Lattice dynamics in VO2 near the metal-insulator transition

We present a comprehensive experimental study of the lattice dynamics in the vicinity of the metal-insulator transition in VO2 by means of combined use of Raman spectroscopy and ultrasonic microscopy. Single crystalline samples of high quality particularly allow quite a complete determination of all Raman modes in the insulating phase at the Γ-point and the observation of an optical soft mode. In addition, the elastic behavior has been successfully investigated by measuring the propagation velocity of ultrasonic surface waves microscopically excited in various crystal directions. Our study reveals a striking coincidence of strong lattice softening attributable to certain acoustic branches and the occurrence of the optical soft mode, which precedes the metal-insulator transition over more than 100 K on approaching the critical temperature.