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PubMed2006

Nonlinear absorption and nonlinear refraction of self-assembled porphyrins.

Nonlinear refraction and nonlinear absorption of self-assembled porphyrins in the nanosecond and picosecond regimes were studied at 532 nm by the Z-scan technique. First, a marked difference in nonlinear refraction was observed between self-assembled zinc porphyrins and free base porphyrins; however, the effects of self-assembly and metallization on nonlinear absorption are small. Second, an enhancement of nonlinear absorption was observed for the monomeric components of self-assembled structures by adding pyridine, while their nonlinear refractions remained almost unchanged as pyridine was added. It is expected that the metallization and addition of ligand can provide more convenient routes to alter the optical nonlinearities of porphyrins than the modifications of molecular structures of traditional covalent-bond organic materials.

Lasers↗
PubMed2006

Protic ionic liquids: solvents with tunable phase behavior and physicochemical properties.

The phase behavior, including glass, devitrification, solid crystal melting, and liquid boiling transitions, and physicochemical properties, including density, refractive index, viscosity, conductivity, and air-liquid surface tension, of a series of 25 protic ionic liquids and protic fused salts are presented along with structure-property comparisons. The protic fused salts were mostly liquid at room temperature, and many exhibited a glass transition occurring at low temperatures between -114 and -44 degrees C, and high fragility, with many having low viscosities, down to as low as 17 mPa.s at 25 degrees C, and ionic conductivities up to 43.8 S/cm at 25 degrees C. These protic solvents are easily prepared through the stoichiometric combination of a primary amine and Brønsted acid. They have poor ionic behavior when compared to the far more studied aprotic ionic liquids. However, some of the other physicochemical properties possessed by these solvents are highly promising and it is anticipated that these, or analogous protic solvents, will find applications beyond those already identified for aprotic ionic liquids. This series of protic fused salts was employed to determine the effect of structural changes on the physicochemical properties, including the effect of hydroxyl groups, increasing alkyl chain lengths, branching, and the differences between inorganic and organic anions. It was found that simple structural modifications provide a mechanism to manipulate, over a wide range, the temperature at which phase transitions occur and to specifically tailor physicochemical properties for potential end-use applications.

Amines↗
PubMed2004

Liquid crystalline gel with refractive index gradient of curdlan.

Curdlan dissolved in aqueous sodium hydroxide was dialyzed to aqueous calcium chloride to form a gel. Transparent and turbid concentric layers observed in the gel cross section perpendicular to the long axis of the dialysis tube were identified as liquid crystalline gels with refractive index gradient and amorphous gels, respectively. The thickness of each layer was proportional to the diameter of the dialysis tube, and the gelation proceeded in proportion to the root of time. The unique pattern formation was attributed to the change of curdlan conformation and calcium-induced cross-linking resulting from a diffusion of calcium cations and hydroxide anions through the dialysis tube. It is suggested that the orderedness of the curdlan molecules decreases by the increase of the curvature of the concentric liquid crystal layers as the layer comes toward the center of the dialysis tube.

Calcium Chloride↗
PubMed2005

Grafted self-assembled monolayers derived from naturally occurring phenolic lipids.

Self-assembled monolayers grafted onto silicon surfaces were obtained from the hydrosilylation products by trialcoxysilanes of naturally occurring phenolic lipid allyl ethers. The as-obtained materials were characterized by various physical and physicochemical methods. Thus, contact angles of water drops showed that they possess very high hydrophobicity. Their excellent regularity was corroborated by AFM microscopy. The frequencies of the stretching CH2 infrared modes indicate the presence of alkyl chains mainly in the trans/trans conformation. Additionally, optical ellipsometry and quartz microbalance measurements enabled us to estimate the thickness of the films. The results, as a whole, are in good agreement with the formation of densely packed monolayers.

Adsorption↗
PubMed2004

In situ formation and characterization of poly(ethylene glycol)-supported lipid bilayers on gold surfaces.

Inclusion of a polymer cushion between a lipid bilayer membrane and a solid surface has been suggested as a means to provide a soft, deformable layer that will allow for transmembrane protein insertion and mobility. In this study, mobile, tethered lipid bilayers were formed on a poly(ethylene glycol) (PEG) support via a two-step adsorption process. The PEG films were prepared by coadsorbing a heterofunctional, telechelic PEG lipopolymer (1,2-distearoyl-sn-glycero-3-phosphoethanolamine-N-poly(ethylene glycol)-2000-N-[3-(2-(pyridyldithio)propionate]) (DSPE-PEG-PDP) and a nonlipid functionalized PEG-PDP from an ethanol/water mixture, as described in a previous paper (Munro, J. C.; Frank, C. W. Langmuir 2004, 20, 3339-3349). Then a two-step lipid adsorption strategy was used. First, lipids were adsorbed onto the PEG support from a hexane solution. Second, vesicles were adsorbed and fused on the surface to create a bilayer in an aqueous environment. Fluorescence recovery after photobleaching experiments show that this process results in mobile bilayers with diffusion coefficients on the order of 2 microm2/s. The mobility of the bilayers is decreased slightly by increasing the density of tethered lipids. The formation of bilayers, and not multilayer structures, is also confirmed by surface plasmon resonance, which was used to determine in situ film thickness, and by fluorimetry, which was used to determine quantitatively the fluorescence intensity for each 18 by 18 mm sample. Unfortunately, fluorescence microscopy also shows that there are large defects on the samples, which limits the utility of this system.

Adsorption↗
PubMed2005

Refractive index of thin, aqueous films between hydrophobic surfaces studied using evanescent wave atomic force microscopy.

We have studied the refractive index of a thin aqueous film between microscopic hydrophobic surfaces using evanescent wave atomic force microscopy (EW-AFM). An evanescent wave, generated at a solid-liquid interface, is scattered by AFM tips or glass particles attached to AFM cantilevers. The scattering of this wave is used to determine the refractive index as a function of separation between these surfaces. Measurements were performed on surfaces that were rendered hydrophobic with octadecyltrichlorosilane, which produces solid-water contact angles in excess of 90 degrees. For AFM tips, the average refractive index in the thin film was always equal to that of water when the film was thicker than approximately 100 nm. At smaller separations, the refractive index was always greater than or equal to that of water. This is inconsistent with the formation of air or vapor films and consistent with a small amount of organic material between the surfaces. For colloidal spheres (R approximately 10 microm), we were not able to detect changes in the refractive index of the thin film between the sphere and plate.

Microscopy, Atomic Force↗
PubMed2005

Surface plasmon interference nanolithography.

A new nanophotolithography technique based on the interference of surface plasmon waves is proposed and demonstrated by using computer simulations. The wavelengths of the surface plasmon waves at metal and dielectric interfaces can reach the nanometer scale while their frequencies remain in the optical range. As a result, the resolution of this surface plasmon interference nanolithography (SPIN) can go far beyond the free-space diffraction limit of the light. Simulation results show that one-dimensional and two-dimensional periodical structures of 40-100 nm features can be patterned using interfering surface plasmons launched by 1D gratings. Detailed characteristics of SPIN such as field distribution and contrast are also investigated.

Computer Simulation↗
PubMed2005

Silica nanorod-array films with very low refractive indices.

The refractive-index contrast is an important figure of merit for dielectric multilayer structures, optical resonators, and photonic crystals. This represents a strong driving force for novel materials that have refractive indices lower than those of conventional optically transparent materials. Silica nanorod-array dielectric films with unprecedented low refractive indices of 1.08 are demonstrated and shown to have viable optical properties including enhanced reflectivity of a single-pair distributed Bragg reflector.

Birefringence↗
PubMed2005

Subwavelength focusing and guiding of surface plasmons.

The constructive interference of surface plasmon polaritons (SPP) launched by nanometric holes allows us to focus SPP into a spot of high near-field intensity having subwavelength width. Near-field scanning optical microscopy is used to map the local SPP intensity. The resulting SPP patterns and their polarization dependence are accurately described in model calculations based on a dipolar model for the SPP emission at each hole. Furthermore, we show that the high SPP intensity in the focal spot can be launched and propagated on a Ag strip guide with a 250 x 50 nm2 cross section, thus overcoming the diffraction limit of conventional optics. The combination of focusing arrays and nano-waveguides may serve as a basic element in planar nano-photonic circuits.

Equipment Design↗
PubMed2005

Three-dimensional mapping of the light intensity transmitted through nanoapertures.

A general method to map the 3D spatial distribution of light emerging from nanoscale apertures is presented that uses photolithographic techniques to create polymer replicas of the intensity distribution. The resulting features varied with aperture diameter and exposure time and showed good correlation with theory. This method provides direct visualization of the intensity distribution in close proximity to nanostructures and overcomes limitations imposed by physical probes where the contribution of the probe to the map requires deconvolution.

Computer Simulation↗
PubMed2005

Basis and lattice polarization mechanisms for light transmission through nanohole arrays in a metal film.

The extraordinary light transmission through double-hole and elliptical nanohole arrays in a thin gold film is investigated for different orientations of the holes relative to the lattice. Even though these bases have similar symmetry characteristics, the polarization follows the orientation of the basis for the ellipse but remains fixed along a lattice vector for the double holes. Furthermore, the maximum transmitted intensity for linearly polarized light is constant for the ellipse, but decreases for the double holes as they are rotated away from being aligned with the lattice. Finite-difference time-domain simulations agree well with the experimental findings. These experiments show how the basis determines both the coupling into the surface plasmon waves and the evanescent transmission through the nanoholes. Both of these effects need to be considered when designing nanophotonic devices using the extraordinary transmission phenomenon.

Anisotropy↗
PubMed2006

Optical interference from pairs and arrays of nanowires.

The angle dependence of the scattered light from pairs and one-dimensional arrays of nanowires was studied. The intensity of the scattered light varied distinctly during rotation of the structure. The results could be theoretically modeled by treating a pair of nanowires as a double slit and an array of nanowires as a grating. The correspondence between theory and experimental results conclusively proves that the variations are due to the proposed interference effects.

Computer Simulation↗
PubMed2006

Nanorice: a hybrid plasmonic nanostructure.

We have designed and fabricated a new hybrid nanoparticle that combines the intense local fields of nanorods with the highly tunable plasmon resonances of nanoshells. This dielectric core-metallic shell prolate spheroid nanoparticle bears a remarkable resemblance to a grain of rice, inspiring the name "nanorice". This geometry possesses far greater structural tunability than either a nanorod or a nanoshell, along with much larger local field intensity enhancements and far greater sensitivity as a surface plasmon resonance (SPR) nanosensor than any dielectric-metal nanostructures reported previously. Invoking the plasmon hybridization picture allows us to understand the plasmon resonances of this geometry, as arising from a hybridization of the primitive plasmons of a solid spheroid and an ellipsoidal cavity inside a continuous metal.

Crystallization↗
PubMed2006

Localized surface plasmon resonance spectroscopy of single silver triangular nanoprisms.

The plasmonic properties of single silver triangular nanoprisms are investigated using dark-field optical microscopy and spectroscopy. Two distinct localized surface plasmon resonances (LSPR) are observed. These are assigned as in-plane dipolar and quadrupolar plasmon excitations using electrodynamic modeling based on the discrete dipole approximation (DDA). The dipole resonance is found to be very intense, and its peak wavelength is extremely sensitive to the height, edge length, and tip sharpness of the triangular nanoprism. In contrast, the intensity of the quadrupole resonance is much weaker relative to the dipole resonance in the single particle spectra than in the ensemble averaged spectrum. Several parameters relevant to the chemical sensing properties of these nanoprisms have been measured. The dependence of the dipole plasmon resonance on the refractive index of the external medium is found to be as high as 205 nm RIU(-1) and the plasmon line width as narrow as approximately 0.17 eV. These data lead to a sensing figure of merit (FOM), the slope of refractive index sensitivity in eV RIU(-1)/line width (eV), as high as 3.3. In addition, the LSPR shift response to alkanethiol chain length was found to be linear with a slope of 4.4 nm per CH2 unit. This is the highest short-range refractive index sensitivity yet measured for a nanoparticle.

