Ultrafast reversible phase engineering in MoTe2 thin film via polaron formation

The emergence of various polymorphs in two-dimensional transition metal dichalcogenides provides an opportunity for robust phase engineering by temperature, strain, laser irradiation, and external charge doping (Keum in Nat. Phys. 11:482, 2015; Song in Nano Lett. 16:188, 2016; Cho in Science 349:625, 2015; Kim in Nano Lett. 17:3363, 2017). This provides means to develop homojunction of metal–semiconductor, enhance mobility, reduce contact resistance, and observe novel quantum critical phenomena in mesoscopic systems. The rich physics paves the way for ultrafast light-induced switching/memory devices and optical data processing in optoelectronics. However, the fundamental temporal evolution of the laser-driven phase transformation, in particular regarding heat and charge carriers, remains elusive. We report an ultrafast reversible structural transformation in MoTe₂ by coherent phonon dynamics through polaron formation at room temperature. At a high photon density, the generated coherent phonons are coupled with excitons to form polarons. The strong exciton–phonon coupling disturbs and dephases the coherent phonons of the semiconducting 2H phase in MoTe₂, and generates lattice distortions to further stabilize new coherent phonons of the metallic 1T’-phase, manifested by the emergence of the corresponding phonons in each phase. This structural transformation is fully reversible within a few picoseconds by switching on/off the laser. The nonlinear response of the phonon intensity to the excited carrier density in the intermediate region indicates a gradual structural transformation through coexisting 2H and 1T’ phases.