Time-Resolved Phonons as a Microscopic Probe for Solid State Processes

Abstract

Phonons reflect most directly the chemical interactions in solids. Hence, time-resolved, lattice-dynamical experiments yield detailed information about the trajectories and mechanisms of solid state reactions on a microscopic scale. The experimental determination of phonons in a wide range of wave vectors and frequencies is a domain of inelastic neutron scattering and requires usually rather long counting times. Real-time investigations therefore need sophisticated techniques in order to access the time regime down to microseconds. In the present contribution, the state of the art of time-resolved inelastic neutrons scattering (TRINS) is reviewed and its capability for the exploration of microscopic mechanisms of chemical processes and phase transitions in solids is demonstrated using two different examples. Demixing processes in model systems are used to show that the evolution of lattice dynamics allows one to distinguish clearly between the mechanisms of nucleation and growth on the one hand, and spinodal decomposition, on the other hand. In the latter case, the interatomic interactions and, hence, the phonon spectra, vary on a time scale of seconds while the average structure of the product phases as reflected by Bragg diffraction needs much longer times to evolve.