Cesium-mediated electron redistribution and electron-electron interaction in high-pressure metallic CsPbI3

Feng Ke, Jiejuan Yan, Shanyuan Niu, Jiajia Wen, Ketao Yin (), Hong Yang, Nathan R. Wolf, Yan-Kai Tzeng, Hemamala I. Karunadasa, Young S. Lee, Wendy L. Mao and Yu Lin ()
Additional contact information
Feng Ke: SLAC National Accelerator Laboratory
Jiejuan Yan: Stanford University
Shanyuan Niu: SLAC National Accelerator Laboratory
Jiajia Wen: SLAC National Accelerator Laboratory
Ketao Yin: Linyi University
Hong Yang: Stanford University
Nathan R. Wolf: Stanford University
Yan-Kai Tzeng: Stanford University
Hemamala I. Karunadasa: SLAC National Accelerator Laboratory
Young S. Lee: SLAC National Accelerator Laboratory
Wendy L. Mao: SLAC National Accelerator Laboratory
Yu Lin: SLAC National Accelerator Laboratory

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract Electron-phonon coupling was believed to govern the carrier transport in halide perovskites and related phases. Here we demonstrate that electron-electron interaction enhanced by Cs-involved electron redistribution plays a direct and prominent role in the low-temperature electrical transport of compressed CsPbI3 and renders Fermi liquid (FL)-like behavior. By compressing δ-CsPbI3 to 80 GPa, an insulator-semimetal-metal transition occurs, concomitant with the completion of a slow structural transition from the one-dimensional Pnma (δ) phase to a three-dimensional Pmn21 (ε) phase. Deviation from FL behavior is observed upon CsPbI3 entering the metallic ε phase, which progressively evolves into a FL-like state at 186 GPa. First-principles density functional theory calculations reveal that the enhanced electron-electron coupling results from the sudden increase of the 5d state occupation in Cs and I atoms. Our study presents a promising strategy of cationic manipulation for tuning the electronic structure and carrier scattering of halide perovskites at high pressure.

Date: 2022
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DOI: 10.1038/s41467-022-34786-5

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