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Highly efficient and stable binary all-polymer solar

cells enabled by sequential deposition processing
Cite this: J. Mater. Chem. C, 2022,
10, 17899 tuned microstructures†
Chaoyue Zhao,‡a Ruijie Ma, ‡*b Jiyeon Oh,c Lihong Wang,a Guoping Zhang,a
Yajie Wang,a Siying He,a Liangxiang Zhu,a Changduk Yang, c Guangye Zhang*a
Published on 03 November 2022. Downloaded on 6/17/2024 3:32:33 AM.

and Gang Li *b

The power conversion efficiency (PCE) and operation stability of all-polymer solar cells (all-PSCs) are
expected to be simultaneously pushed to a high level, that can be considered for further
commercialization. Here the sequential processing (SqP) method is applied to process the PM6:PY-DT all-
polymer system, while the control devices are made from the blend casting (BC) method. As a result, the
efficiency rises to 16.5% in SqP devices from 15.8% of their BC counterparts, which is mainly caused by the
improved fill factor (FF). Device physics study and morphology analysis reveal that optimized crystallinity
and vertical phase separation result in suppressed charge recombination, higher charge collection and
Received 30th September 2022, transport ability, which is responsible for PV performance improvement. In addition, operational stability is
Accepted 3rd November 2022 compared by maximal power point (MPP) tracking: the SqP device has a significantly longer time it takes to
DOI: 10.1039/d2tc04142a degrade to 80% of its initial PCE than the BC device, which could be attributed to the vertical composition
distribution optimization realized by the two-step coating method. This work successfully demonstrates the
rsc.li/materials-c effectiveness and promising future of using an SqP method to boost device performance for all-PSCs.

Introduction stability are more feasible when they contain an active layer with
both polymeric donor(s) and acceptor(s). In other words, all-
Organic solar cells (OSCs) are one of the most promising green polymer solar cells (all-PSCs) have potential in the OSC field.
energy technologies, to realize carbon neutrality.1–6 In the past To date, the main challenge of all-PSCs is their relative low
few decades, researchers put tremendous effort into pursuing efficiencies compared to their small molecular counterparts.
high power conversion efficiency (PCE) for OSCs, and as a Though this gap has been successfully alleviated by the new
consequence values 419% have been reported by many different concept of a polymerized small molecular acceptor (PSMA), speci-
groups.7–17 However, the fruitful development solely of efficiency fically PCEs are now over 16% in multiple cases.21–29 Nonetheless,
enhancement cannot fulfill the requirement of commercialized the operational and mechanical stability difficulties come back
photovoltaic (PV) cargo, where the device stability matters equally again, due to PSMAs partially inheriting the properties of small
importantly.18–20 Due to the intrinsic disadvantages of small molecules.30–33 Since current PSMA-type materials are the most
molecules in morphology stability, OSC devices with superior promising candidates for high-efficiency, more efforts in boosting
device stability are required that rely not only on chemistry
a
College of New Materials and New Energies, Shenzhen Technology University, innovation, but also effective device fabrication methods.
Shenzhen 518118, China. E-mail: [email protected] Compared with traditional blend casting (BC), recently more and
b
Department of Electronic and Information Engineering, Research Institute for more exciting PCE values have been achieved using a sequential
Smart Energy (RISE), Guangdong-Hong Kong-Macao (GHM) Joint Laboratory for
processing (SqP) method,34–36 initially explored in the PCBM era.
Photonic-Thermal-Electrical Energy Materials and Devices, The Hong Kong
Polytechnic University, Hung Hom, Kowloon, Hong Kong, 999077, China.
Not only is simple efficiency enhancement reported using the SqP
E-mail: [email protected], [email protected] method, other advantages like high transparency and improved
c
Department of Energy Engineering, School of Energy and Chemical Engineering, mechanical durability were also found.37–40 All these achievements
Perovtronics Research Center, Low Dimensional Carbon Materials Center, Ulsan suggest tuning the nanostructure of the active layer using an SqP
National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulju-gun,
method in both horizontal and vertical directions at the same time
Ulsan, 44919, South Korea
† Electronic supplementary information (ESI) available. See DOI: https://doi.org/
is a promising choice to realize high PCE and stability for all-PSCs.
10.1039/d2tc04142a Herein, we applied the SqP method to an all-polymer photo-
‡ Equal contribution. voltaic blend (PM6 as donor, PY-DT as acceptor) – which has

