journal article·2025-01-17Open access

Charge doping into spin minority states mediates doubling of TC in ferromagnetic CrGeTe3

Liam Trzaska, Lei Qiao, Matthew D. Watson, Monica Ciomaga Hatnean, Igor Marković, Edgar Abarca Morales, Tommaso Antonelli, Cephise Cacho, Geetha Balakrishnan, Wei Ren, Silvia Picozzi, Phil D. C. King

Abstract

Abstract The recent discovery of the persistence of long-range magnetic order when van der Waals magnets are thinned towards monolayers provides a tunable platform for engineering of novel magnetic structures and devices. Here, we study the evolution of the electronic structure of CrGeTe3 as a function of surface electron doping. From angle-resolved photoemission, we observe spectroscopic fingerprints that this electron doping drives a marked increase in T C, reaching values more than double that of the undoped material, in agreement with recent studies using electrostatic gating. Together with density functional theory calculations and Monte Carlo simulations, we show that, surprisingly, the increased T C is mediated by the population of spin-minority Cr t 2g states, forming a half-metallic 2D electron gas. This promotes a novel variant of double exchange, and unlocks a significant influence of Ge – which was previously thought to be electronically inert in this system – in mediating Cr-Cr exchange.
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Research context

OpenAlex topics: 2D Materials and Applications · Heusler alloys: electronic and magnetic properties · Magnetic and transport properties of perovskites and related materials

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References (35)

