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

Title: Manipulating efficient light emission in two-dimensional perovskite crystals by pressure-induced anisotropic deformation

Abstract

The hybrid nature and soft lattice of organolead halide perovskites render their structural changes and optical properties susceptible to external driving forces such as temperature and pressure, remarkably different from conventional semiconductors. Here, we investigate the pressure-induced optical response of a typical two-dimensional perovskite crystal, phenylethylamine lead iodide. At a moderate pressure within 3.5 GPa, its photoluminescence red-shifts continuously, exhibiting an ultrabroad energy tunability range up to 320 meV in the visible spectrum, with quantum yield remaining nearly constant. First-principles calculations suggest that an out-of-plane quasi-uniaxial compression occurs under a hydrostatic pressure, while the energy is absorbed by the reversible and elastic tilting of the benzene rings within the long-chain ligands. This anisotropic structural deformation effectively modulates the quantum confinement effect by 250 meV via barrier height lowering. The broad tunability within a relatively low pressure range will expand optoelectronic applications to a new paradigm with pressure as a tuning knob.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [4];  [5]; ORCiD logo [4];  [4]; ORCiD logo [5];  [2]; ORCiD logo [6]; ORCiD logo [7]
  1. Tianjin Univ. of Technology (China); Nanyang Technological Univ. (Singapore). Division of Physics and Applied Physics, School of Physical and Mathematical Sciences
  2. Tianjin Univ. of Technology (China)
  3. Inst. of High Performance Computing (Singapore)
  4. Nanyang Technological Univ. (Singapore). Division of Physics and Applied Physics, School of Physical and Mathematical Sciences
  5. Nanyang Technological Univ. (Singapore). School of Materials Science and Engineering
  6. Northwestern Polytechnical Univ. (NPU) (China). Shaanxi Inst. of Flexible Electronics (SIFE)
  7. Nanyang Technological Univ. (Singapore). Division of Physics and Applied Physics, School of Physical and Mathematical Sciences MajuLab, International Joint Research Unit (Singapore); Nanyang Technological Univ. (Singapore). Nanoelectronics Center of Excellence, School of Electrical and Electronic Engineering
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1545866
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
[ Journal Volume: 5; Journal Issue: 7]; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
ENGLISH
Subject:
36 MATERIALS SCIENCE

Citation Formats

Liu, Sheng, Sun, Shishuai, Gan, Chee Kwan, del Águila, Andrés Granados, Fang, Yanan, Xing, Jun, Do, T. Thu Ha, White, Timothy J., Li, Hongguo, Huang, Wei, and Xiong, Qihua. Manipulating efficient light emission in two-dimensional perovskite crystals by pressure-induced anisotropic deformation. United States: N. p., 2019. Web. doi:10.1126/sciadv.aav9445.
Liu, Sheng, Sun, Shishuai, Gan, Chee Kwan, del Águila, Andrés Granados, Fang, Yanan, Xing, Jun, Do, T. Thu Ha, White, Timothy J., Li, Hongguo, Huang, Wei, & Xiong, Qihua. Manipulating efficient light emission in two-dimensional perovskite crystals by pressure-induced anisotropic deformation. United States. doi:10.1126/sciadv.aav9445.
Liu, Sheng, Sun, Shishuai, Gan, Chee Kwan, del Águila, Andrés Granados, Fang, Yanan, Xing, Jun, Do, T. Thu Ha, White, Timothy J., Li, Hongguo, Huang, Wei, and Xiong, Qihua. Mon . "Manipulating efficient light emission in two-dimensional perovskite crystals by pressure-induced anisotropic deformation". United States. doi:10.1126/sciadv.aav9445. https://www.osti.gov/servlets/purl/1545866.
@article{osti_1545866,
title = {Manipulating efficient light emission in two-dimensional perovskite crystals by pressure-induced anisotropic deformation},
author = {Liu, Sheng and Sun, Shishuai and Gan, Chee Kwan and del Águila, Andrés Granados and Fang, Yanan and Xing, Jun and Do, T. Thu Ha and White, Timothy J. and Li, Hongguo and Huang, Wei and Xiong, Qihua},
abstractNote = {The hybrid nature and soft lattice of organolead halide perovskites render their structural changes and optical properties susceptible to external driving forces such as temperature and pressure, remarkably different from conventional semiconductors. Here, we investigate the pressure-induced optical response of a typical two-dimensional perovskite crystal, phenylethylamine lead iodide. At a moderate pressure within 3.5 GPa, its photoluminescence red-shifts continuously, exhibiting an ultrabroad energy tunability range up to 320 meV in the visible spectrum, with quantum yield remaining nearly constant. First-principles calculations suggest that an out-of-plane quasi-uniaxial compression occurs under a hydrostatic pressure, while the energy is absorbed by the reversible and elastic tilting of the benzene rings within the long-chain ligands. This anisotropic structural deformation effectively modulates the quantum confinement effect by 250 meV via barrier height lowering. The broad tunability within a relatively low pressure range will expand optoelectronic applications to a new paradigm with pressure as a tuning knob.},
doi = {10.1126/sciadv.aav9445},
journal = {Science Advances},
number = [7],
volume = [5],
place = {United States},
year = {2019},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Save / Share:

Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Low-Frequency Optical-Phonon Spectrum of Benzil
journal, November 1969


Synthesis of Organic-Inorganic Lead Halide Perovskite Nanoplatelets: Towards High-Performance Perovskite Solar Cells and Optoelectronic Devices
journal, May 2014

  • Ha, Son Tung; Liu, Xinfeng; Zhang, Qing
  • Advanced Optical Materials, Vol. 2, Issue 9
  • DOI: 10.1002/adom.201400106

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

The emergence of perovskite solar cells
journal, July 2014

  • Green, Martin A.; Ho-Baillie, Anita; Snaith, Henry J.
  • Nature Photonics, Vol. 8, Issue 7, p. 506-514
  • DOI: 10.1038/nphoton.2014.134

Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals
journal, January 2015


A hole-conductor-free, fully printable mesoscopic perovskite solar cell with high stability
journal, July 2014


Indirect to direct bandgap transition in methylammonium lead halide perovskite
journal, January 2017

  • Wang, Tianyi; Daiber, Benjamin; Frost, Jarvist M.
  • Energy & Environmental Science, Vol. 10, Issue 2
  • DOI: 10.1039/C6EE03474H

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

High-pressure phases of group-IV, III–V, and II–VI compounds
journal, July 2003


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


Pressure-Induced Metallization of the Halide Perovskite (CH 3 NH 3 )PbI 3
journal, March 2017

  • Jaffe, Adam; Lin, Yu; Mao, Wendy L.
  • Journal of the American Chemical Society, Vol. 139, Issue 12
  • DOI: 10.1021/jacs.7b01162

Structural evolution and photoluminescence properties of a 2D hybrid perovskite under pressure
journal, November 2018

  • Feng, Guoqiang; Qin, Yan; Ran, Cheng
  • APL Materials, Vol. 6, Issue 11
  • DOI: 10.1063/1.5042645

Finite Elastic Strain of Cubic Crystals
journal, June 1947


Lead halide perovskite nanowire lasers with low lasing thresholds and high quality factors
journal, April 2015

  • Zhu, Haiming; Fu, Yongping; Meng, Fei
  • Nature Materials, Vol. 14, Issue 6
  • DOI: 10.1038/nmat4271

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


Predicted band-gap pressure coefficients of all diamond and zinc-blende semiconductors: Chemical trends
journal, August 1999


Visible light response, electrical transport, and amorphization in compressed organolead iodine perovskites
journal, January 2016

  • Ou, Tianji; Yan, Jiejuan; Xiao, Chuanhai
  • Nanoscale, Vol. 8, Issue 22
  • DOI: 10.1039/C5NR07842C

Molecular-Barrier-Enhanced Aromatic Fluorophores in Cocrystals with Unity Quantum Efficiency
journal, January 2018

  • Ye, Huanqing; Liu, Guangfeng; Liu, Sheng
  • Angewandte Chemie International Edition, Vol. 57, Issue 7
  • DOI: 10.1002/anie.201712104

Pressure-Induced Phase Transformation and Band-Gap Engineering of Formamidinium Lead Iodide Perovskite Nanocrystals
journal, July 2018


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

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

Optical study on intrinsic exciton states in high-quality CH 3 NH 3 PbBr 3 single crystals
journal, August 2017


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

Calibration of the ruby pressure gauge to 800 kbar under quasi-hydrostatic conditions
journal, January 1986

  • Mao, H. K.; Xu, J.; Bell, P. M.
  • Journal of Geophysical Research, Vol. 91, Issue B5, p. 4673-4676
  • DOI: 10.1029/JB091iB05p04673

High-Quality Whispering-Gallery-Mode Lasing from Cesium Lead Halide Perovskite Nanoplatelets
journal, July 2016

  • Zhang, Qing; Su, Rui; Liu, Xinfeng
  • Advanced Functional Materials, Vol. 26, Issue 34
  • DOI: 10.1002/adfm.201601690

High-pressure behavior of methylammonium lead iodide (MAPbI 3 ) hybrid perovskite
journal, May 2016

