Electronic structure of americium sesquioxide probed by resonant inelastic x-ray scattering

TL;DR

This study investigates the electronic structure of americium sesquioxide using resonant inelastic x-ray scattering and theoretical models, revealing details about its ground state, electronic states, and hybridization effects.

Contribution

It provides a combined experimental and theoretical analysis of Am$_2$O$_3$, confirming its singlet ground state and characterizing 5f-oxygen hybridization through RIXS and model calculations.

Findings

Am$_2$O$_3$ has a singlet $$ ground state.

Weak Am 5f-O 2p hybridization is indicated by a charge-transfer satellite.

The 5f occupancy is estimated at approximately 6.05 electrons.

Abstract

The Am $5d$-$5f$ resonant inelastic x-ray scattering (RIXS) data of americium sesquioxide were measured at incident photon energies throughout the Am $O_{4,5}$ edges. The experiment was supported by calculations using several model approaches. While the experimental Am $O_{4,5}$ x-ray absorption spectrum of Am$_2$O$_3$ is compared with the spectra calculated in the framework of atomic multiplet and crystal-field multiplet theories and Anderson impurity model (AIM) for the Am(III) system, the recorded Am $5d$-$5f$ RIXS data are essentially reproduced by the crystal-field multiplet calculations. A combination of the experimental scattering geometry and theoretical analysis of the character of the electronic states probed during the RIXS process confirms that the ground state of Am$_2$O$_3$ is singlet $\Gamma_1$. An appearance of the low-intense charge-transfer satellite in the Am $5d$-$5f$ RIXS spectra at an energy loss of $\sim$5.5 eV, suggests weak Am $5f$-O $2p$ hybridization which is in agreement with AIM estimations of the $5f$ occupancy from spectroscopic data in Am$_2$O$_3$ as being 6.05 electrons.