Security labeling and optical information encryption enabled by laser-printed silicon Mie resonators.

Fighting against the falsification of valuable items remains a crucial social-threatening challenge stimulating a never-ending search for novel anti-counterfeiting strategies. The demanding security labels must simultaneously address multiple requirements (high density of the recorded information, high protection degree, etc.) and be realized via scalable and inexpensive technologies. Here, the direct reproducible femtosecond-laser patterning of thin glass-supported amorphous (α-)Si films is proposed for optical information encryption and the scalable and highly reproducible fabrication of security labels composed of Raman-active hemispherical Si nanoparticles (NPs). Laser printing conditions allow the precise control of the diameter of the formed NPs ensuring translation of their dipolar Mie resonance position within the entire visible spectral range. Two-temperature molecular dynamics simulations clarify the origin of α-Si NP formation by rupture of the molten Si layer driven by a negative GPa-range pressure near the liquid-solid interface. Arrangement of the laser-printed Mie-resonant NP allows the creation of hidden security labels offering several easy-to-realize information encryption strategies (for example, local laser-induced post-crystallization or mixing Mie-resonant and non-resonant NPs), additional protection modalities, facile Raman mapping readout and dense information recording (up to 60 000 dots per inch) close to the optical diffraction limit. The developed fabrication strategy is simple, inexpensive, and scalable and can be realized based on cheap Earth-abundant materials and commercially-available equipment justifying its practical applicability and attractiveness for anti-counterfeit and security applications.

Deep Subwavelength Laser-Induced Periodic Surface Structures on Silicon as a Novel Multifunctional Biosensing Platform.

Strong light localization inside the nanoscale gaps provides remarkable opportunities for creation of various medical and biosensing platforms stimulating an active search for inexpensive and easily scalable fabrication at a sub-100 nm resolution. In this paper, self-organized laser-induced periodic surface structures (LIPSSs) with the shortest ever reported periodicity of 70 ± 10 nm were directly imprinted on the crystalline Si wafer upon its direct femtosecond-laser ablation in isopropanol. Appearance of such a nanoscale morphology was explained by the formation of a periodic topography on the surface of photoexcited Si driven by interference phenomena as well as subsequent down-scaling of the imprinted grating period via Rayleigh-Taylor hydrodynamic instability. The produced deep subwavelength LIPSSs demonstrate strong anisotropic anti-reflection performance, ensuring efficient delivery of the incident far-field radiation to the electromagnetic "hot spots" localized in the Si nanogaps. This allows realization of various optical biosensing platforms operating via strong interactions of quantum emitters with nanoscale light fields. The demonstrated 80-fold enhancement of spontaneous emission from the attached nanolayer of organic dye molecules and in situ optical tracing of catalytic molecular transformations substantiate bare and metal-capped deep subwavelength Si LIPSSs as a promising inexpensive multifunctional biosensing platform.

Laser-printed hemispherical silicon Mie resonators.

Subwavelength nanostructures made of high-index low-loss materials have revolutionized the fields of linear and nonlinear nanophotonics, stimulating growing demands for efficient and inexpensive fabrication technologies. Here, we demonstrate high-precision and reproducible printing of hemispherical Si nanoparticles (NPs) via controllable dewetting of glass-supported $\alpha$-Si films driven by a single femtosecond laser pulse. The diameter of the formed nanocrystalline NPs can be fully controlled by initial $\alpha$-Si film thickness as well as lateral size of the laser spot and can be predicted by a simple empirical model based on conservation of energy and mass. A resonant optical response associated with Mie-type resonances supported by hemispherical NPs was confirmed by combining numerical modeling with optical microspectroscopy. Inexpensive and high-performing direct laser printing of nanocrystalline Si Mie resonators with a user-defined arrangement opens a pathway for various applications in optical sensing and nonlinear nanophotonics.

Laser Printing of Plasmonic Nanosponges.

Three-dimensional porous nanostructures made of noble metals represent novel class of nanomaterials promising for nonlinear nanooptics and sensors. Such nanostructures are typically fabricated using either reproducible yet time-consuming and costly multi-step lithography protocols or less reproducible chemical synthesis that involve liquid processing with toxic compounds. Here, we combined scalable nanosecond-laser ablation with advanced engineering of the chemical composition of thin substrate-supported Au films to produce nanobumps containing multiple nanopores inside. Most of the nanopores hidden beneath the nanobump surface can be further uncapped using gentle etching of the nanobumps by an Ar-ion beam to form functional 3D plasmonic nanosponges. The nanopores 10-150 nm in diameter were found to appear via laser-induced explosive evaporation/boiling and coalescence of the randomly arranged nucleation sites formed by nitrogen-rich areas of the Au films. Density of the nanopores can be controlled by the amount of the nitrogen in the Au films regulated in the process of their magnetron sputtering assisted with nitrogen-containing discharge gas.

Single-Mode Lasing from Imprinted Halide-Perovskite Microdisks.

Halide-perovskite microlasers have demonstrated fascinating performance owing to their low-threshold lasing at room temperature and low-cost fabrication. However, being synthesized chemically, controllable fabrication of such microlasers remains challenging, and it requires template-assisted growth or complicated nanolithography. Here, we suggest and implement an approach for the fabrication of microlasers by direct laser ablation of a thin film on glass with donut-shaped femtosecond laser beams. The fabricated microlasers represent MAPbBr xI y microdisks with 760 nm thickness and diameters ranging from 2 to 9 µm that are controlled by a topological charge of the vortex beam. As a result, this method allows one to fabricate single-mode perovskite microlasers operating at room temperature in a broad spectral range (550-800 nm) with Q-factors up to 5500. High-speed fabrication and reproducibility of microdisk parameters, as well as a precise control of their location on a surface, make it possible to fabricate centimeter-sized arrays of such microlasers. Our finding is important for direct writing of fully integrated coherent light sources for advanced photonic and optoelectronic circuitry.

On-Fly Femtosecond-Laser Fabrication of Self-Organized Plasmonic Nanotextures for Chemo- and Biosensing Applications.

Surface-enhanced Raman scattering (SERS) and surface-enhanced photoluminescence (SEPL) are emerging as versatile widespread methods for biological, chemical, and physical characterization in close proximity of nanostructured surfaces of plasmonic materials. Meanwhile, single-step, facile, cheap, and green technologies for large-scale fabrication of efficient SERS or SEPL substrates, routinely demonstrating both broad plasmonic response and high enhancement characteristics, are still missing. In this research, single-pulse spallative micron-size craters in a thick Ag film with their internal nanotexture in the form of nanosized tips are for the first time shown to demonstrate strong polarization-dependent enhancement of SEPL and SERS responses from a nanometer-thick covering Rhodamine 6G layer with average enhancement factors of 40 and 2 × 10(6), respectively. Additionally, the first detailed experimental study is reported for physical processes, underlying the formation mechanisms of ablative nanotextures on such "thick" metal films. Such mechanisms demonstrate a complex "hybrid" fluence-dependent ablation character-appearance of spallative craters, typical for bulk material, at low fluences and formation of upright standing nanotips (frozen nanojets), usually associated with thin-film ablation, in the crater centers at higher fluences. Moreover, special emphasis was made on the possibility to reshape the nanotopography of such spallative craters through multipulse laser-induced merging of their small nanotips into larger ones. The presented approach holds promise to be one of the cheapest and easiest-to-implement ways to mass-fabricate various efficient spallation-nanotextured single-element plasmonic substrates for routine chemo- and biosensing, using MHz-repetition-rate femtosecond fiber laser sources with multiplexed laser-beams.