Ferroelectricity coexisted with p-orbital ferromagnetism and metallicity in two-dimensional metal oxynitrides
Source abstract
Abstract
Abstract Two-dimensional (2D) multiferroics have attracted increasing interests in basic science and technological fields in recent years. However, most reported 2D magnetic ferroelectrics are based on the d-electron magnetism, which makes them rather rare due to the empirical d0 rule and limits their applications for low magnetic phase transition temperature. In this work, we demonstrate that the ferroelectricity can coexist with the p-electron-induced ferromagnetism without the limitation of d0 rule and metallicity in a family of stable 2D MXene-analogous oxynitrides, X2NO2 (X = In, Tl). Remarkably, the itinerant character of p electrons can lead to the strong ferromagnetic metallic states. Furthermore, a possible magnetoelectric effect is manifested in a Tl2NO2/WTe2 heterostructure through the interface engineering. Our findings provide an alternative possible route toward 2D multiferroics and enrich the concept of ferroelectric metals.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: MXene and MAX Phase Materials · 2D Materials and Applications · Multiferroics and related materials
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (64)
Show source-provided references
1. Schmid, H. Multi-ferroic magnetoelectrics. Ferroelectrics 162, 317–338 (1994).10.1080/00150199408245120 ↗
2. Wang, K. F., Liu, J. M. & Ren, Z. F. Multiferroicity: the coupling between magnetic and polarization orders. Adv. Phys. 58, 321–448 (2009).10.1080/00018730902920554 ↗
3. Fiebig, M., Lottermoser, T., Meier, D. & Trassin, M. The evolution of multiferroics. Nat. Rev. Mater. 1, 16046 (2016).10.1038/natrevmats.2016.46 ↗
4. Vaz, C. A. F., Hoffman, J., Ahn, C. H. & Ramesh, R. Magnetoelectric coupling effects in multiferroic complex oxide composite structures. Adv. Mater. 22, 2900–2918 (2010).10.1002/adma.200904326 ↗
5. Dong, S., Liu, J.-M., Cheong, S.-W. & Ren, Z. Multiferroic materials and magnetoelectric physics: symmetry, entanglement, excitation, and topology. Adv. Phys. 64, 519–626 (2015).10.1080/00018732.2015.1114338 ↗
6. Seki, S., Yu, X. Z., Ishiwata, S. & Tokura, Y. Observation of skyrmions in a multiferroic material. Science 336, 198–201 (2012).10.1126/science.1214143 ↗
7. Takahashi, Y., Shimano, R., Kaneko, Y., Murakawa, H. & Tokura, Y. Magnetoelectric resonance with electromagnons in a perovskite helimagnet. Nat. Phys. 8, 121–125 (2012).10.1038/nphys2161 ↗
8. Spaldin, N. A. & Ramesh, R. Advances in magnetoelectric multiferroics. Nat. Mater. 18, 203–212 (2019).10.1038/s41563-018-0275-2 ↗
9. Gajek, M. et al. Tunnel junctions with multiferroic barriers. Nat. Mater. 6, 296–302 (2007).10.1038/nmat1860 ↗
10. Fiebig, M. Revival of the magnetoelectric effect. J. Phys. D: Appl. Phys. 38, R123–R152 (2005).10.1088/0022-3727/38/8/R01 ↗
11. Dong, S., Xiang, H. & Dagotto, E. Magnetoelectricity in multiferroics: a theoretical perspective. Natl Sci. Rev. 6, 629–641 (2019).10.1093/nsr/nwz023 ↗
