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.

References in corpus (12)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Non-adiabatic Kohn-anomaly in a doped graphene monolayer
• Anharmonicity Measure for Materials
• Nonequilibrium Lattice Dynamics in Monolayer MoS2
• Non-adiabatic Kohn Anomaly in Heavily Boron-doped Diamond
• Anharmonic effects in MgB2? A comparative inelastic X-ray scattering and Raman study
• Soft-phonon-driven superconductivity in CaAlSi as seen by inelastic x-ray scattering
• Role of defects in determining the magnetic ground state of ytterbium titanate
• Multi-phonon diffuse scattering in solids from first-principles: Application to layered crystals and 2D materials
• Two-phonon contributions to inelastic x-ray scattering spectra of MgB2
• Full elasticity tensor from thermal diffuse scattering

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• Vibrational dichroism of chiral valley phonons
• Assessing Phonon Coherence Using Spectroscopy
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• Momentum-Resolved Signatures of Carrier Screening Effects on Electron-Phonon Coupling in MoS${}_2$
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• Symmetry-protected topological polarons
• Properties and challenges of hot-phonon physics in metals: MgB${}_2$ and other compounds