The magnetic state of Nitrogen-doped MgO, with N substituting O at concentrations between 1% and the concentrated limit, is calculated with density-functional methods. The N atoms are found to be magnetic with a moment of 1 Bohr magneton per Nitrogen atom and to interact ferromagnetically via the double exchange mechanism. The long-range magnetic order is established above a finite concentration of about 1.5% when the percolation threshold is reached. The Curie temperature increases linearly with the concentration, and is found to be about 30 K for 10% concentration. Besides the substitution of single Nitrogen atoms, also interstitial Nitrogen atoms, clusters of Nitrogen atoms and their structural relaxation on the magnetism are discussed. Possible scenarios of engineering a higher Curie temperature are analyzed, with the conclusion that an increase of the Curie temperature is difficult to achieve, requiring a particular attention to the choice of chemistry.
We show that the magnetic characteristics of Ta|CoFeB|MgO magnetic heterostructures are strongly influenced by doping the Ta underlayer with nitrogen. In particular, the saturation magnetization drops upon doping the Ta underlayer, suggesting that the doped underlayer acts as a boron diffusion barrier. In addition, the thickness of the magnetic dead layer decreases with increasing nitrogen doping. Surprisingly, the interface magnetic anisotropy increases to ~1.8 erg/cm2 when an optimum amount of nitrogen is introduced into the Ta underlayer. These results show that nitrogen doped Ta serves as …
For a nitrogen dimer in insulating MgO, a ferromagnetic coupling between spin-polarized $2p$-holes is revealed by calculations based on the density functional theory amended by an on-site Coulomb interaction and corroborated by the Hubbard model. It is shown that the ferromagnetic coupling is facilitated by a T-shaped orbital arrangement of the $2p$-holes, which is in its turn controlled by an intersite Coulomb interaction due to the directionality of the $p$-orbitals. We thus conjecture that this interaction is an important ingredient of ferromagnetism in band insulators with $2p$ dopants.
We have investigated the room temperature ferromagnetic order that develops in Al-substituted magnesium oxide, Mg(Al)O, nanoparticles with Al fractions of up to 5 at.%. All samples, including undoped MgO nanoparticles, exhibit room temperature ferromagnetism, with the saturation magnetization reaching a maximum of 0.023 emu/g at 2 at.% of Al. X-ray photoelectron spectroscopy identifies the presence of oxygen vacancies in both doped and undoped MgO nanoparticles, with the vacancy concentration increasing upon vacuum annealing of Mg(Al)O, resulting in two-fold enhancement of the saturation magne…
It is shown that substitution of C or N for O recently proposed as a way to create ferromagnetism in otherwise nonmagnetic oxide insulators is curtailed by formation of impurity pairs, and the resultant C2 spin=1 dimers as well as the isoelectronic N2^{2+} interact antiferromagneticallly in p-type MgO. For C-doped ZnO, however, we demonstrate using the HSE hybrid functional that a resonance of the spin-polarized C2 ppπ* states with the host conduction band results in a long-range ferromagnetic interaction. Magnetism of open-shell impurity molecules is proposed as a possible route to d0-ferroma…
We study the possibility of d0 ferromagnetism in the compound MgO doped with nitrogen (N). The Haldane-Anderson impurity model is formulated within the tight-binding approximation for determining the host band-structure and the impurity-host hybridization. Using the quantum Monte Carlo technique, we observe a finite local moment for an N impurity, and long-range ferromagnetic correlations between two N impurities. The ferromagnetic correlations are strongly influenced by the impurity bound state. When the ferromagnetic correlation between a pair of impurities is mapped onto the isotropic Heise…
Using magnetron sputtering, we produced a series of Co/CoO-MgO nanoparticles on Si(100) substrates. High-resolution transmission electron microscopy (HRTEM) image shows that small isolated Co-clusters (core) covered with CoO (shells) with a size of a few nm embedded in a MgO matrix. Resistivity as a function of Co atomic ratio exhibits a distinct percolation threshold with a sharp decrease around 69% Co content. Across the threshold, the resistivity drops about 7 orders of magnitude. For a sample at this percolation critical threshold, we have observed a giant exchange bias field HE=2460 Oe at…
