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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.
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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
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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.
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@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}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acsenergylett.7b00807
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Cited by: 33 works
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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
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Works referenced in this record:

Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells
journal, May 2009

  • Kojima, Akihiro; Teshima, Kenjiro; Shirai, Yasuo
  • Journal of the American Chemical Society, Vol. 131, Issue 17, p. 6050-6051
  • DOI: 10.1021/ja809598r

Cesium-containing triple cation perovskite solar cells: improved stability, reproducibility and high efficiency
journal, January 2016

  • Saliba, Michael; Matsui, Taisuke; Seo, Ji-Youn
  • Energy & Environmental Science, Vol. 9, Issue 6
  • DOI: 10.1039/C5EE03874J

Toward Lead-Free Perovskite Solar Cells
journal, November 2016

Energy conversion approaches and materials for high-efficiency photovoltaics
journal, December 2016

  • Green, Martin A.; Bremner, Stephen P.
  • Nature Materials, Vol. 16, Issue 1
  • DOI: 10.1038/nmat4676

Detailed Balance Limit of Efficiency of p‐n Junction Solar Cells
journal, March 1961

  • Shockley, William; Queisser, Hans J.
  • Journal of Applied Physics, Vol. 32, Issue 3, p. 510-519
  • DOI: 10.1063/1.1736034

High-efficiency solution-processed perovskite solar cells with millimeter-scale grains
journal, January 2015

Electron–phonon coupling in hybrid lead halide perovskites
journal, May 2016

  • Wright, Adam D.; Verdi, Carla; Milot, Rebecca L.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms11755

Formamidinium Lead Halide Perovskite Crystals with Unprecedented Long Carrier Dynamics and Diffusion Length
journal, April 2016

Interface engineering of highly efficient perovskite solar cells
journal, July 2014

Functionalization of perovskite thin films with moisture-tolerant molecules
journal, January 2016

Accelerated degradation of methylammonium lead iodide perovskites induced by exposure to iodine vapour
journal, December 2016

Atomically thin two-dimensional organic-inorganic hybrid perovskites
journal, September 2015

High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells
journal, July 2016

  • Tsai, Hsinhan; Nie, Wanyi; Blancon, Jean-Christophe
  • Nature, Vol. 536, Issue 7616
  • DOI: 10.1038/nature18306

2D Homologous Perovskites as Light-Absorbing Materials for Solar Cell Applications
journal, June 2015

  • Cao, Duyen H.; Stoumpos, Constantinos C.; Farha, Omar K.
  • Journal of the American Chemical Society, Vol. 137, Issue 24
  • DOI: 10.1021/jacs.5b03796

Lead-free solid-state organic–inorganic halide perovskite solar cells
journal, May 2014

  • Hao, Feng; Stoumpos, Constantinos C.; Cao, Duyen Hanh
  • Nature Photonics, Vol. 8, Issue 6
  • DOI: 10.1038/nphoton.2014.82

Compositional engineering of perovskite materials for high-performance solar cells
journal, January 2015

  • Jeon, Nam Joong; Noh, Jun Hong; Yang, Woon Seok
  • Nature, Vol. 517, Issue 7535
  • DOI: 10.1038/nature14133

Ruddlesden–Popper Hybrid Lead Iodide Perovskite 2D Homologous Semiconductors
journal, April 2016

  • Stoumpos, Constantinos C.; Cao, Duyen H.; Clark, Daniel J.
  • Chemistry of Materials, Vol. 28, Issue 8, p. 2852-2867
  • DOI: 10.1021/acs.chemmater.6b00847

Halide Perovskites under Pressure: Accessing New Properties through Lattice Compression
journal, June 2017

Pressure-Induced Effects in Organic–Inorganic Hybrid Perovskites
journal, May 2017

Photovoltaic Hybrid Perovskites under Pressure
journal, May 2017

Electron–Phonon Scattering in Atomically Thin 2D Perovskites
journal, October 2016

Simultaneous band-gap narrowing and carrier-lifetime prolongation of organic–inorganic trihalide perovskites
journal, July 2016

  • Kong, Lingping; Liu, Gang; Gong, Jue
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 32
  • DOI: 10.1073/pnas.1609030113

