Intraband and Interband Competition Drives Ultrafast Modulations of Indium Tin Oxide

Abstract

Transparent conducting oxides near their epsilon-near-zero frequency exhibit near-unity ultrafast modulations of the refractive index which have enabled the field of time-varying metamaterials, yet the underlying carrier dynamics at high driving fluences remain poorly understood. Here, we report ultrafast modulations in the reflectivity and transmissivity of indium tin oxide, and a non-monotonic oscillatory behavior. This is especially evident in the time evolution of the complex Fresnel coefficients retrieved directly from pump-probe spectrograms using a optical gating technique, GRUMPY FROG. The dynamics of the retrieved plasma frequency and damping coefficient are well captured by an extended two-temperature model incorporating a competing nonlinear interband process: at high fluences, Auger-type scattering of hot conduction electrons promotes valence band carriers, increasing the plasma frequency while accelerating hot-electron cooling and raising the damping coefficient. These results clarify the origin of anomalous high-fluence dynamics in indium tin oxide and identify a fluence-tuneable modulation dynamic with direct implications for ultrafast refractive index engineering in time-varying photonic devices and optical switching