Show source-provided references
1. Chaves, A. et al. Bandgap engineering of two-dimensional semiconductor materials. npj 2D Mater. Appl. 4, 29 (2020).10.1038/s41699-020-00162-4 ↗
2. Cao, C. et al. Dimensionality control of electrocatalytic activity in perovskite nickelates. Nano Lett. 20, 2837–2842 (2020).10.1021/acs.nanolett.0c00553 ↗
3. King, P. D. C. et al. Atomic-scale control of competing electronic phases in ultrathin LaNiO3. Nat. Nano 9, 443–447 (2014).10.1038/nnano.2014.59 ↗
4. Peierls, R. On Ising’s model of ferromagnetism. Math. Proc. Camb. Philos. Soc. 32, 477–481 (1936).10.1017/S0305004100019174 ↗
5. Gibertini, M., Koperski, M., Morpurgo, A. F. & Novoselov, K. S. Magnetic 2D materials and heterostructures. Nat. Nanotechnol. 14, 408–419 (2019).10.1038/s41565-019-0438-6 ↗
6. Carteaux, V., Brunet, D., Ouvrard, G. & Andre, G. Crystallographic, magnetic and electronic structures of a new layered ferromagnetic compound Cr2Ge2Te6. J. Phys.: Condens. Matter 7, 69 (1995).
7. Ji, H. et al. A ferromagnetic insulating substrate for the epitaxial growth of topological insulators. J. Appl. Phys. 114, 114907 (2013).10.1063/1.4822092 ↗
8. Liu, Y. & Petrovic, C. Critical behavior of quasi-two-dimensional semiconducting ferromagnet Cr2Ge2Te6. Phys. Rev. B 96, 054406 (2017).10.1103/PhysRevB.96.054406 ↗
9. Verzhbitskiy, I. A. et al. Controlling the magnetic anisotropy in Cr2Ge2Te6 by electrostatic gating. Nat. Electron. 3, 460–465 (2020).10.1038/s41928-020-0427-7 ↗
10. Wang, K., Nikolaev, S., Ren, W. & Solovyev, I. Giant contribution of the ligand states to the magnetic properties of the Cr2Ge2Te6 monolayer. Phys. Chem. Chem. Phys. 21, 9597–9604 (2019).10.1039/C9CP01034C ↗
11. Li, Y. F. et al. Electronic structure of ferromagnetic semiconductor CrGeTe3 by angle-resolved photoemission spectroscopy. Phys. Rev. B 98, 125–127 (2018).
12. Riley, J. M. et al. Negative electronic compressibility and tunable spin splitting in WSe2. Nat. Nanotechnol. 10, 1043–1047 (2015).10.1038/nnano.2015.217 ↗
13. Liu, L. et al. Tunable electronic properties and enhanced ferromagnetism in Cr2Ge2Te6 monolayer by strain engineering. Nanotechnology 32, 485408 (2021).10.1088/1361-6528/ac1a94 ↗
14. Wang, K. et al. Magnetic and electronic properties of Cr2Ge2Te6 monolayer by strain and electric-field engineering. Appl. Phys. Lett. 114, 092405 (2019).10.1063/1.5083992 ↗
15. Lifshitz, I. M. Anomalies of electron characteristics in the high pressure region.Zhur. Eksptl’. i Teoret. Fiz. 38, https://www.osti.gov/biblio/4173345 (1960).
16. Watson, M. D. et al. Direct observation of the energy gain underpinning ferromagnetic superexchange in the electronic structure of CrGeTe3. Phys. Rev. B 101, 205125 (2020).10.1103/PhysRevB.101.205125 ↗
17. Wang, N. et al. Transition from ferromagnetic semiconductor to ferromagnetic metal with enhanced curie temperature in Cr2Ge2Te6 via organic ion intercalation. J. Am. Chem. Soc. 141, 17166–17173 (2019).10.1021/jacs.9b06929 ↗
18. Kang, S., Kang, S. & Yu, J. Effect of coulomb interactions on the electronic and magnetic properties of two-dimensional CrSiTe3 and CrGeTe3 materials. J. Electron. Mater. 48, 1441–1445 (2019).10.1007/s11664-018-6601-2 ↗
19. Haddadi, F., Linscott, E., Timrov, I., Marzari, N. & Gibertini, M. On-site and intersite hubbard corrections in magnetic monolayers: The case of feps3 and cri3. Phys. Rev. Mater. 8, 014007 (2024).10.1103/PhysRevMaterials.8.014007 ↗
20. Torelli, D. et al. High throughput computational screening for 2D ferromagnetic materials: the critical role of anisotropy and local correlations. 2D Mater. 6, 045018 (2019).10.1088/2053-1583/ab2c43 ↗
21. Tang, Q. & Zhu, X. Half-metallic double perovskite oxides: recent developments and future perspectives. J. Mater. Chem. C. 10, 15301–15338 (2022).10.1039/D2TC03199J ↗
22. Baer, D. R. et al. XPS guide: Charge neutralization and binding energy referencing for insulating samples. J. Vac. Sci. Technol. A 38, 031204 (2020).10.1116/6.0000057 ↗
23. Luttinger, J. M. & Ward, J. C. Ground-state energy of a many-fermion system. ii. Phys. Rev. 118, 1417–1427 (1960).10.1103/PhysRev.118.1417 ↗
24. Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865 (1996).10.1103/PhysRevLett.77.3865 ↗
25. Kresse, G. & Hafner, J. Ab initio molecular dynamics for liquid metals. Phys. Rev. B 47, 558 (1993).10.1103/PhysRevB.47.558 ↗
26. Klime, J., Bowler, D. R. & Michaelides, A. Van der Waals density functionals applied to solids. Phys. Rev. B 83, 195131 (2011).10.1103/PhysRevB.83.195131 ↗
27. Klimeš, J., Bowler, D. R. & Michaelides, A. Chemical accuracy for the van der Waals density functional. J. Phys.: Condens. Matter 22, 022201 (2009).
28. Blöchl, P. E. Projector augmented-wave method. Phys. Rev. B 50, 17953 (1994).10.1103/PhysRevB.50.17953 ↗
29. Kresse, G. & Joubert, D. From ultrasoft pseudopotentials to the projector augmented-wave method. Phys. Rev. B 59, 1758 (1999).10.1103/PhysRevB.59.1758 ↗
30. Monkhorst, H. J. & Pack, J. D. Special points for Brillouin-zone integrations. Phys. Rev. B 13, 5188 (1976).10.1103/PhysRevB.13.5188 ↗
31. Fang, Y., Wu, S., Zhu, Z.-Z. & Guo, G.-Y. Large magneto-optical effects and magnetic anisotropy energy in two-dimensional Cr2Ge2Te6. Phys. Rev. B 98, 125416 (2018).10.1103/PhysRevB.98.125416 ↗
32. Evans, R. F. et al. Atomistic spin model simulations of magnetic nanomaterials. J. Phys.: Condens. Matter 26, 103202 (2014).
33. Xiang, H., Lee, C., Koo, H.-J., Gong, X. & Whangbo, M.-H. Magnetic properties and energy-mapping analysis. Dalton Trans. 42, 823–853 (2013).10.1039/C2DT31662E ↗
34. Asselin, P. et al. Constrained Monte Carlo method and calculation of the temperature dependence of magnetic anisotropy. Phys. Rev. B 82, 054415 (2010).10.1103/PhysRevB.82.054415 ↗
35. Trzaska, L. et al. Charge doping into spin minority states mediates doubling of TC in ferromagnetic CrGeTe3 (dataset). Dataset. University of St Andrews Research Portal. https://doi.org/10.17630/d2994e11-d310-46f1-9fa3-927d9895443f (2025).10.17630/d2994e11-d310-46f1-9fa3-927d9895443f ↗