Slow Organic-to-Inorganic Sub-Lattice Thermalization in Methylammonium Lead Halide Perovskites Observed by Ultrafast Photoluminescence
journal, May 2016

  • Chang, Angela Y.; Cho, Yi-Ju; Chen, Kuan-Chen
  • Advanced Energy Materials, Vol. 6, Issue 15
  • DOI: 10.1002/aenm.201600422

Pressure-Induced Bandgap Optimization in Lead-Based Perovskites with Prolonged Carrier Lifetime and Ambient Retainability
journal, December 2016

  • Liu, Gang; Kong, Lingping; Gong, Jue
  • Advanced Functional Materials, Vol. 27, Issue 3
  • DOI: 10.1002/adfm.201604208

Halide perovskite materials for solar cells: a theoretical review
journal, January 2015

  • Yin, Wan-Jian; Yang, Ji-Hui; Kang, Joongoo
  • Journal of Materials Chemistry A, Vol. 3, Issue 17
  • DOI: 10.1039/C4TA05033A

Pressure-Induced Phase Transformation, Reversible Amorphization, and Anomalous Visible Light Response in Organolead Bromide Perovskite
journal, August 2015

  • Wang, Yonggang; Lü, Xujie; Yang, Wenge
  • Journal of the American Chemical Society, Vol. 137, Issue 34
  • DOI: 10.1021/jacs.5b06346

Pressure-Dependent Polymorphism and Band-Gap Tuning of Methylammonium Lead Iodide Perovskite
journal, April 2016

  • Jiang, Shaojie; Fang, Yanan; Li, Ruipeng
  • Angewandte Chemie International Edition, Vol. 55, Issue 22
  • DOI: 10.1002/anie.201601788

Pressure-Induced Structural Evolution and Band Gap Shifts of Organometal Halide Perovskite-Based Methylammonium Lead Chloride
journal, November 2016

Mobile Ions in Organohalide Perovskites: Interplay of Electronic Structure and Dynamics
journal, June 2016

Structural and electronic properties of organo-halide hybrid perovskites from ab initio molecular dynamics
journal, January 2015

  • Quarti, Claudio; Mosconi, Edoardo; De Angelis, Filippo
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 14
  • DOI: 10.1039/C5CP00599J

The Renaissance of Halide Perovskites and Their Evolution as Emerging Semiconductors
journal, September 2015

Synthesis, Single-Crystal Structure and Characterization of (CH 3 NH 3 ) 2 Pb(SCN) 2 I 2
journal, September 2015

  • Daub, Michael; Hillebrecht, Harald
  • Angewandte Chemie International Edition, Vol. 54, Issue 38
  • DOI: 10.1002/anie.201506449

Confinement Effects in Low-Dimensional Lead Iodide Perovskite Hybrids
journal, June 2016

The large-volume high-pressure facility at GSECARS: A “Swiss-army-knife” approach to synchrotron-based experimental studies
journal, May 2009

  • Wang, Yanbin; Rivers, Mark; Sutton, Steve
  • Physics of the Earth and Planetary Interiors, Vol. 174, Issue 1-4
  • DOI: 10.1016/j.pepi.2008.06.017

The large volume press facility at ID06 beamline of the European synchrotron radiation facility as a High Pressure-High Temperature deformation apparatus
journal, August 2015

  • Guignard, Jeremy; Crichton, Wilson A.
  • Review of Scientific Instruments, Vol. 86, Issue 8
  • DOI: 10.1063/1.4928151

Enhanced Structural Stability and Photo Responsiveness of CH 3 NH 3 SnI 3 Perovskite via Pressure-Induced Amorphization and Recrystallization
journal, August 2016

  • Lü, Xujie; Wang, Yonggang; Stoumpos, Constantinos C.
  • Advanced Materials, Vol. 28, Issue 39
  • DOI: 10.1002/adma.201600771

Pressure induced metallization with absence of structural transition in layered molybdenum diselenide
journal, June 2015

  • Zhao, Zhao; Zhang, Haijun; Yuan, Hongtao
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8312
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    Works referencing / citing this record:

    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

    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

    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

    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 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

    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

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

    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

    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
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