Analysis of the Spectra of Jahn-Teller Distorted Radicals

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Date

2018-05

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The Ohio State University

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Abstract

Defining appropriate potential energy surfaces (PES) for Jahn-Teller active molecules remains problematic due to the breakdown of the Born-Oppenheimer approximation. Quantification of the magnitude of the Jahn-Teller geometric distortions is required for regaining understandings of molecular and spectroscopic properties of these molecules. Recent experimental spectra of the cyclopentadienyl radical, C5H5, challenge theoretical understandings of the Jahn-Teller effect. Generalized methodology is developed utilizing ab-initio electronic structure calculations in concert with vibronic eigenfunctions in order to determine the Watson term, h1, an element of rotational model. Tabulated h1 values provide insights to rotational structure of vibrational bands for experimental identification as well as further understanding of the Jahn-Teller potential surfaces. Features of the cyclopentadienyl radical spectra are predicted using this method. Application to the nitrate radical, NO3, underscores insufficiencies in parameterized potentials used in the case of strong Jahn-Teller coupling.

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Spectroscopy, Radicals, Theoretical Chemistry, Jahn-Teller

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