The analogue of Weyl's conformal curvature tensor in a Michal functional geometry

The purpose of this note is to obtain a set of functionals conformally invariant in a Michal functional geometry. The author is indebted to prof.A. D. Michal for calling his attention to this problem and for helpful suggestions and criticisms in the preparation of this paper.     

Evidence for the decay D0-->K(-)pi(+)pi(-)e(+)nu(e)

Using a 281 pb{-1} data sample collected at the psi(3770) with the CLEO-c detector, we present the first absolute branching fraction measurement of the decay D0-->K(-)pi(+)pi(-)e(+)nu(e) at a statistical significance of about 4.0 standard deviations. We find 10 candidates consistent with the decay D0-->K(-)pi(+)pi(-)e(+)nu(e). The probability that a background fluctuation accounts for this signal is less than 4.1 x 10{-5}. We find B(D0-->K(-)pi(+)pi(-)e(+)nu(e)) = [2.8{-1.1}{+1.4}(stat)+/-0.3(syst)]x10{-4}. By restricting the invariant mass of the hadronic system to be consistent with K1(1270), we obtain the product of branching fractions B(D{0}-->K{1}{-}(1270)e{+}nu{e})xB(K1-(1270)-->K{-}pi{+}pi{-})=[2.5{-1.0}{+1.3}(stat)+/-0.2(syst)]x10{-4}. Using B(K1-(1270)-->K{-}pi{+}pi{-})=(33+/-3)%, we obtain B(D{0}-->K{1}{-}(1270)e{+}nu{e})=[7.6{-3.0}{+4.1}(stat)+/-0.6(syst)+/-0.7]x10{-4}. The last error accounts for the uncertainties in the measured K1-(1270)-->K{-}pi{+}pi{-} branching fractions.     

The turbulent wake of a circular cylinder rotating about the streamwise axis

This paper presents measurements in the turbulent wake of a circular cylinder rotating with its axis normal to the free-stream velocity; in other words, the axis of rotation was parallel to the streamwise direction. All three mean velocities and six Reynolds stresses were obtained at three positions downstream of the cylinder, with and without rotation of the free-stream. Most emphasis is given to the latter results because of the better flow quality. The ratio of the circumferential velocity of the cylinder to the free-stream velocity — the swirl number — had a maximum value of 0.6. Measurements for two combinations of the free-stream and angular velocities showed the velocity deficit in the wake to be a multi-valued function of the swirl number, implying that the rotation affected the separation of the cylinder's boundary layer in a complex manner. In the turbulent wake, the rotation did not significantly alter the magnitudes of the normal stresses, but caused large changes to the shape of the profiles of the axial and cross-stream normal stresses. Eventually, the primary (cross-stream) shear stress became almost entirely positive, but there was no corresponding change to the (cross-stream) gradient of the streamwise mean velocity. Despite these alterations to the turbulence, the rotationally-activated generation terms in the Reynolds transport equations never dominated the terms that are common to the wakes of rotating and non-rotating cylinders.This work was supported by the Australian Research Council. Most of the data acquisition software was written by Mr J. J. Smith.     

Designing the Molybdopterin Core through Regioselective Coupling of Building Blocks

Molybdopterin is an essential cofactor for all forms of life. The cofactor is composed of a pterin moiety appended to a dithiolene‐functionalized pyran ring, and through the dithiolene moiety it binds metal ions. Different synthetic strategies for dithiolene‐functionalized pyran precursors that have been designed and synthesized are discussed. These precursors also harbor 1,2‐diketone or osone functionality that has been condensed with 1,2‐diaminobenzene or other heterocycles resulting in several quinoxaline or pterin derivatives. Use of additives improves the regioselectivity of the complexes. The molecules have been characterized by ¹H and ¹³C NMR and IR spectroscopies, as well as by mass spectrometry. In addition, several compounds have been crystallographically characterized. The geometries of the synthesized molecules are more planar than the geometry of the cofactor found in proteins.     

