- 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
  • Open Access

Simulating spin waves in entropy stabilized oxides

Tom Berlijn1,*, Gonzalo Alvarez2, David S. Parker3, Raphaël P. Hermann3, and Randy S. Fishman3

  • 1Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
  • 2Computational Sciences and Engineering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
  • 3Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA

  • *berlijnt@ornl.gov
PDF

Phys. Rev. Research 3, 033273 – Published 22 September, 2021

DOI: https://doi.org/10.1103/PhysRevResearch.3.033273

Abstract

The entropy stabilized oxide Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O exhibits antiferromagnetic order and magnetic excitations, as revealed by recent neutron scattering experiments. This observation raises the question of the nature of spin-wave excitations in such disordered systems. Here, we investigate theoretically the magnetic ground state and the spin-wave excitations using linear spin-wave theory in combination with the supercell approximation to take into account the extreme disorder in this magnetic system. We find that the experimentally observed antiferromagnetic structure can be stabilized by a rhombohedral distortion together with large second-nearest-neighbor interactions. Our calculations show that the spin-wave spectrum consists of a well-defined low energy coherent spectrum in the background of an incoherent continuum that extends to higher energies.

View figure in article

Physics Subject Headings (PhySH)

Article Text

References (51)

  1. D. B. Miracle and O. N. Senkov, A critical review of high entropy alloys and related concepts, Acta Mater. 122, 448 (2017).
  2. C. M. Rost, E. Sachet, T. Borman, A. Moballegh, E. C. Dickey, D. Hou, J. L. Jones, S. Curtarolo, and J.-P. Maria, Entropy-stabilized oxides, Nat. Commun. 6, 8485 (2015).
  3. A. Sarkar, Q. Wang, A. Schiele, M. R. Chellali, S. S. Bhattacharya, D. Wang, T. Brezesinski, H. Hahn, L. Velasco, and B. Breitung, High-entropy oxides: Fundamental aspects and electrochemical properties, Adv. Mater. 31, 1806236 (2019).
  4. D. Bérardan, S. Franger, D. Dragoe, A. K. Meena, and N. Dragoe, Colossal dielectric constant in high entropy oxides, Phys. Status Solidi RRL 10, 328 (2016).
  5. D. Bérardan, S. Franger, A. K. Meena, and N. Dragoe, Room temperature lithium superionic conductivity in high entropy oxides, J. Mater. Chem. A 4, 9536 (2016).
  6. J. L. Braun, C. M. Rost, M. Lim, A. Giri, D. H. Olson, G. N. Kotsonis, G. Stan, D. W. Brenner, J.-P. Maria, and P. E. Hopkins, Charge-induced disorder controls the thermal conductivity of entropy-stabilized oxides, Adv. Mater. 30, 1805004 (2018).
  7. A. Sarkar, R. Djenadic, D. Wang, C. Hein, R. Kautenburger, O. Clemens, and H. Hahn, Rare earth and transition metal based entropy stabilised perovskite type oxides, J. Eur. Ceram. Soc. 38, 2318 (2018).
  8. S. Jiang, T. Hu, J. Gild, N. Zhou, J. Nie, M. Qin, T. Harrington, K. Vecchio, and J. Luo, A new class of high-entropy perovskite oxides, Scr. Mater. 142, 116 (2018).
  9. Y. Sharma, B. L. Musico, X. Gao, C. Hua, A. F. May, A. Herklotz, A. Rastogi, D. Mandrus, J. Yan, H. N. Lee, M. F. Chisholm, V. Keppens, and T. Z. Ward, Single-crystal high entropy perovskite oxide epitaxial films, Phys. Rev. Mater. 2, 060404(R) (2018).
  10. J. Gild, M. Samiee, J. L. Braun, T. Harrington, H. Vega, P. E. Hopkins, K. Vecchio, and J. Luo, High-entropy fluorite oxides, J. Eur. Ceram. Soc. 38, 3578 (2018).
  11. K. Chen, X. Pei, L. Tang, H. Cheng, Z. Li, C. Li, X. Zhang, and L. An, A five-component entropy-stabilized fluorite oxide, J. Eur. Ceram. Soc. 38, 4161 (2018).
