Conical third harmonic generation from volume nanogratings induced by filamentation of femtosecond pulses in transparent bulk materials.

We report on observations of conical third harmonic emission that emerges during supercontinuum generation produced by self-focusing and filamentation of high (20-200 kHz) repetition rate 180 fs, 1035 nm pulses from an amplified Yb:KGW laser in various nonlinear crystals and glasses: YAG, sapphire, YLF, LiF, CaF2, MgF2, LiSAF, fused silica and BK-7 glass. We show that conical third harmonic generation is a phase-matched four-wave mixing process, where noncollinear phase matching is achieved by means of reciprocal lattice vector, inversely proportional to the period of nanograting, which is inscribed by femtosecond filament in the volume of nonlinear material. The existence of a particular period required to phase match conical third harmonic generation was indirectly verified by investigations of periodicity features of high and low spatial frequency laser-induced periodic surface structures, in which matter is reorganized in a similar fashion.

Electron paramagnetic resonance study of ferroelectric phase transition and dynamic effects in a Mn2+ doped [NH4][Zn(HCOO)3] hybrid formate framework.

We present an X- and Q-band continuous wave (CW) and pulse electron paramagnetic resonance (EPR) study of a manganese doped [NH4][Zn(HCOO)3] hybrid framework, which exhibits a ferroelectric structural phase transition at 190 K. The CW EPR spectra obtained at different temperatures exhibit clear changes at the phase transition temperature. This suggests a successful substitution of the Zn2+ ions by the paramagnetic Mn2+ centers, which is further confirmed by the pulse EPR and 1H ENDOR experiments. Spectral simulations of the CW EPR spectra are used to obtain the temperature dependence of the Mn2+ zero-field splitting, which indicates a gradual deformation of the MnO6 octahedra indicating a continuous character of the transition. The determined data allow us to extract the critical exponent of the order parameter (ß = 0.12), which suggests a quasi two-dimensional ordering in [NH4][Zn(HCOO)3]. The experimental EPR results are supported by the density functional theory calculations of the zero-field splitting parameters. Relaxation time measurements of the Mn2+ centers indicate that the longitudinal relaxation is mainly driven by the optical phonons, which correspond to the vibrations of the metal-oxygen octahedra. The temperature behavior of the transverse relaxation indicates a dynamic process in the ordered ferroelectric phase.

Low spatial frequency laser-induced periodic surface structures in fused silica inscribed by widely tunable femtosecond laser pulses.

The formation and evolution of laser-induced periodic surface structures in fused silica under irradiation of widely tunable (in the 1-3 [Formula: see text]m range) linearly polarized femtosecond (200 fs) pulses was studied experimentally. The structures were inscribed in high fluence regime (exceeding the surface ablation threshold for a single pulse) and characterized by using scanning electron microscopy and two dimensional Fourier transform. The results revealed rapid (after irradiation with a few successive pulses) formation of periodic laser-induced periodic surface structures aligned parallel to laser polarization, whose period increases with increasing the inscription wavelength, obeying the [Formula: see text] law. With further increase of number of pulses, the generated structures gradually reorganize into laser polarization-independent low spatial frequency annular structures associated with formation of the damage crater, which fully established after irradiation with a few tens of successive laser pulses. This particular evolution scenario was observed over the entire wavelength tuning range of incident pulses.