E‐Field Control of Exchange Bias and Deterministic Magnetization Switching in AFM/FM/FE Multiferroic Heterostructures

The coexistence of electrical polarization and magnetization in multiferroic materials provides great opportunities for novel information storage systems. In particular, magnetoelectric (ME) effect can be realized in multi­ferroic composites consisting of both ferromagnetic and ferroelectric phases through a strain mediated interaction, which offers the possibility of electric field (E‐field) manipulation of magnetic properties or vice versa, and enables novel multiferroic devices such as magnetoelectric random access memories (MERAMs). These MERAMs combine the advantages of FeRAMs (ferroelectric random access memories) and MRAMs (magnetic random access memories), which are non‐volatile magnetic bits switchable by electric field (E‐field). However, it has been challenging to realize 180° deterministic switching of magnetization by E‐field, on which most magnetic memories are based. Here we show E‐field modulating exchange bias and for the first time realization of near 180° dynamic magnetization switching at room temperature in novel AFM (antiferromagnetic)/FM (ferromagnetic)/FE (ferroelectric) multiferroic heterostructures of FeMn/Ni₈₀Fe₂₀/FeGaB/PZN‐PT (lead zinc niobate–lead titanate). Through competition between the E‐field induced uniaxial anisotropy and unidirectional anisotropy, large E‐field‐induced exchange bias field‐shift up to $ {{{\Delta H_{ex}}}\over{{H_{ex}}}} = 218\%$ and near 180° deterministic magnetization switching were demonstrated in the exchange‐coupled multiferroic system of FeMn/Ni₈₀Fe₂₀/FeGaB/PZN‐PT. This E‐field tunable exchange bias and near 180° deterministic magnetization switching at room temperature in AFM/FM/FE multiferroic heterostructures paves a new way for MERAMs and other memory technologies.     

Tuning a Binary Ferromagnet into a Multistate Synapse with Spin–Orbit‐Torque‐Induced Plasticity

Ferromagnets with binary states are limited for applications as artificial synapses for neuromorphic computing. Here, it is shown how synaptic plasticity of a perpendicular ferromagnetic layer (FM1) can be obtained when it is interlayer exchange‐coupled by another in‐plane ferromagnetic layer (FM2), where a magnetic field‐free current‐driven multistate magnetization switching of FM1 in the Pt/FM1/Ta/FM2 structure is induced by spin–orbit torque. Current pulses are used to set the perpendicular magnetization state, which acts as the synapse weight, and spintronic implementation of the excitatory/inhibitory postsynaptic potentials and spike timing‐dependent plasticity are demonstrated. This functionality is made possible by the action of the in‐plane interlayer exchange coupling field which leads to broadened, multistate magnetic reversal characteristics. Numerical simulations, combined with investigations of a reference sample with a single perpendicular magnetized Pt/FM1/Ta structure, reveal that the broadening is due to the in‐plane field component tuning the efficiency of the spin–orbit torque to drive domain walls across a landscape of varying pinning potentials. The conventionally binary FM1 inside the Pt/FM1/Ta/FM2 structure with an inherent in‐plane coupling field is therefore tuned into a multistate perpendicular ferromagnet and represents a synaptic emulator for neuromorphic computing, demonstrating a significant pathway toward a combination of spintronics and synaptic electronics.     

Strong Damping‐Like Spin‐Orbit Torque and Tunable Dzyaloshinskii–Moriya Interaction Generated by Low‐Resistivity Pd1−xPtx Alloys

Despite their great promise for providing a pathway for very efficient and fast manipulation of magnetization, spin‐orbit torque (SOT) operations are currently energy inefficient due to a low damping‐like SOT efficiency per unit current bias, and/or the very high resistivity of the spin Hall materials. This work reports an advantageous spin Hall material, Pd_1?xPt_x, which combines a low resistivity with a giant spin Hall effect as evidenced with three independent SOT ferromagnetic detectors. The optimal Pd_0.25Pt_0.75 alloy has a giant internal spin Hall ratio of >0.60 (damping‐like SOT efficiency of ≈0.26 for all three ferromagnets) and a low resistivity of ≈57.5 µΩ cm at a 4 nm thickness. Moreover, it is found that the Dzyaloshinskii–Moriya interaction (DMI), the key ingredient for the manipulation of chiral spin arrangements (e.g., magnetic skyrmions and chiral domain walls), is considerably strong at the Pd_1?xPt_x/Fe_0.6Co_0.2B_0.2 interface when compared to that at Ta/Fe_0.6Co_0.2B_0.2 or W/Fe_0.6Co_0.2B_0.2 interfaces and can be tuned by a factor of 5 through control of the interfacial spin‐orbital coupling via the heavy metal composition. This work establishes a very effective spin current generator that combines a notably high energy efficiency with a very strong and tunable DMI for advanced chiral spintronics and spin torque applications.     

