IMPORTANCE OF FULL COULOMB INTERACTIONS FOR UNDERSTANDING THE ELECTRONIC STRUCTURE OF DELTA-Pu

Journal Article · Thu Apr 01 04:00:00 EDT 2010 · Physical Review B, vol. 82, no. 8, August 15, 2010, pp. 085117-1-5

OSTI ID:1015404

Gorelov, E; Kolorenc, J; Wehling, T; Hafermann, H; Lichtenstein, A I; Shick, A B; Rubtsov, A N; Katsnelson, M I; Landa, A; McMahan, A K

The solid-state properties of most elements are now well understood on the basis of quantum physics - with few exceptions, notably the element number 94, plutonium. Plutonium has six crystalline phases at ambient pressure, some of which are separated by unusual phase transitions with large discontinuities in volume, exhibit negative thermal expansion coefficients, or form exotic low-symmetry structures. The main challenge to explain these anomalous properties is that the characteristic ingredient of actinides, the 5f electronic states, are in the cross-over regime between the localized and delocalized (itinerant) behaviour in Pu. The early part of the actinide series with the 5f states being itinerant, i.e. part of the metallic bond, culminates with Pu; starting with Am (Z = 95), the 5f states are localized, nonbonding, and resemble the 4f states in lanthanides. Both itinerant and localized regimes are well covered by existing theories, but they cannot be simply interpolated due to the importance of dynamical electron-electron correlations. Here we present accurate quantum Monte Carlo calculations achieving previously inaccessible resolution. Obtained results demonstrate that interplay of the full Coulomb interaction vertex with spin-orbital coupling is crucial for understanding the experimentally observed spectral properties of plutonium near the Fermi level.

• Research Organization: Lawrence Livermore National Laboratory (LLNL), Livermore, CA
• Sponsoring Organization: USDOE
• DOE Contract Number: W-7405-ENG-48
• OSTI ID: 1015404
• Report Number(s): LLNL-JRNL-427183
• Journal Information: Physical Review B, vol. 82, no. 8, August 15, 2010, pp. 085117-1-5, Journal Name: Physical Review B, vol. 82, no. 8, August 15, 2010, pp. 085117-1-5 Journal Issue: 8 Vol. 82
• Country of Publication: United States
• Language: English

Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
ACTINIDES
ELECTRONIC STRUCTURE
FERMI LEVEL
PHYSICS
PLUTONIUM
RARE EARTHS
RESOLUTION
THERMAL EXPANSION