Anisotropic Resonant Scattering from uranium systems at the U M4 edge

TL;DR

This study investigates anisotropic resonant scattering in uranium compounds at the U M4 edge, revealing how 5f electron distributions influence scattering signals and bonding, supported by experimental data and theoretical modeling.

Contribution

It demonstrates that anisotropic resonant scattering signals originate from aspherical 5f electron charge distributions, confirmed by experiments and FDMNES simulations.

Findings

Resonant signals are independent of temperature.

Good agreement between experiment and theory on azimuthal dependencies.

Reveals the role of 5f electrons in actinide bonding.

Abstract

We have conducted a series of scattering experiments at the uranium M4 absorption edge on low-symmetry uranium compounds (U2N3 and U3O8) produced as epitaxial films. At weak and forbidden reflections, we find a resonant signal, independent of temperature, with an energy dependence resembling the imaginary part of the scattering factor. Theory, using the FDMNES code, shows that these results can be reliably reproduced assuming that they originate from aspherical 5f electron charge distributions around the U nucleus. Such effects arise from the intrinsic anisotropy of the 5f shell and from the mixing of the 5f electrons of uranium with the outer 2p electrons of the anions. The good agreement between theory and experiment includes azimuthal scattering dependencies, as well as polarization states of the scattered photons. The methodology reported here opens the way for a deeper understanding of the role of the 5f electrons in the bonding in actinide compounds.