Spin Reorientation Transition Research Articles

High-temperature concomitant metal-insulator and spin-reorientation transitions in a compressed nodal-line ferrimagnet Mn3Si2Te6

Symmetry-protected band degeneracy, coupled with a magnetic order, is the key to realizing novel magnetoelectric phenomena in topological magnets. While the spin-polarized nodal states have been identified to introduce extremely-sensitive electronic responses to the magnetic states, their possible role in determining magnetic ground states has remained elusive. Here, taking external pressure as a control knob, we show that a metal-insulator transition, a spin-reorientation transition, and a structural modification occur concomitantly when the nodal-line state crosses the Fermi level in a ferrimagnetic semiconductor Mn3Si2Te6. These unique pressure-driven magnetic and electronic transitions, associated with the dome-shaped Tc variation up to nearly room temperature, originate from the interplay between the spin-orbit coupling of the nodal-line state and magnetic frustration of localized spins. Our findings highlight that the nodal-line states, isolated from other trivial states, can facilitate strongly tunable magnetic properties in topological magnets.

Role of Dy 4f electrons on magnetic coupling and reorientation in DyFeO3.

Spin reorientation transition is an ubiquitous phenomenon observed in magnetic rare earth orthferrites RFeO3, which has garnered significant attention in recent years due to the potential applications in spintronics or magnetoelectric devices. Although a plenty of experimental works suggest that the magnetic interaction between R3+ and Fe3+ spins is at the heart of the spin reorientation, but a direct and decisive support from theoretical side is lacking so far, owning to the tricky handling of R 4f electrons. In this paper, we explored DyFeO3 as an example by means of comprehensive first principles calculations, and compared two different recipes, where the Dy 4f electrons are separately treated as core or valence states, respectively, in order to highlight what the role of Dy 4f electrons plays in, especially the spin reorientation transition. The comparison provides a solid piece of evidence for the experimental argument that the Dy3+-Fe3+ magnetic interactions play a vital role in triggering spin reorientation of Fe moments at low temperature. The findings revealed here not only extend our understanding on the underlying mechanism for spin reorientation transition in RFeO3, but also highlight the importance of explicit description of R 4f electrons in rationally reproducing their structural, electronic and magnetic properties.

Magnetic Anisotropy in Heterogeneous Amorphous Thin Films: Insights from Thickness and Temperature-Driven Spin-Reorientation

Abstract Magnetization orientation in thin films is intricately influenced by multiple anisotropy components, with the dominant anisotropy serving as a key determinant. This complexity becomes particularly intriguing when considering thin films composed of subnanometer-scale heterogeneous amorphous structures. Our investigation builds upon this foundation, specifically focusing on the Fe-Ni-B-Nb alloy system, known for its moderate glass-forming ability and susceptibility to nanocrystallization. In this study, we present thickness- and temperature-driven spin-reorientation (SRT) transition, attributed to competing magnetic anisotropy energies in thin films featuring a heterogeneous amorphous structure. Thermogravimetric investigations unveiled a unique heterogeneous amorphous structure, a revelation unattainable through conventional structural analysis methods. The observed spontaneous perpendicular magnetization in amorphous films, as evidenced by transcritical hysteresis loops and magnetic stripe domains, is ascribed to the pronounced residual stress arising from the substantial magnetostriction of the alloy system. The temperature-driven SRT is correlated to the order-disorder magnetic transition of the heterogeneous amorphous phase, characterized by a Curie temperature of ~225 K. This transformative magnetic state of the heterogeneous amorphous matrix limits the exchange interaction among the densely distributed α-Fe nuclei regions, ultimately governing the dynamic magnetic responses with varying temperature. This work provides valuable insights into the dynamic magnetic orientation of thin films, especially those with heterogeneous amorphous structures, contributing to the broader understanding of the underlying mechanisms of magnetization reversals.

