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.
Separate nanoholes with the minimum size down to 35 nm (~λ/15) and nanohole arrays with the hole size about 100 nm (~λ/5) were fabricated in a 50 nm optically "thick" Au/Pd film, using single 532 nm pump nanosecond laser pulses focused to diffraction-limited spots by a specially designed apertureless dielectric fiber probe. Nanohole fabrication in the metallic film was found to result from lateral heat diffusion and center-symmetrical lateral expulsion of the melt by its vapor recoil pressure. The optimized apertureless dielectric microprobe was demonstrated to enable laser fabrication of deep through nanoholes.
Hollow reduced-symmetry resonant plasmonic nanostructures possess pronounced tunable optical resonances in the UV-vis-IR range, being a promising platform for advanced nanophotonic devices. However, the present fabrication approaches require several consecutive technological steps to produce such nanostructures, making their large-scale fabrication rather time-consuming and expensive. Here, we report on direct single-step fabrication of large-scale arrays of hollow parabolic- and cone-shaped nanovoids in silver and gold thin films, using single-pulse femtosecond nanoablation at high repetition rates. The lateral and vertical size of such nanovoids was found to be laser energy-tunable. Resonant light scattering from individual nanovoids was observed in the visible spectral range, using dark-field confocal microspectroscopy, with the size-dependent resonant peak positions. These colored geometric resonances in far-field scattering were related to excitation and interference of transverse surface plasmon modes in nanovoid shells. Plasmon-mediated electromagnetic field enhancement near the nanovoids was evaluated via finite-difference time-domain calculations for their model shapes simulated by three-dimensional molecular dynamics, and experimentally verified by means of photoluminescence microscopy and Raman spectroscopy.
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