Ultrafast dynamics of single-pulse femtosecond laser-induced periodic ripples on the surface of a gold film

The ultrafast dynamics of periodic ripples are studied during their formation on the surface of a gold film with a prefabricated nanogroove. These transient ripples are induced by a single 800-nm, 50-fs laser pulse and are observed by a collinear pump-probe imaging method. When the laser polarization is parallel to the nanogroove, transient ripples begin appearing after an elapsed time of 25--80 ps, and become clear and regular at 400--600 ps. The ripple period increases from 685 to 770 nm as the laser fluence $F$ increases from 0.73 to $3.42\phantom{\rule{0.16em}{0ex}}\mathrm{J}/\mathrm{c}{\mathrm{m}}^{2}$. The evolution of temperature and lattice temperature are theoretically studied using the two-temperature model. When the laser fluence $F$ is above $0.73\phantom{\rule{0.16em}{0ex}}\mathrm{J}/\mathrm{c}{\mathrm{m}}^{2}$, the electron temperature rises to several ${10}^{4}\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, and the collision frequency rises above ${10}^{16}/\mathrm{s}$, which further causes the localization of hot electrons. Moreover, the $d$-band electrons can be excited through two-photon absorption and become free electrons. Using the dielectric constant of the excited states, which includes the effects of hot-electron localization and $d$-band transitions, the period predicted by the surface-plasmon-polarization (SPP) model accords well with experimental results. Both theory and experiment give support to SPP excitations playing a prominent role in the formation of periodic ripples induced by femtosecond laser pulses.

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