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Many fundamental processes in nature, such as chemical reactions and phase transitions involve rearrangement of the constituent atoms. Such changes cannot be directly measured with visible light and occur transiently on time-scales comparable with the natural oscillation periods of atoms (femtoseconds to picoseconds). We present experiments on Ge-111 films irradiated with 100-fs 800-nm light pulses and probed by a time-delayed sub-ps x-ray pulse at 8 keV. After excitation of a dense electron-hole plasma within the 160-nm film, the ultrafast pathway of lattice disordering is measured as a function laser fluence. For close-to-threshold irradiation, inhomogeneous thermal melting, occurring via surface nucleation of the liquid phase and growth into the bulk determines the dynamics of the solid-to-liquid phase transition. For excitation at about twice the melting threshold, a nonthermal pathway, starting from a highly excited cold solid and relaxing into a hot liquid causes ultrafast melting. At long time delays, nearly perfect recrystallization of a (111) crystal is observed.
Many fundamental processes in solids, such as heat transport and phase transitions involve atomic movement on ultrafast time-scales, but cannot be directly measured with visible light. Using ultrafast x-ray diffraction, atomic motion can be measured on its natural time-scale. Photo-excitation of bulk and layered semiconductors was achieved with 800-nm wavelength femtosecond laser pulses. Optical excitation triggers a chain of relaxation processes, causing rapid lattice heating, generation and propagation of stress/strain waves into the bulk and eventual anharmonic decay of coherent acoustic phonons into the thermal bath of the solid. While the first steps of carrier relaxation, excitation and decay of Raman-active optical phonons have been in the past characterized optically at surfaces, the bulk acoustic dynamics at longer times has not. We measure length scales of lattice excitation, thereby detecting ultrafast heat diffusion via fast electrons, coherent acoustic pulse propagation into the bulk or across buried interfaces and anharmonic damping of non-equilibrium acoustic phonons. The measurement is performed with sensitivity on lattice spacing of 10 femtometers (i.e., 3 nuclear diameters).