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Femtosecond pulses have been used to reveal hidden broken symmetry states andinduce transitions to metastable states. However, these states are mostlytransient and disappear after laser removal. Photoinduced phase transitionstowards crystalline metastable states with a change of topological order arerare and difficult to predict and realize experimentally. Here, by usingconstrained density functional perturbation theory and accounting forlight-induced quantum anharmonicity, we show that ultra-fast lasers canpermanently transform the topologically-trivial orthorhombic structure of SnSeinto the topological crystalline insulating rocksalt phase via a first-ordernon-thermal phase transition. We describe the reaction path and evaluate thecritical fluence and the possible decay channels after photoexcitation. Oursimulations of the photoexcited structural and vibrational properties are inexcellent agreement with recent pump-probe data in the intermediate fluenceregime below the transition with an error on the curvature of the quantum freeenergy of the photoexcited state that is smaller than 2%.

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