Ultrafast relaxation of lattice distortion in two-dimensional perovskites

Hao Zhang, Wenbin Li, Joseph Essman, Claudio Quarti, Isaac Metcalf, Wei Yi Chiang, Siraj Sidhik, Jin Hou, Austin Fehr, Andrew Attar, Ming Fu Lin, Alexander Britz, Xiaozhe Shen, Stephan Link, Xijie Wang, Uwe Bergmann, Mercouri G. Kanatzidis, Claudine Katan, Jacky Even, Jean Christophe BlanconAditya D. Mohite

Research output: Contribution to journalArticlepeer-review

Abstract

Direct visualization of ultrafast coupling between charge carriers and lattice degrees of freedom in photoexcited semiconductors has remained a long-standing challenge and is critical for understanding the light-induced physical behaviour of materials under extreme non-equilibrium conditions. Here we obtain a direct visualization of the structural dynamics in monocrystalline 2D perovskites. We achieve this by monitoring the evolution of wavevector-resolved ultrafast electron diffraction intensity following above-bandgap high-density photoexcitation. Our analysis reveals a light-induced ultrafast reduction in antiferro-distortion resulting from a strong interaction between the electron–hole plasma and perovskite lattice, which induces an in-plane octahedra rotation towards a more symmetric phase. Correlated ultrafast spectroscopy performed at the same carrier density as ultrafast electron diffraction reveals that the creation of a dense electron–hole plasma triggers the relaxation of lattice distortion at shorter timescales by modulating the crystal cohesive energy. Finally, we show that the interaction between carrier gas and lattice can be altered by tailoring the rigidity of the 2D perovskite by choosing an appropriate organic spacer layer.

Original languageEnglish (US)
Pages (from-to)545-550
Number of pages6
JournalNature Physics
Volume19
Issue number4
DOIs
StatePublished - Apr 2023
Externally publishedYes

ASJC Scopus subject areas

  • General Physics and Astronomy

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