Electron-phonon interaction in efficient perovskite blue emitters

Nature Materials
Xiwen GongEdward H Sargent

Abstract

Low-dimensional perovskites have-in view of their high radiative recombination rates-shown great promise in achieving high luminescence brightness and colour saturation. Here we investigate the effect of electron-phonon interactions on the luminescence of single crystals of two-dimensional perovskites, showing that reducing these interactions can lead to bright blue emission in two-dimensional perovskites. Resonance Raman spectra and deformation potential analysis show that strong electron-phonon interactions result in fast non-radiative decay, and that this lowers the photoluminescence quantum yield (PLQY). Neutron scattering, solid-state NMR measurements of spin-lattice relaxation, density functional theory simulations and experimental atomic displacement measurements reveal that molecular motion is slowest, and rigidity greatest, in the brightest emitter. By varying the molecular configuration of the ligands, we show that a PLQY up to 79% and linewidth of 20 nm can be reached by controlling crystal rigidity and electron-phonon interactions. Designing crystal structures with electron-phonon interactions in mind offers a previously underexplored avenue to improve optoelectronic materials' performance.

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Citations

Aug 31, 2018·Advanced Materials·Li Na QuanEdward H Sargent
Dec 12, 2019·Nature Communications·Qi WangJinsong Huang
Apr 29, 2020·Nature Communications·Michael SeitzFerry Prins
Jan 16, 2019·Nature Materials·Félix ThouinAjay Ram Srimath Kandada
Dec 19, 2019·Nature Communications·Tianjun LiuOliver Fenwick
Oct 3, 2019·Physical Chemistry Chemical Physics : PCCP·Zhi-Gang Yu
Sep 7, 2018·Advanced Materials·Samuel D StranksFelix Deschler
Apr 25, 2020·Advanced Science·Hongyan LiangEdward H Sargent
Feb 3, 2020·The Journal of Chemical Physics·Shibin DengLibai Huang
Feb 9, 2019·Chemical Communications : Chem Comm·Wouter T M Van GompelDirk Vanderzande
Dec 23, 2020·Advanced Materials·Joao M PinaEdward H Sargent
Dec 6, 2020·Nature Nanotechnology·Jean-Christophe BlanconAditya D Mohite
Apr 11, 2020·ACS Nano·Balaji DhanabalanRoman Krahne
Feb 28, 2021·ACS Nano·Mark BatheSanghamitra Neogi
Mar 9, 2021·The Journal of Physical Chemistry Letters·Nadège MarchalFilippo De Angelis
Mar 5, 2021·Nature Communications·Weijian TaoHaiming Zhu
Mar 21, 2021·Light, Science & Applications·Li ZhangMingjian Yuan

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Methods Mentioned

BETA
XRD
X-ray
elastic neutron scattering
NMR

Software Mentioned

VASP
OLEX2

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