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101.
A potentially biomimetic synthesis of the guanidine-containing marine natural product crambescidin 359 via a double Michael addition of guanidine to a suitably functionalised bis-enone is reported. 相似文献
102.
Nigel J. Newton 《Journal of statistical physics》2008,133(4):711-737
This paper connects non-equilibrium statistical mechanics and optimal nonlinear filtering. The latter concerns the observation-conditional
behaviour of Markov signal processes, and thus provides a tool for investigating statistical mechanics with partial observations. These allow entropy
reduction, illustrating Landauer’s Principle in a quantitative way.
The joint process comprising a signal and its nonlinear filter is irreversible in its invariant distribution, which therefore
corresponds to a non-equilibrium stationary state of the associated joint system. Macroscopic entropy and energy flows are identified for this state. Since these are driven by observations internal to the system, they do not cause entropy increase, and so the joint system makes statistical mechanical sense in reverse
time.
Time reversal yields a dual system in which the signal and filter exchange roles. Despite the structural similarity of the original and dual systems,
there is a substantial asymmetry in their complexities. This reveals the direction of time, despite the systems being in stationary
states that do not produce entropy.
This work was partially supported by Leverhulme Trust Research Fellowship 2003/0426, by MURI Grant F49620-02-1-0325 (Complex
Adaptive Networks for Co-operative Control), by ARO-MURI Grant DAAD19-00-1-0466 (Data Fusion in Large Arrays of Microsensors
(sensor web)) and by NSF-ITR Grant CCR-0325774 Collaborative Research: New Approaches to Experimental Design and Statistical
Analysis of Genomic and Structural Biological Data from Multiple Sources. 相似文献
103.
Nigel Howard 《The Journal of the Operational Research Society》1993,44(6):613-623
This paper addresses two questions. (i) What is the role of emotions in decision-making? (ii) Can emotions be attributed to organizations, and is their role in decisions made between organizations the same as in decisions made between individual people? The answers given to question (ii) are yes and yes. The proposed answer to question (i) is based upon a game-theoretic approach, which considers how emotions may be of strategic benefit to game players. 相似文献
104.
Cheng F Kelly SM Young NA Clark S Francesconi MG Lefebvre F Bradley JS 《Chemical communications (Cambridge, England)》2005,(45):5662-5664
We report a general method for the preparation of transition-metal silicon nitride nanocomposites; for example, mesoporous Pd-Si3N4 nanocomposite materials with high surface area were prepared by pyrolysis of a silicon palladium imide-chloride complex which was synthesized by reaction of silicon diimide gel with palladium chloride. These porous nanocomposites catalyse organic reactions. 相似文献
105.
106.
I.Ralph C. Bick Mohammad A. Hai Nigel W. Preston Rex T. Gallagher 《Tetrahedron letters》1980,21(6):545-546
Aristotelinone and serratoline, two new Aristotelia alkaloids, are shown to have indole and indolenine structures respectively from their spectra and reduction products. 相似文献
107.
We report the first study of the effects of hydrostatic pressure on α-2° KIEs for an enzyme-catalysed H-transfer reaction that occurs by 'deep' tunnelling. High pressure causes a significant decrease in the observed α-2° KIE on the pre-steady-state hydride transfer from NADH to FMN in the flavoprotein morphinone reductase. We have recently shown that high pressure causes a reduction in macroscopic reaction barrier width for this reaction. Using DFT vibrational analysis of a simple active site model, we posit that the decrease in α-2° KIE with pressure may arise due to a decrease in the vibrational coupling between the NADH primary (transferred) and secondary hydrogens in the 'tunnelling ready configuration', which more closely resembles the reactant state than the transition state. 相似文献
108.
Goldenfeld N 《Physical review letters》2006,96(4):044503
I present empirical evidence that turbulent flows are closely analogous to critical phenomena, from a reanalysis of friction factor measurements in rough pipes. The data collapse found here corresponds to Widom scaling near critical points, and implies that a full understanding of turbulence requires explicit accounting for boundary roughness. 相似文献
109.
Muon spin relaxation has been used to study the muon dynamics in the layered zirconium phosphate Zr(H(2)PO(4))(PO(4)).2H(2)O as a function of temperature. Radiofrequency decoupling was used to establish the origin of the local dipolar field as coupling with (1)H spins. Muons were trapped at two sites, one identified as HMuO and the other consistent with PO-Mu on the basis of their zero-field second moments. Although a small decrease in the local nuclear dipolar field was seen with temperature, the muons remained essentially static over the temperature range 20-300 K. 相似文献
110.
Hydrogen transfer--an essential component of most biological reactions--is a quantum problem. A crucial question of great current interest is how enzymes modulate the quantum dynamics of hydrogen transfer to achieve their outstanding catalytic properties. That tunnelling occurs is now widely accepted, with the conceptual frameworks incorporating protein motion into the enzymic H-tunnelling process. Computational simulation can be used to help elucidate how enzymes work and facilitate H-tunnelling at the atomic level. We review the strength of a multidisciplinary approach--combining computational simulations with enzyme kinetics and structural biology--in revealing tunnelling mechanisms in enzymes. We focus on two paradigm systems--aromatic amine dehydrogenase, in which H-tunnelling is facilitated by fast (sub-picosecond) short range motions, and dihydrofolate reductase, in which a network of long-range coupled motions drives the tunnelling event. 相似文献