Hot Phonon and Carrier Relaxation in Si(100) Determined by Transient Extreme Ultraviolet Spectroscopy

TL;DR

This study uses transient extreme-ultraviolet spectroscopy to directly measure hot carrier and phonon thermalization in silicon, revealing detailed scattering processes and structural dynamics from femtoseconds to hundreds of picoseconds.

Contribution

It introduces a novel spectroscopic approach combining theoretical modeling and experimental data to separately quantify electronic and structural contributions to carrier and phonon relaxation in silicon.

Findings

Quantified carrier and phonon populations over time.

Identified electron-phonon and phonon-phonon scattering dynamics.

Linked structural deformations to phonon kinetics.

Abstract

The thermalization of hot carriers and phonons gives direct insight into the scattering processes that mediate electrical and thermal transport. Obtaining the scattering rates for both hot carriers and phonons currently requires multiple measurements with incommensurate timescales. Here, transient extreme-ultraviolet (XUV) spectroscopy on the silicon 2p core level at 100 eV is used to measure hot carrier and phonon thermalization in Si(100) from tens of femtoseconds to 200 ps following photoexcitation of the indirect transition to the {\Delta} valley at 800 nm. The ground state XUV spectrum is first theoretically predicted using a combination of a single plasmon pole model and the Bethe-Salpeter equation (BSE) with density functional theory (DFT). The excited state spectrum is predicted by incorporating the electronic effects of photo-induced state-filling, broadening, and band-gap renormalization into the ground state XUV spectrum. A time-dependent lattice deformation and expansion is also required to describe the excited state spectrum. The kinetics of these structural components match the kinetics of phonons excited from the electron-phonon and phonon-phonon scattering processes following photoexcitation. Separating the contributions of electronic and structural effects on the transient XUV spectra allows the carrier population, the population of phonons involved in inter- and intra-valley electron-phonon scattering, and the population of phonons involved in phonon-phonon scattering to be quantified as a function of delay time.