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

Gang Liu; Lingping Kong; Peijun Guo; Constantinos C. Stoumpos; Qingyang Hu; Zhenxian Liu; Zhonghou Cai; David J. Gosztola; Ho Kwang Mao; Mercouri G. Kanatzidis; Richard D. Schaller

doi:10.1021/acsenergylett.7b00807

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

Gang Liu^*, Lingping Kong, Peijun Guo, Constantinos C. Stoumpos, Qingyang Hu, Zhenxian Liu, Zhonghou Cai, David J. Gosztola, Ho Kwang Mao, Mercouri G. Kanatzidis, Richard D. Schaller

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

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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.

Original language	English (US)
Pages (from-to)	2518-2524
Number of pages	7
Journal	ACS Energy Letters
Volume	2
Issue number	11
DOIs	https://doi.org/10.1021/acsenergylett.7b00807
State	Published - Nov 10 2017

ASJC Scopus subject areas

Chemistry (miscellaneous)
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology
Materials Chemistry

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10.1021/acsenergylett.7b00807

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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.",

author = "Gang Liu and Lingping Kong and Peijun Guo and Stoumpos, {Constantinos C.} and Qingyang Hu and Zhenxian Liu and Zhonghou Cai and Gosztola, {David J.} and Mao, {Ho Kwang} and Kanatzidis, {Mercouri G.} and Schaller, {Richard D.}",

note = "Funding Information: This project was supported by the NSAF (U1530402) and National Science Foundation (CBET-1150617). High-pressure powder structure characterizations were performed at beamline 2-ID-D at APS, Argonne National Laboratory (ANL). The use of APS facilities was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (DE-AC02-06CH11357). Part of this work was performed at the Infrared Lab of the National Synchrotron Light Source (NSLS II), Brookhaven National Laboratory (BNL). Support from ONR (N00014-17-1-2231) is acknowledged. This work was performed, in part, at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. The Infrared Lab was supported by the National Science Foundation (EAR 1606856, COMPRES) and DOE/NNSA (DE-NA-0002006, CDAC). First-principles simulation was conducted at the SR16000 supercomputing facilities of the Center for Computa- tional Materials Science of the Institute for Materials Research, Tohoku University. Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",

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doi = "10.1021/acsenergylett.7b00807",

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AU - Liu, Gang

AU - Kong, Lingping

AU - Guo, Peijun

AU - Stoumpos, Constantinos C.

AU - Hu, Qingyang

AU - Liu, Zhenxian

AU - Cai, Zhonghou

AU - Gosztola, David J.

AU - Mao, Ho Kwang

AU - Kanatzidis, Mercouri G.

AU - Schaller, Richard D.

N1 - Funding Information: This project was supported by the NSAF (U1530402) and National Science Foundation (CBET-1150617). High-pressure powder structure characterizations were performed at beamline 2-ID-D at APS, Argonne National Laboratory (ANL). The use of APS facilities was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (DE-AC02-06CH11357). Part of this work was performed at the Infrared Lab of the National Synchrotron Light Source (NSLS II), Brookhaven National Laboratory (BNL). Support from ONR (N00014-17-1-2231) is acknowledged. This work was performed, in part, at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. The Infrared Lab was supported by the National Science Foundation (EAR 1606856, COMPRES) and DOE/NNSA (DE-NA-0002006, CDAC). First-principles simulation was conducted at the SR16000 supercomputing facilities of the Center for Computa- tional Materials Science of the Institute for Materials Research, Tohoku University. Publisher Copyright: © 2017 American Chemical Society.

PY - 2017/11/10

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N2 - 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.

AB - 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.

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

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