  • Capitani, Francesco; Marini, Carlo; Caramazza, Simone
  • Journal of Applied Physics, Vol. 119, Issue 18
  • DOI: 10.1063/1.4948577

Low-temperature solution-processed wavelength-tunable perovskites for lasing
journal, March 2014

  • Xing, Guichuan; Mathews, Nripan; Lim, Swee Sien
  • Nature Materials, Vol. 13, Issue 5
  • DOI: 10.1038/nmat3911

High pressure photoluminescence and resonant Raman study of GaAs
journal, January 1978


Mechanism of Pressure-Induced Phase Transitions, Amorphization, and Absorption-Edge Shift in Photovoltaic Methylammonium Lead Iodide
journal, August 2016


Pressure-Induced Structural and Optical Properties of Organometal Halide Perovskite-Based Formamidinium Lead Bromide
journal, June 2016


Pressure Effects on Structure and Optical Properties in Cesium Lead Bromide Perovskite Nanocrystals
journal, July 2017

  • Xiao, Guanjun; Cao, Ye; Qi, Guangyu
  • Journal of the American Chemical Society, Vol. 139, Issue 29
  • DOI: 10.1021/jacs.7b05260

A Layered Hybrid Perovskite Solar-Cell Absorber with Enhanced Moisture Stability
journal, September 2014

  • Smith, Ian C.; Hoke, Eric T.; Solis-Ibarra, Diego
  • Angewandte Chemie, Vol. 126, Issue 42
  • DOI: 10.1002/ange.201406466

Temperature-induced ruby fluorescence shifts up to a pressure of 15 GPa in an externally heated diamond anvil cell
journal, January 1999

  • Rekhi, Sandeep; Dubrovinsky, Leonid; Saxena, Surendra
  • High Temperatures-High Pressures, Vol. 31, Issue 3
  • DOI: 10.1068/htrt161

Transcending the slow bimolecular recombination in lead-halide perovskites for electroluminescence
journal, February 2017

  • Xing, Guichuan; Wu, Bo; Wu, Xiangyang
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms14558

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Molecular motion and mobility in an organic single crystal: Raman study and model
journal, December 2009


Two Regimes of Bandgap Red Shift and Partial Ambient Retention in Pressure-Treated Two-Dimensional Perovskites
journal, October 2017


Dielectric confinement effect on excitons in PbI 4 -based layered semiconductors
journal, March 1992


Room-Temperature Near-Infrared High-Q Perovskite Whispering-Gallery Planar Nanolasers
journal, September 2014

  • Zhang, Qing; Ha, Son Tung; Liu, Xinfeng
  • Nano Letters, Vol. 14, Issue 10
  • DOI: 10.1021/nl503057g

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

Efficient planar heterojunction perovskite solar cells by vapour deposition
journal, September 2013

  • Liu, Mingzhen; Johnston, Michael B.; Snaith, Henry J.
  • Nature, Vol. 501, Issue 7467, p. 395-398
  • DOI: 10.1038/nature12509

Nanocube Superlattices of Cesium Lead Bromide Perovskites and Pressure-Induced Phase Transformations at Atomic and Mesoscale Levels
journal, March 2017

  • Nagaoka, Yasutaka; Hills-Kimball, Katie; Tan, Rui
  • Advanced Materials, Vol. 29, Issue 18
  • DOI: 10.1002/adma.201606666

The effects of pressure on the density, dielectric constant, and viscosity of several hydrocarbons and other organic liquids
journal, March 1969

  • Brazier, D. W.; Freeman, G. R.
  • Canadian Journal of Chemistry, Vol. 47, Issue 6
  • DOI: 10.1139/v69-147

Vapor Phase Synthesis of Organometal Halide Perovskite Nanowires for Tunable Room-Temperature Nanolasers
journal, June 2015


Color-stable highly luminescent sky-blue perovskite light-emitting diodes
journal, August 2018


Origin of unusual bandgap shift and dual emission in organic-inorganic lead halide perovskites
journal, October 2016

  • Dar, M. Ibrahim; Jacopin, Gwénolé; Meloni, Simone
  • Science Advances, Vol. 2, Issue 10
  • DOI: 10.1126/sciadv.1601156

Direct Observation of Electron–Phonon Coupling and Slow Vibrational Relaxation in Organic–Inorganic Hybrid Perovskites
journal, October 2016

  • Straus, Daniel B.; Hurtado Parra, Sebastian; Iotov, Natasha
  • Journal of the American Chemical Society, Vol. 138, Issue 42
  • DOI: 10.1021/jacs.6b08175