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Following a recently manifested guide of how to team up infrared transparency and high electrical conductivity within semimetal materials [C. Cui $et$ $al.$ Prog. Mater. Sci. 2023, 136, 101112], we evaluate an applicability of the calcium digermanide (CaGe$_2$) thin film electrodes for the advanced Ge-based optical devices. Rigorous growth experiments were conducted to define the optimal annealing treatment and thickness of the Ca-Ge mixture for producing stable CaGe$_2$ layers with high figure of merit (FOM) as transparent conducting material. Ab-initio electronic band structure calculations and optical modeling confirmed CaGe$_2$ semimetal nature, which is responsible for a demonstrated high FOM. To test CaGe$_2$ electrodes under actual conditions, a planar Ge photodetector (PD) with metal-semiconductor-metal structure was fabricated, where CaGe$_2$/Ge interface acts as Schottky barrier. The resulting Ge PD with semimetal electrodes outperformed commercially available Ge devices in terms of both photoresponse magnitude and operated spectral range. Moreover, by using femtosecond-laser projection lithography, a mesh CaGe$_2$ electrode with the relative broadband transmittance of 90\% and sheet resistance of 20 $\Omega$/sq. was demonstrated, which further enhanced Ge PD photoresponse. Thus, obtained results suggest that CaGe$_2$ thin films have a great potential in numerous applications promoting the era of advanced Ge optoelectronics., Comment: 12 pages, 4 figures

Here, upon systematic studies of femtosecond-laser processing of monocrystalline Si in oxidation-preventing methanol, we showed that the electromagnetic processes dominating at initial steps of the progressive morphology evolution define the onset of the hydrodynamic processes and resulting morphology upon subsequent multi-pulse exposure. In particular, under promoted exposure quasi-regular subwavelength laser-induced periodic surface structures (LIPSSs) were justified to evolve through the template-assisted development of the Rayleigh-Plateau hydrodynamic instability in the molten ridges forming quasi-regular surface patterns with a supra-wavelength periodicity and preferential alignment along polarization direction of the incident light. Subsequent exposure promotes fusion-assisted morphology rearrangement resulting in a spiky surface with a random orientation, yet constant inter-structure distance correlated with initial LIPSS periodicity. Along with the insight onto the physical picture driving the morphology evolution and supra-wavelength nanostructure formation, our experiments also demonstrated that the resulting quasi-regular and random spiky morphology can be tailored by the intensity/polarization distribution of the incident laser beam allowing on-demand surface nanotexturing with diverse hierarchical surface morphologies exhibiting reduced reflectivity in the visible and shortwave IR spectral ranges. Finally, we highlighted the practical attractiveness of the suggested approach for improving near-IR photoresponse and expanding operation spectral range of vertical p-n junction Si photo-detector operating under room temperature and zero-bias conditions via single-step annealing-free laser nanopatterning of its surface., Comment: 13 pages, 6 figures

Ultrashort laser pulses allows to deliver electromagnetic energy to matter causing its localized heating that can be used for both material removal via ablation/evaporation and drive interface chemical reactions. Here, we showed that both mentioned processes can be simultaneously combined within straightforward laser nanotexturing of Si wafer in functionalizing solution to produce a practically relevant metal-semiconductor surface nano-morphology. Such unique hybrid morphology represent deep-subwavelength Si LIPSSs with a extremely short period down to 70 nm with their high-aspect-ratio nanotrenches loaded with controllable amount of plasmonic nanoparticles formed $via$ laser-induced decomposition of the precursor noble-metal salts. Moreover, heat localization driving reduction process was utilized to produce surface morphology locally decorated with dissimilar plasmon-active nanoparticles. Light-absorbing deep-subwavelength Si LIPSSs loaded with controllable amount of noble-metal nanoparticles represent an attractive architecture for plasmon-related applications such as optical nanosensing where efficient coupling of the propagating optical waves to highly localized electromagnetic ``hot spots`` is a mandatory requirement. To support this statement we demonstrated applicability of such hybrid morphology for fluorescence-based detection of nanomolar concentrations of mercury cations in solution., Comment: 10 pages, 5 figures

Textured silicon surface structures, in particular black silicon (b-Si), open up possibilities for Si-based solar cells and photodetectors to be extremely thin and highly sensitive owing to perfect light-trapping and anti-reflection properties. However, near-infrared (NIR) performance of bare b-Si is limited by Si band gap of 1.12 eV or 1100 nm. This work reports a simple method to increase NIR absorption of b-Si by $in$ $vacuo$ silicidation with magnesium. Obtained Mg$_2$Si/b-Si heterostructure has a complex geometry where b-Si nanocones are covered by Mg$_2$Si shells and crowned with flake-like Mg$_2$Si hexagons. Mg$_2$Si formation atop b-Si resulted in 5-fold lower reflectivity and optical absorption to be no lower than 88\% over 200-1800 nm spectral range. More importantly, Mg$_2$Si/b-Si heterostructure is more adjusted to match AM-1.5 solar spectrum with theoretically higher photogenerated current density. The maximal advantage is demonstrated in the NIR region compared to bare b-Si in full accordance with one's expectations about NIR sensitive narrow band gap ($\sim$0.75 eV) semiconductor with high absorption coefficient, which is Mg$_2$Si. Results of optical simulation confirmed the superiority of Mg$_2$Si/b-Si NIR performance. Therefore, this new wide-band optical absorber called black silicide proved rather competitive alongside state-of-the-art approaches to extend b-Si spectral blackness., Comment: 8 pages, 4 figures

