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81.
A. D. Rogers 《Acta Mathematica Hungarica》2006,110(1-2):13-21
Summary A lower bound is established for the strip discrepancy of a broad class of point distributions. The bound implies unbounded
strip discrepancy for equally weighted point distributions under favorable conditions. The methods of proof use notions from
integral geometry. 相似文献
82.
Many of the proprietary additive formulations that have been proposed to control the properties of metal electrodeposits include water soluble macromolecules. Among these are the hydrodynamically interesting polyethylene glycols ‘Polyox’. In the course of a rotating disk electrode study of the effects of additives in copper electrodeposition the present authors had cause to try the effects of low concentrations of Polyox in an acid copper sulphate plating solution. In the presence of an essential trace of chloride ion Polyox very strongly inhibited deposition below a critical overpotential at which current density rises extremely rapidly with increasing overpotential. These results suggest that below the critical overpotential chloride ions hold a film of Polyox onto the electrode surface and may also give the film some lateral cohesion. The film may be a Polyox-cuprous chloride complex. Striking spiral patterns form at the critical overpotential. Their characteristics are explained as the consequences of electrodeposition on a surface containing submicroscopic protrusions and depressions in conditions where current density increases very rapidly with potential. 相似文献
83.
Rogers JE Slagle JE McLean DG Sutherland RL Brant MC Heinrichs J Jakubiak R Kannan R Tan LS Fleitz PA 《The journal of physical chemistry. A》2007,111(10):1899-1906
A comprehensive photophysical study of the linear and nonlinear absorption properties has been carried out on two series of two-photon absorbing dyes to gain insight into how structure-property relationships influence observed nonlinear absorption. The materials studied consist of an electron accepting benzothiazole group connected to an electron donating diphenylamine via a fluorene bridging group. Two series differ from each other by the addition of one phenyl group and for each series one-arm (dipolar, AF240 and AF270), two-arm (quadrupolar, AF287 and AF295), and three-arm (octupolar, AF350 and AF380) versions were studied. Overall the AF240 series exhibits higher intrinsic two-photon absorption (TPA) cross-sections than the AF270 series as well as enhanced nanosecond nonlinear absorption, with an increase with number of branches. The enhanced nanosecond nonlinearity is understood by taking into account the contribution from the singlet and triplet excited states and was verified by a two-photon assisted excited-state absorption model that satisfactorily predicts the nonlinear absorption of the chromophores. 相似文献
84.
D'Souza F Rogers LM O'Dell ES Kochman A Kutner W 《Bioelectrochemistry (Amsterdam, Netherlands)》2005,66(1-2):35-40
Two different fullerene film-modified electrodes were prepared and used for surface immobilization and electrochemical property investigation of horse heart cytochrome c (cyt c). Both a pristine fullerene film and fullerene-palladium (C(60)-Pd) polymer film-modified platinum, glassy carbon and indium-tin-oxide (ITO) electrodes were used. The immobilized cyt c was characterized by piezoelectric microgravimetry at a quartz crystal microbalance (QCM), UV-visible absorption, and X-ray photoelectron spectroscopy (XPS), as well as cyclic voltammetry (CV) techniques. The UV-visible spectral studies revealed a small blue shift of both the Soret and Q band of the heme moiety of cyt c, immobilized on the C(60)-Pd polymer film-modified ITO electrode, as compared to the bands of cyt c in solution suggesting that molecules of cyt c are densely packed onto the surface of the modified electrode. The CV studies revealed a quasi-reversible electrode behavior of the heme moiety indicating the occurrence of kinetically hindered electron transfer. A good agreement was found between the values of cyt c electrode surface coverage determined by piezoelectric microgravimetry and cyclic voltammetry. For piezoelectric microgravimetry, these values ranged from 0.5 x 10(-10) to 2.5 x 10(-10) mol cm(-2), depending upon the amount of cyt c present in solution and the time allowed for immobilization, which compared with a value of 3.6+/-0.4 x 10(-10) mol cm(-2) determined by CV. The possible mechanisms of cyt c immobilization on the C(60) film and C(60)-Pd film-modified electrodes are also discussed. 相似文献
85.
