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

Author

Listed:
  • Feng Ke

    (SLAC National Accelerator Laboratory
    Stanford University)

  • Jiejuan Yan

    (Stanford University)

  • Shanyuan Niu

    (SLAC National Accelerator Laboratory
    Stanford University
    Nanjing University)

  • 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
    Stanford University)

  • Young S. Lee

    (SLAC National Accelerator Laboratory
    Stanford University)

  • Wendy L. Mao

    (SLAC National Accelerator Laboratory
    Stanford University)

  • Yu Lin

    (SLAC National Accelerator Laboratory)

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.

Suggested Citation

  • 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 & Yu Lin, 2022. "Cesium-mediated electron redistribution and electron-electron interaction in high-pressure metallic CsPbI3," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-34786-5
    DOI: 10.1038/s41467-022-34786-5
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