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already been reported with high PCEs in BC processed devices41 – from commercial paths and used without further purification.
to seek a chance of achieving simultaneously efficient and The fabrication schematic diagram of BC and SqP devices are
stable all-PSCs. As a result, the SqP enabled PM6:PY-DT based illustrated in Fig. 1(c), with a conventional structure of ITO/
device delivers an optimal PCE of 16.5% while that of the BC PEDOT:PSS/active layer/PNDIT-F3N/Ag.
processed device is 15.8%. The efficiency improvement comes The normalized ultraviolet-visible (UV-vis) absorption spec-
from concurrently increased open-circuit voltage (VOC), short- tra of neat films of PM6 and PY-DT and their blended films
circuit current density ( JSC) and fill factor (FF). Among them, fabricated using BC or SqP methods, are plotted in Fig. 2(a) and
the betterment of FF is the main contributor. Device physics (b), respectively. Highly close intensities of 0–0 and 0–1 vibra-
study supports that the SqP PM6:PY-DT blend film exhibits tional peaks indicate that PM6 in a film state exhibits H- and
significantly enhanced charge mobility, especially the electron J-aggregation simultaneously. PY-DT’s absorption peak locates
mobility, and correspondingly improved charge collection and at ca. 800 nm, which is generally complementary to that of
suppressed recombination. Morphology characterization PM6. The BC and SqP blend films are generally the same but
clearly shows the graded morphology achieved by SqP, as well with some minor differences, which implies SqP might bring
as more ordered crystallization, which is consistent with mobi- some delicate adjustment in film morphology.
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lity enhancement and recombination suppression. As a final The device performance comparison is shown in Fig. 2(c),
stage, device stabilities of two types of solar cells are evaluated with the current density versus voltage (J–V) characteristics, and
by placing them under maximal power point (MPP) tracking in Table 1. The fabrication details can be found in the ESI.†
under a white LED with 1 sun intensity. Compared with the BC Accordingly, BC devices display a PCE of 15.8%, with a VOC of
device, the SqP one exhibits well maintained VOC and FF, 0.960 V, a JSC of 23.2 mA cm 2 and an FF of 70.8%. Though the
thereby obviously longer T80 (the time it takes for a device to absolute value here is lower than what was reported in the
degrade to 80% of its initial PCE). It is believed that optimized reference, it could be reasonable once we consider the polymer
vertical phase segregation contributes to the stability enhance- batch differences and processing solvent variation.41 Herein,
ment, according to film-depth-dependent light absorption we chose toluene, an eco-friendly solvent, instead of chloroform
spectra (FLAS). This paper presents decent PCE with distin- which was used before. The SqP devices demonstrate optimal
guishable improvement for target devices together with better efficiency as high as 16.5%, among the highest level of PCEs for
operation stability, proving the effectiveness and prospect of non-halogenated solvent processed all-PSCs.42–48 The increase
the SqP method in boosting PV performance for all-PSCs. of PCE mainly comes from FF improvement, but also partially
benefits from slightly higher VOC and JSC. In addition, the
external quantum efficiency (EQE) spectra of these two types
Results and discussion of devices are measured and depicted in Fig. 2(d). The
The chemical structures of donor and acceptor materials PM6 corresponding integral current density values are 22.5 and
and PY-DT are shown in Fig. 1(a), together with the energy level 22.7 mA cm 2, respectively (also listed in Table 1). Therein, the
distribution: highest occupied molecular orbit (HOMO) and measurement error should be smaller than 4% in this report.
lowest unoccupied molecular orbit (LUMO), of all materials To figure out the underlying reason for FF enhancement of
applied in this research in Fig. 1(b).41 All of them are obtained SqP devices, the charge mobility variation is firstly investigated

Fig. 1 (a) Chemical structures of polymer donor PM6 and polymer acceptor PY-DT. (b) Energy level distribution of materials in our devices. (c)
Processing schematic diagram of BC and SqP methods.

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Fig. 2 UV-vis spectra of (a) PM6 and PY-DT neat films, and (b) BC and SqP blend films. (c) J–V characteristics and (d) EQE spectra.

