hin-Lap Yip,* and Yanming Sun*
Copyright WILEY-VCH Verlag GmbH & Co. KGaA, 69469 Weinheim, Germany, 2019.

Supporting Information

Highly Transparent Organic Solar Cells with All Near-Infrared Photoactive Materials

Yuanpeng Xie, Ruoxi Xia, Tengfei Li, Linglong Ye, Xiaowei Zhan, Hin-Lap Yip* and Yanming
Sun*

Device Fabrication: PDTP-DFBT is purchased from 1-Materials. FOIC is synthesized by

Zhan’s group. PDTP-DFBT and FOIC are dissolved in chloroform with ratio of 1:1.5. The
polymer concentration is 4 mg ml-1. ZnO precursor is prepared as follow: 1.0 g zinc acetate
dihydrate and 0.28 mL ethanolamine dissolving in 20 ml 2-methoxyethanol. ITO glass
substrates are cleaned by detergent deionized water, acetone and isopropyl alcohol for
sonication treatment 20 min each, then baked at 110 °C for one light. Later, ZnO precursor is
spin-coated at 4000 rpm and baked at 210 °C to generate 20 nm ZnO. PDTP-DFBT:FOIC
solutions are spin cast at 1600 rpm for 30 s to form a thickness of 75 nm. Finally, 3 nm MoO3
and transparent Ag or Au layer are thermally deposited. The active area is 4 mm2.

Measurements and Characterizations: Cyclic voltammetry (CV) measurement is

performed using three-electrode method, Pt wire is the counter electrode and Ag/Ag+
electrode is the reference electrode on a CHI660E Electrochemical Workstation in a
tetrabutylammonium hexafluorophosphate (Bu4NPF6) (0.1 M) acetonitrile solution with a
scan rate of 50 mV s-1. The ultraviolet-visible (UV) absorption spectra of the neat films are
measured by Shimadzu UV-2600. The thickness is measured by Dektak XT profilometer
(Bruker). All the photographs are taken by HUAWEI Nova 2S. Current density-voltage (J-V)
curves are measured by Keithley 2400 Source. AM 1.5 G solar simulator Measure is provided
by Enli Technology Co., Ltd, SS-F5-3A. EQE spectra awemeasured by QEX10 Solar Cell
IPCE measurement. The charge carrier mobility were measured using SCLC method with
device architecture of ITO/PEDOT:PSS/PDTP-DFBT:FOIC/MoO3/Ag and ITO/ZnO/PDTP-
DFBT:FOIC/PFN-Br/Al, respectively, and current-voltage (J0.5-V) curves was by fitted by J =
9ε0εrμV2/8L3.

1
 100
PDTP-DFBT (LUMO = -3.57 eV HOMO = -5.28 eV)
FOIC (LUMO = -4.02 eV HOMO = -5.43 eV)

Transmittance (%)
80

Current (a.u.)
60

40

20 ITO glass
ITO/glass/ZnO/PDTP-DFBT:FOIC

0
-1.5 -1.0 -0.5 0.0 0.5 1.0 1.5 2.0 300 400 500 600 700 800 900
+ Wavelength (nm)
Potential (V vs Ag/Ag )

Figure S1. (a) The electrochemical cyclic voltammetry (CV) curves of PDTP-DFBT and
FOIC. (b) Transmittance spectra of indium tin oxide (ITO) glass and PDTP-DFBT: FOIC
active layer on ITO glass.
60
3 (a) (b) 1.6
(c)
Current Density (mA cm-2)

50 1.4
0
1.2
40

 cm )
Jsc = 14.61 mA cm-2

-1
-3
EQE(%)

Voc= 0.716V 1.0

30

0.5
-6 FF = 58.0% 0.8

(mA
PCE = 6.07% Jsc,cal = 14.0 mA cm-2
-9 20 0.6

0.5
J
-12 0.4 Hole mobility (3.7 -4cm 2V-1S-1)
10 Electron mobility (8.110-4cm 2V-1S-1)
0.2
-15
0
-0.2 0.0 0.2 0.4 0.6 0.8 300 400 500 600 700 800 900 1000 1 2 3 4 5
Voltage (V)
Voltage (V) Wavelength(nm)
Figure S2 (a) Current-voltage (J-V) curves, b) EQE curves and of the opaque device and (c)
Charge carrier mobility of optimal device.

100

90
EQE+Transmittance (%)

80

70

60

50

40 Top MoO3 thickness

0 nm
30
35 nm
20

10

0
300 400 500 600 700 800 900

Wavelength (nm)

Figure S3. The quantum utilization efficiency curves of the devices without and with 35 nm
top MoO3

2
 Table S1. The detailed parameters of T-OPVs illuminated from top side.

Top MoO3 Jsc Voc FF PCE[a]

(mA cm-2) (V) (%) (%)
0 nm 6.42±0.4 0.665±0.004 56.5±0.4 2.5(2.3)
35 nm 5.49±0.3 0.710±0.003 53.6±0.1 2.2(2.1)
[a] The statistical results obtained from 5 devices.

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