Optically Controlled Stochastic Jumps of Individual Gold Nanorod Rotary Motors

Brownian microparticles diffusing in optical potential energy landscapes constitute a generic testbed for nonequilibrium statistical thermodynamics and has been used to emulate a wide variety of physical systems, ranging from Josephson junctions to Stirling engines. Here we demonstrate that it is possible to scale down this approach to nanometric length-scales by constructing a tilted washboard potential for the rotation of plasmonic gold nanorods. The potential depth and tilt can be precisely adjusted by modulating the light polarization. This allows for a gradual transition from continuous rotation to discrete stochastic jumps, which are found to follow Kramers dynamics in excellent agreement with stochastic simulations. The results widen the possibilities for fundamental experiments in statistical physics and provide new insights in how to construct light-driven nanomachines and multifunctional sensing elements.Comment: 6 pages, 4 figure

Schottky barrier formation and band bending revealed by first principles calculations

An atomistic insight into potential barrier formation and band bending at the interface between a metal and an n-type semiconductor is achieved by ab initio simulations and model analysis of a prototype Schottky diode, i.e., niobium doped rutile titania in contact with gold (Au/Nb:TiO$_2$). The local Schottky barrier height is found to vary between 0 and 1.26 eV depending on the position of the dopant. The band bending is caused by a dopant induced dipole field between the interface and the dopant site, whereas the pristine Au/TiO$_2$ interface does not show any band bending. These findings open the possibility for atomic scale optimization of the Schottky barrier and light harvesting in metal-semiconductor nanostructures

Sensing (un)binding events via surface plasmons: Effects of resonator geometry

The resonance conditions of localized surface plasmon resonances (LSPRs) can be perturbed in any number ways making plasmon nanoresonators viable tools in detection of e.g. phase changes, pH, gasses, and single molecules. Precise measurement via LSPR of molecular concentrations hinge on the ability to confidently count the number of molecules attached to a metal resonator and ideally to track binding and unbinding events in real-time. These two requirements make it necessary to rigorously quantify relations between the number of bound molecules and response of plasmonic sensors. This endeavor is hindered on the one hand by a spatially varying response of a given plasmonic nanosensor. On the other hand movement of molecules is determined by stochastic effects (Brownian motion) as well as deterministic flow, if present, in microfluidic channels. The combination of molecular dynamics and the electromagnetic response of the LSPR yield an uncertainty which is little understood and whose effect is often disregarded in quantitative sensing experiments. Using a combination of electromagnetic finite-difference time-domain (FDTD) calculations of the plasmon resonance peak shift of various metal nanosensors (disk, cone, rod, dimer) and stochastic diffusion-reaction simulations of biomolecular interactions on a sensor surface we clarify the interplay between position dependent binding probability and inhomogeneous sensitivity distribution. We show, how the statistical characteristics of the total signal upon molecular binding are determined. The proposed methodology is, in general, applicable to any sensor and any transduction mechanism, although the specifics of implementation will vary depending on circumstances. In this work we focus on elucidating how the interplay between electromagnetic and stochastic effects impacts the feasibility of employing particular shapes of plasmonic sensors for real-time monitoring of individual binding reactions or sensing low concentrations - which characteristics make a given sensor optimal for a given task. We also address the issue of how particular illumination conditions affect the level of uncertainty of the measured signal upon molecular binding

Realizing strong light-matter interactions between single nanoparticle plasmons and molecular excitons at ambient conditions

Realizing strong light-matter interactions between individual 2-level systems and resonating cavities in atomic and solid state systems opens up possibilities to study optical nonlinearities on a single photon level, which can be useful for future quantum information processing networks. However, these efforts have been hampered by the unfavorable experimental conditions, such as cryogenic temperatures and ultrahigh vacuum, required to study such systems and phenomena. Although several attempts to realize strong light-matter interactions at room-temperature using so-called plasmon resonances have been made, successful realizations on the single nanoparticle level are still lacking. Here, we demonstrate strong coupling between plasmons confined within a single silver nanoprism and excitons in molecular J-aggregates at ambient conditions. Our findings show that the deep subwavelength mode volumes, $V$, together with high quality factors, $Q$, associated with plasmons in the nanoprisms result in strong coupling figure-of-merit -- $Q/\sqrt{V}$ as high as $\sim6\times10^{3}$~$\mu$m$^{-3/2}$ -- a value comparable to state-of-art photonic crystal and microring resonator cavities, thereby suggesting that plasmonic nanocavities and specifically silver nanoprisms can be used for room-temperature quantum optics

Mode-specific directional emission from hybridized particle-on-a-film plasmons

We investigate the electromagnetic interaction between a gold nanoparticle and a thin gold film on a glass substrate. The coupling between the particle plasmons and the surface plasmon polaritons of the film leads to the formation of two localized hybrid modes, one low-energy. film-like. plasmon and one high-energy plasmon dominated by the nanoparticle. We find that the two modes have completely different directional scattering patterns on the glass side of the film. The high-energy mode displays a characteristic dipole emission pattern while the low-energy mode sends out a substantial part of its radiation in directions parallel to the particle dipole moment. The relative strength of the two radiation patterns vary strongly with the distance between the particle and the film, as determined by the degree of particle-film hybridization

