The adsorption of a self-assembled monolayer of molecules on a metal surface commonly causes a red-shift in its surface plasmon resonance. We report that the anomalous dispersion of surface plasmons in a Au nanoslit array structure can cause a blue-shift of optical transmission upon adsorption of a non-absorbing self-assembled monolayer of molecules. We develop a simple model that explains the blue-shift observed in the transmission spectra with monolayer adsorption in terms of the interplay of anomalous dispersion and the cavity resonance of surface plasmons in the nanoslit array.
In this letter, we present a study of the condensation of exciton-polaritons in large etched pillar structures that exhibit shallow edge trapping. The ≈ 100 µm ×100 µm pillars were fabricated using photolithography and a BCl 3 /Cl 2 reactive ion etch. A low energy region emerged along the etched edge, with the minima ≈ 7 µm from the outer edge. The depth of the trap was 0.5 − 1.5 meV relative to the level central region, with the deepest trapping at the corners. We were able to produce a Bose-Einstein condensate in the trap near the edges and corners by pumping non-resonantly in the middle of the pillar. This condensate began as a set of disconnected condensates at various points along the edges, but then became a single mono-energetic condensate as the polariton density was increased. Similar edge traps could be used to produce shallow 1D traps along edges or other more complex traps using various etch geometries and scales.In the past two decades, many experiments have used polaritons resulting from strong coupling between trapped microcavity photons and quantum well (QW) excitons. These bosonic particles have a very light mass (∼ 10 −4 m e ) due to being partially photonic, but also strong particle-particle interactions from being partially excitonic.1 This combination of a light mass and strong interactions leads to the formation of Bose-Einstein condensates (BECs) at relatively high temperatures (∼ 10 K).2-4 Polaritons provide a promising system for studying bosonic particles at even higher temperatures, and polariton lasing has been observed at room temperature in both GaN 5 and organic 6 systems. Many methods of confinement have been used to study polariton dynamics in a variety of geometries. Applying stress to a thin (≈ 100 µm) GaAs sample can be used to shift the exciton energy, resulting in a harmonic trap. 4,7Pumping such a stress trap non-resonantly in the center forms a repulsive barrier and can be used to form a ring geometry.8 Complex pumping geometries can also be used to confine polaritons, including the use of two or more pump spots in various arrangements or using a ring-shaped pump spot.9-13 More permanent methods of confinement include producing a spacer in certain regions of the cavity during the growth process, 14-16 using sub-wavelength gratings as the top mirror, 17,18 depositing metal strips onto the top mirror, 19 and etching the sample after growth to form 1D wires, 2D pillars, and 2D arrays of coupled pillars. 20-25While optically induced trapping potentials have the advantage of being easily reconfigured, etched trapping allows the confinement to be somewhat independent of the pump laser. Post-growth etching also produces much higher potential barriers at the etched edges than the a) Electronic mail: dmm154@pitt.edu b) J. K. Wuenschell is now at Physical Sciences Laboratory, The Aerospace Corporation, El Segundo, CA 90245, USA deposition of metal strips, and it is compatible with our existing sample materials and growth methods, unlike sub-wavelength gratings or modulating the cavi...
We have chemically modified metal nanoslit array surfaces with alkanethiol self-assembled monolayers and have characterized the resulting spectral shift of optical transmission. Adsorption of a self-assembled monolayer ͑1.5 nm thick͒ on a silver nanoslit array ͑slit width of 30-50 nm and grating period of 360 nm͒ is found to cause an 11 nm redshift of the main transmission peak. Strong confinement of optical fields in the narrow slit region allows sensitive transduction of surface modification into a shift of surface plasmon resonance wavelength.
In GaAs/AlGaAs coupled quantum wells, strain-induced traps may be used to confine excitons in in-plane, harmonic traps. Using these traps, we have pursued Bose-Einstein condensation (BEC) of long-lived, spatially-indirect excitons. Here, we report a remarkable transition of the indirect exciton luminescence pattern with increasing strain, increasing exciton density, and decreasing temperature, to a spatial pattern exhibiting a large dark spot at trap center, where we expect the exciton density to be maximum. The mechanism of particle loss is ruled out as an explanation for this dark spot. While the onset criteria are approximately consistent with the conditions for BEC of a weakly interacting gas, the conspicuous proximity in energy of the indirect light-hole states suggests that an explanation employing the single-particle physics of light-hole/heavy-hole mixing may explain the phenomenon. The effect of the strain is modeled, and the resulting landscape of indirect exciton spin states is discussed. The relative oscillator strengths of these states are predicted by an exact numerical solution of the two-particle Schrodinger equation for electrons and holes in coupled quantum wells and an electric field. The contrast in oscillator strengths is sufficient to produce this luminescence pattern, but this analysis suggests a strongly diminished lifetime as stress is increased. The opposite lifetime dependence is observed experimentally. Additionally, the temperature dependence eludes explanation by this mechanism.
We present an analytical study of the dynamic interplay among surface plasmon polarization charges, electromagnetic fields, and energy flow in the metal/dielectric interface and metal nanoslit structure. Particular attention is given to the regime where the energy flow in the metal side is significant compared to that in the dielectric side. The study reveals that a vortex-like circulation of energy is an intrinsic feature of surface plasmon propagation supported by a metal/dielectric interface, and, in general, a vortex can form when the permittivity and permeability values of the materials involved satisfy the following condition: {(epsilon(m)/epsilon(d)) < -1 and (mu(m)/mu(d)) > -1} or {(epsilon(m)/epsilon(d)) > -1 and (mu(m)/mu(d)) < -1}.
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