RESEARCH ARTICLE

www.advenergymat.de

Elucidate the Thermal Degradation Mechanism of Y6-Based

Organic Solar Cells by Establishing Structure-Property
Correlation
Jingming Xin, Chao Zhao, Ziqi Geng, Wenyue Xue, Zhenyu Chen, Chunpeng Song,
Han Yan, Qiuju Liang, Zongcheng Miao,* Wei Ma,* and Jiangang Liu*

Organic solar cells (OSCs) achieved performance booming benefiting from 1. Introduction
the emerging of non-fullerene acceptors, while inadequate device stability Organic solar cells (OSCs) based on
hampers their further application. At present, the prevalent belief attributes the development of non-fullerene accep-
the inevitable thermal degradation of OSC device to morphological instability tors (NFAs), achieve impressive break-
caused by excessive phase separation and crystallization in the active layer through on power conversion efficiency
(PCE) over 19%.[1–3] Considerable de-
during device operation. However, it is inapplicable for state-of-art Y6-based
vice performance and competitive fabri-
devices which strongly degrade before large-scale morphology change. cation cost enable promising industrial-
Herein, an alternative degradation mechanism is elucidated wherein ization potential in manifold application
molecular orientation change and demixing induced performance degradation scenarios.[4,5] However, the stability issue
in Y6-based devices. Distinct from IT-4F-based counterpart, Y6-based devices of OSC devices restrict its practical op-
suffer severe thermal degradation dominated by open-circuit voltage (VOC ) eration, which attracts increasing atten-
tions from the community.[6] Although
and fill factor (FF) losses. The VOC loss is attributed to molecular orientation
extraordinary extrapolated lifetime over
transition of polymer donors from edge-on to face-on, leading to a strong decade has been realized in few OSC
built-in potential reduction and increase in non-radiative loss due to energy systems,[7,8] maintaining eligible device
level shifting. As for FF decay, discontinuous acceptor phases result in lifetime is still a challenge in most high-
electron mobility decrease by over orders of magnitude, originating from the performance systems compared to inor-
ganic photovoltaics. Especially, Y6-based
increased molecular stacking and phase separation. This work reveals the
OSCs with over 15% PCEs only yield
thermal degradation mechanism for Y6-based devices and correlates the operational lifetimes spanning hundred
photoelectric properties with morphology instability, which will offer guidance to thousand hours.[9–11] The inadequate
for improving the stability of high-performance OSCs. stability can be understood as devices
suffer severe performance degradation

J. Xin, C. Song, J. Liu Z. Miao

School of Electronics and Information Technological Institute of Materials & Energy Science (TIMES)
Northwestern Polytechnical University Xi’an Key Laboratory of Advanced Photo-Electronics Materials and
Xi’an 710129, P. R. China Energy Conversion Device
E-mail: jgliu@nwpu.edu.cn School of Electronic Information
C. Zhao, W. Xue, Z. Chen, H. Yan, W. Ma Xijing University
State Key Laboratory for Mechanical Behavior of Materials Xi’an 710123, P. R. China
Xi’an Jiaotong University E-mail: miaozongcheng@nwpu.edu.cn
Xi’an 710049, P. R. China Z. Miao
E-mail: msewma@xjtu.edu.cn School of Artificial Intelligence
Z. Geng, Q. Liang Optics and Electronics (iOPEN)
School of Microelectronics Northwestern Polytechnical University
Northwestern Polytechnical University Xi’an 710072, P. R. China
Xi’an 710129, P. R. China

The ORCID identification number(s) for the author(s) of this article

can be found under https://doi.org/10.1002/aenm.202401433
DOI: 10.1002/aenm.202401433

Adv. Energy Mater. 2024, 2401433 2401433 (1 of 12) © 2024 Wiley-VCH GmbH

www.advancedsciencenews.com
against external stresses and intrinsic instability.[12] Among all
types of degradation, thermal degradation is inevitable due
to high operational temperature under sunlight illumination,
which will affect active layer morphology.[13] Therefore, under-
standing and improving the thermal stability deserves to be a
significant research topic which contributes to device lifetime en-
hancement and further application.
To understand the thermal degradation mechanism, it should
be realized that the optimal morphology is usually kinet-
ically quenched and at thermodynamically non-equilibrium
state.[14–16] Further thermal-induced morphology evolution de-
viates from optimal morphology leading to device performance
degradation.[17,18] Ade and coworkers ascribed the critical fac-
tors controlling stability to demixing, crystallization and dif-
fusion on the basis of thermodynamics and kinetics.[19] This
is valid for most binary blend systems and highly related
to the material selection. Typically, fullerene derivative accep-
tors are known to present aggregation and phase coarsen-
ing forming oversize domains and large crystals even under
slight thermal stress due to their diffusive ability with spheri-
cal structure,[20,21] which are detrimental to exciton dissociation,
photo-generated charge carrier and consequently short-circuit
current density (JSC ).[22,23] Moreover, the spontaneous spinodal
demxing of deeply quenched polymer:fullerene blends occurs
even at room temperature, resulting in abnormal burn-in degra-
dation with large JSC loss at the early stage of device operation.[24]
After fullerene-based acceptors, ITIC-based NFAs were exten-
sively utilized to fabricate temporally high-performance devices
with considerable thermal stability. This is attributed to the large
fused-ring core structure enabling good miscibility with polymer
donors and limited molecular diffusion. It was demonstrated
that ITIC shows diffusion-limited crystallization below its high
glass transition temperature (Tg ≈ 180 °C), which only allows
locally reorganization.[25,26] The large-scale crystal growth and
phase separation are able to happen at extremely high temper-
ature above Tg , ensuring sufficient percolation channel and fa-
vorable morphological stability.[19,27] Interestingly, IT-4F exhibits
diffusion-limited aggregation when blending with different poly-
mer donors. Small isolated NFA molecules become morpholog-
ical traps in the polymer matrix, resulting in strong trap-assisted
recombination and fill factor (FF) degradation.[28] Under current
research background, the primary mechanism of thermal degra-
dation for fullerene- and ITIC-based OSCs has been delineated to
be miscibility and crystallization induced morphology evolution.
In recent years, Y6 and its derivatives achieved remark-
able PCE improvements,[29,30] primarily due to favorable spa-
tial molecular stacking and suitable phase separation.[31–34] Nev-
ertheless, the morphology stability of Y6 is inferior to ITIC-
based acceptors in blend films.[35,36] As Tg has been regarded
as a critical parameter to evaluate morphological stability, a se-
ries of Y6-based acceptors were confirmed to show pretty lower
Tg due to their long lengths of alkyl side chains originally de-
signed to increase the solubility.[37] The lower Tg indicates in-
trinsic instability and raises a performance-stability conundrum
for this type of NFAs. Meanwhile, the high diffusion coefficients
of Y6-based NFAs were measured in terms of bilayer interdiffu-
sion experiment, suggesting strong thermodynamic driven dif-
fusion within the blend films.[37,38] However, Alam et al. sug-
gested the inverted PM6:Y6 devices present gradual degrada-
Adv. Energy Mater. 2024, 2401433 2401433 (2 of 12)
16146840, 0, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/aenm.202401433 by Centro De Investigacion Y De Estudios Avanzados Del Inst, Wiley Online Library on [04/06/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advenergymat.de
tion when annealed much above its Tg , while JSC only exhibit
slightly decrease.[39] Uddin et al. reported strong burn-in loss in
PM6:N3 devices by around 50% PCE dropping without distinct
morphology change, which was speculated to be caused by inter-
face and electrode degradation.[40] We notice that Y6-based sys-
tems appear distinguishing thermal degradation less affected by
large-scale morphology change but the corresponding degrada-
tion mechanism, to our knowledge, is still obscure and rarely
studied. Therefore, analyzing how morphology affect the photo-
electric conversion processes basing on structure-property corre-
lation is urgently demanded for understanding the degradation
mechanism and improving the thermal stability of state-of-art Y6-
based OSC devices.
Herein, we investigate the thermal stability of representative
NFA Y6 combined with high-efficiency polymer donors D18 and
PM6 to elucidate the degradation mechanism of Y6-based devices
in comparison with PM6:IT-4F with favorable performance and
stability. After long-time annealing under 140 °C, significant per-
formance degradation can be observed in Y6-based devices due
to prominent open-circuit voltage (VOC ) and FF losses, which is
distinct from PM6:IT-4F blend and absence in their shelf stability
test. To explore such degradation, we carried out multiple photo-
electrical measurements for the devices before and after thermal
aging. The built-in potential was characterized to interpret VOC
loss with larger reduction for Y6-based devices after aging, which
was further confirmed by upshifted energy levels of D18, PM6
and Y6. Meanwhile, energy loss measurements present much
stronger non-radiative recombination in Y6-based devices, also
suggesting higher voltage loss after aging. Moreover, we noted
the electron mobility show orders of magnitude losses for all
aged blend devices, which is the reason for FF loss. To correlat-
ing the photoelectric degradation with blend film morphology,
X-ray scattering measurements indicate that the molecular ori-
entation of polymers in Y6-based blends apparently turned from
edge-on to face-on, while their molecular stacking and phase sep-
aration were enhanced as well. The increased face-on polymer
molecular orientation can be correlated to built-in potential and
non-radiative loss variation agreeing well with VOC loss, while in-
creased molecular stacking and phase separation break the con-
tinuous acceptor phases resulting in FF decay. Establishing the
correlation between morphology variation and specific device pa-
rameter loss, this work provide profound and novel insight into
thermal stability of representative Y6-based OSCs, which will in-
struct further morphology regulation and device fabrication for
high-performance and stable photovoltaics.
2. Results and Discussion
2.1. Device Performance and Thermal Stability Characterizations
The chemical structures of selected polymer donors (D18 and
PM6) and NFAs (Y6 and IT-4F) are shown in Figure 1a. Binary
OSC devices of D18:Y6, PM6:Y6 and PM6:IT-4F were fabricated
in inverted structure (Figure 1b), and the device fabrication de-
scription can be found in Supporting Information. The current
density-voltage (J-V) curves of optimized devices for three are
shown in Figure 1c, and Table S1 (Supporting Information)
lists the corresponding photovoltaic performance parameters.
Among them, D18:Y6 blend device presents the highest PCE
© 2024 Wiley-VCH GmbH
 16146840, 0, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/aenm.202401433 by Centro De Investigacion Y De Estudios Avanzados Del Inst, Wiley Online Library on [04/06/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advancedsciencenews.com www.advenergymat.de

