Two-dimensional ferromagnetic semiconductors of rare-earth monolayer GdX2 (X = Cl, Br, I) with large perpendicular magnetic anisotropy and high Curie temperature

Two-dimensional (2D) ferromagnetic (FM) semiconductors with high Curie temperature (T c ) and large perpendicular magnetic anisotropy (PMA) are promising for developing next-generation magnetic storage devices. In this work, we investigated the structural, electronic, and magnetic properties of MoF3 and Janus Mo2F3 X 3 (X = Cl, Br, I) monolayers by first-principles methods. These materials are 2D FM semiconductors with large PMA and half-semiconducting character as both VBM and CBM belonging to the spin-up channel. Biaxial strain can modulate band gap, reverse easy magnetization axis, and induce magnetic phase transitions in MoF3 monolayer and its Janus structures. Compared to MoF3 monolayers, Janus Mo2F3 X 3 monolayers can preserve the structural ability and the FM ground state over a wider range of strain. The magnetic anisotropy energies (MAEs) of these 2D materials can be enhanced to greater than 1 meV/Mo by tensile strains. Intrinsic T c of MoF3 monolayer and its Janus structures are less than 110 K and are insensitive to strain. However, hole doping with a feasible concentration can achieve a room-temperature half-metallicity in these 2D materials. The required hole concentration is lower in Janus Mo2F3 X 3 monolayers than MoF3 monolayer. Our results indicate that MoF3 and Janus Mo2F3 X 3 (X = Cl, Br, I) monolayers are promising candidates for 2D spintronic applications and will stimulate experimental and theoretical broad studies.

Two-dimensional (2D) ferromagnetic semiconductors are highly promising candidates for spintronics, but are rarely reported with direct band gaps, high Curie temperatures (Tc), and large magnetic anisotropy. Using first-principles calculations, we predict that two ferromagnetic monolayers, BiXO3 (X = Ru, Os), are such materials with a direct band gap of 2.64 and 1.69 eV, respectively. Monte Carlo simulations reveal that the monolayers show high Tc beyond 400 K. Interestingly, both BiXO3 monolayers exhibit out-of-plane magnetic anisotropy, with magnetic anisotropy energy (MAE) of 1.07 meV per Ru for BiRuO3 and 5.79 meV per Os for BiOsO3. The estimated MAE for the BiOsO3 sheet is one order of magnitude larger than that for the CrI3 monolayer (685 μeV per Cr). Based on the second-order perturbation theory, it is revealed that the large MAE of the monolayers BiRuO3 and BiOsO3 is mainly contributed by the matrix element differences between dxy and dx2-y2 and dyz and dz2 orbitals. Importantly, the ferromagnetism remains robust in 2D BiXO3 under compressive strain, while undergoing a ferromagnetic to antiferromagnetic transition under tensile strain. The intriguing electronic and magnetic properties make BiXO3 monolayers promising candidates for nanoscale electronics and spintronics.

Prediction of novel two-dimensional room-temperature ferromagnetic rare-earth material - GdB2N2 with large perpendicular magnetic anisotropy

Two-dimensional (2D) intrinsic ferromagnetic materials with large magnetic anisotropy (MA) and high Curie temperature (TC) are desirable for low-dimensional spintronic applications. In this work, a highly stable Janus NbXY (X, Y = S, Se and Te, X ≠ Y) monolayers with intrinsic ferromagnetism is investigated by using first-principles calculations. The results demonstrate that the MAE values of the NbSSe, NbSTe and NbSeTe MLs are as high as −2.185 meV, −4.013 meV and −4.495 meV per unit cell, respectively, which is higher than the previously reported 2D intrinsic ferromagnetic materials such as FeBrI, NiI2, and VSSe MLs etc. And they are still large enough for practical applications. The Curie temperature (Tc) is estimated to be 160 K for NbSSe monolayer, 260 K for NbSTe monolayer, and 200 K for NbSeTe monolayer based on Monte Carlo simulation. The MAE and Tc could be effectively controlled and enhanced by the biaxial strains. The MAE of NbSSe, NbSTe and NbSeTe MLs can be increased by 8.7%, 24.9% and 14.1%, and reach up to −2.375, −5.015 and −5.131 meV at 5% compressive strain, respectively. Remarkably, at 5% tensile strain, the room temperature Tc of 300 K can be reached for NbSTe monolayer, which is rather promising for its practical application. The large magnetic anisotropy energy and controllable Curie temperature make the NbXY monolayers a promising candidate for applications in spintronic devices at the nanoscale and in high-density data storage.