High Curie temperature of 900 K has been reported in Cr-doped AlN diluted magnetic semiconductors prepared by various methods, which is exciting for spintronic applications. It is believed that N defects play important roles in achieving the high temperature ferromagnetism in good samples. Motivated by these experimental advances, we use a full-potential density-functional-theory method and supercell approach to investigate N defects and their effects on ferromagnetism of (Al,Cr)N with N vacancies (V_N). Calculated results are in agreement with experimental observations and facts of real Cr-do…
The first-principles full-potential linearized augmented plane-wave method based on density functional theory is used to investigate electronic structure and magnetic properties of hypothetical binary compounds of I$^{A}$ subgroup elements with nitrogen (LiN, NaN, KN and RbN) in assumed three types of cristalline structure (rock salt, wurtzite and zinc-blende). We find that, due to the spin polarized \textit{p} orbitas of N, all four compounds are half-metallic ferromagnets with wide energy bandgaps (up to 2.0 eV). The calculated total magnetic moment in all investigated compounds for all thre…
Nitrogen embedded ZnO:N films prepared by pulsed laser deposition exhibit significant ferromagnetism. The nitrogen ions contained in ZnO confirmed by Secondary Ion Microscopic Spectrum and Raman experiments and the embedded nitrogen ions can be regarded as defects. According to the experiment results, a mechanism is proposed based on one of the electrons in the completely filled d-orbits of Zn that compensates the dangling bonds of nitrogen ions and leads to a net spin of one half in the Zn orbits. These one half spins strongly correlate with localized electrons that are captured by defects to…
Density functional theory with local spin density approximation has been used to propose possible room temperature ferromagnetism in N-doped NaCl-type BaO. Pristine BaO is a wide bandgap semiconductor, however, N induces a large density of states at the Fermi level in the nonmagnetic state, which suggests magnetic instability within the Stoner mean field model. The spin-polarized calculations show that N-doped BaO is a true half- metal, where N has a large magnetic moment, which is mainly localized around the N atoms and a small polarization at the O sites is also observed. The origin of magne…
II-oxide and III-nitride semiconductors doped by nonmagnetic 2p light elements are investigated as potential dilute magnetic semiconductors (DMS). Based on our first-principle calculations, nitrogen doped ZnO, carbon doped ZnO, and carbon doped AlN are predicted to be ferromagnetic. The ferromagnetism of such DMS materials can be attributed to a p-d exchange-like p-p coupling interaction which is derived from the similar symmetry and wave function between the impurity (p-like t_2) and valence (p) states. We also propose a co-doping mechanism, using beryllium and nitrogen as dopants in ZnO, to …
Clear evidence of ferromagnetic behavior at temperatures >400 K as well as spin polarization of the charge carriers have been observed in ZnMnO thin films grown on Al2O3 and MgO substrates. The magnetic properties depended on the exact Mn concentration and the growth parameters. In well-characterized single-phase films, the magnetic moment is 4.8?B/Mn at 350 K, the highest moment yet reported for any Mn doped magnetic semiconductor. Anomalous Hall effect shows that the charge carriers (electrons) are spin polarized and participate in the observed ferromagnetic behavior.
Thin FeRh film was extensively studied recently, and an emergent substrate- and capping-dependent interfacial ferromagnetism (FM) was widely observed in experiments. However, the voltage modulation of this interfacial ferromagnetism is barely studied, which would have profound applications in antiferromagnetic (AFM) FeRh-based magnetoelectric-random access memory (MeRAM). Using ab initio techniques, we comparatively study the interfacial ferromagnetic properties and magnetoelectric responses of ultrathin FeRh films capped by heavy transition metal Ta. We find that Ta capping reverses the phase…
We investigate the structural and magnetic properties of La$_{0.7}$Sr$_{0.3}$CrO$_3$ (LSCO)/La$_{0.7}$Sr$_{0.3}$MnO$_3$(LSMO) heterostructures grown on (001)-oriented MgO by molecular beam epitaxy. Due to the large film-substrate lattice mismatch, strain relaxation is found to occur within the first 2-3 unit cells (uc) of the film as evidenced by reflection high energy electron diffraction and high-resolution synchrotron X-ray reciprocal space mapping. We find that the presence of the LSCO spacer and capping layers leads to ferromagnetism in ultra-thin LSMO layers with thicknesses on the order…
