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NUMBER 1 of 2 Actinide Research Quarterly NUMBER 1 OF 2 Actinide Research Quarterly Foreword “Plutonium Futures—The Science 2018” was the tenth in a series of inter- national conferences focused on the scientific research and technological uses of plutonium and other actinides. The global actinide research and technology community takes great pride in this series as its origins lie in the United Nations “Peaceful Uses of Atomic Energy” conference series initiated in 1958. Co-organized by Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL), and the American Nuclear Society, and supported by the U.S. Department of Energy and the National Nuclear Security Administration (NNSA), Plutonium Futures—The Science 2018 was held at the Wyndham San Diego Bayside, September 9–14, 2018. A total of 218 attendees from around the world participated in talks and discussions—many of these topics presented at Plutonium Futures resonate with those found in the early days of international cooperation. This conference facilitates dialogue among scientists and engineers of diverse scientific disciplines on the science of plutonium and its technological, environmental, health, and socio- economic consequences. This issue of the LANL Actinide Research Quarterly is the first of two issues celebrating the breadth of topics presented at last year’s conference, including: environmental chemistry, metallurgy and materials science, surface science and corrosion, coordination chemistry, nuclear fuel-cycle, detection and speciation analysis, and condensed matter physics. The articles here represent many of the stimulating pieces of research conducted by the global actinide research and technology community. In the tradition of the Plutonium Futures conferences, we recognize here the best student posters (p25). We would also like to recognize the various committees which assisted in organizing and conducting Plutonium Futures—The Science 2018, listed on the facing page. — Franz Freibert, Co-Chair Plutonium Futures 2018 G. T. Seaborg Institute for Transactinium Science Los Alamos National Laboratory Plutonium Futures 2018 Committees: Program Committee International Advisory Committee Los Alamos National Laboratory Corwin Booth Lawrence Berkeley National Laboratory, LBNL Herve’ Bernard CEA Franz Freibert Co-chair Paul Roussel Atomic Weapons Establishment, AWE Claude Guet University of Singapore Albert Migliori Co-chair Sue Ennaceur AWE Gerry Lander Institut Laue-Langevin Susan Ramsay Conference Coordinator Robert J. Hanrahan Jr. NNSA Roberto Caciuffo European Commission, JRC David Clark Benoit Oudot CEA Valduc Thomas Fanghänel European Commission, JRC Andrew Gaunt David Hobart Florida State University David Geeson AWE, Aldermaston George Goff Klaus Luetzenkirchen DG Joint Research Centre JRC Tim Tinsley National Nuclear Laboratory Sarah Hernandez Richard Wilson Argonne National Laboratory Gerrit van der Laan Diamond Light Source Ltd. John Joyce David Shuh LBNL Kerri Blobaum LLNL Stosh Kozimor Krzysztof Gofryk Idaho National Laboratory David Clark LANL Boris Maiorov Philippe Moisy CEA Marcoule Scott McCall LLNL Stuart Maloy Rudy Konings JRC Rodney C. Ewing Stanford University Jeremy Mitchell Mavrik Zavarin LLBL Siegfried Hecker Stanford University David Moore Stepan Kalmykov Lomonosov Moscow State University Jun Li Tsinghua University Dominic Peterson Horst Geckeis Karlsruhe Institute of Technology Vladimir Dremov RFNC-VNIITF Don Reed John Gibson LBNL Boris Nadykto VNIIEF Blas Uberuaga V. Petrovtsev RFNC-VNIITF Marianne Wilkerson Lidia F. Timofeeva VNIINM Ping Yang Yoshinori Haga Japan Atomic Energy Agency Ladislav Havela Charles University, Prague Plutonium Futures The Science 2018 Second Quarter 2019 1 Actinide Research Quarterly Contents Foreword ii Franz Freibert Plutonium Futures 2018 Photo Reel 22 Student Poster Awards 25 2018 Postdoctoral Publication Prize in Actinide Science 44 PLENARY SESSION VI SURFACE SCIENCE AND CORROSION II Fingerprints of Electron Correlations Plutonium Metal Corrosion by Water Vapor 4 in Plutonium Phases 15 An X-Ray Photoelectron Study Electronic Properties of β-Pu Analogs Lionel Jolly, CEA, Centre de Valduc Ladislav Havela, Charles University, Prague PLENARY SESSION VIII CONDENSED MATTER PHYSICS II Probing Actinide Covalency Modeling the High Temperature Phase of 10 Plutonium Electronic Structure Studies 19 Plutonium Using High Energy Resolution X-Ray Boris Dorado, CEA, Centre DAM Ile de France Spectroscopy Tonya Vitova, Karlsruhe Institute of Technology, Germany Paul S. Bagus, University of North Texas POSTER SESSION I Actinide Isotopes for Space Applications 26 Development of Am-241-Based Materials for Radioisotope Power Systems Jean-Francois Vigier, European Commission Joint Research Centre, Karlsruhe, Germany 2 