Ferrimagnetic alloy thin films that exhibit perpendicular (out-of-plane) magnetic anisotropy (PMA) with low saturation magnetization, such as GdCo and Mn4N, were predicted to be favorable for hosting small Neel skyrmions for room temperature applications. Due to the exponential decay of interfacial Dzyaloshinskii-Moriya interaction (DMI) and the limited range of spin-orbit-torques, which can be used to drive skyrmion motion, the thickness of the ferrimagnetic layer has to be small, preferably under 20 nm. While there are examples of sub-20 nm, rare earth-transition metal (RE-TM), ferrimagnetic thin films fabricated by sputter deposition, to date rare-earth-free sub-20 nm Mn4N films with PMA have only been reported to be achieved by molecular beam epitaxy, which is not suitable for massive production. Here we report the successful thermal growth of sub-20 nm Mn4N films with PMA at 400-450 °C substrate temperatures on MgO substrates by reactive sputtering. The Mn4N films were achieved by reducing the surface roughness of MgO substrate through a high-temperature vacuum annealing process. The optimal films showed low saturation magnetization (Ms = 43 emu/cc), low magnetic anisotropy energy (0.7 Merg/cc), and a remanent magnetization to saturation magnetization ratio (Mr/Ms) near 1 at room temperature. Preliminary ab-initio density functional theory (DFT) calculations have confirmed the ferrimagnetic ground state of Mn4N grown on MgO. The magnetic properties, along with the high thermal stability of Mn4N thin films in comparison with RE-TM thin films, provide the platform for future studies of practical skyrmion-based spintronic materials.
In this review we introduce computer modelling and simulation techniques which are used for ferrimagnetic materials. We focus on models where thermal effects are accounted for, atomistic spin dynamics and finite temperature macrospin approaches. We survey the literature of two of the most commonly modelled ferrimagnets in the field of spintronics--the amorphous alloy GdFeCo and the magnetic insulator yttrium iron garnet. We look at how generic models and material specific models have been applied to predict and understand spintronic experiments, focusing on the fields of ultrafast magnetisatio…
Spintronics, which is the basis of a low-power, beyond-CMOS technology for computational and memory devices, remains up to now entirely based on critical materials such as Co, heavy metals and rare-earths. Here, we show that Mn4N, a rare-earth free ferrimagnet made of abundant elements, is an exciting candidate for the development of sustainable spintronics devices. Mn4N thin films grown epitaxially on SrTiO3 substrates possess remarkable properties, such as a perpendicular magnetisation, a very high extraordinary Hall angle (2%) and smooth domain walls, at the millimeter scale. Moreover, doma…
In recent years, antiferromagnetic spintronics has received much attention since ideal antiferromagnets do not produce stray fields and are much more stable to external magnetic fields compared to materials with net magnetization. Akin to antiferromagnets, compensated ferrimagnets have zero net magnetization but have the potential for large spin-polarization and strong out of plane magnetic anisotropy, and, hence, are ideal candidates for high density memory applications. Here, we demonstrate that a fully compensated magnetic state with a tunable magnetic anisotropy is realized in Mn-Pt-Ga bas…
Ferromagnetic materials dominate as the magnetically active element in spintronic devices, but come with drawbacks such as large stray fields, and low operational frequencies. Compensated ferrimagnets provide an alternative as they combine the ultrafast magnetization dynamics of antiferromagnets with a ferromagnet-like spin-orbit-torque (SOT) behavior. However to use ferrimagnets in spintronic devices their advantageous properties must be retained also in ultrathin films (t < 10 nm). In this study, ferrimagnetic Gdx(Fe87.5Co12.5)1-x thin films in the thickness range t = 2-20 nm were grown on h…
Magnetic insulators with strong perpendicular magnetic anisotropy (PMA) play a key role in exploring pure spin current phenomena and developing ultralow-dissipation spintronic devices, thereby it is highly desirable to develop new material platforms. Here we report epitaxial growth of La2/3Sr1/3MnO3 (LSMO)-SrIrO3 (SIO) composite oxide films (LSMIO) with different crystalline orientations fabricated by sequential two-target ablation process using pulsed laser deposition. The LSMIO films exhibit high crystalline quality with homogeneous mixture of LSMO and SIO at atomic level. Ferrimagnetic and …
