Anharmonic phonon behavior via irreducible derivatives: self-consistent perturbation theory and molecular dynamics

Abstract

Cubic phonon interactions are now regularly computed from first principles, and the quartic interactions have begun to receive more attention. Given this realistic anharmonic vibrational Hamiltonian, the classical phonon Green's function can be precisely measured using molecular dynamics, which can then be used to rigorously assess the range of validity for self-consistent diagrammatic approaches in the classical limit. Here we use the bundled irreducible derivative approach to efficiently and precisely compute the cubic and quartic phonon interactions of CaF${}_2$, systematically obtaining the vibrational Hamiltonian purely in terms of irreducible derivatives. non frequency shifts and linewidths, We demonstrate that the 4-phonon sunset diagram has an important contribution to the optical phonon linewidths beyond $T=500$ K. Reasonable results are obtained even at $T=900$ K when performing self-consistency using the 4-phonon loop diagram and evaluating the 3-phonon bubble and 4-phonon sunset diagrams post self-consistency. Further improvements are obtained by performing quasiparticle perturbation theory, where both the 4-phonon loop and the real part of the 3-phonon bubble are employed during self-consistency. Our irreducible derivative approach to self-consistent perturbation theory is a robust tool for studying anharmonic phonons in both the quantum and classical regimes.

arXiv comment8 pages, 5 figures

References in corpus (40)

• Quasiparticle Self-Consistent GW Theory
• Heat transport in silicon from first principles calculations
• 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
• All-electron self-consistent GW approximation: Application to Si, MnO, and NiO
• 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
• 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
• Quantum Crystal Structure in the 250 K Superconducting Lanthanum Hydride
• Quantum Hydrogen-Bond Symmetrization and High-Temperature Superconductivity in Hydrogen Sulfide
• First-Principles Theory of Anharmonicity and the Inverse Isotope Effect in Superconducting Palladium-Hydride Compounds
• 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
• First-Principles Lattice Dynamics Method for Strongly Anharmonic Crystals
• Compressive sensing lattice dynamics. I. General formalism
• Strong anharmonicity induces quantum melting of charge density wave in 2H-NbSe$\_2$ under pressure
• First-principles study of phonon anharmonicity and negative thermal expansion in ScF3
• Anharmonic phonon frequency shift in MgB2
• First-Principles Phonon Quasiparticle Theory Applied to a Strongly Anharmonic Halide Perovskite
• Anharmonic effects in atomic hydrogen: superconductivity and lattice dynamical stability
• Electronic structure of Pu and Am metals by self consistent relativistic GW
• Anharmonic stabilization of the high-pressure simple cubic phase of calcium
• Anomalous thermal conductivity and suppression of negative thermal expansion in ScF3
• A path-integral molecular dynamics simulation of diamond
• Time-Dependent Self Consistent Harmonic Approximation: Anharmonic nuclear quantum dynamics and time correlation functions
• High-pressure phase diagram of hydrogen and deuterium sulfides from first principles: structural and vibrational properties including quantum and anharmonic effects
• Quantum Self-Consistent Ab-Initio Lattice Dynamics
• Path-integral molecular dynamics simulation of 3C-SiC
• Ab initio structural optimization at finite temperatures based on anharmonic phonon theory: Application to the structural phase transitions of BaTiO${}_3$
• A group theoretical approach to computing phonons and their interactions
• Anharmonic Grüneisen theory based on self-consistent phonon theory: Impact of phonon-phonon interaction neglected in the quasiharmonic theory
• Gaussian time-dependent variational principle for the finite-temperature anharmonic lattice dynamics
• Validating First-Principles Phonon Lifetimes via Inelastic Neutron Scattering
• Origin of anomalous anharmonic lattice dynamics of lead telluride
• The generalized quasiharmonic approximation via space group irreducible derivatives
• The microscopic origin of anomalous properties of ice relies on the strong quantum anharmonic regime of atomic vibrations
• LO-mode phonon of KCl and NaCl at 300 K by inelastic X ray scattering measurements and first principles calculations
• Path Integral Monte Carlo study of phonons in the bcc phase of ${}^4$He

Cited by in corpus (2)

• Phonon thermal transport in UO${}_2$ via self-consistent perturbation theory
• Lattice Thermal Transport Beyond the Quasiparticle Approximation: Nontrivial Spectral Competition between Three- and Four-Phonon Interactions