Toward precise simulations of the coupled ultrafast dynamics of electrons and atomic vibrations in materials
arXiv:2009.07958 · doi:10.1103/PhysRevResearch.3.023072
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 (31)
- Phonons and related properties of extended systems from density-functional perturbation theory
- Ultrahigh electron mobility in suspended graphene
- Wannier90: A Tool for Obtaining Maximally-Localised Wannier Functions
- Maximally localized Wannier functions: Theory and applications
- Suspended Graphene: a bridge to the Dirac point
- Kohn Anomalies and Electron-Phonon Interaction in Graphite
- An optically stimulated superconducting-like phase in K3C60 far above equilibrium Tc
- Lattice dynamics of anharmonic solids from first principles
- Measurement of Ultrafast Carrier Dynamics in Epitaxial Graphene
- Temperature dependent effective potential method for accurate free energy calculations of solids
- Theory of double-resonant Raman spectra in graphene: intensity and line shape of defect-induced and two-phonon bands
- Ultrafast collinear scattering and carrier multiplication in graphene
- Snapshots of non-equilibrium Dirac carrier distributions in graphene
- Temperature dependent effective third order interatomic force constants from first principles
- Impact of the electron-electron correlation on phonon dispersions: failure of LDA and GGA functionals in graphene and graphite
- Ultrafast reversal of the ferroelectric polarization
- Perturbo: a software package for ab initio electron-phonon interactions, charge transport and ultrafast dynamics
- Ultrafast Relaxation Dynamics of Hot Optical Phonons in Graphene
- Electron-phonon coupling and energy flow in a simple metal beyond the two-temperature approximation
- Impact of Auger processes on carrier dynamics in graphene
- Ultrafast Hot Carrier Dynamics in GaN and its Impact on the Efficiency Droop
- Theory of Thermal Relaxation of Electrons in Semiconductors
- Mapping momentum-dependent electron-phonon coupling and non-equilibrium phonon dynamics with ultrafast electron diffuse scattering
- Direct determination of mode-projected electron-phonon coupling in the time-domain
- First-principles dynamics of electrons and phonons
- Universal Dynamical Steps in the Exact Time-Dependent Exchange-Correlation Potential
- Nonequilibrium Lattice Dynamics in Monolayer MoS2
- Langevin dynamics with spatial correlations as a model for electron-phonon coupling
- Imaging nonequilibrium atomic vibrations with x-ray diffuse scattering
- Dynamics of photoexcited carriers in graphene
- Photocarrier thermalization bottleneck in graphene
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- Ultrafast dynamics of electrons and phonons: from the two-temperature model to the time-dependent Boltzmann equation
- Accessing the anisotropic non-thermal phonon populations in black phosphorus
- 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
- 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
- Evolution of non-thermal phonon and electron populations in photo-excited germanium on picosecond timescales
- 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
- 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
- Overscreening-free electron-phonon interaction in realistic materials
- Nonlinear phononics in BiTe nanoscale thin films: A theoretical approach
- Phonon-assisted carrier cooling in h-BN/graphene van der Waals heterostructures
- Excitonic effects in the photocarriers dynamics of two-dimensional materials
- Properties and challenges of hot-phonon physics in metals: MgB and other compounds