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At least 343 records · Page 19Linked to original sources
PubMed2003

Spontaneous formation of nanoparticle vesicles from homopolymer polyelectrolytes.

Nanoparticle vesicles were spontaneously assembled from homopolymer polyamine polyelectrolytes and water-soluble, citrate-stabilized quantum dots. The further addition of silica nanoparticles to a solution of quantum dot vesicles generated stable micrometer-sized hollow spheres whose walls were formed of a thick, inner layer of close-packed quantum dots followed by an outer layer of silica. The method employed here to assemble both the nanoparticle vesicles and the hollow spheres is in direct contrast to previous syntheses that use either tailored block copolymers or oil-in-water emulsion templating. We propose that the formation of charge-stabilized hydrogen bonds between the positively charged amines of the homopolymer polyelectrolytes and the negatively charged citrate molecules stabilizing the quantum dots is responsible for the macroscopic phase separation in this completely aqueous system. The ease and processibility of the present approach gives promise for the production of a diverse array of materials ranging in applications from drug delivery to catalysis to micrometer-scale optical devices.

Journal Article↗
PubMed2003

Direct growth of shape-controlled nanocrystals on nanotubes via biological recognition.

The new biological approach was examined to fabricate shape-controlled Ag nanocrystals grown directly on surfaces, inspired by nature that various shapes of nanocrystals are produced accurately and reproducibly in biological systems. Here we demonstrate the direct growth of hexagon-shaped Ag nanocrystals on sequenced peptide-coated nanotubes via biological recognition. When the peptide, Asn-Pro-Ser-Ser-Leu-Phe-Arg-Tyr-Leu-Pro-Ser-Asp, recognizing and effecting the Ag nanocrystal growth on the (111) face, was sequenced and incorporated onto template nanotube surfaces, the biomineralization of Ag ions on the nanotubes led the isotropic hexagon-shaped Ag nanocrystal coating under pH control of the growth solution. Multiple Ag nanocrystal shapes were observed when the peptide mineralized Ag ions without the template nanotubes, and therefore the template nanotube has a significant influence on regulating the majority of Ag nanocrystals into the hexagonal shape. This biological approach, using specific peptide sequences on surfaces to control nanocrystal shapes, may be developed as a simple and economical method to produce building blocks with desired physical properties for new generation of electronics, sensors, and optical devices.

Amino Acid Sequence↗
PubMed2004

Mixed 1D-2D inorganic polymeric zinc ferrocenylphosphonate: crystal structure and electrochemical study.

Needs for ferrocene immobilization on robust host structures are considerable since derivative materials may find applications in medical areas, optical devices, or catalysis. Synthesis of phosphonate functionalized ferrocene allowed its subsequent inorganic polymerization with a zinc salt. The crystallographic structure of the compound obtained, Zn(HO(3)PFc)(2).2H(2)O, shows a unique two-dimensional ferrocene arrangement anchored on a one-dimensional Zn-O-P-O-Zn backbone. The ferrocene packing in the title compound is very similar to the packing found in molecular ferrocene. The electroactivity of Zn(HO(3)PFc)(2).2H(2)O is thoroughly studied. It shows a reversible surface oxidation of ferrocene. Mössbauer spectroscopy for the oxidized compound shows an isomer shift of IS(2b) = 0.432 mm x s(-1) and a quadrupolar splitting of QS(2b) = 0.205 mm x s(-1), which is consistent with a stable S = 1/2 ferrocenium state. The magnetic susceptibility study, Mössbauer spectroscopy, and galvanostatic titration show that only the ferrocene moieties present at the surface of the crystallites are reversibly oxidized. This observation is reinforced by a complex impedance study showing mainly resistive behavior and conductivity measurements indicating weak, thermally assisted, conductivity. The general properties of this compound demonstrate that phosphonato functionalization may be a useful approach for all fields concerned by immobilization of ferrocene.

Journal Article↗
PubMed2004

Tunable photonic band gap crystals based on a liquid crystal-infiltrated inverse opal structure.

Composite materials comprised of nematic liquid crystals (LCs) and SiO(2) inverse opal films were fabricated. Their optical properties were quite different from those of inverse opal films without the LCs. The optical properties could be controlled by changing the refractive indices of the LCs, which vary with orientation, phase, and temperature. In particular, the optical properties were drastically changed by thermal or photoinduced isothermal phase transitions of the LCs. This means that the photonic band structure could be controlled, and tunable photonic crystals have been achieved, based on the inverse opal structure. The mechanism of this change was investigated by the evaluation of the effective refractive indices. As a result, it was found that the change in optical properties was derived from the orientation of the LC molecules in the voids in the inverse opal film. Furthermore, once the mechanism was understood, it was also possible to control the position of the reflection peak by changing the alignment of the LCs. Such materials have the possibility for practical use in optical devices and fundamental research systems.

