Nonlinearity Reversal in Epsilon-Near-Zero Indium Tin Oxide Driven by Few-Cycle Light Pulse

Abstract

Recent breakthrough studies of nonlinearities at extreme pump intensities ($\sim$1 $\text{TW/cm}^2$) in transparent conducting oxides (TCOs) have rewritten our understanding of the dynamics in these materials. However, exploring TCO dynamics beyond these intensities is prohibited by the damage threshold of the material. In this work, we overcome this problem by using a few-cycle pump laser pulse (sub-8\,fs) to maximize the intensity while keeping the optical fluence below the damage threshold. We observe a reversal in the optical response trend starting at optical pump laser intensities of $\sim$5 $\text{TW/cm}^2$ similar to Segal et al. At the highest pump pulse intensities, we obtain a complete change in the sign of the modulation for both transmission and reflection, producing a full-cycle oscillation of the refractive index modulation within 300\,fs. The amplitude of the sign reversal scales quadratically with the intensity. We therefore propose a simple two-photon absorption (TPA) model to explain the observed behaviour. The TPA, which is normally forbidden by the Pauli blocking, is enabled here by intraband excitations from the lower to the upper non-equilibrium states of the conduction band (CB). Such excitations vacate the states at the bottom of the CB, lifting up the blocking and thus making interband TPA possible. The model is in good agreement with experimental results, capturing the essential trends in the observed data and revealing the dynamics of competing channels caused by the interplay between interband and intraband transitions. This intensity-controlled mechanism could be the key to unlocking new applications of TCOs for time-varying photonics such as photonic time crystals.