We report the growth of noncollinear antiferromagnetic (AFM) Mn$_3$Ni$_{0.35}$Cu$_{0.65}$N films and the orientation-dependent anomalous Hall effect (AHE) of (001) and (111) films due to nonzero Berry curvature. We found that post-annealing at 500$^\circ$C can significantly improve the AHE signals, though using the appropriate post-annealing conditions is important. The AHE and magnetization loops show sharp flipping at the coercive field in (111) films, while (001) films are hard to saturate by a magnetic field. The anomalous Hall conductivity of (111) films is an order of magnitude larger than that of (001) films. The present results provide not only a better understanding of the AHE in Mn$_3X$N systems but also further opportunities to study the unique phenomena related to noncollinear AFM.
Antiferromagnetic spintronics is one of the leading candidates for next-generation electronics. Among abundant antiferromagnets, noncollinear antiferromagnets are promising for achieving practical applications due to coexisting ferromagnetic and antiferromagnetic merits. In this perspective, we briefly review the recent progress in the emerging noncollinear antiferromagnetic spintronics from fundamental physics to device applications. Current challenges and future research directions for this field are also discussed.
We have used resonant x-ray diffraction to develop a detailed description of antiferromagnetic ordering in epitaxial superlattices based on two-unit-cell thick layers of the strongly correlated metal LaNiO3. We also report reference experiments on thin films of PrNiO3 and NdNiO3. The resulting data indicate a spiral state whose polarization plane can be controlled by adjusting the Ni d-orbital occupation via two independent mechanisms: epitaxial strain and quantum confinement of the valence electrons. The data are discussed in the light of recent theoretical predictions.
Noncollinear antiferromagnets have promising potential to replace ferromagnets in the field of spintronics as high-density devices with ultrafast operation. To take full advantage of noncollinear antiferromagnets in spintronics applications, it is important to achieve efficient manipulation of noncollinear antiferromagnetic spin. Here, using the anomalous Hall effect as an electrical signal of the triangular magnetic configuration, spin-orbit torque switching with no external magnetic field is demonstrated in noncollinear antiferromagnetic antiperovskite manganese nitride Mn$_3$GaN at room tem…
Combining magnetism with band topology provides various novel phases that are otherwise impossible. Among several cases, noncollinear metallic antiferromagnets can reveal particularly rich topological physics due to their diverse magnetic ground states. However, there are only a few experimental studies due to the lack of suitable materials, especially with triangular lattice antiferromagnets. Here, we report that metallic triangular antiferromagnet Co1/3TaS2 exhibits a substantial anomalous Hall effect (AHE) related to its noncollinear magnetic order. Our first-principles calculations found t…
One of the main bottleneck issues for room-temperature antiferromagnetic spintronic devices is the small signal read-out owing to the limited anisotropic magnetoresistance in antiferromagnets. However, this could be overcome by either utilizing the Berry-curvature-induced anomalous Hall resistance in noncollinear antiferromagnets or establishing tunnel junction devices based on effective manipulation of antiferromagnetic spins. In this work, we demonstrate the giant piezoelectric strain control of the spin structure and the anomalous Hall resistance in a noncollinear antiferromagnetic metal - …
Antiferromagnetic antiperovskites, of the form Mn$_3B$N ($B$ = Ni, Cu, Zn, Sn, Ir, and Pt), have shown an outstanding behavior in which, giant negative thermal expansion and chiral magnetic structures are intertwined. As such, aiming to shed light on the magnetostructural behavior, related to the magnetic ordering and structure of this type of materials, we studied by theoretical first-principles calculations the spin-phonon coupling in the Manganese-based antiperovskite Mn$_3$NiN, as a prototype in the Mn$_3B$N family. We found a strong spin-lattice coupling by means of the understanding of t…
Direct imaging and control of Berry curvature in noncollinear antiferromagnetic single-crystal thin films
University of Wisconsin-Madison（威斯康星大学麦迪逊分校）；University of California, Irvine（加州大学尔湾分校）；University of Nebraska, Lincoln（内布拉斯加大学林肯分校）；University of Oxford（牛津大学）；University College London（伦敦大学学院）；STFC Rutherford Appleton Laboratory（英国科学与技术设施委员会鲁瑟福阿普尔顿实验室）