Journal Article↗
PubMed2005

Porous BCN nanotubular fibers: growth and spatially resolved cathodoluminescence.

Porous boron carbonitride nanotubular fibers with BCN stoichiometry and homogeneous B, C, and N species distribution were fabricated via the CVD method. Spatially resolved cathodoluminescence measurements on individual nanostructures revealed intense ultraviolet emission centered at 319 nm, suggesting the characteristics of a semiconductor with a band gap of 3.89 eV. It is believed that the present nanostructures may have a variety of applications in ultraviolet optical devices, hydrogen storage systems, and field emission apparatus.

Journal Article↗
PubMed2005

Influence of thermal fluctuations on interfacial electron transfer in functionalized TiO2 semiconductors.

The influence of thermal fluctuations on the dynamics of interfacial electron transfer in sensitized TiO2-anatase semiconductors is investigated by combining ab initio DFT molecular dynamics simulations and quantum dynamics propagation of transient electronic excitations. It is shown that thermal nuclear fluctuations speed up the underlying interfacial electron transfer dynamics by introducing nonadiabatic transitions between electron acceptor states, localized in the vicinity of the photoexcited adsorbate, and delocalized states extended throughout the semiconductor material, creating additional relaxation pathways for carrier diffusion. Furthermore, it is shown that room-temperature thermal fluctuations reduce the anisotropic character of charge diffusion along different directions in the anatase crystal and make similar the rates for electron injection from adsorbate states of different character. The reported results are particularly relevant to the understanding of temperature effects on surface charge separation mechanisms in molecular-based photo-optic devices.

Journal Article↗
PubMed2006

Colloidal HgTe nanocrystals with widely tunable narrow band gap energies: from telecommunications to molecular vibrations.

A convenient, aqueous-based synthesis of stable HgTe nanocrystals with widely size-tunable room temperature emission between wavelengths of 1.2 to 3.7 mum is demonstrated. By the choice of the thiols, applied as stabilizers, we optimized the growth dynamics, the luminescence quantum yields (up to 40%), and a ligand-exchange procedure, required to transfer the nanocrystals from water to nonpolar organic solvents. The latter is greatly improved and facilitated by the use of mercaptoethylamine as initial stabilizer. The possibility to tune the HgTe nanocrystal sizes from 3 to 12 nm and to control their surface functionalities (hydrophobic and hydrophilic) makes them very promising for the development of infrared optical devices, emitting in the wavelength region between the telecommunications and the molecular vibrations.

Journal Article↗
PubMed2006

Photocontrolled magnetization of CdS-modified Prussian blue nanoparticles.

The first photocontrollable magnetic nanoparticles containing CdS and Prussian blue (PB) have been created using reverse micelles as nanoreactors. Photoinduced electron transfer from CdS to PB in the reverse micelle changed the magnetic properties of the composite nanoparticles from ferromagnetic to paramagnetic. The magnetization in the ferromagnetic region below 4 K was substantially decreased after UV light illumination and could be restored almost to its original level by thermal treatment at room temperature. This novel strategy of designing composite nanoparticles containing photoconductive semiconductors and magnetic materials to create photoswitchable magnetic materials may open many possibilities in the development of magneto-optical devices.

Journal Article↗
PubMed2006

Strong cooperative enhancement of two-photon absorption in double-strand conjugated porphyrin ladder arrays.

We present the two-photon absorption (2PA) spectra of a series of conjugated porphyrin oligomers containing N = 2, 4, 8, and ca. 13 monomer units, meso-meso connected with butadiyne linkers. We demonstrate that, in the coplanar double-strand arrays, self-assembled upon addition of 4,4'-bipyridyl, the conjugation length increases dramatically, leading to very strong cooperative enhancement of 2PA. We analyze the scaling of 2PA in both the double-strand and rotationally free single-strand arrays and show how the effective conjugation length in both cases is linked to the observed 2PA properties. By introducing a "conjugation signature" for the 2PA strength, we show that, in double-strand arrangement, the conjugation embraces the whole molecule up to the tetramer level, whereas in single-strand arrangement, it is always less than N, except for N = 2, but keeps increasing until N = 8. Our finding of extremely strong 2PA cross section, sigma2 approximately 105 GM, in double-strand oligomers peaking at 1.3 mum can find use for signal processing in fiber-optic devices.

Journal Article↗
PubMed2005

Ab initio and DFT study of the geometric structures and static dipole (hyper)polarizabilities of aromatic anions.

