Investigation of Resonant Photoemission in Gd with X-Ray Linear Dichroism

The constructive summing of direct and indirect channels above the absorption threshold of a core level can cause a massive increase in the emission cross section, leading to a phenomenon called resonant photoemission. Using novel magnetic linear dichroism in angular distribution photoelectron spectroscopy experiments and theoretical simulations, we have probed the nature of the resonant photoemission process in Gd metal. It now appears that temporal matching as well as energy matching is a requirement for true resonant photoemission

Nature of Resonant Photoemission in Gd

The phenomenon of resonant photoemission happens when, in addition to a direct photoemission channel, a second indirect channel opens up as the absorption threshold of a core level is crossed. A massive increase in emission cross section can occur, but the nature of the process remains clouded. Using novel magnetic linear dichroism in photoelectron spectroscopy experiments and theoretical calculations, we can now clearly demonstrate that temporal matching of the processes as well as energy matching is a requirement for true resonant photoemission.

Resonant Photoemission in f-Electron Systems: Pu and Gd

Resonant photoemission in the Pu 5f and Pu 6p states is compared to that in the Gd 4f and Gd 5p states. Spectral simulations, based upon an atomic model with angular momentum coupling, are compared to the Gd and Pu results. Additional spectroscopic measurements of Pu, including core level photoemission and x-ray absorption, are also presented

Experimental Benchmarking of Pu Electronic Structure

The standard method to determine the band structure of a condensed phase material is to (1) obtain a single crystal with a well defined surface and (2) map the bands with angle resolved photoelectron spectroscopy (occupied or valence bands) and inverse photoelectron spectroscopy (unoccupied or conduction bands). Unfortunately, in the case of Pu, the single crystals of Pu are either nonexistent, very small and/or having poorly defined surfaces. Furthermore, effects such as electron correlation and a large spin-orbit splitting in the 5f states have further complicated the situation. Thus, we have embarked upon the utilization of unorthodox electron spectroscopies, to circumvent the problems caused by the absence of large single crystals of Pu with well-defined surfaces. Our approach includes the techniques of resonant photoelectron spectroscopy [1], x-ray absorption spectroscopy [1,2,3,4], electron energy loss spectroscopy [2,3,4], Fano Effect measurements [5], and Bremstrahlung Isochromat Spectroscopy [6], including the utilization of micro-focused beams to probe single-crystallite regions of polycrystalline Pu samples. [2,3,6

L1 Report for the Enhanced Surveillance Campaign Experimental Benchmarking of Pu Electronic Structure

The objective of this work is to develop and/or apply advanced diagnostics to the understanding of aging of Pu. Advanced characterization techniques such as photoelectron and x-ray absorption spectroscopy will provide fundamental data on the electronic structure of Pu phases. These data are crucial for the validation of the electronic structure methods. The fundamental goal of this project is to narrow the parameter space for the theoretical modeling of Pu aging. The short-term goal is to perform experiments to validate electronic structure calculations of Pu. The long-term goal is to determine the effects of aging upon the electronic structure of Pu. Many of the input parameters for aging models are not directly measurable. These parameters will need to be calculated or estimated. Thus a First Principles-Approach Theory is needed, but it is unclear what terms are important in the Hamiltonian (H{Psi} = E{Psi}). Therefore, experimental data concerning the 5f electronic structure are needed, to determine which terms in the Hamiltonian are important. The data obtained in this task are crucial for reducing the uncertainty of Task LL-01-developed models and predictions. The data impact the validation of electronic structure methods, the calculation of defect properties, the evaluation of helium diffusion, and the validation of void nucleation models. The importance of these activities increases if difficulties develop with the accelerating aging alloy approach

Evidence for the Photoemission Nature of Gd 4f Resonant Photoemission

The constructive interference between direct and indirect channels above the absorption threshold of a core level leads to a massive increase in the emission cross section leading to a phenomenon called `resonant photoemission\u27. Using novel magnetic linear dichroism in angular distribution photoelectron spectroscopy experiment we have tried to understand the nature of the resonant photoemission process in Gd metal. The presence of dichroism in Gd 4f photoemission intensity at a photon energy corresponding to resonant photoemission clearly demonstrates the photoemission-like nature of the resonant photoemission process