Janus monolayer TaNF: A new ferrovalley material with large valley splitting and tunable magnetic properties

doi:10.1007/s11467-023-1285-3

Front. Phys.

2023, Vol. 18

Issue (5) : 53302 https://doi.org/10.1007/s11467-023-1285-3

RESEARCH ARTICLE

Janus monolayer TaNF: A new ferrovalley material with large valley splitting and tunable magnetic properties

Guibo Zheng¹, Shuixian Qu¹, Wenzhe Zhou¹(

), Fangping Ouyang^1,^2,³(

)

¹. School of Physics and Electronics, and Hunan Key Laboratory for Super-Microstructure and Ultrafast Process, and Hunan Key Laboratory of Nanophotonics and Devices, Central South University, Changsha 410083, China
². School of Physics and Technology, Xinjiang University, Urumqi 830046, China
³. State Key Laboratory of Powder Metallurgy, and Powder Metallurgy Research Institute, Central South University, Changsha 410083, China

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Abstract

Materials with large intrinsic valley splitting and high Curie temperature are a huge advantage for studying valleytronics and practical applications. In this work, using first-principles calculations, a new Janus TaNF monolayer is predicted to exhibit excellent piezoelectric properties and intrinsic valley splitting, resulting from the spontaneous spin polarization, the spatial inversion symmetry breaking and strong spin−orbit coupling (SOC). TaNF is also a potential two-dimensional (2D) magnetic material due to its high Curie temperature and large magnetic anisotropy energy. The effective control of the band gap of TaNF can be achieved by biaxial strain, which can transform TaNF monolayer from semiconductor to semi-metal. The magnitude of valley splitting at the CBM can be effectively tuned by biaxial strain due to the changes of orbital composition at the valleys. The magnetic anisotropy energy (MAE) can be manipulated by changing the energy and occupation (unoccupation) states of d orbital compositions through biaxial strain. In addition, Curie temperature reaches 373 K under only −3% biaxial strain, indicating that Janus TaNF monolayer can be used at high temperatures for spintronic and valleytronic devices.

Keywords Janus valley splitting Curie temperature magnetic anisotropy energy first-principles calculations

Corresponding Author(s): Wenzhe Zhou,Fangping Ouyang

Issue Date: 21 April 2023

Cite this article:

Guibo Zheng,Shuixian Qu,Wenzhe Zhou, et al. Janus monolayer TaNF: A new ferrovalley material with large valley splitting and tunable magnetic properties[J]. Front. Phys. , 2023, 18(5): 53302.

URL:

https://academic.hep.com.cn/fop/EN/10.1007/s11467-023-1285-3
https://academic.hep.com.cn/fop/EN/Y2023/V18/I5/53302

Fig.1 (a) Top and (b) side views of the crystal structure of the Janus TaNF monolayer. The bond length of Ta−F is longer than that of Ta−N (l₁ > l₂), thus the distance between different sublayers d₁ is longer than d₂. (c) Phonon dispersion and (d) variation of total free energy with time during the ab initio molecular dynamics simulation (AIMD) for Janus TaNF monolayer at 300 K. The inset in (d) corresponds the snapshot taken from the end of the simulation. (e) Top views of the spin-polarized charge density of Janus TaNF monolayer. The spin-up and spin-down charge are indicated by red and green isosurfaces. (f) The differential charge density of F−Ta−N cross section, where the red and blue represent depletion and accumulation of electrons respectively.

Tab.1 Structural parameters and band gap of Janus TaNF monolayer. The lattice constant (a = b), the bond length of Ta−F (l₁) and Ta−N (l₂), the distance between the sublayers of Ta, F(d₁) and Ta, N (d₂) and elastic constants (C₁₁ and C₁₂) are shown. The band gap of Janus TaNF monolayer within PBE + SOC are also shown.

Tab.2 Piezoelectric coefficients (e₁₁, e₃₁, d₁₁, and d₃₁) of Janus TaNF monolayer, along with the ones of some typical TMDs 2D materials.

Fig.2 (a) The spin projected band with SOC and (b) orbital projected band structure of Janus TaNF monolayer. The blue and red solid dots correspond to spin-up and spin-down of z direction.

Fig.3 (a) Dependence of valley splitting (Δ_K−K′) and band gap (E_g) as functions of biaxial strain in the Janus TaNF monolayer. (b) The orbital components of K valley as functions of biaxial strain.

Fig.4 Atomic arrangement of magnetic moments for (a) ferromagnetic and (b, c) antiferromagnetic orders of Janus TaNF monolayer. (b) The schematic plot of magnetic bond energies E_F,1 and E_A,1 between the nearest Ta−Ta moments, and E_F,2 and E_A,2 between the next-nearest Ta−Ta moments. The spin-up and spin-down charge are indicated by yellow and green isosurfaces.

Fig.5 The variations of exchange interaction parameters J₁ and J₂(a), MAE and Curie temperature T_c (b) and projected orbital coupling matrix elements of Ta atoms (c) of the Janus TaNF monolayer as a function of the biaxial strain. (d) The d orbital PDOS near the Fermi level of Ta atom of Janus TaNF monolayer under a −2%, 0% and 3% biaxial strain. The black solid line represents Fermi level, and the two vertical black dashed lines show the bottom of spin-up and spin-down unoccupied states.

Fig.6 (a) The d-orbital-projected-MAE of Ta atom for Janus TaNF monolayer. (b) Temperature variation of the magnetic moment and magnetic susceptibility for the Janus TaNF monolayer.

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