  12. J. Dąbrowa, M. Stygar, A. Mikuła, A. Knapik, K. Mroczka, W. Tejchman, M. Danielewski, and M. Martin, Synthesis and microstructure of the (Co,Cr,Fe,Mn,Ni)3O4 high entropy oxide characterized by spinel structure, Mater. Lett. 216, 32 (2018).
  13. E. Castle, T. Csanádi, S. Grasso, J. Ã. Dusza, and M. Reece, Processing and properties of high-entropy ultra-high temperature carbides, Sci. Rep. 8, 8609 (2018).
  14. X. Yan, L. Constantin, Y. Lu, J.-F. Silvain, M. Nastasi, and B. Cui, (Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)C high-entropy ceramics with low thermal conductivity, J. Am. Ceram. Soc. 101, 4486 (2018).
  15. J. Gild, Y. Zhang, T. Harrington, S. Jiang, T. Hu, M. C. Quinn, W. M. Mellor, N. Zhou, K. Vecchio, and J. Luo, High-entropy metal diborides: A new class of high-entropy materials and a new type of ultrahigh temperature ceramics, Sci. Rep. 6, 37946 (2016).
  16. Z. Deng, A. Olvera, J. Casamento, J. S. Lopez, L. Williams, R. Lu, G. Shi, P. F. P. Poudeu, and E. Kioupakis, Semiconducting high-entropy chalcogenide alloys with ambi-ionic entropy stabilization and ambipolar doping, Chem. Mater. 32, 6070 (2020).
  17. P. B. Meisenheimer, T. J. Kratofil, and J. T. Heron, Giant enhancement of exchange coupling in entropy-stabilized oxide heterostructures, Sci. Rep. 7, 13344 (2017).
  18. J. Zhang, J. Yan, S. Calder, Q. Zheng, M. A. McGuire, D. L. Abernathy, Y. Ren, S. H. Lapidus, K. Page, H. Zheng, J. W. Freeland, J. D. Budai, and R. P. Hermann, Long-range antiferromagnetic order in a rocksalt high entropy oxide, Chem. Mater. 31, 3705 (2019).
  19. M. P. Jimenez-Segura, T. Takayama, D. Bérardan, A. Hoser, M. Reehuis, H. Takagi, and N. Dragoe, Long-range magnetic ordering in rocksalt-type high-entropy oxides, Appl. Phys. Lett. 114, 122401 (2019).
  20. C. G. Shull, W. A. Strauser, and E. O. Wollan, Neutron diffraction by paramagnetic and antiferromagnetic substances, Phys. Rev. 83, 333 (1951).
  21. W. L. Roth, Magnetic structures of MnO, FeO, CoO, and NiO, Phys. Rev. 110, 1333 (1958).
  22. B. A. Frandsen, K. A. Petersen, N. A. Ducharme, A. G. Shaw, E. J. Gibson, B. Winn, J. Yan, J. Zhang, M. E. Manley, and R. P. Hermann, Spin dynamics and a nearly continuous magnetic phase transition in an entropy-stabilized oxide antiferromagnet, Phys. Rev. Mater. 4, 074405 (2020).
  23. A. Z. Menshikov, Yu. A. Dorofeev, A. G. Klimenko, and N. A. Mironova, Magnetic phase diagram of (Ni1−xMgx)O solid solutions, Phys. Status Solidi B 164, 275 (1991).
  24. D. Rodic, V. Spasojevic, V. Kusigerski, R. Tellgren, and H. Rundlof, Magnetic ordering in polycrystalline NixZn1−xO solid solutions, Phys. Status Solidi B 218, 527 (2000).
  25. M. S. Seehra, J. C. Dean, and R. Kannan, Magnetic phase diagrams of diluted fcc antiferromagnets CopMg1−p and EupSr1−pTe, Phys. Rev. B 37, 5864 (1988).
  26. C. M. Rost, Z. Rak, D. W. Brenner, and J.-P. Maria, Local structure of the MgxNixCoxCuxZnxO(x=0.2) entropy-stabilized oxide: An exafs study, J. Am. Ceram. Soc. 100, 2732 (2017).
  27. Zs. Rak, C. M. Rost, M. Lim, P. Sarker, C. Toher, S. Curtarolo, J.-P. Maria, and D. W. Brenner, Charge compensation and electrostatic transferability in three entropy-stabilized oxides: Results from density functional theory calculations, J. Appl. Phys. 120, 095105 (2016).
  28. J. B. Goodenough, An interpretation of the magnetic properties of the perovskite-type mixed crystals La1−xSrxCoO3−λ, J. Phys. Chem. Solids 6, 287 (1958).
  29. J. Kanamori, Superexchange interaction and symmetry properties of electron orbitals, J. Phys. Chem. Solids 10, 87 (1959).
  30. H.-X. Deng, J. Li, S.-S. Li, J.-B. Xia, A. Walsh, and S.-H. Wei, Origin of antiferromagnetism in coo: A density functional theory study, Appl. Phys. Lett. 96, 162508 (2010).
  31. D. Ködderitzsch, W. Hergert, W. M. Temmerman, Z. Szotek, A. Ernst, and H. Winter, Exchange interactions in NiO and at the NiO(100) surface, Phys. Rev. B 66, 064434 (2002).
  32. Zs. Rák and D. W. Brenner, Exchange interactions and long-range magnetic order in the (Mg,Co,Cu,Ni,Zn)O entropy-stabilized oxide: A theoretical investigation, J. Appl. Phys. 127, 185108 (2020).
  33. M. T. Hutchings and E. J. Samuelsen, Measurement of spin-wave dispersion in NiO by inelastic neutron scattering and its relation to magnetic properties, Phys. Rev. B 6, 3447 (1972).
  34. K. Tomiyasu and S. Itoh, Magnetic excitations in coo, J. Phys. Soc. Jpn. 75, 084708 (2006).
  35. Y. Yamamoto and T. Nagamiya, Spin arrangements in magnetic compounds of the rocksalt crystal structure, J. Phys. Soc. Jpn. 32, 1248 (1972).
  36. R. Fishman, J. Fernandez-Baca, and T. Room, Spin-Wave Theory and its Applications to Neutron Scattering and THz Spectroscopy (Morgan & Claypool, San Rafael, 2018).
  37. T. Berlijn, Effects of Disordered Dopants on the Electronic Structure of Functional Materials: Wannier Function-Based First Principles Methods for Disordered Systems, Ph.D. thesis, Stony Brook University, 2011.
  38. https://g1257.github.io/spinGlassSW.html
  39. P. Buczek, L. M. Sandratskii, N. Buczek, S. Thomas, G. Vignale, and A. Ernst, Magnons in disordered nonstoichiometric low-dimensional magnets, Phys. Rev. B 94, 054407 (2016).
  40. X. Bai, J. A. M. Paddison, E. Kapit, S. M. Koohpayeh, J.-J. Wen, S. E. Dutton, A. T. Savici, A. I. Kolesnikov, G. E. Granroth, C. L. Broholm, J. T. Chalker, and M. Mourigal, Magnetic Excitations Of The Classical Spin Liquid MgCr2O4, Phys. Rev. Lett. 122, 097201 (2019).
  41. W. J. L. Buyers, D. E. Pepper, and R. J. Elliott, Spin waves in disordered systems. II. The dilute antiferromagnet (Mn, Zn)F2, J. Phys. C 6, 1933 (1973).
  42. A. M. Samarakoon, A. Banerjee, S.-S. Zhang, Y. Kamiya, S. E. Nagler, D. A. Tennant, S.-H. Lee, and C. D. Batista, Comprehensive study of the dynamics of a classical kitaev spin liquid, Phys. Rev. B 96, 134408 (2017).
  43. S. Baroni, S. de Gironcoli, and P. Giannozzi, Phonon Dispersions In GaxAl1−xAs Alloys, Phys. Rev. Lett. 65, 84 (1990).
  44. T. B. Boykin and G. Klimeck, Practical application of zone-folding concepts in tight-binding calculations, Phys. Rev. B 71, 115215 (2005).
  45. V. Popescu and A. Zunger, Effective Band Structure of Random Alloys, Phys. Rev. Lett. 104, 236403 (2010).
  46. T. Berlijn, D. Volja, and W. Ku, Can Disorder Alone Destroy the eg′ Hole Pockets of NaxCoO2? A Wannier Function Based First-Principles Method for Disordered Systems, Phys. Rev. Lett. 106, 077005 (2011).
  47. S. Thébaud, C. A. Polanco, L. Lindsay, and T. Berlijn, Success and breakdown of the t-matrix approximation for phonon-disorder scattering, Phys. Rev. B 102, 094206 (2020).
  48. D. Berardan, A. K. Meena, S. Franger, C. Herrero, and N. Dragoe, Controlled Jahn-Teller distortion in (MgCoNiCuZn)O-based high entropy oxides, J. Alloys Compd. 704, 693 (2017).
  49. Zs. Rák, J.-P. Maria, and D.W. Brenner, Evidence for Jahn-Teller compression in the (Mg, Co, Ni, Cu, Zn)O entropy-stabilized oxide: A DFT study, Mater. Lett. 217, 300 (2018).
  50. T. Fukushima, H. Katayama-Yoshida, K. Sato, M. Ogura, R. Zeller, and P. H. Dederichs, Local energies and energy fluctuations applied to the high entropy alloy crfeconi, J. Phys. Soc. Jpn. 86, 114704 (2017).
  51. http://energy.gov/downloads/doe-public-access-plan.

Outline

Information

Phys. Rev. Research 3, 033273– Published 22 September, 2021
  • Received 2 November 2020
  • Revised 1 September 2021
  • Accepted 3 September 2021
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