Figure 1. a) The chemical structures of D18, PM6, Y6 and IT-4F, b) scheme of inverted device structure, c) J-V characteristics of optimized D18:Y6,
PM6:Y6 and PM6:IT-4F solar cells devices. The normalized (a) PCE, (b) JSC (c) VOC and d) FF as a function of annealing time for all devices under
140 °C annealing. The device parameters of each system are averaged from ten devices with error bars denoting the standard deviations.

of 17.01% with JSC of 26.78 mA/cm2 , VOC of 0.858 V and FF of
74.04%. PM6:Y6 blend exhibits slightly lower PCE of 15.75% due
to inferior VOC of 0.848 V and FF of 71.84%. As for PM6:IT-4F
blend, insufficient of JSC (19.36 mA/cm2 ) and FF (69.39%) lead
to lower PCE of 11.56% despite higher VOC (0.861 V). The ex-
ternal quantum efficiency (EQE) spectra (Figure S1, Supporting
Information) present the light harvesting and confirm JSC of
three blend devices.
As the photovoltaic devices were well prepared, we investigated
the thermal stability by annealing the fresh devices on 140 °C
hot plate and tracking their performance evolution in nitrogen
glovebox. This temperature is much higher than the Tg of Y6
blends, which could accelerate the morphology evolution. The
normalized performance parameters as a function of anneal-
ing time were presented to delineate the thermal stability. No-
tably, Y6-based devices suffer severe PCE degradation as shown
in Figure 1d, in which only 44% and 50% of the initial PCE were
maintained after 20 hours annealing. Analyzing the specific pa-
rameter evolution, all the three systems present minor current
density loss that over 90% of the initial JSC can be retained af-
ter 20 hours annealing (Figure 1e), while the JSC degradation
of IT-4F based devices is slightly larger than the Y6-based de-
vices. In Figure 1f, D18:Y6 and PM6:Y6 devices show similar loss
trend with about 71% of VOC left after 20 hours annealing, while
PM6:IT-4F devices keep 85% of the initial VOC . In Figure 1g,
D18:Y6 devices show the largest FF loss with only 65% of FF
left, and PM6:IT-4F devices present much smaller decay with
86% of the initial FF after annealing. In between, PM6:Y6 de-
vices still maintain 75% of initial FF compared to fresh devices.
Overall, it is evident to find that Y6-based devices show simi-
larly strong VOC decay induced thermal degradation compared
to more stable IT-4F-based devices during high temperature an-
nealing, which is seldom noticed and needs to be carefully in-
vestigated. Meanwhile, FF decay is also noteworthy for consider-
able contribution to PCE degradation, though it varies in differ-
ent blend systems. Considering interface layer plays an impor-
tant role in device stability, the conventional devices were fabri-
cated and tested under the same condition. As shown in Figure
S2 (Supporting Information), the conventional devices present
much severe degradation within only 10 minutes than inverted
devices, dominating by VOC losses over 44% and 37% of their
initial values for D18:Y6 and PM6:Y6. The instability of elec-
tron transportation layer of PDINO used in conventional devices
has been reported elsewhere.[41] Compared with inverted devices,

