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Over the past years, many applications based on laser-induced refractive index changes in the volume of transparent materials have been demonstrated. Ultrashort pulse lasers offer the possibility to process bulky transparent materials in three dimensions, suggesting that direct laser writing will play a decisive role in the development of integrated micro-optics. At the present time, applications such as 3D long term data storage or embedded laser marking are already into the phase of industrial development. However, a quantitative estimate of the laser-induced refractive index change is still very challenging to obtain. On another hand, several microscopy techniques have been recently developed to characterize bulk refractive index changes in-situ. They have been mostly applied to biological purposes. Among those, spatial light interference microscopy (SLIM), offers a very good robustness with minimal post acquisition data processing. In this paper, we report on using SLIM to measure fs-laser induced refractive index changes in different common glassy materials, such as fused silica and borofloat glass (B33). The advantages of SLIM over classical phase-contrast microscopy are discussed.
Ultrashort pulses lasers are tools of choice for functionalizing the bulk of transparent materials. In particular, direct photoinscription of simple photonic functions have been demonstrated. Those elementary functions rely on the local refractive index change induced when focusing an ultrashort pulse in the volume of a transparent material. The range of possibilities offered by direct photoinscription is still under investigation. To help understanding, optimizing and assessing the full potential of this method, we developed a time-resolved phase contrast microscopy setup. The imaginary part (absorption) and the real part of the laser-induced complex refractive index can be visualized in the irradiated region. The setup is based on a commercially available phase contrast microscope extended into a pump-probe scheme. The originality of our approach is that the illumination is performed by using a pulsed laser source (i.e. a probe beam). Speckle-related issues are solved by employing adequate sets of diffusers. This laser-microscopy technique has a spatial resolution of 650 nm, and the impulse response is about 300 fs. The laser-induced refractive index changes can be tracked up to milliseconds after the energy deposition. The excitation beam (the pump) is focused with a microscope objective (numerical aperture of 0.45) into the bulk of an a-SiO2 sample. The pump beam can be temporally shaped with a SLM-based pulse shaping unit. This additional degree of flexibility allows for observing different interaction regimes. For instance, bulk material processing with femtosecond and picosecond duration pulses will be studied.
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.
In this work, glasses with systematically varied compositions were manufactured and irradiated by single Ti:sapphire fs-laserpulses (800 nm, 120 fs), focused at the surface and into the bulk of the glass materials. The samples were tested for their ablation threshold fluence as well as for structural changes using µ-Raman-spectroscopy. Correlations between the glass composition, the material-ablation on the glass surface and the permanent changes of the refractive index inside the glass volume after the irradiation by fs-laser pulses were obtained. The results show, that the structural modifications found at the surface of the glasses and inside its volume are closely related. However, while the ablation threshold fluence of the glass surface primarily depends on the glass dissociation energy, the permanent refractive index change inside the volume is rather determined by its ability for absorbing the fs-laser pulses and the subsequent relaxation processes. The results of this work provide some guidance on how the glass composition can be varied in order to optimize the fs-laser induced modification of dielectrics.