| Summary: | The changes that appeared in the crystal structure of a natural diamond under the influence of a pulsed femtosecond laser (525 nm) were comprehensively investigated using Fourier-transform infrared (FT-IR), electron paramagnetic resonance (EPR), and photoluminescence (PL) spectroscopy methods. It is shown that changes in the crystal structure occur due to the laser-driven interrelated process of the appearance and migration of interstitial carbon atoms and vacancies. On the one hand, there are atomistic transformations related to a decrease in the concentrations of structural centers that are not associated with vacancies or interstitial atoms—centers A (FT-IR spectroscopy) and P1 and W7 (EPR)—and an increase in the concentration of the H3, NV<sup>0</sup>, and NV<sup>−</sup> (PL) centers, which are associated with vacancies. On the other hand, there are indications of cooperative effects—an increase in the intensity of multi-atomic B2 (platelets, layers of interstitial carbon atoms (FT-IR)) and N2 (fragments of the structure with broken C–C bonds (EPR)) centers.
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