The geometries and the static dipole (hyper)polarizabilities (alpha, beta, gamma) of a series of aromatic anions were investigated at the ab initio (HF, MP2, and MP4) and density functional theory DFT (B3LYP) levels of theory. The anions chosen for the present study are the benzenethiolate (Ph-S-), benzenecarboxylate (Ph-CO2-), benzenesulfinate (Ph-SO2-), benzenesulfonate (Ph-SO3-), and 1,3-benzenedicarboxylate (1,3-Ph-(CO2)2(2-)). For benzenethiolate anion, additional alpha, beta, and gamma calculations were performed at the coupled cluster CCSD level with MP2 optimized geometries. The standard diffuse and polarized 6-31+G(d,p) basis set was employed in conjunction to the ab initio and DFT methods. Additional HF calculations were performed with the 6-311++G(3d,3p) basis set for all the anions. The correlated electric properties were evaluated numerically within the formalism of finite field. The optimized geometries were analyzed in terms of the few reports about the phenolate and sulfonate ions. The results show that electron correlation effects on the polarizabilities are very important in all the anion series. Was found that Ph-SO2- is highly polarizable in terms of alpha and beta, and the Ph-S- is the highest second hyperpolarizable in the series. The results of alpha were rationalized in terms of the analysis of the polarization of charge based in Mulliken atomic population and the structural features of the optimized geometries of anions, whereas the large differences in the beta and gamma values in the series were respectively interpreted in terms of the bond length alternation BLA and the separation of charge in the aromatic ring by effects of the substitution. These results allowed us to suggest the benzenesulfinate and benzenethiolate anions as promising candidates that should be incorporated in ionic materials for second and third-order nonlinear optical devices.

Anions↗
PubMed2005

Diameter-dependent optical constants of gold mesoparticles electrodeposited on aluminum films containing copper.

Electrodeposition of gold mesoparticles on anodized and chemically etched aluminum/copper films deposited on silicon wafers proceeds by instantaneous nucleation and with no diffusion limitations. Both of these phenomena favor the formation of relatively monodispersed gold particles. Under the reported electrodeposition conditions, the relative standard deviation of the particle diameter is 25%. The particle coverage is 7 x 10(8) particles cm(-2). The mean particle diameter varies as a function of electrodeposition time in the range of 40-80 nm. Optical constants of gold mesoparticles are resolved by spectroscopic ellipsometry. A two-layer optical model is constructed to determine both extinction coefficients and refractive indexes of gold mesoparticles as a function of the mean particle diameter. The absorption peak, associated with surface plasmons, is modeled with two Lorentz oscillators. Absorption peak maximums shift from 610 to 675 nm as the mean particle diameter increases from 42 to 74 nm. Electrodeposition of gold particles on technologically relevant substrates, such as aluminum/copper films, is expected to increase the utility of gold particles and facilitate their incorporation in nanostructured materials and a variety of electronic and optical devices.

Journal Article↗
PubMed2006

Enhanced thermal stability of dipole alignment in inorganic-organic hybrid films containing benzothiazole chromophore.

A new thermally stable second-order nonlinear optical (NLO) inorganic-organic hybrid film was successfully prepared by using a sol-gel process of alkoxysilane dye containing a benzothiazole unit. The dye-bonded precursor was synthesized from 3-isocyanatopropyltriethoxysilane and the heterocycle azo dye 2-[4'-(N-ethyl-N-2-hydroxyethyl)-amino-phenylazo]-6-nitrobenzothiazole (EHNBT) via a urethane reaction. Molecular structural characterization for the resultant was achieved by elemental analysis, FTIR, UV-visible spectra, and 1H NMR. The second harmonic coefficients (d33) of poled hybrid films measured by a Maker fringe technique were in the range 15.9-72.1 pm/V at a wavelength of 1064 nm, depending on the concentration of alkoxysilane dye. The hybrid films containing the benzothiazole moiety exhibited higher thermal stability of dipole alignment at elevated temperatures than their analogues with a benzene ring. The d33 value of the poled film remained at 94% of its initial value after heating at 120 degrees C for 6 h, and only 18% decayed in 15 min at 180 degrees C. The result indicates that the hybrid film is suitable for the fabrication of an electro-optic device.

Journal Article↗
PubMed2006

Al2O3:Cr3+ nanotubes synthesized via homogenization precipitation followed by heat treatment.