The antiferromagnet Mn$_5$Si$_3$ has recently attracted attention because a noncollinear spin arrangement has been shown to produce a topological anomalous Hall effect and an inverse magnetocaloric effect. Here we synthesize single crystals of Mn$_5$Si$_3$ using flux growth. We determine the phase diagram through magnetization and measure the magnetoresistance and the Hall effect. We find the collinear and noncollinear antiferromagnetic phases at low temperatures and, in addition, a third magnetic phase, in between the two antiferromagnetic phases which has ferromagnetic character. The latter …
We have investigated the interplay between magnetic and structural degrees of freedom in elemental Mn. The equilibrium volume is shown to depend critically on the magnetic interactions between the Mn atoms. While the standard generalized-gradient-approximation underestimates the equilibrium volume, a more accurate treatment of the effects of electronic localization and magnetism is found to solve this longstanding problem. We capture well the complexity of the large 58 atoms per unit cell $α$-Mn system for the first time, including its charge and spin patterns and the canting of spins with res…
Magnetotransport is at the center of the spintronics. Mn3Sn, an antiferromagnet that has a noncollinear 120° spin order, exhibits large anomalous Hall effect (AHE) at room temperature. But such a behavior has been remained elusive in Mn3Sn films. Here we report the observation of robust AHE up to room temperature in quasi-epitaxial Mn3Sn thin films, prepared by magnetron sputtering. The growth of both (11-20)- and (0001)-oriented Mn3Sn films provides a unique opportunity for comparing AHE in three different measurement configurations. When the magnetic field is swept along (0001) plane, such a…
Noncollinear antiferromagnets with a D0$_{19}$ (space group = 194, P6$_{3}$/mmc) hexagonal structure have garnered much attention for their potential applications in topological spintronics. Here, we report the deposition of continuous epitaxial thin films of such a material, Mn$_{3}$Sn, and characterize their crystal structure using a combination of x-ray diffraction and transmission electron microscopy. Growth of Mn$_{3}$Sn films with both (0001) c-axis orientation and (40$\bar{4}$3) texture is achieved. In the latter case, the thin films exhibit a small uncompensated Mn moment in the basal …
Spin-polarized currents play a key role in spintronics. Recently, it has been found that antiferromagnets with a non-spin-degenerate band structure can efficiently spin-polarize electric currents, even though their net magnetization is zero. Among the antiferromagnetic metals with magnetic space group symmetry supporting this functionality, the noncollinear antiferromagnetic antiperovskites ANMn$_3$ (A = Ga, Ni, Sn, and Pt) are especially promising. This is due to their high Néel temperatures and a good lattice match to perovskite oxide substrates, offering possibilities of high structural qua…
We propose a new type of spin-valley locking (SVL), named $\textit{C}$-paired SVL, in antiferromagnetic systems, which directly connects the spin/valley space with the real space, and hence enables both static and dynamical controls of spin and valley to realize a multifunctional antiferromagnetic material. The new emergent quantum degree of freedom in the $\textit{C}$-paired SVL is comprised of spin-polarized valleys related by a crystal symmetry instead of the time-reversal symmetry. Thus, both spin and valley can be accessed by simply breaking the corresponding crystal symmetry. Typically, …
Predictions of the anisotropic magnetic susceptibility chi below the antiferromagnetic (AFM) ordering temperatures TN of local moment Heisenberg AFMs have been made previously using molecular field theory (MFT) but are very limited in their applicability. Here a MFT calculation of chi(T<=TN) is presented for a wide variety of collinear and noncollinear Heisenberg AFMs containing identical crystallographically equivalent spins without recourse to magnetic sublattices. The results are expressed in terms of directly measurable experimental parameters and are fitted with no adjustable parameters t…
Non-collinear antiferromagnetic materials have received dramatically increasing attention in the field of spintronics as their exotic topological features such as the Berry-curvature-induced anomalous Hall effect and possible magnetic Weyl states could be utilized in future topological antiferromagnetic spintronic devices. In this work, we report the successful integration of the antiferromagnetic metal Mn3Sn thin films onto ferroelectric oxide PMN-PT. By optimizing growth, we realized the large anomalous Hall effect with small switching magnetic fields of several tens mT fully comparable to t…
The anomalous Nernst effect (ANE) - the generation of a transverse electric voltage by a longitudinal heat current in conducting ferromagnets or antiferromagnets - is an appealing approach for thermoelectric power generation in spin caloritronics. The ANE in antiferromagnets is particularly convenient for the fabrication of highly efficient and densely integrated thermopiles as lateral configurations of thermoelectric modules increase the coverage of heat source without suffering from the stray fields that are intrinsic to ferromagnets. In this work, using first-principles calculations togethe…
Our world is composed of various materials with different structures, where spin structures have been playing a pivotal role in spintronic devices of the contemporary information technology. Apart from conventional collinear spin materials such as collinear ferromagnets and collinear antiferromagnetically coupled materials, noncollinear spintronic materials have emerged as hot spots of research attention owing to exotic physical phenomena. In this Review, we firstly introduce two types noncollinear spin structures, i.e., the chiral spin structure that yields real-space Berry phases and the cop…
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 …
$\mathrm{MnBi_2Te_4}$ has recently been established as an intrinsic antiferromagnetic (AFM) topological insulator and predicted to be an ideal platform to realize quantum anomalous Hall (QAH) insulator and axion insulator states. We performed comprehensive studies on the structure, nontrivial surface state and magnetotransport properties of this material. Our results reveal an intrinsic anomalous Hall effect arising from a non-collinear spin structure for the magnetic field parallel to the $c$-axis. We also observed remarkable negative magnetoresistance under arbitrary field orientation below …
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…
Ultrafast optical pump-probe spectroscopy is used to reveal the coexistence of coupled antiferromagnetic/ferroelectric and ferromagnetic orders in multiferroic TbMnO3 films through their time domain signatures. Our observations are explained by a theoretical model describing the coupling between reservoirs with different magnetic properties. These results can guide researchers in creating new kinds of multiferroic materials that combine coupled ferromagnetic, antiferromagnetic and ferroelectric properties in one compound.
The van der Waals material CeOI is predicted to be a layered antiferromagnetic Mott insulator by DFT+U calculation. We successfully grow the CeOI films down to monolayer on graphene/6H-SiC(0001) substrate by using molecular beam epitaxy. Films are studied by {\it in-situ} scanning tunneling microscopy and spectroscopy, which shows a band gap of 4.4 eV. A metallic phase with composition unidentified also exists. This rare earth oxyhalide adds a new member to the two-dimensional magnetic materials.
We investigate the intrinsic magnon spin current in a noncollinear antiferromagnetic insulator. We introduce a definition of the magnon spin current in a noncollinear antiferromagnet and find that it is in general non-conserved, but for certain symmetries and spin polarizations the averaged effect of non-conserving terms can vanish. We formulate a general linear response theory for magnons in noncollinear antiferromagnets subject to a temperature gradient and analyze the effect of symmetries on the response tensor. We apply this theory to single-layer potassium iron jarosite KFe$_3$(OH)$_6$(SO…
We report electrical current switching of noncollinear antiferromagnetic (AFM) Mn$_3$GaN/Pt bilayers at room temperature. The Hall resistance of these bilayers can be manipulated by applying a pulse current of $1.5\times10^6$~A/cm$^2$, whereas no significant change is observed up to $\sim10^8$~A/cm$^2$ in Mn$_3$GaN single films, indicating that the Pt layer plays an important role. In comparison with ferrimagnetic Mn$_3$GaN/Pt bilayers, a lower electrical current switching of noncollinear AFM Mn$_3$GaN is demonstrated, with a critical current density two orders of magnitude smaller. Our result…
Exchange bias has been studied in a series of La2/3Ca1/3MnO3 / La1/3Ca2/3MnO3 bilayers grown on (001) SrTiO3 substrates by ozone-assisted molecular beam epitaxy. The high crystalline quality of the samples and interfaces has been verified using high-resolution X-ray diffractometry and Z-contrast scanning transmission electron microscopy with electron energy loss spectroscopy. The dependence of exchange bias on the thickness of the antiferromagnetic layer has been investigated. A critical value for the onset of the hysteresis loop shift has been determined. An antiferromagnetic anisotropy const…
We report coupling between magnetic and electric orders for antiferromagnetic polycrystalline FeVO4 in which magnetism-induced polarization has been recently found in noncollinear antiferromagnetic state below the second antiferromagnetic phase transition at TN2=15.7K. In this low symmetry phase space group P-1, the magnetic field dependence of electric polarization evidences a clear magnetoelectric coupling in the noncollinear spin-configured antiferromagnetic phase. The discontinuity of magnetodielectric effect observed at the vicinity of the polar to nonpolar transition evidences competitio…
MnN is a centrosymmetric collinear antiferromagnet belonging to the transition metal nitride family with a high Neel temperature, a low anisotropy field, and a large magnetic moment per Mn atom. Despite several recent experimental and theoretical studies, the spin symmetry (magnetic point group) and magnetic domain structure of the material remain unknown. In this work, we use optical second harmonic generation (SHG) to study the magnetic structure of thin epitaxially-grown single-crystal (001) MnN films. Our work shows that spin moments in MnN are tilted away from the [001] direction and the …
We present a comprehensive theory of the magnetic phases in twisted bilayer Cr-trihalides through a combination of first-principles calculations and atomistic simulations. We show that the stacking-dependent interlayer exchange leads to an effective moiré field that is mostly ferromagnetic with antiferromagnetic patches. A wide range of noncollinear magnetic phases can be stabilized as a function of the twist angle and Dzyaloshinskii-Moriya interaction as a result of the competing interlayer antiferromagnetic coupling and the energy cost for forming domain walls. In particular, we demonstrate …
We report a longitudinal spin Seebeck effect (SSE) study in epitaxially grown FeF2(110) antiferromagnetic (AFM) thin films with strong uniaxial anisotropy over the temperature range of 3.8 - 250 K. Both the magnetic field- and temperature-dependent SSE signals below the Néel temperature (TN=70 K) of the FeF2 films are consistent with a theoretical model based on the excitations of AFM magnons without any net induced static magnetic moment. In addition to the characteristic low-temperature SSE peak associated with the AFM magnons, there is another SSE peak at TN which extends well into the para…
Recent study (Yuan et. al., Phys. Rev. B 102, 014422 (2020)) revealed a SOC-independent spin splitting and spin polarization effect induced by antiferromagnetic ordering which do not necessarily require breaking of inversion symmetry or the presence of SOC, hence can exist even in centrosymmetric, low-Z light element compounds, considerably broadening the material base for spin polarization. In the present work we develop the magnetic symmetry conditions enabling such effect, dividing the 1651 magnetic space groups into 7 different spin splitting prototypes (SST-1 to SST-7). We use the 'Invers…
FeSn is a topological semimetal (TSM) and kagome antiferromagnet (AFM) composed of alternating Fe3Sn kagome planes and honeycomb Sn planes. This unique structure gives rise to exotic features in the band structures such as the coexistence of Dirac cones and flatbands near the Fermi level, fully spin-polarized 2D surface Dirac fermions, and the ability to open a large gap in the Dirac cone by reorienting the Néel vector. In this work, we report the synthesis of high quality epitaxial (0001) FeSn films by magnetron sputtering. Using FeSn/Py heterostructures, we show a large exchange bias effect …
We have employed Soft and Hard X-ray Resonant Magnetic Scattering and Polarised Neutron Diffraction to study the magnetic interface and the bulk antiferromagnetic domain state of the archetypal epitaxial Ni$_{81}$Fe$_{19}$(111)/CoO(111) exchange biased bilayer. The combination of these scattering tools provides unprecedented detailed insights into the still incomplete understanding of some key manifestations of the exchange bias effect. We show that the several orders of magnitude difference between the expected and measured value of exchange bias field is caused by an almost anisotropic in-pl…