Table 1 Summary of photovoltaic parameters for PM6 and PY-DT based all-PCSs processed from different methods, measured under AM 1.5 G
illumination at 100 mW cm 2

Active layer VOC [V] JSC [mA cm 2] JEQE [mA cm 2] FF PCEa [%] mh [cm2 V 1
s 1] me [cm2 V 1
s 1]
4 4
BC 0.962  0.001 (0.960) 23.1  0.3 (23.2) 22.5 0.703  0.005 (0.708) 15.6  0.2 (15.8) 5.83  10 5.01  10
4 4
SqP 0.964  0.002 (0.964) 23.2  0.2 (23.6) 22.7 0.728  0.004 (0.725) 16.32  0.10 (16.5) 7.30  10 7.84  10
a
The standard deviations are based on measurements of over at least ten independent devices.

by the space charge limited current (SCLC) method. The decay of the TPV signal is shown in Fig. 3(c), where the fitted
calculation and experimental details are also given in ESI.† recombination lifetime for the BC device is 2.00 ms and that of
The hole-only and electron-only device results are presented in the SqP device is 2.64 ms. The prolonged value here allows the
Fig. 3(a) and (b), and are noted with fitted values for hole reduction of recombination and the boosting of the FF. Mean-
mobility and electron mobility (mh and me). The mh increases while, the charge extraction characteristics are compared by
from 5.83  10 4 cm2 V 1 s 1 to 7.30  10 4 cm2 V 1 s 1 for transient photocurrent (TPC). Fig. 3(d) shows that the extrac-
hole-only devices; and 7.84  10 4 cm2 V 1 s 1 from tion lifetime of the SqP device is a little shorter than its BC
5.01  10 4 cm2 V 1 s 1 for electron-only devices. Accordingly, counterpart (0.15 ms vs. 0.17 ms). Thereby, the vertically opti-
the SqP device promotes the electron transport ability of the mized film possibly facilitates the charge collection, which
active layer significantly, and in a smaller way for hole trans- might contribute to FF. Apart from the direct evidence provided
port. Then the general charge transport of the SqP film is by the TPV and TPC experiments, the light intensity dependent
obviously improved, which is supposed to be beneficial for JSC/VOC and dark current devices are also measured to obtain
achieving higher FF (suppressed charge recombination and more side supports in Fig. S1 (from a to c) (ESI†). The bimo-
more efficient charge extraction). lecular recombination rates are nearly identical, while the
Next, the recombination dynamics is quantitatively studied by diode ideality factor for an SqP device under light and dark,
transient photovoltage (TPV) measurement. The mono-exponential is closer to 1 compared with that of the BC devices. These

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Fig. 3 (a) Hole-only and (b) electron-only device results; (c) TPV + (d) TPC curves.

Fig. 4 2D-GIWAXS patterns and line-cuts of (a) BC and (b) SqP blend films.

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results suggest that the SqP device operates more like an ideal illustrated in Fig. 5(a) and (b) and Fig. S3a, b (ESI†), respec-
diode than a BC device does, which is intrinsically better for tively, for BC and SqP active layers. Meanwhile, the corres-
pursuing high FF. ponding composition weight ratio of PM6 and PY-DT at
Then the morphology study is carried out by atomic force different depths in the films are plotted in Fig. 5(c) and (d). It
microscopy (AFM) as the first stage. The corresponding height is observed in the BC film, that PY-DT assembles at the top
images of PM6, PY-DT neat films, and blend films processed surface and then immediately shows a content drop with
from BC and SqP methods are displayed in Fig. S2a–d (ESI†), it increasing depth. Further monotonous enhancement of the
is shown that PM6 has a smoother surface than PY-DT, but the PY-DT ratio follows the weight ratio of 1 : 1.2 for donor and
SqP surface is smoother than the BC one, indicating more PM6 acceptor. In contrast, the SqP film contains PY-DT’s vertical
aggregates on the top part of the ca. 100 nm thick film. This is distribution with continuous high ratio in the top part of the
contradictory to our hypothesis that PY-DT should take the film, which is beneficial to forming more phases that are
dominant position at the top. However, such phenomenon is continuous vertically, facilitating the charge transport and
also observed in a recent report,49 and can be rationalized once collection. Based on this analysis, the advantage of SqP is
we consider the composition migration driven by thermal further demonstrated. In addition to these results, one more
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annealing or a solvent additive’s slow evaporation.50–53 The important issue is to rationally claim why such vertical dis-
AFM experiments only give us a vague and preliminary impres- tribution appears: (i) the polymerized Y-series acceptor usually
sion of film morphology. For further understanding of mole- has a higher surface free energy than PM6, which supports its
cular packing and crystallinity change in active layers, grazing agglomeration at the bottom top of the active layer in both BC
incidence wide-angle X-ray scattering (GIWAXS) technology is and SqP films; (ii) the polymer acceptor (PY-DT herein) has
applied.54–57 The 2D patterns and derived line cuts of BC and better solubility in solvent additive 1-chloronaphthalene
SqP films are shown in Fig. 4, with calculated parameters of (1-CN), which means it will be partially deposited after the
(010) diffraction peaks presented in Table S1 (ESI†). The removal of the main solvent toluene, and shows a sudden
molecular packing mode is basically the same for two types content ratio increase at the top surface in BC films.59–61
of active layers, but the SqP can promote the crystallization Finally, the operational stability of the BC and SqP devices
quality of p–p stacking: the coherence length increases from are evaluated by placing them under maximal power point
29.6 to 31.4 Å. More ordered p–p packing with similar diffrac- (MPP) tracking (Fig. 6). After 100 hours, the BC device degrades
tion intensity implies that the charge transport property could to 80% of its initial PCE, and it keeps dropping to ca. 70% the
be improved. initial PCE after 160 hours under illumination. The SqP device,
Besides, the vertical distribution of PM6 and PY-DT is on the contrary, keeps the PCE level at about 95% the initial
quantitatively studied by the film-depth-dependent light PCE after 160 hours degradation. Clearly the SqP method is
absorption (FLAS) characterization.58 The raw results are helpful to achieve highly stable all-PSCs, implying the very

