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

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..

arXiv comment7 pages, 3 figures

References in corpus (26)

• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Phonons and related properties of extended systems from density-functional perturbation theory
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Quasiparticle Self-Consistent GW Theory
• Precision and efficiency in solid-state pseudopotential calculations
• Giant Anharmonic Phonon Scattering in PbTe
• Lattice dynamics of anharmonic solids from first principles
• Unified theory of thermal transport in crystals and disordered solids
• Self-consistent phonon calculations of lattice dynamical properties in cubic SrTiO${}_3$ with first-principles anharmonic force constants
• Hydrogen sulphide at high pressure: a strongly-anharmonic phonon-mediated superconductor
• Anharmonic free energies and phonon dispersions from the stochastic self-consistent harmonic approximation: application to platinum and palladium hydrides
• Lattice anharmonicity and thermal conductivity from compressive sensing of first-principles calculations
• Quantum Crystal Structure in the 250 K Superconducting Lanthanum Hydride
• Quartic Anharmonicity of Rattlers and Its Effect on Lattice Thermal Conductivity of Clathrates from First Principles
• Second order structural phase transitions, free energy curvature, and temperature-dependent anharmonic phonons in the self-consistent harmonic approximation: theory and stochastic implementation
• Terahertz-Driven Phonon Upconversion in SrTiO3
• First-Principles Lattice Dynamics Method for Strongly Anharmonic Crystals
• Effect of van Hove singularities on high-Tc superconductivity in H3S
• Phonon Collapse and Second-Order Phase Transition in Thermoelectric SnSe
• First-principles study of phonon anharmonicity and negative thermal expansion in ScF3
• Anharmonic stabilization and band gap renormalization in the perovskite CsSnI${}_3$
• Anharmonicity Measure for Materials
• Anomalous thermal conductivity and suppression of negative thermal expansion in ScF3
• Efficient construction of linear models in materials modeling and applications to force constant expansions
• Common acoustic phonon lifetimes in inorganic and hybrid lead halide perovskites

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