3d-Metal Induced Magnetic Ordering on U(IV) Atoms as a Route toward U(IV) Magnetic Materials
- 13 February 2019
- journal article
- research article
- Published by American Chemical Society (ACS) in Journal of the American Chemical Society
- Vol. 141 (9), 3838-3842
- https://doi.org/10.1021/jacs.9b00345
Abstract
Uranium(IV) 5f2 magnetism is dominated by a transition from a triplet to a singlet ground state at low temperatures. For the first time, we achieved magnetic ordering of U(IV) atoms in a complex fluoride through the incorporation of 3d transition metal cations. This new route allowed us to obtain an unprecedented series of U(IV) ferrimagnetic materials of the new composition Cs2MU3F16 (M = Mn2+, Co2+, and Ni2+), which were comprehensively characterized with respect to their structural and magnetic properties. Magnetic susceptibility measurements revealed ferromagnetic-like phase transitions at temperatures of ∼14.0, 3.5, and 4.8 K for M = Mn2+, Co2+, and Ni2+, respectively. The transition is not observed when the magnetic M cations are replaced by a diamagnetic cation, Zn2+. Neutron diffraction measurements revealed the magnetic moments of 0.91(6)–1.97(3) μB on the U atoms, which are only partially compensated by antiparallel moments of 1.53(14)–3.26(5) μB on the 3d cations. This arrangement promotes suppression of the transition to a diamagnetic ground state characteristic of U(IV), and in doing so, induces magnetic ordering on uranium via 3d–5f exchange coupling.Keywords
Funding Information
- Basic Energy Sciences (DE-SC0018739)
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