Ultrahigh Tunability of Room Temperature Electronic Transport and Ferromagnetism in Dilute Magnetic Semiconductor and PMN‐PT Single‐Crystal‐Based Field Effect Transistors via Electric Charge Mediation

Multiferroic heterostructures composed of complex oxide thin films and ferroelectric single crystals have aroused considerable interest due to the electrically switchable strain and charge elements of oxide films by the polarization reversal of ferroelectrics. Previous studies have demonstrated that the electric‐field‐control of physical properties of such heterostructures is exclusively due to the ferroelectric domain switching‐induced lattice strain effects. Here, the first successful integration of the hexagonal ZnO:Mn dilute magnetic semiconductor thin films with high performance (111)‐oriented perovskite Pb(Mg_1/3Nb_2/3)O₃‐PbTiO₃ (PMN‐PT) single crystals is reported, and unprecedented charge‐mediated electric‐field control of both electronic transport and ferromagnetism at room temperature for PMN‐PT single crystal‐based oxide heterostructures is realized. A significant carrier concentration‐tunability of resistance and magnetization by ≈400% and ≈257% is achieved at room temperature. The electric‐field controlled bistable resistance and ferromagnetism switching at room temperature via interfacial electric charge presents a potential strategy for designing prototype devices for information storage. The results also disclose that the relative importance of the strain effect and interfacial charge effect in oxide film/ferroelectric crystal heterostructures can be tuned by appropriately adjusting the charge carrier density of oxide films.     

Tailoring Multilevel‐Stable Remanence States in Exchange‐Biased System through Spin‐Orbit Torque

Multilevel remanence states have potential applications in ultra‐high‐density storage and neuromorphic computing. Continuous tailoring of the multilevel remanence states by spin‐orbit torque (SOT) is reported in perpendicularly magnetized Pt/Co/IrMn heterostructures. Double‐biased hysteresis loops with only one remanence state can be tuned from the positively or negatively single‐biased loops by SOT controlled sign of the exchange‐bias field. The remanence states associated with the heights of the sub‐loops are continually changed by tuning the ratio of the positively and negatively oriented ferromagnetic domains. The multilevel storage cells are demonstrated by reading the remanent Hall resistance through changing the sign and/or the magnitude of current pulse. The synaptic plasticity behaviors for neuromorphic computing are also simulated by varying the remanent Hall resistance under the consecutive current pulses. This work demonstrates that SOT is an effective method to tailor the remanence states in the double‐biased heavy metal/ferromagnetic/antiferromagnetic system. The multilevel‐stable remanence states driven by SOT show potential applications in future multilevel memories and neuromorphic computing devices.     

Unveiling the Mechanism of Bulk Spin-Orbit Torques within Chemically Disordered FexPt1-x Single Layers

The recent discovery of spin-orbit torques (SOTs) within magnetic single-layers has attracted attention. However, it remains elusive as to how to understand and how to tune the SOTs. Here, utilizing the single layers of chemically disordered Fe_xPt_1-x, the mechanism of the “unexpected” bulk SOTs is unveiled by studying their dependence on the introduction of a controlled vertical composition gradient and temperature. The bulk dampinglike SOT is found to arise from an imbalanced internal spin current that is transversely polarized and independent of the magnetization orientation. The torque can be strong only in the presence of a vertical composition gradient. The SOT efficiency per electric field is insensitive to temperature but changes sign upon reversal of the orientation of the composition gradient, which is analog to the strain behaviors. These characteristics suggest that the imbalanced internal spin current originates from a bulk spin Hall effect and that the associated inversion asymmetry that allows for a non-zero net torque is most likely a strain non-uniformity induced by the composition gradient. The fieldlike SOT is a relatively small bulk effect compared to the dampinglike SOT. This study points to the possibility of developing low-power single-layer SOT devices by strain engineering.     

