- Physical Review Journals
All JournalsPhysics Magazine

Physical Review Research

Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Letter
  • Open Access

Charge multipole correlations and order in Cs2TaCl6

Aria Mansouri Tehrani1,*, Jian-Rui Soh2,*, Jana Pásztorová2, Maximilian E. Merkel1, Ivica Živković2, Henrik M. Rønnow2, and Nicola A. Spaldin1,†

  • 1Materials Theory, ETH Zurich, Wolfgang-Pauli-Strasse 27, 8093 Zürich, Switzerland
  • 2Institute of Physics, Ecole Polytechnique Federale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

  • *These authors contributed equally to this work.
  • †nicola.spaldin@mat.ethz.ch
PDF

Phys. Rev. Research 5, L012010 – Published 26 January, 2023

DOI: https://doi.org/10.1103/PhysRevResearch.5.L012010

Abstract

We examine the role of charge, structural, and spin degrees of freedom in the previously poorly understood phase transition in the 5d1 transition-metal double perovskite Cs2TaCl6 using a combination of computational and experimental techniques. Our heat capacity measurements of single-crystalline Cs2TaCl6 reveal a clear anomaly at the transition temperature, TQ, which was not previously observed in polycrystalline samples. Density functional calculations indicate the emergence of local charge quadrupoles in the cubic phase, mediated by the paramagnetic spins or local structural distortions which then develop into long-range-ordered charge quadrupoles in the tetragonal phase. Our resonant elastic x-ray scattering on Cs2TaCl6 single crystals lends support to our calculations. Our work provides insight into the phase transition in Cs2TaCl6 at TQ, and demonstrates the utility of this unique combination of techniques in understanding the complex physics of hidden orders in paramagnetic spin-orbit-entangled compounds.

View figure in article

Physics Subject Headings (PhySH)

Article Text

References (27)