Disentangling the Unusual Magnetic Anisotropy of the Near‐Room‐Temperature Ferromagnet Fe4GeTe2

AbstractIn the quest for 2D conducting materials with high ferromagnetic ordering temperature the new family of the layered FenGeTe2 compounds, especially the near‐room‐temperature ferromagnet Fe4GeTe2, receives a significant attention. Fe4GeTe2 features a peculiar spin reorientation transition at TSR ≈ 110 K suggesting a non‐trivial temperature evolution of the magnetic anisotropy (MA)—one of the main contributors to the stabilization of the magnetic order in the low‐dimensional systems. An electron spin resonance (ESR) spectroscopic study reported here provides quantitative insights into the unusual magnetic anisotropy of Fe4GeTe2. At high temperatures the total MA is mostly given by the demagnetization effect with a small contribution of the counteracting intrinsic magnetic anisotropy of an easy‐axis type, whose growth below a characteristic temperature Tshape ≈ 150 K renders the sample seemingly isotropic at TSR. Below one further temperature Td ≈ 50 K the intrinsic MA becomes even more complex. Importantly, all the characteristic temperatures found in the ESR experiment match those observed in transport measurements, suggesting an inherent coupling between magnetic and electronic degrees of freedom in Fe4GeTe2. This finding together with the observed signatures of the intrinsic two‐dimensionality should facilitate optimization routes for the use of Fe4GeTe2 in the magneto‐electronic devices, potentially even in the monolayer limit.

Theoretical investigation of the giant magnetocaloric effect in Er0.7Tm0.3Al2

This study presents a theoretical investigation of the giant magnetocaloric effect recently reported in the intermetallic compound Er0.7Tm0.3Al2. Our model Hamiltonian includes the crystalline electrical field, exchange, and Zeeman interactions in both Er3+ and Tm3+ sublattices. A remarkable agreement was achieved between the theoretical calculations and experimental data concerning heat capacity, ΔST and ΔTad (magnetocaloric quantities). Additionally, the analysis of magnetic anisotropy and simulations for the rotating magnetocaloric effect in Er0. 7Tm0.3Al2 were performed. The maximum value for the rotating magnetocaloric effect was predicted around the temperature of spin reorientation transition from the <111>-easy to the <001>-hard magnetization directions.

Spin-reorientation driven emergent phases and unconventional magnetotransport in quasi-2D vdW ferromagnet Fe4GeTe2

Non-trivial spin textures driven by strong exchange interaction, magneto-crystalline anisotropy, and electron correlation in a low-dimensional magnetic material often lead to unusual electronic transitions. Through a combination of transport experiments in exfoliated nanoflakes down to 16 layers and first principle calculations, we unravel emergent electronic phases in quasi-2D van der Waals ferromagnet, Fe4GeTe2, possessing ferromagnetic TC ~ 270 K, along with a spin-reorientation transition (TSR ~ 120 K) with the change of magnetic easy axis. Two electronic transitions are identified. The first transition near TSR exhibits a sharp fall in resistivity, followed by a sign change in the ordinary Hall coefficient (R0), together with, maximum negative magnetoresistance (MR) and anomalous Hall conductivity. Another unusual electronic transition, hitherto unknown, is observed near ~ 40–50 K (TQ), where R0 again changes sign and below which, the resistivity shows a quadratic temperature dependence, and MR becomes positive. An analysis of the experimental data further uncovers the role of competing inelastic scattering processes in anomalous magnetotransport behavior. The density-functional theory based first-principle calculations unveil two possible magnetic phases, followed by a low-energy model Hamiltonian which captures the essence of these phases as well as explains the observed magnetotransport behavior. Thus, we demonstrate an interplay between magnetism and band topology and its consequence on electron transport in Fe4GeTe2, important for spintronic applications.

