A. Hanisch-Blicharski

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.

Epitaxial growth of the topological insulator Bi2Se3 on Si(111): Growth mode, lattice parameter, and strain state

Using spot profile analysis low energy electron diffraction, we studied the growth mode and strain state of ultra-thin epitaxial Bi2Se3(111) films grown by molecular beam epitaxy on Si(111). The first layer grows as complete quintuple layer and covers the Si substrate before the next layer nucleates. Its lateral lattice parameter is increased by 1% compared with the value of a‖ = 4.136 A for a 6-nm-thick film. With increasing film thickness, a continuous change of the lattice parameter is observed to an asymptotic value, which is explained by a van der Waals-like bonding between the Bi2Se3 film and the Si substrate.

Comparing ultrafast surface and bulk heating using time-resolved electron diffraction

From measurements of the transient Debye-Waller effect in Bismuth, we determine the buildup time of the random atomic motion resulting from the electronic relaxation after short pulse laser excitation. The surface sensitive reflection high energy electron diffraction and transmission electron diffraction yield a time constant of about 12 ps and 3 ps, respectively. The different energy transfer rates indicate relatively weak coupling between bulk and surface vibrational modes.

Ultra-fast Time-Resolved Electron Diffraction of Strongly Driven Phase Transitions on Silicon Surfaces

The dynamics of strongly driven phase transitions at surfaces are studied by ultra-fast time-resolved reflection high energy electron diffraction. The surfaces are excited by an intense fs-laser pulse (pump) and probed by an ultra-short electron pulse with variable time delay. The order-disorder phase transition from a c(4×2) to a (2×1) of the bare Si(001) surface shows a transient decrease of the intensity of the c(4×2) spots which recovers on a time scale of a few hundred picoseconds indicating the excitation of the phase transition. On Si(111) a monolayer of Indium induces a (4×1) reconstruction which undergoes a Peierls like phase transition to a (8ד2”) reconstruction below 100 K. Upon laser excitation at a temperature of 40 K the phase transition was strongly driven. The (8ד2”)-diffraction spots instantaneously disappears, while the intensity of the (4×1)-spots increases. This increase of the (4×1) spot intensity excludes an explanation by the Debye-Waller-Effect and is evidence for a true structural phase transition at a surface.