Trifluoroethanol and 19F magic angle spinning nuclear magnetic resonance as a basic surface hydroxyl reactivity probe for zirconium(IV) hydroxide structures

A novel technique for determining the relative accessibility and reactivity of basic surface hydroxyl sites by reacting various zirconium(IV) hydroxide materials with 2,2,2-trifluoroethanol (TFE) and characterizing the resulting material using (19)F magic angle spinning (MAS) nuclear magnetic resonance (NMR) is presented here. Studied here are three zirconium hydroxide samples, two unperturbed commercial materials, and one commercial material that is crushed by a pellet press. Factors, such as the ratio of bridging/terminal hydroxyls, surface area, and pore size distribution, are examined and found to affect the ability of the zirconium(IV) hydroxide to react with TFE. X-ray diffraction, nitrogen isotherms, and (1)H MAS NMR were used to characterize the unperturbed materials, while thermogravitric analysis with gas chromatography and mass spectrometry along with the (19)F MAS NMR were used to characterize the materials that were reacted with TFE. Zirconium hydroxide materials with a high surface area and a low bridging/terminal hydroxyl ratio were found to react TFE in the greatest amounts.     

Comparison of solution and crystal structures of preQ1 riboswitch reveals calcium-induced changes in conformation and dynamics

Riboswitches regulate gene expression via specific recognition of cognate metabolites by their aptamer domains, which fold into stable conformations upon ligand binding. However, the recently reported solution and crystal structures of the Bacillus subtilis preQ(1) riboswitch aptamer show small but significant differences, suggesting that there may be conformational heterogeneity in the ligand-bound state. We present a structural and dynamic characterization of this aptamer by solution NMR spectroscopy. The aptamer-preQ(1) complex is intrinsically flexible in solution, with two regions that undergo motions on different time scales. Three residues move in concert on the micro-to-millisecond time scale and may serve as the lid of the preQ(1)-binding pocket. Several Ca(2+) ions are present in the crystal structure, one of which binds with an affinity of 47 ± 2 μM in solution to a site that is formed only upon ligand binding. Addition of Ca(2+) to the aptamer-preQ(1) complex in solution results in conformational changes that account for the differences between the solution and crystal structures. Remarkably, the Ca(2+) ions present in the crystal structure, which were proposed to be important for folding and ligand recognition, are not required for either in solution.     

Accurate ab initio ro-vibronic spectroscopy of the X̃2Π CCN radical using explicitly correlated methods

Explicitly correlated CCSD(T)-F12b calculations have been carried out with systematic sequences of correlation consistent basis sets to determine accurate near-equilibrium potential energy surfaces for the X(2)Π and a(4)Σ(-) electronic states of the CCN radical. After including contributions due to core correlation, scalar relativity, and higher order electron correlation effects, the latter utilizing large-scale multireference configuration interaction calculations, the resulting surfaces were employed in variational calculations of the ro-vibronic spectra. These calculations also included the use of accurate spin-orbit and dipole moment matrix elements. The resulting ro-vibronic transition energies, including the Renner-Teller sub-bands involving the bending mode, agree with the available experimental data to within 3 cm(-1) in all cases. Full sets of spectroscopic constants are reported using the usual second-order perturbation theory expressions. Integrated absorption intensities are given for a number of selected vibronic band origins. A computational procedure similar to that used in the determination of the potential energy functions was also utilized to predict the formation enthalpy of CCN, ΔH(f)(0K) = 161.7 ± 0.5 kcal/mol.     

Units of compatible nearrings

We study singly-generated wavelet systems on ${\mathbb {R}^2}$ that are naturally associated with rank-one wavelet systems on the Heisenberg group N. We prove a necessary condition on the generator in order that any such system be a Parseval frame. Given a suitable subset I of the dual of N, we give an explicit construction for Parseval frame wavelets that are associated with I. We say that ${g\in L^2(I\times \mathbb {R})}$ is Gabor field over I if, for a.e. ${\lambda \in I}$ , |??|^1/2 g(??, ·) is the Gabor generator of a Parseval frame for ${L^2(\mathbb {R})}$ , and that I is a Heisenberg wavelet set if every Gabor field over I is a Parseval frame (mother-)wavelet for ${L^2(\mathbb {R}^2)}$ . We then show that I is a Heisenberg wavelet set if and only if I is both translation congruent with a subset of the unit interval and dilation congruent with the Shannon set.     

Cupric superoxo-mediated intermolecular C-H activation chemistry

The new cupric superoxo complex [LCu(II)(O(2)(?-))](+), which possesses particularly strong O-O and Cu-O bonding, is capable of intermolecular C-H activation of the NADH analogue 1-benzyl-1,4-dihydronicotinamide (BNAH). Kinetic studies indicated a first-order dependence on both the Cu complex and BNAH with a deuterium kinetic isotope effect (KIE) of 12.1, similar to that observed for certain copper monooxygenases.