  1. K. Morikawa, T. Mizokawa, K. Kobayashi, A. Fujimori, H. Eisaki, S. Uchida, F. Iga, and Y. Nishihara, Spectral weight transfer and mass renormalization in Mott-Hubbard systems SrVO3 and CaVO3: Influence of long-range Coulomb interaction, Phys. Rev. B 52, 13711 (1995).
  2. C. C. Hays, J.-S. Zhou, J. T. Markert, and J. B. Goodenough, Electronic transition in La1−xSrxTiO3, Phys. Rev. B 60, 10367 (1999).
  3. H. D. Zhou and J. B. Goodenough, Evidence for two electronic phases in Y1−xLaxTiO3 from thermoelectric and magnetic susceptibility measurements, Phys. Rev. B 71, 184431 (2005).
  4. K. Samanta and T. Saha-Dasgupta, Comparative study of electronic structure and magnetic properties of osmate double perovskites: Ca2FeOsO6 versus Ca2Co(Ni)OsO6, J. Phys. Soc. Jpn. 87, 041007 (2018).
  5. G. Chen, R. Pereira, and L. Balents, Exotic phases induced by strong spin-orbit coupling in ordered double perovskites, Phys. Rev. B 82, 174440 (2010).
  6. W. Liu, R. Cong, E. Garcia, A. P. Reyes, H. O. Lee, I. R. Fisher, and V. F. Mitrović, Phase diagram of Ba2NaOsO6, a Mott insulator with strong spin orbit interactions, Phys. B: Condens. Matter 536, 863 (2018).
  7. L. Lu, M. Song, W. Liu, A. P. Reyes, P. Kuhns, H. O. Lee, I. R. Fisher, and V. F. Mitrović, Magnetism and local symmetry breaking in a Mott insulator with strong spin orbit interactions, Nat. Commun. 8, 14407 (2017).
  8. D. Hirai and Z. Hiroi, Successive symmetry breaking in a Jeff=3/2 quartet in the spin–orbit coupled insulator Ba2MgReO6, J. Phys. Soc. Jpn. 88, 064712 (2019).
  9. D. Hirai, H. Sagayama, S. Gao, H. Ohsumi, G. Chen, T.-h. Arima, and Z. Hiroi, Detection of multipolar orders in the spin-orbit-coupled 5d Mott insulator Ba2MgReO6, Phys. Rev. Res. 2, 022063(R) (2020).
  10. D. Hirai and Z. Hiroi, Possible quadrupole order in tetragonal Ba2CdReO6 and chemical trend in the ground states of 5d1 double perovskites, J. Phys.: Condens. Matter 33, 135603 (2021).
  11. H. Ishikawa, T. Takayama, R. K. Kremer, J. Nuss, R. Dinnebier, K. Kitagawa, K. Ishii, and H. Takagi, Ordering of hidden multipoles in spin-orbit entangled 5d1 Ta chlorides, Phys. Rev. B 100, 045142 (2019).
  12. H. Yun and G.-J. Jang, Dicaesium hexachlorotantalate(IV), Cs2TaCl6, Acta Crystallographica Section E Structure Reports Online 63, i22 (2007).
  13. M.-T. Suzuki, H. Ikeda, and P. M. Oppeneer, First-principles theory of magnetic multipoles in condensed matter systems, J. Phys. Soc. Jpn. 87, 041008 (2018).
  14. G. Trimarchi, Z. Wang, and A. Zunger, Polymorphous band structure model of gapping in the antiferromagnetic and paramagnetic phases of the Mott insulators MnO, FeO, CoO, and NiO, Phys. Rev. B 97, 035107 (2018).
  15. J. Varignon, M. Bibes, and A. Zunger, Mott gapping in 3dABO3 perovskites without Mott-Hubbard interelectronic repulsion energy U, Phys. Rev. B 100, 035119 (2019).
  16. A. Mansouri Tehrani and N. A. Spaldin, Untangling the structural, magnetic dipole, and charge multipolar orders in Ba2MgReO6, Phys. Rev. Mater. 5, 104410 (2021).
  17. G. Kresse and J. Hafner, Ab initio molecular dynamics for liquid metals, Phys. Rev. B 47, 558 (1993).
  18. G. Kresse and J. Furthmüller, Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set, Phys. Rev. B 54, 11169 (1996).
  19. G. Kresse and D. Joubert, From ultrasoft pseudopotentials to the projector augmented-wave method, Phys. Rev. B 59, 1758 (1999).
  20. P. E. Blöchl, Projector augmented-wave method, Phys. Rev. B 50, 17953 (1994).
  21. J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized Gradient Approximation Made Simple, Phys. Rev. Lett. 77, 3865 (1996).
  22. S. L. Dudarev, G. A. Botton, S. Y. Savrasov, C. J. Humphreys, and A. P. Sutton, Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study, Phys. Rev. B 57, 1505 (1998).
  23. F. Cricchio, F. Bultmark, O. Grånäs, and L. Nordström, Itinerant Magnetic Multipole Moments of Rank Five as the Hidden Order in URu2Si2, Phys. Rev. Lett. 103, 107202 (2009).
  24. N. A. Spaldin, M. Fechner, E. Bousquet, A. Balatsky, and L. Nordström, Monopole-based formalism for the diagonal magnetoelectric response, Phys. Rev. B 88, 094429 (2013).
  25. F. Bultmark, F. Cricchio, O. Grånäs, and L. Nordström, Multipole decomposition of LDA+U energy and its application to actinide compounds, Phys. Rev. B 80, 035121 (2009).
  26. The Elk Code, http://elk.sourceforge.net.
  27. M. E. Merkel, Multipyles v1.0.0, https://doi.org/10.5281/zenodo.6907024.

Outline

Information

Phys. Rev. Research 5, L012010– Published 26 January, 2023
  • Received 26 July 2022
  • Revised 29 September 2022
  • Accepted 2 November 2022
Crossmark - Check for updates button
Creative Commons Logo

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

Published by the American Physical Society

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation