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We used ultrafast electron diffraction and density-functional theory calculations to gain insight into the charge density wave (CDW) formation on In/Si(111). Weak excitation by a femtosecond-laser pulse results in the melting of the CDW. The immediate freezing is hindered by a barrier for the motion of atoms during the phase transition: The melted CDW constitutes a long-lived, supercooled phase and is strong evidence for a first-order transition. The freezing into the CDW is triggered by preexisting adsorbates. Starting at these condensation nuclei, the CDW expands one dimensionally on the In/Si(111) surface, with a constant velocity of more than 80 m/s.
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 (8 × "2") reconstruction below 100 K. Upon laser excitation with a fluence of 3.4 mJ/cm 2 at a temperature of 72 K the phase transition was strongly driven. The (8 × "2")-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. © 2010 Materials Research Society.
With time resolved ultrafast electron diffraction the cooling process across the interface between a thin film and the underlying substrate was studied after excitation with short laser pulses. From the exponential decay of the surface temperature evolution a thermal boundary conductance of 1430 W/(cm2K) is determined for a 9.7 nm thin Bi(111) film on Si(111). A linear dependence between laser fluence and initial temperature rise was measured for film-thicknesses between 2.5 nm and 34.5 nm. The ratio of initial temperature rise and laser fluence for different film-thicknesses is compared to a model taking multilayer optics into account. The data agree well with this model.