Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 122, Issue 38, Pages 22125-22136Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.8b04374
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Funding
- DFG Deutsche Forschungsgemeinschaft [BA 3580/22-1, PA 794/28-1]
- Alexander von Humboldt fellowship
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Laser-inducd fragmentation is a promising tool for controlling the particle size of ligand-free colloidal nanoparticles and to synthesize ligand-free gold nanoclusters. However, because the underlying mechanisms are not fully understood, increasing the yield of this process remains challenging. In this work, we examine the pulsed laser fragmentation of gold nanoparticles in liquid under statistical single-pulse conditions with high-fluence nanosecond pulses and correlate them with the educt particle size, number of pulses, and laser fluence. We conclusively prove that the fragmentation process of gold nanoparticles is a one-pulse and one-step event, which yields monomodal particles of << 10 nm down to 2.8 +/- 0.1 rim when exceeding a pulse peak power of 1.6 X 10(12) W/m(2) and when all educt particles are larger than 13.4 nm. This size threshold for quantitative fragmentation fits well with the size limit of 13.1 nm calculated with respect to the evaporation-heat-energy balance. Furthermore, we found strong evidence that the number of irradiation cycles, varied within the regime of one to four laser pulses/colloid volume, can be used to tune the surface chemistry and surface charge of the resulting nanoparticles in an aqueous medium.
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