Photoelectron Spectra of Gd2O2− and Non-Monotonic Photon-Energy Dependent Variations in Populations of Close-Lying Neutral States

Abstract

<p>Photoelectron spectra of Gd<sub>2</sub>O<sub>2</sub><sup>−</sup> obtained with photon energies from 2.033 eV to 3.495 eV exhibit numerous close-lying neutral states with photon-energy-dependent relative intensities. Transitions to states falling within the electron binding energy window of 0.9 and 1.6 eV are attributed to one- or two-electron transitions to the ground and low-lying excited neutral states. An additional, manifold of electronic states observed in the 2.1 to 2.8 eV window cannot be assigned to any simple one-electron transitions. Because of the relatively simple electronic structure from the half-filled 4<i>f<sup>7</sup> </i>subshell occupancy in Gd<sub>2</sub>O<sub>2</sub><sup>–</sup>, the numerous transitions observed in the spectra are fairly well-resolved, allowing a detailed view of the changes in relative intensities of individual transitions with photon energy. With supporting calculations on the numerous close-lying electronic states, we suggest a description of strong photoelectron-valence electron interactions that result in the photon-energy dependent shake-up transitions and switching between ferro- and antiferromagnetic coupling. </p>

A Density Functional Theory Investigation of the Reaction of Water with Ce2O-

“…The approach used here follows from our previous experience working with such systems as well as studies reported by other groups. 46,47,51,[69][70][71][72][73][74][75] 3 Results…”

∆SCF Dyson Orbitals and Pole Strengths from Natural Ionization Orbitals

“…Indeed, over the last few years we have employed NIO analysis in studies of complicated photoelectron spectra of transition metal and lanthanide containing clusters. 20,21,[23][24][25]83,84 In We note that the remainder of this discussion focuses on electron detachment; analogous expressions can be derived for electron attachment processes.…”