Title: Regulating Exciton–Phonon Coupling to Achieve a Near‐Unity Photoluminescence Quantum Yield in One‐Dimensional Hybrid Metal Halides

Abstract

Abstract Low‐dimensional hybrid metal halides are emerging as a highly promising class of single‐component white‐emitting materials for their unique broadband emission from self‐trapped excitons (STEs). Despite substantial progress in the development of these metal halides, many challenges remain to be addressed to obtain a better fundamental understanding of the structure–property relationship and realize the full potentials of this class of materials. Here, via pressure regulation, a near 100% photoluminescence quantum yield (PLQY) of broadband emission is achieved in a corrugated 1D hybrid metal halide C ₅ N ₂ H ₁₆ Pb ₂ Br ₆ , which possesses a highly distorted structure with an initial PLQY of 10%. Compression reduces the overlap between STE states and ground state, leading to a suppressed phonon‐assisted non‐radiative decay. The PL evolution is systematically demonstrated to be controlled by the pressure‐regulated exciton–phonon coupling which can be quantified using Huang–Rhys factor S . Detailed studies of the S ‐PLQY relation for a series of 1D hybrid metal halides (C ₅ N ₂ H ₁₆ Pb ₂ Br ₆ , C ₄ N ₂ H ₁₄ PbBr ₄ , C ₆ N ₂ H ₁₆ PbBr ₄ , and (C ₆ N ₂ H ₁₆ ) ₃more » Pb ₂ Br ₁₀ ) reveal a quantitative structure–property relationship that regulating S factor toward 28 leads to the maximum emission.« less

Authors:

Luo, Hui ^[1]; Guo, Songhao ^[1]; Zhang, Yubo ^[2]; Bu, Kejun ^[1]; Lin, Haoran ^[3]; Wang, Yingqi ^[1]; Yin, Yanfeng ^[4]; Zhang, Dongzhou ^[5]; Jin, Shengye ^[4]; Zhang, Wenqing ^[2]; Yang, Wenge ^[1]; Ma, Biwu ^[6]; Lü, Xujie  ^[1]

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+ Show Author Affiliations

1. Center for High Pressure Science and Technology Advanced Research (HPSTAR) 1690 Cailun Rd, Pudong Shanghai 201203 China
2. Department of Physics and Shenzhen Institute for Quantum Science and Engineering Southern University of Science and Technology Shenzhen Guangdong 518055 China
3. Hoffmann Institute of Advanced Materials Shenzhen Polytechnic Shenzhen Guangdong 518055 China
4. State Key Laboratory of Molecular Reaction Dynamics and Dynamics Research Center for Energy and Environmental Materials Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian Liaoning 116023 China
5. Hawaii Institute of Geophysics and Planetology University of Hawaii Manoa Honolulu HI 96822 USA
6. Department of Chemistry and Biochemistry Florida State University Tallahassee FL 32306 USA

Publication Date:

Sat May 22 00:00:00 EDT 2021

Research Org.:

Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF)

OSTI Identifier:

1784401

Alternate Identifier(s):

OSTI ID: 1784403; OSTI ID: 1815033

Grant/Contract Number:  

AC02-06CH11357; FG02-94ER14466; U1930401; 51527801; FA9550-18-1-0231; EAR-1634415; EAR-1606856; EAR-1531583

Resource Type:

Published Article

Journal Name:

Advanced Science

Additional Journal Information:

Journal Name: Advanced Science Journal Volume: 8 Journal Issue: 14; Journal ID: ISSN 2198-3844

Publisher:

Wiley Blackwell (John Wiley & Sons)

Country of Publication:

Germany

Language:

English

Subject:

36 MATERIALS SCIENCE