First-principles theory of multipolar order in actinide dioxides

Nicola Magnani; Michi-To Suzuki; Peter M. Oppeneer

doi:10.1016/j.crhy.2014.07.003

First-principles theory of multipolar order in actinide dioxides

Nicola Magnani ¹ ; Michi-To Suzuki ^2,³; Peter M. Oppeneer ⁴

¹ European Commission, Joint Research Centre, Institute for Transuranium Elements, Postfach 2340, 76125 Karlsruhe, Germany
² CCSE, Japan Atomic Energy Agency, 5-1-5, Kashiwanoha, Kashiwa, Chiba, 277-8587, Japan
³ RIKEN, Center for Emergent Matter Science (CEMS), Wako, Saitama, 351-0198, Japan
⁴ Department of Physics and Astronomy, Uppsala University, Box 516, 75120 Uppsala, Sweden

Comptes Rendus. Physique, Emergent phenomena in actinides, Volume 15 (2014) no. 7, pp. 580-586.

Abstract
Résumé

Magnetic phase transitions that involve multipolar degrees of freedom have been widely studied during the last couple of decades, challenging the common approximation which assumes that the physical properties of a magnetic material could be effectively described by purely dipolar degrees of freedom. Due to the complexity of the problem and to the large number of competing interactions involved, the simple (fcc) crystal structure of the actinide dioxides made them the ideal playground system for such theoretical and experimental studies. In the present paper, we summarize our recent attempts to provide an ab initio description of the ordered phases of UO₂, NpO₂, and AmO₂ by means of state-of-the-art $LDA + U$ first-principles calculations. This systematic analysis of the electronic structures is here naturally connected to the local crystalline fields of the 5f states in the actinide dioxide series. Related to these we find that the mechanisms which lead to the experimentally observed insulating ground states work in distinctly different ways for each compound.

Les transitions de phases magnétiques impliquant des degrés de liberté multipolaires ont été beaucoup étudiées au cours des vingt dernières années, remettant en question l'approximation usuelle selon laquelle les propriétés physiques d'un matériau magnétique pourraient être convenablement décrites par des degrés de liberté purement dipolaires. Les problèmes à résoudre sont compliqués à cause du grand nombre d'interactions concurrentes concernées. C'est pour cette raison que les dioxydes d'actinides, avec leur structure cristallographique simple (cubique à faces centrées), représentent une classe de composés idéale pour aborder l'étude des ordres multipolaires, tant du point de vue théorique qu'expérimental. Dans cet article, nous résumons nos tentatives récentes, qui visent à fournir une description ab initio des phases ordonnées des composés UO₂, NpO₂, et AmO₂ au moyen de calculs $LDA + U$ avancés. Cette analyse systématique de la structure électronique est ici intrinsèquement reliée au champ cristallin local qui détermine la composition des états 5f des ions actinides. Corrélativement à ceux-ci, nous mettons en évidence le fait que les mécanismes qui conduisent aux états fondamentaux isolants, observés expérimentalement, agissent de manière clairement différente pour chacun des composés de la série.

Published online: 2014-08-01

DOI: 10.1016/j.crhy.2014.07.003

Keywords: Actinide dioxides, $ \mathrm{LDA}+\mathrm{U}$ theory, Multipolar ordering
Mots-clés : Dioxydes d'actinides, Théorie $ \mathrm{LSDA}+\mathrm{U}$, Ordre multipolaire

Author's affiliations:

Nicola Magnani ¹; Michi-To Suzuki ^{2, 3}; Peter M. Oppeneer ⁴

¹ European Commission, Joint Research Centre, Institute for Transuranium Elements, Postfach 2340, 76125 Karlsruhe, Germany
² CCSE, Japan Atomic Energy Agency, 5-1-5, Kashiwanoha, Kashiwa, Chiba, 277-8587, Japan
³ RIKEN, Center for Emergent Matter Science (CEMS), Wako, Saitama, 351-0198, Japan
⁴ Department of Physics and Astronomy, Uppsala University, Box 516, 75120 Uppsala, Sweden

@article{CRPHYS_2014__15_7_580_0,
     author = {Nicola Magnani and Michi-To Suzuki and Peter M. Oppeneer},
     title = {First-principles theory of multipolar order in actinide dioxides},
     journal = {Comptes Rendus. Physique},
     pages = {580--586},
     publisher = {Elsevier},
     volume = {15},
     number = {7},
     year = {2014},
     doi = {10.1016/j.crhy.2014.07.003},
     language = {en},
}

