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A novel non-active model to account for the leak of zero-point energy in trajectory calculations. Application to H + O2 reaction near threshold

✍ Scribed by A.J.C. Varandas


Publisher
Elsevier Science
Year
1994
Tongue
English
Weight
971 KB
Volume
225
Category
Article
ISSN
0009-2614

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✦ Synopsis


A novel non-active model to correct for the leak of zero-point energy in quasi-classical trajectory calculations is proposed. It consists of eliminating every trajectory that fails to satisfy the zero-point energy requirement of quantum mechanics at the end of the trajectory, and then correct the results using a unified statistical approach which takes into account the relative probabibties of the reactive and non-reactive events. The correction factor assumes a simple analytic form, adding no extra cost to the traditional quasiclassical trajectory approach. Test calculations are presented for the total reactivity of the H+ Oa reaction out of the initial vibrational-rotational state (u, i) = (0, 0), keeping the total angular momentum .I= 0. Comparison of the results with quantum mechanical reactivities calculated on the same (DMBE IV) potential energy surface shows good agreement. A possible generalization of the model to require a local zero-point energy along the trajectory is pointed out.