VO2 Does Not Host a Photoinduced Long-lived Monoclinic Metallic Phase

Femtosecond laser pulses can trigger phase transitions and sometimes even achieve transient nonequilibrium states that are not accessible in equilibrium. Vanadium dioxide (VO2) exhibits a first-order insulator-to-metal transition accompanied by a monoclinic-to-rutile structural transition near room temperature. Recently there is extensive debate over whether VO2 hosts a transient long-lived monoclinic metallic phase with femtosecond photoexcitation. We developed a new method to synthesize quasi-single-crystal freestanding VO2 films and reexamined the photoinduced phase transition with mega-electron-volt ultrafast electron diffraction. Benefitting from the well separated diffraction spots and high temporal resolution, we found no evidence for the transient monoclinic metallic phase through the accurate measurements of the photoinduced evolution of the diffraction intensity in the momentum space. Based on the laser fluence thresholds measured at various temperatures, we suggest that the phase transition threshold is thermally driven although the transition occurs within 200 femtoseconds, highlighting the interplay of the electron-electron correlation and the lattice vibrations in driving the phase transition in VO2.