Computer-generated holograms for producing fractal speckles

When a diffuser is illuminated by the coherent light with a negative power-law distribution, fractal speckles are produced in the far-field diffraction region. Fractal speckles have extremely long spatial correlation functions of the intensity distributions in comparison with ordinary speckles, which implies that they may extend measurement ranges in various metrological applications based on the spatial correlation of speckles. To have fractal speckles with satisfactory statistical properties, it is required to produce a power-law illumination profile with high quality. In this paper, we report on the computer-generated holograms for producing power-law intensities on the basis of the method of stationary phase, with the error-reduction algorithm combined with to suppress strong ringing of the intensity.     

Photocatalytic activity of R3MO7 and R2Ti2O7 (R=Y, Gd, La; M=Nb, Ta) for water splitting into H2 and O2

The photocatalytic activities of R3MO7 and R2Ti2O7 (R=Y, Gd, La; M=Nb, Ta) strongly depended on the crystal structure. Overall, photocatalytic water splitting into H2 and O2 proceeded over La3TaO7 and La3NbO7, which have an orthorhombic weberite structure, Y2Ti2O7 and Gd2Ti2O7, which have a cubic pyrochlore structure, and La2Ti2O7, which has a monoclinic perovskite structure. All of these materials are composed of a network of corner-shared octahedral units of metal cations (TaO6, NbO6, or TiO6); materials without such a network were inactive. The octahedral network certainly increased the mobility of electrons and holes, thereby enhancing photocatalytic activity.     

Squeezing visible light waves into a 3-nm-thick and 55-nm-long plasmon cavity

We demonstrate controlled squeezing of visible light waves into nanometer-sized optical cavities. The light is perpendicularly confined in a few-nanometer-thick SiO2 film sandwiched between Au claddings in the form of surface plasmon polaritons and exhibits Fabry-Perot resonances in a longitudinal direction. As the thickness of the dielectric core is reduced, the plasmon wavelength becomes shorter; then a smaller cavity is realized. A dispersion relation down to a surface plasmon wavelength of 51 nm for a red light, which is less than 8% of the free-space wavelength, was experimentally observed. Any obvious breakdowns of the macroscopic electromagnetics based on continuous dielectric media were not disclosed for 3-nm-thick cores.     

Intramolecular bromo-amination of 1,4-cyclohexadiene aminal: one-pot discrimination of two olefins and concise asymmetric synthesis of (-)-gamma-lycorane

The reaction of cyclohexa-2,5-dienyl-1-methylaldehyde and optically pure 1,2-diaryl-1,2-diamine followed by intramolecular bromo-amination produced a one-pot discrimination of two olefins in the cyclohexane system, which was used for the asymmetric synthesis of (-)-gamma-lycorane.     

Extreme fluorescence sensitivity of some aniline derivatives to aqueous and nonaqueous environments: mechanistic study and its implication as a fluorescent probe

Effects of solvent water on the photophysical properties of a series of meta- and para-substituted anilines have been investigated by means of time-resolved fluorescence, transient absorption, and photoacoustic measurements. Some aniline derivatives exhibit extremely short fluorescence lifetime (tau(f)) and small quantum yield (Phi(f)) in water (e.g., tau(f) = 45 ps and Phi(f) = 0.0019 for m-cyanoaniline (m-ANCN) in H(2)O), which is in marked contrast with their much larger values in nonaqueous solvents (tau(f) = 7.3 ns and Phi(f) = 0.14 for m-ANCN in acetonitrile). Photoacoustic and transient absorption measurements show that the remarkable fluorescence quenching of m-ANCN in water is attributed almost exclusively to fast internal conversion. The lifetime measurements of m-ANCN in H(2)O/acetonitrile binary solvent mixtures reveal that the quenching is related to variation of hydrogen-bonding interactions between the amino group and water molecules and the conformational change of the amino group upon electronic excitation. Similar fluorescence quenching due to solvent water is also found for N-alkylated m-ANCNs. The drastic differences in the fluorescence intensity and lifetime of m-ANCNs under hydrophobic and hydrophilic environments and also the large solvent polarity dependence of the fluorescence band position suggest the possibility that they can be utilized as fluorescent probes for investigating the microenvironment of biological systems. In suspensions of human serum albumin (HSA) in water, remarkable enhancement of the fluorescence intensity and lifetime is observed for m-ANCN and its N-alkylated derivatives, demonstrating that m-ANCNs can be a candidate for novel fluorescent probe with small molecular size.     

