Solution and displacement in monolayer and multilayer binary films of SF6 and CF4 on graphite.

Infrared reflection absorption spectroscopy is used to study the evolution of binary physisorbed films on graphite. A predeposited monolayer of SF6 is exposed to slowly increasing pressure of CF4 at constant temperature between 80 and 113 K. Shifts in the frequencies of the dominant vibrational mode of each species due to resonant dipole-dipole coupling serve as proxies for the areal density of each species in the monolayer. If the initial SF6 film is far below saturation (coexistence with bulk solid), the SF6 can be largely displaced by continuous solution of CF4. However, if the initial SF6 layer is at or near saturation, a layer of CF4 condenses on top at a well defined CF4 pressure after only 2%-3% dilution of the SF6 layer. Simultaneously, most of the dissolved CF4 is withdrawn from the SF6 layer. With further increase in CF4 pressure, the CF4 layer is compressed and additional layers condense, while the SF6 layer is again diluted. Still, the SF6 layer retains about 90% concentration until the CF4 pressure is very close to saturation, at which point the SF6 is rapidly displaced, apparently going into dilute solution in the rapidly growing CF4 multilayer. Monte Carlo simulations are used to quantitatively relate measured frequency shifts to concentrations in the binary monolayer.

Effect of vector asymmetry of radially polarized beams in solid immersion microscopy.

We theoretically and experimentally investigate the effect of imperfect vector symmetry on radially polarized beams focused by an aplanatic solid immersion lens at a numerical aperture of 3.3. We experimentally achieve circularly symmetric focused spot with a full-width-half-maximum of ~λ0/5.7 at λ0 = 1,310 nm, free-space wavelength. The tight spatial confinement and overall circular symmetry of the focused radially polarized beam are found to be sensitive to perturbations of its cylindrical polarization symmetry. The addition of a liquid crystal based variable retarder to the optical path can effectively ensure the vector symmetry and achieve circularly symmetric focused spots at such high numerical aperture conditions.

Radially polarized Bessel-Gauss beams: decentered Gaussian beam analysis and experimental verification.

We derive solutions for radially polarized Bessel-Gauss beams in free-space by superimposing decentered Gaussian beams with differing polarization states. We numerically show that the analytical result is applicable even for large semi-aperture angles, and we experimentally confirm the analytical expression by employing a fiber-based mode-converter.

Structure of plasmonic aerogel and the breakdown of the effective medium approximation.

A method for making aerogel doped with gold nanoparticles (GNPs) produces a composite material with a well-defined localized surface plasmon resonance peak at 520 nm. The width of the extinction feature indicates the GNPs are well dispersed in the aerogel, making it suited to optical study. A simple effective medium approximation cannot explain the peak extinction wavelengths. The plasmonic field extends on a scale where aerogel cannot be considered isotropic, so a new model is required: a 5 nm glass coating on the GNPs models the extinction spectrum of the composite material, with air (aerogel), methanol (alcogel), or toluene filling the pores.

Large-core acetylene-filled photonic microcells made by tapering a hollow-core photonic crystal fiber.

We report on kagomé-lattice photonic microcells with low losses, large outer diameters, and large cores. The large (40-70microm) cores are accommodated by tapering the fibers and splicing the reduced ends to a single-mode fiber. We demonstrate the repeatability of this process and obtain splice losses of 0.6dB by optimizing the taper transition length. Narrow electromagnetically induced transparencies and saturable absorption are demonstrated in an acetylene-filled photonic microcell.

Tapered fibers embedded in silica aerogel.

We have embedded thin tapered fibers (with diameters down to 1 microm) in silica aerogel with low loss. The aerogel is rigid but behaves refractively like air, protecting the taper without disturbing light propagation along it. This enables a new class of fiber devices exploiting volume evanescent interactions with the aerogel itself or with dopants or gases in the pores.

Emission and nonradiative decay of nanodiamond NV centers in a low refractive index environment.

The nitrogen vacancy (NV) center is the most widely studied single optical defect in diamond with great potential for applications in quantum technologies. Development of practical single-photon devices requires an understanding of the emission under a range of conditions and environments. In this work, we study the properties of a single NV center in nanodiamonds embedded in an air-like silica aerogel environment which provides a new domain for probing the emission behavior of NV centers in nanoscale environments. In this arrangement, the emission rate is governed primarily by the diamond crystal lattice with negligible contribution from the surrounding environment. This is in contrast to the conventional approach of studying nanodiamonds on a glass coverslip. We observe an increase in the mean lifetime due to the absence of a dielectric interface near the emitting dipoles and a distribution arising from the irregularities in the nanodiamond geometry. Our approach results in the estimation of the mean quantum efficiency (~0.7) of the nanodiamond NV emitters.

Porous silicon nanocrystals in a silica aerogel matrix.

Silicon nanoparticles of three types (oxide-terminated silicon nanospheres, micron-sized hydrogen-terminated porous silicon grains and micron-size oxide-terminated porous silicon grains) were incorporated into silica aerogels at the gel preparation stage. Samples with a wide range of concentrations were prepared, resulting in aerogels that were translucent (but weakly coloured) through to completely opaque for visible light over sample thicknesses of several millimetres. The photoluminescence of these composite materials and of silica aerogel without silicon inclusions was studied in vacuum and in the presence of molecular oxygen in order to determine whether there is any evidence for non-radiative energy transfer from the silicon triplet exciton state to molecular oxygen adsorbed at the silicon surface. No sensitivity to oxygen was observed from the nanoparticles which had partially H-terminated surfaces before incorporation, and so we conclude that the silicon surface has become substantially oxidised. Finally, the FTIR and Raman scattering spectra of the composites were studied in order to establish the presence of crystalline silicon; by taking the ratio of intensities of the silicon and aerogel Raman bands, we were able to obtain a quantitative measure of the silicon nanoparticle concentration independent of the degree of optical attenuation.