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1.
H.W. Galbraith C.W. Patterson B.J. Krohn W.G. Harter 《Journal of Molecular Spectroscopy》1978,73(3):475-493
For states of high angular momentum we obtain expressions for the transition frequencies in the triply degenerate fundamental of a “heavy” spherical top, that are accurate to spectroscopic resolution, without tedious calculation of octahedral (or tetrahedral) vector coupling coefficients or diagonalization of matrices. Our calculations are based upon the physical assumption that as the molecule rotates with larger angular momentum it behaves like a symmetric top with the coupled pure rotational angular momentum quantized along either the four- or threefold body-fixed axes. We find that the approximate calculation which involves only 3-J symbols quite accurately reproduces the result of a complete diagonalization of the Hamiltonian, so that for all but the most accurate saturated absorption spectra theoretical analysis may be carried out without reference to the octahedral (or tetrahedral) subgroup of the rotation group. 相似文献
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We report the observation of giant quantum coherence effects in the localized modes of ionized hydrogen in synthetic fluorite. Infrared free induction decay experiments on the substitutional H- center show dramatic modulations at negative delay times due to interference between multiple vibrational levels. Spectrally resolving the degenerate four wave mixing signal allows unambiguous assignments of the participating vibrational states. The dependence of the signal intensity upon the delay path between the exciting free electron laser pulses can be accounted for in terms of the resonant third order polarization with a common dephasing time for the excited states. 相似文献
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Watari M Galbraith J Lang HP Sousa M Hegner M Gerber C Horton MA McKendry RA 《Journal of the American Chemical Society》2007,129(3):601-609
Free-standing cantilevers, which directly translate specific biochemical reactions into micromechanical motion, have recently attracted much attention as label-free biosensors and micro/nano robotic devices. To exploit this mechanochemical sensing technology, it is essential to develop a fundamental understanding of the origins of surface stress. Here we report a detailed study into the molecular basis of stress generation in aqueous environments focusing on the pH titration of model mercaptohexadecanoic acid self-assembled monolayers (SAMs), using in situ reference cantilevers coated with nonionizable hexadecanethiol SAMs. Semiautomated data analysis and a statistical model were developed to quantify cyclic deprotonation/protonation reactions on multiple arrays. In-plane force titrations were found to have the sensitivity to detect ionic hydrogen bond formation between protonated and nonprotonated carboxylic acid groups in the proximity of the surface pK1/2, which generated a mean tensile differential surface stress of +1.2 +/- 0.3 mN/m at pH 6.0, corresponding to 1 pN attractive force between two adjacent MHA molecules. Conversely, the magnitude of compressive differential surface stress was found to increase progressively with pH >/= 7.0, reaching a maximum of -14.5 +/- 0.5 mN/m at pH 9.0, attributed to enhanced electrostatic repulsion between deprotonated carboxylic acid groups. However, striking differences were observed in the micromechanical responses to different ionic strength and ion species present in the aqueous environment, highlighting the critical role of counter- and co-ions on surface stress. Our findings provide fundamental insights into the molecular mechanisms of in-plane mechanochemistry, which may be exploited for biosensing and nanoactuation applications. 相似文献
6.
10,25-Di-tert-alkyl-14,21-dimethyl-3,6,14,21-tetraazatricyclo[21.3.1.18,12]octacosa-1(27),2,6,8,10,12(28),23,25-octaene-27,28-diol macrocycles form Ni(II) and Cu(II) complexes in which the metal cation and the sulfate anion are bound in separated sites in a zwitterionic form of the ligand. The nonyl-substituted macrocycle shows a higher affinity for SO(4)(2-) and a lower binding strength for Cu(2+) than open chain analogues, the pH-dependences for which fall in ranges which allow loading of CuSO(4) at pH approximately 4 and easy stripping to recycle the ligand. X-Ray structure determinations of the Cu(II) and Ni(II) sulfate complexes of the tert-butyl substituted ligand suggest that the de-tuning of M(2+)-binding results from a distortion from planarity of the "salen" N(2)O(2)(2-) donor set imposed by the incorporation of the hexamethylene strap in the ligand and reveal that the sulfate is bound as a hydrate in a 2:2:2:2, ligand-M(2+)-SO(4)(2-)-H(2)O, assembly. 相似文献
7.
