An electronic-based model of the optical nonlinearity of low-electron-density-Drude materials

Abstract: Low electron density Drude (LEDD) materials such as indium tin oxide (ITO) are receiving considerable attention because of their combination of CMOS compatibility, unique epsilon-near-zero (ENZ) behavior, and giant ultrafast nonlinear thermo-optic response. However, the understanding of the electronic and optical response of LEDD materials is so far based on simplistic extensions of known models of noble metals, frequently without the inclusion of the interplay among the lower electron density, relatively high Debye energy, and the non-parabolic band structure. To bridge this knowledge gap, this work provides a complete understanding of the nonlinear electronic-thermal-optical response of LEDD materials. In particular, we rely on state-of-the-art electron dynamics modeling, as well as the newly derived time-dependent permittivity model for LEDD materials under optical pumping within the adiabatic approximation. We find that unlike noble metals, the electron temperatures can reach the Fermi temperature, in which case the effective chemical potential dramatically decreases and even becomes negative, thus, transiently converting the Drude metal into a semiconductor. We further show that the nonlinear optical response of LEDD materials originating from the changes to the real part of the permittivity is due to the generation of non-thermal electrons. This resolves the argument about the rise time of the permittivity and shows that it is instantaneous. In this vein, we show that referring to the LEDD permittivity as having a ``saturable'' nonlinearity is unsuitable since its permittivity dynamics does not originate from population inversion. Finally, we analyze the probe pulse dynamics and unlike previous work, we obtain a quantitative agreement with the results of recent experiments.