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91.
The source of the effect of N-alkylation on the redox properties of Ni(II/I) and Cr(III/II) cyclam complexes has been investigated using DFT calculations. The structures of the anhydrous and hydrated complexes were optimized in the gas phase, and single point calculations were performed in a polarized continuum. The main results are the following: the decrease in outer sphere solvation upon N-alkylation is the major source of the relative stabilization of the lower oxidation state complexes by the tertiary amine ligands; tertiary amine nitrogen donors are stronger sigma-donors than the secondary amines, as predicted from the inductive effect of alkyls; steric strain elongates the metal-nitrogen bonds in the tertiary complexes and decreases the ligand strain energies; and the site of water binding to the complexes differs because of their different electronic structures (i.e., in the Ni complexes, the water molecules bind to the M[bond]N[bond]H sites, whereas in the Cr complexes they bind to the central metal cation). Outer sphere hydrogen bonding of water to the ligands in the coordination sphere lowers the ionization potentials by charge delocalization. 相似文献
92.
Annals of Global Analysis and Geometry - In the present paper, we consider star-shaped mean convex hypersurfaces of the real, complex and quaternionic hyperbolic space evolving by a class of... 相似文献
93.
Matthias Hoschneider 《Communications in Mathematical Physics》1994,160(3):457-473
In this paper we want to give a new definition of fractal dimensions as small scale behavior of theq-energy of wavelet transforms. This is a generalization of previous multi-fractal approaches. With this particular definition we will show that the 2-dimension (=correlation dimension) of the spectral measure determines the long time behavior of the time evolution generated by a bounded self-adjoint operator acting in some Hilbert space ?. It will be proved that for φ, ψ∈? we have $$\mathop {\lim \inf }\limits_{T \to \infty } \frac{{\log \int_0^T {d\omega \left| {\left\langle {\psi \left| {e^{ - iA\omega } } \right.\phi } \right\rangle } \right|^2 } }}{{\log T}} = - \kappa ^ + (2)$$ and that $$\mathop {\lim \sup }\limits_{T \to \infty } \frac{{\log \int_0^T {d\omega \left| {\left\langle {\psi \left| {e^{ - iA\omega } } \right.\phi } \right\rangle } \right|^2 } }}{{\log T}} = - \kappa ^ - (2),$$ wherek ±(2) are the upper and lower correlation dimensions of the spectral measure associated with ψ and ?. A quantitative version of the RAGE theorem shall also be given. 相似文献
94.
Michael Meyberg Elvezio Morenzoni Thomas Wutzke Uwe Zimmermann Franz Kottmann Klaus Jungmann Björn Matthias Thomas Prokscha 《Hyperfine Interactions》1994,87(1):1075-1081
At PSI we are investigating the technique of decelerating an existing very intense secondary beam of surface
+ (4 MeV) to an energy of 10 eV using appropriate moderators. These
+ can then be used as a source of a tertiary beam of low energy muons with tunable kinetic energy between 10 eV and 10 keV.With a 1000 A layer of solid Argon deposited on an Al substrate we obtain a moderation efficiency (with respect to the number of incoming surface
+) of the order of 10–4.Results of our investigations and the present status of the project are presented together with future plans and possibilities. 相似文献
95.
Matthias Schmidt 《Zeitschrift für Physik B Condensed Matter》1994,95(3):327-330
We consider theq=3 Potts model in three dimensions by Monte Carlo simulations. The microcanonical density of states is calculated as a function of the internal energy of the system. We extrapolate the data for the simulated finite systems to the thermo-dynamic limit and find a discontinuous phase transition. This method is checked in the two-dimensional case, where exact results are known. 相似文献
96.
Morenzoni E. Birke M. Hofer A. Kottmann F. Litterst J. Matthias B. Meyberg M. Niedermayer Ch. Prokscha Th. Schatz G. Wutzke Th. 《Hyperfine Interactions》1996,97(1):395-406
During the last few decades, a variety of methods has been developed which makes use of polarized positive muons as a microscopic probe of the magnetic properties of condensed matter (muon spin rotation, relaxation, resonance,SR). Until now, available beams for SR studies have delivered 100% polarized muons with energies in the MeV range, resulting in a deep penetration of the muons into the sample material under investigation. This presently limits the applications of theSR technique to the study of the bulk characteristics of matter. To be able to control the implantation depth, a very low energy beam of polarized muons is being developed at the Paul Scherrer Institute. Very slow polarized muons (kinetic energy 10 eV, polarization 90%) are obtained from the moderation of a high energy muon beam in a thin film of an appropriate condensed gas. These muons can be used as a source for a beam of tunable energy between a few tens of eV and some tens of keV. Implantation depths in the range of few to a few hundreds of nanometers can thus be achieved by varying the energy. 相似文献
97.
