A method for time-resolved x-ray diffraction studies has been demonstrated. As a test case, coherent acoustic phonon propagation into crystalline InSb is observed using a laser plasma x-ray source. An extended x-ray topogram of the semiconductor's surface was projected onto a high spatial resolution x-ray detector and acoustic phonons were excited by rapidly heating the crystal's surface with a femtosecond laser pulse. A correlation between the spatial position on the x-ray detector and the time of arrival of the laser pulse was encoded into the experimental geometry by tilting the incident laser pulse with an optical grating. This approach enabled a temporal window of 200 ps to be sampled in a single topogram, thereby negating the disadvantages of pulse-to-pulse fluctuations in the intensity and spectrum of the laser-plasma source. (C) 2002 American Institute of Physics.

We have performed experiments where DKDP has been irradiated by short (100 fs), laser pulses. Subsequently X-ray pulses with a duration of 100 ps were used as a probe. Time-resolved X-ray diffraction enables monitoring of the transitions between the paraelectric and ferroelectric phases. By recording the intensity of a peak only present in the paraelectric phase, we observe indications of a phase-transition following laser-irradiation of DKDP in the ferroelectric phase. We have estimated the laser heating effect, by measuring the strain (peak shifts) in the diffraction patterns. Furthermore, the orientation of the ferroelectric domains has been observed. In spite of the fact that the temperature did not rise above the Curie temperature, following interaction with this radiation, the polarization of ferroelectric domains was modified. This indicates a mechanism where short pulses impulsively excite phonons. which enable either reversal of entire domains, the shift of domain walls and/or the broadening of the domain wall widths. (C) 2003 Elsevier B.V. All rights reserved.

Coherent folded acoustic phonons in a multilayered GaSb/InAs epitaxial heterostructure were generated by femtosecond laser pulses and studied by means of ultrafast x-ray diffraction. Coherent phonons excited simultaneously in the fundamental acoustic branch and the first back-folded branch were detected. This represents the first clear evidence for phonon branch folding based directly on the atomic motion to which x-ray diffraction is sensitive. From a comparison of the measured phonon-modulated x-ray reflectivity with simulations, evidence was found for a reduction of the laser penetration depth. This reduction can be explained by the self-modulation of the refractive index due to photogenerated free carriers.

The motion of atoms on interatomic potential energy surfaces is fundamental to the dynamics of liquids and solids. An accelerator-based source of femtosecond x-ray pulses allowed us to follow directly atomic displacements on an optically modified energy landscape, leading eventually to the transition from crystalline solid to disordered liquid. We show that, to first order in time, the dynamics are inertial, and we place constraints on the shape and curvature of the transition-state potential energy surface. Our measurements point toward analogies between this nonequilibrium phase transition and the short-time dynamics intrinsic to equilibrium liquids.

We have used time-resolved X-ray diffraction to monitor the resolidification process of molten InSb. Melting was induced by an ultra-short laser pulse and the measurement conducted in a high-repetition-rate multishot experiment. The method gives direct information about the nature of the transient regrowth and permanently damaged layers. It does not rely on models based on surface reflectivity or second harmonic generation (SHG). The measured resolidification process has been modeled with a 1-D thermodynamic heat-conduction model. Important parameters like sample temperature, melting depth and amorphous surface layer thickness come directly out of the data, while mosaicity of the sample and free carrier density can be quantified by comparing with models. Melt depths up to 80 nm have been observed and regrowth velocities in the range 2-8 m/s have been measured.

The melting dynamics of laser excited InSb have been studied with femtosecond x-ray diffraction. These measurements observe the delayed onset of diffusive atomic motion, signaling the appearance of liquidlike dynamics. They also demonstrate that the root-mean-squared displacement in the [111] direction increases faster than in the [110] direction after the first 500 fs. This structural anisotropy indicates that the initially generated fluid differs significantly from the equilibrium liquid.

A semiconductor (InSb) showed transient metal- like heat conduction after excitation of a dense electron- hole plasma via short and intense light pulses. A related ultrafast strain relaxation was detected using picosecond time-resolved x-ray diffraction. The deduced heat conduction was, by a factor of 30, larger than the lattice contribution. The anomalously high heat conduction can be explained once the contribution from the degenerate photocarrier plasma is taken into account. The magnitude of the effect could provide the means for guiding heat in semiconductor nanostructures. In the course of this work, a quantitative model for the carrier dynamics in laser-irradiated semiconductors has been developed, which does not rely on any adjustable parameters or ad hoc assumptions. The model includes various light absorption processes (interband, free carrier, two photon, and dynamical Burstein- Moss shifts), ambipolar diffusion, energy transport (heat and chemical potential), electrothermal effects, Auger recombination, collisional excitation, and scattering (elastic and inelastic). The model accounts for arbitrary degrees of degeneracy.