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arXiv · 2103.00745

First-Principles Phonon Quasiparticle Theory Applied to a Strongly Anharmonic Halide Perovskite

Terumasa Tadano·Wissam A. Saidi
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Abstract

Understanding and predicting lattice dynamics in strongly anharmonic crystals is one of the long-standing challenges in condensed matter physics. Here we propose a first-principles method that gives accurate quasiparticle (QP) peaks of the phonon spectrum with strong anharmonic broadening. On top of the conventional first-order self-consistent phonon (SC1) dynamical matrix, the proposed method incorporates frequency renormalization effects by the bubble self-energy within the QP approximation. We apply the developed methodology to the strongly anharmonic $\alpha$-CsPbBr$_3$ that displays phonon instability within the harmonic approximation in the whole Brillouin zone. While the SC1 theory significantly underestimates the cubic-to-tetragonal phase transition temperature (\tc) by more than 50\%, we show that our approach yields \tc = 404--423~K, in excellent agreement with the experimental value of 403~K. We also demonstrate that an accurate determination of QP peaks is paramount for quantitative prediction and elucidation of phonon linewidth..

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Terumasa Tadano, Wissam A. Saidi. 2021-03-01. First-Principles Phonon Quasiparticle Theory Applied to a Strongly Anharmonic Halide Perovskite. https://doi.org/10.1103/physrevlett.129.185901

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