871 resultados para Half-metallicity


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Discusses the half pay and pensions of Officers living within His Majesty's Dominions. At the bottom, there is also a comment made by Robert Morrogh to Daniel Shannon concerning the above notice.

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Half-penny token struck for general circulation in Upper Canada, about 1816. The token is one of a few issues which commemorate Sir Issac Brock. The name Brock is misspelled "Brook" on this token. The other side bears the picture of a sailing vessel and the motto "Success to the Commerce of Upper Canada".

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The present thesis describes syntheses, structural studies, and catalytic reactivity of new non-classical silane complexes of ruthenium and iron. The ruthenium complexes CpRu(PPri3)CI(T]2-HSiR3) (1) (SiR3 = SiCh (a), SiClzMe (b), SiCIMe2 (c), SiH2Ph (d), SiMe2Ph (e» were prepared by reactions of the new unsaturated complex CpRu(PPri3)CI with silanes. According to NMR studies and X-ray analyses, the complexes la-c exhibit unusual simultaneous Si··· H and Si··· CI-Ru interactions. The complex CpRu(PPri3)CI was also used for the preparation of the first examples of late transition metal agostic silylamido complexes CpRu(PPri3)(N(T]2-HSiMe2)R) (2) (R= Ar or But), which were characterized by NMR spectroscopy. The iron complexes CpFe(PMePri2)H2(SiR3) (3) (SiR3 = SiCh (a), SiClzMe (b), SiCIMe2 (c), SiH2Ph (d), SiMe2Ph (e» were synthesized by the reaction of the new borohydride iron complex CpFe(PMePri2)(B~) with silanes in the presence NEt3. The complexes 3 exhibit unprecedented two simultaneous and equivalent Si··· H interactions, which was confirmed by X-ray analyses and DFT calculations. A series of cationic ruthenium complexes [CpRu(PR3)(CH3CN)(112-HSiR'3)]BAF (PR3 = PPri 3 (4), PPh3 (5); SiR'3 = SiCh (a), SiClzMe (b), SiClMe2 (c), SiH2Ph (d), SiMe2Ph (e» was obtained by substitution of one of the labile acetonitrile ligands in [CpRu(PR3)(CH3CNh]BAF with sHanes. Analogous complexes [TpRu(PR3)(CH3CN)(T]2 -HSiR' 3)]BAF (5) were obtained by the reaction of TpRu(PR3)(CH3CN)CI with LiBAF in the presence of silanes. The complexes 4-5 were characterized by NMR spectroscopy, and the observed coupling constants J(Si-H) allowed us to estimate the extent of Si-H bond activation in these compounds. The catalytic activity in hydrosilylation reactions of all of the above complexes was examined. The most promising results were achieved with the cationic ruthenium precatalyst [CpRu(PPri3)(CH3CN)2t (6). Complex 6 shows good to excellent catalytic activity in the hydrosilylation of carbonyls, dehydrogenative coupling of silanes with alcohols, amines, acids, and reduction of acid chlorides. We also discovered very selective reduction of nitriles and pyridines into the corresponding N-silyl imines and l,4-dihydropyridines, respectively, at room temperature with the possibility of catalyst recycling. These chemoselective catalytic methods have no analogues in the literature. The reactions were proposed to proceed via an ionic mechanism with intermediate formation of the silane a-complexes 4.

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Sir George Yonge (1732-1812) was a baronet, politician and colonial governor. He was a Member of Parliament for Honiton from 1754-1761 and 1763-1796, British Secretary at War from 1782-1783 and 1783-1794, and Governor of the Cape colony from 1799-1801.

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A List of Officers of the reduced Independent Companies who are to receive half pay from the days hereafter mentioned, to the 24th of December 1791, both days inclusive, or to the days of their death or Provision respectively. The document includes 153 names of Captains, Lieutenants, and Ensigns. Among the names are Isaac Brock and his brother Irwin Brock. It is signed by George Yonge.

