Theory for Temperature-Dependent Phonons

P. Söderlind, L. Yang, and A. Landa

Collaborators:
P. Souvatzis and O. Eriksson (Uppsala University, Sweden).

A microscopic explanation for temperature stabilization of the body-centered cubic (bcc) phase in the actinide metals is proposed. We show that for a prototype actinide, uranium, phonon-phonon interaction promotes bcc γ-U when heated even though at low temperatures it is mechanically a strongly unstable phase. Utilizing the recently developed self-consistent ab initio lattice dynamics (SCAILD) scheme in conjunction with highly accurate and fully relativistic density functional theory we obtain phonon dispersion and density of states that compare well with data acquired from inelastic neutron-scattering experiments. The investigation thus establishes that high-temperature lattice dynamics can be modeled from ab initio theory even for complex materials with substantial electron correlation including the actinides.

Selected Publications

1. P. Söderlind, B. Grabowski, L. Yang, and A. Landa, T. Bjorkman, P. Souvatzis, and O. Eriksson, "High-temperature phonon stabilization of γ-uranium from relativistic first-principles theory" Phys. Rev. B 85, 060301(R) (2012).
2. P. Souvatzis, O. Eriksson, M. I. Katsnelson, and S. P. Rudin, "Entropy Driven Stabilization of Energetically Unstable Crystal Structures Explained from First Principles Theory" Phys. Rev. Lett. 100, 095901 (2008).
3. J. M. Wills, M. Alouani, P. Andersson, A. Delin, O. Eriksson, and A. Grechnev, Full-Potential Electronic Structure Method, Energy and Force Calculations with Density Functional and Dynamical Mean Field Theory (Springer Series in Solid-State Science) 167, (2010).
4. M. E. Manley, B. Fultz, R. J. McQueeney, C. M. Brown, W. L. Hults, J. L. Smith, D. J. Thoma, R. Osborn, and J. L. Robertson, "Large Harmonic Softening of the Phonon Density of States of Uranium" Phys. Rev. Lett. 86, 3076 (2001).

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