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Title: A One-Dimensional Organic Lead Chloride Hybrid with Excitation-Dependent Broadband Emissions

Abstract

Organic–inorganic metal halide hybrids have emerged as a new class of materials with fascinating optical and electronic properties. The exceptional structure tunability has enabled the development of materials with various dimensionalities at the molecular level, from three-dimensional (3D) to 2D, 1D, and 0D. Here, we report a new 1D lead chloride hybrid, C4N2H14PbCl4, which exhibits unusual inverse excitation-dependent broadband emission from bluish-green to yellow. Density functional theory calculations were performed to better understand the mechanism of this excitation-dependent broadband emission. This 1D hybrid material is found to have two emission centers, corresponding to the self-trapped excitons (STEs) and vacancy-bound excitons. The excitation-dependent emission is due to different populations of these two types of excitons generated at different excitation wavelengths. Furthermore, this work shows the rich chemistry and physics of organic–inorganic metal halide hybrids and paves the way to achieving novel light emitters with excitation-dependent broadband emissions at room temperature.

Authors:
 [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [5];  [1]; ORCiD logo [6];  [6];  [6]; ORCiD logo [3]; ORCiD logo [7]; ORCiD logo [1]
  1. Fudan Univ., Shanghai (China)
  2. FAMSU-FSU College of Engineering, Tallahassee, FL (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); East China Normal Univ., Shanghai (China)
  5. East China Normal Univ., Shanghai (China)
  6. Florida State Univ., Tallahassee, FL (United States)
  7. FAMSU-FSU College of Engineering, Tallahassee, FL (United States); Florida State Univ., Tallahassee, FL (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) (SC-22)
OSTI Identifier:
1440827
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 3; Journal Issue: 6; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Wu, Guanhong, Zhou, Chenkun, Ming, Wenmei, Han, Dan, Chen, Shiyou, Yang, Dong, Besara, Tiglet, Neu, Jennifer, Siegrist, Theo, Du, Mao -Hua, Ma, Biwu, and Dong, Angang. A One-Dimensional Organic Lead Chloride Hybrid with Excitation-Dependent Broadband Emissions. United States: N. p., 2018. Web. doi:10.1021/acsenergylett.8b00661.
Wu, Guanhong, Zhou, Chenkun, Ming, Wenmei, Han, Dan, Chen, Shiyou, Yang, Dong, Besara, Tiglet, Neu, Jennifer, Siegrist, Theo, Du, Mao -Hua, Ma, Biwu, & Dong, Angang. A One-Dimensional Organic Lead Chloride Hybrid with Excitation-Dependent Broadband Emissions. United States. doi:10.1021/acsenergylett.8b00661.
Wu, Guanhong, Zhou, Chenkun, Ming, Wenmei, Han, Dan, Chen, Shiyou, Yang, Dong, Besara, Tiglet, Neu, Jennifer, Siegrist, Theo, Du, Mao -Hua, Ma, Biwu, and Dong, Angang. Wed . "A One-Dimensional Organic Lead Chloride Hybrid with Excitation-Dependent Broadband Emissions". United States. doi:10.1021/acsenergylett.8b00661. https://www.osti.gov/servlets/purl/1440827.
@article{osti_1440827,
title = {A One-Dimensional Organic Lead Chloride Hybrid with Excitation-Dependent Broadband Emissions},
author = {Wu, Guanhong and Zhou, Chenkun and Ming, Wenmei and Han, Dan and Chen, Shiyou and Yang, Dong and Besara, Tiglet and Neu, Jennifer and Siegrist, Theo and Du, Mao -Hua and Ma, Biwu and Dong, Angang},
abstractNote = {Organic–inorganic metal halide hybrids have emerged as a new class of materials with fascinating optical and electronic properties. The exceptional structure tunability has enabled the development of materials with various dimensionalities at the molecular level, from three-dimensional (3D) to 2D, 1D, and 0D. Here, we report a new 1D lead chloride hybrid, C4N2H14PbCl4, which exhibits unusual inverse excitation-dependent broadband emission from bluish-green to yellow. Density functional theory calculations were performed to better understand the mechanism of this excitation-dependent broadband emission. This 1D hybrid material is found to have two emission centers, corresponding to the self-trapped excitons (STEs) and vacancy-bound excitons. The excitation-dependent emission is due to different populations of these two types of excitons generated at different excitation wavelengths. Furthermore, this work shows the rich chemistry and physics of organic–inorganic metal halide hybrids and paves the way to achieving novel light emitters with excitation-dependent broadband emissions at room temperature.},
doi = {10.1021/acsenergylett.8b00661},
journal = {ACS Energy Letters},
number = 6,
volume = 3,
place = {United States},
year = {2018},
month = {5}
}

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Works referencing / citing this record:

Organic cation directed hybrid lead halides of zero-dimensional to two-dimensional structures with tunable photoluminescence properties
journal, January 2019

  • Yue, Cheng-Yang; Sun, Hai-Xiao; Liu, Quan-Xiu
  • Inorganic Chemistry Frontiers, Vol. 6, Issue 10
  • DOI: 10.1039/c9qi00684b

Locally collective hydrogen bonding isolates lead octahedra for white emission improvement
journal, November 2019


Two low-dimensional metal halides: ionothermal synthesis, photoluminescence, and nonlinear optical properties
journal, January 2019

  • Deng, Yuandan; Dong, Xuehua; Yang, Meng
  • Dalton Transactions, Vol. 48, Issue 47
  • DOI: 10.1039/c9dt04102h

Broadband white light emission from one-dimensional zigzag edge-sharing perovskite
journal, January 2020


Locally collective hydrogen bonding isolates lead octahedra for white emission improvement
journal, November 2019


Two low-dimensional metal halides: ionothermal synthesis, photoluminescence, and nonlinear optical properties
journal, January 2019

  • Deng, Yuandan; Dong, Xuehua; Yang, Meng
  • Dalton Transactions, Vol. 48, Issue 47
  • DOI: 10.1039/c9dt04102h

Broadband white light emission from one-dimensional zigzag edge-sharing perovskite
journal, January 2020


Organic cation directed hybrid lead halides of zero-dimensional to two-dimensional structures with tunable photoluminescence properties
journal, January 2019

  • Yue, Cheng-Yang; Sun, Hai-Xiao; Liu, Quan-Xiu
  • Inorganic Chemistry Frontiers, Vol. 6, Issue 10
  • DOI: 10.1039/c9qi00684b