Fabrication and hard X-ray photoemission analysis of photocathodes with sharp solar-blind sensitivity using AlGaN films grown on Si substrates

Photocathode devices operating in reflection-mode, where the photoemission is detected on the same side as the light irradiation, were developed for the detection of deep ultraviolet light by using p-Al_xGa_1−xN films grown on Si(1 1 1) substrates. The external quantum efficiencies were as high as 20-15% at 200 nm and 280 nm, while the value was as low as 10⁻²% at 310 nm. The on-off ratio was more than four orders of magnitude, which represents high solar-blind sensitivity. The escape probability of Al_xGa_1−xN photocathode was decreased with increase of AlN mole fraction. The effective barrier potential against the photoelectron emission near the surface was reduced due to the upward shift of conduction band of Al_xGa_1−xN. The photoemission from the Al_xGa_1−xN films terminated with Cs-O adatoms will be discussed in terms of band diagrams that were evaluated by hard X-ray photoelectron spectroscopy.     

Time-resolved infrared spectroscopy of K3Ta3B2O12 photocatalysts for water splitting

Electrons photoexcited in K(3)Ta(3)B(2)O(12), an efficient photocatalyst for the water-splitting reaction driven by ultraviolet light, were observed using time-resolved IR absorption spectroscopy with microsecond resolution. When the catalyst was irradiated with 266 nm light pulses, a structureless absorption appeared at 3000-1500 cm(-1). The absorption was assigned to the optical transition of electrons that were band gap-excited and then trapped in mid-gap states. The absorbance decayed with a time delay because of the electron-hole recombination. The rate of recombination in an argon atmosphere was sensitive to the composition of the starting material used in the catalyst preparation. The electron decay was accelerated by exposing the catalyst to water vapor. The degree of acceleration was qualitatively correlated with the H(2) production rate observed during steady-state light irradiation.     

Rhodium-catalyzed allyl transfer from homoallyl alcohols to aldehydes via retro-allylation followed by isomerization into ketones

Retro-allylation of homoallyl alcohol by rhodium catalysis occurs to generate allylrhodium species. This allylrhodium reacts with aldehydes to give the corresponding secondary alcohols in situ. Isomerization of these alcohols proceeds in the same pots to furnish the corresponding saturated ketones in good yields. [reaction: see text]     

Cobalt-mediated cross-coupling reactions of primary and secondary alkyl halides with 1-(trimethylsilyl)ethenyl- and 2-trimethylsilylethynylmagnesium reagents

[reaction: see text] This paper describes cobalt-mediated cross-coupling reactions of alkyl halides with 1-(trimethylsilyl)ethenylmagnesium bromide and 2-(trimethylsilyl)ethynylmagnesium bromide, respectively. The cobalt system allows for employing secondary as well as primary alkyl halides as the substrates. The reactions offer facile formations of alkyl-alkenyl and alkyl-alkynyl bonds. The reaction mechanism would include single-electron transfer from a cobalt complex to alkyl halide to generate the corresponding alkyl radical. The cobalt system thus enables sequential radical cyclization/alkenylation and cyclization/alkynylation reactions of 6-halo-1-hexene derivatives.     

Magnetic neutron scattering magnetic behaviour of a low-carrier density Kondo-lattice system ceas

Abstract

We have determined the magnetic structure of a low-carrier Kondo-lattice system CeAs, and have observed a softening of the crystalline electric field excitations. Despite the prediction of a recent magnetic polaron model in which CeAs and CeP are expected to show a stacking order of T₇ and T₈ layers, CeAs does not show such a stacking structure under pressure. The ordering in the intermediate phase is a regular ferromagnetic order and that of the low-temperature phase is a canted type-I AF.