12. Hill, N. A. Why are there so few magnetic ferroelectrics? J. Phys. Chem. B 104, 6694–6709 (2000).10.1021/jp000114x ↗
13. Wang, J. et al. Epitaxial BiFeO3 multiferroic thin film heterostructures. Science 299, 1719–1722 (2003).10.1126/science.1080615 ↗
14. Lee, J. H. et al. A strong ferroelectric ferromagnet created by means of spin–lattice coupling. Nature 466, 954–958 (2010).10.1038/nature09331 ↗
15. Kenzelmann, M. et al. Magnetic Inversion Symmetry Breaking and Ferroelectricity in TbMnO3. Phys. Rev. Lett. 95, 087206 (2005).10.1103/PhysRevLett.95.087206 ↗
16. Ai, H., Song, X., Qi, S., Li, W. & Zhao, M. Intrinsic multiferroicity in two-dimensional VOCl2 monolayers. Nanoscale 11, 1103–1110 (2019).10.1039/C8NR08270G ↗
17. Xu, C. et al. Electric-field switching of magnetic topological charge in type-i multiferroics. Phys. Rev. Lett. 125, 037203 (2020).10.1103/PhysRevLett.125.037203 ↗
18. Lai, Y. et al. Two-dimensional ferromagnetism and driven ferroelectricity in van der Waals CuCrP2S6. Nanoscale 11, 5163–5170 (2019).10.1039/C9NR00738E ↗
19. Zhang, J.-J. et al. Type-II multiferroic Hf2VC2F2 mxene monolayer with high transition temperature. J. Am. Chem. Soc. 140, 9768–9773 (2018).10.1021/jacs.8b06475 ↗
20. Huang, C. et al. Prediction of intrinsic ferromagnetic ferroelectricity in a transition-metal halide monolayer. Phys. Rev. Lett. 120, 147601 (2018).10.1103/PhysRevLett.120.147601 ↗
21. Zhou, Y. et al. Out-of-plane piezoelectricity and ferroelectricity in layered α-In2Se3 nanoflakes. Nano Lett. 17, 5508–5513 (2017).10.1021/acs.nanolett.7b02198 ↗
22. Li, H., Ruan, S. & Zeng, Y.-J. Intrinsic Van Der Waals magnetic materials from bulk to the 2D limit: new frontiers of spintronics. Adv. Mater. 31, 1900065 (2019).10.1002/adma.201900065 ↗
23. Feng, X., Ma, X., Sun, L., Liu, J. & Zhao, M. Tunable ferroelectricity and antiferromagnetism via ferroelastic switching in an FeOOH monolayer. J. Mater. Chem. C 8, 13982–13989 (2020).10.1039/D0TC04400H ↗
24. Chu, J. et al. 2D polarized materials: ferromagnetic, ferrovalley, ferroelectric materials, and related heterostructures. Adv. Mater. 33, 2004469 (2021).10.1002/adma.202004469 ↗
25. Coey, J. M. D. d0 ferromagnetism. Solid State Sci. 7, 660–667 (2005).10.1016/j.solidstatesciences.2004.11.012 ↗
26. Fu, L. et al. Graphitic-nitrogen-enhanced ferromagnetic couplings in nitrogen-doped graphene. Phys. Rev. B 102, 094406 (2020).10.1103/PhysRevB.102.094406 ↗
27. Pan, H. et al. Room-temperature ferromagnetism in carbon-doped ZnO. Phys. Rev. Lett. 99, 127201 (2007).10.1103/PhysRevLett.99.127201 ↗
28. Anderson, P. W. & Blount, E. I. Symmetry considerations on martensitic transformations: “ferroelectric” metals? Phys. Rev. Lett. 14, 217–219 (1965).10.1103/PhysRevLett.14.217 ↗
29. Shi, Y. et al. A ferroelectric-like structural transition in a metal. Nat. Mater. 12, 1024–1027 (2013).10.1038/nmat3754 ↗
30. Fei, Z. et al. Ferroelectric switching of a two-dimensional metal. Nature 560, 336–339 (2018).10.1038/s41586-018-0336-3 ↗