A combination of concave/convex surfaces for field-enhancement optimization: the indented nanocone

We introduce a design strategy to maximize the Near Field (NF) enhancement near plasmonic antennas. We start by identifying and studying the basic electromagnetic effects that contribute to the electric near field enhancement. Next, we show how the concatenation of a convex and a concave surface allows merging all the effects on a single, continuous nanoantenna. As an example of this NF maximization strategy, we engineer a nanostructure, the indented nanocone. This structure, combines all the studied NF maximization effects with a synergistic boost provided by a Fano-like interference effect activated by the presence of the concave surface. As a result, the antenna exhibits a NF amplitude enhancement of ∼ 800, which transforms into ∼1600 when coupled to a perfect metallic surface. This strong enhancement makes the proposed structure a robust candidate to be used in field enhancement based technologies. Further elaborations of the concept may produce even larger and more effective enhancements.This work was supported by the Etortek-2011 project nanoiker of the Department of Industry of the Basque Government, project FIS2010-19609-C02-01 of the Spanish Ministry of Science and Innovation and the Swedish Foundation for Strategic Research through the project RMA08 Functional Electromagnetic Metamaterials.Peer Reviewe

Coloring fluorescence emission with silver nanowires

We demonstrate that emission from Rhodamine-6G fluorophores adsorbed on silver nanowires experiences a spectral redshift upon propagation to the distal ends of the nanowire, with the shift being proportional to the propagation distance. The end of a nanowire thus constitutes a tunable fluorescence source controlled by a single easily adjustable parameter, i.e., the position of the excitation focal spot. The effect is made possible by a combination of radiatively undamped plasmon propagation and dispersive ohmic losses in the silver nanowire. The results may be important for the development of plasmonic waveguides, fast fluorescent color switches and various nanoscale fluorescence sensors. (C) 2010 American Institute of Physics. [doi: 10.1063/1.3355545

Symmetry-dependent screening of surface plasmons in ultrathin supported films: The case of Al/Si(111)

A joint theoretical and experimental study of plasmon excitations for Al overlayers on Si(111) has been carried out. The presence of the substrate is found to drastically modify the hybridization and charge density response of the surface plasmons of the metal overlayers. The symmetric mode, which is polarized toward the Al/Si interface, is strongly damped in intensity and significantly redshifted in energy. However, the antisymmetric mode, which is polarized to the metal-vacuum interface, is essentially unaffected by the presence of the substrate. A low-energy acoustic plasmon mode is also found in a one monolayer Al film and is almost unaffected by the substrate. The calculated plasmon dispersions with substrate are in good agreement with experimental data measured by electron energy loss spectroscopy. Our results suggest that interaction and screening at the subnanometer scale are symmetry dependent, a conclusion that may have general implications in other thin films and related structures

Intrinsic Fano Interference of Localized Plasmons in Pd Nanoparticles

Palladium (Pd) nanoparticles exhibit broad optical resonances that have been assigned to so-called localized surface plasmons (LSPs). The resonance's energy varies with particle shape in a similar fashion as is well known for LSPs in gold and silver nanoparticles, but the line-shape is always anomalously asymmetric. We here show that this effect is due to an intrinsic Fano interference caused by the coupling between the plasmon response and a structureless background originating from interband transitions. The conclusions are supported by experimental and numerical simulation data of Pd particles of different shape and phenomenologically analyzed in terms of the point dipole polarizability of spheroids. The latter analysis indicates that the degree of Fano asymmetry is simply linearly proportional to the imaginary part of the interband contribution to the metal dielectric function

Comparative study of plasmonic antennas for strong coupling and quantum nonlinearities with single emitters

Realizing strong coupling between a single quantum emitter (QE) and an optical cavity is of crucial importance in the context of various quantum optical applications. While Rabi splitting of single quantum emitters coupled to high-Q diffraction limited cavities have been reported in numerous configurations, attaining single emitter Rabi splitting with a plasmonic nanostructure is still elusive. Here, we establish the analytical condition for strong coupling between a single QE and a plasmonic nanocavity and apply it to study various plasmonic arrangements that were shown to enable Rabi splitting. We investigate numerically the optical response and the resulting Rabi splitting in metallic nanostructures such as bow-tie nanoantennas, nanosphere dimers and nanospheres on a surface and find the optimal geometries for emergence of the strong coupling regime with single QEs. We also provide a master equation approach to show the saturation of a single QE in the gap of a silver bow-tie nanoantenna. Our results will be useful for implementation of realistic quantum plasmonic nanosystems involving single QEs.Comment: 9 pages, 7 figure