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The many-body contributions to the interaction polarisability and hyperpolarisability of He
n (n=3,4, 5), for various configurations and distances have been determined and analysed. Several cases have been found where the three-body terms contribute more than 20% to or of He
n
. The remarkable dependence of the above interaction properties on the internuclear distances and the shape of the cluster has been demonstrated. The interaction hyperpolarisabilities are shown to be uniquely sensitive probes of the electronic structure changes induced by variation of the cluster configuration. The results were computed by employing a computational procedure which relies on anab initio wave function, McWeeny's et al. coupled Hartree-Fock perturbation theory and an efficient algorithm for the determination of hyperpolarisabilities starting from a non-orthogonal basis set. The function counterpoise method has been used to reduce the basis set superposition error. 相似文献
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The effects of pH and light on the interaction between fulvic acid and iron have been investigated through studies of the kinetics of exchange of iron between fulvic acid and 1,10-pehnanthroline(a strong iron(II) complexing agent), and of the quenching of intrinsic fulvic acid fluorescence by iron in solutions of pH 4.0 and 6.5 containing an excess of fulvic acid. The results enable the iron-fulvic acid interaction to be described in terms of operationally defined iron-fulvic acid groupings, the proportions of which are markedly dependent on pH and light conditions. At pH 4.0 fulvic acid exhibits considerable reducing ability with the result that a substantial portion of iron is present in reduced, unbound form. Irradiation of fulvic acids at this pH markedly increases their reducing ability. Iron that is not reduced is present as small (ultrafilterable), strongly bound iron(III) complexes. Iron bound in this form is an effective quencher of intrinsic fulvic acid fluorescence. At higher pH, essentially all of the iron is relatively strongly bound, with most being in the form of large (non-ultrafilterable) iron(III)—fulvic acid groupings. These groupings are not altered significantly by irradiation and iron bound in this form is not a very effective quencher of intrinsic fulvic acid fluorescence. 相似文献
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The kinetics of Fe(II) oxidation in the presence of various citrate concentrations have been investigated in aqueous solutions over the pH range 6.0-8.0 using colorimetry and speciation modeling. Oxidation of Fe(II) was interpreted and quantitatively modeled in terms of oxidation of various Fe(II)-citrate species. Using the model, it is possible to predict whether the presence of citrate would dominate the Fe(II) oxidation and thus enhance/retard the oxidation rate of Fe(II) and vice versa. The study also supports the presence of other Fe(II)-citrate species rather than just the monomeric species at circumneutral pH. At low pH and in a system where complexation of Fe(II) by citrate is dominant, oxidation of Fe(II) is controlled by the oxidation of both Fecit- and Fecit24-. As the pH increases, the oxidation of Fe(OH)cit25- becomes increasingly important and dominates the oxidation of Fe(II) at pH 8.0. Rate constants for the oxidation of all five suggested Fe(II)-citrate species have been estimated and may be used to predict the rate of Fe(II) oxidation at any combination of pH and citrate concentration. 相似文献
36.
Sparks SM Waite CL Harmon AM Nusblat LM Roth CM Uhrich KE 《Macromolecular bioscience》2011,11(9):1192-1200
New materials that can bind and deliver oligonucleotides such as short interfering RNA (siRNA) without toxicity are greatly needed to fulfill the promise of therapeutic gene silencing. Amphiphilic macromolecules (AMs) were functionalized with linear ethyleneimines to create cationic AMs capable of complexing with siRNA. Structurally, the parent AM is formed from a mucic acid backbone whose tetra-hydroxy groups are alkylated with 12-carbon aliphatic chains to form the hydrophobic component of the macromolecule. This alkylated mucic acid is then mono-functionalized with poly(ethylene glycol) (PEG) as a hydrophilic component. The resulting AM contains a free carboxylic acid within the hydrophobic domain. In this work, linear ethyleneimines were conjugated to the free carboxylic acid to produce an AM with one primary amine (1N) or one primary amine and four secondary amines (5N). Further, an AM with amine substitution both to the free carboxylic acid in the hydrophobic domain and also to the adjacent PEG was synthesized to produce a polymer with one primary amine and eight secondary amines (9N), four located on each side of the AM hydrophobic domain. All amine-functionalized AMs formed nanoscale micelles but only the 5N and 9N AMs had cationic zeta potentials, which increased with increasing number of amines. All AMs exhibited less inherent cytotoxicity than linear polyethyleneimine (L-PEI) at concentrations of 10 μM and above. By increasing the length of the cationic ethyleneimine chain and the total number of amines, successful siRNA complexation and cellular siRNA delivery was achieved in a malignant glioma cell line. In addition, siRNA-induced silencing of firefly luciferase was observed using complexes of siRNA with the 9N AM and comparable to L-PEI, yet showed better cell viability at higher concentrations (above 10 μM). This work highlights the promise of cationic AMs as safe and efficient synthetic vectors for siRNA delivery. Specifically, a novel polymer (9N) was identified for efficient siRNA delivery to cancer cells and will be further evaluated. 相似文献
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Saxton OH Schalk T Schumm BA Schwiening J Serbo VV Shapiro G Sinev NB Snyder JA Staengle H Stahl A Stamer P Steiner H Su D Suekane F Sugiyama A Suzuki A Swartz M Taylor FE Thom J Torrence E Usher T Va'vra J Verdier R Wagner DL Waite AP Walston S 《Physical review letters》2000,85(24):5059-5063
We present the first direct measurement of A(s), the parity-violating coupling of the Z0 boson to the strange quark, using approximately 550 000 e(+)e(-)-->Z0-->hadrons events recorded by the SLC Large Detector with a polarized e(-) beam. We tagged Z0-->s&smacr; events by the absence of B or D hadrons and the presence in each hemisphere of a high momentum K+/- or K(0)(s). Fitting the polar angle distributions of the strangeness-signed thrust axis gave A(s) = 0.895+/-0.066(stat)+/-0.062(syst). The analyzing power and uu+d&dmacr; background were constrained using the data, greatly reducing any model dependence. 相似文献