Strain-tunable magnetic property of ferromagnetic square CoSe monolayer

Two-dimensional (2D) ferromagnetic semiconductors (FMSs) hold exciting and promising potential for application in spintronic devices at the nanoscale. Currently, most 2D FMSs are based on 3d electrons; 4f electrons can provide nontrivial magnetism but have been much less studied to date. This paper presents a theoretical study, via first-principles calculations, of EuSn2X2 (X = P, As) monolayers based on rare-earth cations with f-electrons. The results show that EuSn2X2 monolayers possess a large magnetization (7 μB/Eu), a controllable magnetic anisotropy energy, and a unique d-electron-mediated f–f exchange mechanism. Both types of EuSn2X2 (X = P, As) monolayers are FMSs with indirect bandgaps of 1.00 and 0.99 eV, respectively, based on the Heyd–Scuseria–Ernzerhof (HSE06) method, which can be transform to direct bandgap semiconductors under biaxial strain. Interestingly, under the latter, spin–orbit coupling interaction gradually replaces the dipole–dipole interaction in the dominant position of magnetic anisotropy, resulting in the magnetic easy axis changing from in-plane to the more desirable out-of-plane. Considering their excellent dynamic, thermal, and mechanical stabilities and small cleavage energy, these EuSn2X2 monolayers can be exfoliated from their synthesized bulk. Our study not only helps to understand the properties of 2D 4f rare-earth magnets but also signposts a route toward improving the performance of EuSn2X2 monolayers in nano-electronic devices.

Two-dimensional (2D) ferromagnets with high Curie temperatures (TC) and large perpendicular magnetic anisotropy (PMA) are rare, but have great potential in the field of spintronics. The present work investigates the electronic and magnetic properties of GdX (X = Cl and Br) monolayers and the two layers of GdCl/GdBr heterojunctions by conducting in-depth theoretical calculations. As expected, both GdCl and GdBr monolayers are ferromagnetic and have large magnetic moments of ∼8 μB per Gd atom. Besides, they both show large PMA with magnetic anisotropy energies of 0.88 and 0.85 meV/unit cell and ultrahigh TC of 826 and 704 K, respectively. Significantly, they both have topological properties and spin-orbit-induced energy band reversion. In addition, we found two stable stacking configurations for the GdCl/GdBr bilayer heterojunction. The ultrahigh TC and topological properties are maintained in the two stacking configurations. Their easy magnetization axes shift from out-of-plane to in-plane directions as a result of the competition mainly between the Gd p and Gd d orbitals. These properties endow GdCl and GdBr monolayers with great potential for practical applications in the field of spintronic devices at the nanoscale.

A perpendicularly magnetized spin injector with a high Curie temperature is a prerequisite for developing spin optoelectronic devices on two-dimensional (2D) materials working at room temperature (RT) with zero applied magnetic field. Here, we report the growth of Ta/CoFeB/MgO structures with large perpendicular magnetic anisotropy (PMA) on full-coverage monolayer (ML) molybdenum disulfide (MoS2). A large perpendicular interface anisotropy energy of 0.975 mJ/m2 has been obtained at the CoFeB/MgO interface, comparable to that observed in magnetic tunnel junction systems. It is found that the insertion of MgO between the ferromagnetic (FM) metal and the 2D material can effectively prevent the diffusion of the FM atoms into the 2D material. Moreover, the MoS2 ML favors a MgO(001) texture and plays a critical role in establishing the large PMA. First-principles calculations on a similar Fe/MgO/MoS2 structure reveal that the MgO thickness can modify the MoS2 band structure, from a direct band gap with 3ML-MgO to an indirect band gap with 7 ML-MgO. The proximity effect induced by Fe results in splitting of 10 meV in the valence band at the Γ point for the 3ML-MgO structure, while it is negligible for the 7 ML-MgO structure. These results pave the way to develop RT spin optoelectronic devices based on 2D transition-metal dichalcogenide materials.