TY  - JOUR
AU  - Nicola Magnani
AU  - Michi-To Suzuki
AU  - Peter M. Oppeneer
TI  - First-principles theory of multipolar order in actinide dioxides
JO  - Comptes Rendus. Physique
PY  - 2014
SP  - 580
EP  - 586
VL  - 15
IS  - 7
PB  - Elsevier
DO  - 10.1016/j.crhy.2014.07.003
LA  - en
ID  - CRPHYS_2014__15_7_580_0
ER  -

%0 Journal Article
%A Nicola Magnani
%A Michi-To Suzuki
%A Peter M. Oppeneer
%T First-principles theory of multipolar order in actinide dioxides
%J Comptes Rendus. Physique
%D 2014
%P 580-586
%V 15
%N 7
%I Elsevier
%R 10.1016/j.crhy.2014.07.003
%G en
%F CRPHYS_2014__15_7_580_0

Nicola Magnani; Michi-To Suzuki; Peter M. Oppeneer. First-principles theory of multipolar order in actinide dioxides. Comptes Rendus. Physique, Emergent phenomena in actinides, Volume 15 (2014) no. 7, pp. 580-586. doi : 10.1016/j.crhy.2014.07.003. https://comptes-rendus.academie-sciences.fr/physique/articles/10.1016/j.crhy.2014.07.003/

References
Cited by

[1] P. Santini; S. Carretta; G. Amoretti; R. Caciuffo; N. Magnani; G.H. Lander Multipolar interactions in f-electron systems: the paradigm of actinide dioxides, Rev. Mod. Phys., Volume 81 (2009), p. 807

[2] K.W.H. Stevens Matrix elements and operator equivalents connected with the magnetic properties of rare earth ions, Proc. Phys. Soc., Volume 65 (1952), p. 209

[3] D.J. Newman; B. Ng Crystal Field Handbook, Cambridge University Press, Cambridge, UK, 2000

[4] J.A. Mydosh; P.M. Oppeneer Colloquium: hidden order, superconductivity, and magnetism: the unsolved case of ${URu}_{2} {Si}_{2}$ , Rev. Mod. Phys., Volume 83 (2011), p. 1301

[5] S.J. Allen Spin–lattice interaction in UO₂. II. Theory of the first-order phase transition, Phys. Rev., Volume 167 (1968), p. 492

[6] J. Faber; G.H. Lander Neutron diffraction study of UO₂: antiferromagnetic state, Phys. Rev. B, Volume 14 (1976), p. 1151

[7] P. Giannozzi; P. Erdös Theoretical analysis of the 3-k magnetic structure and distortion of uranium dioxide, J. Magn. Magn. Mater., Volume 67 (1987), p. 75

[8] G. Amoretti; A. Blaise; R. Caciuffo; J.M. Fournier; M.T. Hutchings; R. Osborn; A.D. Taylor 5f-electron states in uranium dioxide investigated using high-resolution neutron spectroscopy, Phys. Rev. B, Volume 40 (1989), p. 1856

[9] R. Caciuffo; G. Amoretti; P. Santini; G.H. Lander; J. Kulda; P. de V. Du Plessis Magnetic excitations and dynamical Jahn–Teller distortions in UO₂, Phys. Rev. B, Volume 59 (1999), p. 13892

[10] S.B. Wilkins; R. Caciuffo; C. Detlefs; J. Rebizant; E. Colineau; F. Wastin; G.H. Lander Direct observation of electric-quadrupolar order in UO₂, Phys. Rev. B, Volume 73 (2006), p. 060406

[11] R. Caciuffo; P. Santini; S. Carretta; G. Amoretti; A. Hiess; N. Magnani; L.-P. Regnault; G.H. Lander Multipolar, magnetic, and vibrational lattice dynamics in the low-temperature phase of uranium dioxide, Phys. Rev. B, Volume 84 (2011), p. 104409

[12] P. Santini; G. Amoretti Magnetic-octupole order in neptunium dioxide?, Phys. Rev. Lett., Volume 85 (2000), p. 2188

[13] J.A. Paixão; C. Detlefs; M.J. Longfield; R. Caciuffo; P. Santini; N. Bernhoeft; J. Rebizant; G.H. Lander Triple-q octupolar ordering in NpO₂, Phys. Rev. Lett., Volume 89 (2002), p. 187202

[14] A. Kiss; P. Fazekas Octupolar ordering of $Γ_{8}$ ions in a magnetic field, Phys. Rev. B, Volume 68 (2003), p. 174425

