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Controlling the Pulsed-Laser-Induced Size Reduction of Au and Ag Nanoparticles via Changes in the External Pressure, Laser Intensity, and Excitation Wavelength

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Department of Optical Science and Technology, The University of Tokushima, Tokushima 770-8506, Japan
Cite this: Langmuir 2013, 29, 4, 1295–1302
Publication Date (Web):December 21, 2012
Copyright © 2012 American Chemical Society

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    The laser-induced size reduction of aqueous noble metal nanoparticles has been the subject of intensive research, because of the mechanistic interest in the light–nanoparticle interactions and its potential application to size control. The photothermal evaporation hypothesis has gained solid support. However, the polydispersity of the final products is considered as an inherent drawback of the method. It is likely that the polydispersity arises from the uncontrolled heat dissipation caused by vapor bubble formation in the ambient atmosphere. To overcome this problem, we applied high pressures of 30–100 MPa. The particle size was regulated by adjusting three parameters: the pressure, laser intensity, and excitation wavelength. For example, starting from a colloidal solution of 100 nm diameter gold nanoparticles, highly monodisperse (±3–5%) spheres with various diameters ranging from 90 to 30 nm were fabricated by tuning the laser intensity at 100 MPa, using an excitation wavelength of 532 nm. Further size reduction of the diameter to 20 nm was achieved by reducing the pressure and switching the excitation wavelength to 355 nm. It was found that the application of high pressures led to the heat loss-controlled size-reduction of the gold nanoparticles. More complicated results were obtained for 100 nm silver nanoparticles, possibly because of the different size-dependent light-absorbing nature of these particles. Based on our extensive experimental studies, a detailed picture was developed for the nanosecond laser-induced fabrication of gold and silver nanoparticles, leading to unprecedented size control.

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    Particle images (TEM micrographs) and corresponding size distribution of 100 nm Au NPs, extinction spectra of 100 nm Au NPs after laser irradiation, particle images (TEM micrographs) and corresponding size distributions after laser irradiation at 0.1 MPa, particle images and corresponding histograms for Au NPs prepared at 60 MPa, changes in the extinction spectra for ≈100 nm diameter Ag NPs after laser irradiation at 60 MPa, particle images (TEM micrographs), absorption cross section spectra (Cabs) for Au NPs (d = 100, 80, 50 nm) in water, depending on the refractive index (n) of the medium and the particle temperature (n = 1.33), and particle images (TEM micrographs) and changes in the extinction spectra for Au NPs after centrifugation. This material is available free of charge via the Internet at

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    17. . Nanomaterials. 2021, 40-90.
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