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1.
We investigate the method of conjugate gradients, exploiting inaccurate matrix‐vector products, for the solution of convex quadratic optimization problems. Theoretical performance bounds are derived, and the necessary quantities occurring in the theoretical bounds estimated, leading to a practical algorithm. Numerical experiments suggest that this approach has significant potential, including in the steadily more important context of multiprecision computations.  相似文献   
2.
The first diastereo- and enantioselective cyclopropanation reactions of electron-deficient allenes with donor-acceptor and diacceptor diazo reagents are described. The desired enantioenriched alkylidenecyclopropanes (ACPs) were obtained in high yields with high diastereo- and enantioselectivities in the presence of Rh2((S)-TCPTAD)4 or Rh2((R)-BTPCP)4 catalysts (up to 95 % yield, >95 : 5 d.r. and 99 : 1 e.r.). This methodology gave a direct access to ACPs bearing multiple electron-deficient substituents and allows to further expand the availability of ACPs chemistry. Interestingly, during the examination of the scope of this reaction, the asymmetric intramolecular C−H insertion reaction into tert-butyl group was observed as a side reaction with up to 94 : 6 e.r.  相似文献   
3.
Nain  Philippe  Vardoyan  Gayane  Guha  Saikat  Towsley  Don 《Queueing Systems》2022,101(3-4):291-328
Queueing Systems - We study a quantum switch that distributes tripartite entangled states to sets of users. The entanglement switching process requires two steps: First, each user attempts to...  相似文献   
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We report the dramatic impact of the addition of N-heterocyclic carbenes (NHCs) on the reactivity and selectivity of heterogeneous Ru catalysts in the context of C−H activation reactions. Using a simple and robust method, we prepared a series of new air-stable catalysts starting from commercially available Ru on carbon (Ru/C) and differently substituted NHCs. Associated with C−H deuteration processes, depending on Ru/C-NHC ratios, the chemical outcome can be controlled to a large extent. Indeed, tuning the reactivity of the Ru catalyst with NHC enabled: 1) increased chemoselectivity and the regioselectivity for the deuteration of alcohols in organic media; 2) the synthesis of fragile pharmaceutically relevant deuterated heterocycles (azine, purine) that are otherwise completely reduced using unmodified commercial catalysts; 3) the discovery of a novel reactivity for such heterogeneous Ru catalysts, namely the selective C-1 deuteration of aldehydes.  相似文献   
6.
The present work focuses on studying the contribution of the Auger electron emission in proton-induced interactions in biological matter. The Monte Carlo track-structure code, TILDA-V, was then used for modeling the protons beams of 10 keV to 100 MeV in biological matter, namely, water vapor and hydrated DNA. The main ionizing processes are described by means of an extensive set of ab initio differential and total cross sections computed within a quantum-mechanical CDW-EIS approximation.  相似文献   
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We review the continuous monitoring of a qubit through its spontaneous emission, at an introductory level. Contemporary experiments have been able to collect the fluorescence of an artificial atom in a cavity and transmission line, and then make measurements of that emission to obtain diffusive quantum trajectories in the qubit's state. We give a straightforward theoretical overview of such scenarios, using a framework based on Kraus operators derived from a Bayesian update concept; we apply this flexible framework across common types of measurements including photodetection, homodyne, and heterodyne monitoring and illustrate its equivalence to the stochastic master equation formalism throughout. Special emphasis is given to homodyne (phase-sensitive) monitoring of fluorescence. The examples we develop are used to illustrate basic methods in quantum trajectories, but also to introduce some more advanced topics of contemporary interest, including the arrow of time in quantum measurement, and trajectories following optimal measurement records derived from a variational principle. The derivations we perform lead directly from the development of a simple model to an understanding of recent experimental results.  相似文献   
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The use of a strongly donating “(bis‐dialkylphosphine)Ni” fragment promotes the catalytic coupling of a large range of ArCl and ArZnCl derivatives under mild conditions. Stoichiometric mechanistic investigations and DFT calculations prove that a Ni0/NiII cycle is operative in this system.  相似文献   
10.
A fully automated countercurrent chromatography system has been constructed to rapidly screen the commonly used heptane/ethyl acetate/methanol/water solvent system series and translate the results to preparative scale separations. The system utilizes “on‐demand” preparation of the heptane/ethyl acetate/methanol/water solvent system upper and lower phases. Elution‐extrusion countercurrent chromatography was combined with non‐dynamic equilibrium injection reducing the screening time for each heptane/ethyl acetate/methanol/water system to 17 min. The result enabled solvent system development to be reduced to under 2 h. The countercurrent chromatography system was interfaced with a mass spectrometer to allow selective detection of target components in crude medicinal chemistry reaction mixtures. Mass‐directed preparative countercurrent chromatography purification was demonstrated for the first time using a synthetic tetrazole epoxide derived from a routine medicinal chemistry support workflow.  相似文献   
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