TY - JOUR
T1 - Achieving Uniform Phase Structure for Layer-by-Layer Processed Binary Organic Solar Cells with 20.2% Efficiency
AU - Wang, Hao
AU - Zhang, Busheng
AU - Wang, Liming
AU - Guo, Xia
AU - Mei, Le
AU - Cheng, Bo
AU - Sun, Wei
AU - Kan, Lixuan
AU - Xia, Xinxin
AU - Hao, Xiaotao
AU - Geue, Thomas
AU - Liu, Feng
AU - Zhang, Maojie
AU - Chen, Xian-Kai
PY - 2025/7/14
Y1 - 2025/7/14
N2 - Layer-by-layer (LBL) deposition has become a facile and promising method to fabricate highly efficient organic solar cells (OSCs). However, characterization and optimization of 3D morphology remain a grand challenge for LBL-processed active layers, and their correlation with photovoltaic properties of OSC devices is not clear to date. Here, to address this issue, the morphology and its formation mechanisms of LBL-processed active layer based on the classical D18/L8-BO blend were investigated systematically. Intriguingly, a unique 3D nanomorphology is achieved and uncovered within the LBL processed active layer, which highlights a highly uniform and “zigzag”-shaped phase structure formed by the intersection of donor and acceptor aggregates along horizontal direction in the middle-depth layer, rarely found in bulk heterojunction (BHJ) films processed by blend casting. Our results revealed that solid additive DBM with a twisted conformation plays a crucial role in achieving the uniform phase structure of LBL-deposited active layer. Consequently, the characteristic 3D morphology of LBL-processed device significantly improves short-circuit current and fill factor, enabling an impressive PCE of 20.2% in such binary device. Therefore, this work unambiguously demonstrates a unique 3D nanomorphology within LBL active layer, unveils the morphology manipulation mechanism, and their correlation with optoelectronic properties of OSCs. © 2025 Wiley-VCH GmbH.
AB - Layer-by-layer (LBL) deposition has become a facile and promising method to fabricate highly efficient organic solar cells (OSCs). However, characterization and optimization of 3D morphology remain a grand challenge for LBL-processed active layers, and their correlation with photovoltaic properties of OSC devices is not clear to date. Here, to address this issue, the morphology and its formation mechanisms of LBL-processed active layer based on the classical D18/L8-BO blend were investigated systematically. Intriguingly, a unique 3D nanomorphology is achieved and uncovered within the LBL processed active layer, which highlights a highly uniform and “zigzag”-shaped phase structure formed by the intersection of donor and acceptor aggregates along horizontal direction in the middle-depth layer, rarely found in bulk heterojunction (BHJ) films processed by blend casting. Our results revealed that solid additive DBM with a twisted conformation plays a crucial role in achieving the uniform phase structure of LBL-deposited active layer. Consequently, the characteristic 3D morphology of LBL-processed device significantly improves short-circuit current and fill factor, enabling an impressive PCE of 20.2% in such binary device. Therefore, this work unambiguously demonstrates a unique 3D nanomorphology within LBL active layer, unveils the morphology manipulation mechanism, and their correlation with optoelectronic properties of OSCs. © 2025 Wiley-VCH GmbH.
KW - Aggregation kinetics
KW - Layer-by-layer deposition
KW - Organic solar cells
KW - Phase structure
KW - Twisted additive
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U2 - 10.1002/anie.202508257
DO - 10.1002/anie.202508257
M3 - RGC 21 - Publication in refereed journal
SN - 1433-7851
VL - 64
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 29
M1 - e202508257
ER -