Compensation-Like Temperature and Spin-Flip Switch in Strained Thulium Iron Garnet Thin Films: Tuning Sublattice Interactions for Ferrimagnetic Spintronics
Multiferroic materials, in which ferroelectric and magnetic ordering coexist, are of fundamental interest for the development of novel memory devices that allow for electrical writing and non-destructive magnetic readout operation. The great challenge is to create room temperature multiferroic materials with strongly coupled ferroelectric and ferromagnetic (or ferrimagnetic) orderings. BiFeO3 has been the most heavily investigated single-phase multiferroic to date due to the coexistence of its magnetic order and ferroelectric order at room temperature. However, there is no net magnetic moment …
The research into insulating ferrimagnetic garnets has gained enormous momentum in the past decade. This is partly due to the improvement in the techniques to grow high-quality ultrathin films with desirable properties and the advances in understanding the spin transport within the ferrimagnetic garnets and through their interfaces with conducting materials. In recent years, we have seen remarkable progress in controlling the magnetization state of ferrimagnetic garnets by electrical means in suitable heterostructures and device architectures. These advances have readily placed ferrimagnetic g…
Ferrimagnetic Skyrmions in a Tetragonal Mn1.9Co0.1Sb Single Crystal at Room Temperature
Anhui University（安徽大学）；Wuhan University of Technology（武汉理工大学）；High Magnetic Field Laboratory, HFIPS, Chinese Academy of Sciences（中国科学院合肥物质科学研究院强磁场科学中心）
The use of epitaxial layers for domain wall-based spintronic applications is often hampered by the presence of pinning sites. Here, we show that when depositing Mn4N(10 nm) epitaxial films, the replacement of MgO(001) by SrTiO3(001) substrates allows minimizing the misfit, and to obtain an improved crystalline quality, a sharper switching, a full remanence, a high anisotropy and remarkable millimeter-sized magnetic domains, with straight and smooth domain walls. In a context of rising interest for current-induced domain wall motion in rare
Determining the angular momentum compensation temperature of ferrimagnets is an important step towards ferrimagnetic spintronics, but is not generally easy to achieve it experimentally. We propose a way to estimate the angular momentum compensation temperature of ferrimagnets. We find a linear relation between the compensation temperatures of the magnetization and angular momentum in GdFeCo ferrimagnetic materials, which is proved by theoretically as well as experimentally. The linearity comes from the power-law criticality and is governed by the Curie temperature and the Landé g factors of th…
We predict through our first-principles calculations that four double perovskite oxides of Bi2ABO6 (AB = FeMo, MnMo, MnOs, CrOs) are half-metallic ferrimagnets. Our calculated results shows that the four optimized structures have negative formation energy, from -0.42 to -0.26 eV per formula unit, which implies that they could probably be realized. In the case of Bi2FeMoO6, the half-metallic gap and Curie temperature are predicted to reach to 0.71 eV and 650 K, respectively, which indicates that high spin polarization could be kept at high temperatures far beyond room temperature. It is believe…
Owing to the experimental discovery of magnetic skyrmions stabilized by the Dzyaloshinskii-Moriya and/or dipolar interactions in thin films, there is a recent upsurge of interest in magnetic skyrmions with antiferromagnetic spins in order to overcome the fundamental limitations inherent with skyrmions in ferromagnetic materials. Here, we report on the observation of compact ferrimagnetic skyrmions for the class of amorphous alloys consisting of 4f rare-earth and 3d transition-metal elements with perpendicular magnetic anisotropy, using a DyCo$_3$ film, that are identified by combining x-ray ma…
Despite the potential advantages of information storage in antiferromagnetically coupled materials, it remains unclear whether one can control the magnetic moment orientation efficiently because of the cancelled magnetic moment. Here, we report spin-orbit torque induced magnetization switching of ferrimagnetic Co1-xTbx films with perpendicular magnetic anisotropy. Current induced switching is demonstrated in all of the studied film compositions, including those near the magnetization compensation point. The spin-orbit torque induced effective field is further quantified in the domain wall moti…
Synthesizing half-metallic fully-compensated ferrimagnets that form in the inverse Heusler phase could lead to superior spintronic devices. These materials would have high spin polarization at room temperature with very little fringing magnetic fields. Previous theoretical studies indicated that Cr2CoAl should form in a stable inverse Heusler lattice due to its low activation energy. Here, stoichiometric Cr2CoAl samples were arc-melted and annealed at varying temperatures, followed by studies of their structural and magnetic properties. High-resolution synchrotron X-ray diffraction revealed a …
Recently, theorists have predicted many materials with a low magnetic moment and large spin-polarization for spintronic applications. These compounds are predicted to form in the inverse Heusler structure, however, many of these compounds have been found to phase segregate. In this study, ordered Cr2CoGa thin films were synthesized without phase segregation using molecular beam epitaxy. The present as-grown films exhibit a low magnetic moment from antiferromagnetically coupled Cr and Co atoms as measured with SQUID magnetometry and soft X-ray magnetic circular dichroism. Electrical measurement…
Magnetic skyrmions are swirling magnetic textures with novel characteristics suitable for future spintronic and topological applications. Recent studies confirmed the room-temperature stabilization of skyrmions in ultrathin ferromagnets. However, such ferromagnetic skyrmions show undesirable topological effect, the skyrmion Hall effect, which leads to their current-driven motion towards device edges, where skyrmions could easily be annihilated by topographic defects. Recent theoretical studies have predicted enhanced current-driven behaviour for antiferromagnetically exchange-coupled skyrmions…
Magnon-polarons are coherently mixed quasiparticles that originate from the strong magnetoelastic coupling of lattice vibrations and spin waves in magnetic-ordered materials. Recently, magnon-polarons have attracted a lot of attention since they provide a powerful tool to manipulate magnons, which is essential for magnon-based spintronic devices. In this work, we report the experimental observation of facet-dependent magnon-polarons in epitaxial ferrimagnetic Fe3O4 thin films via spin Seebeck effect measurement. The critical magnetic fields for the magnon-polarons in the (110)- and (100)-orien…
We report on an element- and time-resolved investigation of femtosecond laser induced ultrafast dynamics of 3d and 4f spins in a ferrimagnetic Co80Dy20 alloy as a function of temperature. We observe an increase of the Co3d characteristic demagnetization time and a decrease of the Dy4f demagnetization time when the temperature is approaching the Curie temperature. It suggests that the critical slowing down regime, which affects the laser induced ultrafast dynamics in pure 3d transition metals and 4f rare-earth ferromagnetic layers, vanishes for the Dy sublattice in the CoDy alloy, in line with …
Anomalous hysteresis loops of ferrimagnetic amorphous alloys in high magnetic field and in the vicinity of the compensation temperature have so far been explained by sample inhomogeneities. We obtain H-T magnetic phase diagram for ferrimagnetic GdFeCo alloy using a two-sublattice model in the paramagnetic rare-earth ion approximation and taking into account rare-earth (Gd) magnetic anisotropy. It is shown that if the magnetic anisotropy of the $f$-sublattice is larger than that of the $d$-sublattice, the tricritical point can be at higher temperature than the compensation point. The obtained p…
Electrical manipulation of magnetism via spin-orbit torques (SOTs) promises efficient spintronic devices. In systems comprising magnetic insulators and heavy metals, SOTs have started to be investigated only recently, especially in systems with interfacial Dzyaloshinskii-Moriya interaction (iDMI). Here, we quantitatively study the SOT efficiency and iDMI in a series of gadolinium gallium garnet (GGG) / thulium iron garnet (TmIG) / platinum (Pt) heterostructures with varying TmIG and Pt thicknesses. We find that the non-monotonic SOT efficiency as a function of the magnetic layer thickness is n…
This work demonstrates dramatically modified spin dynamics of magnetic insulator (MI) by the spin-momentum locked Dirac surface states of the adjacent topological insulator (TI) which can be harnessed for spintronic applications. As the Bi-concentration x is systematically tuned in 5 nm thick (BixSb1-x)2Te3 TI film, the weight of the surface relative to bulk states peaks at x = 0.32 when the chemical potential approaches the Dirac point. At this concentration, the Gilbert damping constant of the precessing magnetization in 10 nm thick Y3Fe5O12 MI film in the MI/TI heterostructures is enhanced …
