Nonmagnetic ground state of PuO2

摘要: The correlated band theory implemented as a combination of the local density approximation with exact diagonalization Anderson impurity model is applied to PuO${}_{2}$. We obtain an insulating electronic structure consistent experimental photoemission spectra. calculations yield gap 1.8 eV and nonmagnetic singlet ground state that characterized by noninteger filling plutonium $f$ shell (${n}_{f}\ensuremath{\approx}4.5$). Due sizable hybridization $p$ states oxygen, more complex than four-electron Russell-Saunders ${}^{5}{I}_{4}$ manifold split crystal field. inclusion improves agreement between experiment for magnetic susceptibility.