Multi-phonon diffuse scattering in solids from first-principles: Application to layered crystals and 2D materials

Abstract

Time-resolved diffuse scattering experiments have gained increasing attention due to their potential to reveal non-equilibrium dynamics of crystal lattice vibrations with full momentum resolution. Although progress has been made in interpreting experimental data on the basis of one-phonon scattering, understanding the role of individual phonons can be sometimes hindered by multi-phonon excitations. In Ref. [{\it arXiv:2103.10108}] we have introduced a rigorous approach for the calculation of the all-phonon inelastic scattering intensity of solids from first-principles. In the present work, we describe our implementation in detail and show that multi-phonon interactions are captured efficiently by exploiting translational and time-reversal symmetries of the crystal. We demonstrate its predictive power by calculating the scattering patterns of monolayer molybdenum disulfide (MoS${}_2$), bulk MoS${}_2$, and black phosphorus (bP), and we obtain excellent agreement with our measurements of thermal electron diffuse scattering. Remarkably, our results show that multi-phonon excitations dominate in bP across multiple Brillouin zones, while in MoS${}_2$ they play a less pronounced role. We expand our analysis for each system and examine the effect of individual atomic and interatomic vibrational motion on the diffuse scattering signals. We further demonstrate the high-throughput capability of our approach by reporting all-phonon scattering maps of 2D MoSe2, WSe2, WS2, graphene, and CdI2, rationalizing in each case the effect of multi-phonon processes. As a side point, we show that the special displacement method reproduces the thermally distorted configuration that generates precisely the all-phonon diffuse pattern.

References in corpus (47)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Phonons and related properties of extended systems from density-functional perturbation theory
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Separable Dual Space Gaussian Pseudo-potentials
• Relativistic separable dual-space Gaussian Pseudopotentials from H to Rn
• Two-dimensional materials from high-throughput computational exfoliation of experimentally known compounds
• Isolation and characterization of few-layer black phosphorus
• 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
• Non-adiabatic Kohn-anomaly in a doped graphene monolayer
• Anharmonic free energies and phonon dispersions from the stochastic self-consistent harmonic approximation: application to platinum and palladium hydrides
• Density functional perturbation theory for gated two-dimensional heterostructures: Theoretical developments and application to flexural phonons in graphene
• One-shot calculation of temperature-dependent optical spectra and phonon-induced band-gap renormalization
• Electron-phonon coupling and energy flow in a simple metal beyond the two-temperature approximation
• Mapping momentum-dependent electron-phonon coupling and non-equilibrium phonon dynamics with ultrafast electron diffuse scattering
• Theory of the special displacement method for electronic structure calculations at finite temperature
• Stochastic approach to phonon-assisted optical absorption
• Momentum-Resolved View of Electron-Phonon Coupling in Multilayer WSe${}_2$
• Direct determination of mode-projected electron-phonon coupling in the time-domain
• Beyond the molecular movie: dynamics of bands and bonds during a photo-induced phase transition
• Anharmonic stabilization and band gap renormalization in the perovskite CsSnI${}_3$
• Toward precise simulations of the coupled ultrafast dynamics of electrons and atomic vibrations in materials
• Compact femtosecond electron diffractometer with 100 keV electron bunches approaching the single-electron pulse duration limit
• Efficient first-principles calculation of phonon assisted photocurrent in large-scale solar cell devices
• Mechanisms of electron-phonon coupling unraveled in momentum and time: The case of soft-phonons in TiSe${}_2$
• Nonequilibrium Lattice Dynamics in Monolayer MoS2
• Tracking the Ultrafast Non-Equilibrium Energy Flow between Electronic and Lattice Degrees of Freedom in Crystalline Nickel
• Accurate optical spectra through time-dependent density functional theory based on screening-dependent hybrid functionals
• First-Principles Electron Transport with Phonon Coupling: Large-Scale at Low Cost
• Unified theory of electron-phonon renormalization and phonon-assisted optical absorption
• Accessing the anisotropic non-thermal phonon populations in black phosphorus
• Fully Anharmonic, Non-Perturbative Theory of Vibronically Renormalized Electronic Band Structures
• Time- and momentum-resolved phonon population dynamics with ultrafast electron diffuse scattering
• Imaging nonequilibrium atomic vibrations with x-ray diffuse scattering
• Non-adiabatic Kohn Anomaly in Heavily Boron-doped Diamond
• Anisotropic Nonequilibrium Lattice Dynamics of Black Phosphorus
• Soft-phonon-driven superconductivity in CaAlSi as seen by inelastic x-ray scattering
• Direct Measurement of Anharmonic Decay Channels of a Coherent Phonon
• Efficient first-principles methodology for the calculation of the all-phonon inelastic scattering in solids
• Two-phonon contributions to inelastic x-ray scattering spectra of MgB2
• Full elasticity tensor from thermal diffuse scattering
• Observation of large multiple scattering effects in ultrafast electron diffraction on single crystal silicon
• Phonon-assisted processes in the ultraviolet transient optical response of graphene
• Boron phosphide as a \emph{p}-type transparent conductor: optical absorption and transport through electron-phonon coupling
• Temperature dependence of the optical properties of silicon nanocrystals
• Ab initio investigation on the experimental observation of metallic hydrogen

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• Momentum-Resolved Signatures of Carrier Screening Effects on Electron-Phonon Coupling in MoS${}_2$
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• 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