Abstract

In this paper, the optical response to a terahertz pulse was investigated in the transition metal chalcogenide Ta2NiSe5, a candidate excitonic insulator. First, by irradiating a terahertz pulse with a relatively weak electric field (0.3 MV/cm), the spectral changes in reflectivity near the absorption edge due to third-order optical nonlinearity were measured, and the absorption peak characteristic of the excitonic phase just below the interband transition was identified. Next, by irradiating a strong terahertz pulse with a strong electric field of 1.65 MV/cm, the absorption of the excitonic phase was found to be reduced, and a Drude-like response appeared in the mid-infrared region. These responses can be interpreted as carrier generation by exciton dissociation induced by the electric field, resulting in the partial melting of the excitonic phase and metallization. The presence of a distinct threshold electric field for carrier generation indicates exciton dissociation via quantum-tunneling processes. The spectral change due to metallization by the electric field is significantly different from that due to the strong optical excitation across the gap, which can be explained by the different melting mechanisms of the excitonic phase in the two types of excitations. Published by the American Physical Society 2024