Fig. 5 FLAS of (a) BC and (b) SqP blended films. Calculated vertical ratio of PM6 and PY-DT for (c) BC and (d) SqP blended films.

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to compare the performance, and seek a chance of achieving

better efficiency and stability simultaneously. As a result, the
BC device demonstrates a PCE of 15.8% (lower than reported
values, possibly due to batch differences and non-halogen
solvents as the processing medium), and the SqP has higher
efficiency of 16.5% which is mainly contributed by the enhance-
ment of FF. Further characterization reveals that optimized
vertical distribution and crystallinity of the active layer leads to
promoted charge transport and suppressed recombination as
well as charge collection, which well supports the PV perfor-
mance improvement. Meanwhile, the stability is considered
using MPP tracking results, which show that the SqP device is
obviously more stabe than its BC counterpart, which can be
understood by the tuned vertical composition distribution.
Published on 03 November 2022. Downloaded on 6/17/2024 3:32:33 AM.

This paper further emphasizes the prospect and effectiveness

of the SqP method in pursuing better device performance for
all-PSCs.

Author contributions
Chaoyue Zhao: investigation, formal analysis; Ruijie Ma: super-
vision, writing – original draft, project administration; Jiyeon
Oh: investigation; Lihong Wang: investigation; Guoping Zhang:
investigation; Yajie Wang: investigation; Siying He: investiga-
tion; Liangxiang Zhu: investigation; Changduk Yang: resources;
Guangye Zhang: conceptualization, supervision; Gang Li:
resources, writing – review and editing, supervision.

Conflicts of interest
There are no conflicts to declare.
Fig. 6 MPP tracking results for BC and SqP devices: (a) VOC, (b) JSC,
(c) FF and (d) PCE.

Acknowledgements
promising future of using this fabrication to propel the com-
G. Zhang appreciates the support from the Guangdong Basic
mercialization of OSCs.
and Applied Basic Research Foundation (2022A1515010875,
Principally, it is also understandable for improved PCE in
2021A1515110017), Natural Science Foundation of Top Talent
SqP devices – from the point of thermodynamics62,63 – that
of SZTU (grant no. 20200205), Project of Education Commis-
morphology degradation of the donor–acceptor heterojunction
sion of Guangdong Province of China (2021KQNCX080), Educa-
involves complete separation from each other since they have
tion Department of Guangdong Province (2021KCXTD045).
very different surface free energies. Besides, the larger surface
G. Li acknowledges the support from Research Grants Council
free energy acceptor will concentrate at the bottom, and PM6
of Hong Kong (Project No. 15221320, C5037-18G, C7018-20G),
should agglomerate at the top. The SqP film successfully tunes
RGC Senior Research Fellowship Scheme (SRFS2223-5S01),
the vertical distribution of PM6 and PY-DT, which increases the
Hong Kong Innovation and Technology Commission (GHP/
difficulty to achieve the final balance of thermodynamics,
205/20SZ), Shenzhen Science and Technology Innovation Com-
therefore better device stability.
mission (JCYJ20200109105003940), the Hong Kong Polytechnic
University Internal Research Funds: (Sir Sze-yuen Chung
Conclusion Endowed Professorship Fund (8-8480), YW4R, SAC5), and
Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-
In summary, we choose a reported highly efficient binary all- Thermal-Electrical Energy Materials and Devices (GDSTC No.
polymer photovoltaic blend PM6:PY-DT as the research object, 2019B121205001). R. M. thanks the support by PolyU distin-
and fabricate a series of devices based on BC and SqP methods, guished Postdoctoral Fellowship.

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