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Microscale filamentation of 0.25 NA-focused, linearly and circularly polarized 1030 nm and 515 nm ultrashort laser pulses of variable pulse widths in fused silica, fluorite, and natural and synthetic diamonds demonstrates the Raman–Kerr effect in the form of critical pulse power magnitudes, proportional to squared wavelength and inversely proportional to laser pulse width of 0.3–10 ps. The first trend represents the common spectral relationship between the quantities, while the second indicates its time-integrated inertial contribution of Raman-active lattice polarization, appearing in transmission spectra via ultrafast optical-phonon Raman scattering. The optical-phonon contribution to the nonlinear polarization could come from laser field-induced spontaneous/stimulated Raman scattering and coherent optical phonons generated by electron–hole plasma with its clamped density in the nonlinear focus. Almost constant product value of the (sub)picosecond laser pulse widths and corresponding critical pulse powers for self-focusing and filamentation in the dielectrics (“critical pulse energy”) apparently implies constant magnitude of the nonlinear polarization and other “clamped” filamentation parameters at the given wavelength.

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The speed of the laser-supported hydrothermal wave is experimentally measured in porous polystyrene with overcritical average density. The results of the experiments are in agreement with the simulations performed with the MULTI-FM code, modeling the state of partly homogenized plasma. The measured velocity is 2 times smaller than the shock wave velocity calculated in simulations under the same conditions of laser irradiation in a homogeneous substance of the same density. The obtained results allow us to better investigate the possibility of using porous matter of overcritical density as an effective absorber-ablator in laser thermonuclear fusion targets.

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Ultrashort-pulse laser surface and bulk nano- and micromachining of dielectrics have multiple promising applications in micro-optics, microfluidics, and memory storage. The fundamental principles relate intrinsic inter-band multi-photon (MPA) and laser-induced intra-band free-carrier absorption (FCA) to particular ablation mechanisms and features. These principles are yet to be quantified into a complete set of basic experimental laser-matter interaction parameters, describing photoexcitation, relaxation, and final ablation. In this study, we considered the characteristic double-crater structure of single-shot ablation spots on dielectric surfaces and single-shot transmission spectra to extract crucial information about the underlying basic processes of ultrafast photoexcitation and laser energy deposition. Specifically, energy-dependent crater profiles and accompanying prompt self-phase modulation (SPM) spectral broadening were studied in single-shot surface ablation experiments on fluorite (CaF2) surface photo-excited by tightly focused 515- or 1030-nm, 300-fs laser pulses. Crater size dependence demonstrated two slopes, scaling proportionally to the squared focal 1/e-radius at higher energies (intensities) for larger ablated spots, and a much smaller squared 1/e-radius at lower energies (intensities) for (sub) micron-wide ablated spots, indicating a transition from 1D to 3D-ablation. As a result, these slopes were related to lower-intensity wavelength-dependent multi-photon inter-band transitions and wavelength-independent higher-intensity linear absorption in the emerging near-critical electron-hole plasma (EHP), respectively. Crater depth dependences on the local laser intensity fitted in the corresponding ranges by multi- and one-photon absorption provided the corresponding absorption coefficients. Spectral broadening measurements indicated even values for the red and blue shoulders of the laser pulse spectrum, representing the SPM effect in the weakly excited fluorite at the leading pulse front and providing the corresponding Kerr coefficient. In the second regime, the blue-shoulder broadening value saturated, indicating the appearance of near-critical plasma screening at the trailing pulse front, which is consistent with our calculations. These complementary experiments and related analysis provided an important set of key basic parameters, characterizing not only surface ablation, but also propagation of high-intensity ultrashort laser pulses in bulk fluorite, and enabling precise forecasting of optimal energy deposition for high-efficiency ultrashort-laser micro-structuring of this dielectric material.

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.

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.