Amorphous silicon ($\alpha$-Si) film present an inexpensive and promising material for optoelectronic and nanophotonic applications. Its basic optical and optoelectronic properties are known to be improved via phase transition from amorphous to polycrystalline phase. Infrared femtosecond laser radiation can be considered to be a promising nondestructive and facile way to drive uniform in-depth and lateral crystallization of $\alpha$-Si films that are typically opaque in UV-visible spectral range. However, so far only a few studies reported on use of near-IR radiation for laser-induced crystallization of $\alpha$-Si providing less information regarding optical properties of the resultant polycrystalline Si films demonstrating rather high surface roughness. The present work demonstrates efficient and gentle single-pass crystallization of $\alpha$-Si films induced by their direct irradiation with near-IR femtosecond laser pulses coming at sub-MHz repetition rate. Comprehensive analysis of morphology and composition of laser-annealed films by atomic-force microscopy, optical, micro-Raman and energy-dispersive X-ray spectroscopy, as well as numerical modeling of optical spectra, confirmed efficient crystallization of $\alpha$-Si and high-quality of the obtained films. Moreover, we highlight localized laser-induced crystallization of $\alpha$-Si as a promising way for optical information encryption, anti-counterfeiting and fabrication of micro-optical elements.

Recently, highly uniform thermochemical laser-induced periodic surface structures (TLIPSS) have attracted significant research attention due to their practical applicability for upscalable fabrication of periodic surface morphologies important for surface functionalization, diffraction optics, sensors, etc. When processed by femtosecond (fs) laser pulses in oxygen-containing environments, TLIPSS are formed on the material surface as parallel protrusions upon local oxidation in the maxima of the periodic intensity pattern coming from interference of the incident and scattered waves. From an application point of view, it is important to control both the TLIPSS period and nanoscale morphology of the formed protrusions that can be expectedly achieved by scalable shrinkage of the laser-processing wavelength as well as by varying the ambient environment. However, so far, the fabrication of uniform TLIPSS was reported only for near-IR wavelength in air. In this work, TLIPSS formation on the surface of titanium (Ti) films was systematically studied using near-IR (1026 nm), visible (513 nm) and UV (256 nm) wavelengths revealing linear scalability of the protrusion period versus the fs-laser wavelength. By changing the ambient environment from air to vacuum (10⁻² atm) and pressurized nitrogen gas (2.5 atm) we demonstrate tunability of the composition and morphology of the Ti TLIPSS protrusions. In particular, Raman spectroscopy revealed formation of TiN together with dominating TiO₂ (rutile phase) in the TLIPSS protrusions produced in the nitrogen-rich atmosphere.

Amorphous silicon (α-Si) film present an inexpensive and promising material for optoelectronic and nanophotonic applications. Its basic optical and optoelectronic properties are known to be improved via phase transition from amorphous to polycrystalline phase. Infrared femtosecond laser radiation can be considered as a promising nondestructive and facile way to drive uniform in-depth and lateral crystallization of α-Si films that are typically opaque in UV-visible spectral range. However, so far only a few studies reported on utilization of near-IR radiation for laser-induced crystallization of α-Si providing no information regarding optical properties of the resultant polycrystalline Si films. The present work demonstrates efficient and gentle single-pass crystallization of α-Si films induced by their direct irradiation with near-IR femtosecond laser pulses coming at sub-MHz repetition rate. Comprehensive analysis of morphology and composition of laser-annealed films by atomic-force microscopy, optical, micro-Raman and energy-dispersive X-ray spectroscopy, as well as numerical modeling of optical spectra, confirmed efficient crystallization of α-Si and high-quality of the obtained films. Moreover, we highlight localized laser-driven crystallization of α-Si as a promising way for optical information encryption, anti-counterfeiting and fabrication of micro-optical elements.