Dynamics of ultrafast phase transitions in MgF triggered by laser-induced THz coherent phonons.

The advent of free-electron lasers opens new routes for experimental high-pressure physics, which allows studying dynamics of condensed matter with femtosecond resolution. A rapid compression, that can be caused by laser-induced shock impact, leads to the cascade of high-pressure phase transitions. Despite many decades of study, a complete understanding of the lattice response to such a compression remains elusive. Moreover, in the dynamical case (in contrast to quasi-static loading) the thresholds of phase transitions can change significantly. Using the third harmonic pump-probe technique combined with molecular dynamics to simulate the terahertz (THz) spectrum, we revealed the dynamics of ultrafast laser-induced phase transitions in MgF in all-optical experiment. Tight focusing of femtosecond laser pulse into the transparent medium leads to the generation of sub-TPa shock waves and THz coherent phonons. The laser-induced shock wave propagation drastically displaces atoms in the lattice, which leads to phase transitions. We registered a cascade of ultrafast laser-induced phase transitions (P42/mnm ⇒ Pa-3  ⇒ Pnam) in magnesium fluoride as a change in the spectrum of coherent phonons. The phase transition has the characteristic time of 5-10 ps, and the lifetime of each phase is on the order of 40-60 ps. In addition, phonon density of states, simulated by molecular dynamics, together with third-harmonic time-resolved spectra prove that laser-excited phonons in a bulk of dielectrics are generated by displacive excitation (DECP) mechanism in plasma mediated conditions.