Formation of mesostructured titania thin films using iospropoxide precursors

Mesostructured titania thin films were prepared by an evaporation-induced self-assembly process. The highly acidic sot precursors contained titanium(IV) tetraisopropoxide (TTIP) as a titanium source, a tri-block copolymer Pluronic P123 as a template, and acetylacetonate and HCl as hydrolysis inhibitors. Characteristics of the resultant titania thin films were studied using X-ray diffraction (XRD) analysis, N-2-adsorption/desorption analysis, and transmission electron microscopy (TEM). XRD and TEM investigations on the as-synthesised films revealed the appearance of cubic-like, pseudohexagonal, and lamellar mesophases; depending on the amount of water in the sols of film precursors. Template removal by a calcination process yields high surface area (320-360 m(2)/g) mesoporous materials with crystalline anatase frameworks. Water content also influences the degree of anatase crystallinity of the calcined films. Higher water content resulted in improved anatase crystallinity. These nanostructured materials are of interest for photocatalysts, pbotoelectrochemical solar cells and other photonic devices. (C) 2003 Elsevier B.V. All rights reserved.

Postsynthesis stabilization of free-standing mesoporous silica films

Mixed ammonia-water vapor postsynthesis treatment provides a simple and convenient method for stabilizing mesostructured silica films. X-ray diffraction, transmission electron microscopy, nitrogen adsorption/desorption, and solid-state NMR (C-13, Si-29) were applied to study the effects of mixed ammonia-water vapor at 90 degreesC on the mesostructure of the films. An increased cross-linking of the silica network was observed. Subsequent calcination of the silica films was seen to cause a bimodal pore-size distribution, with an accompanying increase in the volume and surface area ratios of the primary (d = 3 nm) to secondary (d = 5-30 nm) pores. Additionally, mixed ammonia-water treatment was observed to cause a narrowing of the primary pore-size distribution. These findings have implications for thin film based applications and devices, such as sensors, membranes, or surfaces for heterogeneous catalysis.

Coherence of polaronic transport in layered metals

Layered systems show anisotropic transport properties. The interlayer conductivity shows a general temperature dependence for a wide class of materials. This can be understood if conduction occurs in two different channels activated at different temperatures. We show that the characteristic temperature dependence can be explained using a polaron model for the transport. The results show an intuitive interpretation in terms of coherent and incoherent quasi-particles within the layers. Further, we extract results for the magnetoresistance, thermopower, spectral function and optical conductivity for the model and discuss application to experiments.

Molecular dynamics simulation of the structural and dynamic properties of dioctadecyldimethyl ammoniums in organoclays

The structural and dynamic properties of dioctadecyldimethylammoniums (DODDMA) intercalated into 2:1 layered clays are investigated using isothermal-isobaric (NPT) molecular dynamics (MD) simulation. The simulated results are in reasonably good agreement with the available experimental measurements, such as X-ray diffraction (XRD), atom force microscopy (AFM), Fourier transform infrared (FTIR), and nuclear magnetic resonance (NMR) spectroscopies. The nitrogen atoms are found to be located mainly within two layers close to the clay surface whereas methylene groups form a pseudoquadrilayer structure. The results of tilt angle and order parameter show that interior two-bond segments of alkyl chains prefer an arrangement parallel to the clay surface, whereas the segments toward end groups adopt a random orientation. In addition, the alkyl chains within the layer structure lie almost parallel to the clay surface whereas those out of the layer structure are essentially perpendicular to the surface. The trans conformations are predominant in all cases although extensive gauche conformations are observed, which is in agreement with previous simulations on n-butane. Moreover, an odd-even effect in conformation distributions is observed mainly along the chains close to the head and tail groups. The diffusion constants of both nitrogen atoms and methylene groups in these nanoconfined alkyl chains increase with the temperature and methelene position toward the tail groups.

Growing semiconductor nanocrystals directly in a conducting polymer

We describe a single step method to synthesise lead sulphide (PbS) nanocrystals directly in the conjugated polymer poly (2-methoxy-5-(2'-ethyl-hexyloxy)-p-phenylene vinylene) (MEH-PPV). This method allows size control of the nanocrystal via co-solvent ratios. We find good agreement between nanocrystal sizes determined by transmission electron microscopy and sizes theoretically determined from the absorption edge of the nanocrystals. Finally we show that this synthesis technique is not restricted to MEH-PPV and demonstrate that nanocrystals can be grown in Poly(3-hexylthiophene-2,5-diyl) (P3HT). (C) 2005 Elsevier B.V. All rights reserved.

Lead sulfide nanocrystal: conducting polymer solar cells

In this paper, we report photovoltaic devices fabricated from lead sulfide nanocrystals and the conducting polymer poly(2-methoxy-5-(2'-ethyl-hexyloxy)-p-phenylene vinylene). This composite material was produced via a new single-pot synthesis which solves many of the issues associated with existing methods. Our devices have white light power conversion efficiencies under AM 1.5 illumination of 0.7% and single wavelength conversion efficiencies of 1.1%. Additionally, they exhibit remarkably good ideality factors (n = 1.15). Our measurements show that these composites have significant potential as soft optoelectronic materials.

Spin exchange and superconductivity in a t-J(')-V model for two-dimensional quarter-filled systems

The effect of antiferromagnetic spin fluctuations on two-dimensional quarter-filled systems is studied theoretically. An effective t-J(')-V model on a square lattice which accounts for checkerboard charge fluctuations and next-nearest-neighbor antiferromagnetic spin fluctuations is considered. From calculations based on large-N theory on this model it is found that the exchange interaction J(') increases the attraction between electrons in the d(xy) channel only, so that both charge and spin fluctuations work cooperatively to produce d(xy) pairing.

