Real-space imaging of non-collinear antiferromagnetic order with a single spin magnetometer
I. Gross, W. Akhtar, V. Garcia, L. J. Martínez, S. Chouaieb, K. Garcia, C. Carrétéro, A. Barthélémy, P. Appel, P. Maletinsky, J. -V. Kim, J. Y. Chauleau, N. Jao… 展开作者
I. Gross, W. Akhtar, V. Garcia, L. J. Martínez, S. Chouaieb, K. Garcia, C. Carrétéro, A. Barthélémy, P. Appel, P. Maletinsky, J. -V. Kim, J. Y. Chauleau, N. Jaouen, M. Viret, M. Bibes, S. Fusil, V. Jacques
While ferromagnets are at the heart of daily life applications, their large magnetization and resulting energy cost for switching bring into question their suitability for reliable low-power spintronic devices. Non-collinear antiferromagnetic systems do not suffer from this problem and often possess remarkable extra functionalities: non-collinear spin order may break space-inversion symmetry and thus allow electric-field control of magnetism, or produce emergent spin-orbit effects, which enable efficient spin-charge interconversion. To harness these unique traits for next-generation spintronics, the nanoscale control and imaging capabilities that are now routine for ferromagnets must be developed for antiferromagnetic systems. Here, using a non-invasive scanning nanomagnetometer based on a single nitrogen-vacancy (NV) defect in diamond, we demonstrate the first real-space visualization of non-collinear antiferromagnetic order in a magnetic thin film, at room temperature. We image the spin cycloid of a multiferroic BiFeO$_3$ thin film and extract a period of $\sim70$ nm, consistent with values determined by macroscopic diffraction. In addition, we take advantage of the magnetoelectric coupling present in BiFeO$_3$ to manipulate the cycloid propagation direction by an electric field. Besides highlighting the unique potential of NV magnetometry for imaging complex antiferromagnetic orders at the nanoscale, these results demonstrate how BiFeO$_3$ can be used as a versatile platform for the design of reconfigurable nanoscale spin textures.
Electric susceptibility of antiferromagnetic multiferroics with cycloidal spin order at magnetoelectric effect associated with collinear component of spins
We investigate topological features of electronic structures which produce large anomalous Hall effect in the non-collinear antiferromagnetic metallic states of anti-perovskite manganese nitrides by first-principles calculations. We first predict the stable magnetic structures of these compounds to be non-collinear antiferromagnetic structures characterized by either $T_{1g}$ or $T_{2g}$ irreducible representation by evaluating the total energy for all of the magnetic structures classified according to the symmetry and multipole moments. The topology analysis is next performed for the Wannier …
The non-collinear antiferromagnetic (AFM) structure makes Mn3Sn exhibit exotic properties. At present, it has been found that both the hydrostatic pressure and the strain introduced by interstitial N atoms have a great influence on this magnetic structure. Here, the effect of the residual strain (RS) on it is investigated. AC and DC magnetic measurement results suggest that Mn3Sn without RS has the non-collinear AFM structure only in the temperature range of 285 K to 400 K; while Mn3Sn with RS has a non-coplanar AFM structure in the entire temperature range from 5 K to 400 K. Both anomalous Ha…
By the first-principles electronic structure calculations, we find that the ground state of PbO-type tetragonal $α$-FeTe is in a bi-collinear antiferromagnetic state, in which the Fe local moments ($\sim2.5μ_B$) are ordered ferromagnetically along a diagonal direction and antiferromagnetically along the other diagonal direction on the Fe square lattice. This bi-collinear order results from the interplay among the nearest, next nearest, and next next nearest neighbor superexchange interactions $J_1$, $J_2$, and $J_3$, mediated by Te $5p$-band. In contrast, the ground state of $α$-FeSe is in the…
A novel setup for the measurement of magnetic fields external to certain antiferromagnets and generally weakly remanent magnetic materials is presented. The setup features a highly sensitive Super Conducting Quantum Interference Device (SQUID) magnetometer with a magnetic field resolution of approx. 10 fT, non-electric thermalization of the sample space for a temperature range of 1.5 - 65 K with a non-electric sample movement drive and optical position encoding. To minimize magnetic susceptibility effects, the setup components are degaussed and realized with plastic materials in sample proximi…
