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Title: Reaching 90% Photoluminescence Quantum Yield in One-Dimensional Metal Halide C 4N 2H 14PbBr 4 by Pressure-Suppressed Nonradiative Loss

Abstract

Low-dimensional perovskite-related metal halides have emerged as a new class of light-emitting materials with tunable broadband emission from self-trapped excitons (STEs). Although various types of low-dimensional structures have been developed, fundamental understating of the structure–property relationships for this class of materials is still very limited, and further improvement of their optical properties remains greatly important. Here, we report a significant pressure-induced photoluminescence (PL) enhancement in a one-dimensional hybrid metal halide C 4N 2H 14PbBr 4, and the underlying mechanisms are investigated using in situ experimental characterization and first-principles calculations. Under a gigapascal pressure scale, the PL quantum yields (PLQYs) were quantitatively determined to show a dramatic increase from the initial value of 20% at ambient conditions to over 90% at 2.8 GPa. With in situ characterization of photophysical properties and theoretical analysis, we found that the PLQY enhancement was mainly attributed to the greatly suppressed nonradiative decay. Pressure can effectively tune the energy level of self-trapped states and increase the exciton binding energy, which leads to a larger Stokes shift. The resulting highly localized excitons with stronger binding reduce the probability for carrier scattering, to result in the significantly suppressed nonradiative decay. Overall, our findings clearly show that the characteristicsmore » of STEs in low-dimensional metal halides can be well-tuned by external pressure, and enhanced optical properties can be achieved.« less

Authors:
ORCiD logo [1];  [2];  [2];  [3];  [3];  [4]; ORCiD logo [2]; ORCiD logo [5]; ORCiD logo [3];  [2]; ORCiD logo [2]
  1. Center for High Pressure Science & Technology Advanced Research, Shanghai (China); Univ. of Washington, Seattle, WA (United States)
  2. Center for High Pressure Science & Technology Advanced Research, Shanghai (China)
  3. Florida State Univ., Tallahassee, FL (United States)
  4. Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1661225
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 142; Journal Issue: 37; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Excitons; metals; inorganic compounds; recombination; halogens; low-dimensional hybrid metal halide; high pressure; self-trapped excitons; enhanced photoluminescence quantum yield; PL lifetime; non-radiative recombination

Citation Formats

Wang, Yingqi, Guo, Songhao, Luo, Hui, Zhou, Chenkun, Lin, Haoran, Ma, Xuedan, Hu, Qingyang, Du, Mao-hua, Ma, Biwu, Yang, Wenge, and Lü, Xujie. Reaching 90% Photoluminescence Quantum Yield in One-Dimensional Metal Halide C4N2H14PbBr4 by Pressure-Suppressed Nonradiative Loss. United States: N. p., 2020. Web. doi:10.1021/jacs.0c07166.
Wang, Yingqi, Guo, Songhao, Luo, Hui, Zhou, Chenkun, Lin, Haoran, Ma, Xuedan, Hu, Qingyang, Du, Mao-hua, Ma, Biwu, Yang, Wenge, & Lü, Xujie. Reaching 90% Photoluminescence Quantum Yield in One-Dimensional Metal Halide C4N2H14PbBr4 by Pressure-Suppressed Nonradiative Loss. United States. https://doi.org/10.1021/jacs.0c07166
Wang, Yingqi, Guo, Songhao, Luo, Hui, Zhou, Chenkun, Lin, Haoran, Ma, Xuedan, Hu, Qingyang, Du, Mao-hua, Ma, Biwu, Yang, Wenge, and Lü, Xujie. Tue . "Reaching 90% Photoluminescence Quantum Yield in One-Dimensional Metal Halide C4N2H14PbBr4 by Pressure-Suppressed Nonradiative Loss". United States. https://doi.org/10.1021/jacs.0c07166.
@article{osti_1661225,
title = {Reaching 90% Photoluminescence Quantum Yield in One-Dimensional Metal Halide C4N2H14PbBr4 by Pressure-Suppressed Nonradiative Loss},
author = {Wang, Yingqi and Guo, Songhao and Luo, Hui and Zhou, Chenkun and Lin, Haoran and Ma, Xuedan and Hu, Qingyang and Du, Mao-hua and Ma, Biwu and Yang, Wenge and Lü, Xujie},
abstractNote = {Low-dimensional perovskite-related metal halides have emerged as a new class of light-emitting materials with tunable broadband emission from self-trapped excitons (STEs). Although various types of low-dimensional structures have been developed, fundamental understating of the structure–property relationships for this class of materials is still very limited, and further improvement of their optical properties remains greatly important. Here, we report a significant pressure-induced photoluminescence (PL) enhancement in a one-dimensional hybrid metal halide C4N2H14PbBr4, and the underlying mechanisms are investigated using in situ experimental characterization and first-principles calculations. Under a gigapascal pressure scale, the PL quantum yields (PLQYs) were quantitatively determined to show a dramatic increase from the initial value of 20% at ambient conditions to over 90% at 2.8 GPa. With in situ characterization of photophysical properties and theoretical analysis, we found that the PLQY enhancement was mainly attributed to the greatly suppressed nonradiative decay. Pressure can effectively tune the energy level of self-trapped states and increase the exciton binding energy, which leads to a larger Stokes shift. The resulting highly localized excitons with stronger binding reduce the probability for carrier scattering, to result in the significantly suppressed nonradiative decay. Overall, our findings clearly show that the characteristics of STEs in low-dimensional metal halides can be well-tuned by external pressure, and enhanced optical properties can be achieved.},
doi = {10.1021/jacs.0c07166},
url = {https://www.osti.gov/biblio/1661225}, journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 37,
volume = 142,
place = {United States},
year = {2020},
month = {9}
}

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