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111.
112.
Synthesis and Rearrangement of P‐Nitroxyl‐Substituted PIII and PV Phosphanes: A Combined Experimental and Theoretical Case Study 下载免费PDF全文
Tobias Heurich Dr. Zheng‐Wang Qu Dr. Senada Nožinović Dr. Gregor Schnakenburg Dr. Hideto Matsuoka Prof. Dr. Stefan Grimme Prof. Dr. Olav Schiemann Prof. Dr. Rainer Streubel 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(29):10102-10110
Low‐temperature generation of P‐nitroxyl phosphane 2 (Ph2POTEMP), which was obtained by the reaction of Ph2PH ( 1 ) with two equivalents of TEMPO, is presented. Upon warming, phosphane 2 decomposed to give P‐nitroxyl phosphane P‐oxide 3 (Ph2P(O)OTEMP) as one of the final products. This facile synthetic protocol also enabled access to P‐sulfide and P‐borane derivatives 7 and 13 , respectively, by using Ph2P(S)H ( 6 ) or Ph2P(BH3)H ( 11 ) and TEMPO. Phosphane sulfide 7 revealed a rearrangement to phosphane oxide 8 (Ph2P(O)STEMP) in CDCl3 at ambient temperature, whereas in THF, thermal decomposition of sulfide 7 yielded salt 10 ([TEMP‐H2][Ph2P(S)O]). As well as EPR and detailed NMR kinetic studies, indepth theoretical studies provided an insight into the reaction pathways and spin‐density distributions of the reactive intermediates. 相似文献
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Chu Rainer Kwang-Hua 《Journal of Experimental and Theoretical Physics》2016,123(5):822-826
We illustrate the possible acceleration of cosmic rays passing through a kind of amplification channel (via diffusion modes of propagating plane-wave fronts) induced by a rotating system. Our analysis is mainly based on the quantum discrete kinetic model (considering a discrete Uehling-Uhlenbeck collision term), which has been used to study the propagation of plane (e.g., acoustic) waves in a system of rotating gases. 相似文献
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An approach to evaluate the second-order exchange-induction energies of symmetry-adapted intermolecular perturbation theory (SAPT) for single-determinant ground-state monomer wavefunctions has been derived. This approach is correct to all orders of the intermonomer overlap, that is, it takes multiple electron exchange between the monomers into account. The resulting formulae can be written in a compact way and implemented efficiently. Here, the method is employed to investigate the performance of the S 2- or single-exchange approximation at the Hartree-Fock-SAPT level. The list of test systems comprises the prototypical van der Waals- and hydrogen-bridge complexes Ne2, Ar–HF, and (H2O)2, but also the systems HeCl?, NeNa+ and Li+F? involving closed-shell ions. It was found that the errors introduced by the S 2-approximation are more pronounced for the second-order exchange-induction energy than for the first-order exchange energy. While these errors tend to be negligible throughout the well region of complexes such as the neon dimer, they start to be significant in the repulsive part of the well regions of systems such as the water dimer, and in particular for the ionic lithium fluoride molecule. The consequences of these findings for the Hartree-Fock level estimate of higher-order induction plus exchange-induction energies, which is frequently employed in SAPT are also discussed. 相似文献
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Piotr T. Chruściel Erwann Delay Paul Klinger Andreas Kriegl Peter W. Michor Armin Rainer 《Letters in Mathematical Physics》2018,108(9):2009-2030
We prove existence of large families of solutions of Einstein-complex scalar field equations with a negative cosmological constant, with a stationary or static metric and a time-periodic complex scalar field. 相似文献
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Abstract Solids like layer silicates (kaolinite and montmorillonite) as well as ZnO are in use in pharmacy. They are pressure treated and subsequently analyzed by means of ESR spectroscopy. The structural changes indicated by Fe3+ ions and paramagnetic defects are reponsible for the enhanced chemical activity of the pressurized systems. Especially active Fe-O-species are formed which can react with intercacalated organic molecules. The most probable first step of such reactions will be a solid state single electron transfer. Spin probes and spin traps were used to prove this statements. The activation of the drug delivery systems by mechanical treatments is of importance for the stability of the drugs incorporated. 相似文献
119.
Johannes W. R. Martini Martin Schlather G. Matthias Ullmann 《Journal of mathematical chemistry》2013,51(2):696-714
In the first part of this work we formulated the decoupled sites representation for two different types of ligands and highlighted special properties of the case of n binding sites for ligand L 1 and one binding site for ligand L 2. Moreover, for this case, we identified the microstate constants as unique components all decoupled molecules share. In the second part on hand, we investigate the cases with (n, 2) and (n, 3) binding sites. As it is difficult to solve the system of equations occurring when a molecule with more than one binding site for both ligands shall be decoupled, we present applicable calculation methods which exploit the special structure of the system of equations. Moreover, we investigate which unique properties all decoupled molecules share and show that for two different decoupled molecules with the same binding polynomial, not all microstate constants of a certain macrostate are permutations of the microstate constants of the other molecule. 相似文献
120.
Lisa Roeder Philipp Bender Andreas Tschöpe Rainer Birringer Annette M. Schmidt 《Journal of polymer science. Part A, Polymer chemistry》2012,50(24):1772-1781
The mechanical characterization of complex soft matter by quasi-static magnetometry using nanoscopic magnetic probes is demonstrated for model hydrogels doped with two types of elongated magnetic nanoparticles. Chemically crosslinked poly(acrylamide) (PAAm) hydrogels serve as the matrix in which nickel nanorods or weakly magnetized hematite (α-Fe2O3) ellipsoids are embedded as local probes. We investigated the swelling behavior of the ferrogels in order to verify that their equilibrium swelling degree in water is not influenced by the probes, shows a good correlation with the Frenkel–Flory–Rehner model. The proposed magnetomechanical method relies on a correlation between the shear modulus of the PAAm hydrogel matrix and the coercive fields of the corresponding isotropic ferrogels. By extending the Stoner–Wohlfarth model for single-domain blocked magnetic particles by a term for particle rotation in an elastic matrix, information on the shear modulus of the matrix can be obtained. Comparison of the results with the expected relation from rubber elasticity theory illustrates both the general potential as well as the limits of the approach. © 2012 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2012 相似文献