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arXiv · 2608.25129

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

Koya Shimaoka·Yusuke Kondo·Kazunori Shibata·Mitsuharu Uemoto
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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.

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Koya Shimaoka, Yusuke Kondo, Kazunori Shibata, Mitsuharu Uemoto. 2026-08-25. First-Principles Prediction of Nonlinear Optical Response in TiO$_2$ for High-Power Dielectric Mirror Applications. https://arxiv.org/abs/2608.25129

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