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1.
Dr. Zhoulong Fan Katherine L. Bay Dr. Xiangyang Chen Zhe Zhuang Han Seul Park Dr. Kap-Sun Yeung Prof. Dr. K. N. Houk Prof. Dr. Jin-Quan Yu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(12):4800-4807
A simple and efficient nitrile-directed meta-C−H olefination, acetoxylation, and iodination of biaryl compounds is reported. Compared to the previous approach of installing a complex U-shaped template to achieve a molecular U-turn and assemble the large-sized cyclophane transition state for the remote C−H activation, a synthetically useful phenyl nitrile functional group could also direct remote meta-C−H activation. This reaction provides a useful method for the modification of biaryl compounds because the nitrile group can be readily converted to amines, acids, amides, or other heterocycles. Notably, the remote meta-selectivity of biphenylnitriles could not be expected from previous results with a macrocyclophane nitrile template. DFT computational studies show that a ligand-containing Pd–Ag heterodimeric transition state (TS) favors the desired remote meta-selectivity. Control experiments demonstrate the directing effect of the nitrile group and exclude the possibility of non-directed meta-C−H activation. Substituted 2-pyridone ligands were found to be key in assisting the cleavage of the meta-C−H bond in the concerted metalation–deprotonation (CMD) process. 相似文献
2.
Stability of a Model of Relativistic Quantum Electrodynamics 总被引:1,自引:0,他引:1
The relativistic “no pair” model of quantum electrodynamics uses the Dirac operator, D(A) for the electron dynamics together with the usual self-energy of the quantized ultraviolet cutoff electromagnetic field
A– in the Coulomb gauge. There are no positrons because the electron wave functions are constrained to lie in the positive
spectral subspace of some Dirac operator, D, but the model is defined for any number, N, of electrons, and hence describes a true many-body system. In addition to the electrons there are a number, K, of fixed nuclei with charges ≤Z. If the fields are not quantized but are classical, it was shown earlier that such a model is always unstable (the ground
state energy E=−∞) if one uses the customary D(0) to define the electron space, but is stable (E > − const.(N+K)) if one uses D(A) itself (provided the fine structure constant α and Z are not too large). This result is extended to quantized fields here, and stability is proved for α= 1/137 and Z≤ 42. This formulation of QED is somewhat unusual because it means that the electron Hilbert space is inextricably linked
to the photon Fock space. But such a linkage appears to better describe the real world of photons and electrons.
Received: 8 September 2001 / Accepted: 18 March 2002 相似文献
3.
James K. Freericks Elliott H. Lieb Daniel Ueltschi 《Communications in Mathematical Physics》2002,227(2):243-279
The Falicov–Kimball model is a simple quantum lattice model that describes light and heavy electrons interacting with an
on-site repulsion; alternatively, it is a model of itinerant electrons and fixed nuclei. It can be seen as a simplification
of the Hubbard model; by neglecting the kinetic (hopping) energy of the spin up particles, one gets the Falicov–Kimball model.
We show that away from half-filling, i.e. if the sum of the densities of both kinds of particles differs from 1, the particles
segregate at zero temperature and for large enough repulsion. In the language of the Hubbard model, this means creating two
regions with a positive and a negative magnetization.
Our key mathematical results are lower and upper bounds for the sum of the lowest eigenvalues of the discrete Laplace operator
in an arbitrary domain, with Dirichlet boundary conditions. The lower bound consists of a bulk term, independent of the shape
of the domain, and of a term proportional to the boundary. Therefore, one lowers the kinetic energy of the itinerant particles
by choosing a domain with a small boundary. For the Falicov- Kimball model, this corresponds to having a single “compact”
domain that has no heavy particles.
Received: 21 June 2001 / Accepted: 4 January 2002 相似文献
4.
Fully and partially observed stochastic control of systems with nonlinear dynamics and terminal and running costs are considered.
Measure changes are introduced which allow both state and observation dynamics to be thought of as linear. In the case when
the terms of the cost have a special form the measure change transformation “cancels out” the nonlinearities and changes the
original nonlinear problem into a classical LQG one and standard results can be applied. We also consider unnormalized conditional
densities of the whole path as state variables and obtain dynamic programming and verification results.
R. J. Elliott wishes to acknowledge support of the Natural Sciences and Engineering Research Council of Canada, Grant A7964. 相似文献
5.
