Laser-Induced Periodic Surface Structures on Layered GaSe Crystals: Structural Coloring and Infrared Antireflection.

We study structural and morphological transformations caused by multipulse femtosecond-laser exposure of Bridgman-grown ϵ-phase GaSe crystals, a van der Waals semiconductor promising for nonlinear optics and optoelectronics. We unveil, for the first time, the laser-driven self-organization regimes in GaSe allowing the formation of regular laser-induced periodic surface structures (LIPSSs) that originate from interference of the incident radiation and interface surface plasmon waves. LIPSSs formation causes transformation of the near-surface layer to amorphous Ga2Se3 at negligible oxidation levels, evidenced from comprehensive structural characterization. LIPSSs imprinted on both output crystal facets provide a 1.2-fold increase of the near-IR transmittance, while the ability to control local periodicity by processing parameters enables multilevel structural color marking of the crystal surface. Our studies highlight direct fs-laser patterning as a multipurpose application-ready technology for precise nanostructuring of promising van der Waals semiconductors, whose layered structure restricts application of common nanofabrication approaches.

Hierarchical anti-reflective laser-induced periodic surface structures (LIPSSs) on amorphous Si films for sensing applications.

Here, we applied direct laser-induced periodic surface structuring to drive the phase transition of amorphous silicon (a-Si) into nanocrystalline (nc) Si imprinted as regular arrangement of Si nanopillars passivated with a SiO2 layer. By varying the laser beam scanning speed at a fixed pulse energy, we successfully tailored the resulting unique surface morphology of the formed LIPSSs that change from ordered arrangement of conical protrusions to highly uniform surface gratings, where sub-wavelength scale ripples decorate the valleys between near-wavelength scale ridges. Along with the surface morphology, the nc-Si/SiO2 volume ratio can also be controlled via laser processing parameters allowing the tailoring of the optical properties of the produced textured surfaces to achieve anti-reflection performance or partial transmission in the visible spectral range. Diverse hierarchical LIPSSs can be fabricated and replicated over large-scale areas opening a pathway for various applications including optical sensors, nanoscale temperature management, and solar light harvesting. By taking advantage of good wettability, enlarged surface area and remarkable light-trapping characteristics of the produced hierarchical morphologies, we demonstrated the first LIPSS-based surface enhanced fluorescent sensor that allowed the identification of metal cations providing a sub-nM detection limit unachievable by conventional fluorescence measurements in solutions.

Plasmonic Nanolenses Produced by Cylindrical Vector Beam Printing for Sensing Applications.

Interaction of complex-shaped light fields with specially designed plasmonic nanostructures gives rise to various intriguing optical phenomena like nanofocusing of surface waves, enhanced nonlinear optical response and appearance of specific low-loss modes, which can not be excited with ordinary Gaussian-shaped beams. Related complex-shaped nanostructures are commonly fabricated using rather expensive and time-consuming electron- and ion-beam lithography techniques limiting real-life applicability of such an approach. In this respect, plasmonic nanostructures designed to benefit from their excitation with complex-shaped light fields, as well as high-performing techniques allowing inexpensive and flexible fabrication of such structures, are of great demand for various applications. Here, we demonstrate a simple direct maskless laser-based approach for fabrication of back-reflector-coupled plasmonic nanorings arrays. The approach is based on delicate ablation of an upper metal film of a metal-insulator-metal (MIM) sandwich with donut-shaped laser pulses followed by argon ion-beam polishing. After being excited with a radially polarized beam, the MIM configuration of the nanorings permitted to realize efficient nanofocusing of constructively interfering plasmonic waves excited in the gap area between the nanoring and back-reflector mirror. For optimized MIM geometry excited by radially polarized CVB, substantial enhancement of the electromagnetic near-fields at the center of the ring within a single focal spot with the size of 0.37λ2 can be achieved, which is confirmed by Finite Difference Time Domain calculations, as well as by detection of 100-fold enhanced photoluminescent signal from adsorbed organic dye molecules. Simple large-scale and cost-efficient fabrication procedure offering also a freedom in the choice of materials to design MIM structures, along with remarkable optical and plasmonic characteristics of the produced structures make them promising for realization of various nanophotonic and biosensing platforms that utilize cylindrical vector beam as a pump source.

Zero-orbital-angular-momentum laser printing of chiral nanoneedles.

Laser irradiation of various materials including metals, polymers, and semiconductors with vortex beams was previously shown to "twist" transiently molten matter providing the direct easy-to-implement way to obtain chiral surface relief. Specifically for metals, this effect was attributed to transfer of an orbital angular momentum (OAM) carried by a vortex beam. In this Letter, we report the formation of twisted metallic nanoneedles on surfaces of silver and gold films under their irradiation by a zero-OAM laser beam with a spiral-shaped intensity distribution. Our comparative experiments clearly demonstrate, for the first time to the best of our knowledge, that the formation of the chiral nanoneedles on the noble-metal films is mainly governed by the temperature-gradient-induced chiral thermocapillary mass transfer, rather than by OAM-driven rotation of the molten matter.

Direct laser printing of chiral plasmonic nanojets by vortex beams.

Donut-shaped laser radiation, carrying orbital angular momentum, namely optical vortex, was recently shown to provide vectorial mass transfer, twisting transiently molten material and producing chiral micro-scale structures on surfaces of different bulk materials upon their resolidification. In this paper, we show that at high-NA focusing nanosecond laser vortices can produce chiral nanoneedles (nanojets) of variable size on thin films of such plasmonic materials, as silver and gold films, covering thermally insulating substrates. Main geometric parameters of the produced chiral nanojets, such as height and aspect ratio, were shown to be tunable in a wide range by varying metal film thickness, supporting substrates, and the optical size of the vortex beam. Donut-shaped vortex nanosecond laser pulses, carrying two vortices with opposite handedness, were demonstrated to produce two chiral nanojets twisted in opposite directions. These results suggest optical interference of the incident and reflected laser beams as a source of complex surface intensity distributions in metal films, possessing spiral components and driving both center-symmetric and spiral thermocapillary melt flows to yield in frozen nanoneedles with their pre-determined spiral nanocarving.