Pulsed laser postprocessing (PLPP) of colloidal nanoparticles and related laser fragmentation in liquid (LFL) using a liquid jet setup have become an acknowledged tool to reduce the nanoparticle diameter down to a few nanometers, alter the crystal phase, or increase the defect density under high-purity and continuous-flow conditions. In recent studies on LFL that were conducted with a cylindrical liquid jet, intensity gradients and related incomplete illumination of the volume element passing through the laser beam path were reported to cause a broadening of the product particle size distribution, melting, and phase segregation. In this paper, we present a new flat jet design, which reduces the deviation of the laser intensity up to 10 times compared to the conventional cylindrical liquid jet. The experimental threshold intensity for gold nanoparticle fragmentation found with the cylindrical setup strongly deviates from the theoretical prediction, while they are in very good agreement for the flat jet setup. Additionally, a narrow product size fraction of 3 ± 2 nm was found for the flat jet, while the main product fraction gained from the cylindrical jet was 10 ± 8 nm in size under the same conditions. Consequently, the flat jet setup allows us not only to study laser fragmentation mechanisms with higher precision but also to gain product particles with narrow particle size distribution at single pulse per particle conditions even at elevated mass concentrations (>50 mg L). In future studies, these promising results also render the flat jet setup relevant for the other disciplines of PLPP such as laser melting and defect engineering.
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http://dx.doi.org/10.1021/acs.jpca.0c08787 | DOI Listing |
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