Seminarium Oddziału Badań Magnetyków
Microsoft Teams
Lattice dynamics, thermal expansion, magnetism, phase stability, and electron correlations in actinides
Prof. Dominik Legut
VSB Technical University of Ostrava in Czech Republic
Seminarium odbędzie się zdalnie w aplikacji Microsoft Teams. W celu wzięcia udziału w wydarzeniu należy dołączyć do zespołu Seminarium OBM. Można do niego dołączyć na stałe przy użyciu kodu dostępu ol7omod (dotyczy to osób posiadających konto w domenie intibs.pl, pozostałe osoby proszę o kontakt z prof. dr. hab. Adamem Pikulem, prof. INTiBS PAN ())
The seminar will be held remotely via the Microsoft Teams application. In order to participate in the event, you must join the Seminarium OBM team. You can join it permanently using the access code ol7omod (this applies to people with an account in the intibs.pl domain, other people please contact Prof. Adam Pikul , Prof. INTiBS PAN ())
Abstract:
There are number of 1:1 properties that could be directly compared between quantum mechanical calculations (using density functional theory) based on lattice dynamics and the experimental measurements. One of the examples is lattice heat capacity, thermal expansion, and thermal conductivity. The latter two are the key parameters of the potential nuclear fuels, the former one can shed much light on the magnetic systems of actinide hydrides. Actinides and especially their carbides as prospective nuclear fuel materials for the generation IV reactors were investigated using the density functional theory. We demonstrate that their electronic, magnetic, elastic, and thermal properties can be at present well described if the spin-orbit interaction and partial delocalization 5f electrons is properly included in the computational approaches. One can well reproduce not only basic electronic structure but also elastic constants, phonon dispersions, and their density of states, provided by XPS, UPS, BIS, and inelastic neutron scattering data [1-4]. Often, the localization of the 5f electrons could be captured using a moderate value of the on-site Coulomb interaction parameter. The case s tudies include a realistic description of the ground-state properties of elemental metals as Th, U and their monocarbides ThC and UC. In this study, published in Ref. 2 and 4, the realistic description of the electronic structure and lattice dynamics (phonons) explains why there is much higher thermal expansion in pure actinides (as Th) comparing with respective actinide monocarbides. The modeling also gives an insight up to which temperature the heat transport depends on lattice vibrations and where the electron transport starts to dominate. We analyzed the force constants of defected systems in order to reveal the effect of the oxygen impurity and vacancy at carbon site on the thermal expansion, summarized in Ref. 4. Additionally investigated thermodynamic properties, such as for instance heat capacity, were compared to the experimental data in the large temperature scan showing very excellent agreement up to 2000K and explained some additional features of phonon DOS not presented before. In the second part, we present the calculations of the stability, mechanical, and magnetic properties of the uranium hydrides including 3 different cubic compounds, α- and β-UH3 and UH2, all undergoing ferromagnetic ordering. Our first-principles calculations revealed a complex (non-collinear) magnetic order in β-UH3. Unlike the other uranium hydrides, α-UH3 and UH2, β-UH3 with two different U sites exhibits a site-dependent size and direction of U magnetic moments. While the U moments at the 2a sites are locked in the body diagonal direction, the moments at the 6c sites are inclined by approx. 15 degrees. The difference stems from 5f orbital moments. Comparison of results for all 3 species reveals that the U-U spacing is not the primary parameter to control the magnetism in uranium hydrides. Further insight is provided by evaluating individual exchange interactions between different neighbours, yielding the transition temperatures in a reasonable agreement with the experiment [5-7,9] as well as the lattice dynamics of all uranium-based hydrides[8]. At the end we present the outlook to understand the increase of Curie temperature in substituted β-UH3.
References:
[1] U. D. Wdowik, P. Piekarz, D. Legut, and G. Jaglo, Phys. Rev. B 94, 054303 (2016).
[2] L. Kývala and D. Legut, Phys. Rev. B 101, 075117 (2020).
[3] Y. Yun, D. Legut and P. M. Oppeneer, J. Nucl. Mat. 426, 109 (2012).
[4] U. D. Wdowik, V. Buturlim, L. Havela, and D. Legut, J. Nucl. Mat. 545, 152547 (2021).
[5] L Havela, M Paukov, M Dopita, L Horak, D Drozdenko, M Divis, I Turek, D Legut, L Kývala, T Gouder, A Seibert, and F Huber., Inorg. Chem. 57, 14727 (2018).
[6] J. Prchal, V. Buturlim, J. Valenta, M. Dopita, M. Divis, I. Turek, L. Kyvala, D. Legut, L. Havela, J. Magn. Mag. Mater. 497, 65993 (2020).
[7] L. Havela, M. Paukov, M. Dopita, L. Horak, M. Cieslar, D. Drozdenko, P. Minarik, I. Turek, M. Divis, D. Legut, L. Kývala, T. Gouder, F. Huber, A. Seibert, E. Tereshina-Chitrova, J. Elect. Spectr. and Rel. Phenom. 239, 146904 (2020).
[8] L. Kývala, L. Havela, A. P. Kądzielawa, and D. Legut, J. Nucl. Mater. 567, 153817 (2022).
[9] L. Havela, D. Legut, J. Kolorenč, Rep. Prog. Phys. 88, 056501 (2023).
