In synthetic diamond plate, the intrapulse correlated dynamics of self-phase modulation and spontaneous Raman scattering by optical phonons were for the first time directly investigated for tightly focused (focusing numerical aperture NA = 0.25) positively-chirped visible-range ultrashort laser pulses with variable durations (0.3-9.5 ps) and energies, transmitted through the sample. The observed modulation of the transmitted light spectra and Stokes Raman scattering spectra for the different pulse durations were related to nonthermal excitation of nonlinear phonon polarization and its eventual picosecond-scale suppression due to thermal decay of optical phonons on the timescale of electron-phonon thermalization in the material.

The investigation of plasma channels induced by focused ultra-short 1030-nm laser pulses in bulk of synthetic HPHT diamond revealed strong dependence of their size and shape on the used numerical aperture of the lens (NA=0.15-0.45). It was shown that at loose focusing conditions, it is possible to significantly increase the length of the plasma channel with a slight increase in pulse power, while tight focusing allows to obtain more compact structures in the same range of used powers. Such dependence paves the way to new possibilities in 3D processing of transparent dielectrics, allowing, for example, to vary the spatial parameters of modified regions without changing the setup, but only by controlling the lens aperture, which seems very promising for industrial applications.

Self-phase modulation (SPM) broadening of laser spectra was studied in a transmission mode in natural and synthetic diamonds at variable laser wavelengths (515 and 1030 nm), pulse energies and widths (0.3 - 12 ps, positively chirped pulses), providing their filamentary propagation. Besides the monotonous SPM broadening of the laser spectra versus pulse energy, more pronounced for the (sub)picosecond pulsewiths and more doped natural diamond, periodical low-frequency modulation was observed in the spectra at the shorter laser pulsewidths, indicating dynamic Bragg filtering of the supercontinuum due to ultrafast plasma and nanoplasmonic effects. Damping of broadening and ultramodulation for the longer picosecond pulsewidths was related to thermalized electron-hole plasma regime established for the laser pulsewidths longer, than 2 ps. Unexpectedly, at higher pulse energies and corresponding longer microfilaments, the number of spectral modulation features increases, indicating dynamic variation of the periods in the longitudinal plasma Bragg gratings along the filaments due to prompt secondary laser-plasmon interactions.

Inscription of embedded photoluminescent microbits inside a bulk natural diamond, LiF and CaF2 crystals was performed in sub-filamentation (geometrical focusing) regime by 525nm 0.2ps laser pulses focused by 0.65NA micro-objective as a function of pulse energy, exposure and inter-layer separation. The resulting microbits were visualized by 3Dscanning confocal Raman/photoluminescence microscopy as conglomerates of photo-induced quasi-molecular color centers and tested regarding their annealing. Minimal lateral and longitudinal microbit separations, enabling their robust read-out, were measured in LiF as 1.5 and 13 microns, respectively, to be improved regarding information storage capacity by more elaborate focusing systems. These findings pave a way to novel optical storage platforms utilizing ultrashort-pulse laser inscription of photoluminescent microbits as carriers of archival memory.