[15] P. Santini; S. Carretta; N. Magnani; G. Amoretti; R. Caciuffo Hidden order and low-energy excitations in NpO₂, Phys. Rev. Lett., Volume 97 (2006), p. 207203

[16] N. Magnani; S. Carretta; R. Caciuffo; P. Santini; G. Amoretti; A. Hiess; J. Rebizant; G.H. Lander Inelastic neutron scattering study of the multipolar order parameter in NpO₂, Phys. Rev. B, Volume 78 (2008), p. 104425

[17] M.-T. Suzuki; N. Magnani; P.M. Oppeneer First-principles theory of multipolar order in neptunium dioxide, Phys. Rev. B, Volume 82 (2010), p. 241103

[18] M.-T. Suzuki; N. Magnani; P.M. Oppeneer Microscopic theory of the insulating electronic ground states of the actinide dioxides AnO₂ (An = U, Np, Pu, Am, and Cm), Phys. Rev. B., Volume 88 (2013), p. 195146

[19] A.B. Shick; J. Kolorenč; L. Havela; T. Gouder; R. Caciuffo Nonmagnetic ground state of PuO₂, Phys. Rev. B, Volume 89 (2014), p. 041109

[20] F. Zhou; V. Ozoliņš Crystal field and magnetic structure of UO₂, Phys. Rev. B, Volume 83 (2011), p. 085106

[21] T. Livneh Coupling of multi-LO phonons to crystal-field excitations in UO₂ studied by Raman spectroscopy, J. Phys. Condens. Matter, Volume 20 (2008), p. 085202

[22] R. Laskowski; G.K.H. Madsen; P. Blaha; K. Schwarz Magnetic structure and electric-field gradients of uranium dioxide: an ab initio study, Phys. Rev. B, Volume 69 (2004), p. 140408

[23] K. Ikushima; S. Tsutsui; Y. Haga; H. Yasuoka; R.E. Walstedt; N.M. Masaki; A. Nakamura; S. Nasu; Y. Onuki First-order phase transition in UO₂: ${}^{235}U$ and ${}^{17}O$ NMR study, Phys. Rev. B, Volume 63 (2001), p. 104404

[24] S. Carretta; P. Santini; R. Caciuffo; G. Amoretti Quadrupolar waves in uranium dioxide, Phys. Rev. Lett., Volume 105 (2010), p. 167201

[25] F. Bultmark; F. Cricchio; O. Grånäs; L. Nordström Multipole decomposition of $LDA + U$ energy and its application to actinide compounds, Phys. Rev. B, Volume 80 (2009), p. 035121

[26] S.-T. Pi; R. Nanguneri; S. Savrasov Calculation of multipolar exchange interactions in spin–orbital coupled systems, Phys. Rev. Lett., Volume 112 (2014), p. 077203

[27] N.M. Edelstein; G.H. Lander Magnetic properties, The Chemistry of the Actinide and Transactinide Elements, vol. 4, Springer, The Netherlands, 2011

[28] Y. Tokunaga; T. Nishi; S. Kambe; M. Nakada; A. Itoh; Y. Homma; H. Sakai; H. Chudo NMR evidence for the 8.5 K phase transition in americium dioxide, J. Phys. Soc. Jpn., Volume 79 (2010), p. 053705

[29] N. Magnani; P. Santini; G. Amoretti; R. Caciuffo Perturbative approach to J mixing in f-electron systems: application to actinide dioxides, Phys. Rev. B, Volume 71 (2005), p. 054405

[30] M.M. Abraham; L.A. Boatner; C.B. Finch; R.W. Reynolds Electron-paramagnetic-resonance investigations of $5 f^{5}$ configuration ions in cubic single crystals: Pu³⁺ in ThO₂ and SrCl₂, and Am⁴⁺ in ThO₂, Phys. Rev. B, Volume 3 (1971), p. 2864

[31] T. Hotta Microscopic analysis of multipole susceptibility of actinide dioxides: a scenario of multipole ordering in AmO₂, Phys. Rev. B, Volume 80 (2009), p. 024408

[32] Y. Tokunaga; T. Nishi; M. Nakada; A. Itoh; H. Sakai; S. Kambe; Y. Homma; F. Honda; D. Aoki; R.E. Walstedt Self-radiation effects and glassy nature of magnetic transition in AmO₂ revealed by ${}^{17}O$ -NMR, Phys. Rev. B, Volume 89 (2014), p. 214416

Cited by Sources:

Comments - Policy