Perylenocarbazole‐Based Polycyclic Aromatic Self‐Assembled Monolayers with Tailored Electrostatic Potentials for High‐Performance Organic and Perovskite Solar Cells
Abstract
ABSTRACT The development of universal hole‐transporting layers for organic and perovskite solar cells (OSCs/PSCs) remains challenging due to the lack of molecular strategies that precisely control interfacial energetics, molecular packing, and active layer morphology. Here, we report an electrostatic potential (ESP)‐guided approach to construct nitrogen‐containing polycyclic aromatic self‐assembled monolayers (SAMs) that address this challenge. By integrating a rigid, planar perylenocarbazole (PCz) core with extended π‐conjugation, alkyl chain optimization, and bromination, we designed two novel SAMs, 4PCzBr and 6PCzBr, with precisely tailored ESP distributions. Compared to conventional carbazole‐based SAMs, these designs substantially elevate the average ESP, strengthen intermolecular π–π interactions, and promote dense, ordered monolayer formation on ITO, thereby enhancing work function alignment and hole extraction. Interestingly, the elevated ESP of 6PCzBr strengthens electrostatic interactions with the donor PM6, driving preferential donor crystallization at the buried interface and establishing an ideal vertical phase separation for efficient charge transport. Leveraging this synergy, 6PCzBr‐based OSCs deliver an outstanding efficiency of 20.16%, while inverted PSCs achieve a remarkable efficiency of 26.20% with decent operation stability. This work establishes ESP‐engineered polycyclic aromatic SAMs as a versatile interfacial platform bridging organic and perovskite photovoltaics, offering a broadly applicable molecular design paradigm for high‐efficiency and stable solar cells.
Article Details
Authors (18)
Xing Chen
Institute of Molecular Plus, Department of Chemistry, Tianjin University and Haihe Laboratory of Sustainable Chemical Transformations, 92 Weijin Road, Tianjin 300072, China
Shuzhen Liao
Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education/National Engineering Research Center for Carbohydrate Synthesis College of Chemistry and Materials Jiangxi Normal University Nanchang China
Yonglong Yang
College of Chemistry and Materials/Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education/National Engineering Research Center for Carbohydrate Synthesis, Jiangxi Normal University Nanchang P. R. China
Yuang Fu
Department of Physics, The Chinese University of Hong Kong, Shatin, New Territories, Hong Kong, China
Mingtao Liu
Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education/National Engineering Research Center for Carbohydrate Synthesis College of Chemistry and Materials Jiangxi Normal University Nanchang China
Peipei Zhu
Weilin Zhou
Manjiang Yu
College of Biological and Chemical Engineering Jiaxing University Jiaxing China
Jin Li
Dan Liu
Yaoyao Zhu
Lin Hu
The High Magnetic Field Laboratory, Hefei Institutes of Physical Science
Yong Huo
Frontier Science Center for Rare Isotopes, School of Nuclear Science and Technology
Xiaopeng Xu
Aihui Liang
College of Chemistry and Materials/Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang 330022, China
Xinhui Lu
Department of Physics
Xunfan Liao
Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education/National Engineering Research Center for Carbohydrate Synthesis College of Chemistry and Materials Jiangxi Normal University Nanchang China
Yiwang Chen
College of Chemistry and Chemical Engineering/Film Energy Chemistry for Jiangxi Provincial Key Laboratory (FEC), Nanchang University, Nanchang, China.