Time-resolved diffraction profiles and atomic dynamics in short-pulse laser-induced structural transformations: Molecular dynamics study

Abstract

The diffraction profiles and density correlation functions are calculated for transient atomic configurations generated in molecular dynamics simulations of a $20\phantom{\rule{0.3em}{0ex}}\mathrm{nm}$ Au film irradiated with $200\phantom{\rule{0.3em}{0ex}}\mathrm{fs}$ laser pulses of different intensity. The results of the calculations provide an opportunity to directly relate the detailed information on the atomic-level structural rearrangements available from the simulations to the diffraction spectra measured in time-resolved x-ray and electron diffraction experiments. Three processes are found to be responsible for the evolution of the diffraction profiles. During the first several picoseconds after the laser excitation, the decrease of the intensity of the diffraction peaks is largely due to the increasing amplitude of thermal atomic vibrations and can be well described by the Debye-Waller factor. The effect of thermoelastic deformation of the film prior to melting is reflected in shifts and splittings of the diffraction peaks, providing an opportunity for experimental probing of the ultrafast deformations. Finally, the onset of the melting process results in complete disappearance of the crystalline diffraction peaks. The homogeneous nucleation of a large number of liquid regions throughout the film is found to be more effective in reducing long-range correlations in atomic positions and diminishing the diffraction peaks as compared to the heterogeneous melting by melting front propagation. For the same fraction of atoms retaining the local crystalline environment, the diffraction peaks are more pronounced in heterogeneous melting. A detailed analysis of the real space correlations in atomic positions is also performed and the atomic-level picture behind the experimentally observed fast disappearance of the correlation peak corresponding to the second nearest neighbors in the fcc lattice during the laser heating and melting processes is revealed.