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This thesis describes syntheses and catalytic reactivity of several half-sandwich complexes of ruthenium. The neutral ruthenium trihydride complex, Cp(PPri3)RuH3(1), can efficiently catalyse the H/D exchange reaction between various organic substrates and deuterium sources, such as benzene-d6. Moreover, the H/D exchange reactions of polar substrates were also observed in D2O, which is the most attractive deuterium source due to its low cost and low toxicity. Importantly, the H/D exchange under catalytic conditions was achieved not only in aromatic compounds but also in substituted liphatic compounds. Interestingly, in the case of alkanes and alkyl chains, highly selective deuterium incorporation in the terminal methyl positions was observed. It was discovered that the methylene units are engaged in exchange only if the molecule contains a donating functional group, such as O-and N-donors, C=C double bonds, arenes and CH3. The cationic half-sandwich ruthenium complex [Cp(PPri3)Ru(CH3CN)2]+(2) catalyses the chemoselective mono-addition of HSiMe2Ph to pyridine derivatives to selectively give the 1,4-regiospecific, N-silylated products. An ionic hydrosilylation mechanismis suggested based on the experiments. To support this mechanistic proposal, kinetic studies under catalytic conditions were performed. Also, the 1,4-regioselective mono-hydrosilylation of nitrogen containing compounds such as phenanthroline, quinoline and acridine can be achieved with the related Cp*complex [Cp*(phen)Ru(CH3CN)]+(3) (phen = 1,10-phenanthroline) and HSiMe2Ph under mild conditions. The cationic ruthenium complex 2 can also be used as an efficient catalyst for transfer hydrogenation of various organic substrates including carbonyls, imines, nitriles and esters. Secondary alcohols, amines, N-isopropylidene amines and ether compounds can be obtained in moderate to high yields. In addition, other ruthenium complexes, 1,3 and [Cp*(PPri3)Ru(CH3CN)2]+(4), can catalyse transfer hydrogenation of carbonyls although the reactions were sluggish compared to the ones of 2. The possible intermediate, Cp(PPri3)Ru(CH3CN)(H), was characterized by NMR at low temperature and the kinetic studies for the transfer hydrogenation of acetophenone were performed. Recently, chemoselective reduction of acid chlorides to aldehydes catalysed by the complex 2 was reported. To extend the catalytic reactivity of 2, reduction of iminoyl chlorides, which can be readily obtained from secondary amides, to the corresponding imines and aldehydes was investigated. Various substituted iminoyl chlorides were converted into the imines and aldehydes under mild conditions and several products were isolated with moderate yields.

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The character of the electronic ground state of La0.5Ca0.5MnO3 has been addressed with quantum chemical calculations on large embedded clusters. We find a charge ordered state for the crystal structure reported by Radaelli et al. [Phys. Rev. B 55, 3015 (1997)] and Zener polaron formation in the crystal structure with equivalent Mn sites proposed by Daoud-Aladine et al. [Phys. Rev. Lett. 89, 097205 (2002)]. Important O to Mn charge transfer effects are observed for the Zener polaron.

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Half a century, from 1947 to 2010, is enough for us to take stock of the impact of the “ideology of Development” on Heritage. An ideology induced by UNESCO and by ICOM. What has changed and what is still in an impasse? What effects has this ideology had on Heritage? It is after making this assessment that we can better understand the extent to which the theme of this 22nd ICOM General Conference – Shangai 2010 is ultimately an obvious product of that influence.

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Simulations of the last 500 yr carried out using the Third Hadley Centre Coupled Ocean-Atmosphere GCM (HadCM3) with anthropogenic and natural (solar and volcanic) forcings have been analyzed. Global-mean surface temperature change during the twentieth century is well reproduced. Simulated contributions to global-mean sea level rise during recent decades due to thermal expansion (the largest term) and to mass loss from glaciers and ice caps agree within uncertainties with observational estimates of these terms, but their sum falls short of the observed rate of sea level rise. This discrepancy has been discussed by previous authors; a completely satisfactory explanation of twentieth-century sea level rise is lacking. The model suggests that the apparent onset of sea level rise and glacier retreat during the first part of the nineteenth century was due to natural forcing. The rate of sea level rise was larger during the twentieth century than during the previous centuries because of anthropogenic forcing, but decreasing natural forcing during the second half of the twentieth century tended to offset the anthropogenic acceleration in the rate. Volcanic eruptions cause rapid falls in sea level, followed by recovery over several decades. The model shows substantially less decadal variability in sea level and its thermal expansion component than twentieth-century observations indicate, either because it does not generate sufficient ocean internal variability, or because the observational analyses overestimate the variability.

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We consider boundary value problems for the elliptic sine-Gordon equation posed in the half plane y > 0. This problem was considered in Gutshabash and Lipovskii (1994 J. Math. Sci. 68 197–201) using the classical inverse scattering transform approach. Given the limitations of this approach, the results obtained rely on a nonlinear constraint on the spectral data derived heuristically by analogy with the linearized case. We revisit the analysis of such problems using a recent generalization of the inverse scattering transform known as the Fokas method, and show that the nonlinear constraint of Gutshabash and Lipovskii (1994 J. Math. Sci. 68 197–201) is a consequence of the so-called global relation. We also show that this relation implies a stronger constraint on the spectral data, and in particular that no choice of boundary conditions can be associated with a decaying (possibly mod 2π) solution analogous to the pure soliton solutions of the usual, time-dependent sine-Gordon equation. We also briefly indicate how, in contrast to the evolutionary case, the elliptic sine-Gordon equation posed in the half plane does not admit linearisable boundary conditions.

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We study the effect of varying the boundary condition on: the spectral function of a finite one-dimensional Hubbard chain, which we compute using direct (Lanczos) diagonalization of the Hamiltonian. By direct comparison with the two-body response functions and with the exact solution of the Bethe ansatz equations, we can identify both spinon and holon features in the spectra. At half-filling the spectra have the well-known structure of a low-energy holon band and its shadow-which spans the whole Brillouin zone-and a spinon band present for momenta less than the Fermi momentum. Features related to the twisted boundary condition are cusps in the spinon band. We show that the spectral building principle, adapted to account for both the finite system size and the twisted boundary condition, describes the spectra well in terms of single spinon and holon excitations. We argue that these finite-size effects are a signature of spin-charge separation and that their study should help establish the existence and nature of spin-charge separation in finite-size systems.