Observation of topological hall effect and skyrmions in Pt/Co/Ir/Co/Pt system

Abstract The interlayer exchange coupling (IEC) between two ferromagnetic (FM) layers separated by a non-magnetic (NM) spacer layer gives rise to different types of coupling with the variation of spacer layer thickness. When the NM is metallic, the IEC is attributed to the well-known Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction which shows an oscillatory decaying nature with increasing thickness. Due to this, it is possible to tune the coupling between the two FM to be either ferromagnetic or antiferromagnetic. In this work we have studied a Pt/Co/Ir/Co/Pt system where the Co thickness has been taken in the strong perpendicular magnetic anisotropy regime which is much less than the spin reorientation transition thickness. By tuning the Ir thickness to 2.0 nm, a canted state of magnetization reversal in the system is observed which gives rise to a possibility of nucleating topologically non-trivial spin textures like skyrmions. Further, with the combination of transport and magnetic force microscopy (MFM) measurements, we have confirmed the presence of skyrmions in our system. These findings may be useful for potential applications in emerging spintronic and data storage technologies using skyrmions.

Thermally generated magnonic spin currents in a polycrystalline gadolinium iron garnet thin film with perpendicular magnetic anisotropy

Rare-earth iron garnets (REIGs) are the benchmark systems for magnonics, including the longitudinal spin Seebeck effect (LSSE). While most research has focused on single-crystalline REIGs on complimentary garnet substrates, moving to more, cost-effective complementary metal-oxide semiconductor (CMOS)-compatible substrates is important to integrate REIG thin films with existing technology. In this regard, we grow a 130 nm-thick polycrystalline gadolinium iron garnet (GdIG) film on the Si/SiO2 substrate and investigate the temperature-dependent LSSE. Interestingly, the polycrystalline GdIG film exhibits perpendicular magnetic anisotropy (PMA) at room temperature which is induced by tensile in-plane (IP)-strain originating from the thermal-expansion mismatch between the GdIG film and the substrate during rapid thermal annealing. Further, a spin-reorientation transition from the out-of-plane IP direction below TS = 180 K is observed. Additionally, the film reveals a magnetic compensation temperature, TComp, of ≈240 K. The LSSE voltage not only demonstrates a sign-inversion around TComp, but also shows noticeable changes around TS. As compared to a single-crystalline GdIG film, the lower LSSE voltage for the polycrystalline GdIG is attributed to the higher effective magnetic anisotropy and enhanced magnon scattering at the grain boundaries. Our study not only paves the way for the cost-effective growth of CMOS-compatible REIG-based systems with PMA for magnonic memory and information processing applications, but also highlights the fact that the spincaloritronic and spin-insulatronic properties of the polycrystalline REIGs follow those of their single-crystalline counterparts with reduced spin-to-charge conversion efficiency through LSSE which can be tuned further by controlling the average gran size and interface engineering.

Sm substitution induced spin reorientation and stabilization of double perovskite structure resulting in enhanced magnetoelectricity in LaYFe2O6

We report an enhanced magnetoelectric (ME) effect in spin–phonon coupled single-phase La1−xSmxYFe2O6 (0 ≤ x ≤ 1). The structural, electric, magnetic, and ME properties have been investigated to establish their interplay leading to magnetoelectricity. X-ray diffraction study suggests the facilitation of the P21nm phase (double perovskite lattice arrangements) formation and improved structural order due to the substitution of Sm in the lattice. Antiferromagnetic (AFM) transition ∼700 K along with a spin-reorientation transition around room temperature (RT) and below is observed in the thermomagnetic curve. The indication of short range ordering in the magnetization data in the form of a non-Griffiths-like phase (nGP) is observed. The short range ordering could be minimized along with consequent improvement in AFM ordering, due to Sm substitution. An enhanced (∼31% with respect to x = 0) RT first-order ME coupling coefficient ∼0.59 mV cm−1 Oe−1 in x = 0.75 composition is observed. The findings reported here open the door to exercise spin-reorientation transition in the spin–phonon coupled double perovskites for spintronic device applications.

