AB INITIO STUDY OF THE ELECTRONIC SPECTRUM OF THE $NCl_{2}$ RADICAL

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1994

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Ohio State University

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The equilibrium geometries, excitation energies force constant and vibrational frequencies for the low-lying electronic states X $^{2}B_{1+} ^{2}A_{1+}, ^{2}B_{2}$ and $^{2}A_{2}$ of the $NCl_{8}$ radical have been calculated at the MRSDCI/DZ--P level. Our calculations indicate that the $X ^{2}B_{1} \rightarrow ^{2}A_{2}$ transition may correspond to the $\bar{X} \rightarrow \bar{X}$ band system which lies between 275--314 mm in absorption spectrum of refs. [1.2]. Our calculated excitation energies for X $^{2}B_{2} \rightarrow ^{2}A_{1}$ AND $X ^{2}B_{1} \rightarrow ^{2}A_{2}$, vibrational frequencies for the X $^{2}B_{1}$ and $^{2}A_{2}$ states and the geometry for the $X ^{2}B_{1}$ state are in agreement with available experimental data. The electronic transition dipale moments, oscillator strengths for the $^{2}A_{2} \rightarrow X ^{2}B_{1}$ and $^{2}A_{2} \rightarrow X ^{1}B_{1}$ transitions and radiative lifetimes for the $^{2}A_{1}$ and $^{2}A_{g}$ states are calculated based on the MRSDCI wavefunctions, predicting value of the radiative lifetime for the $^{2}A_{1}$ state also in reasonable agreement with experiment.

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$^{1}$A.G. Briggs ad R.G.W. Norrish, Proc. Roy. Soc. A278, 27 (1964). $^{2}$V.V. Azatyan {et al}., Dokl. Phys. Chem, 249, 1056 (1980).
Author Institution: Group 325, Department of Chemistry, Nanjing University of Science and Technology

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