Toward precise simulations of the coupled ultrafast dynamics of electrons and atomic vibrations in materials

Abstract

Ultrafast spectroscopies can access the dynamics of electrons and nuclei at short timescales, shedding light on nonequilibrium phenomena in materials. However, development of accurate calculations to interpret these experiments has lagged behind as widely adopted simulation schemes are limited to sub-picosecond timescales or employ simplified interactions lacking quantitative accuracy. Here we show a precise approach to obtain the time-dependent populations of nonequilibrium electrons and atomic vibrations (phonons) up to tens of picoseconds, with a femtosecond time resolution. Combining first-principles electron-phonon and phonon-phonon interactions with a parallel numerical scheme to time-step the coupled electron and phonon Boltzmann equations, our method provides unprecedented microscopic insight into scattering mechanisms in excited materials. Focusing on graphene as a case study, we demonstrate calculations of ultrafast electron and phonon dynamics, transient optical absorption, structural snapshots and diffuse X-ray scattering. Our first-principles approach paves the way for quantitative atomistic simulations of ultrafast dynamics in materials.

References in corpus (7)

• Ultrahigh electron mobility in suspended graphene
• Suspended Graphene: a bridge to the Dirac point
• Theory of double-resonant Raman spectra in graphene: intensity and line shape of defect-induced and two-phonon bands
• Impact of the electron-electron correlation on phonon dispersions: failure of LDA and GGA functionals in graphene and graphite
• Theory of Thermal Relaxation of Electrons in Semiconductors
• First-principles dynamics of electrons and phonons
• Nonequilibrium Lattice Dynamics in Monolayer MoS2

Cited by in corpus (21)

• Ultrafast dynamics of electrons and phonons: from the two-temperature model to the time-dependent Boltzmann equation
• Efficient first-principles methodology for the calculation of the all-phonon inelastic scattering in solids
• Multi-phonon diffuse scattering in solids from first-principles: Application to layered crystals and 2D materials
• Magnetotransport in semiconductors and two-dimensional materials from first principles
• Vibrational dichroism of chiral valley phonons
• Quantum theory of light-driven coherent lattice dynamics
• Strain-induced activation of chiral-phonon emission in monolayer WS${}_2$
• Revealing Ultrafast Phonon Mediated Inter-Valley Scattering through Transient Absorption and High Harmonic Spectroscopies
• Ab initio electron dynamics in high electric fields: accurate predictions of velocity-field curves
• Excitation and Relaxation of Nonthermal Electron Energy Distributions in Metals with Application to Gold
• Momentum-Resolved Signatures of Carrier Screening Effects on Electron-Phonon Coupling in MoS${}_2$
• Fingerprints of hot-phonon physics in time-resolved correlated quantum lattice dynamics
• Advancing Simulations of Coupled Electron and Phonon Nonequilibrium Dynamics Using Adaptive and Multirate Time Integration
• Dominant two-dimensional electron-phonon interactions in the bulk Dirac semimetal Na3Bi
• Pausing ultrafast melting by timed multiple femtosecond-laser pulses
• Element-specific ultrafast lattice dynamics in monolayer WSe2
• Phonon-assisted carrier cooling in h-BN/graphene van der Waals heterostructures
• Overscreening-free electron-phonon interaction in realistic materials
• Nonlinear phononics in Bi${}_2$Te${}_3$ nanoscale thin films: A theoretical approach
• Properties and challenges of hot-phonon physics in metals: MgB${}_2$ and other compounds
• Excitonic effects in the photocarriers dynamics of two-dimensional materials