Modification of metal nanoparticles with laser light has been a well-known technique for several years. Still, selective tailoring of certain sizes or shapes of nanoparticles has remained a challenge. In this paper, we present recent studies on tailoring the size and shape of supported nanoparticles with continuous-wave and femtosecond
pulsed laser light and compare them to our results obtained with ns pulsed laser light. The underlying method is based on the size and shape dependent plasmon resonance frequencies of the nanoparticles. In principle, irradiation with a given laser photon energy excites and heats nanoparticles of certain sizes or/and shapes and leads to diffusion and evaporation of surface atoms. Thus, tailoring the dimensions of the nanoparticles can be accomplished. In our experiments, gold and silver nanoparticles were prepared under ultrahigh vacuum conditions by deposition of atoms and subsequent diffusion and nucleation, i.e. Volmer-Weber growth. This gives particle ensembles with size and shape distributions of approximately 30% - 40%. The nanoparticle ensembles were irradiated with laser light either during or after growth. It turns out, that irradiation with cw or ns laser light makes possible selective modification of the nanoparticles. In contrast, application of fs laser pulses results in non-selective modification. For example, post-grown irradiation of supported gold nanoparticles with ns laser pulses (photon energy = 1.9 eV) causes a clear reduction of the width of the surface plasmon resonance from 0.52 eV to 0.20 eV (HWHM). Similar experiments were carried out with fs pulsed laser light (photon energy = 1.55 eV), which result in a slightly reduced line width but also, to an overall decrease of the extinction. A
comparison of all experiments revealed, that for size or shape tailoring of supported metal nanoparticles best results have been achieved with ns pulsed laser light.
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