热效应对电流驱动磁开关的影响

回顾了热助磁开关理论的发展,包括了Neel-Brown弛豫时间理论和Z.Li小组的有效温度或势垒降低模型,前者很好地解释了磁场驱动磁化矢量翻转的热开关过程,但是不能解释电流驱动磁开关工作机理;后者弥补了Neel-Brown理论的不足,较好地说明了电流驱动的磁开关机制,与实验基本符合。有效温度模型解释了开关电流随温度和测量脉冲宽度的下降;按照不同的脉冲宽度划分了开关的热开关和磁动力学开关工作区。在热开关区,临界电流较小,具有低的功耗,但是器件临界电流随温度而变,工作不够稳定且开关速度较慢;在磁动力学开关区,开关速度高,临界电流不随温度变化,工作稳定,但是功耗较大。实际应用中,应考虑适当的折衷。     

Spatially Resolved Electric‐Field Manipulation of Magnetism for CoFeB Mesoscopic Discs on Ferroelectrics

Electric‐field control of magnetism in ferromagnetic/ferroelectric multiferroic heterostructures is a promising way to realize fast and nonvolatile random‐access memory with high density and low‐power consumption. An important issue that has not been solved is the magnetic responses to different types of ferroelectric‐domain switching. Here, for the first time three types of magnetic responses are reported induced by different types of ferroelectric domain switching with in situ electric fields in the CoFeB mesoscopic discs grown on PMN‐PT(001), including type I and type II attributed to 109°, 71°/180° ferroelectric domain switching, respectively, and type III attributed to a combined behavior of multiferroelectric domain switching. Rotation of the magnetic easy axis by 90° induced by 109° ferroelectric domain switching is also found. In addition, the unique variations of effective magnetic anisotropy field with electric field are explained by the different ferroelectric domain switching paths. The spatially resolved study of electric‐field control of magnetism on the mesoscale not only enhances the understanding of the distinct magnetic responses to different ferroelectric domain switching and sheds light on the path of ferroelectric domain switching, but is also important for the realization of low‐power consumption and high‐speed magnetic random‐access memory utilizing these materials.     

Field-Free Spin-Orbit Torque Switching in Synthetic Ferro and Antiferromagents with Exchange Field Gradient

Deterministic switching of perpendicularly magnetized synthetic antiferromagnets using spin-orbit torque (SOT) usually requires an in-plane auxiliary magnetic field, which limits its practical applications. Here, an exchange field gradient is introduced into perpendicularly magnetized synthetic ferro- and antiferromagnets (SFs and SAFs) through the insertion of a slightly wedged Ru between two thin ferromagnetic layers, which induces field-free switching of perpendicular SFs and SAFs with a switching ratio up to 81% regardless of the nature of the coupling. Temperature-dependent measurement shows a robust field-free switching even at low temperature. The experimental results show that the field-free switching ratio and the effective SOT field are directly related to the exchange field gradient. The theoretical model and numerical simulation indicate that the dynamic noncollinear spin textures induced by the exchange field gradient lead to the field-free switching, while the sign of the exchange field gradient determines the field-free switching polarity. It is further revealed that the SOT efficiency is positively correlated with the antiferromagnetic exchange field for both Ru wedged and non-wedged samples. These results provide a new avenue for simultaneously achieving field-free switching and high SOT efficiency of perpendicularly magnetized SAFs for highly stable, high-density, low-stray-field, and low-power magnetic memory devices.     

Magnetic Anisotropy of Cr7Ni Spin Clusters on Surfaces

The problem of the experimental and theoretical determination of magnetic anisotropy in isolated molecular spin clusters is addressed here. To this end, the case of molecular Cr₇Ni rings sublimated in ultrahigh vacuum conditions and assembled in an ordered fashion on Au(111) surface is addressed and investigated using X‐ray magnetic dichroism (XMCD) and theoretical calculations. Fixing the experimental conditions at a temperature T = 8 K and a magnetic field of 5 T, the angular‐dependence of the dichroic signal reveals an easy‐axis anisotropy for the Ni magnetization along the direction perpendicular to the ring while the magnetization of the whole Cr₇Ni molecule is preferentially aligned within the ring plane. These features are well reproduced by spin Hamiltonian simulations, which reflect the character of the S = 3/2 first excited multiplet, dominating at T = 8 K and 5 T. Density functional theory (DFT) calculations show that local spin orbit interactions determine an easy axis anisotropy at the Ni site while the Cr magnetic moment turns out to be more isotropic. This is the first direct observation of the interplay between the single ion and the overall magnetic anisotropy in complex (polynuclear) molecular systems.     