The spin-splitter effect is theoretically predicted to generate an unconventional spin current with $\mathit{x}$- and $\mathit{z}$- spin polarization via the spin-split band in antiferromagnets. The generated torque, namely spin-splitter torque, is effective for the manipulation of magnetization in an adjacent magnetic layer without an external magnetic field for spintronic devices such as MRAM. Here, we study the generation of torque in collinear antiferromagnetic RuO$_2$ with (100), (101), and (001) crystal planes. Next we find all $\mathit{x}$-, $\mathit{y}$-, and $\mathit{z}$-polarized spi…
This focused issue attempts to provide a comprehensive introduction into the field of antiferromagnetic spintronics. Apart from the brief overview below, it features five review articles. The intention is to cover in a coherent and complementary way key physical aspects of the antiferromagnetic spintronics research. These range from microelectronic memory devices and optical manipulation and detection of antiferromagnetic spins, to the fundamentals of antiferromagnetic dynamics in uniform or spin-textured systems, and to the interplay of antiferromagnetic spintronics with topological phenomena…
Cavity spintronics explores light matter interactions at the interface between spintronic and quantum phenomena. Until now, studies have focused on the hybridization between ferromagnets and cavity photons.In this article, we realize antiferromagnetic cavity-magnon polaritons. The collective spin motion in single hematite crystals (α-Fe2O3) hybridizes with 18 - 45 GHz microwave cavity photons with required specific symmetries. We show theoretically and experimentally that the photon-magnon coupling in the collinear phase is mediated by the dynamical Neel vector and the weak magnetic moment in …
Antiferromagnetic thin films are currently generating considerable excitement for low dissipation magnonics and spintronics. However, while tuneable antiferromagnetic textures form the backbone of functional devices, they are virtually unknown at the submicron scale. Here we image a wide variety of antiferromagnetic spin textures in multiferroic BiFeO3 thin films that can be tuned by strain and manipulated by electric fields through room temperature magnetoelectric coupling. Using piezoresponse force microscopy and scanning NV magnetometry in self-organized ferroelectric patterns of BiFeO3, we…
We provide a complete and systematic first-principles study of the thermodynamic stability, structural parameters, and magnetic properties of the T1 non-collinear antiferromagnetic L1$_2$-IrMn$_3$ surface and L1$_2$-IrMn$_3$/Fe heterostructure. Furthermore, we investigate the exchange-bias effect in the heterostructure and describe its previously unknown complex magnetic coupling at the interface. We consider four atomic configurations and four magnetic arrangements, finding two stable terminations for the surface and for the heterostructure, which are in good agreement with experimental HR-TE…
Anomalous Hall enhancement in fully compensated non-collinear antiferromagnetic Cr-doped Mn3Sn
National University of Singapore（新加坡国立大学）；National University of Singapore (Chongqing) Research Institute（新加坡国立大学（重庆）研究院）；Nanyang Technological University（南洋理工大学）；Nanjing University（南京大学）；Central South University（中南大学）
By combining two independent approaches, inelastic neutron scattering measurements and density functional theory calculations, we study the spin-waves in the high-temperature collinear antiferromagnetic phase (AFM2) of Mn$_5$Si$_3$. We obtain its magnetic ground-state properties and electronic structure. This study allowed us to determine the dominant magnetic exchange interactions and magnetocrystalline anisotropy in the AFM2 phase of Mn$_5$Si$_3$. Moreover, the evolution of the spin excitation spectrum is investigated under the influence of an external magnetic field perpendicular to the ani…
Antiferromagnetic materials are of great interest for spintronics. Here we present a comprehensive study of the growth, structural characterization, and resulting magnetic properties of thin films of the non-collinear antiferromagnet Mn$_{3}$Ir. Using epitaxial engineering on MgO (001) and Al$_{2}$O$_{3}$ (0001) single crystal substrates, we control the growth of cubic $γ$-Mn$_{3}$Ir in both (001) and (111) crystal orientations, and discuss the optimization of growth conditions to achieve high-quality crystal structures with low surface roughness. Exchange bias is studied in bilayers, with exc…