Adv. Energy Mater. 2024, 2401433 2401433 (3 of 12) © 2024 Wiley-VCH GmbH

www.advancedsciencenews.com
Figure 2. a–c) Jph -Veff curves for fresh and aged D18:Y6, PM6:Y6 and PM6:IT-4F devices, d) ionization potential diagram for pristine films before and
after aging obtained from UPS measurements, insert is the scheme of energy level determining Vbi , e) simulated J-V curves with varied Vbi .
the excessive degradation of conventional Y6-based devices, espe-
cially on VOC , can be attributed to interface deterioration. Hence,
the inverted structure can effectively lower the influence of in-
terface layer induced degradation during thermal annealing. In
addition, ZnO layer shows high photocatalytic activity with ac-
tive layer materials leading to photocatalytic degradation.[42] To
clarify the influence, shelf stability was also measured (Figure
S3, Supporting Information) at room temperature in glovebox,
showing satisfactory shelf stability Y6-based devices even better
than PM6:IT-4F after 20 hours storage. Compared to annealed
devices, shelf devices show similar JSC decay trend but negligi-
ble VOC and FF loss, indicating barely photocatalytic degradation
and the high temperature annealing induced losses in Y6-based
devices.
2.2. Voltage Loss Analysis and Charge Carrier Investigation
Since Y6-based devices lead similar and strong VOC loss trend
during thermal degradation, we carried out a series of investiga-
tion to explain this phenomenon. In OSC devices, built-in poten-
tial (Vbi ) is a critical parameter to affect the internal electric field
and the upper limit of VOC , which can be defined as the effec-
tive work function difference between electrodes often relating to
Fermi level of electrode and vacuum level of semiconductor.[43–45]
In order to obtain Vbi value, the photocurrent densities (Jph = JL –
JD ) were characterized and plotted as a function of effective volt-
age (Veff = Vbi – Vappl ) in Figure 2a–c, where JL and JD are the cur-
rent densities under light and dark conditions, Vappl is the applied
Adv. Energy Mater. 2024, 2401433 2401433 (4 of 12)
16146840, 0, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/aenm.202401433 by Centro De Investigacion Y De Estudios Avanzados Del Inst, Wiley Online Library on [04/06/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advenergymat.de
voltage, and Vbi can be extracted by the voltage at Jph = 0. Consid-
ering the major degradation occurs within 5 hours, all aged sam-
ples in this work are the films or devices annealed at 140 °C for
5 hours. The results show that the Vbi of fresh D18:Y6 and
PM6:Y6 devices are 0.907 and 0.902 V, while they dramatically de-
crease to 0.743 and 0.742 V after aging. Nevertheless, PM6:IT-4F
device shows moderate Vbi degradation from 0.945 to 0.852 V af-
ter aging. To understand such Vbi variation, it should be learned
that Fermi-pinning effect limits effective work function of elec-
trode contact, and thus Vbi of the device.[44,46] Three possible fac-
tors would affect Vbi , which are electrode work function, ener-
getic states of electrode/buffer layer interface energetic state and
active layer. If the former two factors are dominating, the Ohmic
contact will be damaged resulting in “S” shaped J-V curve and
extremely serious degradation even worse than in the conven-
tional devices.[43] They have also been studied and indicated the
validity of improving device stability by optimizing interface layer
toward high Vbi .[47,48] In our case, we only noticed the significant
Vbi losses in Y6-based devices which share the same electrodes
and interfacial layers with PM6:IT-4F. Without excessive degra-
dation in conventional devices, we are able to rationally specu-
late that the degradation is mainly attributed to the active layer,
though it is incapable to completely exclude the effect of inter-
face layer. The structural change of active layer induces different
energy level change, leading to distinct Vbi reduction in three in-
verted devices.
Ultraviolet photoelectron spectroscopy (UPS) was applied to
measure ionization potential and evaluate the highest occupied
molecular orbital (HOMO) level variation. Fresh and aged
© 2024 Wiley-VCH GmbH

www.advancedsciencenews.com
Table 1. Voltage loss parameters for fresh and aged D18:Y6, PM6:Y6 and PM6:IT-4F devices.
Device Eg [eV] qVOC VOC SQ
[eV] [eV]
D18:Y6 Fresh 1.413 0.852 1.000
Aged 1.391 0.670 0.981
PM6:Y6 Fresh 1.423 0.842 1.01
Aged 1.396 0.680 0.991
PM6:IT-4F Fresh 1.579 0.873 1.162
Aged 1.574 0.810 1.152
pristine films were prepared using the same condition in blend
films to measure energy level change of donor and acceptor,
respectively, as shown in Figures 2d and S4 (Supporting Informa-
tion). Apparently, D18 shows the largest HOMO level upshifting
of 0.28 eV from 5.42 to 5.17 eV and Y6 presents downshifting
HOMO level from 5.69 to 5.87 eV after aging. PM6 (processed by
CF with CN) presents large HOMO level upshifting from 5.20 to
5.03 eV and the HOMO level of aged Y6 processed with CN shifts
from 5.75 to 5.82 eV. As for PM6 and IT-4F combination, only
minor HOMO level upshifting of PM6 (processed by CB with
DIO) can be observed from 5.14 to 5.07 eV, while IT-4F slightly
downshift from 5.85 to 5.87 eV. According to the results, promi-
nent upshifted HOMO levels of polymer donors in Y6-based
systems can be connected to the larger Vbi reduction as depicted
in the insert scheme of Figure 2d. Usually, band bending at
anode contact is correlated to the energetic offset between donor
and anode. When two electrodes with different work functions
align, the corresponding band bending can be used to determine
Vbi . The fresh films with lower-lying HOMO levels form initially
large band bending as well as Vbi . After long-time annealing,
the HOMO level of polymer largely upshifts, minishing the
band bending with anode and consequently decreasing Vbi . The
significantly reduced Vbi results in severe VOC decay for Y6-based
devices. Nevertheless, PM6 (processed by CB with DIO) shows
small HOMO shifting leading to less reduced Vbi and VOC in
IT-4F based devices. As for acceptors, moderate downshifted
HOMO levels of Y6 can help to estimate the lowest unoccupied
molecular orbital (LUMO) levels downshifting of aged Y6, while
IT-4F presents negligible change after aging. The downshifted
LUMO levels reduce the band bending at cathode contact, which
further decrease Vbi for aged Y6-based devices.
To further verify the decline of Vbi resulting in VOC degrada-
tion, we also conduct electrical simulation to obtain J-V curves
based on the drift-diffusion-generation (DDG) model with Vbi as
a variable. As shown in Figure 2e, the simulated J-V curves ex-
hibit obvious decreasing of VOC from 0.815 to 0.655 V as the Vbi
was set from 0.94 to 0.75 V. The similar degradation trend con-
firms that built-in potential reduction is the reason of VOC loss,
which is significantly detrimental to the device thermal stability.
In parallel, energy loss (Eloss ) characterization is an effective
and frequently-used method to elucidate the voltage difference
in OSCs, which can be applied in our study for the fresh and
aged devices. The energy loss derive from the sum of ΔE1 , ΔE2
and ΔE3 , where ΔE1 and ΔE2 denote radiative recombination
above and below the band gap, and ΔE3 is due to non-radiative re-
combination. We first calculated photovoltaic band gap (Eg PV ) in
Adv. Energy Mater. 2024, 2401433 2401433 (5 of 12)
16146840, 0, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/aenm.202401433 by Centro De Investigacion Y De Estudios Avanzados Del Inst, Wiley Online Library on [04/06/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advenergymat.de
VOC rad ΔE1 ΔE2 [eV] ΔE3 [eV] Eloss [eV]
[eV] [eV]
0.920 0.413 0.080 0.181 0.674
0.906 0.410 0.075 0.224 0.709
0.927 0.414 0.082 0.134 0.629
0.908 0.405 0.083 0.196 0.685
1.049 0.418 0.113 0.212 0.742
1.037 0.421 0.115 0.231 0.767
terms of the derivative of sensitive EQE (sEQE) spectra. As shown
in Figure S5 (Supporting Information) and Table 1, Eg PV values
are 1.413, 1.423, and 1.579 eV for fresh D18:Y6, PM6:Y6 and
PM6:IT-4F, while the aged Eg PV are 1.391, 1.396 and 1.574 eV. The
stronger band gap narrowing of aged Y6-based devices agrees
with larger voltage degradation. These Y6-based devices show mi-
nor ΔE1 and ΔE2 changes after aging indicating the radiative re-
combination can hardly affect energy loss for long-time annealed
devices. Then, we measured electroluminescence (EL) spectra
for three systems to evaluate ΔE3 . As shown in Figure 3a–c, the
D18:Y6 and PM6:Y6 present larger EQEEL value reduction after
aging than the PM6:IT-4F counterpart, though their EQEEL val-
ues of fresh devices are higher. As a consequence, ΔE3 changes
from 0.181 to 0.224 eV, 0.134 to 0.196 eV and 0.212 to 0.231 eV
for aged D18:Y6, PM6:Y6 and PM6:IT-4F, respectively. Since
HOMO offset has been proved to greatly impact on ΔE3 ,[49,50]
the large upshifted donor HOMO levels and moderately down-
shifted Y6 HOMO levels result in increased HOMO offset ac-
cording to UPS results. This is consistent to the apparently larger
ΔE3 enhancements of Y6-based devices than PM6:IT-4F, which
indicates much stronger non-radiative recombination in aged Y6
devices. In addition, photoluminescence (PL) spectra show ap-
parently PL intensity decline of aged D18:Y6 and PM6:Y6 com-
pared to the fresh films in Figure S6 (Supporting Information).
As PL intensity is related to the radiative and non-radiative recom-
bination rate, such PL intensity decline confirms significantly
increased non-radiative recombination.[51,52] As for PM6:IT-4F
films in Figure S7c (Figure 2d), negligible PL enhancement af-
ter aging agrees with smaller ΔE3 change. Thus, the total Eloss of
Y6-based devices increase mainly due to enhanced non-radiative
recombination loss (Figure 3d and Table 1), which explain their
remarkable VOC loss.
To study the dramatic FF degradation of aged devices, the
charge-carrier recombination processes of different devices be-
fore and after aging were characterized in terms of the depen-
dence of VOC on different light intensity. In Figure 4a–c, the
slopes (S) of VOC as a function of light intensity were extracted
to be 1.08, 1.32 and 1.07 kT/q for D18:Y6, PM6:Y6 and PM6:IT-
4F, respectively, suggesting bimolecular recombination is pre-
dominant but relatively higher trap-assisted recombination in
PM6:Y6. After aging, the S values of D18:Y6 and PM6:Y6 slightly
decrease to 1.03 and 1.29 kT q−1 , while PM6:IT-4F increases to
1.09 kT q−1 showing stronger trap-assisted recombination. These
results suggest long-time aging barely change the recombination
type of Y6-based devices, though large performance degradation
can be found.
© 2024 Wiley-VCH GmbH