Andrew Mills Anne Lepre Nicholas Elliott Sharan Bhopal Ivan P. Parkin S. A. ONeill 《Journal of photochemistry and photobiology. A, Chemistry》2003,160(3):213-224
Pilkington Glass Activ™ represents a possible suitable successor to P25 TiO2, especially as a benchmark photocatalyst film for comparing other photocatalyst or PSH self-cleaning films. Activ™ is a glass product with a clear, colourless, effectively invisible, photocatalytic coating of titania that also exhibits PSH. Although not as active as a film of P25 TiO2, Activ™ vastly superior mechanical stability, very reproducible activity and widespread commercial availability makes it highly attractive as a reference photocatalytic film. The photocatalytic and photo-induced superhydrophilitic (PSH) properties of Activ™ are studied in some detail and the results reported. Thus, the kinetics of stearic acid destruction (a 104 electron process) are zero order over the stearic acid range 4–129 monolayers and exhibit formal quantum efficiencies (FQE) of 0.7×10−5 and 10.2×10−5 molecules per photon when irradiated with light of 365±20 and 254 nm, respectively; the latter appears also to be the quantum yield for Activ™ at 254 nm. The kinetics of stearic acid destruction exhibit Langmuir–Hinshelwood-like saturation type kinetics as a function of oxygen partial pressure, with no destruction occurring in the absence of oxygen and the rate of destruction appearing the same in air and oxygen atmospheres. Further kinetic work revealed a Langmuir adsorption type constant for oxygen of 0.45±0.16 kPa−1 and an activation energy of 19±1 kJ mol−1. A study of the PSH properties of Activ™ reveals a high water contact angle (67°) before ultra-bandgap irradiation reduced to 0° after prolonged irradiation. The kinetics of PSH are similar to those reported by others for sol–gel films using a low level of UV light. The kinetics of contact angle recovery in the dark appear monophasic and different to the biphasic kinetics reported recently by others for sol–gel films [J. Phys. Chem. B 107 (2003) 1028]. Overall, Activ™ appears a very suitable reference material for semiconductor film photocatalysis. 相似文献
6.
In a seminal paper, Martin Clark (Communications Systems and Random Process Theory, Darlington, 1977, pp. 721–734, 1978) showed how the filtered dynamics giving the optimal estimate of a Markov chain observed in Gaussian noise can be expressed
using an ordinary differential equation. These results offer substantial benefits in filtering and in control, often simplifying
the analysis and an in some settings providing numerical benefits, see, for example Malcolm et al. (J. Appl. Math. Stoch.
Anal., 2007, to appear).
Clark’s method uses a gauge transformation and, in effect, solves the Wonham-Zakai equation using variation of constants.
In this article, we consider the optimal control of a partially observed Markov chain. This problem is discussed in Elliott
et al. (Hidden Markov Models Estimation and Control, Applications of Mathematics Series, vol. 29, 1995). The innovation in our results is that the robust dynamics of Clark are used to compute forward in time dynamics for a simplified
adjoint process. A stochastic minimum principle is established. 相似文献
7.
The qualitative behavior of buckled states of two different models of elastic beams is studied. It is assumed that random imperfections affect the governing nonlinear equations. It is shown that near the first critical value of the buckling load the stochastic bifurcation is described asymptotically by an algebraic equation whose coeffficients are Gaussian random variables. The corresponding asymptotic expansion for the displacement is to lowest order a Gaussian stochastic process.Work supported by NSF Grant No. DCR81-14726.Work supported by NSF Grant No. DMS87-01895. 相似文献
8.
Previous studies using dideuterium as a solute have demonstrated the importance for orientation of the interaction between the solute molecular quadrupole moment and the average electric field gradient present in liquid crystals. With the aim of learning about additional orientational mechanisms, we have studied the temperature dependence of the 2H-NMR spectra of the liquid crystal 5CB-d19 as the solute in three liquid crystal mixtures: 55 wt % 1132/EBBA, 56·5 wt % 1132/EBBA and 70 wt % 5CB/EBBA. In these mixtures, the contribution from the environment to the average electric field gradient at the 2H nucleus of dideuterium is zero. The spectra of 5CB-d19 in the mixtures 55 wt % 1132/EBBA and 56·5 wt % 1132/EBBA are equivalent, but are different from those in 70 wt % 5CB/EBBA. The spectra of 5CB in 55 wt % 1132/EBBA and 70 wt % 5CB/EBBA are analysed using two different models for the short range potential, and param eters of the models are used to compare the potentials in the different mixtures. For a given spectral splitting of the chain C1 deuteron, the reduced short range potential is the same in all three mixtures studied. The spectral differences observed are a consequence of different nematic-isotropic phase transition temperatures combined with the effect of trans/gauche-isomerization in the hydrocarbon chain. 相似文献
9.
Rupert L. Frank Ari Laptev Elliott H. Lieb Robert Seiringer 《Letters in Mathematical Physics》2006,77(3):309-316
Inequalities are derived for power sums of the real part and the modulus of the eigenvalues of a Schrödinger operator with a complex-valued potential. 相似文献
10.
M. Bahra D. Elliott M. Reading R. Ryan 《Journal of Thermal Analysis and Calorimetry》1992,38(4):543-555
A novel instrument is described called the Thin film Analyser (TFA) which quantitatively measures changes in mechanical and rheological properties of drying films in-situ on a test panel. It is based around a simple force-sensing device, capable of carrying various probes, which can be positioned in anX-Y plane over the panel. Temperature control is achieved by means of a heating block under the sample. By imposing a thermal gradient along the block, measurements can be obtained at a series of temperatures in a single experiment. Several applications of the TFA to the drying of curable and latex-based coatings are discussed, as well as some more specialized uses. The TFA concept represents a novel approach to the thermal analysis of thin films.The authors gratefully acknowledge the design, engineering and software development work of the Instrument Group at ICI Paints, in particular John Hayton, Neil Burrows, Tony Evans and Ian Francis, who have now built three versions of the TFA. 相似文献