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81.
82.
David W. Schwenke Steven L. Mielke Donald G. Truhlar 《Theoretical chemistry accounts》1991,79(3-4):241-269
Summary We have developed efficient and accurate techniques for the calculation of quantum mechanical reaction probabilities of atom-diatom exchange reactions in the gas phase, and we have optimized a computer code employing these techniques and applied it sucessfully to several systems. In this paper we consider further strategies for improving the algorithm to allow even more demanding applications. In this context, improvement means that equivalent results can be obtained using fewer computational resources (computer time or storage) or that an equivalent expenditure of resources can yield higher accuracy. The new strategies discussed here lead to improvement in both of these areas. Two areas of special focus in the present paper are (i) the finite difference boundary value method used for calculating distorted wave Green's functions and regular solutions for scattering by the distortion potential and (ii) the choice of the distortion potential itself. Among other results included here is the first application of the outgoing wave or scattered wave variational principle to reactive scattering. 相似文献
83.
The hydrogen abstraction reaction of O(^3P) with Si2H6 has been studied theoretially. Two transition states of ^3A″ and ^3A′ symmetries have been located for this abstraction reaction. Geometries have been optimized at the UMP2 leve with 6-311G (d) basis set. G3MP2 has been used for the final single-point energy calculation. The rate constants have been calculated over a wide temperature range of 200-3000K using canonical variational transition-state sheory (CVT) with small curvature tunneling effect(SCT). The calculated CVT/SCT rate constants match well with the experimental value. 相似文献
84.
A. Linnemann 《Journal of Optimization Theory and Applications》1982,38(4):483-511
In this paper, we present a unified theory of first-order and higher-order necessary optimality conditions for abstract vector optimization problems in normed linear spaces. We prove general multiplier rules, from which nearly all known first-order, second-order, and higher-order necessary conditions can be derived. In the last section, we prove higher-order necessary conditions for semi-infinite programming problems.This work was developed within the Forschungsschwerpunkt Dynamische Systeme, Universität Bremen, Bremen, West Germany.The author wishes to thank Prof. Dr. D. Hinrichsen for his helpful remarks and discussions during the preparation of this work. 相似文献
85.
Danny K. Long Wolfgang Bangerth Derek R. Handwerk Christopher B. Whitehead Patrick D. Shipman Richard G. Finke 《Journal of computational chemistry》2022,43(1):43-56
In order to quantitatively predict nano- as well as other particle-size distributions, one needs to have both a mathematical model and estimates of the parameters that appear in these models. Here, we show how one can use Bayesian inversion to obtain statistical estimates for the parameters that appear in recently derived mechanism-enabled population balance models (ME-PBM) of nanoparticle growth. The Bayesian approach addresses the question of “how well do we know our parameters, along with their uncertainties?.” The results reveal that Bayesian inversion statistical analysis on an example, prototype nanoparticle formation system allows one to estimate not just the most likely rate constants and other parameter values, but also their SDs, confidence intervals, and other statistical information. Moreover, knowing the reliability of the mechanistic model's parameters in turn helps inform one about the reliability of the proposed mechanism, as well as the reliability of its predictions. The paper can also be seen as a tutorial with the additional goal of achieving a “Gold Standard” Bayesian inversion ME-PBM benchmark that others can use as a control to check their own use of this methodology for other systems of interest throughout nature. Overall, the results provide strong support for the hypothesis that there is substantial value in using a Bayesian inversion methodology for parameter estimation in particle formation systems. 相似文献
86.
Mass transfer from irregular-shaped naphthalene particles (100-200 inn in size) was studitd in an electrodynamic balance. Charged particles were suspended in an electrostatic field directly in line with a calibrated air jet. Mass and size change histories were obtained under ambient conditions, and under steady- and pulsed-flow conditions. For natural convection, the time-averaged Sherwood number was similar to that for spheres. Forced-convection Sherwood number under steady-flow conditions was strongly dependent on particle shape and panicle Reynolds number, and was consistently higher than values predicted for spheres at comparable Reynolds numbers. This study validates the technique and indicates the shape effect on mass transfer form single particles. 相似文献
87.
This article considers a co-reinsurance strategy that (1) protects insurance companies against catastrophic risks; (2) enables insurers to gather sufficient information about the different risk attitudes of reinsurers and diversify their reinsured risks; (3) enables insurers to create better risk-sharing profiles by balancing the risk tolerances of reinsurers; (4) has the benefit of allowing reinsurers to accumulate experience with risks with which they are unfamiliar; (5) reduces the overall direct cost of a reinsurance contract; (6) allows a government to back some insurance products, such as the terrorism insurance programs that were established in many countries after the September 11th terrorist attacks; and (7) reflects the practical reinsurance industry of some countries, such as Iran. Such a co-reinsurance strategy can be fully determined by estimating its parameters whenever three optimal criteria are satisfied and prior information about the unknown parameters is available. Two simulation-based studies have been conducted to demonstrate (1) the practical applications of our findings and (2) the possible impact of any type of dependency between the co-reinsurance’s parameters and the evaluated optimal co-reinsurance strategy. 相似文献
88.
Eugene Santos Qi Gu Eunice E. Santos 《International Journal of Approximate Reasoning》2013,54(8):1000-1012
For a knowledge-based system that fails to provide the correct answer, it is important to be able to tune the system while minimizing overall change in the knowledge-base. There are a variety of reasons why the answer is incorrect ranging from incorrect knowledge to information vagueness to incompleteness. Still, in all these situations, it is typically the case that most of the knowledge in the system is likely to be correct as specified by the expert (s) and/or knowledge engineer (s). In this paper, we propose a method to identify the possible changes by understanding the contribution of parameters on the outputs of concern. Our approach is based on Bayesian Knowledge Bases for modeling uncertainties. We start with single parameter changes and then extend to multiple parameters. In order to identify the optimal solution that can minimize the change to the model as specified by the domain experts, we define and evaluate the sensitivity values of the results with respect to the parameters. We discuss the computational complexities of determining the solution and show that the problem of multiple parameters changes can be transformed into Linear Programming problems, and thus, efficiently solvable. Our work can also be applied towards validating the knowledge base such that the updated model can satisfy all test-cases collected from the domain experts. 相似文献
89.
《International Journal of Approximate Reasoning》2014,55(5):1235-1251
We develop a global sensitivity analysis to measure the robustness of the Bayesian estimators with respect to a class of prior distributions. This class arises when we consider multiplicative contamination of a base prior distribution. A similar structure was presented by van der Linde [12]. Some particular specifications for this multiplicative contamination class coincide with well known families of skewed distributions. In this paper, we explore the skew-normal multiplicative contamination class for the prior distribution of the location parameter of a normal model. Results of a Bayesian conjugation and expressions for some measures of distance between posterior means and posterior variance are obtained. We also elaborate on the behavior of the posterior means and of the posterior variances through a simulation study. 相似文献
90.
《数学研究通讯:英文版》2016,(4):325-331
In this paper, we consider the problem of determining the order of INAR(q) model on the basis of the Bayesian estimation theory. The Bayesian es-timator for the order is given with respect to a squared-error loss function. The consistency of the estimator is discussed. The results of a simulation study for the estimation method are presented. 相似文献