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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