Equilibrium spin configurations and their stability limits have been calculated for models of magnetic superlattices with a finite number of thin ferromagnetic layers coupled antiferromagnetically through (non-magnetic) spacers as Fe/Cr and Co/Ru multilayers. Depending on values of applied magnetic field and unaxial anisotropy, the system assumes collinear(antiferromagnetic, ferromagnetic, various "ferrimagnetic") phases, or spatially inhomogeneous (symmetric spin-flop phase and asymmetric, canted and twisted, phases)via series of field induced continuous and discontinuous transitions. Contrar…
We report on Cr doping effect in Mn3Sn polycrystalline films with both uniform and modulation doping. It is found that Cr doping with low concentration does not cause notable changes to the structural and magnetic properties of Mn3Sn, but it significantly enhances the anomalous Hall conductivity, particularly for modulation-doped samples at low temperature. A Hall conductivity as high as 184.8 Ω-1 cm-1 is obtained for modulation-doped samples at 50 K, in a sharp contrast to vanishingly small values for undoped samples at the same temperature. We attribute the enhancement to the change of Fermi…
Magnetic nanostructures on non-magnetic or magnetic substrates have attracted strong attention due to the development of new experimental methods with atomic resolution. Motivated by this progress we have extended the full-potential Korringa-Kohn-Rostoker (KKR) Green function method to treat non-collinear magnetic nanostructures on surfaces. We focus on magnetic 3d impurity nanoclusters, sitting as adatoms on or in the first surface layer on Ni(001), and investigate the size and orientation of the local moments and moreover the stabilization of non-collinear magnetic solutions. While clusters …
Antiferromagnetic spintronic devices have the potential to outperform conventional ferromagnetic devices due to their ultrafast dynamics and high data density. A challenge in designing these devices is the control and detection of the orientation of the anti-ferromagnet. One of the most promising ways to achieve this is through the exchange bias effect. This is of particular importance in large scale multigranular devices. Due to the large system sizes, previously, only micromagnetic simulations have been possible, these have an assumed distribution of antiferromagnetic anisotropy directions. …
Although a cubic phase of Mn$_3$Ga with an antiferromagnetic order has been theoretically predicted, it has not been experimentally verified in a bulk or film form. Here, we report the structural, magnetic, and electrical properties of antiferromagnetic cubic Mn$_3$Ga (C-Mn$_3$Ga) thin films, in comparison with ferrimagnetic tetragonal Mn$_3$Ga (T-Mn3Ga). The structural analyses reveal that C-Mn$_3$Ga is hetero-epitaxially grown on MgO substrate with the Cu$_3$Au-type cubic structure, which transforms to T-Mn$_3$Ga as the RF sputtering power increases. The magnetic and magnetotransport data sh…
Parity symmetric photoemission spectra are ubiquitous in solid state research, being prevalent in many highly active areas, such as unconventional superconductors, nonmagnetic and antiferromagnetic topological insulators, and weakly relativistic collinear magnets, among others. The direct observation of parity-violating metallic Kramers degenerate bands has remained hitherto experimentally elusive. Here we observe the antiferromagnetic parity violation (APV) in the bandstructure of Mn$_2$Au thin films by using momentum microscopy with sub-$mu$m spatial resolution, allowing momentum resolved ph…
We report on the ultrafast dynamics of magnetic order in a single crystal of CuO at a temperature of 207 K in response to strong optical excitation using femtosecond resonant x-ray diffraction. In the experiment, a femtosecond laser pulse induces a sudden, nonequilibrium increase in magnetic disorder. After a short delay ranging from 400 fs to 2 ps, we observe changes in the relative intensity of the magnetic ordering diffraction peaks that indicate a shift from a collinear commensurate phase to a spiral incommensurate phase. These results indicate that the ultimate speed for this antiferromag…