Revealing Controllable Anisotropic Magnetoresistance in Spin–Orbit Coupled Antiferromagnet Sr2IrO4

Antiferromagnetic spintronics actively introduces new principles of magnetic memory, in which the most fundamental spin‐dependent phenomena, i.e., anisotropic magnetoresistance effects, are governed by an antiferromagnet instead of a ferromagnet. A general scenario of the antiferromagnetic anisotropic magnetoresistance effects mainly stems from the magnetocrystalline anisotropy related to spin–orbit coupling. Here magnetic field driven contour rotation of the fourfold anisotropic magnetoresistance in bare antiferromagnetic Sr₂IrO₄/SrTiO₃ (001) thin films hosting a strong spin–orbit coupling induced J_eff = 1/2 Mott state is demonstrated. Concurrently, an intriguing minimal in the magnetoresistance emerges. Through first principles calculations, the bandgap engineering due to rotation of the Ir isospins is revealed to be responsible for these emergent phenomena, different from the traditional scenario where relatively more conductive state is obtained usually when magnetic field is applied along the magnetic easy axis. These findings demonstrate a new efficient route, i.e., via the novel J_eff = 1/2 state, to realize controllable anisotropic magnetoresistance in antiferromagnetic materials.     

Deterministic Current-Induced Perpendicular Switching in Epitaxial Co/Pt Layers without an External Field

Current-induced spin-orbit torques (SOTs) have emerged as a powerful tool to control magnetic elements and non-uniform magnetic textures such as domain walls and skyrmions. SOT-induced switching of perpendicular magnetization generally requires an external field to break the rotational symmetry of the spin-orbit effective fields responsible for the deterministic reversal. The proposed mechanisms to eliminate this requirement often rely on complex multilayer structures that necessitate laborious optimization in the material and spin transport properties, making them less attractive for applications. Herein, current-induced, external field-free switching of an epitaxial MgO/Pt/Co trilayer with an extremely large perpendicular anisotropy in excess of 3 Tesla is reported. It is found that switching occurs due to the interplay of strong SOTs, local anisotropy fluctuations, and the Dzyaloshinkii-Moriya interaction inherent to this epitaxial system. Given that these layers constitute the base stack of a magnetic tunnel junction, this switching mechanism offers the most technologically viable path toward devices such as field-free SOT-based magnetic random-access memories.     

Magnetoresistive Memory with Ultralow Critical Current for Magnetization Switching

The data writing and thermal stability of information storage are studied theoretically for a magnetic random access memory (MRAM) composed of a magnetic tunnel junction or multilayer exhibiting giant magnetoresistance. The theoretical analysis focuses on the magnetization switching in the “free” layer of a MRAM cell, which is induced by a spin‐polarized current imposing a spin‐transfer torque (STT) on the magnetization. It is shown that the writing current in such an STT‐MRAM reduces dramatically near a spin reorientation transition (SRT) driven by lattice strains and/or surface magnetic anisotropy and even tends to zero under certain conditions. In particular, at the size‐driven SRT in the perpendicular‐anisotropy CoFeB‐MgO tunnel junctions, the critical current densities for magnetization reorientations between the parallel and antiparallel states are expected to fall to low values of about 1.3 × 10⁵ and ?3.3 × 10⁴ A cm^?2. Remarkably, STT‐MRAMs may combine low writing current with very high thermal stability of information storage (retention over 10 years) even at a high density ≈500 Gbit inch^?2.     

Intrinsic Half‐Metallicity in 2D Ternary Chalcogenides with High Critical Temperature and Controllable Magnetization Direction

Searching for 2D ferromagnetic materials with a high critical temperature, large spin polarization, and controllable magnetization direction is a key challenge for their broad applications in spintronics. Here, through a systematic study on a series of 2D ternary chalcogenides with first‐principles calculations, it is demonstrated that a family of experimentally available 2D CoGa₂X₄ (X = S, Se, or Te) are half‐metallic ferromagnets, and they exhibit high critical temperature, fully polarized spin state, and strain‐dependent magnetization direction simultaneously. Following the Goodenough–Kanamori rules, the half‐metallic ferromagnetism of CoGa₂X₄ family is caused by superexchange interaction mediated by Co? X? Co bonds. The half‐metal gaps are large enough (>0.5 eV) to ensure that the half‐metallicity is stable against the spin flipping at room temperature. Magnetocrystalline anisotropy energy calculations indicate that CoGa₂X₄ favor easy plane magnetization. Under achievable biaxial tensile strain (2–6%), the magnetization directions of CoGa₂X₄ can change from in‐plane to out‐of‐plane, providing a route to control the efficiency of spin injection/detection. Further, the critical temperatures T_c of ferromagnetic phase transition for CoGa₂X₄ are close to room temperature. Belonging to the big family of layered AB₂X₄ compounds, the proposed CoGa₂X₄ systems will enrich the available 2D candidates and their heterojunctions for various applications.     