Recent advances in the understanding of spin orbital effects in ultrathin magnetic heterostructures have opened new paradigms to control magnetic moments electrically. The Dzyaloshinskii-Moriya interaction (DMI) is said to play a key role in forming a Neel-type domain wall that can be driven by the spin Hall torque, a torque resulting from the spin current generated in a neighboring non-magnetic layer via the spin Hall effect. Here we show that the sign of the DMI, which determines the direction to which a domain wall moves with current, can be changed by modifying the adjacent non-magnetic la…
We investigated the electronic and optical properties of bilayer AB stacked Boron and Nitrogen vacancies in hexagonal Boron Nitride (h-BN) using density functional theory (DFT). The density of states (DOS) and electronic band structure showed that Boron vacancy in bilayer h-BN results in a magnetic and conducting ground state. The band gap energy ranges from 4.56 eV for the pristine BN bilayer to 0.12 eV for a single Nitrogen vacancy in the bilayer. Considering the presence of 1,3,4-Boron vacancy, half metallic character is observed. However, the 2-boron vacancy configuration resulted in metal…
The effect of additional doping of charge impurities was investigated in a ferromagnetic semiconductor Zn$_{1-x}$Cr$_{x}$Te. It was found that the doping of iodine, which is expected to act as an n-type dopant in ZnTe, brought about a drastic enhancement of the ferromagnetism in Zn$_{1-x}$Cr$_{x}$Te while the grown films remained electrically insulating. In particular, at a fixed Cr composition of x = 0.05, the ferromagnetic transition temperature Tc increased up to 300K at maximum due to the iodine doping from Tc = 30K of the undoped counterpart, while the ferromagnetism disappeared due to th…
Nitrogen-Vacancy-Mediated Magnetism in Sputtered GdN Thin Films
Indian Institute of Science（印度科学研究所）；Jawaharlal Nehru Center for Advanced Scientific Research（贾瓦哈拉尔·尼赫鲁高级科学研究中心）；Indian Institute of Technology Madras（马德拉斯印度理工学院）；IISER Thiruvananthapuram（特凡纳普拉姆印度科学教育研究院）；BITS Pilani K. K. Birla Goa Campus（比拉工业与科学研究所皮拉尼校区K.K.比尔拉果阿分校）
We study the electronic structure of the recently discovered diluted magnetic semiconductor Ga$_{1-x}$Cr$_{x}$N ($x$ = 0.01-0.10). A systematic study of the changes in the $occupied$ and $unoccupied$ ligand (N) partial density of states (DOS) of the host lattice is carried out using N 1$s$ soft x-ray emission and absorption spectroscopy, respectively. X-ray absorption measurements confirm the wurtzite N 2$p$ DOS and substitutional doping of Cr into Ga-sites. Coupled changes in the $occupied$ and $unoccupied$ N 2$p$ character DOS of Ga$_{1-x}$Cr$_{x}$N identify states responsible for ferromagne…
The spin-polarization and magnetic coupling character of N-doped SrTiO3 and BaTiO3 are studied through first-principles calculations. The substitutional N doping at O sites leads to a half-metallic property and produces a magnetic moment of 1.0 μB. The magnetic interaction between the nearest and next-nearest N dopants results in a strong ferromagnetic coupling. When the distance between the N dopants is larger than 7 Å, the ground state of the system tends to be paramagnetic. A nitrogen-concentration threshold to produce the ferromagnetism is estimated. The calculated results give a good expl…
Recent advances in the understanding of spin orbital effects in ultrathin magnetic heterostructures have opened new paradigms to control magnetic moments electrically. The Dzyaloshinskii-Moriya interaction (DMI) is said to play a key role in forming a Neel-type domain wall that can be driven by the spin Hall torque, a torque resulting from the spin current generated in a neighboring non-magnetic layer via the spin Hall effect. Here we show that the strength and sign of the DMI can be changed by modifying the adjacent heavy metal underlayer (X) in perpendicularly magnetized X|CoFeB|MgO heterstr…
BaMF4 (M=Fe, Co, Ni and Mn) family are typical multiferroic materials, having antiferromagnetism at around liquid nitrogen temperature. In this work, polycrystalline BaFeF4 has been prepared by solid state reaction. The slight deficiency of Fe leads to the coexistence of valence states of +2 and +3, facilitating the electrons to hop between the neighboring Fe2+ and Fe3+ ions through the middle F- ion, leading to the strong double exchange interaction with weak ferromagnetism above room temperature. A bifurcation at about 170 K between the zero-field-cooled and field-cooled temperature dependen…
We present a study of p-type doping of CdTe and Cd$_{1-x}$Mn$_x$Te quantum wells from surface states. We show that this method is as efficient as usual modulation doping with nitrogen acceptors, and leads to hole densities exceeding $2 \times 10^{11}$ cm$^{-2}$. Surface doping was successfully applied to obtain carrier-induced ferromagnetism in a Cd$_{1-x}$Mn$_x$Te quantum well. The observed temperature dependence of photoluminescence spectra, and the critical temperature, correspond well to those previously reported for ferromagnetic quantum wells doped with nitrogen.
