Scott Richmond

The Valence-Fluctuating Ground State of Plutonium

Determination of plutonium’s fluctuating electronic and magnetic ground state resolves long-standing “missing” magnetism puzzle. A central issue in material science is to obtain understanding of the electronic correlations that control complex materials. Such electronic correlations frequently arise because of the competition of localized and itinerant electronic degrees of freedom. Although the respective limits of well-localized or entirely itinerant ground states are well understood, the intermediate regime that controls the functional properties of complex materials continues to challenge theoretical understanding. We have used neutron spectroscopy to investigate plutonium, which is a prototypical material at the brink between bonding and nonbonding configurations. Our study reveals that the ground state of plutonium is governed by valence fluctuations, that is, a quantum mechanical superposition of localized and itinerant electronic configurations as recently predicted by dynamical mean field theory. Our results not only resolve the long-standing controversy between experiment and theory on plutonium’s magnetism but also suggest an improved understanding of the effects of such electronic dichotomy in complex materials.

The solubility of hydrogen and deuterium in alloyed, unalloyed and impure plutonium metal

Pressure-Composition-Temperature (PCT) data are presented for the plutonium-hydrogen (Pu-H) and plutonium-deuterium (Pu-D) systems in the solubility region up to terminal solubility (precipitation of PuH2). The heats of solution for PuHS and PuDS are determined from PCT data in the ranges 350-625°C for gallium alloyed Pu and 400-575°C for unalloyed Pu. The solubility of high purity plutonium alloyed with 2 at.% gallium is compared to high purity unalloyed plutonium. Significant differences are found in hydrogen solubility for unalloyed Pu versus gallium alloyed Pu. Differences in hydrogen solubility due to an apparent phase change are observable in the alloyed and unalloyed solubilities. The effect of iron impurities on Pu-Ga alloyed Pu is shown via hydrogen solubility data as preventing complete homogenization.

High-Concentration Tritium Sensor

A bi-layer device was fabricated and tested for the direct collection of electrons emitted by tritium beta decay. The sensor functions at high pressures and concentrations where previously no simple and cost effective direct measurement technique existed for tritium. A polished KOVARTM (Fe-Ni-Co alloy) rod was coated with a 1-μm thick insulating layer of alumina using electron-beam evaporation, physical vapor deposition (PVD) of alumina with oxygen dosing. The alumina deposition process was optimized to minimize pinholes and obtain a stable coating with high resistivity. The detector exhibited a nanoampere electrical response over a few decades of tritium concentration, up to pure tritium at 200 kPa. The sensor has been in service for several months now without showing signs of degradation and no discernible physical damage or change in efficiency has been observed.