Signatures of Small Morphological Anisotropies in the Plasmonic and Vibrational Responses of Individual Nano-objects.

The plasmonic and vibrational properties of single gold nanodisks patterned on a sapphire substrate are investigated via spatial modulation and pump-probe optical spectroscopies. The features of the measured extinction spectra and time-resolved signals are highly sensitive to minute deviations of the nanodisk morphology from a perfectly cylindrical one. An elliptical nanodisk section, as compared to a circular one, lifts the degeneracy of the two nanodisk in-plane dipolar surface plasmon resonances, which can be selectively excited by controlling the polarization of the incident light. This splitting effect, whose amplitude increases with nanodisk ellipticity, correlates with the detection of additional vibrational modes in the context of time-resolved spectroscopy. Analysis of the measurements is performed through the combination of optical and acoustic numerical models. This allows us first to estimate the dimensions of the investigated nanodisks from their plasmonic response and then to compare the measured and computed frequencies of their detectable vibrational modes, which are found to be in excellent agreement. This study demonstrates that single-particle optical spectroscopies are able to provide access to fine morphological characteristics, representing in this case a valuable alternative to traditional techniques aimed at postfabrication inspection of subwavelength nanodevice morphology.