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:
-
- Center for High Pressure Science and Technology Advanced Research, Shanghai (China); Carnegie Inst. of Washington, Washington, D.C. (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Northwestern Univ., Evanston, IL (United States)
- Center for High Pressure Science and Technology Advanced Research, Shanghai (China)
- Carnegie Inst. of Washington, Washington, D.C. (United States)
- 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.
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. https://doi.org/10.1021/acsenergylett.7b00807
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. https://doi.org/10.1021/acsenergylett.7b00807. https://www.osti.gov/servlets/purl/1494594.
@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}
}
Web of Science
Figures / Tables:

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