Anharmonic lattice dynamics via the special displacement method

Abstract

On the basis of the self-consistent phonon theory and the special displacement method, we develop an approach for the treatment of anharmonicity in solids. We show that this approach enables the efficient calculation of temperature-dependent anharmonic phonon dispersions, requiring very few steps to achieve minimization of the system's free energy. We demonstrate this methodology in the regime of strongly anharmonic materials which exhibit a multi-well potential energy surface, like cubic SrTiO${}_3$, CsPbBr${}_3$, CsPbI${}_3$, CsSnI${}_3$, and Zr. Our results are in good agreement with experiments and previous first-principles studies relying on stochastic nonperturbative and molecular dynamics simulations. We achieve a very robust workflow by using harmonic phonons of the polymorphous ground state as the starting point and an iterative mixing scheme of the dynamical matrix. We also suggest that the phonons of the polymorphous ground state might provide an excellent starting approximation to explore anharmonicity. Given the simplicity, efficiency, and stability of the present treatment to anharmonicity, it is especially suitable for use with any electronic structure code and for investigating electron-phonon couplings in strongly anharmonic systems.

arXiv comment10 figures

References in corpus (43)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• 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
• Optimized norm-conserving Vanderbilt pseudopotentials
• The PseudoDojo: Training and grading a 85 element optimized norm-conserving pseudopotential table
• Electron-phonon interactions from first principles
• EPW: Electron-phonon coupling, transport and superconducting properties using maximally localized Wannier functions
• Lattice dynamics of anharmonic solids from first principles
• Temperature dependent effective potential method for accurate free energy calculations of solids
• Self-consistent phonon calculations of lattice dynamical properties in cubic SrTiO${}_3$ with first-principles anharmonic force constants
• Anharmonic free energies and phonon dispersions from the stochastic self-consistent harmonic approximation: application to platinum and palladium hydrides
• Entropy driven stabilization of energetically unstable crystal structures explained from first principles theory
• Lattice anharmonicity and thermal conductivity from compressive sensing of first-principles calculations
• Thermal properties of materials from ab-initio quasi-harmonic phonons
• First-Principles Theory of Anharmonicity and the Inverse Isotope Effect in Superconducting Palladium-Hydride Compounds
• One-shot calculation of temperature-dependent optical spectra and phonon-induced band-gap renormalization
• The Stochastic Self-Consistent Harmonic Approximation: Calculating Vibrational Properties of Materials with Full Quantum and Anharmonic Effects
• The polymorphous nature of cubic halide perovskites
• Second order structural phase transitions, free energy curvature, and temperature-dependent anharmonic phonons in the self-consistent harmonic approximation: theory and stochastic implementation
• Electron-Phonon Scattering in the Presence of Soft Modes and Electron Mobility in SrTiO${}_3$ Perovskite from First Principles
• Ab initio Green-Kubo Approach for the Thermal Conductivity of Solids
• Theory of the special displacement method for electronic structure calculations at finite temperature
• Stochastic approach to phonon-assisted optical absorption
• Anharmonic phonon frequency shift in MgB2
• Anharmonic stabilization and band gap renormalization in the perovskite CsSnI${}_3$
• Anharmonic phonon spectra of PbTe and SnTe in the self-consistent harmonic approximation
• Anharmonic and Quantum Fluctuations in Molecular Crystals: A First-Principles Study of the Stability of Paracetamol
• Anharmonic stabilization of the high-pressure simple cubic phase of calcium
• First-principles calculations of phonon frequencies, lifetimes and spectral functions from weak to strong anharmonicity: the example of palladium hydrides
• Direct evidence of weakly dispersed and strongly anharmonic optical phonons in hybrid perovskites
• Anomalous thermal conductivity and suppression of negative thermal expansion in ScF3
• Nonequilibrium Lattice Dynamics in Monolayer MoS2
• First-Principles Electron Transport with Phonon Coupling: Large-Scale at Low Cost
• Accurate and efficient band-gap predictions for metal halide perovskites at finite temperature
• Fully Anharmonic, Non-Perturbative Theory of Vibronically Renormalized Electronic Band Structures
• Unified approach to polarons and phonon-induced band structure renormalization
• Zero-point Renormalization of the Band Gap of Semiconductors and Insulators Using the PAW Method
• Quantum Self-Consistent Ab-Initio Lattice Dynamics
• Direct view of phonon dynamics in atomically thin MoS${}_2$
• Understanding the lattice thermal conductivity of SrTiO3 from an ab initio perspective
• Computational protocol to evaluate electron-phonon interactions within density matrix perturbation theory

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