Bond Dissociation Energies and Electronic Calculations on the Actinide Halides ThX and UX (X = Cl, Br, I)

Kawagoe, Thomas T.; Merriles, Dakota M.; Morse, Michael D.; Peterson, Kirk A.

doi:10.1021/acs.jpca.5c04025

Bond Dissociation Energies and Electronic Calculations on the Actinide Halides ThX and UX (X = Cl, Br, I)

Journal Article · Thu Aug 14 00:00:00 EDT 2025 · The Journal of Physical Chemistry A

DOI:https://doi.org/10.1021/acs.jpca.5c04025· OSTI ID:2589738

Kawagoe, Thomas T. ^[1]; Merriles, Dakota M. ^[1]; ^[1]; ^[2]

University of Utah, Salt Lake City, UT (United States)
Washington State University, Pullman, WA (United States)

Resonant two-photon ionization spectroscopy has been used to locate predissociation thresholds in the spectra of the actinide halides ThX and UX, where X = Cl, Br, and I. These predissociation thresholds are identified as the bond dissociation energies (BDEs) of the molecules. The resulting values show very similar BDEs for the corresponding ThX and UX species, with the thorium molecules being slightly more strongly bound: D₀(ThCl) = 5.077(6) eV, D₀(ThBr) = 4.391(4) eV, D₀(ThI) = 3.537(8) eV, D₀(UCl) = 4.989(3) eV, D₀(UBr) = 4.313(3) eV, and D₀(UI) = 3.449(8) eV. Here, the estimated error limit is given in parentheses in units of the last reported digit. Spinor-based coupled cluster calculations have also been carried out on the halides of this work, including also ThF and UF. Here, the final D₀ values after including contributions due to basis set incompleteness, outer-core-correlation, picture-change, and QED effects are within 0.04 eV of the present experimental values in each case.

View Accepted Manuscript (DOE)

Research Organization:: Washington State University, Pullman, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0008501; SC0022111

OSTI ID:: 2589738

Journal Information:: The Journal of Physical Chemistry A, Journal Name: The Journal of Physical Chemistry A Journal Issue: 34 Vol. 129; ISSN 1089-5639; ISSN 1520-5215

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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energy
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Bond Dissociation Energies and Electronic Calculations on the Actinide Halides ThX and UX (X = Cl, Br, I)

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