Development of Global Three-Dimensional Potentials for OH/D-Ar($^{2}\Sigma^{*}$) and $OH/D-Kr(^{2}\Sigma^{+}$): Fitting and Assigning Experimental Data.

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1992

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Ohio State University

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We have calculated vibrational energy intervals for the A state van der Waals molecules OH/D-Ar and OH/D-Kr (v=0 and v=1). In the calculations we used an exact method for zero rotational angular momentum (N=0) and a centrifugal sudden approximation for N=1. The development of the potentials was based on modifications of our previous two-dimensional $surface^{1}$. In the new surfaces we included explicit OH/D vibrational dependence. By a trial-and-error procedure the potential parameters were optimized, for each potential, to give good agreement with the observed vibrational intervals and isotope shifts. The calculated rotational constants were also found to be in good agreement with the experimental values. A novel inverse isotope $effect^{2}$, noted for the van der Waals stretching vibration, was predicted and rationalized by this calculations. It was found that the inverse isotope effect is smaller in OH/D-Kr compared to OH/D-Ar. This is due to the fact the OH/D-Kr is bound approximately twice as strongly as OH/D-Ar.

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1. J.M. Bowman, B. Gazdy, P. Schafer, and M.C. Heaven, J. Chem. Phys. 94, 2226 (1990); 8858E, (1990). 2. U. Schnupf, J.M. Bowman, and M.C. Heaven, Vibrational Calculations and Potential Determination for ArOH/D (v=0,1), Chem. Phys. Lett., in press.
Author Institution: Department of Chemistry, Emory University

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