Nanoscale thermally assisted hydrodynamic melt perturbations induced by ultrafast laser energy deposition in noble-metal films produce irreversible nanoscale translative mass redistributions and results in formation of radially-symmetric frozen surface structures. We demonstrate that the final three-dimensional (3D) shape of the surface structures formed after re-solidification of the molten part of the film is governed by incident laser fluence and, more importantly, predicted theoretically via molecular dynamics modeling. Considering the underlying physical processes associated with laser-induced energy absorption, electron-ion energy exchange, acoustic relaxation and hydrodynamic flows, the theoretical approach separating "slow" and "fast" physical processes and combining hybrid analytical two-temperature calculations, scalable molecular-dynamics simulations, and a semi-analytical thin-shell model was shown to provide accurate prediction of the final nanoscale solidified morphologies, fully consistent with direct electron-microscopy visualization of nanoscale focused ion-beam cuts of the surface structures produced at different incident laser fluences. Finally, these results are in reasonable quantitative agreement with mass distribution profiles across the surface nanostructures, provided by their noninvasive and non-destructive nanoscale characterization based on energy-dispersive x-ray fluorescence spectroscopy, operating at variable electron-beam energies.

Large-scale surface nanopatterning of a commercial silicon (Si) wafer in the form of regular 1D arrays of high-aspect-ratio vertical nanosheets (NSs) for antifouling and other potential promising optoelectronic, nanophotonic, and sensing applications was performed via multishot picosecond IRlaser ablation under a 5-mm-thick carbon disulfide liquid layer. Specifically, the nanopatterned surface layer demonstrates the broad ultralow mid-IR transmittance and the high content of sulfur, carbon, and even oxygen in the modified submicron-thick top layer, preventing the appearance of a Staphylococcus aureus bacterial biofilm. High-resolution transmission electron microscopy studies exhibit the anticorrelating inner versus outer surface abundance of donor sulfur versus adverse carbon and oxygen components and the amorphous structure of the sulfur-hyperdoped NSs atop their crystalline basements. These NSs indicate their appearance via the interfacial vapor/ plume bubble-mediated codeposition of Si ablation nanoplumes from the regular trenches and sulfur-containing products of carbon disulfide decomposition in the bubble. Numerical modeling indicates the nanoplasmonic origin of the Si NSs, self-limited in both the 100 nm periods and the submicron heights.

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Ultrafast intense photoexcitation of a silicon surface is complementarily studied experimentally and theoretically, with its prompt optical dielectric function obtained by means of time resolved optical reflection microscopy and the underlying electron-hole plasma dynamics modeled numerically, using a quantum kinetic approach. The corresponding transient surface plasmon-polariton (SPP) dispersion curves of the photo excited material were simulated as a function of the electron-hole plasma density, using the derived optical dielectric function model, and directly mapped at several laser photon energies, measuring spatial periods of the corresponding SPP mediated surface relief nanogratings. The unusual spectral dynam ics of the surface plasmon resonance, initially increasing with the increase in the electron-hole plasma den sity but damped at high interband absorption losses induced by the high density electron-hole plasma through instantaneous bandgap renormalization, was envisioned through the multi color mapping.

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