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Covalency in Americium(III) Hexachloride.

Justin N Cross1, Jing Su1, Enrique R Batista1

  • 1Los Alamos National Laboratory , Los Alamos, New Mexico 87545, United States.

Journal of the American Chemical Society
|June 15, 2017
PubMed
Summary
This summary is machine-generated.

Understanding covalency is crucial for material properties. This study quantifies covalent bonding in Am-Cl interactions using X-ray absorption spectroscopy, confirming Seaborg's hypothesis on americium's 5f-orbital covalency.

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Area of Science:

  • Chemical Bonding
  • Spectroscopy
  • Materials Science

Background:

  • Covalency, or orbital mixing, is fundamental to chemical and physical properties.
  • Quantifying covalency is challenging, leading to scientific debate, notably regarding americium's behavior.
  • Previous hypotheses on americium 5f-orbital covalency have remained debated for decades.

Purpose of the Study:

  • To quantify the extent of covalent bonding in the Am-Cl interaction within AmCl63-.
  • To investigate the role of 5f and 6d orbital mixing in americium compounds.
  • To compare covalency in AmCl63- with isoelectronic systems like EuCl63-.

Main Methods:

  • Ligand K-edge X-ray absorption spectroscopy (XAS) was employed.
  • Electronic structure calculations were performed to analyze orbital interactions.
  • Spectroscopic and computational data were used to quantify covalent bonding.

Main Results:

  • Both 5f and 6d orbitals of Am mixed with Cl 3p orbitals.
  • Orbital mixing from Am 6d-orbitals was more substantial than from 5f-orbitals.
  • Results confirmed Seaborg's hypothesis regarding Am 5f-orbital covalency being greater than Eu 4f-orbital mixing.

Conclusions:

  • The study successfully quantified covalency in the challenging Am-Cl system.
  • Ligand K-edge XAS and electronic structure calculations provide robust methods for studying orbital mixing.
  • Findings validate long-standing hypotheses about the nature of bonding in actinide compounds.