Cr0.68Se single crystals with two-dimensional (2D) character have been grown, and the detailed magnetization M(T), electrical transport properties (including longitudinal resistivity and Hall resistivity and thermal transport ones (including heat capacity Cp(T) and thermoelectric power (TEP) S(T)) have been measured. There are some interesting phenomena: (i) Cr0.68Se presents a non-collinear antiferromagnetic (AFM) semiconducting behavior with the Neel temperature TN = 42 K and the activated energy Eg=3.9 meV; (ii) It exhibits the anomalous Hall effect (AHE) below TN and large negative magneto…
We present a thorough theoretical assessment of the stability of non-collinear spin arrangements in small palladium clusters. We generally find that ferromagnetic order is always preferred, but that antiferromagnetic and non-collinear configurations of different sorts exist and compete for the first excited isomers. We also show that the ground state is insensitive to the choice of atomic configuration for the pseudopotential used and to the approximation taken for the exchange and correlation potential. Moreover, the existence and relative stability of the different excited configurations als…
We investigate the magnetic properties of Ru$_{2}$Mn$Z$ ($Z$ = Sn, Sb, Ge, Si) chemically ordered full Heusler compounds for zero as well as finite temperatures. Based on first principles calculations we derive the interatomic isotropic bilinear and biquadratic couplings between Mn atoms from the paramagnetic state. We find frustrated isotropic couplings for all compounds and in case of $Z$ = Si and Sb a nearest-neighbor biquadratic coupling that favors perpendicular alignment between the Mn spins. By using an extended classical Heisenberg model in combination with spin dynamics simulations we…
Using a first principles based, magnetic tight-binding total energy model, the magnetization energy and moments are computed for various ordered spin configurations in the high pressure polymorphs of iron (fcc, or $γ$-Fe, and hcp, or $ε$-Fe), as well ferromagnetic bcc iron ($α$-Fe). For hcp, a non-collinear, antiferromagnetic, spin configuration that minimizes unfavorable ferromagnetic nearest neighbor ordering is the lowest energy state and is more stable than non-magnetic $ε$ iron up to about 75 GPa. Accounting for non-collinear magnetism yields better agreement with the experimental equatio…
The present study reports on the structural and magnetic phase transitions in Pr-doped polycrystalline Tb0.6Pr0.4MnO3, using high-resolution neutron powder diffraction (NPD) collected at SINQ spallation source (PSI), to emphasize the suppression of the sinusoidal magnetic structure of pure TbMnO3 and the evolution to a collinear A-type antiferromagnetic ordering. The phase purity, Jahn-Teller distortion, and one-electron bandwidth for eg orbital of Mn3+ cation have been calculated for polycrystalline Tb0.6Pr0.4MnO3, in comparison to the parent materials TbMnO3 and PrMnO3, through the Rietveld …
We report the anomalous Hall effect (AHE) in antiperovskite Mn$_{3}$NiN with substantial doping of Cu on the Ni site (i.e. Mn$_{3}$Ni$_{1-x}$Cu$_{x}$N), which stabilizes a noncollinear antiferromagnetic (AFM) order compatible with the AHE. Observed on both sintered polycrystalline pieces and single crystalline films, the AHE does not scale with the net magnetization, contrary to the conventional ferromagnetic case. The existence of the AHE is explained through symmetry analysis based on the $Γ_{\rm 4g}$ AFM order in Cu doped Mn$_{3}$NiN. DFT calculations of the intrinsic contribution to the AH…
We show that strong electromagnon peaks can be found in absorption spectra of non-collinear magnets exhibiting a linear magnetoelectric effect. The frequencies of these peaks coincide with the frequencies of antiferromagnetic resonances and the ratio of the spectral weights of the electromagnon and antiferromagnetic resonance is related to the ratio of the static magnetoelectric constant and magnetic susceptibility. Using a Kagome lattice antiferromagnet as an example, we show that frustration of spin ordering gives rise to magnetoelastic instabilities at strong spin-lattice coupling, which tr…
We consider a synthetic antiferromagnetic spin-torque oscillator with anisotropic interlayer exchange coupling. This system exhibits exceptional points in its linearized dynamics. We find the non-linear dynamics and the dynamical phase diagram of the system both analytically and numerically. Moreover, we show that, near one of the exceptional points, the power of the oscillator depends extremely sensitively on the injected spin current. Our findings may be useful for designing sensitive magnetometers and for other applications of spin-torque oscillators.
