Issue 10, 2023

Phonon-driven transient bandgap renormalization in perovskite single crystals

Abstract

Tailoring the electronic structure of perovskite materials on ultrafast timescales is expected to shed light on optimizing optoelectronic applications. However, the transient bandgap renormalization observed upon photoexcitation is commonly explained by many-body interactions of optically created electrons and holes, which shrink the original bandgap by a few tens of millielectronvolts with a sub-picosecond time constant, while the accompanying phonon-induced effect remains hitherto unexplored. Here we unravel a significant contribution of hot phonons in the photo-induced transient bandgap renormalization in MAPbBr3 single crystals, as evidenced by asymmetric spectral evolutions and transient reflection spectral shifts in the picosecond timescale. Moreover, we performed a spatiotemporal study upon optical excitation with time-resolved scanning electron microscopy and identified that the surface charge carrier diffusion and transient bandgap renormalization are strongly correlated in time. These findings highlight the need to re-evaluate current theories on photo-induced bandgap renormalization and provide a new approach for precisely controlling the optical and electronic properties of perovskite materials, enabling the design and fabrication of high-performance optoelectronic devices with exceptional efficiency and unique properties.

Graphical abstract: Phonon-driven transient bandgap renormalization in perovskite single crystals

Supplementary files

Article information

Article type
Communication
Submitted
16 4 2023
Accepted
04 7 2023
First published
04 7 2023
This article is Open Access
Creative Commons BY-NC license

Mater. Horiz., 2023,10, 4192-4201

Phonon-driven transient bandgap renormalization in perovskite single crystals

L. Wang, H. Wang, R. Nughays, W. Ogieglo, J. Yin, L. Gutiérrez-Arzaluz, X. Zhang, J. Wang, I. Pinnau, O. M. Bakr and O. F. Mohammed, Mater. Horiz., 2023, 10, 4192 DOI: 10.1039/D3MH00570D

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