Catechol-TiO₂ hybrids for photocatalytic H₂ production and photocathode assembly

Visible-light driven H₂ evolution in water is achieved using catechol-photosensitised TiO₂ nanoparticles with a molecular nickel catalyst. Layer-by-layer immobilisation of catechol-TiO₂ onto tin-doped indium oxide electrodes generates photocathodic currents in the presence of an electron acceptor. This approach represents a new strategy for controlling photocurrent direction in dye-sensitised photoelectrochemical applications.We gratefully acknowledge financial support by the EPSRC and World Premier International Research Center Initiative, MEXT, Japan

Scope and Mechanistic Study of the Coupling Reaction of α,β-Unsaturated Carbonyl Compounds with Alkenes: Uncovering Electronic Effects on Alkene Insertion vs Oxidative Coupling Pathways

The cationic ruthenium-hydride complex [(C6H6)(PCy3)(CO)RuH]+BF4– (1) was found to be a highly effective catalyst for the intermolecular conjugate addition of simple alkenes to α,β-unsaturated carbonyl compounds to give (Z)-selective tetrasubstituted olefin products. The analogous coupling reaction of cinnamides with electron-deficient olefins led to the oxidative coupling of two olefinic C–H bonds in forming (E)-selective diene products. The intramolecular version of the coupling reaction efficiently produced indene and bicyclic fulvene derivatives. The empirical rate law for the coupling reaction of ethyl cinnamate with propene was determined as follows: rate = k[1]1[propene]0[cinnamate]−1. A negligible deuterium kinetic isotope effect (kH/kD = 1.1 ± 0.1) was measured from both (E)-C6H5CH═C(CH3)CONHCH3 and (E)-C6H5CD═C(CH3)CONHCH3 with styrene. In contrast, a significant normal isotope effect (kH/kD = 1.7 ± 0.1) was observed from the reaction of (E)-C6H5CH═C(CH3)CONHCH3 with styrene and styrene-d8. A pronounced carbon isotope effect was measured from the coupling reaction of (E)-C6H5CH═CHCO2Et with propene (13C(recovered)/13C(virgin) at Cβ = 1.019(6)), while a negligible carbon isotope effect (13C(recovered)/13C(virgin) at Cβ = 0.999(4)) was obtained from the reaction of (E)-C6H5CH═C(CH3)CONHCH3 with styrene. Hammett plots from the correlation of para-substituted p-X-C6H4CH═CHCO2Et (X = OCH3, CH3, H, F, Cl, CO2Me, CF3) with propene and from the treatment of (E)-C6H5CH═CHCO2Et with a series of para-substituted styrenes p-Y-C6H4CH═CH2 (Y = OCH3, CH3, H, F, Cl, CF3) gave the positive slopes for both cases (ρ = +1.1 ± 0.1 and +1.5 ± 0.1, respectively). Eyring analysis of the coupling reaction led to the thermodynamic parameters, ΔH⧧ = 20 ± 2 kcal mol–1 and ΔS⧧ = −42 ± 5 eu. Two separate mechanistic pathways for the coupling reaction have been proposed on the basis of these kinetic and spectroscopic studies

Observation of Large CP Violation in the Neutral B Meson System

We present a measurement of the Standard Model CP violation parameter sin 2phi_1 based on a 29.1 fb^{-1} data sample collected at the Upsilon(4S) resonance with the Belle detector at the KEKB asymmetric-energy e+e- collider. One neutral B meson is fully reconstructed as a J/psi Ks, psi(2S) Ks, chi_c1 Ks, eta_c Ks, J/psi K_L or J/psi K^{*0} decay and the flavor of the accompanying B meson is identified from its decay products. From the asymmetry in the distribution of the time intervals between the two B meson decay points, we determine sin 2phi_1 = 0.99 +- 0.14(stat) +- 0.06(syst). We conclude that we have observed CP violation in the neutral B meson system.Comment: 4 figures, to appear in Phys. Rev. Letter

