Characterization of berkelium(III) dipicolinate and borate compounds in solution and the solid state

Mark A. Silver; Samantha K. Cary; Jason A. Johnson; Ryan E. Baumbach; Alexandra A. Arico; Morgan Luckey; Matthew Urban; Jamie C. Wang; Matthew J. Polinski; Alexander Chemey; Guokui Liu; Kuan Wen Chen; Shelley M. Van Cleve; Matthew L. Marsh; Teresa M. Eaton; Lambertus J. Van De Burgt; Ashley L. Gray; David E. Hobart; Kenneth Hanson; Laurent Maron; Frédéric Gendron; Jochen Autschbach; Manfred Speldrich; Paul Kögerler; Ping Yang; Jenifer Braley; Thomas E. Albrecht-Schmitt

doi:10.1126/science.aaf3762

Characterization of berkelium(III) dipicolinate and borate compounds in solution and the solid state

Mark A. Silver, Samantha K. Cary, Jason A. Johnson, Ryan E. Baumbach, Alexandra A. Arico, Morgan Luckey, Matthew Urban, Jamie C. Wang, Matthew J. Polinski, Alexander Chemey, Guokui Liu, Kuan Wen Chen, Shelley M. Van Cleve, Matthew L. Marsh, Teresa M. Eaton, Lambertus J. Van De Burgt, Ashley L. Gray, David E. Hobart, Kenneth Hanson, Laurent MaronFrédéric Gendron, Jochen Autschbach, Manfred Speldrich, Paul Kögerler, Ping Yang, Jenifer Braley, Thomas E. Albrecht-Schmitt

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Abstract

Berkelium is positioned at a crucial location in the actinide series between the inherently stable half-filled 5f7 configuration of curium and the abrupt transition in chemical behavior created by the onset of a metastable divalent state that starts at californium. However, the mere 320-day half-life of berkelium's only available isotope, 249Bk, has hindered in-depth studies of the element's coordination chemistry. Herein, we report the synthesis and detailed solid-state and solution-phase characterization of a berkelium coordination complex, Bk(III)tris(dipicolinate), as well as a chemically distinct Bk(III) borate material for comparison.We demonstrate that berkelium's complexation is analogous to that of californium. However, from a range of spectroscopic techniques and quantum mechanical calculations, it is clear that spin-orbit coupling contributes significantly to berkelium's multiconfigurational ground state.

Original language	English
Article number	aaf3762
Journal	Science
Volume	353
Issue number	6302
DOIs	https://doi.org/10.1126/science.aaf3762
State	Published - Aug 26 2016
Externally published	Yes

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Silver, M. A., Cary, S. K., Johnson, J. A., Baumbach, R. E., Arico, A. A., Luckey, M., Urban, M., Wang, J. C., Polinski, M. J., Chemey, A., Liu, G., Chen, K. W., Van Cleve, S. M., Marsh, M. L., Eaton, T. M., Van De Burgt, L. J., Gray, A. L., Hobart, D. E., Hanson, K., ... Albrecht-Schmitt, T. E. (2016). Characterization of berkelium(III) dipicolinate and borate compounds in solution and the solid state. Science, 353(6302), Article aaf3762. https://doi.org/10.1126/science.aaf3762

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title = "Characterization of berkelium(III) dipicolinate and borate compounds in solution and the solid state",

abstract = "Berkelium is positioned at a crucial location in the actinide series between the inherently stable half-filled 5f7 configuration of curium and the abrupt transition in chemical behavior created by the onset of a metastable divalent state that starts at californium. However, the mere 320-day half-life of berkelium's only available isotope, 249Bk, has hindered in-depth studies of the element's coordination chemistry. Herein, we report the synthesis and detailed solid-state and solution-phase characterization of a berkelium coordination complex, Bk(III)tris(dipicolinate), as well as a chemically distinct Bk(III) borate material for comparison.We demonstrate that berkelium's complexation is analogous to that of californium. However, from a range of spectroscopic techniques and quantum mechanical calculations, it is clear that spin-orbit coupling contributes significantly to berkelium's multiconfigurational ground state.",