G. T. Seaborg Institute for Transactinium Science Los Alamos National Laboratory About the cover: The (pressure, temperature) phase diagram of elemental plutonium has been a central and long-debated aspect of actinide science. This plot shows unusual behavior, such as the multitude of allotropes or distinct crystallo- graphic phases of elemental plutonium—see p19 for a more detailed view. The forthcoming second part in the Plutonium Futures conference series (third quater 2019, right) will continue with seven more articles adapted from talks during the 2018 meeting. COORDINATION CHEMISTRY II In Stream Monitoring of Off-Gasses 31 from Plutonium Dioxide Fluorination Amanda Casella, Pacific Northwest National Laboratory METALLURGY AND MATERIALS SCIENCE II Nuclear Materials Science at the 36 Micron Scale Jon Schwantes, Pacific Northwest National Laboratory 2 Temperature (°C) 600 Pressure (kbar) 4 400 6 8 COORDINATION CHEMISTRY I 200 10 Plutonium Hybrid Materials δ δ’ 1.260 40 Supramolecular Assembly and Bonding0 ε R. Gian Surbella, Pacific Northwest National Laboratory1.080 γ 1.191 1.060 ζ 1.125 1.040 1.061 Length β 1.020 1.000 1.000 600 0 α 2 400 4 6 200 Temperature (°C) Pressure (kbar) 8 Second Quarter 2019 3 10 0 Actinide Research Quarterly Fingerprints of Electron Correlations in Plutonium Phases: Electronic Properties of β-Pu Analogs Ladislav Havela,1 Silvie Maskova,1 Pavel Javorsky,1 Jindrich Kolorenc,2 Eric Colineau,3 Jean-Christophe Griveau,3 Rachel Eloirdi,3 Thomas Gouder3 The properties of plutonium are largely determined by electrons that occupy the open 5f electronic shell. These electrons are poised between localization and delocal- ization, and are difficult to describe using conventional theoretical frameworks which do not accurately account for pair correlations between electrons. Understanding such correlations and their impact on material properties is key to predicting the Ladislav Havela behavior of plutonium systems. Prof. Ladislav Havela from Charles Metal properties in general depend on electrons in open shells—i.e., shells that University, Prague, presented his are only partially filled. In most cases, they are outer s and p shells which strongly talk titled "Fingerprints of Electron overlap between neighboring atoms in a crystal lattice, mediating the bonding Correlations in Various Phases of between positive ions. Such electrons form a weakly-interacting fermionic liquid Plutonium: Electronic Properties of and occupy states with gradually increasing energy up to the so-called Fermi level, Pu19Os Simulating β-Pu" at Pu Futures EF. The basic properties of metals depend on how many states per atom are in close 2018 as a plenary speaker in Plenary vicinity of the Fermi energy, because only those electrons can be thermally excited Session VI. or redistributed by common external fields. Hence thermal, transport, and magnetic properties are critically dependent on this parameter, called density of states at the Fermi level, N(EF). In some metals there are open shells of electrons that reside deep in the ionic core, with negligible overlap between neighboring ions. This is the case for the lanthanide 4f electrons. They do not contribute to bonding, but they can yield ionic magnetic moments, as spin and orbital moments within each 4f atomic shell are non-zero. Such localized electrons naturally do not contribute to N(EF). The above two types of open shells are well understood by existing theories. In the case of the outer shells (i.e., delocalized electrons), conventional density functional theory (DFT) describes electron energetics as dependent on pair electron- electron (e-e) interactions in an implicit way, and the electronic states form bands of possible energies. For the inner shells (localized electrons), e-e correlations remain within the ion on which the particular electrons are localized. Electronic states remain discrete in the energy scale. 1Charles University, Faculty of Mathematics and Physics, Ke Karlovu 3, CZ-12116 Prague 2, Czech Republic; 2Institute of Physics, Czech Academy of Sciences, Na Slovance 2, CZ-182 21 Prague 8, Czech Republic; 3European Commission, Joint Research Centre (JRC), Directorate for Nuclear Safety and Security, D-76125 Karlsruhe, Germany. 4 G. T. Seaborg Institute for Transactinium Science Los Alamos National Laboratory 500 400 ) 2 300 (mJ/mol Pu K (mJ/mol Pu T / 200 p C η-Pu19Os β-Pu (ζ-Pu19Os) δ-Pu (Pu-6.1% Ce) 100 α-Pu * Black outline indicates γ sample of different mass 0 0 100 200 300 400 500 T2 (K2) 2 Figure 1. Temperature dependence of low-temperature heat capacity in the Cp/T vs. T representation for ζ- and η-Pu19Os phases. The best low-temperature fits are shown, which give the Sommerfeld coefficientγ) ( values as the vertical axis intercepts. The very high γ values
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