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PreprintarXiv licencearXiv

First-Principles Prediction of Nonlinear Optical Response in TiO2 for High-Power Dielectric Mirror Applications

Abstract

Dielectric multilayer mirrors are essential components in optical experiments using high-power lasers, where titanium dioxide (TiO2) is widely employed as a high-refractive-index dielectric material. In this study, we investigate the nonlinear optical response of TiO2 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 TiO2 nanofilms using a multiscale Maxwell-TDDFT framework. Direct evaluation of the reflected and transmitted fields shows reduced reflectance at high intensities (I ∼ 1013 W/cm2), demonstrating a pronounced nonlinear optical response. Furthermore, the optical response properties are compared among various stable and metastable crystalline phases of TiO2-rutile, anatase, brookite, TiO2-II, and TiO2-B-as well as an amorphous supercell model. These results provide microscopic insight into intensity-dependent optical degradation in TiO2-based dielectric optical components exposed to intense femtosecond laser fields.

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BibTeX
@misc{shimaoka2026firstprinciples,
  title = {{First-Principles Prediction of Nonlinear Optical Response in TiO$_2$ for High-Power Dielectric Mirror Applications}},
  author = {Koya Shimaoka and Yusuke Kondo and Kazunori Shibata and Mitsuharu Uemoto},
  howpublished = {arXiv},
  year = {2026},
  month = aug,
  doi = {10.48550/arxiv.2608.25129},
  eprint = {2608.25129},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2608.25129},
}
RIS
TY  - UNPB
TI  - First-Principles Prediction of Nonlinear Optical Response in TiO_2 for High-Power Dielectric Mirror Applications
AU  - Koya Shimaoka
AU  - Yusuke Kondo
AU  - Kazunori Shibata
AU  - Mitsuharu Uemoto
PY  - 2026
DA  - 2026/08/27
PB  - arXiv
DO  - 10.48550/arxiv.2608.25129
UR  - https://arxiv.org/abs/2608.25129
AB  - 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 ∼ 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.
ER  -