Single vs. multimode laser beams have been compared for laser ablation on steel samples. Laser plasma properties and analytical capabilities (precision, limit of detection) were used as key parameters for comparison. Peak fluence at focal spot has been observed to be higher for Gaussian beam despite ~14-fold lower pulse energy. A comparison of Gaussian and multimode beams with equal energy was carried out in order to estimate influence of beam profile only. Single mode lasing (Gaussian beam) results in better reproducibility of analytical signals compared to multimode lasing while laser energy reproducibility was the same for both cases. Precision improvements were attributed to more stable laser ablation due to better reproducibility of beam profile fluence at laser spot. Plasma temperature and electron density were higher for Gaussian laser beam. Calibration curves were obtained for four elements under study (Cr, Mn, Si, Cu). Two sampling (drilling and scanning procedures) and two optical detection schemes (side-view and optical fiber) were used to compare Gaussian and multimode beam profile influence on analytical capabilities of LIBS. We have found that multimode beam sampling was strongly influenced by surface effects (impurities, defects etc.). For all sampling and detection schemes, better precision was obtained if Gaussian beam was used for sampling. In case of single-spot sampling better limits of detection were achieved for multimode beam. If laser sources have same wavelength and equal energy than quality of laser beam became a crucial parameter which determined plasma properties and analytical capabilities of LIBS.
The ultrashort-laser photoexcitation and structural modification of buried atomistic optical impurity centers in crystalline diamonds are the key enabling processes in the fabrication of ultrasensitive robust spectroscopic probes of electrical, magnetic, stress, temperature fields, and single-photon nanophotonic devices, as well as in “stealth” luminescent nano/microscale encoding in natural diamonds for their commercial tracing. Despite recent remarkable advances in ultrashort-laser predetermined generation of primitive optical centers in diamonds even on the single-center level, the underlying multi-scale basic processes, rather similar to other semiconductors and dielectrics, are almost uncovered due to the multitude of the involved multi-scale ultrafast and spatially inhomogeneous optical, electronic, thermal, and structural elementary events. We enlighten non-linear wavelength-, polarization-, intensity-, pulsewidth-, and focusing-dependent photoexcitation and energy deposition mechanisms in diamonds, coupled to the propagation of ultrashort laser pulses and ultrafast off-focus energy transport by electron–hole plasma, transient plasma- and hot-phonon-induced stress generation and the resulting variety of diverse structural atomistic modifications in the diamond lattice. Our findings pave the way for new forthcoming groundbreaking experiments and comprehensive enlightening two-temperature and/or atomistic modeling both in diamonds and other semiconductor/dielectric materials, as well as innovative technological breakthroughs in the field of single-photon source fabrication and “stealth” luminescent nano/microencoding in bulk diamonds for their commercial tracing.
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