Magnetic topological quantum materials have attracted great attention due to their exotic topological quantum physics induced by the interplay among crystalology, magnetism, and topology, which is of profound importance to fundamental research and technology applications. However, limited materials are experimentally available, most of whom are realized by magnetic impurity doping or heterostructural constructions. In this work, based on the first-principles calculations, we predict that double perovskite Ba2CdReO6 is an intrinsic ferromagnetic topological semi-half-metal, while the ferrimagne…
The evolution of chiral spin structures is studied in ferrimagnet Ta/Ir/Fe/GdFeCo/Pt multilayers as a function of temperature using scanning electron microscopy with polarization analysis (SEMPA). The GdFeCo ferrimagnet exhibits pure right-hand Néel-type domain wall (DW) spin textures over a large temperature range. This indicates the presence of a negative Dzyaloshinskii-Moriya interaction (DMI) that can originate from both the top Fe/Pt and the Co/Pt interfaces. From measurements of the DW width, as well as complementary magnetic characterization, the exchange stiffness as a function of temp…
Skyrmions and antiskyrmions are topologically protected spin structures with opposite topological charge. Particularly in coexisting phases, these two types of magnetic quasi-particles may show fascinating physics and potential for spintronic devices. While skyrmions are observed in a wide range of materials, until now antiskyrmions were exclusive to materials with D2d symmetry. In this work, we show first and second-order antiskyrmions stabilized by magnetic dipole-dipole interaction in Fe/Gd-based multilayers. We modify the magnetic properties of the multilayers by Ir insertion layers. Using…
The manipulation of magnetism with a gate voltage is expected to lead the way towards the realization of energy-efficient spintronics devices and high-performance magnetic memories. Exploiting magneto-ionic effects under micro-patterned electrodes in solid-state devices adds the possibility to modify magnetic properties locally, in a non-volatile and reversible way. Tuning magnetic anisotropy, magnetization and Dzyaloshinskii-Moriya interaction allows modifying at will the dynamics of non trivial magnetic textures such as skyrmions and chiral domain walls in magnetic race tracks. In this work,…
Interfacial mixing of elements is a well-known phenomenon found in thin film deposition. For thin-film magnetic heterostructures, interfacial compositional inhomogeneities can have drastic effects on the resulting functionalities. As such, care must be taken to characterize the compositional and magnetic properties of thin films intended for device use. Recently, ferrimagnetic Mn$_4$N thin films have drawn considerable interest due to exhibiting perpendicular magnetic anisotropy, high domain-wall mobility, and good thermal stability. In this study, we employed X-ray photoelectron spectroscopy …
Antiferromagnetic spintronics is an emerging research field which aims to utilize antiferromagnets as core elements in spintronic devices. A central motivation toward this direction is that antiferromagnetic spin dynamics is expected to be much faster than ferromagnetic counterpart because antiferromagnets have higher resonance frequencies than ferromagnets. Recent theories indeed predicted faster dynamics of antiferromagnetic domain walls (DWs) than ferromagnetic DWs. However, experimental investigations of antiferromagnetic spin dynamics have remained unexplored mainly because of the immunit…
Using photo-emission electron microscopy with X-ray magnetic circular dichroism as a contrast mechanism, new insights into the all-optical magnetization switching (AOS) phenomenon in GdFe based rare-earth transition metal ferrimagnetic alloys are provided. From a sequence of static images taken after single linearly polarized laser pulse excitation, the repeatability of AOS can be measured with a correlation coefficient. It is found that low coercivity enables thermally activated domain wall motion, limiting in turn the repeatability of the switching. Time-resolved measurement of the magnetiza…
We report the structural, magnetic, and interfacial spin transport properties of epitaxial terbium iron garnet (TbIG) ultrathin films deposited by magnetron sputtering. High crystallinity was achieved by growing the films on gadolinium gallium garnet (GGG) substrates either at high temperature, or at room temperature followed by thermal annealing, above 750 °C in both cases. The films display large perpendicular magnetic anisotropy (PMA) induced by compressive strain, and tunable structural and magnetic properties through growth conditions or the substrate lattice parameter choice. The ferrima…
