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Ultrafast lasers pulses induced ablation of nickel-titanium (NiTi) alloy substrates immersed in deionized water yielded a high-throughput of polycrystalline core - amorphous shell NiTi nanoparticles (NPs) owing to the high pulse energy of femtosecond (fs) lasers. In this study, the alloy NPs were fabricated by varying the laser fluences from 15 to 45 J/cm2. The polycrystalline core - amorphous shell NiTi were confirmed by selected area diffraction patterns via High resolution - Transmission Electron microscopy. Theoretical investigations were carried out via hybrid simulation approach of molecular dynamics simulation and analytical modelling. Molecular dynamics study revealed the spatial and temporal evolution of electron and lattice temperature of NiTi melt pool due to ablation at various laser fluences. The subsequent temporal dynamics of melt-pool temperature along the depth revealed the phase separation via spinodal decomposition process after 40 picoseconds post irradiation of NiTi with ultrafast laser pulse. The analytical modelling incorporating phase explosion theory estimated the thermophysical expansion of ablated chunks and subsequent fragmentation of NiTi melt pool in liquid-vapor co-existing phase. The parameters of mathematical modelling were evaluated in-conjunction with the experimental results of size distribution of NPs at the laser fluence of 15 J/cm2. Later, the hybrid mathematical model was employed to predict the size of NiTi NPs ablated at higher laser fluences of 30 J/cm2 and 45 J/cm2 and the results were experimentally verified.
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