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

TL;DR

This paper demonstrates how ultrafast electron-phonon interactions in monolayer hexagonal boron nitride can be effectively studied using a combination of computational methods, revealing insights into valley dynamics and charge relaxation.

Contribution

It introduces a multi-trajectory Ehrenfest dynamics approach integrated with real-time TDDFT and tight-binding models for simulating ultrafast electron-phonon phenomena in solids.

Findings

Validated the method with transient absorption spectra

Analyzed high harmonic generation signals

Captured valley selective excitation and intra-band relaxation

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.