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

Abstract

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 an atomic reconfiguration mechanism. We identify two distinct regimes of compression dominated by the softer organic and less compressible inorganic sublattices. 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];  [6];  [2];  [1]; ORCiD logo [3]; ORCiD logo [7]
  1. Center for High Pressure Science and Technology Advanced Research, Shanghai 201203, China; Geophysical Laboratory, Carnegie Institution of Washington, Washington, DC 20015, United States
  2. Center for Nanoscale Materials, Argonne National Laboratory, Argonne, Illinois 60439, United States
  3. Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
  4. Center for High Pressure Science and Technology Advanced Research, Shanghai 201203, China
  5. Geophysical Laboratory, Carnegie Institution of Washington, Washington, DC 20015, United States
  6. Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States
  7. Center for Nanoscale Materials, Argonne National Laboratory, Argonne, Illinois 60439, United States; Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1409634
Report Number(s):
BNL-114686-2017-JA¿¿¿
Journal ID: ISSN 2380-8195
DOE Contract Number:
SC0012704
Resource Type:
Journal Article
Resource Relation:
Journal Name: ACS Energy Letters; Journal Volume: 2; Journal Issue: 11
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 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. 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., and Schaller, Richard D. 2017. "Two Regimes of Bandgap Red Shift and Partial Ambient Retention in Pressure-Treated Two-Dimensional Perovskites". United States. doi:10.1021/acsenergylett.7b00807.
@article{osti_1409634,
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 = {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 an atomic reconfiguration mechanism. We identify two distinct regimes of compression dominated by the softer organic and less compressible inorganic sublattices. 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 =
}