Light-Induced Nonthermal Phase Transition to the Topological Crystalline Insulator State in SnSe

Femtosecond pulses have been used to reveal hidden broken symmetry states and induce transitions to metastable states. However, these states are mostly transient and disappear after laser removal. Photoinduced phase transitions toward crystalline metastable states with a change of topological order are rare and difficult to predict and realize experimentally. Here, by using constrained density functional perturbation theory and accounting for light-induced quantum anharmonicity, we show that ultrafast lasers can permanently transform the topologically trivial orthorhombic structure of SnSe into the topological crystalline insulating rocksalt phase via a first-order nonthermal phase transition. We describe the reaction path and evaluate the critical fluence and possible decay channels after photoexcitation. Our simulations of the photoexcited structural and vibrational properties are in excellent agreement with recent pump–probe data in the intermediate fluence regime below the transition with an error on the curvature of the quantum free energy of the photoexcited state that is smaller than 2%.