Ultrafast Insulator-Metal Phase Transition in VO2 Studied by Multiterahertz Spectroscopy

Abstract: The ultrafast photoinduced insulator-metal transition in VO2 is studied at different temperatures and excitation fluences using multi-THz probe pulses. The spectrally resolved mid-infrared response allows us to trace separately the dynamics of lattice and electronic degrees of freedom with a time resolution of 40 fs. The critical fluence of the optical pump pulse which drives the system into a long-lived metallic state is found to increase with decreasing temperature. Under all measurement conditions we observe a modulation of the eigenfrequencies of the optical phonon modes induced by their anharmonic coupling to the coherent wave packet motion of V-V dimers at 6.1 THz. Furthermore, we find a weak quadratic coupling of the electronic response to the coherent dimer oscillation resulting in a modulation of the electronic conductivity at twice the frequency of the wave packet motion. The findings are discussed in the framework of a qualitative model based on an approximation of local photoexcitation of the vanadium dimers from the insulating state.