Electron-electron interactions can render an otherwise conducting material insulating, with the insulator-metal phase transition in correlated-electron materials being the canonical macroscopic manifestation of the competition between charge-carrier itinerancy and localization. The transition can arise from underlying microscopic interactions among the charge, lattice, orbital and spin degrees of freedom, the complexity of which leads to multiple phase-transition pathways. For example, in many transition metal oxides, the insulator-metal transition has been achieved with external stimuli, including temperature, light, electric field, mechanical strain or magnetic field. Vanadium dioxide is particularly intriguing because both the lattice and on-site Coulomb repulsion contribute to the insulator-to-metal transition at 340 K (ref. 8). Thus, although the precise microscopic origin of the phase transition remains elusive, vanadium dioxide serves as a testbed for correlated-electron phase-transition dynamics. Here we report the observation of an insulator-metal transition in vanadium dioxide induced by a terahertz electric field. This is achieved using metamaterial-enhanced picosecond, high-field terahertz pulses to reduce the Coulomb-induced potential barrier for carrier transport. A nonlinear metamaterial response is observed through the phase transition, demonstrating that high-field terahertz pulses provide alternative pathways to induce collective electronic and structural rearrangements. The metamaterial resonators play a dual role, providing sub-wavelength field enhancement that locally drives the nonlinear response, and global sensitivity to the local changes, thereby enabling macroscopic observation of the dynamics. This methodology provides a powerful platform to investigate low-energy dynamics in condensed matter and, further, demonstrates that integration of metamaterials with complex matter is a viable pathway to realize functional nonlinear electromagnetic composites.

The metal-insulator transition temperature Tc in VO2 is experimentally shown to be almost the same as a magnetic transition temperature Tm characterized by an abrupt decrease in susceptibility, suggesting the evidence of the same underlying origin for both transitions. The measurement of susceptibility shows that it weakly increases on cooling for temperature range of T > Tm, sharply decreases near Tm and then unusually increases on further cooling. A theoretical approach for such unusual observations in susceptibility near Tm or below is performed by modeling electrons from each two adjacent V4+ ions distributed along V-chains as a two-electron system, which indicates that the spin exchange between electrons could cause a level splitting into a singlet (S = 0) level of lower energy and a triplet (S = 1) level of higher energy. The observed abrupt decrease in susceptibility near Tm is explained to be due to that the sample enters the singlet state in which two electrons from adjacent V4+ ions are paired into dimers in spin antiparallel. By considering paramagnetic contribution of unpaired electrons created by the thermal activation from singlet to triplet levels, an expression for susceptibility is proposed to quantitatively explain the unusual temperature-dependent susceptibility observed at low temperatures. Based on the approach to magnetic features, the observed metal-insulator transition is explained to be due to a transition from high-temperature Pauli paramagnetic metallic state of V4+ions to low-temperature dimerized state of strong electronic localization.