Revealing Ultrafast Phonon Mediated Inter-Valley Scattering through Transient Absorption and High Harmonic Spectroscopies

Abstract

Processes involving ultrafast laser driven electron-phonon dynamics play a fundamental role in the response of quantum systems in a growing number of situations of interest, as evidenced by phenomena such as strongly driven phase transitions and light driven engineering of material properties. To show how these processes can be captured from a computational perspective, we simulate the transient absorption spectra and high harmonic generation signals associated with valley selective excitation and intra-band charge carrier relaxation in monolayer hexagonal boron nitride. We show that the multi-trajectory Ehrenfest dynamics approach, implemented in combination with real-time time-dependent density functional theory and tight-binding models, offers a simple, accurate and efficient method to study ultrafast electron-phonon coupled phenomena in solids under diverse pump-probe regimes which can be easily incorporated into the majority of real-time ab-initio software packages.

16 pages, 9 figures

References in corpus (33)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Valley polarization in MoS2 monolayers by optical pumping
• The Valley Hall Effect in MoS2 Transistors
• A tight-binding approach to uniaxial strain in graphene
• Terahertz-Field-Induced Ferroelectricity in Quantum Paraelectric SrTiO${}_3$
• Metastable ferroelectricity in optically strained $SrTi{O}_3$
• Impact of the electronic band structure in high-harmonic generation spectra of solids
• Continuous Mott transition in semiconductor moiré superlattices
• Ellipticity dependence of high-harmonic generation in solids: unraveling the interplay between intraband and interband dynamics
• Ab initio Electron Mobility and Polar Phonon Scattering in GaAs
• Theoretical Challenges in Polaritonic Chemistry
• Microscopic theory for the light-induced anomalous Hall effect in graphene
• Light-Induced Valleytronics in Pristine Graphene
• Ab initio calculations of ultra-short carrier dynamics in 2D materials: valley depolarization in single-layer WSe${}_2$
• Optical Stabilization of Fluctuating High Temperature Ferromagnetism in YTiO${}_3$
• First-principles dynamics of electrons and phonons
• Phonon driven Floquet matter
• Ultrafast dynamics of electrons and phonons: from the two-temperature model to the time-dependent Boltzmann equation
• Capturing Vacuum Fluctuations and Photon Correlations in Cavity Quantum Electrodynamics with Multi-Trajectory Ehrenfest Dynamics
• Nonequilibrium Lattice Dynamics in Monolayer MoS2
• Accurate nonadiabatic quantum dynamics on the cheap: making the most of mean field theory with master equations
• Attosecond magnetization dynamics in non-magnetic materials driven by intense femtosecond lasers
• Are there universal signatures of topological phases in high harmonic generation? Probably not
• Spin and Valley Control of Free Carriers in Single-Layer WS${}_2$
• Spectral and thermodynamic properties of the Holstein polaron: Hierarchical equations of motion approach
• High order harmonic generation in semiconductors driven at near- and mid-IR wavelengths
• Terahertz-induced high-order harmonic generation and nonlinear charge transport in graphene
• Quantum theory of light-driven coherent lattice dynamics
• Real-time non-adiabatic dynamics in the one-dimensional Holstein model: Trajectory-based vs exact methods
• A Reciprocal-Space Formulation of Mixed Quantum-Classical Dynamics
• A Mean-Field Treatment of Vacuum Fluctuations in Strong Light-Matter Coupling
• Ab initio simulation of laser-induced electronic and vibrational coherence

Cited by in corpus (7)

• Exciton migration in two-dimensional materials
• Attosecond All-Optical Retrieval of Valley Polarization via Circular Dichroism in Transient Absorption
• Mixed quantum-classical modeling of exciton-phonon scattering in solids: Application to optical linewidths of monolayer MoS2
• Creation and control of valley currents in graphene by few cycle light pulses
• Mixed Quantum-Classical Dynamics Yields Anharmonic Rabi Oscillations
• Bulk photogalvanic current control and gap spectroscopy in 2D hexagonal materials
• Ultrafast Saddletronics