Demonstration of a simple entangling optical gate and its use in bell-state analysis

We demonstrate a new architecture for an optical entangling gate that is significantly simpler than previous realizations, using partially polarizing beam splitters so that only a single optical mode-matching condition is required. We demonstrate operation of a controlled-z gate in both continuous-wave and pulsed regimes of operation, fully characterizing it in each case using quantum process tomography. We also demonstrate a fully resolving, nondeterministic optical Bell-state analyzer based on this controlled-z gate. This new architecture is ideally suited to guided optics implementations of optical gates.     

Search for the lepton-number-violating decay Xi(-)-->pmu(-)mu(-)

A sensitive search for the lepton-number-violating decay Xi(-)-->pmu(-)mu(-) has been performed using a sample of approximately 10(9) Xi(-) hyperons produced in 800 GeV/c p-Cu collisions. We obtain B(Xi(-)-->pmu(-)mu(-))<4.0x10(-8) at 90% confidence, improving on the best previous limit by 4 orders of magnitude.     

Terahertz wide aperture reflection tomography

We describe a powerful imaging modality for terahertz (THz) radiation, THz wide aperture reflection tomography (WART). Edge maps of an object's cross section are reconstructed from a series of time-domain reflection measurements at different viewing angles. Each measurement corresponds to a parallel line projection of the object's cross section. The filtered backprojection algorithm is applied to recover the image from the projection data. To our knowledge, this is the first demonstration of a reflection computed tomography technique using electromagnetic waves. We demonstrate the capabilities of THz WART by imaging the cross sections of two test objects.     

Ultrasound-assisted hydrogenation of cinnamaldehyde

The hydrogenation, employing hydrogen gas, of cinnamaldehyde was performed using Pd-black and Raney Ni catalysts at 298+/-3 K in a water-cooled (jacketed) reaction vessel. Sampling at pre-determined time intervals and GC/MS analysis yielded time-dependent product state distribution information. A kinetic modeling of the data revealed that cinnamaldehyde was both hydrogenated directly to the final product benzenepropanol, as well as a fraction being converted to the intermediate benzenepropanal, where the latter was subsequently hydrogenated to benzenepropanol. Comparing the ultrasound-assisted and blank (stirred) experiments revealed that a higher maximum relative concentration of the intermediate benzenepropanal was formed in the ultrasound experiments compared to the stirred experiment. The activity of the ultrasound experiments compared to blank were 9-fold and 20-fold greater for the Pd-black and Raney Ni catalysts, respectively. Finally, an application of the Bell-Evans-Polanyi principle to yield an estimate of the ratio of rate coefficients for benzenepropanal and benzenepropanol formation was performed by considering chemical group energy differences and surface adsorption energy differences in the first mechanistic step of hydrogenation.     

Characterisation of derivatised monomeric and prepolymeric isocyanates by matrix-assisted laser desorption/ionisation time-of-flight mass spectrometry and structural elucidation by tandem mass spectrometry

Isocyanates are an important class of compounds in occupational hygiene monitoring due mainly to their behaviour as respiratory sensitisers. Here, we demonstrate the application of matrix-assisted laser desorption/ionisation mass spectrometry (MALDI-MS) and MALDI tandem mass spectrometry (MS-MS) to the analysis of derivatised isocyanate monomers and prepolymers. The aim of the work has been to gauge the selectivity obtainable from the direct analysis of isocyanate mixtures without prior separation. Monomeric and prepolymeric isocyanate mixtures were analysed as their 1-(2-methoxyphenyl) piperazine derivatives and the potential of MALDI time-of-flight (ToF)-MS for an NCO monitoring program was assessed. The results obtained demonstrated the possibility of direct mixture analysis by this method. MALDI-MS-MS was used for the elucidation of fragment structures in the prepolymer samples. The developed methodology was then applied to the analysis of swabs from an occupational hygiene monitoring scheme and enabled the identification of the isocyanate species detected.     

A study of N-nitrosoamide-mediated friedel-crafts type benzylation of benzene-toluene and benzene-Anisole(1)(a)