Computer Simulation↗
PubMed2006

Optically pumped surface-emitting lasing using self-assembled block-copolymer-distributed Bragg reflectors.

A thin-film organic laser cavity using a block-copolymer-based one-dimensional (1D) photonic crystal was fabricated. Polymeric distributed Bragg reflectors (DBRs) were prepared through the self-assembly of a lamellar-forming poly(styrene-b-isoprene) (PS-b-PI) diblock copolymer having a 1D photonic stop band overlapping with the fluorescence spectrum of a gain medium. Optically pumped surface-emitting lasing was obtained using poly(methyl methacrylate) (PMMA) doped with 1,4-di-(2-methylstyryl)benzene (Bis-MSB) as an organic gain medium and the polymeric self-assembled DBR as a spectral-band selective feedback element.

Crystallization↗
PubMed2006

Direct evidence for surface plasmon-mediated enhanced light transmission through metallic nanohole arrays.

This paper provides direct evidence for the role of surface plasmons in the enhanced optical transmission of light through metallic nanoscale hole arrays. Near-field optical images directly confirmed the presence of surface plasmons on gold nanohole arrays with interhole spacings larger than the surface plasmon wavelength. A simple interference model provides an intuitive explanation of the two types of fringe wavelengths observed in the near-field optical images. Far-field spectroscopy revealed a surface plasmon band that contributed a factor > 8 to the transmission enhancement. Furthermore, silicon nanohole arrays did not exhibit any features in the near-field, which demonstrates that metallic materials are necessary for enhanced light transmission through nanohole arrays.

Computer Simulation↗
PubMed1995

Solubilisation of drugs in micellar systems studied by eluent gel permeation chromatography.

PURPOSE: The purpose of the study was to investigate the potential of a chromatographic method which is based on elution gel chromatography (EGPC) in the study of solubilisation of drugs in micellar solutions. METHODS: The EGPC method differs from conventional GPC in the use of a solution of the associating surfactant as eluent (rather than solvent) and the injection of a small volume of solution of different concentration (or alternatively injection of solvent alone) to probe the association equilibrium in the eluent. The technique was applied to a study of the solubilisation of selected drugs in aqueous micellar solutions of a triblock copolymer (Synperonic-PE F127) composed of oxyethylene [E, OCH2CH2] and oxypropylene [P, OCH2CH(CH3)] units with nominal molecular formula E98P67E98. RESULTS: EGPC curves were obtained showing vacancy peaks at the elution volumes of the drugs, clearly demonstrating their solubilisation. In addition, the micelle-molecule equilibrium of the copolymer surfactant could be monitored at all times. Quantitative determination of the partition of solute between micelles and solvent phase was not possible due to the incomplete conversion of molecules to micelles in solutions of the selected copolymer. CONCLUSIONS: The EGPC technique provides evidence for the solubilisation of the drugs in aqueous solutions of Synperonic F127; a more thorough assessment of its potential for quantitative measurement of solubilisation requires the use of a surfactant which is wholly (or at least mainly) in the micellar state under the conditions of use.

Adsorption↗
PubMed1994

Formulation and intestinal absorption enhancement evaluation of water-in-oil microemulsions incorporating medium-chain glycerides.

We developed self-emulsifying water-in-oil (w/o) microemulsions incorporating medium-chain glycerides and measured their conductance, viscosity, refractive index and particle size. Formulation of Calcein (a water-soluble marker molecule, MW = 623), or SK&F 106760 (a water-soluble RGD peptide, MW = 634) in a w/o microemulsion having a composition of Captex 355/Capmul MCM/Tween 80/Aqueous (65/22/10/3, % w/w), resulted in significant bioavailability enhancement in rats relative to their aqueous formulations. Upon intraduodenal administration the bioavailability was enhanced from 2% for Calcein in isotonic Tris, pH 7.4 to 45% in the microemulsion and from 0.5% for SK&F 106760 in physiological saline to 27% in the microemulsion formulation. The microemulsion did not induce gross changes in GI mucosa at a dosing volume of 3.3 ml/kg. These results suggest that water-in-oil microemulsion systems may be utilized for enhancement of intestinal drug absorption.

Absorptiometry, Photon↗