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Molecular and electronic structure of terminal and alkali metal-capped uranium(V) nitride complexes

Author

Listed:
  • David M. King

    (School of Chemistry, University of Nottingham)

  • Peter A. Cleaves

    (School of Chemistry, University of Manchester)

  • Ashley J. Wooles

    (School of Chemistry, University of Manchester)

  • Benedict M. Gardner

    (School of Chemistry, University of Manchester)

  • Nicholas F. Chilton

    (School of Chemistry, University of Manchester)

  • Floriana Tuna

    (School of Chemistry and Photon Science Institute, University of Manchester)

  • William Lewis

    (School of Chemistry, University of Nottingham)

  • Eric J. L. McInnes

    (School of Chemistry and Photon Science Institute, University of Manchester)

  • Stephen T. Liddle

    (School of Chemistry, University of Manchester)

Abstract

Determining the electronic structure of actinide complexes is intrinsically challenging because inter-electronic repulsion, crystal field, and spin–orbit coupling effects can be of similar magnitude. Moreover, such efforts have been hampered by the lack of structurally analogous families of complexes to study. Here we report an improved method to U≡N triple bonds, and assemble a family of uranium(V) nitrides. Along with an isoelectronic oxo, we quantify the electronic structure of this 5f1 family by magnetometry, optical and electron paramagnetic resonance (EPR) spectroscopies and modelling. Thus, we define the relative importance of the spin–orbit and crystal field interactions, and explain the experimentally observed different ground states. We find optical absorption linewidths give a potential tool to identify spin–orbit coupled states, and show measurement of UV···UV super-exchange coupling in dimers by EPR. We show that observed slow magnetic relaxation occurs via two-phonon processes, with no obvious correlation to the crystal field.

Suggested Citation

  • David M. King & Peter A. Cleaves & Ashley J. Wooles & Benedict M. Gardner & Nicholas F. Chilton & Floriana Tuna & William Lewis & Eric J. L. McInnes & Stephen T. Liddle, 2016. "Molecular and electronic structure of terminal and alkali metal-capped uranium(V) nitride complexes," Nature Communications, Nature, vol. 7(1), pages 1-14, December.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms13773
    DOI: 10.1038/ncomms13773
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    Cited by:

    1. Arun Ramanathan & Jensen Kaplan & Dumitru-Claudiu Sergentu & Jacob A. Branson & Mykhaylo Ozerov & Alexander I. Kolesnikov & Stefan G. Minasian & Jochen Autschbach & John W. Freeland & Zhigang Jiang & , 2023. "Chemical design of electronic and magnetic energy scales of tetravalent praseodymium materials," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Xiaoqing Xin & Iskander Douair & Thayalan Rajeshkumar & Yue Zhao & Shuao Wang & Laurent Maron & Congqing Zhu, 2022. "Photochemical Synthesis of Transition Metal-Stabilized Uranium(VI) Nitride Complexes," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    3. Qingyu Meng & Laura Abella & Yang-Rong Yao & Dumitru-Claudiu Sergentu & Wei Yang & Xinye Liu & Jiaxin Zhuang & Luis Echegoyen & Jochen Autschbach & Ning Chen, 2022. "A charged diatomic triple-bonded U≡N species trapped in C82 fullerene cages," Nature Communications, Nature, vol. 13(1), pages 1-10, December.

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