Observation of the decay B^0->D+D*-

We report the first observation of the decay B^0->D+-D*-+ with the Belle detector at the KEKB e^+e^- collider operated at the Upsilon(4S) resonance. The sum of branching fractions B(B^0->D+D*-)+B(B^0->D-D*+) is measured to be (1.17+-0.26+0.22-0.25)x10^-3 using the full reconstruction method where both charmed mesons from B^0 decays are reconstructed. A consistent value ((1.48+-0.38+0.28-0.31)x10^-3) is obtained using a partial reconstruction technique that only uses the slow pion from the D*- ->bar D^0pi- decay and a fully reconstructed D+ to reconstruct the B^0.Comment: 10 pages, 3 figure

Observation of Double cc bar Production in e+ e- Annihilation at sqrt{s} ~ 10.6 GeV

We report the observation of prompt J/psi via double ccbar production from the e+e- continuum. In this process one ccbar pair fragments into a J/psi meson while the remaining pair either produces a bound charmonium state or fragments into open charm. Both cases have been observed: the first by studying the mass spectrum of the system recoiling against the J/psi, and the second by reconstructing the J/psi together with a charmed meson. We find cross-sections of \sigma(e+ e- -> J/psi eta_c (gamma)) * BR (eta_c -> >=4 charged) = 0.033 (+0.007 -0.006)(stat) \pm 0.009(syst)pb and \sigma(e+ e- -> J/psi D*+ X) = 0.53 (+0.19 -0.15)(stat) \pm 0.14(syst) pb, and infer \sigma(e+ e- -> J/psi c cbar) / \sigma(e+ e- -> J/psi X) = 0.59 (+0.15 -0.13)(stat) \pm 0.12(syst). These results are obtained from a 46.2/fb data sample collected near the Upsilon(4S) resonance, with the Belle detector at the KEKB asymmetric energy e+ e- collider.Comment: 7 pages, 2 figures, to be submitted to Physical Review Letter

Observation of the eta_c(2S) in exclusive B-->K KsK-pi+ decays

We report the observation of a narrow peak in the KsK-pi+ invariant mass distribution in a sample of exclusive B-->K KsK-pi+ decays collected with the Belle detector at the KEKB asymmetric energy e+e- collider. The measured mass of the peak is M=3654+-6(stat)+-8(syst) MeV/c^2 and we place a 90% confidence level upper limit on the width of Gamma<55 MeV/c^2. The properties agree with heavy-quark potential model expectations for the eta_c(2S), the n=2 singlet S charmonium state.Comment: 10 pages, 3 figures, submitted to Physical Review Letter

Study of Exclusive B decays to Charmed Baryons

Using 29.1fb-1 of data accumulated at the Upsilon(4S) with the Belle detector at KEKB, we have studied the decay modes B0bar->Lambda_c+ pbar pi+pi-, B- -> Lambda_c+ pbar pi-, and B0bar ->Lambda_c+ pbar. We report branching fractions of exclusive B decays to charmed baryons with four-, three- and two-body final states, including intermediate Sigma_c++ and Sigma_c0 states. We observed B0bar -> Sigma_c(2455)++pbar pi- for the first time with a branching fraction of (2.38+0.63-0.55+-0.41+-0.62)x10-4 and observed evidence for the two-body decay B- ->Sigma_c(2455)0 pbar with a branching fraction of (0.45+0.26-0.19+-0.07+-0.12)x10-4. We also set improved upper limits for the two-body decays B0bar -> Lambda_c+ pbar and B- -> Sigma_c(2520)0 pbar.Comment: accepted for publication in Phys. Rev.

Measurement of Inclusive Production of Neutral Pions from Upsilon(4S) Decays

Using the Belle detector operating at the KEKB e+e- storage ring, we have measured the mean multiplicity and the momentum spectrum of neutral pions from the decays of the Upsilon(4S) resonance. We measure a mean of 4.70 +/- 0.04 +/- 0.22 neutral pions per Upsilon(4S) decay.Comment: 15 pages, 4 figs. Submitted to Phys.Rev.