Interlayer ferromagnetic coupling in nonmagnetic elements doped CrI<sub>3</sub> thin films

doi:10.1007/s11467-024-1435-2

Front. Phys.

2024, Vol. 19

Issue (6) : 63209 https://doi.org/10.1007/s11467-024-1435-2

Interlayer ferromagnetic coupling in nonmagnetic elements doped CrI₃ thin films

Xuqi Li¹, Xuyan Chen², Shiyang Sun¹, Huihui Zhang¹, Haidan Sang¹, Xiaonan Wang³, Shifei Qi^1,⁴(

), Zhenhua Qiao⁴(

)

¹. College of Physics and Hebei Advanced Thin Film Laboratory, Hebei Normal University, Shijiazhuang 050024, China
². School of Gifted Young, University of Science and Technology of China, Hefei 230026, China
³. School of Chemistry and Materials Science, Hebei Normal University, Shijiazhuang 050024, China
⁴. International Center for Quantum Design of Functional Materials, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, and Department of Physics, University of Science and Technology of China, Hefei 230026, China

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Abstract

The exploration of magnetism in two-dimensional layered materials has attracted extensive research interest. For the monoclinic phase CrI₃ with interlayer antiferromagnetism, finding a static and robust way of realizing the intrinsic interlayer ferromagnetic coupling is desirable. In this work, we study the electronic structure and magnetic properties of the nonmagnetic element (e.g., O, S, Se, N, P, As, and C) doped bi- and triple-layer CrI₃ systems via first-principles calculations. Our results demonstrate that O, P, S, As, and Se doped CrI₃ bilayer can realize interlayer ferromagnetism. Further analysis shows that the interlayer ferromagnetic coupling in the doped few-layer CrI₃ is closely related to the formation of localized spin-polarized state around the doped elements. Further study presents that, for As-doped tri-layer CrI₃, it can realize interlayer ferromagnetic coupling. This work proves that nonmagnetic element doping can realize the interlayer ferromagnetically-coupled few-layer CrI₃ while maintaining its semiconducting characteristics without introducing additional carriers.

Keywords ferromagnetism magnetic doping

Corresponding Author(s): Shifei Qi,Zhenhua Qiao

Issue Date: 06 August 2024

Cite this article:

Xuqi Li,Xuyan Chen,Shiyang Sun, et al. Interlayer ferromagnetic coupling in nonmagnetic elements doped CrI₃ thin films[J]. Front. Phys. , 2024, 19(6): 63209.

URL:

https://academic.hep.com.cn/fop/EN/10.1007/s11467-024-1435-2
https://academic.hep.com.cn/fop/EN/Y2024/V19/I6/63209

Fig.1 (a) Side and top views of crystal structures of high-temperature monoclinic bilayer CrI₃ phase and the substitution sites are labeled as I₁ and I₂. Formation energies of (b) O, S, Se, N and (c) P, As, or C element-doped bilayer CrI₃ as a function of the host element chemical potentials. Possible interstitial sites (d) and the formation energy (e) as a function of chemical potential for interstitial and substitutional configurations in the N doped bilayer CrI₃.

Structure	$Δ$ $E$ ( $↑$ $↓$ $↑$ )	$Δ$ $E$ ( $↑$ $↑$ $↓$ )	$Δ$ $E$ ( $↑$ $↓$ $↓$ )	$Δ$ $E$ ( $↑$ $↑$ $↑$ )

CrI₃	1.99	4.55	12.89	0
As₁	15.15	119.91	121.58	11.52
As₂	37.22	127.3	147.85	20.44
As₃	78.56	100.28	85.28	0

Tab.1 The structural and magnetic properties of As doped trilayer CrI₃. The spin direction of each layer is denoted by the up/down arrow. The ground state of each dopant is denoted by red. The energy differences between the specific structure and ground state are shown. The energy is in unit of meV.

Fig.2 (a) Energy difference between interlayer ferromagnetic (FM) and antiferromagnetic (AFM) states. (b) Difference of interlayer distance between doping configuration and pristine CrI₃. (c) Charge difference between Cr atoms near doping site in the doped and pristine bilayer CrI₃. (d) Schematic illustration of localized spin-polarized state-mediated interlayer ferromagneitic coupling in doped bilayer CrI₃.

Fig.3 Differential charge density of (a) pristine and (b) As-doped bilayer CrI₃. Spin density of (c) pristine and (d) As-doped bilayer CrI₃. Local density of states from (e) PBE+U and (f) HSE06 calculations in As-doped bilayer CrI₃. Yellow and blue isosurfaces represent respectively charge accumulation and reduction. Red and green isosurfaces represent respectively spin up and spin down. Cr-d, I-p and As-p orbitals in each layer of CrI₃ are displayed. In addition, band-decomposed charge density of the localized electron state is shown in the inset of (f).

Fig.4 The density of states in ferromagnetic state of (a) O, (b) P, (c) S, and (d) Se doped CrI₃ bilayer from PBE+U calculations. The density of states in ferromagnetic state of (e) O, (f) P, (g) S, and (h) Se doped CrI₃ bilayer from HSE06 calculations. Band-decomposed charge density of the localized electron state in ferromagnetic state of (i) O, (j) P, (k) S, and (l) Se doped CrI₃ bilayer from HSE06 calculations. The shadow part indicates the formation of spin-polarized state.

Fig.5 (a) Side view of crystal structure of trilayer CrI₃ with one As substitution at three sites I₁, I₂, and I₃. (b) Schematic illustration of ferromagnetic and three antiferromagnetic states in trilayer CrI₃.

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