The ultrafast interaction of tightly focused femtosecond laser pulses with bulk dielectric media in direct laser writing (inscription) regimes is known to proceed via complex multi-scale light, plasma and material modification nanopatterns, which are challenging for exploration owing to their mesoscopic, transient and buried character. In this study, we report on the first experimental demonstration, analysis and modeling of hierarchical multi-period coupled longitudinal and transverse nanogratings in bulk lithium niobate inscribed in the focal region by 1030 nm, 300 fs laser pulses in the recently proposed sub-filamentary laser inscription regime. The longitudinal Bragg-like topography nanogratings, possessing the laser-intensity-dependent periods ≈ 400 nm, consist of transverse birefringent nanogratings, which are perpendicular to the laser polarization and exhibit much smaller periods ≈ 160 nm. Our analysis and modeling support the photonic origin of the longitudinal nanogratings, appearing as prompt electromagnetic and corresponding ionization standing waves in the pre-focal region due to interference of the incident and plasma-reflected laser pulse parts. The transverse nanogratings could be assigned to the nanoscale material modification by interfacial plasmons, excited and interfered in the resulting longitudinal array of the plasma sheets in the bulk dielectric material. Our experimental findings provide strong support for our previously proposed mechanism of such hierarchical laser nanopatterning in bulk dielectrics, giving important insights into its crucial parameters and opening the way for directional harnessing of this technology.

Ferroelectric nanodomains were formed in bulk lithium niobate single crystals near nanostructured microtracks laser-inscribed by 1030-nm 0.3-ps ultrashort laser pulses at variable pulse energies in sub- and weakly filamentary laser nanopatterning regimes. The microtracks and related nanodomains were characterized by optical, scanning probe and confocal second-harmonic generation microscopy methods. The nanoscale material sub-structure in the microtracks was visualized in the sample cross-sections by atomic force microscopy (AFM), appearing weakly birefringent in polarimetric microscope images. The piezoresponce force microscopy (PFM) revealed sub-100 nm ferroelectric domains formed in the vicinity of the embedded microtrack seeds, indicating a promising opportunity to arrange nanodomains in the bulk ferroelectric crystal in on-demand positions. These findings open a new modality in direct laser writing technology, which is related to nanoscale writing of ferroelectric nanodomains and prospective three-dimensional micro-electrooptical and nanophotonic devices in nonlinear-optical ferroelectrics.

Laser inscription of form-birefringent nanograting layers inside fused silica by ultrashort (femto-picosecond) laser pulses at 515 nm was studied as a function of laser, average power and pulsewidth in terms of fabrication regimes. Retardance magnitudes were acquired for single birefringent layers inscribed at different laser parameters, enabling fabrication of polarization-based spectral micro-filters in the form of few-layer microdevices and of microfluidic multi-color refractive-index chemo/biosensor.

The inscription regimes and formation mechanisms of form-birefringent microstructures inside nano-porous fused silica by tightly focused 1030- and 515-nm ultrashort laser pulses of variable energy levels and pulsewidths in the sub-filamentary regime were explored. Energy-dispersion X-ray micro-spectroscopy and 3D scanning confocal Raman micro-spectroscopy revealed the micro-tracks compacted by the multi-shot laser exposure with the nanopores hydrodynamically driven on a microscale to their periphery. Nearly homogeneous polarimetrically acquired subwavelength-scale form-birefringence (refractive index modulation ~10⁻³) was simultaneously produced as birefringent nanogratings inside the microtracks of wavelength-, energy- and pulsewidth-dependent lengths, enabling the scaling of their total retardance for perspective phase-modulation nanophotonic applications. The observed form-birefringence was related to the hierarchical multi-scale structure of the microtracks, envisioned by cross-sectional atomic-force microscopy and numerical modeling.