We investigate the Gilbert damping parameter for rare earth (RE)-transition metal (TM) ferrimagnets over a wide temperature range. Extracted from the field-driven magnetic domain-wall mobility, the Gilbert damping parameter was as low as 0.0072 and was almost constant across the angular momentum compensation temperature, starkly contrasting previous predictions that the Gilbert damping parameter should diverge at the angular momentum compensation temperature due to vanishing total angular momentum. Thus, magnetic damping of RE-TM ferrimagnets is not related to the total angular momentum but is…
We measured the spin-orbit torques (SOTs), current-induced switching, and domain wall (DW) motion in synthetic ferrimagnets consisting of Co/Tb layers with differing stacking order grown on a Pt underlayer. We find that the SOTs, magnetic anisotropy, compensation temperature and SOT-induced switching are highly sensitive to the stacking order of Co and Tb and to the element in contact with Pt. Our study further shows that Tb is an efficient SOT generator when in contact with Co, such that its position in the stack can be adjusted to generate torques additive to those generated by Pt. With opti…
Recently, two-dimensional materials and nanoparticles with robust ferromagnetism are even of great interest to explore basic physics in nanoscale spintronics. More importantly, room-temperature magnetic semiconducting materials with high Curie temperature is essential for developing next-generation spintronic and quantum computing devices. Here, we develop a theoretical model on the basis of density functional theory calculations and the Ruderman-Kittel-Kasuya-Yoshida theory to predict the thermal stability of two-dimensional magnetic materials. Compared with other rare-earth (dysprosium (Dy) …
Thermal Evolution of Skyrmions in Synthetic Ferrimagnets of Co/Gd Heterostructure for Topological Spintronic Applications
National Institute of Science Education and Research (NISER)（印度科学教育研究所）；Homi Bhabha National Institute (HBNI)（霍米·巴巴国立大学）；Indian Institute of Science Education and Research (IISER) Mohali（印度科学教育研究学院莫哈利分校）；Durham University（杜伦大学）
Nowdays, multiferroic materials with magnetoelectric coupling have many real-world applications in the fields of novel memory devices. It is challenging is to create multiferroic materials with strongly coupled ferroelectric and ferrimagnetic orderings at room temperature. The single crystal of ferric selenide (Fe3Se4) shows type-II multiferroic due to the coexistence of ferroelectric as well as magnetic ordering at room temperature. We have investigated the lattice instability, electronic structure, ferroelectric, ferrimagnetic ordering and transport properties of ferroelectric metal Fe3Se4. …
The ability to tune the competition between the in-plane and out-of-plane orientation of magnetization provides a means to construct thermal sensors with a sharp spin re-orientation transition at specific temperatures. We have observed such a tuneable, temperature driven spin re-orientation in structurally amorphous, ferrimagnetic rare earth-transition metal (RE-TM) alloy thin films using scanning transmission X-ray microscopy (STXM) and magnetic measurements. The nature of the spin re-orientation transition in FeGd can be fully explained by a non-equilibrium, nanoscale modulation of the chemi…
Ferrimagnets, which contain the advantages of both ferromagnets (detectable moments) and antiferromagnets (ultrafast spin dynamics), have recently attracted great attention. Here we report the optimization of epitaxial growth of a tetragonal perpendicularly magnetized ferrimagnet Mn2Ga on MgO. Electrical transport, magnetic properties and the anomalous Hall effect (AHE) were systematically studied. Furthermore, we successfully integrated high-quality epitaxial ferrimagnetic Mn2Ga thin films onto ferroelectric PMN-PT single crystals with a MgO buffer layer. It was found that the AHE of such a f…
Ultrafast laser-induced magnetic switching in rare earth, transition metal ferrimagnetic alloys has recently been reported to occur by ultrafast heating alone. Using atomistic simulations and a ferrimagnetic Landau-Lifshitz-Bloch formalism, we demonstrate that for switching to occur it is necessary that angular momentum is transferred from the longitudinal to transverse magnetization components. This dynamical path leads to magnetization switching and subsequent ultrafast precession caused by the inter-sublattice exchange field on the nanoscale.