Equivalence between two-mode spin squeezed states and pure entangled states with equal spin

We prove that a pure entangled state of two subsystems with equal spin is equivalent to a two-mode spin-squeezed state under local operations except for a set of bipartite states with measure zero, and provide a counterexample to the generalization of this result to two subsystems of unequal spin.

5,6-Dihydroxyindole-2-carboxylic acid: a first principles density functional study

We report first principles density functional calculations for 5,6-dihydroxyindole-2-carboxylic acid (DHICA) and several oxidised forms. DHICA and 5,6-dihydroxyindole (DHI) are believed to be the basic building blocks of the eumelanins. Our results show that carboxylation has a significant effect on the physical properties of the molecules. In particular, the relative stabilities and the highest occupied molecular orbital-lowest unoccupied molecular orbital gaps (calculated with the DeltaSCF method) of the various redox forms are strongly affected. We predict that, in contrast to DHI, the density of unpaired electrons, and hence the ESR signal, in DHICA is negligibly small. (C) 2004 Elsevier B.V. All rights reserved.

Measurement-based teleportation along quantum spin chains

We examine the teleportation of an unknown spin-1/2 quantum state along a quantum spin chain with an even number of sites. Our protocol, using a sequence of Bell measurements, may be viewed as an iterated version of the 2-qubit protocol of C. H. Bennett et al. [Phys. Rev. Lett. 70, 1895 (1993)]. A decomposition of the Hilbert space of the spin chain into 4 vector spaces, called Bell subspaces, is given. It is established that any state from a Bell subspace may be used as a channel to perform unit fidelity teleportation. The space of all spin-0 many-body states, which includes the ground states of many known antiferromagnetic systems, belongs to a common Bell subspace. A channel-dependent teleportation parameter O is introduced, and a bound on the teleportation fidelity is given in terms of O.

A quantum yield map for synthetic eumelanin

The quantum yield of synthetic eumelanin is known to be extremely low and it has recently been reported to be dependent on excitation wavelength. In this paper, we present quantum yield as a function of excitation wavelength between 250 and 500 nm, showing it to be a factor of 4 higher at 250 nm than at 500 nm. In addition, we present a definitive map of the steady-state fluorescence as a function of excitation and emission wavelengths, and significantly, a three-dimensional map of the specific quantum yield: the fraction of photons absorbed at each wavelength that are subsequently radiated at each emission wavelength. This map contains clear features, which we attribute to certain structural models, and shows that radiative emission and specific quantum yield are negligible at emission wavelengths outside the range of 585 and 385 nm (2.2 and 3.2 eV), regardless of excitation wavelength. This information is important in the context of understanding melanin biofunctionality, and the quantum molecular biophysics therein. (c) 2005 American Institute of Physics.

Optical scatter imaging using digital Fourier microscopy

An approach reported recently by Alexandrov et al (2005 Int. J Imag. Syst. Technol. 14 253-8) on optical scatter imaging, termed digital Fourier microscopy (DFM), represents an adaptation of digital Fourier holography to selective imaging of biological matter. The holographic mode of the recording of the sample optical scatter enables reconstruction of the sample image. The form-factor of the sample constituents provides a basis for discrimination of these constituents implemented via flexible digital Fourier filtering at the post-processing stage. As in dark-field microscopy, the DFM image contrast appears to improve due to the suppressed optical scatter from extended sample structures. In this paper, we present the theoretical and experimental study of DFM using a biological phantom that contains polymorphic scatterers.

Quantitative fluorescence excitation spectra of synthetic eumelanin

Previously reported excitation spectra for eumelanin are sparse and inconsistent. Moreover, these studies have failed to account for probe beam attenuation and emission reabsorption within the samples, making them qualitative at best. We report for the first time quantitative excitation spectra for synthetic eumelanin, acquired for a range of solution concentrations and emission wavelengths. Our data indicate that probe beam attenuation and emission reabsorption significantly affect the spectra even in low-concentration eumelanin solutions and that previously published data do not reflect the true excitation profile. We apply a correction procedure (previously applied to emission spectra) to account for these effects. Application of this procedure reconstructs the expected relationship of signal intensity with concentration, and the normalized spectra show a similarity in form to the absorption profiles. These spectra reveal valuable information regarding the photophysics and photochemistry of eumelanin. Most notably, an excitation peak at 365 urn (3.40 eV), whose position is independent of emission wavelength, is possibly attributable to a 5,6-dihydroxyindole-2-carboxylic acid (DHICA) component singly linked to a polymeric structure.

Surface morphology dependent photoluminescence from colloidal silicon nanocrystals

Monodisperse 1-2 nm silicon nanocrystals are synthesized in reverse micelles and have their surfaces capped with either allylamine or 1-heptene to produce either hydrophilic or hydrophobic silicon nanocrystals. Optical characterization (absorption, PL, and time-resolved PL) is performed on colloidal solutions with the two types of surface-capped silicon nanocrystals with identical size distributions. Direct evidence is obtained for the modification of the optical properties of silicon nanocrystals by the surface-capping molecule. The two different surface-capped silicon nanocrystals show remarkably different optical properties.

On the Schrodinger equation involving a critical Sobolev exponent and magnetic field

We consider the semilinear Schrodinger equation -Delta(A)u + V(x)u = Q(x)vertical bar u vertical bar(2* -2) u. Assuming that V changes sign, we establish the existence of a solution u not equal 0 in the Sobolev space H-A,V(1) + (R-N). The solution is obtained by a min-max type argument based on a topological linking. We also establish certain regularity properties of solutions for a rather general class of equations involving the operator -Delta(A).