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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)
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. https://doi.org/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. https://doi.org/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 = {Wed May 23 00:00:00 EDT 2018},
month = {Wed May 23 00:00:00 EDT 2018}
}

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Figures / Tables:

Figure 1 Figure 1: Structural characterization of 1D C4N2H14PbCl4 single crystal. (a) Structure of C4N2H14PbCl4 (red spheres: lead atoms; green spheres: chloride atoms; blue spheres: nitrogen atoms; grey spheres: carbon atoms; purple polyhedrons: PbCl64- octahedrons; hydrogen atoms were hidden for clarity). (b) View of a single lead chloride quantum wire wrapped bymore » organic cations. (c) View of a single lead chloride quantum wire with edge sharing octahedrons. (d) Powder X-ray diffraction (PXRD) pattern of 1D C4N2PbCl4 crystals. The simulated PXRD pattern is also provided for comparison.« less

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