Electric field dependent structural and vibrational properties of the Si(100)-H(2 \times 1) surface and its implications for STM induced hydrogen desorption

TL;DR

This study uses first principles calculations to analyze how electric fields influence the structural and vibrational properties of the Si(100)-H(2x1) surface, shedding light on STM-induced hydrogen desorption mechanisms.

Contribution

It introduces a first principles model of vibrational modes under electric fields and explores their role in hydrogen desorption via inelastic electron scattering.

Findings

Local one-phonon excitations have short lifetimes (~10 ps) at room temperature.

Multi-phonon excitations have longer lifetimes (~10 ns) due to anharmonic effects.

Inelastic scattering with energy transfer n>1 significantly contributes to hydrogen desorption.

Abstract

We report a first principles study of the structure and the vibrational properties of the Si(100)-H(2 \times 1) surface in an electric field. The calculated vibrational parameters are used to model the vibrational modes in the presence of the electric field corresponding to a realistic STM tip-surface geometry. We find that local one-phonon excitations have short lifetimes (10 ps at room temperature) due to incoherent lateral diffusion, while diffusion of local multi-phonon excitations are suppressed due to anharmonic frequency shifts and have much longer lifetimes (10 ns at room temperature). We calculate the implications for current induced desorption of H using a recently developed first principles model of electron inelastic scattering. The calculations show that inelastic scattering events with energy transfer $n \hbar \omega$, where n>1, play an important role in the desorption process.