Hybrid Improper Ferroelectricity in Multiferroic Superlattices: Finite‐Temperature Properties and Electric‐Field‐Driven Switching of Polarization and Magnetization

The so‐called hybrid improper ferroelectricity (HIF) mechanism allows to create an electrical polarization by assembling two nonpolar materials within a superlattice. It may also lead to the control of the magnetization by an electric field when these two nonpolar materials are magnetic in nature, which is promising for the design of novel magneto‐electric devices. However, several issues of fundamental and technological importance are presently unknown in these hybrid improper ferroelectrics. Examples include the behaviors of its polarization and dielectric response with temperature, and the paths to switch both the polarization and magnetization under electric fields. Here, an effective Hamiltonian scheme is used to study the multiferroic properties of the model superlattice (BiFeO₃)₁/(NdFeO₃)₁. Along with the development of a novel Landau‐type potential, this approach allows to answer and understand all the aforementioned issues at both microscopic and macroscopic levels. In particular, the polarization and dielectric response are both found to adopt temperature dependences, close to the phase transition, that agree with the behavior expected for first‐order improper ferroelectrics. And most importantly, a five‐state path resulting in the switching of polarization and magnetization under an electric field, via the reversal of antiphase octahedral tiltings, is also identified.     

Substrate‐Dependent Spin–Orbit Coupling in Hybrid Perovskite Thin Films

Solution‐processing hybrid metal halide perovskites are promising materials for developing flexible thin‐film devices. This work reports the substrate effects on the spin–orbit coupling (SOC) in perovskite films through thermal expansion under thermal annealing. X‐ray diffraction (XRD) measurements show that using a flexible polyethylene naphthalate (PEN) substrate introduces a smaller mechanical strain in perovskite MAPbI_3?xCl_x films, as compared to conventional glass substrates. Interestingly, the linear/circular photoexcitation‐modulated photocurrent studies find that decreasing mechanical strain gives rise to a weaker orbit–orbit interaction toward decreasing the SOC in the MAPbI_3?xCl_x films prepared on flexible PEN substrates relative to rigid glass substrates. Simultaneously, decreasing the mechanical strain causes a reduction in the internal magnetic parameter inside the MAPbI_3?xCl_x films, providing further evidence to show that introducing mechanical strain can affect the SOC in hybrid perovskite films upon using flexible substrates toward developing flexible perovskite thin‐film devices. Furthermore, thermal admittance spectroscopy indicates that the trap states are increased in the perovskite films prepared on flexible PEN substrates as compared to glass substrates. Consequently, PEN and rigid glass substrates lead to shorter and longer photoluminescence lifetimes, respectively. Clearly, these findings provide an insightful understanding on substrate effects on optoelectronic properties in flexible perovskite thin‐film devices.     

Ultrafast Photo-Thermal Switching of Terahertz Spin Currents

Dissipationless and scattering-free spin-based terahertz electronics is the futuristic technology for energy-efficient information processing. Femtosecond light pulse provides an ideal pathway for exciting the ferromagnet (FM) out-of-equilibrium, causing ultrafast demagnetization and superdiffusive spin transport at sub-picosecond timescale, giving rise to transient terahertz radiation. Concomitantly, light pulses also deposit thermal energy at short timescales, suggesting the possibility of abrupt change in magnetic anisotropy of the FM that could cause ultrafast photo-thermal switching (PTS) of terahertz spin currents. Here, a single light pulse induced PTS of the terahertz spin current manifested through the phase reversal of the emitted terahertz photons is demonstrated. The switching of the transient spin current is due to the reversal of the magnetization state across the energy barrier of the FM layer. This demonstration opens a new paradigm for on-chip spintronic devices enabling ultralow-power hybrid electronics and photonics fueled by the interplay of charge, spin, thermal, and optical signals.     

