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

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 C5N2H16Pb2Br6, 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 (C5N2H16Pb2Br6, C4N2H14PbBr4, C6N2H16PbBr4, and (C6N2H16)3Pb2Br10) reveal a quantitative structure–property relationship that regulating S factor toward 28 leads to the maximum emission.

Document Details

Document Type
Pub Defense Publication
Publication Date
May 22, 2021
Source ID
10.1002/advs.202100786

Entities

People

  • Biwu Ma
  • Dongzhou Zhang
  • Haoran Lin
  • Hui Luo
  • Kejun Bu
  • Shengye Jin
  • Songhao Guo
  • Wenge Yang
  • Wenqing Zhang
  • Xujie Lü
  • Yanfeng Yin
  • Yingqi Wang
  • Yubo Zhang

Organizations

  • Air Force Office of Scientific Research
  • Argonne National Laboratory
  • Center for High Pressure Science and Technology Advanced Research
  • Dalian Institute of Chemical Physics
  • Florida State University
  • Shenzhen Polytechnic University
  • Southern University of Science and Technology
  • University of Hawaiʻi System

Tags

Fields of Study

  • Materials science

Readers

  • Materials Science and Engineering.
  • Quantum spin resonance or Electron Paramagnetic Resonance spectroscopy.
  • Systems Analysis and Design

Technology Areas

  • Microelectronics
  • Quantum Computing