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.

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Cited by in corpus (14)

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• Anharmonic electron-phonon coupling in ultrasoft and locally disordered perovskites
• Direct visualization of polaron formation in the thermoelectric SnSe
• Direct view of phonon dynamics in atomically thin MoS${}_2$
• Efficient first-principles methodology for the calculation of the all-phonon inelastic scattering in solids
• Vibrational dichroism of chiral valley phonons
• 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