Indian Institute of Technology Palakkad（印度理工学院帕拉卡德分校）；Indian Institute of Technology Bombay（印度理工学院孟买分校）；Indian Institute of Technology Kharagpur（印度理工学院卡拉格普尔分校）；Central University of Haryana（哈里亚纳邦中央大学）；Indian Institute of Science Education and Research, Thiruvananthapuram（印度科学教育与研究机构，特鲁万得琅校区）；UGC-DAE Consortium for Scientific Research（UGC-DAE科学研究联盟）；Bhabha Atomic Research Centre（巴哈原子研究中心）；Homi Bhabha National Institute（霍米·巴巴国立研究所）
Spintronics provides an efficient platform for realizing non-volatile memory and logic devices. In these systems, data is stored in the magnetization of magnetic materials, and magnetization is switched in the writing process. In conventional spintronic devices, ferromagnetic materials are used which have a magnetization dynamics timescale of around the nanoseconds, setting a limit for the switching speed. Increasing the magnetization switching speed has been one of the challenges in spintronic research. In this work we take advantage of the ultrafast magnetization dynamics in ferrimagnetic ma…
We show that it is possible to engineer magnetic multi-domain configurations without domain walls in a prototypical rare earth/transition metal ferrimagnet using keV He+ ion bombardment. We additionally shown that these patterns display a particularly stable magnetic configuration due to a deep minimum in the free energy of the system which is caused by flux closure and the corresponding reduction of the magnetostatic part of the total free energy. This is possible because light-ion bombardment differently affects an elements relative contribution to the effective properties of the ferrimagnet…
Manipulation of the intersublattice interaction strengh (JRE-TM) in rare earth (RE)-transition metal (TM) alloys is a key issue to understand how efficiently the laser-induced angular momentum transfers from 3d to 4f spins and to have a better control of the ultrafast spin dynamics. In this work, the relationships between laser-induced demagnetization process and the intersublattice 3d-4f interaction for the GdCoFe alloys were systematically studied. The ultrafast two-stage demagnetization process could change into a one-stage mode as the angular momentum transferring channel between 3d and 4f…
Spin-transfer torque (STT) and spin-orbit torque (SOT) are spintronic phenomena allowing magnetization manipulation using electrical currents. Beyond their fundamental interest, they allow developing new classes of magnetic memories and logic devices, in particular based on domain wall (DW) motion. In this work, we report the study of STT driven DW motion in ferrimagnetic manganese nickel nitride (Mn4-xNixN) films, in which a fine adjustment of the Ni content allows setting the magnetic compensation at room temperature. The reduced magnetization, combined with the large spin polarization of co…
The spin-orbit torque switching of ferrimagnetic Gd$_x$(Fe$_{90}$Co$_{10}$)$_{100-x}$ films was studied for both transition metal (TM)-rich and rare earth (RE)-rich configurations. The spin-orbit torque driven magnetization switching follows the same handedness in TM-rich and RE-rich samples with respect to the total magnetization, but the handedness of the switching is reversed with respect to the TM magnetization. This indicates that the sign of the spin-orbit-torque-driven magnetic switching follows the total magnetization, although transport based techniques such as anomalous Hall effect a…
We review and discuss the process of single-shot helicity-independent all-optical switching of magnetization by which a single suitably-ultrafast excitation, under the right conditions, toggles magnetization from one stable state to another. For almost a decade, this phenomenon was only consistently observed in specific rare-earth-transition-metal ferrimagnetic alloys of GdFeCo, but breakthrough experiments in recent years have revealed that the same behavior can be achieved in a wide range of multi-sublattice magnets including TbCo alloys doped with minute amounts of Gd, Gd/Co and Tb/Co synth…
Trirutile-type LiFe$_2$F$_6$ is a charge-ordered material with Fe$^{2+}$/Fe$^{3+}$ configuration. Here its physical properties, including magnetism, electronic structure, phase transition, and charge ordering, are studied theoretically. On one hand, the charge ordering leads to improper ferroelectricity with a large polarization. On the other hand, its magnetic ground state can be tuned from the antiferromagnetic to ferrimagnetic by moderate compressive strain. Thus, LiFe$_2$F$_6$ can be a rare multiferroic with both large magnetization and polarization. Most importantly, since the charge orde…
The ruthenium content of half-metallic Mn$_2$Ru$_x$Ga thin films, with a biaxially-strained inverse Heusler structure, controls the ferrimagnetism that determines their magnetic and electronic properties. An extensive study of Mn$_y$Ru$_x$Ga films on MgO (100) substrates with $1.8 \leq y \leq 2.6$ and $x = 0.5$, 0.7 or 0.9, including crystallographic, magnetic order, magneto-transport and spin polarisation is undertaken to map specific composition-dependent properties in this versatile ternary system. A comparison of experimental densities obtained from X-ray reflectivity with calculated densi…