www.advancedsciencenews.com
Figure 3. EQEEL spectra for fresh and aged a) D18:Y6, b) PM6:Y6 and c) PM6:IT-4F devices, d) energy loss diagram including ΔE1 , ΔE2 , and ΔE3 for all
fresh and aged devices.
Besides, charge-carrier mobility was measured by space-
charge-limited current (SCLS) method (Figure S8, Supporting
Information) for hole and electron only devices. As shown
in Figure 4d and Table S3 (Supporting Information), fresh
D18:Y6 device with the best performance presents the highest
hole mobility (μh ) of 3.15 × 10−4 cm2 V−1 S−1 and electron
mobility (μe ) of 2.82 × 10−4 cm2 V−1 S−1 among all devices,
while aged device shows one order of magnitude smaller
μh of 4.55 × 10−5 cm2 V−1 S−1 and severe degraded μe of
9.27 × 10−7 cm2 V−1 S−1 over two orders of magnitude. The strong
degradation of both μh and μe as well as unbalanced charge-
carrier mobility lead to the largest FF loss for D18:Y6 devices.
Before and after aging, PM6:Y6 shows slight reduction of μh from
2.52 × 10−4 to 1.91 × 10−4 cm2 V−1 S−1 , and μe also greatly de-
creases from 9.08 × 10−5 to 1.06 × 10−6 cm2 V−1 S−1 . This allows
the smaller FF loss of PM6:Y6 than D18:Y6. As for PM6:IT-4F,
the μh increases from 1.14 × 10−4 to 1.83 × 10−4 cm2 V−1 S−1 , and
μe largely decreases from 8.34 × 10−5 to 6.05 × 10−7 cm2 V−1 S−1 .
We notice the thermal aging results in much more serious
degradation of μe than μh , which can be correlated to morphol-
ogy change and discussed in the following section. Furthermore,
we simulated J-V curves with varied charge mobility μ to verify
the charge mobility resulting in FF degradation. Due to the
accuracy limit of calculation, the charge mobility was controlled
from 3 × 10−4 to 5 × 10−5 cm2 V−1 S−1 obtaining decreasing
of FF from 79.09 to 72.61% in Figure 4e, which suggests the
importance of charge mobility affecting FF during the thermal
degradation.
Adv. Energy Mater. 2024, 2401433 2401433 (6 of 12)
16146840, 0, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/aenm.202401433 by Centro De Investigacion Y De Estudios Avanzados Del Inst, Wiley Online Library on [04/06/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advenergymat.de
In addition, the exciton dissociation efficiencies (Pdiss ) of de-
vices were evaluated from Jph -Veff curves (Figure 2a–c) to decrease
from 92.80% to 92.72% for D18:Y6 and increase from 90.29%
to 92.86% for PM6:Y6 after long-time annealing. The slightly in-
creased Pdiss can be attributed to the smallest dark current density
(Figure S9, Supporting Information) and increased saturated cur-
rent density after aging. Such minor changes and over 90% Pdiss
of Y6-based devices promise the relatively high and stable JSC . As
for PM6:IT-4F device, the Pdiss decreases from 85.31% to 83.53%
confirming the slightly larger loss of JSC .
2.3. Morphology Characterization and Calculation
Morphology evolution has always been regarded as a critical
factor in thermal stability research. Therefore, we characterized
the active layer morphology for fresh and aged films. Grazing
incident wide angle X-ray scattering (GIWAXS) measurements
were employed to detect the molecular stacking and orientation
respect to substrate. As the GIWAXS 2D patterns shown in
Figure S10 (Supporting Information), the well-defined and
broad 𝜋–𝜋 stacking peaks of acceptors can be observed in out-
of-plane direction and mixed lamellar stacking peaks of polymer
and NFAs for all three fresh and aged films. The 1D line-cuts
are plotted in Figure 5a, and the corresponding parameters are
summarized in Table 2 based on scattering line-cuts fitting.
The (010) peaks of Y6 locate at 1.74 and 1.75 Å−1 (d-spacing
of 3.61 and 3.58 Å) with coherence length (CL) of 2.75 and
© 2024 Wiley-VCH GmbH

