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A computational method based on a first-principles multiscale simulation hasbeen used for calculating the optical response and the ablation threshold of anoptical material irradiated with an ultrashort intense laser pulse. The methodemploys Maxwell's equations to describe laser pulse propagation andtime-dependent density functional theory to describe the generation ofconduction band electrons in an optical medium. Optical properties, such asreflectance and absorption, were investigated for laser intensities in therange $10^{10} \, \mathrm{W/cm^{2}}$ to $2 \times 10^{15} \, \mathrm{W/cm^{2}}$based on the theory of generation and spatial distribution of the conductionband electrons. The method was applied to investigate the changes in theoptical reflectance of $\alpha$-quartz bulk, half-wavelength thin-film andquarter-wavelength thin-film and to estimate their ablation thresholds. Despitethe adiabatic local density approximation used in calculating theexchange--correlation potential, the reflectance and the ablation thresholdobtained from our method agree well with the previous theoretical andexperimental results. The method can be applied to estimate the ablationthresholds for optical materials in general. The ablation threshold data can beused to design ultra-broadband high-damage-threshold coating structures.

First-principles simulation of the optical response of bulk and thin-film \alpha-quartz irradiated with an ultrashort intense laser pulse