In this paper we consider the disjoint paths problem. Given a graphG and a subsetS of the edge-set ofG the problem is to decide whether there exists a family of disjoint circuits inG each containing exactly one edge ofS such that every edge inS belongs to a circuit inC. By a well-known theorem of P. Seymour the edge-disjoint paths problem is polynomially solvable for Eulerian planar graphsG. We show that (assumingPNP) one can drop neither planarity nor the Eulerian condition onG without losing polynomial time solvability. We prove theNP-completeness of the planar edge-disjoint paths problem by showing theNP-completeness of the vertex disjoint paths problem for planar graphs with maximum vertex-degree three. This disproves (assumingPNP) a conjecture of A. Schrijver concerning the existence of a polynomial time algorithm for the planar vertex-disjoint paths problem. Furthermore we present a counterexample to a conjecture of A. Frank. This conjecture would have implied a polynomial algorithm for the planar edge-disjoint paths problem. Moreover we derive a complete characterization of all minorclosed classes of graphs for which the disjoint paths problem is polynomially solvable. Finally we show theNP-completeness of the half-integral relaxation of the edge-disjoint paths problem. This implies an answer to the long-standing question whether the edge-disjoint paths problem is polynomially solvable for Eulerian graphs.Supported by Sonderforschungsbereich 303 (DFG) 相似文献
98.
[reaction: see text] A novel cycloaldol approach to the isobenzofuran core common to many of the eunicellin diterpenes is described. The cycloaldol precursor was prepared by aldol addition of (S)-(+)-carvone and methacrolein followed by etherification to a glycolate ester. Chemoselective enolization of the glycolate ester led to the cycloaldol adduct in high yield and diastereoselectivity. An oxidative rearrangement-allylic diazene rearrangement sequence established the requisite cis ring fusion. 相似文献
99.
Boudier A Bromm LO Lotz M Knochel P 《Angewandte Chemie (International ed. in English)》2000,39(24):4414-4435
In the second half of the twentieth century much effort was invested in the preparation of highly reactive polar organometallic reagents. The high reactivity of these reagents precluded the presence of many functional groups and often good chemoselectivities and stereoselectivities could only by achieved by transmetalation reactions. The synthesis of increasingly complex target molecules and the desire to avoid tedious protection-deprotection steps has led inevitably to the use of functionalized organometallic reagents in retrosynthesis. In the last fifteen years, the generation of organic derivatives of numerous metals and metalloids (Li, Mg, B, Zn, Sn) was investigated. In this review the most important preparations and applications of organometallic reagents in organic synthesis will be covered, with particular emphasis on organozinc reagents. 相似文献
100.
Russell SC Czerwieniec G Lebrilla C Tobias H Fergenson DP Steele P Pitesky M Horn J Srivastava A Frank M Gard EE 《Journal of the American Society for Mass Spectrometry》2004,15(6):900-909
The appearance of informative signals in the mass spectra of laser-ablated bio-aerosol particles depends on the effective ionization probabilities (EIP) of individual components during the laser ionization process. This study investigates how bio-aerosol chemical composition governs the EIP values of specific components and the overall features of the spectra from the bio-aerosol mass spectrometry (BAMS). EIP values were determined for a series of amino acid, dipicolinic acid, and peptide aerosol particles to determine what chemical features aid in ionization. The spectra of individual amino acids and dipicolinic acid, as well as mixtures, were examined for extent of fragmentation and the presence of molecular ion dimers, which are indicative of ionization conditions. Standard mixtures yielded information with respect to the significance of secondary ion plume reactions on observed spectra. A greater understanding of how these parameters affect EIP and spectra characteristics of bio-aerosols will aid in the intelligent selection of viable future biomarkers for the identification of bio-terrorism agents. 相似文献