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31.
Molecular orbital calculations using CNDO/S parameters are employed to determine bond-orders, charge-densities and the shielding of the 15N and 13C nuclei of a series of ureas and thioureas. For the sterically uncrowded molecules a linear relationship is noticed between the 15N chemical shifts and C---N bond-orders. When steric crowding occurs this simple relationship is no longer applicable. 相似文献
32.
Michael R. Detty James W. Hassett Bruce J. Murray George A. Reynolds 《Tetrahedron》1985,41(21):4853-4859
The O-, S-, Se- and Te-containing Δ4,4' -2,2?,6,6'-tetramethyl-, -tetra-t-butyl- and -tetraphenyl-4-(chalcogenapyranyl)-4H-chalcogenapyrans were prepared from the corresponding chalcogenapyran-4-ones. The thia-, selena- and tellurapyran-4-ones were prepared by sodium borohydride reduction of the appropriate chalcogen and addition of the disodium chalcogenide to a 1,4-diyn-3-one. The comparative electrochemistry of all three series was examined by cyclic voltammetry. Within each scries the first oxidation (E1) became more difficult with increasing chalcogen size. The radical-cation states of the tetra-t-butyl analogues were examined by ESR. The O and S analogues gave well-defined five-line spectra, but the Se and Te analogues gave broad single lines. The g value increased with increasing size of the heteroatom. A linear correlation exists between g value and spin-orbit coupling constants λ for the chalcogens, suggesting that the electron densities on the heteroatoms are similar in each heteroatom analogue. 相似文献
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Bricaud Q Fabre RM Brookins RN Schanze KS Reynolds JR 《Langmuir : the ACS journal of surfaces and colloids》2011,27(8):5021-5028
We present a study of Fo?rster resonance energy transfer (FRET) between two emissive conjugated polyelectrolytes (CPEs) in layer-by-layer (LbL) self-assembled films as a means of examining their organization and architecture. The two CPEs are a carboxylic acid functionalized polyfluorene (PFl-CO(2)) and thienylene linked poly(phenylene ethynylene) (PPE-Th-CO(2)). The PFl-CO(2) presents a maximum emission at 418 nm, while the PPE-Th-CO(2) has an absorption λ(max) centered at 431 nm, in sufficient proximity for effective FRET. Several LbL films have been constructed using varied concentrations of the deposition solutions and identity of the buffer layers separating the two emissive layers, using a system of either weak polyelectrolytes, poly(allylamine hydrochloride) (PAH)/poly(sodium methacrylate) (PMA), or strong polyelectrolytes, poly(diallylammonium chloride) (PDDA)/poly(styrene sulfonate) sodium (PSS). The efficiency of FRET has been monitored using fluorescence spectroscopy. Initially, the fluorescence of the PFl-CO(2) (E(g) ~ 3.0 eV), which emits at 420 nm, is quenched by the lower band gap PPE-Th-CO(2) (E(g) ~ 2.5 eV). For films using the PAH/PMA system as buffer bilayers and deposited from 1 mM solutions, the PFl-CO(2) fluorescence is progressively recovered as the number of intervening buffer bilayers is increased. Ellipsometry measurements indicate that energy transfer between the two emissive layers is efficient to a distance of ca. 7 nm. 相似文献
35.
The axial resolution of optical coherence tomography images is primarily dependent on the bandwidth of the illumination source. Continuum generation is one way to generate the single-mode, high-bandwidth light needed for point illumination. We present an inexpensive and easy-to-implement augmentation to a Ti:sapphire laser that widens the bandwidth from 20 to over 200 nm with commerically available ultrahigh-numerical-aperture fiber. This technique can provide a readily available broad-bandwidth source for researchers and a practical enhancement to a fiber-optic optical coherence tomography system. 相似文献
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Wear KA Laib A Stuber AP Reynolds JC 《The Journal of the Acoustical Society of America》2005,117(5):3319-3324
Biot's theory for elastic propagation in porous media has previously been shown to be useful for modeling the dependence of phase velocity on porosity in bovine cancellous bone in vitro. In the present study, Biot's theory is applied to measurements of porosity-dependent phase velocity in 53 human calcanea in vitro. Porosity was measured using microcomputed tomography for some samples (n = 23) and estimated based on bone mineral densitometry for the remaining samples (n = 30). The phase velocity at 500 kHz was measured in a water tank using a through-transmission technique. Biot's theory performed well for the prediction of the dependence of sound speed on porosity. The trend was quasilinear, but both the theory and experiment show similar slight curvature. The root mean square error (RMSE) of predicted versus measured sound speed was 15.8 m/s. 相似文献
40.
Reynolds AM 《Journal of colloid and interface science》2004,275(1):328-335
The statistical properties of fluid velocities along particle trajectories in turbulent flows have a conditional dependency upon particle velocity. It is shown that the formulation of Lagrangian stochastic (LS) models for particle trajectories in terms of the well-mixed condition for these conditional velocity statistics is exactly analogous to the formulation of second-order LS models for fluid-particle trajectories. The particle aerodynamic response time is shown to be incorporated at second order, which together with the Lagrangian timescale introduced at first order, defines the Stokes number. Reynolds-number effects can be incorporated at third order. The corresponding Fokker-Planck equation is shown to be identical to that advocated by Pozorski and Minier [Phys. Rev. E 59 (1999) 855], who included the fluid velocities "seen" by a particle in the probability density function (pdf) formalism of Reeks and co-workers as a means of circumventing the closure problem (prescribing a closure for the particle flux induced by the fluid) associated with that approach. It is demonstrated that the neglect of Stokes-number effects accounts, in part, for the tendency of first-order LS models to underpredict particle deposition velocities in the diffusion-impaction regime. 相似文献