Efficient first-principles methodology for the calculation of the all-phonon inelastic scattering in solids

Abstract

Inelastic scattering experiments are key methods for mapping the full dispersion of fundamental excitations of solids in the ground as well as non-equilibrium states. A quantitative analysis of inelastic scattering in terms of phonon excitations requires identifying the role of multi-phonon processes. Here, we develop an efficient first-principles methodology for calculating the all-phonon quantum mechanical structure factor of solids. We demonstrate our method by obtaining excellent agreement between measurements and calculations of the diffuse scattering patterns of black phosphorus, showing that multi-phonon processes play a substantial role. The present approach constitutes a step towards the interpretation of static and time-resolved electron, X-ray, and neutron inelastic scattering data.

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Cited by in corpus (16)

• Ultrafast dynamics of electrons and phonons: from the two-temperature model to the time-dependent Boltzmann equation
• Anharmonic electron-phonon coupling in ultrasoft and locally disordered perovskites
• Accessing the anisotropic non-thermal phonon populations in black phosphorus
• Direct visualization of polaron formation in the thermoelectric SnSe
• Direct view of phonon dynamics in atomically thin MoS${}_2$
• Multi-phonon diffuse scattering in solids from first-principles: Application to layered crystals and 2D materials
• Vibrational dichroism of chiral valley phonons
• Assessing Phonon Coherence Using Spectroscopy
• Understanding chiral charge-density wave by frozen chiral phonon
• Momentum-Resolved Signatures of Carrier Screening Effects on Electron-Phonon Coupling in MoS${}_2$
• Ultrafast Phonon-Diffuse Scattering as a Tool for Observing Chiral Phonons in Monolayer Hexagonal Lattices
• Fingerprints of hot-phonon physics in time-resolved correlated quantum lattice dynamics
• Ultrafast Electron Diffuse Scattering as a Tool for Studying Phonon Transport: Phonon Hydrodynamics and Second Sound Oscillations
• Ultrafast Electron Diffraction: Visualizing Dynamic States of Matter
• Properties and challenges of hot-phonon physics in metals: MgB${}_2$ and other compounds
• Symmetry-protected topological polarons