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    Rights statement: This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright ©2018 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/jacs.8b09436

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Energy-Degeneracy-Driven Covalency in Actinide Bonding

Research output: Contribution to Journal/Magazine › Journal article › peer-review

Published

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Energy-Degeneracy-Driven Covalency in Actinide Bonding. / Su, Jing; Batista, Enrqiue R.; Boland, Kevin S. et al.
In: Journal of the American Chemical Society, Vol. 140, 26.12.2018, p. 17977-17984.

Research output: Contribution to Journal/Magazine › Journal article › peer-review

Harvard

Su, J, Batista, ER, Boland, KS, Bone, SE, Bradley, JA, Cary, SK, Clark, DL, Conradson, SD, Ditter, AS, Kaltsoyannis, N, Keith, JM, Kerridge, A, Kozimor, SA, Loble, MW, Martin, RL, Minasian, SG, Mocko, V, La Pierre, HS, Seidler, GT, Shuh, DK, Wilkerson, MP, Wolfsberg, LE & Yang, P 2018, 'Energy-Degeneracy-Driven Covalency in Actinide Bonding', Journal of the American Chemical Society, vol. 140, pp. 17977-17984. https://doi.org/10.1021/jacs.8b09436

APA

Su, J., Batista, E. R., Boland, K. S., Bone, S. E., Bradley, J. A., Cary, S. K., Clark, D. L., Conradson, S. D., Ditter, A. S., Kaltsoyannis, N., Keith, J. M., Kerridge, A., Kozimor, S. A., Loble, M. W., Martin, R. L., Minasian, S. G., Mocko, V., La Pierre, H. S., Seidler, G. T., ... Yang, P. (2018). Energy-Degeneracy-Driven Covalency in Actinide Bonding. Journal of the American Chemical Society, 140, 17977-17984. https://doi.org/10.1021/jacs.8b09436

Vancouver

Su J, Batista ER, Boland KS, Bone SE, Bradley JA, Cary SK et al. Energy-Degeneracy-Driven Covalency in Actinide Bonding. Journal of the American Chemical Society. 2018 Dec 26;140:17977-17984. Epub 2018 Dec 12. doi: 10.1021/jacs.8b09436

Author

Su, Jing ; Batista, Enrqiue R. ; Boland, Kevin S. et al. / Energy-Degeneracy-Driven Covalency in Actinide Bonding. In: Journal of the American Chemical Society. 2018 ; Vol. 140. pp. 17977-17984.

Bibtex

@article{c8c6f78bc40d4b77a195394aee02bfa8,
title = "Energy-Degeneracy-Driven Covalency in Actinide Bonding",
abstract = "Evaluating the nature of chemical bonding for actinide elements represents one of the most important and long-standing problems in actinide science. We directly address this challenge and contribute a Cl K-edge X-ray absorption spectroscopy and relativistic density functional theory study that quantitatively evaluates An–Cl covalency in AnCl62– (AnIV = Th, U, Np, Pu). The results showed significant mixing between Cl 3p- and AnIV 5f- and 6d-orbitals (t1u*/t2u* and t2g*/eg*), with the 6d-orbitals showing more pronounced covalent bonding than the 5f-orbitals. Moving from Th to U, Np, and Pu markedly changed the amount of M–Cl orbital mixing, such that AnIV 6d- and Cl 3p-mixing decreased and metal 5f- and Cl 3p-orbital mixing increased across this series.",
author = "Jing Su and Batista, {Enrqiue R.} and Boland, {Kevin S.} and Bone, {Sharon E.} and Bradley, {Joseph A.} and Cary, {Samantha K.} and Clark, {David L.} and Conradson, {Steven D.} and Ditter, {Alex S.} and Nikolas Kaltsoyannis and Keith, {Jason M.} and Andrew Kerridge and Kozimor, {Stosh A.} and Loble, {Matthias W.} and Martin, {Richard L.} and Minasian, {Stefan G.} and Veronika Mocko and {La Pierre}, {Henry S.} and Seidler, {Gerald T.} and Shuh, {David K.} and Wilkerson, {Marianne P.} and Wolfsberg, {Laura E.} and Ping Yang",
note = "This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright {\textcopyright}2018 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/jacs.8b09436",
year = "2018",
month = dec,
day = "26",
doi = "10.1021/jacs.8b09436",
language = "English",
volume = "140",
pages = "17977--17984",
journal = "Journal of the American Chemical Society",
issn = "0002-7863",
publisher = "AMER CHEMICAL SOC",

}

RIS

TY - JOUR

T1 - Energy-Degeneracy-Driven Covalency in Actinide Bonding

AU - Su, Jing

AU - Batista, Enrqiue R.

AU - Boland, Kevin S.

AU - Bone, Sharon E.

AU - Bradley, Joseph A.

AU - Cary, Samantha K.

AU - Clark, David L.

AU - Conradson, Steven D.

AU - Ditter, Alex S.

AU - Kaltsoyannis, Nikolas

AU - Keith, Jason M.

AU - Kerridge, Andrew

AU - Kozimor, Stosh A.

AU - Loble, Matthias W.

AU - Martin, Richard L.

AU - Minasian, Stefan G.

AU - Mocko, Veronika

AU - La Pierre, Henry S.

AU - Seidler, Gerald T.

AU - Shuh, David K.

AU - Wilkerson, Marianne P.

AU - Wolfsberg, Laura E.

AU - Yang, Ping

N1 - This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright ©2018 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/jacs.8b09436

PY - 2018/12/26

Y1 - 2018/12/26

N2 - Evaluating the nature of chemical bonding for actinide elements represents one of the most important and long-standing problems in actinide science. We directly address this challenge and contribute a Cl K-edge X-ray absorption spectroscopy and relativistic density functional theory study that quantitatively evaluates An–Cl covalency in AnCl62– (AnIV = Th, U, Np, Pu). The results showed significant mixing between Cl 3p- and AnIV 5f- and 6d-orbitals (t1u*/t2u* and t2g*/eg*), with the 6d-orbitals showing more pronounced covalent bonding than the 5f-orbitals. Moving from Th to U, Np, and Pu markedly changed the amount of M–Cl orbital mixing, such that AnIV 6d- and Cl 3p-mixing decreased and metal 5f- and Cl 3p-orbital mixing increased across this series.

AB - Evaluating the nature of chemical bonding for actinide elements represents one of the most important and long-standing problems in actinide science. We directly address this challenge and contribute a Cl K-edge X-ray absorption spectroscopy and relativistic density functional theory study that quantitatively evaluates An–Cl covalency in AnCl62– (AnIV = Th, U, Np, Pu). The results showed significant mixing between Cl 3p- and AnIV 5f- and 6d-orbitals (t1u*/t2u* and t2g*/eg*), with the 6d-orbitals showing more pronounced covalent bonding than the 5f-orbitals. Moving from Th to U, Np, and Pu markedly changed the amount of M–Cl orbital mixing, such that AnIV 6d- and Cl 3p-mixing decreased and metal 5f- and Cl 3p-orbital mixing increased across this series.

U2 - 10.1021/jacs.8b09436

DO - 10.1021/jacs.8b09436

M3 - Journal article

VL - 140

SP - 17977

EP - 17984

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

ER -