Magnetocaloric effect in Er[formula omitted]Gd[formula omitted]Al2 ([formula omitted]) alloys

Measurements of magnetization (M) were performed on a series of Er1−xGdxAl2 (x= 0.1, 0.25, and 0.5) alloys. ErAl2 and GdAl2 are ferromagnets with the Curie temperatures (TC) of 14 K and 168 K, respectively. Er1−xGdxAl2 also showed a ferromagnetic order at TC= 21 K for x= 0.1, 57 K for x= 0.25, and 89 K for x= 0.5. Upon cooling, M(B) curves of Er1−xGdxAl2 for 0.1≤x≤0.5 exhibited a metamagnetic behavior. The field cooled M for Er1−xGdxAl2 increased below 30 K, indicating a spin-reorientation transition. The magnetic entropy change (ΔSm) for x=0.1 peaked at TC, while a peak or kink was observed for x= 0.25 and 0.5 in ΔSm near 25 K, distinct from a ferromagnetic order. The spin-reorientation due to the Gd substitution is attributed to the magnetic properties and broadened ΔSm(T) curves for Er1−xGdxAl2 alloys.

Unusual multiple magnetic transitions and anomalous Hall effect observed in antiferromagnetic Weyl semimetal, Mn2.94Ge (Ge-rich).

We report on the magnetic and Hall effect measurements of the magnetic Weyl semimetal, Mn2.94Ge (Ge-rich) single crystal. From the magnetic properties study, we identify unusual multiple magnetic transitions below the Ne'el temperature of 353 K, such as the spin-reorientation (TSR) and ferromagnetic-like transitions. Consistent with the magnetic properties, the Hall effect study shows unusual behavior around the spin-reorientation transition. Specifically, the anomalous Hall conductivity increases with increasing temperature, reaching a maximum atTSR, which then gradually decreases with increasing temperature. This observation is quite in contrast to the Mn3+δGe (Mn-rich) system, though both compositions share the same hexagonal crystal symmetry. This study unravels the sensitivity of magnetic and topological properties on the Mn concentration.

Discovery and Characterization of Antiferromagnetic UFe5As3.

This work presents a study on a new uranium iron arsenide UFe5As3. By implementing Bi-flux synthesis, we were able to grow mm-sized single crystals of this compound, which show twinning. UFe5As3 is one of only two known uranium iron arsenides. It adopts a monoclinic, UCr5P3-type crystal structure (space group P21/m, Pearson symbol mP18, a = 7.050(2) Å, b = 3.8582(9) Å, c = 9.634(1) Å, β = 100.25(1)°). The magnetic susceptibility of UFe5As3 indicates it to be an antiferromagnet with TN = 47 K and μeff = 4.94 μB per formula unit, signaling that both U and Fe are likely magnetic in this material. The material appears to be anisotropic, with a small (likely ferromagnetic) spin reorientation transition around T = 29 K. The Sommerfeld coefficient γ0 = 135 mJ mol-1 K-2 suggests enhanced effective electron mass in UFe5As3, while electrical resistivity indicates metallic, Kondo-like behavior.

Electron-Assisted Generation and Straight Movement of Skyrmion Bubble in Kagome TbMn6Sn6.

Topological magnetic textures are promising candidates as binary data units for the next-generation memory device. The precise generation and convenient control of nontrivial spin topology at zero field near room temperature endows the critical advantages in skyrmionic devices but is not simultaneously integrated into one material. Here, in the Kagome plane of quantum TbMn6Sn6, the expedient generation of the skyrmion bubbles in versatile forms of lattice, chain, and isolated one by converging the electron beam, where the electron intensity gradient contributes to the dynamic generation from local anisotropy variation near spin reorientation transition (SRT) is reported. Encouragingly, by utilizing the dynamic shift of the SRT domain interface, the straight movement is actualized with the skyrmion bubble slave to the SRT domain interface forming an elastic composite object, avoiding the usual deflection from the skyrmion Hall effect. The critical contribution of the SRT domain interface via conveniently electron-assisted heating is further theoretically validated in micromagnetic simulation, highlighting the compatible application possibility in advanced devices.

Origin of Multiferroism in VOX2 (X = Cl, Br, I) Monolayers.