31. Shen, L., An, Y., Cao, D., Wu, Z. & Liu, J. Room-temperature ferromagnetic enhancement and crossover of negative to positive magnetoresistance in N-doped In2O3 films. J. Phys. Chem. C. 121, 26499–26506 (2017).10.1021/acs.jpcc.7b08732 ↗
32. Ding, W. et al. Prediction of intrinsic two-dimensional ferroelectrics in In2Se3 and other III2-VI3 van der Waals materials. Nat. Commun. 8, 14956 (2017).10.1038/ncomms14956 ↗
33. Shao, X. et al. Electronic properties of a pi-conjugated Cairo pentagonal lattice: Direct band gap, ultrahigh carrier mobility, and slanted Dirac cones. Phys. Rev. B 98, 085437 (2018).10.1103/PhysRevB.98.085437 ↗
34. Putzky, D. et al. Strain-induced structural transition in DyBa2Cu3O7−x films grown by atomic layer-by-layer molecular beam epitaxy. Appl. Phys. Lett. 117, 072601 (2020).10.1063/5.0019673 ↗
35. Grimme, S., Antony, J., Ehrlich, S. & Krieg, H. A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu. J. Chem. Phys. 132, 154104 (2010).10.1063/1.3382344 ↗
36. Ai, H., Ma, X., Shao, X., Li, W. & Zhao, M. Reversible out-of-plane spin texture in a two-dimensional ferroelectric material for persistent spin helix. Phys. Rev. Mater. 3, 054407 (2019).10.1103/PhysRevMaterials.3.054407 ↗
37. Anasori, B., Lukatskaya, M. R. & Gogotsi, Y. 2D metal carbides and nitrides (MXenes) for energy storage. Nat. Rev. Mater. 2, 16098 (2017).10.1038/natrevmats.2016.98 ↗
38. Hoover, W. G. Canonical dynamics: equilibrium phase-space distributions. Phys. Rev. A 31, 1695–1697 (1985).10.1103/PhysRevA.31.1695 ↗
39. Maździarz, M. Comment on ‘The Computational 2D Materials Database: high-throughput modeling and discovery of atomically thin crystals’. 2D Mater. 6, 048001 (2019).10.1088/2053-1583/ab2ef3 ↗
40. Mouhat, F. & Coudert, F.-X. Necessary and sufficient elastic stability conditions in various crystal systems. Phys. Rev. B 90, 224104 (2014).10.1103/PhysRevB.90.224104 ↗
41. Andrew, R. C., Mapasha, R. E., Ukpong, A. M. & Chetty, N. Mechanical properties of graphene and boronitrene. Phys. Rev. B 85, 125428 (2012).10.1103/PhysRevB.85.125428 ↗
42. Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865 (1996).10.1103/PhysRevLett.77.3865 ↗
43. Heyd, J., Scuseria, G. E. & Ernzerhof, M. Hybrid functionals based on a screened Coulomb potential. J. Chem. Phys. 118, 8207–8215 (2003).10.1063/1.1564060 ↗
44. Peng, H. et al. Origin and enhancement of hole-induced ferromagnetism in first-row d0 semiconductors. Phys. Rev. Lett. 102, 017201 (2009).10.1103/PhysRevLett.102.017201 ↗
45. Huang, B. et al. Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit. Nature 546, 270–273 (2017).10.1038/nature22391 ↗
46. Zhuang, H. L., Kent, P. R. C. & Hennig, R. G. Strong anisotropy and magnetostriction in the two-dimensional Stoner ferromagnet Fe3GeTe2. Phys. Rev. B 93, 134407 (2016).10.1103/PhysRevB.93.134407 ↗
47. Deng, Y. et al. Gate-tunable room-temperature ferromagnetism in two-dimensional Fe3GeTe2. Nature 563, 94–99 (2018).10.1038/s41586-018-0626-9 ↗
