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181.
The experimental charge density distribution of dimethyl-trans-2-oxohexahydro-pyrimidine-4,6-dicarboxylate 1 has been determined using single-crystal X-ray diffraction data measured at 100 K, in terms of the rigid-pseudoatom formalism. Multipole refinement converged at R(F) = 0.034 for 7283 reflections with I > 3 sigma (I) and sin theta/lambda < or = 1.13 A(-1). Covalent and hydrogen bonding interactions are analyzed using a topological analysis of the Laplacian of the charge density. The experimentally derived electrostatic potential mapped onto the reactive surface of the molecule reveals the potential binding sites of 1. 相似文献
182.
Albone DP Challenger S Derrick AM Fillery SM Irwin JL Parsons CM Takada H Taylor PC Wilson DJ 《Organic & biomolecular chemistry》2005,3(1):107-111
Amination of C-H bonds activated by ether oxygen atoms is facile with chloramine-T as nitrene source and copper(I) chloride in acetonitrile as catalyst. For cyclic ethers the hemiaminal products are generally stable and can be isolated pure. For acyclic ethers, the hemiaminal products, as expected, fragment with elimination of alcohol to yield imines. When activation of benzylic positions is remote through a conjugated system, stable benzylamine derivatives are isolated. Mechanistic studies are consistent with concerted insertion of an electrophilic nitrenoid into the C-H bond in the rate-determining step, though in an asynchronous manner with a more activated substrate. 相似文献
183.
According to the universal entropy bound, the entropy (and hence information capacity) of a complete weakly self-gravitating
physical system can be bounded exclusively in terms of its circumscribing radius and total gravitating energy. The bound’s
correctness is supported by explicit statistical calculations of entropy, gedanken experiments involving the generalized second
law, and Bousso’s covariant holographic bound. On the other hand, it is not always obvious in a particular example how the
system avoids having too many states for given energy, and hence violating the bound. We analyze in detail several purported
counterexamples of this type, and exhibit in each case the mechanism behind the bound’s efficacy.
In memoriam Asher Peres. 相似文献
184.
We use Monte Carlo simulations to identify the mechanism that allows for phase transitions in dipolar spin ice to occur and survive for an applied magnetic field H much larger in strength than that of the spin-spin interactions. In the most generic and highest symmetry case, the spins on one out of four sublattices of the pyrochlore decouple from the total local exchange+dipolar+applied field. In the special case where H is aligned perfectly along the [110] crystallographic direction, spin chains perpendicular to H show a transition to q=X long-range order, which proceeds via a one- to three-dimensional crossover. We propose that these transitions are relevant to the origin of specific heat features observed in powder samples of the Dy2Ti2O7 spin ice material for H above 1 Tesla. 相似文献
185.
Suppose given a Galois étale cover YX of proper non-singular curves over an algebraically closed field k of prime characteristic p. Let H be its Galois group, and G any finite extension of H by a p-group P. We give necessary and sufficient conditions on G to be the Galois group of an étale cover of X dominating YX.in final form: 16 September 2003 相似文献
186.
Very few Banach spaces E are known for which the lattice of closed ideals in the Banach algebra of all (bounded, linear) operators on E is fully understood. Indeed, up to now the only such Banach spaces are, up to isomorphism, Hilbert spaces and the sequence spaces c0 and ?p for 1?p<∞. We add a new member to this family by showing that there are exactly four closed ideals in for the Banach space E?(⊕?2n)c0, that is, E is the c0-direct sum of the finite-dimensional Hilbert spaces ?21,?22,…,?2n,… . 相似文献
187.
When a nonvolatile liquid film dewets from a partly compatible liquid substrate, the advancing dewetting front leaves behind droplets formed through a Rayleigh instability mechanism at its rim. We have found that these droplets continue to move in the direction of the dewetting front for extended periods (of order one day) with an initial droplet velocity varying linearly with the droplet size, and a displacement varying logarithmically with time. We attribute this persistent motion to a transient surface tension gradient on the substrate liquid surface trailing the dewetting front. 相似文献
188.
189.
Wessel N Konvicka J Weidermann F Nestmann S Neugebauer R Schwarz U Wessel A Kurths J 《Chaos (Woodbury, N.Y.)》2004,14(1):23-29
In the last decade, there has been an increasing interest in compensating thermally induced errors to improve the manufacturing accuracy of modular tool systems. These modular tool systems are interfaces between spindle and workpiece and consist of several complicatedly formed parts. Their thermal behavior is dominated by nonlinearities, delay and hysteresis effects even in tools with simpler geometry and it is difficult to describe it theoretically. Due to the dominant nonlinear nature of this behavior the so far used linear regression between the temperatures and the displacements is insufficient. Therefore, in this study we test the hypothesis whether we can reliably predict such thermal displacements via nonlinear temperature-displacement regression functions. These functions are estimated first from learning measurements using the alternating conditional expectation (ACE) algorithm and then tested on independent data sets. First, we analyze data that were generated by a finite element spindle model. We find that our approach is a powerful tool to describe the relation between temperatures and displacements for simulated data. Next, we analyze the temperature-displacement relationship in a silent real experimental setup, where the tool system is thermally forced. Again, the ACE algorithm is powerful to estimate the deformation with high precision. The corresponding errors obtained by using the nonlinear regression approach are 10-fold lower in comparison to multiple linear regression analysis. Finally, we investigate the thermal behavior of a modular tool system in a working milling machine and again get promising results. The thermally induced errors can be estimated with 1-2 microm accuracy using this nonlinear regression analysis. Therefore, this approach seems to be very useful for the development of new modular tool systems. 相似文献
190.
Seferos DS Banach DA Alcantar NA Israelachvili JN Bazan GC 《The Journal of organic chemistry》2004,69(4):1110-1119
The selective cleavage of arylmethyl thioethers provides a convenient protocol for the synthesis of all-E isomers of alpha, omega-bis(thioacetyl)oligophenyenevinylene molecules (OPVs). The S-methyl group is tolerant of Wittig-type and Heck-type reactions for forming OPV structures and can be converted to the S-acetyl group by treatment with sodium thiomethoxide and acetyl chloride. The thermal conditions of the deprotection/reprotection step concurrently isomerize the conjugated chromophore to the all-E isomer, regardless of the stereochemistry of the starting olefins. This approach is demonstrated for a variety of linear and [2.2]paracyclophane containing OPVs, which have been characterized by electrochemical and spectroscopic techniques. Additionally, these S-acetyl-terminated OPVs self-assemble on gold surfaces. Monolayers containing these molecules were characterized by water contact angle measurements, ellipsometry, and X-ray photoelectron spectroscopy. 相似文献