Femtosecond time-resolved small and wide-angle x-ray diffuse scattering techniques are applied to investigate the
ultrafast nucleation processes that occur during the ablation process in semiconducting materials. Following intense
optical excitation, a transient liquid state of high compressibility characterized by large-amplitude density fluctuations is
observed and the build-up of these fluctuations is measured in real-time. Small-angle scattering measurements reveal
the first steps in the nucleation of nanoscale voids below the surface of the semiconductor and support MD simulations
of the ablation process.
The melting dynamics of laser excited InSb have been studied with femtosecond x-ray diffraction. These measurements demonstrate that the initial stage of crystal disordering results from inertial motion on a laser softened potential energy surface. These inertial dynamics dominate for the first half picosecond following laser excitation, indicating that inter-atomic forces minimally influence atomic excursions from the equilibrium lattice positions, even for motions in excess of an Å. This also indicates that the atoms disorder initially without losing memory of their lattice reference.
Although the realisation of femtosecond X-ray free electron laser (FEL) X-ray pulses is still some time away, X-ray diffraction experiments within the sub-picosecond domain are already being performed using both synchrotron and laser- plasma based X-ray sources. Within this paper we summarise the current status of some of these experiments which, to date, have mainly concentrated on observing non-thermal melt and coherent phonons in laser-irradiated semiconductors. Furthermore, with the advent of FEL sources, X-ray pulse lengths may soon be sufficiently short that the finite response time of monochromators may themselves place fundamental limits on achievable temporal resolution. A brief review of time-dependent X-ray diffraction relevant to such effects is presented.
Time-dependent x-ray diffraction has been measured from laser-irradiated semiconductor crystals. Laser pulses with 100 fs duration and 800 nm wavelength excite the sample inducing phase transitions. 5 keV x-rays from the Advanced Light Source are diffracted by a sagittally-focusing Si (111) crystal and then by the sample crystal, InSb (111), onto an avalanche photodiode. By detecting individual pulses of synchrotron radiation, which have a duration of 70 ps, the diffracted intensity is observed to decrease because of photoabsorption in a disordered surfaced layer. Rocking curves measured after the laser irradiation show a tail, which results from a strained region caused by expansion of the crystal lattice.