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741.
We report a new catalytic protocol for highly selective C-H arylation of pyridines containing common and synthetically versatile electron-withdrawing substituents (NO(2), CN, F and Cl). The new protocol expands the scope of catalytic azine functionalization as the excellent regioselectivity at the 3- and 4-positions well complements the existing methods for C-H arylation and Ir-catalyzed borylation, as well as classical functionalization of pyridines. Another important feature of the new method is its flexibility to adapt to challenging substrates by a simple modification of the carboxylic acid ligand or the use of silver salts. The regioselectivity can be rationalized on the basis of the key electronic effects (repulsion between the nitrogen lone pair and polarized C-Pd bond at C2-/C6-positions and acidity of the C-H bond) in combination with steric effects (sensitivity to bulky substituents). 相似文献
742.
We study the influence of the softness of the interparticle interactions on the fragility of a glass former by considering three model binary mixture glass formers. The interaction potential between particles is a modified Lennard-Jones type potential, with the repulsive part of the potential varying with an inverse power q of the interparticle distance, and the attractive part varying with an inverse power p. We consider the combinations (12,11) (model I), (12,6) (model II), and (8,5) (model III) for (q,p) such that the interaction potential becomes softer from model I to III. We evaluate the kinetic fragilities from the temperature variation of diffusion coefficients and relaxation times, and a thermodynamic fragility from the temperature variation of the configurational entropy. We find that the kinetic fragility increases with increasing softness of the potential, consistent with previous results for these model systems, but at variance with the thermodynamic fragility, which decreases with increasing softness of the interactions, as well as expectations from earlier results. We rationalize our results by considering the full form of the Adam-Gibbs relation, which requires, in addition to the temperature dependence of the configurational entropy, knowledge of the high temperature activation energies in order to determine fragility. We show that consideration of the scaling of the high temperature activation energy with the liquid density, analyzed in recent studies, provides a partial rationalization of the observed behavior. 相似文献
743.
744.
Intramolecular Diels-Alder approach to construct the fused AB ring of trinervitane has been demonstrated efficiently. The key intermediate for the Diels-Alder cyclization has been achieved following highly stereoselective Julia-Kocienski olefination, Sharpless epoxidation and Evan’s asymmetric alkylation as the key reactions. 相似文献
745.
Selective excitation of LI2 by chirped laser pulses with all possible interstate radiative couplings
We have numerically explored the feasibility and the mechanism of population transfer to the excited E (1)Σ(g) electronic state of Li(2) from the v=0 level of the ground electronic state X (1)Σ(g) using the A (1)Σ(u) state as an intermediate. In this system, the use of transform limited pulses with a frequency difference greater than the maximum Rabi frequency does not produce population transfer when all possible radiative couplings are taken into account. We have employed two synchronous pulses far detuned from the allowed transition frequencies, mainly with the lower frequency pulse positively chirped, and both pulses coupling the successive pair of states, X-A and A-E. The adiabaticity of the process has been investigated by a generalized Floquet calculation in the basis of 12 field dressed molecular states, and the results have been compared with those obtained from the full solution of time dependent Schro?dinger equation. The conventional representation of the process in terms of three (or four) adiabatic potentials is not valid. It has been found that for cases of almost complete population transfer in full calculations with the conservation of the vibrational quantum number, adiabatic passage is attained with the 12 state Floquet model but not with the six state model. The agreement between the full calculations and the 12 state Floquet calculations is generally good when the transfer is adiabatic. Another characteristic feature of this work is the gaining of control over the vibrational state preparation in the final electronic state by careful tuning of the laser parameters as well as the chirp rate sign. This causes time dependent changes in the adiabatic potentials and nonadiabatic transfers can be made to occur between them. 相似文献
746.
Haji-saeed B Sengupta SK Goodhue W Khoury J Woods CL Kierstead J 《Optics letters》2006,31(13):1969-1971
We introduce a dynamic range image compression technique for nonlinear deconvolution; the impulse response of the distortion function and the noisy distorted image are jointly transformed to pump a clean reference beam in a two-beam coupling arrangement. The Fourier transform of the pumped reference beam contains the deconvolved image and its conjugate. In contrast to standard deconvolution approaches, for which noise can be a limiting factor in the performance, this approach allows the retrieval of distorted signals embedded in a very high-noise environment. 相似文献
747.
Sengupta SK Pandey OP Rai A Sinha A 《Spectrochimica acta. Part A, Molecular and biomolecular spectroscopy》2006,65(1):139-142
A series of new coordination complexes of La(III) and Pr(III) with hydrazones, derived from 1,1-diacetylferrocene and different aromatic acid hydrazides have been synthesized and characterized by elemental analyses, electrical conductance, magnetic moment, IR, (1)H NMR, UV-vis spectra and molar conductance. The thermal behaviour of the complexes under non-isothermal condition was investigated by TG and DTG techniques. The antifungal activity of hydrazones and their corresponding complexes were also investigated. 相似文献
748.
The technique described enables the user to detect the presence and proliferation of bacteria through an increase in the bulk capacitance (C) of the suspension, which is proportional to the bacteria count, at practical frequencies less than 1 MHz. The geometry of the micro-capillary design employed increases the bulk resistance (R) of the medium, thus increasing its RC time. This makes the measured reactance sensitive to changes in the bulk capacitance, which is usually masked by the much larger surface capacitance. The sensitivity is further enhanced by the existence of a minimum in the value of the reactance at a frequency proportional to the inverse medium RC time. The value of this reactance minimum and the frequency at which the minimum is recorded are dependent on the bacteria count and permit the detection of an initial concentration of approximately 100 CFU ml(-1) of E. coli within 3 hours of incubation, in comparison with the previous reported values of about 8 hours, with an initial load of 1000 CFU ml(-1). 相似文献
749.
We prove that, under suitable conditions, certain Siegel Poincaré series of exponential type of even integer weight and degree 2 do not vanish identically. We also find estimates for twisted Kloosterman sums and Salié sums in all generality. 相似文献
750.