Third-harmonic generation in excitonic insulators

TL;DR

This paper investigates third-harmonic generation in excitonic insulators, revealing how collective excitations influence nonlinear optical responses and proposing THG as a probe for excitonic order.

Contribution

It derives the THG susceptibility considering collective excitations in an excitonic insulator, highlighting the role of order parameter dynamics in nonlinear optical responses.

Findings

Three resonant peaks in THG susceptibility at specific energies related to the band gap.

Collective excitations significantly influence THG in the BCS regime.

Temperature dependence of THG intensity can reveal excitonic collective modes.

Abstract

We study third-harmonic generation (THG) in an excitonic insulator (EI) described in a two-band correlated electron model. Employing the perturbative expansion with respect to the external electric field, we derive the THG susceptibility taking into account the collective dynamics of the excitonic order parameter. In the inversion-symmetric EI, the collective order parameter motion is activated at second order of the external field and its effects arise in THG. We find three peaks in the THG susceptibility at energies $\hbar \Omega = \Delta_g/3$, $\Delta_g/2$, and $\Delta_g$, where $\Delta_g$ is the band gap. While the THG response at $\Delta_g/3$ is caused by bare three-photon excitation of the independent particle across the band gap, the latter two peaks involve the motion of the order parameter activated at second order. The resulting resonant peaks are prominent in particular in the BCS regime but they become less significant in the BEC regime. We demonstrate that the resonant peak originated by the collective excitation is observable in the temperature profile of the THG intensity. Our study suggests that the THG measurement should be promising for detecting the excitonic collective nature of materials.