Noncollinear antiferromagnets have recently been attracting considerable interest partly due to recent surprising discoveries of the anomalous Hall effect (AHE) in them and partly because they have promising applications in antiferromagnetic spintronics. Here we study the anomalous Nernst effect (ANE), a phenomenon having the same origin as the AHE, and also the spin Nernst effect (SNE) as well as AHE and the spin Hall effect (SHE) in noncollinear antiferromagnetic Mn$_3X$ ($X$ = Sn, Ge, Ga) within the Berry phase formalism based on {\it ab initio} relativistic band structure calculations. For…
We report direct imaging of boundary magnetization associated with antiferromagnetic domains in magnetoelectric epitaxial Cr2O3 thin films using diamond nitrogen vacancy microscopy. We found a correlation between magnetic domain size and structural grain size which we associate with the domain formation process. We performed field cooling, i.e., cooling from above to below the Néel temperature in the presence of magnetic field, which resulted in the selection of one of the two otherwise degenerate 180 degree domains. Lifting of such a degeneracy is achievable with a magnetic field alone due to…
FeSn is a room-temperature antiferromagnet expected to host Dirac fermions in its electronic structure. The interplay of magnetic degree of freedom and the Dirac fermions makes FeSn an attractive platform for spintronics and electronic devices. While stabilization of thin film FeSn is needed for the development of such devices, there exist no previous report of epitaxial growth of single crystalline FeSn. Here we report the realization of epitaxial thin films of FeSn (001) grown by molecular beam epitaxy on single crystal SrTiO$_{3}$ (111) substrates. By combining X-ray diffraction, electrical…
The magnetic properties of Zn$_{1-x}$Co$_x$O ($x=0.07$ and 0.10) thin films, which were homo-epitaxially grown on a ZnO(0001) substrates with varying relatively high oxygen pressure, have been investigated using x-ray magnetic circular dichroism (XMCD) at Co $2p$ core-level absorption edge. The line shapes of the absorption spectra are the same in all the films and indicate that the Co$^{2+}$ ions substitute for the Zn sites. The magnetic-field and temperature dependences of the XMCD intensity are consistent with the magnetization measurements, indicating that except for Co there are no additi…
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…
Spintronic phenomena to date have been established in magnets with collinear moments, where the spin injection through the spin Seebeck effect (SSE) is always along the out-of-plane direction. Here, we report the observation of a vector SSE in a noncollinear antiferromagnet (AF) LuFeO$_3$, where temperature gradient along the out-of-plane and also the in-plane directions can both inject a pure spin current and generate a voltage in the heavy metal via the inverse spin Hall effect (ISHE). We show that the thermovoltages are due to the magnetization from canted spins in LuFeO$_3$. Furthermore, i…
Based on first-principles calculations, we investigated the topological transport properties of Mn$_3$GaN with coplanar noncollinear magnetic structures. The intrinsic anomalous Hall conductivity (IAHC) displays a significant dependence with respect to the in-plane magnetization direction between the $Γ_{5g}$ and $Γ_{4g}$ magnetic configurations, where large anomalous Nernst effect (ANE) can be induced by tailoring the magnetization direction. Moreover, we observed strong piezospintronic effect in Mn$_3$GaN, where large IAHC can be induced by moderate epitaxial strain. Symmetry analysis reveal…
We study magnon-magnon interactions and their effects in a spiral magnet induced by combination of an antiferromagnetic Heisenberg interaction and a Dzyaloshinsky-Moriya interaction. We show that the main effect of magnon-magnon interactions on low-energy magnons is to renormalize the coefficient of energy dispersion. This could explain why some experiments are consistent with the noninteracting theory. We also show that although the magnon-magnon interactions induce the pair amplitude for low-energy magnons, its effect on the excitation energy is negligible. This suggests that for magnons the…
We prepare the high quality epitaxial MgO(001)[100]/Pt(001)[100]/NiO(001)[100]/FeNi/SiO2 films to investigate the spin transport in the NiO antiferromagnetic insulator. The ferromagnetic resonance measurements of the FeNi under a spin current injection from the Pt by the spin Hall effect revealed the change of the ferromagnetic resonance linewidth depending on the amount of the spin current injection. The results can be interpreted that there is an angular momentum transfer through the NiO. A high efficient angular momentum transfer we observed in the epitaxial NiO can be attributed to the wel…
