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

Title: Two Regimes of Bandgap Red Shift and Partial Ambient Retention in Pressure-Treated Two-Dimensional Perovskites

Abstract

Here, the discovery of elevated environmental stability in two-dimensional (2D) Ruddlesden-Popper hybrid perovskites represents a significant advance in low-cost, high-efficiency light absorbers. In comparison to 3D counterparts, 2D perovskites of organo-lead-halides exhibit wider, quantum-confined optical bandgaps that reduce the wavelength range of light absorption. Here, we characterize the structural and optical properties of 2D hybrid perovskites as a function of hydrostatic pressure. We observe bandgap narrowing with pressure of 633 meV that is partially retained following pressure release due to atomic reconfiguration mechanism. We identify two distinct regimes of compression dominated by the softer organic and less compressible inorganic sub-lattices, respectively. Our findings, which also include PL enhancement, correlate well with density functional theory calculations and establish structure-property relationships at the atomic scale. These concepts can be expanded into other hybrid perovskites and suggest that pressure/strain processing could offer a new route to improved materials-by-design in applications.

Authors:
 [1];  [1]; ORCiD logo [2]; ORCiD logo [3];  [4];  [5];  [2];  [2];  [1]; ORCiD logo [3]; ORCiD logo [6]
+ Show Author Affiliations
  1. Center for High Pressure Science and Technology Advanced Research, Shanghai (China); Carnegie Inst. of Washington, Washington, D.C. (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Northwestern Univ., Evanston, IL (United States)
  4. Center for High Pressure Science and Technology Advanced Research, Shanghai (China)
  5. Carnegie Inst. of Washington, Washington, D.C. (United States)
  6. Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1494594
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 2; Journal Issue: 11; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Liu, Gang, Kong, Lingping, Guo, Peijun, Stoumpos, Constantinos C., Hu, Qingyang, Liu, Zhenxian, Cai, Zhonghou, Gosztola, David J., Mao, Ho-kwang, Kanatzidis, Mercouri G., and Schaller, Richard D. Two Regimes of Bandgap Red Shift and Partial Ambient Retention in Pressure-Treated Two-Dimensional Perovskites. United States: N. p., 2017. Web. doi:10.1021/acsenergylett.7b00807.
Copy to clipboard
Liu, Gang, Kong, Lingping, Guo, Peijun, Stoumpos, Constantinos C., Hu, Qingyang, Liu, Zhenxian, Cai, Zhonghou, Gosztola, David J., Mao, Ho-kwang, Kanatzidis, Mercouri G., & Schaller, Richard D. Two Regimes of Bandgap Red Shift and Partial Ambient Retention in Pressure-Treated Two-Dimensional Perovskites. United States. doi:10.1021/acsenergylett.7b00807.
Copy to clipboard
Liu, Gang, Kong, Lingping, Guo, Peijun, Stoumpos, Constantinos C., Hu, Qingyang, Liu, Zhenxian, Cai, Zhonghou, Gosztola, David J., Mao, Ho-kwang, Kanatzidis, Mercouri G., and Schaller, Richard D. Tue . "Two Regimes of Bandgap Red Shift and Partial Ambient Retention in Pressure-Treated Two-Dimensional Perovskites". United States. doi:10.1021/acsenergylett.7b00807. https://www.osti.gov/servlets/purl/1494594.
Copy to clipboard
@article{osti_1494594,
title = {Two Regimes of Bandgap Red Shift and Partial Ambient Retention in Pressure-Treated Two-Dimensional Perovskites},
author = {Liu, Gang and Kong, Lingping and Guo, Peijun and Stoumpos, Constantinos C. and Hu, Qingyang and Liu, Zhenxian and Cai, Zhonghou and Gosztola, David J. and Mao, Ho-kwang and Kanatzidis, Mercouri G. and Schaller, Richard D.},
abstractNote = {Here, the discovery of elevated environmental stability in two-dimensional (2D) Ruddlesden-Popper hybrid perovskites represents a significant advance in low-cost, high-efficiency light absorbers. In comparison to 3D counterparts, 2D perovskites of organo-lead-halides exhibit wider, quantum-confined optical bandgaps that reduce the wavelength range of light absorption. Here, we characterize the structural and optical properties of 2D hybrid perovskites as a function of hydrostatic pressure. We observe bandgap narrowing with pressure of 633 meV that is partially retained following pressure release due to atomic reconfiguration mechanism. We identify two distinct regimes of compression dominated by the softer organic and less compressible inorganic sub-lattices, respectively. Our findings, which also include PL enhancement, correlate well with density functional theory calculations and establish structure-property relationships at the atomic scale. These concepts can be expanded into other hybrid perovskites and suggest that pressure/strain processing could offer a new route to improved materials-by-design in applications.},
doi = {10.1021/acsenergylett.7b00807},
journal = {ACS Energy Letters},
number = 11,
volume = 2,
place = {United States},
year = {2017},
month = {10}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI:  10.1021/acsenergylett.7b00807
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 33 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: In situ high pressure PL and TRPL characterizations on (BA)2(MA)Pb2I7. (a) Pressure-dependent static PL signal in compression. The traces are normalized by dividing every PL intensity value at relative wavelength by the magnitude of PL peak intensity at respective pressure. (b) High pressure TRPL measurements (dots) and singlemore » exponential fittings (lines) on an (BA)2(MA)Pb2I7 sample. (c) Pressure dependence of carrier lifetime. The symbol size covers the size of the error bars.« less
All figures and tables (5 total)
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referencing / citing this record:

Metal halide perovskites under compression
journal, January 2019

  • Li, Qian; Zhang, Liming; Chen, Zhongwei
  • Journal of Materials Chemistry A, Vol. 7, Issue 27
  • DOI: 10.1039/c9ta04930d

Pressure-induced semiconductor-to-metal phase transition of a charge-ordered indium halide perovskite
journal, November 2019

  • Lin, Jia; Chen, Hong; Gao, Yang
  • Proceedings of the National Academy of Sciences, Vol. 116, Issue 47
  • DOI: 10.1073/pnas.1907576116

Metal halide perovskites under compression
journal, January 2019

  • Li, Qian; Zhang, Liming; Chen, Zhongwei
  • Journal of Materials Chemistry A, Vol. 7, Issue 27
  • DOI: 10.1039/c9ta04930d

Pressure-induced semiconductor-to-metal phase transition of a charge-ordered indium halide perovskite
journal, November 2019

  • Lin, Jia; Chen, Hong; Gao, Yang
  • Proceedings of the National Academy of Sciences, Vol. 116, Issue 47
  • DOI: 10.1073/pnas.1907576116

Substrate‐Dependent Spin–Orbit Coupling in Hybrid Perovskite Thin Films
journal, July 2019

  • Zhang, Qi; Yu, Haomiao; Zhao, Fenggui
  • Advanced Functional Materials, Vol. 29, Issue 35
  • DOI: 10.1002/adfm.201904046

Large Band Gap Narrowing and Prolonged Carrier Lifetime of (C 4 H 9 NH 3 ) 2 PbI 4 under High Pressure
journal, June 2019

Pressure‐Induced Emission (PIE) and Phase Transition of a Two‐dimensional Halide Double Perovskite (BA) 4 AgBiBr 8 (BA=CH 3 (CH 2 ) 3 NH 3 + )
journal, October 2019

  • Fang, Yuanyuan; Zhang, Long; Wu, Lianwei
  • Angewandte Chemie International Edition, Vol. 58, Issue 43
  • DOI: 10.1002/anie.201906311

Pressure-induced effects in the inorganic halide perovskite CsGeI 3
journal, January 2019

  • Liu, Diwen; Li, Qiaohong; Jing, Huijuan
  • RSC Advances, Vol. 9, Issue 6
  • DOI: 10.1039/c8ra10251a

Emission enhancement and bandgap retention of a two-dimensional mixed cation lead halide perovskite under high pressure
journal, January 2019

  • Chen, Yaping; Fu, Ruijing; Wang, Lingrui
  • Journal of Materials Chemistry A, Vol. 7, Issue 11
  • DOI: 10.1039/c8ta11992a

Searching for stability at lower dimensions: current trends and future prospects of layered perovskite solar cells
journal, January 2019

  • Thrithamarassery Gangadharan, Deepak; Ma, Dongling
  • Energy & Environmental Science, Vol. 12, Issue 10
  • DOI: 10.1039/c9ee01591d

Pressure responses of halide perovskites with various compositions, dimensionalities, and morphologies
journal, January 2020

  • Li, Mei; Liu, Tianbiao; Wang, Yonggang
  • Matter and Radiation at Extremes, Vol. 5, Issue 1
  • DOI: 10.1063/1.5133653

Isothermal pressure-derived metastable states in 2D hybrid perovskites showing enduring bandgap narrowing
journal, July 2018

  • Liu, Gang; Gong, Jue; Kong, Lingping
  • Proceedings of the National Academy of Sciences, Vol. 115, Issue 32
  • DOI: 10.1073/pnas.1809167115

Manipulating efficient light emission in two-dimensional perovskite crystals by pressure-induced anisotropic deformation
journal, July 2019

    [ × clear filter / sort ]

    Figures / Tables found in this record:

    Figure 1 (p. 17)figure
    Figure 2 (p. 18)figure
    Figure 3 (p. 19)figure
    Figure 4 (p. 21)figure
    Figure 5 (p. 22)figure
      [ × clear filter / sort ]
      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

      Similar Records in DOE PAGES and OSTI.GOV collections: