Phonon-driven transient bandgap renormalization in perovskite single crystals

Lijie Wang, Hong Wang, Razan Nughays, Wojciech Ogieglo, Jun Yin, Luis Gutiérrez-Arzaluz, Xinyuan Zhang, Jian Xin Wang, Ingo Pinnau, Osman M. Bakr, Omar F. Mohammed*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

1 Scopus citations


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.

Original languageEnglish (US)
Pages (from-to)4192-4201
Number of pages10
JournalMaterials Horizons
Issue number10
StateAccepted/In press - 2023

ASJC Scopus subject areas

  • General Materials Science
  • Mechanics of Materials
  • Process Chemistry and Technology
  • Electrical and Electronic Engineering


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