Cr3+-doped NH4Al(OH)2CO3 nanotubes, templated by surfactant assemblies, were successfully synthesized via the homogenization precipitation method, and various crystallographic phase Al2O3:Cr3+ nanotubes were also obtained by postannealing at different temperatures. The characteristic R1, R2 doublet line transitions of ruby can be observed in the high crystalline alpha-Al2O3 nanotubes calcined at temperatures higher than 1200 degrees C. The results also indicate that the formation mechanism of the tubular nanostructures should result from the self-rolling action of layered compound NH4Al(OH)2CO3 under the assistance of the surfactant soft-template. The convenient synthetic procedure, excellent reproducibility, clean reactions, high yield, and fine quality of products in this work make the present route attractive and significant. Aluminum oxide nanotubes with high specific surface area could be used as fabricating nanosized optical devices doped with different elements and stable catalyst supports of metal clusters.

Journal Article↗
PubMed2004

Gold nanoparticle patterning of silicon wafers using chemical e-beam lithography.

This paper demonstrates a novel facile method for fabrication of patterned arrays of gold nanoparticles on Si/SiO2 by combining electron beam lithography and self-assembly techniques. Our strategy is to use direct-write electron beam patterning to convert nitro functionality in self-assembled monolayers of 3-(4-nitrophenoxy)-propyltrimethoxysilane to amino functionality, forming chemically well-defined surface architectures on the 100 nm scale. These nanopatterns are employed to guide the assembly of citrate-passivated gold nanoparticles according to their different affinities for amino and nitro groups. This kind of nanoparticle assembly offers an attractive new option for nanoparticle patterning a silicon surface, as relevant, for example, to biosensors, electronics, and optical devices.

Journal Article↗
PubMed2005

Synthesis of colloidal silica dumbbells.

We describe the synthesis and characterization of stable suspensions of monodisperse fluorescently labeled silica dumbbell particles. Pure dispersions of silica dumbbells with center-to-center lengths from 174 nm to 2.3 microm were produced with a variety of aspect ratios. Individual particles in concentrated dispersions of these particles could be imaged with confocal microscopy. These particles can be used as a colloidal model system for addressing fundamental questions about crystal and glass formation of low-aspect-ratio anisotropic particles. They also have potential in photonic applications and electro-optical devices.

Journal Article↗
PubMed2006

3D-ordered macroporous materials comprising DNA.

Macroporous materials comprising DNA were fabricated with the colloidal crystal template. First, DNA and diazoresin (DR) molecules are fully filled into the voids of a colloidal crystal template. After thermal treatment and removal of the colloids, DNA porous materials with highly ordered structure were obtained. In the process of thermal treatment the cross-linking reaction takes place between DR and DNA, which plays an important role for sustaining the porous framework. The DNA porous materials will turn into a fluorescent DNA/dye composite after staining with Hoechst 33258 (Hoe), a characteristic fluorescent dye for DNA. This kind of composite DNA porous material may have potential applications in optical devices.

Animals↗
PubMed2006

Role of surface anchoring and geometric confinement on focal conic textures in smectic-A liquid crystals.

A high surface area-to-volume ratio in microchannels increases the importance of surface interactions within them. In layered liquids, such as smectic liquid crystals, surface interactions play an important role in the formation of defect textures. We use 8CB liquid crystal, which is in the smectic-A phase at room temperature, as a model layered liquid. PDMS surfaces can be tuned to be hydrophilic or hydrophobic, and due to the nature of liquid crystalline molecules, we show that this results in planar or homeotropic anchoring conditions, respectively. In a confined system, contrary to the bulk, generated defects cannot grow freely. In the present work, we show that the confinement offered by PDMS microchannels along with the capability of creating mixed anchoring conditions within them results in the formation of particular ordered defect textures through increased surface interactions in smectic-A liquid crystals. Our observations imply that microscale confinement is useful for controlling the size, size distribution, and packing structure of microscale defect structures within these materials. In addition, we show that by placing a droplet of smectic-A liquid crystal on a PDMS surface containing microscale parallel cracks, ordered focal conic defects form between two adjacent cracks. The distance between two adjacent cracks dictates the size of the defects. These observations could lead to useful ideas for exploring new technologies for flexible optical devices or displays that utilize smectic-A liquid crystals.

Journal Article↗
PubMed2005

Carbon nanotubes loaded with magnetic particles.

We describe a simple and versatile technique to produce magnetic tubes by filling carbon nanotubes (CNTs) with paramagnetic iron oxide particles ( approximately 10 nm diameter). Commercial ferrofluids were used to fill CNTs with an average outer diameter of 300 nm made via chemical vapor deposition into alumina membranes. Transmission electron microscopy study shows a high density of particles inside the CNT. Experiments using external magnetic fields demonstrate that almost 100% of the nanotubes become magnetic and can be easily manipulated in magnetic field. These one-dimensional magnetic nanostructures can find numerous applications in nanotechnology, memory devices, optical transducers for wearable electronics, and in medicine.

Colloids↗