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We discuss the dynamics of ultrashort pulsed laser excitation in bulk optical silica-based glasses (fused silica and borosilicate BK7) well-above the permanent modification threshold. We indicate subsequent structural and thermomechanical energy relaxation paths that translate into positive and negative refractive index changes, compression and rarefaction zones. If fast electronic decay occurs at low excitation levels in fused silica via self-trapping of excitons, for carrier densities in the vicinity of the critical value at the incident wavelength, persistent long-living absorptive states indicate the achievement of low viscosity matter states manifesting pressure relaxation, rarefaction, void opening and compaction in the neighboring domains. An intermediate ps-long excited carrier dynamics is observed for BK7 in the range corresponding to structural expansion and rarefaction. The amount of excitation and the strength of the subsequent hydrodynamic evolution is critically dependent on the pulse time envelope, indicative of potential optimization schemes.
We report on the observation of subcycle interferences of electron wave packets released during strong field ionization of $\text{H}_{2}$ with cycle-shaped two-color laser fields. With a reaction microscope we measure three-dimensional momentum distributions of photoelectrons correlated with either $\text{H}_{2}^{+}$ or protons within different energy ranges generated by dissociation of $\text{H}_{2}^{+}$. We refer to these different types of photoelectrons as channels. Our results show that the subcycle interference structures of electron wave packets are very sensitive to the cycle shape of the two-color laser field. We explain this behavior by the dependence of the ionization time within an optical cycle on the shape of the laser field cycle. The subcycle interference structures can be further used to obtain insight into the subcycle dynamics of molecules during strong field interaction.
The interactions of strong-field few-cycle laser pulses with metastable states of noble gas atoms are examined. Metastable noble gas atoms offer a combination of low ionization potential and a relatively simple atomic structure, making them excellent targets for examining ionization dynamics in varying experimental conditions. A review of the current work performed on metastable noble gas atoms is presented.
Over the past decade the integration of ultrafast spectroscopy with nanoscience has greatly propelled the development of nanoscience, as the key information gleaned from the mechanistic studies with the assistance of ultrafast spectroscopy enables a deeper understanding of the structure–function interplay and various interactions involved in the nanosystems. This mini-review presents an overview of the recent advances achieved in our ultrafast spectroscopy laboratory that address the ultrafast dynamics and related mechanisms in several representative nanomaterial complex systems by means of femtosecond time-resolved transient absorption spectroscopy. We attempt to convey instructive, consistent information regarding the important processes, pathways, dynamics, and interactions involved in the nanomaterial complex systems, most of which exhibit excellent performance in photocatalysis.
We demonstrate that the methodology of frequency-resolved optical gating (FROG) is applicable to time-resolved reflection spectroscopy of a plasma mirror in the vacuum-ultraviolet (VUV) region. Our recent study [R. Itakura et al. Opt. Express 23, 10914 (2015)] has shown that a VUV waveform can be retrieved from a VUV reflection spectrogram of a plasma mirror formed on a fused silica (FS) surface by irradiation with an intense femtosecond laser pulse. Simultaneously, the increase in the reflectivity with respect to the Fresnel reflection of the unexcited FS surface can be obtained as a time-dependent reflectivity of the plasma mirror. In this study, we update the FROG analysis procedure using the least-square generalized projections algorithm. This procedure can reach convergence much faster than the previous one and has no aliasing problem. It is demonstrated that a significantly chirped VUV pulse as long as 1 ps can be precisely characterized.