Galbraith SG Wang Q Li L Blake AJ Wilson C Collinson SR Lindoy LF Plieger PG Schröder M Tasker PA 《Chemistry (Weinheim an der Bergstrasse, Germany)》2007,13(21):6091-6107
Amide-functionalised salen ligands capable of extracting metal salts have been synthesised and characterised. Single-crystal X-ray structure determinations of complexes of NiSO4, [Ni(L)(SO4)], confirm that the ionophores are in a zwitterionic form with Ni(II) bound in the deprotonated salen moiety and the SO4(2-) ion associated with protonated pendant N'-amidopiperazine groups. Treatment of [Ni(L)(SO4)] with base removes the protons from the pendant amido-amine group resulting in loss of the SO4(2-) ion and formation of metal-only complexes of type [Ni(L-2H)], which have been characterized by single-crystal X-ray diffraction. Three of the ligands with solubilities suitable for solvent extraction studies show loading and stripping pH-profiles that are suitable for the recovery of CuSO4 or CuCl2 from industrial leach solutions. The copper-only complexes, [Cu(L-2H)], are selective for Cl- over SO4(2-) in both solvent extraction and bulk liquid membrane transport experiments and were found to bind Cl- in two steps via the formation of a 1:1:1 [Cu(L-H)Cl] assembly, followed by a 1:1:2 [Cu(L)Cl2] assembly as the pH of the aqueous phase is lowered. The anion transport selectivity was evaluated for a number of other mono-charged anions and interestingly the ligands were found to display a preference for the Br- ion. To probe the influence of the Hofmeister bias on the selectivity of anion complexation, single-phase potentiometric titration experiments were employed to investigate the binding of SO4(2-) and Cl- by one of the copper only complexes, [Cu(L-2H)] in 95 %/5 % MeOH/water. Under these conditions selectivity was reversed (SO4(2-)>Cl-) confirming that the Hofmeister bias, which reflects the relative hydration energies of the anions, dominates the selectivity of anion extraction from aqueous media into CHCl3. 相似文献
8.
Lipschitz regularity for solutions to nonsmooth problems in the calculus of variations is considered, where we allow for extended-real-valued Lagrangians. Conditions for regularity are given in terms of subdifferentiability properties of the value function. In particular, it is shown that there exists a Lipschitz minimizer as long as the limiting subgradient of the value function is nonempty at the point in question. The results improve upon previous results in the literature, even in the case of finite Lagrangians. 相似文献
9.
This paper is concerned with algorithms for computing in the divisor class group of a nonsingular plane curve of the form which has only one point at infinity. Divisors are represented as ideals, and an ideal reduction algorithm based on lattice reduction is given. We obtain a unique representative for each divisor class and the algorithms for addition and reduction of divisors run in polynomial time. An algorithm is also given for solving the discrete logarithm problem when the curve is defined over a finite field.
10.
P.J. Bussey C. Raine J.G. Rutherglen P.S.L. Booth L.J. Carroll G.R. Court P.R. Daniel A.W. Edwards R. Gamet C.J. Hardwick P.J. Hayman J.R. Holt J.N. Jackson W.H. Range F.H. Combley W. Galbraith V.H. Rajaratnam C. Sutton 《Nuclear Physics B》1979,154(3):492-502
The polarisation parameters Σ, P and T have been measured for the process γp→π0p in the photon energy range 1300–2100 MeV and c.m. angles between 30° and 110°, in an experiment with a polarised beam and polarised target. The results are compared with a recent theoretical analysis which fits data from threshold to 16 GeV. The new data are in general agreement with the analysis, but with some significant discrepancies in detail. 相似文献