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.

arXiv comment16 pages, 9 figures

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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