Metal Nanoparticle Ensembles: Tunable Laser Pulses Distinguish Monomer from Dimer Vibrations

Resonant interaction of laser pulses with plasmons is used to identify vibrations associated with isolated spheres and pairs of contacting spheres in a system of gold nanoparticles. The optical pulses generate coherent mechanical oscillations of both monomers and dimers in the 5–150 GHz range, the amplitudes of which exhibit a strong enhancement when the laser central wavelength is tuned to resonate with the corresponding plasmon. Because of the resonant selection in the excitation process, the widths of the acoustic modes are significantly smaller than broadening caused by the spread in radii in the ensemble.