Ultrafast laser-induced modification of optical glasses : a spectroscopy insight into the microscopic mechanisms

2012 
Local refractive index changes (RIC) are the building blocks of laser-induced optical functions in bulk transparent materials, where the use of a fused silica as a target material plays a paramount role. Depending on the regime of laser interaction ultra-short pulses can induce positive isotropic refractive index changes (usually denoted as type I) or produce self-arranged nano-scale layered structures resulting in form birefringence (type II). In this thesis we have studied two objectives related to these material transformations. From the one side, we qualitatively determined the effects of the focused ultra-short laser pulses on the fused silica and borosilicate glasses. With the independent control of the energetic dose, pulse duration and focusing conditions, the isotropic type I and birefringent type II traces could be performed with the certain optical properties. Finally, complex polarization sensitive devices were designed and fabricated. From the other side, as these types of RIC have consequences in the functionality and the performances of 3D embedded optical devices, an investigation of the laser-induced structures is particularly useful. We applied photoluminescence and Raman microscopy (RM) to investigate defect formation and glass network reorganization paths. The proposed spectroscopy study distinguishes type I and type II regions by presence and distribution of silicon clusters and non-bridging oxygen hole centers (NBOHC). RM reveals signs of compaction of the glass network in the RIC regions. At the same time, zones with high concentration of NBOHC where no visible RIC and densification signs were detected. Assuming that these zones are precursors of permanent visible modification, we propose a scenario of cold defect-assisted densification realized in type I irradiation regime. This, thereby, revises the densification paths in fused silica
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