skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

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. 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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science

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

Save / Share:

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

Bulk Assembly of Corrugated 1D Metal Halides with Broadband Yellow Emission
journal, December 2018

  • Lin, Haoran; Zhou, Chenkun; Neu, Jennifer
  • Advanced Optical Materials, Vol. 7, Issue 6
  • DOI: 10.1002/adom.201801474

Negative Thermal Quenching of Efficient White‐Light Emission in a 1D Ladder‐Like Organic/Inorganic Hybrid Material
journal, July 2019

  • Barkaoui, Hamdi; Abid, Haitham; Zelewski, Szymon
  • Advanced Optical Materials, Vol. 7, Issue 20
  • DOI: 10.1002/adom.201900763

Single‐Component White‐Light Emission in 2D Hybrid Perovskites with Hybridized Halogen Atoms
journal, September 2019

  • Zhou, Guojun; Li, Mingze; Zhao, Jing
  • Advanced Optical Materials, Vol. 7, Issue 24
  • DOI: 10.1002/adom.201901335

Recent advances in one-dimensional halide perovskites for optoelectronic applications
journal, January 2018


[DMEDA]PbCl 4 : a one-dimensional organic lead halide perovskite with efficient yellow emission
journal, January 2020

  • Sun, Chen; Yue, Yun-Di; Zhang, Wei-Feng
  • CrystEngComm, Vol. 22, Issue 8
  • DOI: 10.1039/c9ce01816f

Semiconducting crystalline inorganic–organic hybrid metal halide nanochains
journal, January 2020

  • Wang, Guan-E; Sun, Cai; Wang, Ming-Sheng
  • Nanoscale, Vol. 12, Issue 8
  • DOI: 10.1039/c9nr10164k

High performance low-dimensional perovskite solar cells based on a one dimensional lead iodide perovskite
journal, January 2019

  • Ma, Chunqing; Shen, Dong; Huang, Bin
  • Journal of Materials Chemistry A, Vol. 7, Issue 15
  • DOI: 10.1039/c9ta01859j

Zero-dimensional metal oxide Li 4 TiO 4
journal, January 2019


White light emission in low-dimensional perovskites
journal, January 2019

  • Cortecchia, Daniele; Yin, Jun; Petrozza, Annamaria
  • Journal of Materials Chemistry C, Vol. 7, Issue 17
  • DOI: 10.1039/c9tc01036j

Electronic shell structures, self-trapped excitons, and defect-bound excitons in Li 2 B 12 H 12
journal, January 2019

  • Du, Mao-Hua; Shi, Hongliang; Zhang, S. B.
  • Journal of Materials Chemistry C, Vol. 7, Issue 45
  • DOI: 10.1039/c9tc04150h

Synthetic strategy towards halometallates with imidazo[1,5- a ]pyridinium-based counterions
journal, January 2020

  • Vassilyeva, Olga Yu.; Buvaylo, Elena A.; Linnik, Rostyslav P.
  • CrystEngComm, Vol. 22, Issue 30
  • DOI: 10.1039/d0ce00018c

Microscopic origin of multiple exciton emission in low-dimensional lead halide perovskites
journal, November 2019

  • Du, Mao-Hua
  • The Journal of Chemical Physics, Vol. 151, Issue 18
  • DOI: 10.1063/1.5127933

Optical anisotropy of one-dimensional perovskite C 4 N 2 H 14 PbI 4 crystals
journal, January 2020


    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.