Atomic‐Scale Structural Distortion Drives Exciton Localization for Near‐Unity Photoluminescence in Copper–Iodide Clusters

H Haifeng Zhu (State Key Laboratory of Integrated Optoelectronics, JLU Region, College of Electronic Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China) S Shengrong He (State Key Laboratory of Integrated Optoelectronics, JLU Region, College of Electronic Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China) Z Zhihao Xiao G Guangming Niu Y Yanxue Yin (State Key Laboratory of Superhard Materials Synergetic Extreme Condition High‐Pressure Science Center College of Physics Jilin University 2699 Qianjin Street Changchun 130012 P.R. China) S Shengqiao Wang (State Key Laboratory of Integrated Optoelectronics Key Laboratory of Automobile Materials of MOE Key Laboratory of Material Simulation Methods & Software of MOE School of Materials Science and Engineering Jilin University 2699 Qianjin Street Changchun 130012 P.R. China) L Laizhi Sui (State Key Laboratory of Molecular Reaction Dynamics and Dalian Coherent Light Source) X Xinyi Yang (School of Materials Science and Engineering, Tianjin University, Tianjin, China.) B Bo Zou (State Key Laboratory of High Pressure and Superhard Materials, College of Physics) L Lijun Zhang (Key Laboratory of Functionalized Molecular Solids of Ministry of Education, Anhui Laboratory of Molecule-Based Materials, College of Chemistry and Materials Science) Z Zhennan Wu (State Key Laboratory of Integrated Optoelectronics, JLU Region, College of Electronic Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China) Y Yu Zhang (Xiangya Hospital, Central South University Changsha China) X Xue Bai

Abstract

Abstract Engineering structural distortions presents a powerful strategy for tailoring the optoelectronic properties of luminescent materials, while a fundamental understanding of how atomic‐scale distortions govern photoluminescence in copper‐iodide clusters has remained elusive. Herein, we report a model van der Waals solid based on copper–iodide clusters, where two vertically oriented and alternately arranged [Cu 2 I 4 ] 2− clusters are assembled via protection and interaction afforded by peripheral long‐alkyl‐chain cetyltrimethylammonium bromide ligands. This unique architecture affords a cooperative distortion response and exceptional buffering capacity, enabling precise control and direct probing of atomic‐scale structural distortions under pressure. We demonstrate that hydrostatic pressure induces controlled atomic distortions and an isostructural phase transition, which collectively enhance exciton localization. This leads to a dramatic amplification of self‐trapped emission, boosting the photoluminescence quantum yield from 32.25% to near‐unity (99.82%). Our work establishes atomic‐distortion engineering as a general principle for achieving ultimate control over light emission in hybrid semiconductors.

Article Details

Volume / Issue Vol. 65, Issue 5
Published January 28, 2026
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (13)

H

Haifeng Zhu

State Key Laboratory of Integrated Optoelectronics, JLU Region, College of Electronic Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China

S

Shengrong He

State Key Laboratory of Integrated Optoelectronics, JLU Region, College of Electronic Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China

Z

Zhihao Xiao

G

Guangming Niu

Y

Yanxue Yin

State Key Laboratory of Superhard Materials Synergetic Extreme Condition High‐Pressure Science Center College of Physics Jilin University 2699 Qianjin Street Changchun 130012 P.R. China

S

Shengqiao Wang

State Key Laboratory of Integrated Optoelectronics Key Laboratory of Automobile Materials of MOE Key Laboratory of Material Simulation Methods & Software of MOE School of Materials Science and Engineering Jilin University 2699 Qianjin Street Changchun 130012 P.R. China

L

Laizhi Sui

State Key Laboratory of Molecular Reaction Dynamics and Dalian Coherent Light Source

X

Xinyi Yang

School of Materials Science and Engineering, Tianjin University, Tianjin, China.

B

Bo Zou

State Key Laboratory of High Pressure and Superhard Materials, College of Physics

L

Lijun Zhang

Key Laboratory of Functionalized Molecular Solids of Ministry of Education, Anhui Laboratory of Molecule-Based Materials, College of Chemistry and Materials Science

Z

Zhennan Wu

State Key Laboratory of Integrated Optoelectronics, JLU Region, College of Electronic Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China

Y

Yu Zhang

Xiangya Hospital, Central South University Changsha China

X

Xue Bai