author = "Silver, {Mark A.} and Cary, {Samantha K.} and Johnson, {Jason A.} and Baumbach, {Ryan E.} and Arico, {Alexandra A.} and Morgan Luckey and Matthew Urban and Wang, {Jamie C.} and Polinski, {Matthew J.} and Alexander Chemey and Guokui Liu and Chen, {Kuan Wen} and {Van Cleve}, {Shelley M.} and Marsh, {Matthew L.} and Eaton, {Teresa M.} and {Van De Burgt}, {Lambertus J.} and Gray, {Ashley L.} and Hobart, {David E.} and Kenneth Hanson and Laurent Maron and Fr{\'e}d{\'e}ric Gendron and Jochen Autschbach and Manfred Speldrich and Paul K{\"o}gerler and Ping Yang and Jenifer Braley and Albrecht-Schmitt, {Thomas E.}",

year = "2016",

month = aug,

day = "26",

doi = "10.1126/science.aaf3762",

language = "English",

volume = "353",

journal = "Science",

issn = "0036-8075",

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Silver, MA, Cary, SK, Johnson, JA, Baumbach, RE, Arico, AA, Luckey, M, Urban, M, Wang, JC, Polinski, MJ, Chemey, A, Liu, G, Chen, KW, Van Cleve, SM, Marsh, ML, Eaton, TM, Van De Burgt, LJ, Gray, AL, Hobart, DE, Hanson, K, Maron, L, Gendron, F, Autschbach, J, Speldrich, M, Kögerler, P, Yang, P, Braley, J & Albrecht-Schmitt, TE 2016, 'Characterization of berkelium(III) dipicolinate and borate compounds in solution and the solid state', Science, vol. 353, no. 6302, aaf3762. https://doi.org/10.1126/science.aaf3762

TY - JOUR

T1 - Characterization of berkelium(III) dipicolinate and borate compounds in solution and the solid state

AU - Silver, Mark A.

AU - Cary, Samantha K.

AU - Johnson, Jason A.

AU - Baumbach, Ryan E.

AU - Arico, Alexandra A.

AU - Luckey, Morgan

AU - Urban, Matthew

AU - Wang, Jamie C.

AU - Polinski, Matthew J.

AU - Chemey, Alexander

AU - Liu, Guokui

AU - Chen, Kuan Wen

AU - Van Cleve, Shelley M.

AU - Marsh, Matthew L.

AU - Eaton, Teresa M.

AU - Van De Burgt, Lambertus J.

AU - Gray, Ashley L.

AU - Hobart, David E.

AU - Hanson, Kenneth

AU - Maron, Laurent

AU - Gendron, Frédéric

AU - Autschbach, Jochen

AU - Speldrich, Manfred

AU - Kögerler, Paul

AU - Yang, Ping

AU - Braley, Jenifer

AU - Albrecht-Schmitt, Thomas E.

PY - 2016/8/26

Y1 - 2016/8/26

N2 - Berkelium is positioned at a crucial location in the actinide series between the inherently stable half-filled 5f7 configuration of curium and the abrupt transition in chemical behavior created by the onset of a metastable divalent state that starts at californium. However, the mere 320-day half-life of berkelium's only available isotope, 249Bk, has hindered in-depth studies of the element's coordination chemistry. Herein, we report the synthesis and detailed solid-state and solution-phase characterization of a berkelium coordination complex, Bk(III)tris(dipicolinate), as well as a chemically distinct Bk(III) borate material for comparison.We demonstrate that berkelium's complexation is analogous to that of californium. However, from a range of spectroscopic techniques and quantum mechanical calculations, it is clear that spin-orbit coupling contributes significantly to berkelium's multiconfigurational ground state.

AB - Berkelium is positioned at a crucial location in the actinide series between the inherently stable half-filled 5f7 configuration of curium and the abrupt transition in chemical behavior created by the onset of a metastable divalent state that starts at californium. However, the mere 320-day half-life of berkelium's only available isotope, 249Bk, has hindered in-depth studies of the element's coordination chemistry. Herein, we report the synthesis and detailed solid-state and solution-phase characterization of a berkelium coordination complex, Bk(III)tris(dipicolinate), as well as a chemically distinct Bk(III) borate material for comparison.We demonstrate that berkelium's complexation is analogous to that of californium. However, from a range of spectroscopic techniques and quantum mechanical calculations, it is clear that spin-orbit coupling contributes significantly to berkelium's multiconfigurational ground state.

UR - http://www.scopus.com/inward/record.url?scp=84984914447&partnerID=8YFLogxK

U2 - 10.1126/science.aaf3762

DO - 10.1126/science.aaf3762

M3 - Article

AN - SCOPUS:84984914447

SN - 0036-8075

VL - 353

JO - Science

JF - Science

IS - 6302

M1 - aaf3762

ER -

Characterization of berkelium(III) dipicolinate and borate compounds in solution and the solid state

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