We study the magnetic properties of small Mn ring shaped clusters on a Pt(111) surface in the framework of density functional theory. We find that the Mn atoms possess large magnetic moments, of the order of 4uB/atom, and have dominating antiferromagnetic interatomic exchange interactions. A quantum confinement effect within the ring like clusters was found, indicating that even very small clusters can be seen as quantum corrals. The antiferromagnetic exchange couplings lead to collinear magnetic arrangements in simple corrals, as well as complex non-collinear ordering, as vortex-like structur…
We propose Raman-induced collinear difference-frequency generation (DFG) as a method to manipulate dynamical magnetization. When a fundamental beam propagates along a threefold rotational axis, this coherent second-order optical process is permitted by angular momentum conservation through the rotational analogue of the Umklapp process. As a demonstration, we experimentally obtained polarization properties of collinear magnetic DFG along a [111] axis of a single crystal of antiferromagnetic NiO with micro multidomain structure, which excellently agreed with the theoretical prediction.
Electrical detection of the 180 deg spin reversal, which is the basis of the operation of ferromagnetic memories, is among the outstanding challenges in the research of antiferromagnetic spintronics. Analogous effects to the ferromagnetic giant or tunneling magnetoresistance have not yet been realized in antiferromagnetic multilayers. Anomalous Hall effect (AHE), which has been recently employed for spin reversal detection in non-collinear antiferromagnets, is limited to materials that crystalize in ferromagnetic symmetry groups. Here we demonstrate electrical detection of the 180 deg Néel vec…
Ni-Mn-Ga is interesting as a prototype of a magnetic shape-memory alloy showing large magnetic field induced strains. We present here results for the magnetic ordering of Mn-rich Ni-Mn-Ga alloys based on both experiments and theory. Experimental trends for the composition dependence of the magnetization are measured by a vibrating sample magnetometer (VSM) in magnetic fields of up to several tesla and at low temperatures. The saturation magnetization has a maximum near the stoichiometric composition and it decreases with increasing Mn content. This unexpected behaviour is interpreted via first…
Spin photogalvanic effect (SPGE) is an efficient method to generate a spin current by photoexcitation in a contactless and ultra-fast way. In two-dimensional (2D) collinear antiferromagnetic (AFM) materials that preserve the combined time-reversal (T) and inversion (I) symmetry (i.e., TI symmetry), we find that the photogalvanic currents in two magnetic sublattices carry different kinds of spins and propagate in opposite direction if the spin-orbit coupling is negligible, resulting in a pure spin current without net charge current. Based on the first-principles calculations, we show that two e…
We set forth the structural and magnetic properties of the frustrated spin-$5/2$ triangle lattice antiferromagnet Na$_3$Fe(PO$_4$)$_2$ examined via x-ray diffraction, magnetization, heat capacity, and neutron diffraction measurements on the polycrystalline sample. No structural distortion was detected from the temperature-dependant x-ray diffraction down to 12.5 K, except a systematic lattice contraction. The magnetic susceptibility at high temperatures agrees well with the high-temperature series expansion for a spin-$5/2$ isotropic triangular lattice antiferromagnet with an average exchange …
A combined experimental, using X-ray Magnetic Circular Dichroism and theoretical investigation, using full-potential Korringa-Kohn-Rostoker (KKR) Green function method, is carried out to study the spin structure of small magnetic Cr adatom--clusters on the surface of 3 monolayers of $fcc$ Fe deposited on Cu(001). The exchange interaction between the different Cr adatoms as well as between the Cr atoms and the Fe atoms is of antiferromagnetic nature and of comparable magnitude, leading due to frustration to complex non-collinear magnetic configurations. The presence of non-collinear magnetic co…
The triangular spin lattice of NiBr$_{2}$ is a canonical example of a frustrated helimagnet that shows a temperature-driven phase transition from a collinear commensurate antiferromagnetic structure to an incommensurate spin helix on cooling. Employing neutron diffraction, bulk magnetization, and magnetic susceptibility measurements, we have studied the f\hspace*{.5pt}ield-induced magnetic states of the NiBr$_{2}$ single crystal. Experimental f\hspace*{.5pt}indings enable us to recapitalize the driving forces of the spin spiral ordering in the triangular spin-lattice systems, in general. Neutr…
