The dephasing of particle plasmons is investigated using light-scattering spectroscopy on individual gold nanoparticles. We find a drastic reduction of the plasmon dephasing rate in nanorods as compared to small nanospheres due to a suppression of interband damping. The rods studied here also show very little radiation damping, due to their small volumes. These findings imply large local-field enhancement factors and relatively high light-scattering efficiencies, making metal nanorods extremely interesting for optical applications. Comparison with theory shows that pure dephasing and interface damping give negligible contributions to the total plasmon dephasing rate.
Using a near-field optical antenna effect, we measure the homogeneous line shape of the surface-plasmon resonance in single gold nanoparticles. The surface-plasmon dephasing times extracted from the near-field spectra of the individual particles vary around 8 fs. This mean value agrees with calculations based on Mie theory, which neglect surface effects. Deviations of individual particles from this value are interpreted as being due to variations in the local nanoenvironment. We also observe double-peaked line shapes caused by electromagnetic coupling between close-lying particles.
We report the study of optical dephazing of Wannier-Stark ladder excitations in a semiconductor superlattice by means of transient degenerate four-wave mixing. We observe pronounced modulations of the signal with a time period varying linearly with the electric field. The time period is found to equal the temporal periodicity of Bloch oscillations, in agreement with theory. In addition, we find that the dephazing time decreases with increasing localization of the Wannier-Stark states, which is attributed to carrier escape out of the lowest miniband.
Light emission at the particle plasmon frequency is observed in optically excited spherical gold nanoparticles. We find a photoluminescence efficiency of , which is essentially independent of particle size and four orders of magnitude higher than the efficiencies determined from metal films. Our experimental findings are explained with a process in which excited -band holes recombine nonradiatively with electrons, emitting particle plasmons. These plasmons subsequently radiate, giving rise to the photoluminescence observed in the experiment. We determine the quantum efficiencies involved in this process.
We have developed a simple, fast, and flexible technique to measure optical scattering spectra of individual metallic nanoparticles. The particles are placed in an evanescent field produced by total internal reflection of light from a halogen lamp in a glass prism. The light scattered by individual particles is collected using a conventional microscope and is spectrally analyzed by a nitrogen-cooled charge-coupled-device array coupled to a spectrometer. This technique is employed to measure the effect of particle diameter on the dephasing time of the particle plasmon resonance in gold nanoparticles. We also demonstrate the use of this technique for measurements in liquids, which is important for the potential application of particle plasmons in chemical or biological nanosensors.