www.advancedsciencenews.com
Figure 4. Light intensity dependent VOC curves for fresh and aged a) D18:Y6, b) PM6:Y6 and c) PM6:IT-4F devices, d) charge carrier mobility of fresh
and aged devices, e) simulated J-V curves with varied charge mobility.
2.53 nm for fresh D18:Y6 and PM6:Y6 film, respectively. The
aged films present narrower (010) d-spacing of 3.58 and 3.56 Å
and enhanced CL of 3.06 and 3.00 nm for D18:Y6 and PM6:Y6,
respectively, which confirms more ordered 𝜋–𝜋 stacking of
Y6 molecules. In contrast, IT-4F shows (010) peak at 1.75 Å−1
(d-spacing of 3.59 Å), of which the CL increases from 2.38 to
2.53 nm after aging. We found enhanced 𝜋–𝜋 stacking of Y6,
which can be confirmed by the redshift of Y6 absorption peaks
in ultraviolet-visible (UV–vis) absorption spectra (Figure S11a,b,
Supporting Information). Nevertheless, IT-4F shows slightly
increased molecular stacking without obvious change in absorp-
tion spectra after aging. Moreover, we focus on the (11-1) peaks
of Y6 as this molecular arrangement has been proved to facilitate
to vertical charge transport.[31] In D18:Y6 blend, the (11-1) peaks
shift from 0.42 to 0.40 Å−1 (d-spacing increase from 14.81 to
15.74 Å) with CL decreasing from 6.23 to 5.90 nm after aging.
The (11-1) peaks in PM6:Y6 blend locate at 0.44 and 0.43 Å−1
(d-spacing of 14.04 and 14.57 Å) before and after aging with
CL of 11.7 and 20.90 nm. As for the polymer donors in blends,
the (100) peak of D18 locates at 0.30 Å−1 (d-spacing of 20.73 Å)
with enhanced CL from 7.05 to 8.76 nm, while (100) CL of PM6
increases from 11.63 to 13.69 nm. The (100) CL of PM6 in IT-4F
blend increases from 22.27 to 26.94 nm, which are significantly
Adv. Energy Mater. 2024, 2401433 2401433 (7 of 12)
16146840, 0, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/aenm.202401433 by Centro De Investigacion Y De Estudios Avanzados Del Inst, Wiley Online Library on [04/06/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advenergymat.de
larger than that in PM6:Y6 blend. The molecular stacking of
polymer donors are prominently enhanced in all three blends.
The molecular orientation distribution are analyzed by extract-
ing the pole figures of (100) and (010) scattering peaks for three
blends denoting the orientation change of polymer donors and
NFAs, respectively. In Figure 5b–d, scattering intensity was cor-
rected by pole angle and normalized, then plotted as a function
of pole angle, where the pole angle is defined to be the angle be-
tween substrate normal and lamellar stacking direction. For all
blend films, polymer donors present edge-on dominant orienta-
tion as the apparently higher intensity from 0 to 35°. Interest-
ingly, the aged D18 and PM6 in Y6 blend films show increased
face-on orientation in terms of the elevated intensity from 40 to
90°, while annealing has no clear impact on the orientation of
PM6 in IT-4F blend. To quantitatively analyze orientation change,
we calculated the proportion of face-on and edge-on stacking.
Both face-on proportion of D18 and PM6 after annealing in-
crease from 6.86% to 10.97% and from 20.41% to 24.75%, re-
spectively, while PM6 in IT-4F blend shows barely face-on tran-
sition from 15.81% to 15.94%. As for the acceptor orientation
based on (010) pole figures, Y6 molecules present slightly en-
hanced face-on orientation after aging, which is confirmed by
the face-on proportion from 90.43% to 93.67% in D18:Y6 and
© 2024 Wiley-VCH GmbH
 16146840, 0, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/aenm.202401433 by Centro De Investigacion Y De Estudios Avanzados Del Inst, Wiley Online Library on [04/06/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advancedsciencenews.com www.advenergymat.de

Figure 5. a) GIWAXS 1D line-cuts along in-plane (IP) and out-of-plane (OOP) direction of fresh and aged films for D18:Y6, PM6:Y6 and PM6:IT-4F
blends, (100) and (010) pole figures of fresh and aged films for b) D18:Y6, c) PM6:Y6 and d) PM6:IT-4F blends, distribution of frontier molecular orbitals
(HOMO) for e) edge-on and f) face-on D18 monomers at B3LYP/6-31G level of theory.

from 92.18% to 93.40% in PM6:Y6. IT-4F maintains stable face-
on orientation from 86.14% to 86.05%. Overall, the polymers in
Y6 blend present strikingly molecular orientation transition from
edge-on to face-on after aging, while PM6 and IT-4F maintain
their original orientations with negligible change.
Molecular orientation can effectively alter the energy level
of conjugated molecules by affecting electronic polarization
direction and electrostatic interaction,[53–55] whereas orienta-
tion dependent polarization energy quantitatively determines
the energy level of solid film.[56] Since D18 exhibits obvious
energy level shifting after orientation transition, we further
introduced density functional theory (DFT) simulation on
simplified D18 monomers without side-chain to evaluate their
frontier molecular orbitals in edge-on and face-on orientation
(Figure 5e,f; Figure S12, Supporting Information). It is promi-
nent to see less HOMO energy of −4.77 eV for face-on packing
D18 molecules with increased 𝜋–𝜋 stacking compared to edge-
on (−4.85 eV), which correlates molecular orientation with
energy level and confirms the upshifted HOMO level in UPS
results.
After investigating the molecular packing and orientation
change, we turned to miscibility and phase separation character-
ization. First, contact angle measurements were conducted for
pure donor and acceptor films as shown in Figure S13 and Table
S4 (Supporting Information). The corresponding Flory-Huggins
interaction parameters (𝜒) of D18:Y6, PM6:Y6 and PM6:IT-4F
were calculated to be 0.74, 0.45 and 0.99, respectively. A small 𝜒
of PM6:Y6 blend denotes highly miscible nature, while PM6 and

Table 2. Morphology parameters for fresh and aged blend films based on GIWAXS and RSoXS scattering curves fitting.

Sample In-plane (100) Out-of-plane (010) Domain size Relative

/nm domain
Location/Å−1 d-spacing/Å CL/nm Location/Å−1 d-spacing/Å CL/nm purity

D18:Y6 Fresh 0.303 20.73 7.05 1.741 3.61 2.75 17.6 1.00
Aged 0.300 20.90 8.76 1.754 3.58 3.06 25.2 0.74
PM6:Y6 Fresh 0.295 21.29 11.63 1.751 3.59 2.53 27.0 1.00
Aged 0.295 21.29 13.69 1.764 3.56 3.00 34.1 0.83
PM6:IT-4F Fresh 0.298 21.07 22.27 1.749 3.59 2.38 45.6 0.88
Aged 0.295 21.29 26.94 1.750 3.59 2.53 41.4 1.00

