A. A. Rudenko

Enhancement of ultrafast electron photoemission from metallic nanoantennas excited by a femtosecond laser pulse

We have demonstrated for the first time that an array of nanoantennas (central nanotips inside sub-micrometer pits) on an aluminum surface, fabricated using a specific double-pulse femtosecond laser irradiation scheme, results in a 28-fold enhancement of the non-linear (three-photon) electron photoemission yield, driven by a third intense IR femtosecond laser pulse. The supporting numerical electrodynamic modeling indicates that the electron emission is increased not owing to a larger effective aluminum surface, but due to instant local electromagnetic field enhancement near the nanoantenna, contributed by both the tip’s ‘lightning rod’ effect and the focusing effect of the pit as a microreflector and annular edge as a plasmonic lens.

Nanoscale hydrodynamic instability in a molten thin gold film induced by femtosecond laser ablation

A mechanism of the formation of a nanotip with a nanoparticle at its top that appears in a thin metal film irradiated by a single femtosecond laser pulse has been studied experimentally and theoretically. It has been found that the nanotip appears owing to a melt flow and a nanojet formation, which is cooled and solidified. Within a proposed hydrodynamic model, the development of thermocapillary instability in the melted film is treated with the use of the Kuramoto-Sivashinsky-type hydrodynamic equation. The simulation shows that the nanojet nucleates in the form of a nanopeak in a pit on the top of a microbump (linear stage) and, then, grows in a nonlinear (explosive) regime of an increase in thermocapillary instability in good agreement with experimental data.

Formation of nanobumps and nanoholes in thin metal films by strongly focused nanosecond laser pulses

Nanobumps and nanoholes have been formed in gold and silver films with various thicknesses on a dielectric substrate by strongly focused single nanosecond pulses of a Nd:YAG laser. An apertureless dielectric fiber probe and an aspherical lens with a numerical aperture of 0.5 were used to focus laser radiation into a diffraction-limited spot on the surface of gold and silver films, respectively. Atomic force and electron microscopy studies have demonstrated that the shape and dimension of nanostructures, as well as the threshold parameters of laser radiation for their formation, are determined by the thickness of a modified film (“size effect”) and by the duration of a laser pulse owing to the lateral heat conduction in films (nonlocal energy deposition effect). Mechanisms of the dynamic formation of such structures in metallic films by nanosecond laser pulses due to phase transformations of their material have been discussed.

Nanoscale boiling during single-shot femtosecond laser ablation of thin gold films

A nanoscale chaotic relief structure appears as a result of subthreshold single-shot femtosecond laser ablation of gold films in the regimes of fabrication of microbumps and nanospikes, but only for a relatively thick film. The observed nanoablation tendency versus film thickness makes it possible to suppose the existence of a sub-surface temperature maximum in thicker gold films and its absence within thinner film, which results from competing evaporative cooling and electronic heat conduction, as demonstrated by numerical simulations of the thermal dynamics.

Nanoscale surface boiling in sub-threshold damage and above-threshold spallation of bulk aluminum and gold by single femtosecond laser pulses

The sub and near-threshold topographic signatures of the spallation of nanometer-thick melt layers during single-shot femtosecond laser ablation of bulk aluminum and gold were experimentally observed for the first time, using scanning electron microscopy with high spatial resolution. The novel ablative nanofeatures—sub-threshold boiling nanopits, the partially detached ultrathin solidified melt layer, and the lamellar surface structure under the layer along the spallative crater border, as well as the foam-like nanostructure of the crater bottom—indicate the boiling origin of the spallation threshold, rather than the thermomechanical rupture of the molten surface layer in a propagating unloading wave. These ablative surface nanofeatures were also revealed in trenches of single-shot, near-wavelength normal interference ripples on the aluminum surface, indicating their spallative nature and being promising for biosensing applications.

Silicon as a virtual plasmonic material: Acquisition of its transient optical constants and the ultrafast surface plasmon-polariton excitation

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 dynamics of the surface plasmon resonance, initially increasing with the increase in the electron-hole plasma density 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.

Focusing of intense femtosecond surface plasmon-polaritons

Nonlinear propagation and focusing within a metallic ring of intense (near or higher than metal ablation threshold) surface plasmon-polaritons excited by a femtosecond laser pulse was experimentally and theoretically studied. Fundamental possibility of local fluence increasing at focus of such plasmonic lens (the ring) by two orders of magnitude was shown. Formation of surface nanostructures as a result of the surface plasmon-polaritons focusing was experimentally observed.

Structure and laser-fabrication mechanisms of microcones on silver films of variable thickness

Submicron dimensions, nanoscale crystalline structure, and fabrication mechanisms of microcones on silver films of variable (50–380 nm) thickness deposited onto glass substrates by single strongly focused femtosecond laser pulses of different fluences are experimentally studied using scanning electron microscopy. Fabrication mechanisms for nanoholes and microcones are discussed for films of the different thickness, as well as the extraordinary shapes of their constituent nanocrystallites, strongly elongated along the melt flow direction in thin films.

Flash-imprinting of intense femtosecond surface plasmons for advanced nanoantenna fabrication

In this work, we demonstrate an all-laser method of fabrication of optical nanoantennas (ONAs) with an additional coupling/focusing diffractive element. This method is based on double-shot femtosecond laser nanoablation of a thin supported metallic film, inducing a sequence of electrodynamic (surface plasmon-polariton [SPP] excitation and interference), thermal (melting, ablation and ultrafast cooling), and hydrodynamic processes. In particular, the thermal and hydrodynamic processes are important for ONA formation after the first laser shot, while second spatially shifted laser shot via an induced SPP wave results in a radial surface grating near the nanoantenna. Such gratings provide efficient coupling between incident laser radiation and SPP waves, thus significantly improving the ONA efficiency.

Nonlinear optical dynamics during femtosecond laser nanostructuring of a silicon surface

Non-linear cumulative self-organization dynamics of femtosecond laser-induced surface relief ripples was for the first time experimentally revealed on a silicon surface as their primary appearance, degradation and revival, reflecting ultrafast non-linear dynamics of corresponding optical interference surface patterns. Such dynamics were revealed by electrodynamic modeling to be directly driven by related instantaneous surface optical patterns, which are sensitive not only to cumulative ripple deepening (steady-state feedback factor), but to laser-induced instantaneous variation of surface dielectric function, providing either positive or negative fluence-dependent optical feedbacks.