Decelerated lattice excitation and absence of bulk phonon modes at surfaces: Ultra-fast electron diffraction from Bi(111) surface upon fs-laser excitation.

Ultrafast reflection high-energy electron diffraction is employed to follow the lattice excitation of a Bi(111) surface upon irradiation with a femtosecond laser pulse. The thermal motion of the atoms is analyzed through the Debye-Waller effect. While the Bi bulk is heated on time scales of 2 to 4 ps, we observe that the excitation of vibrational motion of the surface atoms occurs much slower with a time constant of 12 ps. This transient nonequilibrium situation is attributed to the weak coupling between bulk and surface phonon modes which hampers the energy flow between the two subsystems. From the absence of a fast component in the transient diffraction intensity, it is in addition concluded that truncated bulk phonon modes are absent at the surface.

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

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/cm2 incident pump fluence. The observed time constants τ int of decay of diffraction spot intensity depend on the momentum transfer Δk 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 ΔI > 0.2. An analysis of more than 20 diffraction spots with a large variation in Δk gave a consistent value for the time constant τT 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.

Ultra-fast electron diffraction at surfaces: from nanoscale heat transport to driven phase transitions.

Many fundamental processes of structural changes at surfaces occur on a pico- or femtosecond time scale. In order to study such ultra-fast processes, we have combined modern surface science techniques with fs-laser pulses in a pump-probe scheme. Reflection high energy electron diffraction (RHEED) with grazing incident electrons ensures surface sensitivity for the probing electron pulses. Utilizing the Debye-Waller effect, we studied the cooling of vibrational excitations in monolayer adsorbate systems or the nanoscale heat transport from an ultra-thin film through a hetero-interface on the lower ps-time scale. The relaxation dynamics of a driven phase transition far away from thermal equilibrium is demonstrated with the In-induced (8×2) reconstruction on Si(111). This surface exhibits a Peierls-like phase transition at 100K from a (8×2) ground state to (4×1) excited state. Upon excitation by a fs-laser pulse, this structural phase transition is driven into an excited (4×1) state at a sample temperature of 20K. Relaxation into the (8×2) ground state occurs after more than 150 ps.