Adv. Energy Mater. 2024, 2401433 2401433 (8 of 12) © 2024 Wiley-VCH GmbH

www.advancedsciencenews.com
Figure 6. RSoXS 1D profiles of fresh and aged films for a) D18:Y6, b) PM6:Y6, and c) PM6:IT-4F blends, molecular conformation side view of d) edge-on
D18 with Y6, e) face-on D18 with Y6 and f) edge-on D18 with IT-4F from DFT calculation at GGA/BLYP level of theory.
IT-4F are prone to form large phase separation morphology due
to the largest 𝜒 value.
Then, resonant soft X-ray scattering (RSoXS) measurements
were applied to analyze the phase separation for fresh and aged
blend films. Figure 6a–c plot the RSoXS profiles acquired at
285.2 eV X-ray exposure for desired material contrast. The log-
normal distribution scattering peaks denote the length scale
of phase separation, which need to be contrasted with surface
roughness acquired at 270 eV (Figure S14, Supporting Informa-
tion). We noted that the peak positions of Y6-based films shift to
lower q after aging, indicating increased phase separation. The
quantitative domain sizes were calculated (Table 2) to be 17.6 and
25.2 nm for fresh and aged D18:Y6 blends, and increase from
27.0 to 34.1 nm for PM6:Y6 blends. The larger domain size of
PM6:Y6 can be attributed to the addition of CN in spite of its
smallest 𝜒. Moreover, the relative domain purities before and
after aging were evaluated to be from 1.00 to 0.74 for D18:Y6
and from 1.00 to 0.83 for PM6:Y6, which indicates to form more
mixed but large-size phases after long time annealing. As for
PM6:IT-4F, the fresh and aged films present domain sizes of
45.6 and 41.4 nm prominently larger than the Y6 counterparts,
agreeing with the largest Flory-Huggins interaction parameter.
Although no domain size enlarges after annealing, the relative
domain purity of this blend increases from 0.88 to 1.00. We think
it is due to the annealing temperature is still lower than the Tg of
IT-4F (≈170 °C),[57] which only allows local molecular ordering
forming purer domains instead of phase coarsening.
We noticed that the phase separation change is consistent with
the extent of orientation transition in three blends, in which Y6-
based blends with the large domain size enhancements show
Adv. Energy Mater. 2024, 2401433 2401433 (9 of 12)
16146840, 0, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/aenm.202401433 by Centro De Investigacion Y De Estudios Avanzados Del Inst, Wiley Online Library on [04/06/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advenergymat.de
the prominent orientation transition, but no orientation transi-
tion in an immiscible IT-4F-based blend. These suggest differ-
ent polymer:NFA combinations exhibit distinct impact on orien-
tation change after aging. It is rational to infer that the molec-
ular orientation transition in aging blend can be correlated to
intermolecular interaction induced demixing.[58] We attempt to
verify this argument by DFT simulation for the interaction be-
tween orientated D18 and two NFAs. The molecular electrostatic
potential (ESP) maps of them were calculated and show reverse
ESP values of D18 and acceptors at the conjugated planes in
Figure S15 (Supporting Information), which suggest stronger in-
termolecular interaction for parallel arrangement of D/A conju-
gated planes. Then, we calculated the intermolecular binding en-
ergy (EInt ) between edge-on/face-on D18 with two acceptors. As
shown in Figure 6d,e, it is no doubt that edge-on D18 presents
smaller EInt of −5.94 kJ mol−1 with Y6 than face-on D18 with Y6
(−7.42 kJ mol−1 ), indicating lower interaction between edge-on
D18 with Y6 and tending to demix and transform into face-on
with higher interaction. As for edge-on D18 blending with IT-4F,
the larger EInt of −6.62 kJ mol−1 suggests their stronger inter-
molecular interaction and stable phase behavior during thermal
aging.
2.4. Degradation Mechanism Discussion
Having the photoelectric and morphological results, we attempt
to correlate them together to analyze the underlying reason of
thermal degradation in Y6-based devices that VOC and FF losses
leading predominate parameter decay rather than JSC (depicted
© 2024 Wiley-VCH GmbH

www.advancedsciencenews.com
Figure 7. Scheme of morphology change induced thermal degradation.
in Figure 7). Considering the VOC degradation, prominently re-
duced Vbi and increased non-radiative recombination loss were
simultaneously probed to interpret voltage loss of aged Y6-based
devices. Taking account of the morphology change, molecular
orientation transitions of polymer donors appear from edge-on
to face-on after aging. The increasing face-on orientations of D18
and PM6 result in upshifted HOMO levels then lower Vbi af-
ter aging. Meanwhile, more face-on orientation alignment can
lead to higher non-radiative recombination then larger energy
loss, which is interpreted that face-on with larger electronic cou-
pling induces more charge recombination via charge-transfer
state decay.[59] Besides, the enhanced molecular stacking are well-
known factors in lowering device voltage. As for PM6:IT-4F films,
thermal aging show very little impact on molecular orientation
enabling fairly stability of aged devices.
The FF loss is primarily derived from drastic decay of electron
mobility in aged devices. Since the (11-1) packing of Y6 shows
prominent correlation with charge mobility and FF according to
Liu et al.’s work,[31] we notice the reduced CL (Table S5, Support-
ing Information) in D18:Y6, indicating less (11-1) packing and
smaller crystallite size after aging. This is probably due to the
demixing and strong aggregation of D18 which breaks the inter-
penetrating packing network of Y6 into dispersed crystallites in
terms of lower domain purity. Such unfavorable morphology is
detrimental to electron transportation, leading to the most dra-
matic mobility and FF decay in the corresponding devices. The
increased (11-1) CL and lower purity of aged PM6:Y6 suggest less
impact of demixing on Y6 packing, resulting in less mobility and
FF degradation. The slightly degraded FF in aged PM6:IT-4F is
ascribed to more trap-assistant recombination due to local demix-
ing in terms of increased domain purity.
The JSC degradation, which is common in other systems, is
barely observed in Y6-based devices during thermal stability test.
Referring to GIWAXS and RSoXS results, the molecular order-
ing and domain size are apparently enhanced after long-time
annealing above the Tg of Y6. Nevertheless, the crystallites in
Y6-based blends neither damage the optimized morphology nor
Adv. Energy Mater. 2024, 2401433 2401433 (10 of 12)
16146840, 0, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/aenm.202401433 by Centro De Investigacion Y De Estudios Avanzados Del Inst, Wiley Online Library on [04/06/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advenergymat.de
short-circuit the charge transportation channels. And their do-
main sizes are slightly exceeding the ideal phase separation size
but within the large exciton diffusion length in Y6 blends,[60,61]
which ensures sufficient photocurrent generation and prevents
drastic JSC loss. Thus, it would be rational to acknowledge that
thermal induced crystallization and phase separation are not the
reason for Y6-based device degradation. On the contrary, the an-
nealing temperature of 140 °C span a polymorphic phase tran-
sition of IT-4F, which can be confirmed by increased purity but
slightly decreased domain size. This results in relatively larger
JSC loss, even if the Tg of IT-4F is much higher than Y6. The
polymorphic effect of IDTT-based NFAs has been reported to im-
pact device performance and stability by our previous work and
elsewhere.[26,62]
3. Conclusion
In summary, the thermal stability of Y6-based OSCs was carefully
investigated to uncover the degradation mechanism in compar-
ison with PM6:IT-4F. Instead of JSC decay, D18:Y6 and PM6:Y6
devices exhibit drastic VOC and FF losses under 140 °C annealing,
resulting in larger device performance degradation. The device
characterizations before and after aging reveal prominent built-in
potential decline and strong non-radiative loss in aged Y6-based
devices leading to the VOC loss. Meanwhile, great electron mobil-
ity depression can be found to suggest the degradation of FF. To
correlate the photoelectric properties deterioration with thermal
induced morphology change, we further carried on morphology
characterizations. Although molecular stacking and phase sepa-
ration are enhanced after annealing, the polymer molecular ori-
entation turning from edge-on to face-on and D/A orientation
alignment are the critical factors affecting energy level and built-
in potential which ultimately lower the VOC of devices. More-
over, the FF degradation is due to the isolated NFA phases breaks
the electron transportation channel. Our investigation elucidate
the thermal degradation mechanism in efficient Y6-based devices
and correlated with thermal induced morphology change, which
© 2024 Wiley-VCH GmbH