Nitrogen-separated carbocation-carboxylate ion pairs were employed as sources of carbocations in the alkylation of aromatic compounds. The N-nitrosoamide approach to these nitrogenous-molecule-separated ion pairs is an excellent alternative to the standard acid-catalyzed Friedel-Crafts approach for studies of the alkylation because of the following variables: high reactivity of the electrophile, stability of the products, strict kinetic control, homogeneity, lack of overalkylation, straightforward chemistry, and good product balance. In deaminative benzylations of benzene-toluene and anisole-benzene mixtures, the values of k(X)/k(B) and % meta isomer are significantly different from those observed in the standard benzylations in a manner that indicates the deaminative electrophiles are more reactive than those generated by the standard Friedel-Crafts approach. The reactions show a direct proportionality between inter- and intramolecular selectivities and thus follow the Brown selectivity relationship (BSR). The benzylation of 2,4, 6-trideuteriotoluene provided no evidence for deuterium rearrangements (or coupled benzyl rearrangements) in the arenium ion intermediate. Kinetic isotope effects were not detected. The methyl substituent on toluene appears to affect intermolecular selectivity (k(T)/k(B)) and intramolecular selectivity (o, m, p distribution) to similar degrees. A mechanism is proposed in which both selectivities are determined by activation energy differences in the transition states leading to the sigma-complex intermediates. The observation that most standard Friedel-Crafts benzylations do not follow the BSR is discussed in terms of possible systematic errors in those cases. Silver ion-assisted Friedel-Crafts benzylations were performed under dry, basic conditions to investigate whether the standard approach could lead to data that obey the BSR.     

Mechanism and molecular-electronic structure correlations in a novel series of osmium(V) hydrazido complexes

Reaction between the Os(VI) nitrido (OsVI identical to N+) complexes [OsVI(L3)(Cl)2(N)]+ (L3 is 2,2':6',2"-terpyridine (tpy) or tris(1-pyrazolyl)methane (tpm)) and secondary amines (HN(CH2)4O = morpholine, HN(CH2)4CH2 = piperidine, and HN(C2H5)2 = diethylamine) gives Os(V)-hydrazido complexes, [OsV(L3)(Cl)2(NNR2)]+ (NR2 = morpholide, piperidide, or diethylamide). They can be chemically or electrochemically oxidized to Os(VI) or reduced to Os(IV) and Os(III). The Os-N bond lengths and Os-N-N angles in the structures of these complexes are used to rationalize the bonding between the dianionic hydrazido ligand and Os. The rate law for formation of the Os(V) hydrazido complexes with morpholine as the base is first order in [OsVI(L3)(Cl)2(N)]+ and second order in HN(CH2)4O with ktpy(25 degrees C, CH3CN) = (581 +/- 12) M-2 s-1 and ktpm(25 degrees C, CH3CN) = 2683 +/- 40 M-2 s-1. The proposed mechanism involves initial nucleophilic attack of the secondary amine on the Os(VI) nitrido group to give a protonated Os(IV)-hydrazido intermediate. It is subsequently deprotonated and then oxidized by OsVI identical to N+ to Os(V). The extensive redox chemistry for these complexes can be explained by invoking a generalized bonding model. It can also be used to assign absorption bands that appear in the electronic from the visible-near-infrared spectra including a series of d pi-->d pi interconfigurational bands at low energy.     

The size of the singular set in mean curvature flow of mean-convex sets

We prove that when a compact mean-convex subset of (or of an -dimensional riemannian manifold) moves by mean-curvature, the spacetime singular set has parabolic hausdorff dimension at most . Examples show that this is optimal. We also show that, as , the surface converges to a compact stable minimal hypersurface whose singular set has dimension at most . If , the convergence is everywhere smooth and hence after some time , the moving surface has no singularities

     

First On-line beta-NMR on oriented nuclei: magnetic dipole moments of the (nup(1/2))(-1) 1/2(-) ground state in 67Ni and (pip(3/2))(+1) 3/2(-) ground state in 69Cu

The first fully on-line use of the angular distribution of beta emission in detection of NMR of nuclei oriented at low temperatures is reported. The magnetic moments of the single valence particle, intermediate mass, isotopes 67Ni(nup(-1)(1/2);1/2(-)) and 69Cu(pip(1)(3/2);3/2(-)) are measured to be +0.601(5) &mgr;(N) and +2.84(1) &mgr;(N), respectively, revealing only a small deviation from the neutron p(1/2) single-particle value in the former and a large deviation from the proton p(3/2) single-particle value in the latter. Quantitative interpretation is given in terms of core polarization and meson-exchange currents.     

Gamma-ray spectra and positive parity bands in 158Gd

A Ge(Li)-NaI(Tl) pair spectrometer and a Ge(Li)-NaI(Tl) anti-Compton spectrometer were used to measure γ-rays from the reaction ¹⁵⁷Gd(n, γ)¹⁵⁸Gd. A detailed decay scheme for levels of ¹⁵⁸Gd was constructed up to an excitation energy of 2504 keV. Branching ratios for transitions from members of the positive parity bands to members of the ground state band were determined. It is shown that a single band-mixing parameter is not sufficient to explain the experimental results, and that even a four-band-mixing calculation does not provide satisfactory agreement. The binding energy of the last neutron is determined to be 7937.4±0.7 keV.