The prospects of half-metallic ferromagnetism being induced by the incorporation of C atoms into alkaline-earth-metal-oxides are investigated by the first principle calculation. The origin of the ferromagnetism is discussed through the calculation of the electronic structure and exchange coupling constant by using the pseudo-potential-like self-interaction-corrected local spin density method. The Curie temperature ($T_c$) is also predicted by employing the Monte Carlo simulation. It is shown that by taking the electron self-interaction into account, the half-metallic ferromagnetism induced by …
Quantum anomalous Hall effect (QAHE) has been experimentally observed in magnetically doped topological insulators. However, ultra-low temperature (usually below 300 mK), which is mainly attributed to inhomogeneous magnetic doping, becomes a daunting challenge for potential applications. Here, a \textit{nonmagnetic}-doping strategy is proposed to produce ferromagnetism and realize QAHE in topological insulators. We numerically demonstrated that magnetic moments can be induced by nitrogen or carbon substitution in Bi$_2$Se$_3$, Bi$_2$Te$_3$, and Sb$_2$Te$_3$, but only nitrogen-doped Sb$_2$Te$_3…
Pressure Dependence of Ferromagnetism in Uranium Hydride UH$_3$ up to 20 GPa Revealed by NV Centers Magnetometry
CEA DAM, DIF；Université Paris-Saclay（巴黎萨克雷大学）；CEA（法国原子能和替代能源委员会）；Laboratoire Matière en Conditions Extrêmes（极端条件物质实验室）；CNRS（法国国家科学研究中心）；ENS Paris-Saclay（巴黎萨克雷高等师范学院）；Centralesupelec（中央理工-电院）
A magneto-structural phase transition is investigated in single crystal CrN thin films grown by rf plasma molecular beam epitaxy on MgO(001) substrates. While still within the vacuum environment following MBE growth, $\it in-situ$ low-temperature scanning tunneling microscopy, and $\it in-situ$ variable low-temperature reflection high energy electron diffraction are applied, revealing an atomically smooth and metallic CrN(001) surface, and an $\it in-plane$ structural transition from 1$\times$1 (primitive CrN unit cell) to $\mathrm{\sqrt{2}\times\sqrt{2}-R45^\circ}$ with a transition temperatu…
We present a systematic study of the ferromagnetic transition induced by the holes in nitrogen doped Zn1-xMnxTe epitaxial layers, with particular emphasis on the values of the Curie-Weiss temperature as a function of the carrier and spin concentrations. The data are obtained from thorough analyses of the results of magnetization, magnetoresistance and spin-dependent Hall effect measurements. The experimental findings compare favorably, without adjustable parameters, with the prediction of the Rudermann-Kittel-Kasuya-Yosida (RKKY) model or its continuous-medium limit, that is, the Zener model, …
Two-dimensional (2D) magnetic van der Waals materials provide a powerful platform for studying fundamental physics of low-dimensional magnetism, engineering novel magnetic phases, and enabling ultrathin and highly tunable spintronic devices. To realize high quality and practical devices for such applications, there is a critical need for robust 2D magnets with ordering temperatures above room temperature that can be created via exfoliation. Here the study of exfoliated flakes of cobalt substituted Fe5GeTe2 (CFGT) exhibiting magnetism above room temperature is reported. Via quantum magnetic ima…
We have performed x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) studies of the diluted ferromagnetic semiconductor Zn$_{1-\textit{x}}$Cr$_\textit{x}$Te doped with iodine (I) or nitrogen (N), corresponding to electron or hole doping, respectively. From the shape of the Cr $2p$ absorption peak in the XAS spectra, it was concluded that Cr ions in the undoped, I-doped and lightly N-doped samples are divalent (Cr$^{2+}$), while Cr$^{2+}$ and trivalent (Cr$^{3+}$) coexist in the heavily N-doped sample. This result indicates that the doped nitrogen atoms act as acce…
Control of magnetic states by external factors has garnered a mainstream status in spintronic research for designing low power consumption and fast-response information storage and processing devices. Previously, magnetic-cation substitution is the conventional means to induce ferromagnetism in an intrinsic antiferromagnet. Theoretically, the anion-doping is proposed to be another effect means to change magnetic ground states. Here we demonstrate the synthesis of high-quality single-phase chromium oxynitride thin films using in-situ nitrogen doping. Unlike antiferromagnetic monoanionic chromiu…
We demonstrate room-temperature ferromagnetism with in-plane magnetic anisotropy in thin flakes of the CrTe$_2$ van der Waals ferromagnet. Using quantitative magnetic imaging with a single spin magnetometer based on a nitrogen-vacancy defect in diamond, we infer a room-temperature in-plane magnetization in the range of $M\sim 27$ kA/m for flakes with thicknesses down to $20$ nm. In addition, our measurements indicate that the orientation of the magnetization is not determined solely by shape anisotropy in micron-sized CrTe$_2$ flakes, which suggest the existence of a non-negligible magnetocrys…