Recent progress in hybrid nanomaterials composed of dissimilar constituents permitted to improve performance and functionality of novel devices developed for optoelectronics, catalysis, medical diagnostic and sensing. However, the rational combination of such contrasting materials as noble metals and semiconductors within individual hybrid nanostructures $via$ a ready-to-use and lithography-free fabrication approach is still a standing challenge. Here, we report on a two-step synthesis of Au-Si microspheres generated by laser ablation of silicon in isopropanol followed by laser irradiation of the produced Si nanoparticles in presence of HAuCl$_4$. Thermal reduction of [AuCl$_4$]$^-$ species to metallic gold phase, along with its subsequent mixing with silicon under laser irradiation creates a nanostructured material with a unique composition and morphology revealed by electron microscopy, tomography and elemental analysis. Combination of such basic plasmonic and nanophotonic materials as gold and silicon within a single microsphere allows for efficient light-to-heat conversion, as well as single-particle SERS sensing with temperature feedback modality and expanded functionality. Moreover, the characteristic Raman signal and hot-electron induced nonlinear photoluminescence coexisting within Au-Si hybrids, as well as commonly criticized randomness of the nanomaterials prepared by laser ablation in liquid, were proved useful for realization of anti-counterfeiting labels based on physically unclonable function approach., Comment: 10 pages; 4 figures

Security labels combining facile structural color readout and physically unclonable one-way function (PUF) approach provide promising strategy for fighting against forgery of marketable products. Here, we justify direct femtosecond-laser printing, a simple and scalable technology, for fabrication of high-resolution (12500 dots per inch) and durable PUF labels with a substantially large encoding capacity of 10$^{895}$ and a simple spectroscopy-free optical signal readout. The proposed tags are comprised of laser-printed plasmonic nanostructures exhibiting unique light scattering behavior and unclonable 3D geometry. Uncontrollable stochastic variation of the nanostructure geometry in the process of their spot-by-spot printing results in random and broadband variation of the scattering color of each laser printed "pixel", making laser-printed patterns unique and suitable for PUF labeling., Comment: 5 pages, 3 figures

Donut-shaped laser radiation, carrying orbital angular momentum, namely optical vortex, recently was 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 for the first time that 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. The results provide new important insights into fundamental physics of the vectorial laser-beam assisted mass transfer in metal films and demonstrate the great potential of this technique for fast easy-to-implement fabrication of chiral plasmonic nanostructures., Comment: 7 pages, 4 figures

We propose to use femtosecond direct laser writing technique to realize dielectric optical elements from photo-resist materials for the generation of structured light from purely geometrical phase transformations. This is illustrated by the fabrication and characterization of spin-to-orbital optical angular momentum couplers generating optical vortices of topological charge from 1 to 20. In addition, the technique is scalable and allows obtaining microscopic to macroscopic flat optics. These results thus demonstrate that direct 3D photopolymerization technology qualifies for the realization of spin-controlled geometric phase optical elements., Comment: 6 figures

Simple high-performance two-stage hybrid technique was developed for fabrication of different plasmonic nanostructures, including nanorods, nanorings, as well as more complex structures on glass substrates. In this technique a thin noble metal film on a dielectric substrate is irradiated by a tightly focused single nanosecond laser pulse and then the modified region is slowly polished by an accelerated argon ion (Ar+) beam. As a result, each nanosecond laser pulse locally modifies the initial metal film through initiation of fast melting and subsequent hydrodynamic processes, while the following Ar+-ion polishing removes the rest of the film, revealing the hidden topography features and fabricating separate plasmonic structures on the glass substrate. We demonstrate that the shape and lateral size of the resulting functional plasmonic nanostructures depends on the laser pulse energy and metal film thickness, while subsequent Ar+-ion polishing enables to vary height of the resulting nanostructures. The plasmonic properties of the fabricated nanostructures were characterized by dark-field micro-spectroscopy, Raman and photoluminescence measurements from single nanofeatures, as well as by supporting numerical calculations of the related electromagnetic near-fields and Purcell factors. The developed simple two-stage technique represents a next step towards direct large-scale laser-induced fabrication of highly-ordered arrays of complex plasmonic nanostructures., Comment: Manuscript: 28 pages and 6 figures. Supplementary information: 2 pages and 3 figures