MCSCF STUDY OF THE LOW-LYING ELECTRONIC STATES OF $NO_{2}$ MCSCF

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1974

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Ohio State University

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Abstract

wave functions have been constructed for seven low-lying electronic states of $NO_{2}$ using the Optimized Valence Configurations (OVC) formalism developed by Das and Wahl. The combination of a double-zeta quality basis with extensive treatment of molecular correlation is expected to yield results of significantly higher accuracy than those reported previously for $NO_{2}$. The ordering of states for vertical excitation is in agreement with the work of $Hay.^{1}$ However, geometry optimization for all states reveals the striking prediction that the minima of the $^{2}B_{2}$ and $^{2}A_{2}$ states lie 0.54 eV and 0.76 eV, respectively, above the minimum of the $^{2}A_{1}$ ground state. The implications of our results for the spectroscopic behavior of $NO_{2}$ will be discussed. Preliminary calculations employing d-functions in the basis will also be presented; these are expected to yield nearly quantitative geometrical parameters, excitation energies, and vibrational frequencies.

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This work was supported, in part, by the Air Force, Delivery Order F33615-72-M-5015 and by the National Science Foundation. $^{1}$P. J. Hay, J. Cham. Phys. 58, 4706 (1973).
Author Institution: Department s of Chemistry, Biophysics Michigan State University; Chemistry Division, Argonne National Laboratory Argonne; National Bureau of Standards, Argonne National Laboratory Argonne

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