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 3.42J/cm2. The evolution of temperature and lattice temperature are theoretically studied using the two-temperature model. When the laser fluence F is above 0.73J/cm2, the electron temperature rises to several 104K, and the collision frequency rises above 1016/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.