First-Principles Prediction of Nonlinear Optical Response in TiO${}_2$ for High-Power Dielectric Mirror Applications

Abstract

Dielectric multilayer mirrors are essential components in optical experiments using high-power lasers, where titanium dioxide (TiO${}_2$) is widely employed as a high-refractive-index dielectric material. In this study, we investigate the nonlinear optical response of TiO${}_2$ under intense ultrashort laser pulses using real-time first-principles electron-dynamics simulations based on time-dependent density functional theory (TDDFT). We reveal intensity-dependent absorption driven by multiphoton excitation and optically excited free carriers, and simulate the resulting electron-light coupled dynamics in TiO${}_2$ nanofilms using a multiscale Maxwell-TDDFT framework. Direct evaluation of the reflected and transmitted fields shows reduced reflectance at high intensities ($I\sim 10^{13}$ W/cm${}^2$), demonstrating a pronounced nonlinear optical response. Furthermore, the optical response properties are compared among various stable and metastable crystalline phases of TiO${}_2$-rutile, anatase, brookite, TiO${}_2$-II, and TiO${}_2$-B-as well as an amorphous supercell model. These results provide microscopic insight into intensity-dependent optical degradation in TiO${}_2$-based dielectric optical components exposed to intense femtosecond laser fields.

25 pages, 7 figures