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

Science Advances
Sheng LiuQihua Xiong

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.

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Citations

Jun 2, 2020·Nanoscale Horizons : the Home for Rapid Reports of Exceptional Significance in Nanoscience and Nanotechnolgy·Hao LiuBo Zou
Jul 1, 2020·Proceedings of the National Academy of Sciences of the United States of America·Lingping KongHo-Kwang Mao
Jan 6, 2021·Chemical Society Reviews·Mingze Li, Zhiguo Xia
Feb 4, 2021·Chemical Communications : Chem Comm·Qiao-Qiao SunShuang-Quan Zang
Dec 12, 2020·Nature Communications·Yicheng ZhaoChristoph J Brabec
Dec 6, 2020·Nature Nanotechnology·Jean-Christophe BlanconAditya D Mohite
Dec 22, 2020·Advanced Science·Linglong ZhangYuerui Lu
May 15, 2021·ACS Nano·Hyeongwoo LeeKyoung-Duck Park
May 27, 2020·The Journal of Physical Chemistry Letters·Long ZhangBo Zou
May 28, 2020·Nano Letters·T Thu Ha DoQihua Xiong
Jul 3, 2021·Nature Materials·Rui SuQihua Xiong
Oct 19, 2021·The Journal of Physical Chemistry Letters·Algirdas DučinskasMichael Grätzel

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Methods Mentioned

BETA
chemical vapor deposition
x-ray diffraction
pull down

Software Mentioned

Vienna Ab initio Simulation Package

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