www.advancedsciencenews.com
contribute to stability improving strategy for high-performance
OSC devices.
Supporting Information
Supporting Information is available from the Wiley Online Library or from
the author.
Acknowledgements
The project was supported by the National Natural Science Foundation
of China (52073231, 62304181), the Shaanxi Provincial High level Tal-
ent Introduction Project (5113220044), the Shaanxi Outstanding Youth
Project (2023-JC-JQ-33), the Youth Science and Technology Talent Pro-
motion Project of Jiangsu Association for Science and Technology (TJ-
2022-088), the China Postdoctoral Science Foundation (2023TQ0273,
2023TQ0274), the Natural Science Basic Research Program of Shaanxi
(2023-JC-QN-0726), Guangdong Basic and Applied Basic Research Foun-
dation (2022A1515110286), the Fundamental Research Funds for the Cen-
tral Universities (G2022KY05108, G2023KY0605), the NWPU research
fund for young scholars (G2022WD01014), the Natural Science Foun-
dation of Chongqing, China (cstc2021jcyj-msxmX0990), the Basic Re-
search Programs of Taicang, 2021 (TC2021JC08), the Suzhou Science
and Technology Development Plan Innovation Leading Talent Project
(ZXL2023183) and the NWPU Degree and Graduate Education Fund
(2022AJ12, 2022AJ22). X-ray data was acquired at beamlines 7.3.3 and
11.0.1.2 at the Advanced Light Source, which was supported by the Di-
rector, Office of Science, Office of Basic Energy Sciences, of the U.S. De-
partment of Energy under Contract No. DE-AC02-05CH11231. The authors
thank Dr. Eric Schaible and Dr. Chenhui Zhu at beamline 7.3.3, and Dr.
Cheng Wang at beamline 11.0.1.2 for assistance with data acquisition.
Conflict of Interest
The authors declare no conflict of interest.
Data Availability Statement
The data that support the findings of this study are available from the cor-
responding author upon reasonable request.
Keywords
molecular orientation, non-fullerene acceptor, organic solar cells, phase
separation, stability
Received: March 29, 2024
Revised: April 23, 2024
Published online:
[1] Y. Wei, Z. Chen, G. Lu, N. Yu, C. Li, J. Gao, X. Gu, X. Hao, G. Lu, Z.
Tang, J. Zhang, Z. Wei, X. Zhang, H. Huang, Adv. Mater. 2022, 34,
2204718.
[2] L. Zhu, M. Zhang, J. Xu, C. Li, J. Yan, G. Zhou, W. Zhong, T. Hao,
J. Song, X. Xue, Z. Zhou, R. Zeng, H. Zhu, C.-C. Chen, R. C. I.
MacKenzie, Y. Zou, J. Nelson, Y. Zhang, Y. Sun, F. Liu, Nat. Mater.
2022, 21, 656.
Adv. Energy Mater. 2024, 2401433 2401433 (11 of 12)
16146840, 0, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/aenm.202401433 by Centro De Investigacion Y De Estudios Avanzados Del Inst, Wiley Online Library on [04/06/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advenergymat.de
[3] W. Gao, F. Qi, Z. Peng, F. R. Lin, K. Jiang, C. Zhong, W. Kaminsky, Z.
Guan, C.-S. Lee, T. J. Marks, H. Ade, A. K. Y. Jen, Adv. Mater. 2022, 34,
2202089.
[4] J. Guo, J. Min, Adv. Energy Mater. 2019, 9, 1802521.
[5] Y.-F. Shen, H. Zhang, J. Zhang, C. Tian, Y. Shi, D. Qiu, Z. Zhang, K.
Lu, Z. Wei, Adv. Mater. 2023, 35, 2209030.
[6] Q. Burlingame, M. Ball, Y.-L. Loo, Nat. Energy 2020, 5, 947.
[7] Q. Burlingame, X. Huang, X. Liu, C. Jeong, C. Coburn, S. R. Forrest,
Nature 2019, 573, 394.
[8] X. Du, T. Heumueller, W. Gruber, A. Classen, T. Unruh, N. Li, C. J.
Brabec, Joule 2019, 3, 215.
[9] X. Xu, D. Li, J. Yuan, Y. Zhou, Y. Zou, EnergyChem 2021, 3,
100046.
[10] W. Li, D. Liu, T. Wang, Adv. Funct. Mater. 2021, 31, 2104552.
[11] J. Luke, E. J. Yang, C. Labanti, S. Y. Park, J.-S. Kim, Nat. Rev. Mater.
2023, 8, 839.
[12] P. Cheng, X. Zhan, Chem. Soc. Rev. 2016, 45, 2544.
[13] L. Ye, M. Gao, J. Hou, Sci. China: Chem. 2021, 64, 1875.
[14] L. Ye, S. Li, X. Liu, S. Zhang, M. Ghasemi, Y. Xiong, J. Hou, H. Ade,
Joule 2019, 3, 443.
[15] L. Ye, B. A. Collins, X. Jiao, J. Zhao, H. Yan, H. Ade, Adv. Energy Mater.
2018, 8, 1703058.
[16] Q. Liang, W. Li, H. Lu, Z. Yu, X. Zhang, Q. Dong, C. Song, Z. Miao, J.
Liu, ACS Appl. Energy Mater. 2023, 6, 31.
[17] J. Xin, J. Feng, B. Lin, H. B. Naveed, J. Xue, N. Zheng, W. Ma, Small
2022, 18, 2200608.
[18] Q. Liang, Y. C., C. Liang, H. Zhu, Z. Guo, J. Liu, Acta Phys.-Chim. Sin.
2023, 39, 2212006.
[19] M. Ghasemi, H. Hu, Z. Peng, J. J. Rech, I. Angunawela, J. H.
Carpenter, S. J. Stuard, A. Wadsworth, I. McCulloch, W. You, Joule
2019, 3, 1328.
[20] S. Pont, F. Foglia, A. M. Higgins, J. R. Durrant, J. T. Cabral, Adv. Funct.
Mater. 2018, 28, 1802520.
[21] A. D. de Zerio, C. Müller, Adv. Energy Mater. 2018, 8, 1702741.
[22] J. Bergqvist, C. Lindqvist, O. Bäcke, Z. Ma, Z. Tang, W. Tress, S.
Gustafsson, E. Wang, E. Olsson, M. R. Andersson, O. Inganäs, C.
Müller, J. Mater. Chem. A 2014, 2, 6146.
[23] C. Müller, J. Bergqvist, K. Vandewal, K. Tvingstedt, A. S. Anselmo, R.
Magnusson, M. I. Alonso, E. Moons, H. Arwin, M. Campoy-Quiles,
O. Inganäs, J. Mater. Chem. 2011, 21, 10676.
[24] N. Li, J. D. Perea, T. Kassar, M. Richter, T. Heumueller, G. J. Matt, Y.
Hou, N. S. Güldal, H. Chen, S. Chen, S. Langner, M. Berlinghof, T.
Unruh, C. J. Brabec, Nat. Commun. 2017, 8, 14541.
[25] L. Yu, D. Qian, S. Marina, F. A. A. Nugroho, A. Sharma, S. Hultmark,
A. I. Hofmann, R. Kroon, J. Benduhn, D.-M. Smilgies, K. Vandewal,
M. R. Andersson, C. Langhammer, J. Martín, F. Gao, C. Müller, ACS
Appl. Mater. Interfaces 2019, 11, 21766.
[26] J. Xin, H. Zhao, J. Xue, S. Seibt, B. A. Collins, W. Ma, Sol. RRL 2022,
6, 2200819.
[27] J. Xin, X. Meng, X. Xu, Q. Zhu, H. B. Naveed, W. Ma, Matter 2019, 1,
1316.
[28] X. Du, T. Heumueller, W. Gruber, O. Almora, A. Classen, J. Qu, F. He,
T. Unruh, N. Li, C. J. Brabec, Adv. Mater. 2020, 32, 1908305.
[29] J. Yuan, Y. Zhang, L. Zhou, G. Zhang, H.-L. Yip, T.-K. Lau, X. Lu, C.
Zhu, H. Peng, P. A. Johnson, M. Leclerc, Y. Cao, J. Ulanski, Y. Li, Y.
Zou, Joule 2019, 3, 1140.
[30] Y. Liu, B. Liu, C.-Q. Ma, F. Huang, G. Feng, H. Chen, J. Hou, L. Yan, Q.
Wei, Q. Luo, Q. Bao, W. Ma, W. Liu, W. Li, X. Wan, X. Hu, Y. Han, Y. Li,
Y. Zhou, Y. Zou, Y. Chen, Y. Li, Y. Chen, Z. Tang, Z. Hu, Z.-G. Zhang,
Z. Bo, Sci. China: Chem. 2022, 65, 224.
[31] L. Zhu, M. Zhang, G. Zhou, T. Hao, J. Xu, J. Wang, C. Qiu, N. Prine, J.
Ali, W. Feng, X. Gu, Z. Ma, Z. Tang, H. Zhu, L. Ying, Y. Zhang, F. Liu,
Adv. Energy Mater. 2020, 10, 1904234.
[32] D. Li, X. Zhang, D. Liu, T. Wang, J. Mater. Chem. A 2020, 8, 15607.
© 2024 Wiley-VCH GmbH