High Curie temperature and large perpendicular magnetic anisotropy in two-dimensional half metallic OsI3 monolayer with quantum anomalous Hall effect

Prediction of two-dimensional M2As (M = Mn, Fe) with high Curie temperature and large perpendicular magnetic anisotropy

Two-dimensional (2D) intrinsic ferromagnetic semiconductors (FMSs) with high Curie temperatures (TC) and large perpendicular magnetic anisotropy (PMA) have immense potential in spintronic applications. Recently, the TC of the discovered 2D intrinsic FMSs is below room temperature, and the easy magnetization axis (EMA) is oriented in the in-plane direction. Here, using the first-principle calculations and the Monte Carlo simulations, we investigate the effect of V doping on structure, electronic structure, and magnetic properties of the CrVS2I2 monolayer. The calculated formation energy, phonon dispersion, ab initio molecular dynamics simulations, and elastic constants of the CrVS2I2 monolayer indicate that it is stable at room temperature. More importantly, V doping converts the EMA direction of the CrVS2I2 monolayer from in-plane to out-of-plane, accompanied by a significant enhancement of magnetic anisotropy energy from 0.0011 to 0.997 meV/atom, and it also enhances TC from 175 to 352 K. Moreover, the CrVS2I2 monolayer remains as a semiconductor with a direct band gap of 0.38 eV. Our findings provide a feasible route for the realization of high TC and large PMA in 2D intrinsic FMSs.

Two-dimensional ferromagnetic materials with large perpendicular magnetic anisotropy (PMA) hold great potential in realizing low critical switching current, high thermal stability and high density nonvolatile storage in magnetic random-access memories. Our first-principles calculations reveal that CrOF and CrOCl monolayers (MLs) are two-dimensional (2D) ferromagnetic semiconductors with out-of-plane magnetic easy axis, and PMAs of CrOF and CrOCl MLs are mainly contributed by Cr atoms. The magnetic anisotropy of CrOF and CrOCl MLs can be controlled and enhanced by applying biaxial strain. Tensile strain can further enhance PMAs of CrOF and CrOCl MLs by 82.9% and 161.0% higher than those of unstrained systems, respectively. In addition, appropriate compressive strain can switch the magnetic easy axis of CrOF and CrOCl MLs from out-of-plane direction to in-plane direction. The semiconductor natures of CrOF and CrOCl MLs robust against biaxial strain, the band gaps of these systems under biaxial strain are in the range of 1.26 eV to 2.40 eV. By applying biaxial strain, the Curie temperatures of CrOF and CrOCl MLs increase up to 282 K and 163 K, respectively. These tunable properties suggest that CrOF and CrOCl MLs have great application potentials for magnetic data storage.

Magnetic tunnel junction based on the CoFeB/MgO/CoFeB structures is of great interest due to its application in the spin-transfer-torque magnetic random access memory (STT-MRAM). Large interfacial perpendicular magnetic anisotropy (PMA) is required to achieve high thermal stability. Here, we use the first-principles calculations to investigate the magnetic anisotropy energy (MAE) of the MgO/CoFe/capping layer structures, where the capping materials include 5d metals Hf, Ta, Re, Os, Ir, Pt, and Au and 6p metals Tl, Pb, and Bi. We demonstrate that it is feasible to enhance PMA by using proper capping materials. Relatively large PMA is found in the structures with the capping materials of Hf, Ta, Os, Ir, and Pb. More importantly, the MgO/CoFe/Bi structure gives rise to giant PMA (6.09 mJ/m2), which is about three times larger than that of the MgO/CoFe/Ta structure. The origin of the MAE is elucidated by examining the contributions to MAE from each atomic layer and orbital. These findings provide a comprehensive understanding of the PMA and point towards the possibility to achieve the advanced-node STT-MRAM with high thermal stability.

Large perpendicular magnetic anisotropy, high curie temperature, and half-metallicity in monolayer CrSI induced by substitution doping

The heterostructures with high perpendicular magnetic anisotropy (PMA) have advantages for the application of the nonvolatile memories with long data retention time and small size. The interface structure and magnetic anisotropy energy (MAE) of Co2FeAl/MgAl2O4 heterostructures were studied by first principles calculations. The stable interface atomic arrangement is the Co or FeAl layer located above the equatorial oxygen coordinate in the distorted oxygen octahedrons. The Co–O interface can induce large effective PMA up to 4.54 mJ m−2, but this structure is a metastable structure. Meanwhile, the effective MAE decreases linearly as the thickness of the ferromagnetic layer increase. The effective MAE for the FeAl–O interface is only 1.3 mJ m−2, while the maximum thickness of Co2FeAl layer that maintains the PMA effect is about 1.717 nm. These values are very close to the experimental results. Through d-orbital-resolved MAE, we confirm that the interface PMA is mainly originated from the hybridization between and orbitals of interface 3d atoms. In addition, the compressive strain, negative electric field and hole doping can significantly enhance the effective PMA of FeAl–O interface. At the same time, Co–O interface will become the most stable structure by tuning the Mg/Al ratio in the spinel layers. The large effective PMA makes the Co2FeAl/MgAl2O4 junction a perfect candidate for the next-generation of non-volatile spintronic devices.