Stimulated Raman Adiabatic Passage (STIRAP) as a Route to Achieving Optical Control in Plasmonics

Optical properties of ensembles of three-level quantum emitters coupled to plasmonic systems are investigated employing a self-consistent model. It is shown that stimulated Raman adiabatic passage (STIRAP) technique can be successfully adopted to control optical properties of hybrid materials with collective effects present and playing an important role in light-matter interactions. We consider a core-shell nanowire comprised of a silver core and a shell of coupled quantum emitters and utilize STIRAP scheme to control scattering efficiency of such a system in a frequency and spatial dependent manner. After the STIRAP induced population transfer to the final state takes place, the core-shell nanowire exhibits two sets of Rabi splittings with Fano lineshapes indicating strong interactions between two different atomic transitions driven by plasmon near-fields.Comment: 11 pages, 6 figures, accepted, Physical Review

On the Experimental Estimation of Surface Enhanced Raman Scattering (SERS) Cross Sections by Vibrational Pumping

We present an in-depth analysis of the experimental estimation of cross sections in Surface Enhanced Raman Scattering (SERS) by vibrational pumping. The paper highlights the advantages and disadvantages of the technique, pinpoints the main aspects and limitations, and provides the underlying physical concepts to interpret the experimental results. Examples for several commonly used SERS probes are given, and a discussion on future possible developments is also presented.Comment: To be submitted to J. Phys. Chem.

Enhancement factor distribution around a single SERS Hot-spot and its relation to Single Molecule detection

We provide the theoretical framework to understand the phenomenology and statistics of single-molecule (SM) signals arising in Surface-Enhanced Raman Scattering (SERS) under the presence of so-called electromagnetic hot-spots (HS's). We show that most characteristics of the SM-SERS phenomenon can be tracked down to the presence of tail-like (power law) distribution of enhancements and we propose a specific model for it. We analyze, in the light of this, the phenomenology of SM-SERS and show how the different experimental manifestations of the effect reported in the literature can be analyzed and understood under a unified ``universal'' framework with a minimum set of parameters.Comment: 13 pages, 4 figures, submitted to J. Chem. Phy

Surface plasmon lifetime in metal nanoshells

The lifetime of localized surface plasmon plays an important role in many aspects of plasmonics and its applications. In small metal nanostructures, the dominant mechanism restricting plasmon lifetime is size-dependent Landau damping. We performed quantum-mechanical calculations of Landau damping for the bright surface plasmon mode in a metal nanoshell. In contrast to the conventional model based on the electron surface scattering, we found that the damping rate decreases as the nanoshell thickness is reduced. The origin of this behavior is traced to the spatial distribution of plasmon local field inside the metal shell. We also found that, due to interference of electron scattering amplitudes from nanoshell's two metal surfaces, the damping rate exhibits pronounced quantum beats with changing shell thickness.Comment: 9 pages, 4 Figure