www.advancedsciencenews.com
[33] L. Zhu, M. Zhang, W. Zhong, S. Leng, G. Zhou, Y. Zou, X. Su, H. Ding,
P. Gu, F. Liu, Y. Zhang, Energy Environ. Sci. 2021, 14, 4341.
[34] J. Xin, W. Li, Y. Zhang, Q. Liang, C. Song, Y. Zhao, Z. He, J. Liu, W. Ma,
Battery Energy 2023, 2, 20220040. [50]
[35] Y. Wang, J. Lee, X. Hou, C. Labanti, J. Yan, E. Mazzolini, A. Parhar, J. [51]
Nelson, J.-S. Kim, Z. Li, Adv. Energy Mater. 2021, 11, 2003002.
[36] Y. Liang, D. Zhang, Z. Wu, T. Jia, L. Lüer, H. Tang, L. Hong, J. Zhang,
K. Zhang, C. J. Brabec, N. Li, F. Huang, Nat. Energy 2022, 7, 1180. [52]
[37] Y. Qin, N. Balar, Z. Peng, A. Gadisa, I. Angunawela, A. Bagui, S.
Kashani, J. Hou, H. Ade, Joule 2021, 5, 2129. [53]
[38] M. Ghasemi, N. Balar, Z. Peng, H. Hu, Y. Qin, T. Kim, J. J. Rech, M.
Bidwell, W. Mask, I. McCulloch, W. You, A. Amassian, C. Risko, B. T.
O’Connor, H. Ade, Nat. Mater. 2021, 20, 525. [54]
[39] S. Alam, H. Aldosari, C. E. Petoukhoff, T. Váry, W. Althobaiti, M. [55]
Alqurashi, H. Tang, J. I. Khan, V. Nádaždy, P. Müller-Buschbaum, G.
C. Welch, F. Laquai, Adv. Funct. Mater. 2024, 34, 2308076. [56]
[40] L. Duan, Y. Zhang, M. He, R. Deng, H. Yi, Q. Wei, Y. Zou, A. Uddin,
ACS Appl. Mater. Interfaces 2020, 12, 27433. [57]
[41] H. Bin, J. Wang, J. Li, M. M. Wienk, R. A. J. Janssen, Adv. Mater. 2021,
33, 2008429. [58]
[42] Y. Jiang, L. Sun, F. Jiang, C. Xie, L. Hu, X. Dong, F. Qin, T. Liu, L. Hu,
X. Jiang, Y. Zhou, Mater. Horiz. 2019, 6, 1438. [59]
[43] C. Zhao, C. G. Tang, Z.-L. Seah, Q.-M. Koh, L.-L. Chua, R.-Q. Png, P.
K. H. Ho, Nat. Commun. 2021, 12, 2250. [60]
[44] M. Mingebach, C. Deibel, V. Dyakonov, Phys. Rev. B 2011, 84, 153201.
[45] B. Liu, R.-Q. Png, J.-K. Tan, P. K. H. Ho, Adv. Energy Mater. 2014, 4,
1200972. [61]
[46] N. Tessler, J. Appl. Phys. 2015, 118, 215501.
[47] Y. Wang, W. Lan, N. Li, Z. Lan, Z. Li, J. Jia, F. Zhu, Adv. Energy Mater.
2019, 9, 1900157. [62]
[48] Y. Wang, J. Han, L. Cai, N. Li, Z. Li, F. Zhu, J. Mater. Chem. A 2020, 8,
21255.
[49] D. Qian, Z. Zheng, H. Yao, W. Tress, T. R. Hopper, S. Chen, S. Li, J.
Liu, S. Chen, J. Zhang, X.-K. Liu, B. Gao, L. Ouyang, Y. Jin, G. Pozina,
Adv. Energy Mater. 2024, 2401433 2401433 (12 of 12)
16146840, 0, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/aenm.202401433 by Centro De Investigacion Y De Estudios Avanzados Del Inst, Wiley Online Library on [04/06/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advenergymat.de
I. A. Buyanova, W. M. Chen, O. Inganäs, V. Coropceanu, J.-L. Bredas,
H. Yan, J. Hou, F. Zhang, A. A. Bakulin, F. Gao, Nat. Mater. 2018, 17,
703.
D. He, F. Zhao, C. Wang, Y. Lin, Adv. Funct. Mater. 2022, 32, 2111855.
M. S. Gaponenko, A. A. Lutich, N. A. Tolstik, A. A. Onushchenko, A.
M. Malyarevich, E. P. Petrov, K. V. Yumashev, Phys. Rev. B 2010, 82,
125320.
A. D. Platt, M. J. Kendrick, M. Loth, J. E. Anthony, O. Ostroverkhova,
Phys. Rev. B 2011, 84, 235209.
Y. Fu, T. H. Lee, Y.-C. Chin, R. A. Pacalaj, C. Labanti, S. Y. Park, Y.
Dong, H. W. Cho, J. Y. Kim, D. Minami, J. R. Durrant, J.-S. Kim, Nat.
Commun. 2023, 14, 1870.
B. J. Topham, Z. G. Soos, Phys. Rev. B 2011, 84, 165405.
J. Liu, H. Lu, Y. Yin, K. Wang, P. Wei, C. Song, Z. Miao, Q. Liang, Battery
Energy 2022, 1, 20220013.
H. Yoshida, K. Yamada, J. y. Tsutsumi, N. Sato, Phys. Rev. B 2015, 92,
075145.
L. Ciammaruchi, O. Zapata-Arteaga, E. Gutiérrez-Fernández, J.
Martin, M. Campoy-Quiles, Mater. Adv. 2020, 1, 2846.
Q. Liang, M. Duan, Z. Geng, M. Zhang, W. Xu, H. Geng, Z. He, J. Liu,
Chem. Eng. J. 2024, 488, 150783.
Y. Yi, V. Coropceanu, J.-L. Brédas, J. Am. Chem. Soc. 2009, 131,
15777.
N. Tokmoldin, S. M. Hosseini, M. Raoufi, L. Q. Phuong, O. J.
Sandberg, H. Guan, Y. Zou, D. Neher, S. Shoaee, J. Mater. Chem. A
2020, 8, 7854.
N. Tokmoldin, J. Vollbrecht, S. M. Hosseini, B. Sun, L. Perdigón-Toro,
H. Y. Woo, Y. Zou, D. Neher, S. Shoaee, Adv. Energy Mater. 2021, 11,
2100804.
S. Marina, A. D. Scaccabarozzi, E. Gutierrez-Fernandez, E. Solano, A.
Khirbat, L. Ciammaruchi, A. Iturrospe, A. Balzer, L. Yu, E. Gabirondo,
X. Monnier, H. Sardon, T. D. Anthopoulos, M. Caironi, M. Campoy-
Quiles, C. Müller, D. Cangialosi, N. Stingelin, J. Martin, Adv. Funct.
Mater. 2021, 31, 2103784.
© 2024 Wiley-VCH GmbH