Ultrafast electron diffraction from a Bi(111) surface: Impulsive lattice excitation and Debye–Waller analysis at large momentum transfer

Abstract

The lattice response of a Bi(111) surface upon impulsive femtosecond laser excitation is studied with time-resolved reflection high-energy electron diffraction. We employ a Debye-Waller analysis at large momentum transfer of 9.3 Å^-1 ≤ Δ <i>k</i> ≤ 21.8 Å^-1 in order to study the lattice excitation dynamics of the Bi surface under conditions of weak optical excitation up to 2 mJ/cm² incident pump fluence. The observed time constants <i>τ</i> _int of decay of diffraction spot intensity depend on the momentum transfer Δ<i>k</i> and range from 5 to 12 ps. This large variation of <i>τ</i> _int is caused by the nonlinearity of the exponential function in the Debye-Waller factor and has to be taken into account for an intensity drop Δ<i>I</i> > 0.2. An analysis of more than 20 diffraction spots with a large variation in Δ<i>k</i> gave a consistent value for the time constant <i>τ_T</i> of vibrational excitation of the surface lattice of 12 ± 1 ps independent on the excitation density. We found no evidence for a deviation from an isotropic Debye-Waller effect and conclude that the primary laser excitation leads to thermal lattice excitation, i.e., heating of the Bi surface.