We theoretically study the carrier doping effect for magnetism in a stacked-kagome system $\rm{{Co}_3{Sn}_2{S}_2}$ based on an effective model and the Hartree-Fock method. We show the electron filling and temperature dependences of the magnetic order parameter. The perpendicular ferromagnetic ordering is suppressed by hole doping, wheres undoped $\rm{{Co}_3{Sn}_2{S}_2}$ shows magnetic Weyl semimetal state. Additionally, in the electron-doped regime, we find a non-collinear antiferromagnetic ordering. Especially, in the non-collinear antiferromagnetic state, by considering a certain spin-orbit …
We analyze and compare the effect of spatial and spin anisotropy on spin conductivity in a two dimensional S=1/2 Heisenberg quantum magnet on a square lattice. We explore the model in both the Neel antiferromagnetic (AF) phase and the collinear antiferromagnetic (CAF) phase. We find that in contrast to the effects of spin anisotropy in the Heisenberg model, spatial anisotropy in the AF phase does not suppress the zero temperature regular part of the spin conductivity in the zero frequency limit - rather it enhances it. We also explore the finite temperature effects on the Drude weight in the A…
Antiferromagnetic (AFM) spintronics has emerged as a subfield of spintronics driven by the advantages of antiferromagnets producing no stray fields and exhibiting ultrafast magnetization dynamics. The efficient method to detect an AFM order parameter, known as the Néel vector, by electric means is critical to realize concepts of AFM spintronics. Here, we demonstrate that non-collinear AFM metals, such as Mn3Sn, exhibit a momentum dependent spin polarization which can be exploited in AFM tunnel junctions to detect the Néel vector. Using first-principles calculations based on density functional …
We present a thorough theoretical assessment of the stability of non-collinear spin arrangements in small palladium clusters. We generally find that ferromagnetic order is always preferred, but that antiferromagnetic and non-collinear configurations of different sorts exist and compete for the first excited isomers. We also show that the relative stability of all these states is rather insensitive to the choice of atomic configuration for the pseudopotential used and to the approximation taken for the exchange and correlation potential. This result stands in stark contrast with the situation f…
Electrical spin-current generation is among the core phenomena driving the field of spintronics. Using {\em ab initio} calculations we show that a room-temperature metallic collinear antiferromagnet RuO$_2$ allows for highly efficient spin-current generation, arising from anisotropically-split bands with conserved up and down spins along the Néel vector axis. The zero net moment antiferromagnet acts as an electrical spin-splitter with a 34$^\circ$ propagation angle between spin-up and spin-down currents. Correspondingly, the spin-conductivity is a factor of three larger than the record value f…
Collinear and non-collinear spin structures of wurtzite phase CoO often appearing in nano-sized samples are investigated using first-principles density functional theory calculations. We examined the total energy of several different spin configurations, electronic structure and the effective magnetic coupling strengths. It is shown that the AF3-type antiferromagnetic ordering is energetically most stable among possible collinear configurations. Further, we found that a novel spiral spin order can be stabilized by including the relativistic spin-orbit coupling and the non-collinearity of spin …
The anomalous Hall effect (AHE) is a well-known fundamental property of ferromagnetic metals, commonly associated with the presence of a net magnetization. Recently, an AHE has been discovered in non-collinear antiferromagnetic (AFM) metals. Driven by non-vanishing Berry curvature of AFM materials with certain magnetic space group symmetry, anomalous Hall conductivity (AHC) is very sensitive to the specific type of magnetic ordering. Here, we investigate the appearance of AHC in antiperovskite GaNMn$_{3}$ as a representative of broader materials family ANMn$_{3}$ (A is a main group element), w…
Ferrimagnets containing several partially compensated magnetic sublattices are considered the most promising materials for all-optical data storage and for ultrafast communications based on spin waves. There are two magnetic phases of the ferrimagnets: collinear and non-collinear ones. Up to now spin dynamics in ferrimagnets has been studied mostly in the collinear state without paying much attention to the kind of the magnetic phase. Here we investigate laser induced ultrafast spin dynamics in a rare-earth iron garnet film in the noncollinear phase as well. We identify a crucial influence of …
