Ablation of bulk chalcogenide glass As₂Se₃ by high-repetition-rate femtosecond laser pulses

   Femtosecond laser processing of chalcogenide glasses is a promising method for high-precision modification of their structure and properties for the development of optical elements for infrared photonics. One of the key challenges is to increase the processing speed while maintaining high spatial accuracy and minimal thermal damage. When using laser irradiation modes with a high pulse repetition rate, which ensures increased productivity of technologies, the mechanisms of phase-chemical transformations change and the contribution of accumulative heating increases. However, the dynamics of these processes in bulk material remains insufficiently studied. This paper studies the mechanism of phase and chemical composition transformation of As₂Se₃ bulk chalcogenide glass under the action of femtosecond laser pulses in the intense ablation modes.

   The objects of study are plates of chalcogenide glass As₂Se₃ irradiated by femtosecond laser pulses with a wavelength of 515 nm at repetition rates up to 1 MHz.

   The irradiated samples are analyzed using digital optical microscopy and Raman spectroscopy. Theoretical analysis includes both calculations of photoexcitation and heating of the semiconductor by a single laser pulse as well as calculations of accumulative heating of the sample surface, taking into account three-dimensional heat removal. The single-pulse laser ablation threshold was established at a laser pulse repetition rate of 1 kHz and the parameters of the power-law dependence of the ablation threshold on the number of pulses (incubation effect) were determined. A detailed analysis of the morphology of the irradiated samples and the chemical composition of the laser ablation products was carried out revealing the formation of amorphous selenium (a-Se) and arsenolite crystals (As₂O₃). Theoretical analysis allowed us to estimate the degree of heating and photoexcitation of As₂Se₃ chalcogenide glass by a single laser pulse and revealed a significant contribution of the heat accumulation effect to the surface temperature rise at a pulse repetition rate of 1 MHz. Based on the combined experimental and theoretical results obtained, a vapor-phase mechanism of phase and chemical transformation in As₂Se₃ bulk glass has been established during femtosecond laser ablation with a pulse repetition rate of 1 MHz. These findings open up prospects for the development of high-performance technologies for femtosecond laser microstructuring of chalcogenide materials in photonics and sensing applications.

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