Integrated within an appropriate theoretical framework, molecular dynamics (MD) simulations are a powerful tool to complement experimental studies of solvation dynamics. Together, experiment, theory, and simulation have provided substantial insight into the dynamic behavior of polar solvents. MD investigations of solvation dynamics are especially valuable when applied to the heterogeneous environments found in biological systems, where the calculated response of the environment to the electrostatic perturbation of the probe molecule can easily be decomposed by component (e.g., aqueous solvent, biomolecule, ions), greatly aiding the molecular-level interpretation of experiments. A comprehensive equilibrium and nonequilibrium MD study of the solvation dynamics of the fluorescent dye Hoechst 33258 (H33258) in aqueous solution is presented. Many fluorescent probes employed in experimental studies of solvation dynamics in biological systems, such as the DNA minor groove binder H33258, have inherently more conformational flexibility than prototypical fused-ring chromophores. The role of solute flexibility was investigated by developing a fully flexible force-field for the H33258 molecule and by simulating its solvation response. While the timescales for the total solvation response calculated using both rigid (0.16 and 1.3 ps) and flexible (0.17 and 1.4 ps) models of the probe closely matched the experimentally measured solvation response (0.2 and 1.2 ps), there were subtle differences in the response profiles, including the presence of significant oscillations for the flexible probe. A decomposition of the total response of the flexible probe revealed that the aqueous solvent was responsible for the overall decay, while the oscillations result from fluctuations in the electrostatic terms in the solute intramolecular potential energy. A comparison of equilibrium and nonequilibrium approaches for the calculation of the solvation response confirmed that the solvation dynamics of H33258 in water is well-described by linear response theory for both rigid and flexible models of the probe. 相似文献
86.
This study applies the theory of stochastic processes to the equilibrium statistical physics of polymers in solution. The topics treated include random copolymers and randomly branching polymers, with self-consistent mean field effects. A new and more natural way of dealing with Boltzmann weighting is discussed, which makes it possible from the beginning of a calculation to consider only the physical polymer conformations. We also show that in general the random copolymer problem can be reduced to the ordinary polymer problem, and treat the self-consistent field problem for a general branching polymer. 相似文献
87.
The reaction of the diazo compounds 1a-o with 4-phenyl-1,2,4-triazolin-3,5-dione (2) in dichloromethane-ethanol leads to the urazoles 5a-o; they arise from the primarily formed unstable azomethinhnine dipoles 4a-o by ethanol addition. Acidic hydrolysis of 5k and 5o yields the α-diketones 8 and 10 besides 4-phenyl urazole (9). Bistriazolindiones (13a,b) react analogously with diazo compounds (1l, m) in the presence of ethanol to give the bisurazoles 14a-c. 相似文献
88.
89.
The infrared (IR)-vacuum ultraviolet (VUV)-pulsed field ionization-photoelectron (IR-VUV-PFI-PE) spectrum for C2H4(X1A(g), v11 = 1, N'(Ka'Kc') = 3(03)) in the VUV range of 83,000-84,800 cm(-1) obtained using a single mode infrared laser revealed 24 rotationally resolved vibrational bands for the ion C2H4(+)(X2B(3u)) ground state. The frequencies and symmetry of the vibrational bands thus determined, together with the anharmonic frequency predictions calculated at the CCSD(T)/aug-cc-pVQZ level, have allowed the unambiguous assignment of these vibrational bands. These bands are mostly combination bands. The measured frequencies of these bands yield the fundamental frequencies for v8+ = 1103 +/- 10 cm(-1) and v10+ = 813 +/- 10 cm(-1) of C2H4(+)(X2B(3u)), which have not been determined previously. The present IR-VUV-PFI-PE study also provides truly rovibrationally selected and resolved state-to-state cross sections for the photoionization transitions C2H4(X1A(g); v11, N'(Ka'Kc')) --> C2H4(+)(X2B(3u); vi+, N+(Ka+Kc+)), where N'(Ka'Kc') denotes the rotational level of C2H4(X1A(g); v11), and vi+ and N+(Ka+Kc+) represent the vibrational and rotational states of the cation. 相似文献
90.
Kim In S. Barrow Kevin D. Rogers Peter L. 《Applied biochemistry and biotechnology》2000,84(1-9):357-370
The fermentation characteristics and effects of lignocelulosic toxic compounds on recombinant Zymomonas mobilis ZM4(pZB5), which is capable of converting both glucose and xylose to ethanol, and its parental strain, ZM4, were characterized
using 13C and 31P nuclear magnetic resonance (NMR) in vivo. From the 31P NMR data, the levels of nucleoside triphosphates (NTP) of ZM(pZB5) using xylose were lower than those of glucose. This can
be related to the intrinsically slower assimilation and/or metabolism of xylose compared to glucose and is evidence of a less
energized state of ZM4(pZB5) cells during xylose fermentation. Acetic acid was shown to be strongly inhibitory to ZM4(pZB5)
on xylose medium, with xylose utilization being completely inhibited at pH 5.0 or lower in the presence of 10.9 g/L of sodium
acetate. From the 31P NMR results, the addition of sodium acetate caused decreased NTP and sugar phosphates, together with acidification of the
cytoplasm. Intracellular deenergization and acidification appear to be the major mechanisms by which acetic acid exerts its
toxic effects on this recombinant strain. 相似文献