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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  k  ≤ 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/cm 2  incident pump fluence. The observed time constants  τ  int  of decay of diffraction spot intensity depend on the momentum transfer Δ k  and range from 5 to 12 ps. This large variation of  τ  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  > 0.2. An analysis of more than 20 diffraction spots with a large variation in Δ k  gave a consistent value for the time constant  τ T   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.

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