Enhancement of Spin–Orbit Torque by Strain Engineering in SrRuO3 Films

Complex oxides with 4d/5d transition metal ions, e.g., SrRuO₃, usually possess strong spin–orbit coupling, which potentially leads to efficient charge-spin interconversion. As the electrical transport property of SrRuO₃ can be readily tuned via structure control, it serves as a platform for studying the manipulation of charge-spin interconversion. Here, a factor of twenty enhancement of spin–orbit torque (SOT) efficiency via strain engineering in a SrRuO₃/Ni₈₁Fe₁₉ bilayer is reported. The results show that an orthorhombic SrRuO₃ leads to a higher SOT efficiency than the tetragonal one. By changing the strain from compressive to tensile in the orthorhombic SrRuO₃, the SOT efficiency can be increased from an average value of 0.04 to 0.89, corresponding to a change of spin Hall conductivity from 27 to 441 × ħ/e (S cm⁻¹). The first-principles calculations show that the intrinsic Berry curvature can give rise to a large spin Hall conductivity (SHC) via the strain control, which is consistent with the experimental observations. The results provide a route to further enhance the SOT efficiency in complex oxide-based heterostructures, which will potentially promote the application of complex oxides in energy-efficient spintronic devices.     

Concentric Sub‐micrometer‐Sized Cables Composed of Ni Nanowires and Sub‐micrometer‐Sized Fullerene Tubes

Highly ordered arrays of submicrometer‐sized coaxial cables composed of submicrometer‐sized C₆₀ and C₇₀ tubes filled with Ni nanowires are successfully prepared by combining a sol–gel method with an electrodeposition process. The wall thickness of the submicrometer‐sized tubes can be adjusted by the concentration of fullerenes and the immersion time. The thermal stability of the submicrometer‐sized C₆₀ tubes is studied by Raman spectroscopy and it is found that these structures can be easily decomposed to form carbon nanotubes at relatively low temperatures (above 573 K) in an alumina template. These novel coaxial cable structures have been characterized by transmission electron microscopy (TEM), high‐resolution TEM (HRTEM), scanning electron microscopy (SEM), field‐emission SEM (FESEM), Raman spectroscopy, elemental mapping, energy dispersive X‐ray (EDX) spectroscopy, X‐ray diffraction (XRD), vibrating sample magnetometer (VSM) experiments, and superconducting quantum interference device (SQUID) measurements. Magnetic measurements show that these submicrometer‐sized cables exhibit enhanced ferromagnetic behavior as compared to bulk nickel. Moreover, submicrometer‐sized C₇₀/Ni cables show uniaxial magnetic anisotropy with the easy magnetic axis being parallel to the long axis of the Ni nanowires. C₇₀/Ni cables also exhibit a new magnetic transition at ca. 10 K in the magnetization–temperature (M–T) curve, which is not observed for the analogous C₆₀/Ni structures. The origin of this transition is not yet clear, but might be related to interactions between the Ni nanowires and C₇₀ molecules. There is no preferred magnetization axis in submicrometer‐sized C₆₀/Ni cables, which implies that the Ni nanocrystals have different packing modes in the two composites. These different crystalline packing modes lead to different magnetic anisotropy in the two composites, although the Ni nanocrystals have the same face‐centered cubic (fcc) structure in both cases.     

Controlling Chiral Spin States of a Triangular‐Lattice Magnet by Cooling in a Magnetic Field

Magnetic materials with a non‐collinear and non‐coplanar arrangement of magnetic moments hosting a nonzero scalar spin‐chirality exhibit unique magnetic and spin‐dependent electronic transport properties. The spin chirality often occurs in materials where competing exchange interactions lead to geometrical frustrations between magnetic moments and to a strong coupling between the crystal lattice and the magnetic structure. These characteristics are particularly strong in Mn‐based antiperovskites where the interactions and chirality can be tuned by substitutional modifications of the crystalline lattice. This study presents evidence for the formation of two unequal chiral spin states in magnetically ordered Mn_3.338Ni_0.651N antiperovskite based on density functional theory calculations and supported by magnetization measurements after cooling in a magnetic field. The existence of two scalar spin‐chiralities of opposite sign and different magnitude is demonstrated by a vertical shift of the magnetic‐field dependent magnetization and Hall effect at low fields and from an asymmetrical magnetoresistivity when the applied magnetic field is oriented parallel or antiparallel to the direction of the cooling field. This opens up the possibility of manipulating the spin chirality for potential use in the emerging field of chiral spintronics.