N‐Heterocycle‐Activated π‐Cooperative Coordination for Enhancing Structural Stability of Perovskite Solar Cells

Y Yuanshan Xiao (Centre for Advanced Optoelectronics School of Intelligent Manufacturing and Future Energy Gannan Normal University Ganzhou China) J Jie Chen H Haixia Lu X Xu Li X Xinyu Cheng (The MOE Basic Research and Innovation Center for the Targeted Therapeutics of Solid Tumors, School of Basic Medical Sciences, The Second Affiliated Hospital, Jiangxi Medical College, Nanchang University, Nanchang, Jiangxi, China.) S Shaoyu Liu (Centre for Advanced Optoelectronics School of Intelligent Manufacturing and Future Energy Gannan Normal University Ganzhou China) Y Yuxin Zhou Z Zhonggao Zhou (College of Chemistry and Materials Science Analysis and Testing Center Key Laboratory of Jiangxi University for Functional Materials Chemistry Jiangxi Provincial Key Laboratory of Bamboo Fiber Composite Gannan Normal University Ganzhou China) J Junlei Zhou (State Key Laboratory of Precision Spectroscopy, School of Physics, East China Normal University 1 , Shanghai 200241,) Z Zhengchi Yang (Centre for Advanced Optoelectronics School of Intelligent Manufacturing and Future Energy Gannan Normal University Ganzhou China) G Gengling Liu (College of Chemistry and Chemical Engineering Gannan Normal University Ganzhou Jiangxi China) Z Zhi Xing (School of Chemistry and Chemical Engineering Gannan Normal University Ganzhou Jiangxi P. R. China) J Jinwei Gao Y Yiwang Chen (College of Chemistry and Chemical Engineering/Film Energy Chemistry for Jiangxi Provincial Key Laboratory (FEC), Nanchang University, Nanchang, China.)

Abstract

ABSTRACT The chemistry of buried interfaces critically dictates the crystallization behavior of perovskite semiconductors in inverted perovskite solar cells, yet remains poorly controlled, giving rise to interfacial coordination disorder that disrupts the organization of self‐assembled monolayers (SAMs) during crystallization. Here, we report an N‐heterocycle‐activated coordination strategy that stabilizes SAM organization while enabling precise regulation of precursor chemistry and crystallization at SAM‐perovskite interfaces. Imidazolium‐derived molecules integrated into SAMs establish cooperative coordination interactions with neighbouring lead polyhalide species, thereby reshaping the local precursor environment and directing nucleation and crystal growth. This process gives rise to a π‐cooperative coordination interaction at the buried interface, which suppresses interfacial grooves and voids, reduces residual solvent–complex intermediates, and promotes the direct formation of phase‐pure α‐perovskite films. Devices based on this molecularly regulated interface achieve a power conversion efficiency of 26.83% and retain 93.8% of their initial efficiency after 936 h of continuous maximum power point operation. These results establish coordination‐mediated interfacial design as a molecular route to couple interfacial order with crystallization control in perovskite semiconductors.

Article Details

Volume / Issue Vol. 38, Issue 43
Published August 01, 2026
ISSN 0935-9648
Publisher Unknown Publisher

Journal Info

Advanced Materials

Unknown Publisher

ISSN: 0935-9648 Physical Sciences

Authors (14)

Y

Yuanshan Xiao

Centre for Advanced Optoelectronics School of Intelligent Manufacturing and Future Energy Gannan Normal University Ganzhou China

J

Jie Chen

H

Haixia Lu

X

Xu Li

X

Xinyu Cheng

The MOE Basic Research and Innovation Center for the Targeted Therapeutics of Solid Tumors, School of Basic Medical Sciences, The Second Affiliated Hospital, Jiangxi Medical College, Nanchang University, Nanchang, Jiangxi, China.

S

Shaoyu Liu

Centre for Advanced Optoelectronics School of Intelligent Manufacturing and Future Energy Gannan Normal University Ganzhou China

Y

Yuxin Zhou

Z

Zhonggao Zhou

College of Chemistry and Materials Science Analysis and Testing Center Key Laboratory of Jiangxi University for Functional Materials Chemistry Jiangxi Provincial Key Laboratory of Bamboo Fiber Composite Gannan Normal University Ganzhou China

J

Junlei Zhou

State Key Laboratory of Precision Spectroscopy, School of Physics, East China Normal University 1 , Shanghai 200241,

Z

Zhengchi Yang

Centre for Advanced Optoelectronics School of Intelligent Manufacturing and Future Energy Gannan Normal University Ganzhou China

G

Gengling Liu

College of Chemistry and Chemical Engineering Gannan Normal University Ganzhou Jiangxi China

Z

Zhi Xing

School of Chemistry and Chemical Engineering Gannan Normal University Ganzhou Jiangxi P. R. China

J

Jinwei Gao

Y

Yiwang Chen

College of Chemistry and Chemical Engineering/Film Energy Chemistry for Jiangxi Provincial Key Laboratory (FEC), Nanchang University, Nanchang, China.