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Plieger PG Ehler DS Duran BL Taylor TP John KD Keizer TS McCleskey TM Burrell AK Kampf JW Haase T Rasmussen PG Karr J 《Inorganic chemistry》2005,44(16):5761-5769
The ligand 4,5-dicarboxyimidazole (H(2)DCI) and its methyl derivative 1-methyl-4,5-dicarboxyimidazole (H(2)MDCI) have been shown to bind to Be(II) forming a zwitterionic species that has been structurally characterized. A new dicarboxyimidazole-based polymer has been prepared and its Be-binding properties have been studied using NMR ((1)H and (9)Be) and fluorescence spectroscopy; it represents a rare example of beryllium binding to a polymer. Models of the mononuclear and polymeric Be(II)-binding sites have been studied using density functional theory (DFT), and the (9)Be NMR chemical shifts of these model materials have been calculated for the purpose of direct comparison to experimentally observed values. Differences in the binding modes of the mononuclear and polymeric species are discussed. 相似文献
3.
Koren AB Curtis MD Francis AH Kampf JW 《Journal of the American Chemical Society》2003,125(17):5040-5050
Syntheses are reported of new 4,4'-dialkyl-2,2'-bithiazole oligomers that have alkenoxy side chains that are capable of easy conversion to oligomers with functionalized side chains, e.g., terminally substituted hydroxy chains. The crystal structures of two representative oligomers (4,4',4' ',4' "-tetra-(2-propenoxymethyl)-2,2',5',5' ',2' ',2' "-quaterthiazole (3P2) and 4,4',4' ',4' "-tetra-(3-hydroxypropyloxymethyl)-2,2',5',5' ',2' ',2' "-quaterthiazole (3H2)) were determined; 3P2 crystallizes in a pi-stacked motif with two molecules per unit cell, whereas 3H2 forms pi-stacks that are linked with hydrogen bonds to form infinite two-dimensional sheets with one molecule per unit cell. A comparison of the UV-vis spectra of the compounds in solution and in the solid state provides unequivocal evidence for the presence of a Davydov splitting, W(D) approximately 0.2 eV, in solid 3P2. The spectra are interpreted in the framework of molecular exciton theory to extract a value of the intermolecular transfer integral, J approximately 0.2 eV, for a total exciton bandwidth of ca. 0.8 eV. Monte Carlo calculations were used to determine the density of states of the exciton band and the absorption and emission line shapes of the 0 <-- 0 transition. It is suggested that the "three-humped" absorption profile typical of partially crystalline, regioregular polymers is the "optical signature" of pi-stacking. 相似文献
4.
Gottfried AC Wang J Wilson EE Beck LW Banaszak Holl MM Kampf JW 《Inorganic chemistry》2004,43(24):7665-7670
The combination of 2 equiv of bis[bis(trimethylsilyl)amide]germylene (5) with 2 equiv of 4-phenyl-1,2,4-triazoline-3,5-dione (PTAD) in tetrahydrofuran (THF) results in the ring-opening of 1 equiv of THF to form 2,2,8,8-tetrakis(1,1,1,3,3,3-hexamethyl-disilazan-2-yl)-5,16-diphenyl-7,9,14-trioxa-1,3,5,16,18,19-hexaaza-2,8-digerma-tricyclo[13.2.1.13,6]nonadeca-6(19),15(18)-diene-4,17-dione (6). This fast and nearly quantitative reaction builds a 15-membered ring from five different molecules. The new ring, structurally assigned by X-ray crystallography, contains a flexible methylene chain that moves rapidly on the NMR time scale. 相似文献
5.
Rajendiran TM Kirk ML Setyawati IA Caudle MT Kampf JW Pecoraro VL 《Chemical communications (Cambridge, England)》2003,(7):824-825
Binuclear manganese complexes Mn2(III/IV)(dtsalpn)2DCBI, 1, Mn2(III/III)(dtsalpn)2HDCBI, 2, containing the ligand dicarboxyimidazole (DCBI) have been prepared in order to address the issue of imidazole bridged and ferromagnetically coupled Mn sites in high oxidation states of the OEC in Photosystem II (PS II). Temperature dependent magnetic susceptibility studies of 1 indicates that the interaction between the two Mn(III)/Mn(IV) ions is ferromagnetic (J = +1.4 cm(-1)). Variable temperature EPR spectra of 1 shows that a g = 2 multiline is as an excited state signal corresponding to S = 1/2. 相似文献
6.
C.H. Ziener T. Kampf P.M. Jakob W.R. Bauer 《Journal of magnetic resonance (San Diego, Calif. : 1997)》2010,202(1):38-42
The diffusion in the magnetic dipolar field around a sphere is considered. The diffusion is restricted to the space between two concentric spheres, where the inner sphere is the source of the magnetic dipolar field. Analytical expressions for the CPMG transverse relaxation rate as well as the free induction decay and the spin echo time evolution are given in the Gaussian approximation. The influence of the inter-echo time is analyzed. The limiting cases of small and large inter-echo times as well as the short and long time behavior are evaluated. 相似文献
7.
Ziener CH Kampf T Melkus G Jakob PM Bauer WR 《Journal of magnetic resonance (San Diego, Calif. : 1997)》2007,184(1):169-175
Simple scaling laws are useful tools in understanding the effect of changing parameters in MRI experiments. In this paper the general scaling behavior of the transverse relaxation times is discussed. We consider the dephasing of spins diffusing around a field inhomogeneity inside a voxel. The strong collision approximation is used to describe the diffusion process. The obtained scaling laws are valid over the whole dynamic range from motional narrowing to static dephasing. The dependence of the relaxation times on the external magnetic field, diffusion coefficients of the surrounding medium, and the characteristic scale of the field inhomogeneity is analyzed. For illustration the generally valid scaling laws are applied to the special case of a capillary, usually used as a model of the myocardial BOLD effect. 相似文献
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9.
We present a calculation of the electronic Raman cross section for the scattering of light across the energy gap of an antiferromagnetic insulator. The antiferromagnet is described in terms of a spin density wave state for the Hubbard model at half filling. We consider the coupling of the light to the current density and the inverse mass tensor on equal footing. A comparison of the cross section for different scattering geometries is given. 相似文献
10.