48. Halilov, S. V., Perlov, A. Y., Oppeneer, P. M., Yaresko, A. N. & Antonov, V. N. Magnetocrystalline anisotropy energy in cubic Fe, Co, and Ni: applicability of local-spin-density theory reexamined. Phys. Rev. B 57, 9557–9560 (1998).10.1103/PhysRevB.57.9557 ↗
49. Zhuang, H. L., Xie, Y., Kent, P. R. C. & Ganesh, P. Computational discovery of ferromagnetic semiconducting single-layer CrSnTe3. Phys. Rev. B 92, 035407 (2015).10.1103/PhysRevB.92.035407 ↗
50. Kan, M., Adhikari, S. & Sun, Q. Ferromagnetism in MnX2 (X = S, Se) monolayers. Phys. Chem. Chem. Phys. 16, 4990–4994 (2014).10.1039/c3cp55146f ↗
51. Shirodkar, S. N. & Waghmare, U. V. Emergence of ferroelectricity at a metal-semiconductor transition in a 1T monolayer of MoS2. Phys. Rev. Lett. 112, 157601 (2014).10.1103/PhysRevLett.112.157601 ↗
52. Gao, W. & Chelikowsky, J. R. Prediction of intrinsic ferroelectricity and large piezoelectricity in monolayer arsenic chalcogenides. Nano Lett. 20, 8346–8352 (2020).10.1021/acs.nanolett.0c03511 ↗
53. Sharma, P. et al. A room-temperature ferroelectric semimetal. Sci. Adv. 5, eaax5080 (2019).10.1126/sciadv.aax5080 ↗
54. Luo, W., Xu, K. & Xiang, H. Two-dimensional hyperferroelectric metals: a different route to ferromagnetic-ferroelectric multiferroics. Phys. Rev. B 96, 235415 (2017).10.1103/PhysRevB.96.235415 ↗
55. Obeid, M. M., Bafekry, A., Ur Rehman, S. & Nguyen, C. V. A type-II GaSe/HfS2 van der Waals heterostructure as promising photocatalyst with high carrier mobility. Appl. Surf. Sci. 534, 147607 (2020).10.1016/j.apsusc.2020.147607 ↗
56. Hohenberg, P. & Kohn, W. Inhomogeneous electron gas. Phys. Rev. 136, B864–B871 (1964).10.1103/PhysRev.136.B864 ↗
57. Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54, 11169 (1996).10.1103/PhysRevB.54.11169 ↗
58. Blöchl, P. E. Projector augmented-wave method. Phys. Rev. B 50, 17953–17979 (1994).10.1103/PhysRevB.50.17953 ↗
59. Monkhorst, H. J. & Pack, J. D. Special points for Brillouin-zone integrations. Phys. Rev. B 13, 5188–5192 (1976).10.1103/PhysRevB.13.5188 ↗
60. Bengtsson, L. Dipole correction for surface supercell calculations. Phys. Rev. B 59, 12301–12304 (1999).10.1103/PhysRevB.59.12301 ↗
61. Baroni, S., de Gironcoli, S., Dal Corso, A. & Giannozzi, P. Phonons and related crystal properties from density-functional perturbation theory. Rev. Mod. Phys. 73, 515–562 (2001).10.1103/RevModPhys.73.515 ↗
62. Togo, A., Oba, F. & Tanaka, I. First-principles calculations of the ferroelastic transition between rutile-type and CaCl2-type SiO2 at high pressures. Phys. Rev. B 78, 134106 (2008).10.1103/PhysRevB.78.134106 ↗
63. Henkelman, G., Uberuaga, B. P. & Jónsson, H. A climbing image nudged elastic band method for finding saddle points and minimum energy paths. J. Chem. Phys. 113, 9901–9904 (2000).10.1063/1.1329672 ↗
64. Liu, L., Chen, S., Lin, Z. & Zhang, X. A symmetry-breaking phase in two-dimensional FeTe2 with ferromagnetism above room temperature. J. Phys. Chem. Lett. 11, 7893–7900 (2020).10.1021/acs.jpclett.0c01911 ↗