ABSOLUTE INFRARED INTENSITIES OF FUNDAMENTAL MODES OF $H_{2}O$. CALCULATIONS AND EXPERIMENTS WITH MATRIX-ISOLATED $H_{2}O$

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1987

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Ohio State University

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Ab initio MO calcutations of infrared intensities of $H_{2}O$ predict infrared intensities for the fundmental modes that differ considerably from the reported experimental values. Even when these calculations are made at the highest level of theory (the dipole derivatives were calculated with a very large basis set, using fourth order MBPT and CCSD + T(CCSD)) the predictions for the intensity of $\nu_{1}$ and for $\nu_{2}$ are too high, compared with experimental values. This discrepancy has inspired us to measure relative intensities of these fundamental modes for samples of $H_{2}O$ isolated in Ar, $N_{2}$ and CO matrices. The results will be discussed critically in an attempt to resolve the discrepancy between theory and experiment for this important test $molecule.

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^{1}$ Work done at the Department of Chemistry, University of Florida, Gainesville, FL 32611, Work supported by NIH Grant No. GM32988 and by CRDEC Contract No. DAA15-85-COO34. $^{2}$ On leave 1986-7 from the Institute of Physics, Polish Academy of Science, 02668 Warsaw, Poland.
Author Institution: Department of Chemistry, University of Florida

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