Spectroscopy and electronic structure of the low-energy states of ThN

Schmitz, Joel R.; Heaven, Michael C.

doi:10.1016/j.jms.2021.111426

Spectroscopy and electronic structure of the low-energy states of ThN

Journal Article · Thu Feb 04 00:00:00 EST 2021 · Journal of Molecular Spectroscopy

DOI:https://doi.org/10.1016/j.jms.2021.111426· OSTI ID:1849366

Schmitz, Joel R. ^[1]; Heaven, Michael C. ^[2]

Emory Univ., Atlanta, GA (United States). Dept. of Chemistry; Emory Univ., Atlanta, GA (United States)
Emory Univ., Atlanta, GA (United States). Dept. of Chemistry

The electronic spectrum of ThN over the range 19,600–21,200 cm^-1 is remarkably congested, showing at least twenty vibronic bands originating from the ground state zero-point level. Rotationally resolved spectra for eleven of these bands have been examined to probe the underlying reasons for the dense manifold of states. Dispersed fluorescence spectra and fluorescence decay lifetimes were measured to provide addition insights. Our experimental measurements were complemented by electronic structure calculations for the low-energy doublet and quartet states. The ab initio calculations yielded a density of excited states that was consistent with the congested spectrum. These states were derived from the formal configurations Th³⁺(6d)N^3-, Th²⁺(7s²)N^2-(2p⁵) and Th²⁺(7s6d)N²-(2p⁵). The calculations indicated that the rotational and vibrational constants would be characteristic of the electronic configurations. This prediction was not borne out by the experimental data, suggesting that the full range of inter-configurational state interactions were not captured by the computational model.

View Accepted Manuscript (DOE)

Research Organization:: Emory Univ., Atlanta, GA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: FG02-01ER15153

OSTI ID:: 1849366

Alternate ID(s):: OSTI ID: 1775982

Journal Information:: Journal of Molecular Spectroscopy, Journal Name: Journal of Molecular Spectroscopy Journal Issue: C Vol. 377; ISSN 0022-2852

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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