Understanding long-lived metastable phases in ultrafast optical experiments

A puzzling and so far unexplained aspect of some so-called nonlinear phononics experiments is that the observed lifetimes of the optically created metastable phases are sometimes orders of magnitude longer than expected based on the nonlinear phononics mechanism assumed in most works.

We use a combination of phenomenological theory and first-principles calculations to demonstrate that strong coupling between different lattice degrees of freedom (strains and Raman-active phonons) can give rise to a long-lived metastable phase recently observed in experiments on perovskite LaAlO3 [Hortensius et al. npj Quantum Mater. 5 95 (2020)]. We show that the long-timescale oscillatory response in the experimental optical reflectivity data is not due solely to shear strains, as originally suggested, but arises from a “hybrid” mode involving displacements of Raman-active phonons of the same symmetry.