Ultrafast laser-induced refractive index changes in Ge_15As_15S_70 chalcogenide glass

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Understanding and controlling laser-induced refractive index modifications in bulk chalcogenide glasses is important for a range of photonics applications targeting the mid-infrared spectral region. We focus here on material engineering aspects and pulse spatio-temporal design characteristics that are able to induce and maintain positive refractive index changes in laser-irradiated Sulfur-based chalcogenide glass, mandatory for 3D photonic design. Specifically we study the photoinscription process of a Ge-doped Sulfur-based chalcogenide glass, Ge15As15S70, irradiated by focused ultrafast near-infrared laser pulses where Ge doping plays a determinant role in generating high-contrast positive index changes. By means of aposteriori and real-time in situ observations we show that positive refractive index changes (type I) are the result of a restructuring of the glass matrix and a photo-induced contraction process initiated by two-photon electronic excitation leading to bond softening, molecular mobility, structural changes and rearrangements. Oppositely, negative refractive index changes (type II) could be associated with two different processes: photo-expansion at higher intensities and hydrodynamic evolution initiated by plasma generation and laser heating, with thermomechanical relaxation and stress unload. Alongside the role of Ge in setting various degrees of the matrix connectivity, the structural arrangement developed under different thermal history schemes for glass preparation is equally important as it defines to which extent further structural flexibility is possible. Thus we indicate the role of glass matrix metastability in generated high-contrast refractive index changes and we show that a higher degree of relaxation is an impediment for contrasted positive index changes, while these are developing in unrelaxed glasses, where several degrees of structural flexibility exist. Alongside dynamic time-resolved imaging experiments probing the development and relaxation of excitation, we also show, via static Raman analysis of the modified regions, that significant structural changes are induced by laser irradiation and we discuss the potential processes involved.