Advances in Chemical Physics, Vol. 115 by Ilya Prigogine, Stuart A. Rice

By Ilya Prigogine, Stuart A. Rice

The Advances in Chemical Physics sequence presents the chemical physics and actual chemistry fields with a discussion board for severe, authoritative reviews of advances in each quarter of the self-discipline. jam-packed with state of the art learn pronounced in a cohesive demeanour now not discovered somewhere else within the literature, each one quantity of the Advances in Chemical Physics sequence serves because the ideal complement to any complicated graduate type dedicated to the research of chemical physics.

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A physically intuitive approach to global optimization was provided by simulated annealing [l85]. The system is equilibrated at a high energy and cooled slowly enough to maintain equilibrium until the low-energy state is reached. Problems may arise when the identity of the global free energy minimum changes as the temperature is decreased. The system may then be trapped in what becomes only a local minimum. The multiple-funnel landscapes discussed in some of the following sections correspond to such a scenario.

2 2 ~This . result suggests that the pathways passing over the highest-energy transition state on the lowest-energy pathway determine the interfunnel dynamics. E, for icos + fcc, however, is significantly lower than the overall potential barrier for the reverse process, which is 3 . 5 4 ~starting , from the lowest-energy icosahedral minimum. We can analyze these results further from a simple model of the dynamics between two funnels, A and B. First, we assign the label 1 to the lowest- 52 DAVID J.

Minima only connected to one other minimum) that had a very low equilibrium occupation probability. The solution of the master equation can provide the time evolution of the occupation probabilities of all the minima, but it is not immediately obvious how to extract interfunnel rate constants from this information when there are many different pathways between the funnels. , A + B with “forward” and “reverse” rate constants k + and k - . 51) At sufficiently low temperature only the two funnels will be significantly occupied at equilibrium.

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