New insights into the electronic structure ofα-U andδ-Pu.

This work presents the results of a theoretical study of the electronic structure of two actinide metals,α-U andδ-Pu. We compare ourab-initioresults obtained with the recently developed self-consistent Vertex corrected GW approach with previously published experimental measurements such as photo-electron spectroscopy, for the occupied density of states, and bremsstralung isochromat spectroscopy (BIS) and inverse photo-electron spectroscopy (IPES), for the unoccupied density of states. Ourab-initioapproach includes all important relativistic effects (it is based on Dirac's equation) and it represents the first application of the Vertex corrected GW approach in the physics of actinides. Overall, our theoretical results are in good agreement with the experimental data, which supports the level of approximations which our theoretical method is based upon. By comparing our vertex corrected GW results with our results obtained with less sophisticated approaches (local density approximation and self-consistent GW) we differentiate the strength of correlation effects in Uranium and Plutonium. Also, our theoretical results allow us to elucidate the subtle differences between the previously published experimental BIS and IPES data on the unoccupied density of states inα-U.

An instrument for the investigation of actinides with spin resolved photoelectron spectroscopy and bremsstrahlung isochromat spectroscopy.

A new system for spin resolved photoelectron spectroscopy and bremsstrahlung isochromat spectroscopy has been built and commissioned at Lawrence Livermore National Laboratory for the investigation of the electronic structure of the actinides. Actinide materials are very toxic and radioactive and therefore cannot be brought to most general user facilities for spectroscopic studies. The technical details of the new system and preliminary data obtained therein will be presented and discussed.

Emergent magnetic moments produced by self-damage in plutonium.

Plutonium possesses the most complicated phase diagram in the periodic table, driven by the complexities of overlapping 5f electron orbitals. Despite the importance of the 5f electrons in defining the structure and physical properties, there is no experimental evidence that these electrons localize to form magnetic moments in pure Pu. Instead, a large temperature-independent Pauli susceptibility indicates that they form narrow conduction bands. Radiation damage from the alpha-particle decay of Pu creates numerous defects in the crystal structure, which produce a significant temperature-dependent magnetic susceptibility, chi(T), in both alpha-Pu and delta-Pu (stabilized by 4.3 atomic percent Ga). This effect can be removed by thermal annealing above room temperature. By contrast, below 35 K the radiation damage is frozen in place, permitting the evolution in chi(T) with increasing damage to be studied systematically. This result leads to a two-component model consisting of a Curie-Weiss term and a short-ranged interaction term consistent with disorder-induced local moment models. Thus, it is shown that self-damage creates localized magnetic moments in previously nonmagnetic plutonium.

Probing the population of the spin-orbit split levels in the actinide 5f states.

Spin-orbit interaction in the 5f states is believed to strongly influence exotic behaviors observed in actinide metals and compounds. Understanding these interactions and how they relate to the actinide series is of considerable importance. To address this issue, the branching ratio of the white-line peaks of the N4,5 edge for the light actinide metals, alpha-Th, alpha-U, and alpha-Pu were recorded using electron energy-loss spectroscopy (EELS) in a transmission electron microscope (TEM) and synchrotron-radiation-based X-ray absorption spectroscopy (XAS). Using the spin-orbit sum rule and the branching ratios from both experimental spectra and many-electron atomic spectral calculations, accurate values of the spin-orbit interaction, and thus the relative occupation of the j = 5/2 and 7/2 levels, are determined for the actinide 5f states. Results show that the spin-orbit sum rule works very well with both EELS and XAS spectra, needing little or no correction. This is important, since the high spatial resolution of a TEM can be used to overcome the problems of single-crystal growth often encountered with actinide metals, allowing acquisition of EELS spectra, and subsequent spin-orbit analysis, from nm-sized regions. The relative occupation numbers obtained by our method have been compared with recent theoretical results and they show a good agreement in their trend.

Applicability of the spin-orbit sum rule for the actinide 5f states.

The branching ratio of core-valence transitions in electron energy-loss spectroscopy and x-ray absorption spectroscopy is linearly related to the expectation value of the spin-orbit operator of the valence states. Here, we analyze the branching ratio of the N(4,5) edges in the actinides and find that the spin-orbit sum rule gives an accurate result without the need to include the core-valence interactions. The branching ratio is not only useful to study the variations in the 5f spin-orbit interaction, it also allows us to constrain the 5f count for given angular-momentum coupling conditions.

Failure of Russell-Saunders coupling in the 5f states of plutonium.

Using high energy-electron energy loss spectroscopy, transmission electron microscopy, and synchrotron-radiation-based x-ray absorption spectroscopy, we provide the first experimental evidence that Russell-Saunders (LS) coupling fails for the 5f states of Pu. These results support the assumption that only the use of jj or intermediate coupling is appropriate for the 5f states of Pu. High energy-electron energy loss spectroscopy experiments were performed by use of a transmission electron microscope and are coupled with image and diffraction data; therefore, the measurements are completely phase specific.

Pitfalls in laparoscopic cholecystectomy: unrecognized carcinoma of another site.

Laparoscopic cholecystectomy has been rapidly adopted as a standard surgical treatment in symptomatic cholelithiasis. Its advantages over laparotomy are well described. However, its risks and long-term results have not been fully evaluated. We experienced three patients in whom intra-abdominal carcinomas failed to be recognized during laparoscopic surgery. The clinical manifestations, laboratory findings, and radiologic findings were carefully reviewed in each case. Limited exploration of the abdominal cavity is one of the technical pitfalls in laparoscopic cholecystectomy; so surgeons can miss the carcinoma of extrabiliary system. To prevent such problems, a careful taking of the history and physical examination should be repeated by the responsible surgeon, who must be aware of the differential diagnosis of cholelithiasis, especially in elderly patients. If needed, additional radiologic studies are recommended.