Based on the proposed microscopic model, we investigate the multiferroic characteristics of VOX2 (X = Cl, Br, I) monolayers using a Green's function method. The dependence of the microscopic parameters of the ferroelectric system (pseudo-spin arrangement and flipping rate) on the magnitude and sign of the exchange magnetic interaction along the b-axis and the value of the Dzyaloshinskii-Moria vector have been investigated and qualitatively explained. The possibility of observing a spin-reorientation transition with a change in the character of spin ordering from antiferromagnetic to ferromagnetic is investigated. It is found that the antisymmetric magnetoelectric interaction may be responsible for the spin-reorientation transition without a change in the ordering of magnetic moments. Changing the sign of the exchange magnetic interaction along the b-axis leads to ferromagnetic ordering without observing a spin-reorientation transition. The dependence of isotropic and antisymmetric magnetic interactions on the microscopic parameters of the ferroelectric system is qualitatively explained. A mechanism for the occurrence of the spin-reorientation transition is presented based on the proposed microscopic model. The obtained results qualitatively coincide with Density Functional Theory calculations.

Spatially reconfigurable antiferromagnetic states in topologically rich free-standing nanomembranes

Antiferromagnets hosting real-space topological textures are promising platforms to model fundamental ultrafast phenomena and explore spintronics. However, they have only been epitaxially fabricated on specific symmetry-matched substrates, thereby preserving their intrinsic magneto-crystalline order. This curtails their integration with dissimilar supports, restricting the scope of fundamental and applied investigations. Here we circumvent this limitation by designing detachable crystalline antiferromagnetic nanomembranes of α-Fe2O3. First, we show—via transmission-based antiferromagnetic vector mapping—that flat nanomembranes host a spin-reorientation transition and rich topological phenomenology. Second, we exploit their extreme flexibility to demonstrate the reconfiguration of antiferromagnetic states across three-dimensional membrane folds resulting from flexure-induced strains. Finally, we combine these developments using a controlled manipulator to realize the strain-driven non-thermal generation of topological textures at room temperature. The integration of such free-standing antiferromagnetic layers with flat/curved nanostructures could enable spin texture designs via magnetoelastic/geometric effects in the quasi-static and dynamical regimes, opening new explorations into curvilinear antiferromagnetism and unconventional computing.

Evidence of Temperature-Dependent Interplay between Spin and Orbital Moment in van der Waals Ferromagnet VI3.

van der Waals materials provide a versatile toolbox for the emergence of new quantum phenomena and fabrication of functional heterostructures. Among them, the trihalide VI3 stands out for its unique magnetic and structural landscape. Here we investigate the spin and orbital magnetic degrees of freedom in the layered ferromagnet VI3 by means of temperature-dependent X-ray absorption spectroscopy and X-ray magnetic circular and linear dichroism. We detect localized electronic states and reduced magnetic dimensionality, due to electronic correlations. We furthermore provide experimental evidence of (a) an unquenched orbital magnetic moment (up to 0.66(7) μB/V atom) in the ferromagnetic state and (b) an instability of the orbital moment in the proximity of the spin reorientation transition. Our results support a coherent picture where electronic correlations give rise to a strong magnetic anisotropy and a large orbital moment and establish VI3 as a prime candidate for the study of orbital quantum effects.

Spontaneous Topological (Anti)meron Chains in the Domain Walls of Centrosymmetric Rare‐Earth Magnet

AbstractExploration and manipulation of topological protected magnetic swirls, such as skyrmion, antiskyrmion, meron, and vortex, holds significance for fundamental research and practical applications in high‐density magnetic information storage and spintronics because of their high storage density and low driven current. This study unveils the existence of field‐free spontaneous (anti)meron chains with a topological charge of ±1/2 in the centrosymmetric rare‐earth magnet Tb6Co2.17Si2.5 via in situ real‐space observation. The spin reorientation transition from in‐plane to uniaxial anisotropy contributes to the spontaneous transformation from straight domain walls to topological (anti)meron chains and to stripe domains along the [110] zone axis during in situ cooling. The study further confirms the critical role of the noncollinear magnetic structure of Tb atoms in the formation of topological (anti)meron chains via real‐space observations, first‐principles calculations, and micromagnetic simulations. The spontaneous topological magnetic texture is strongly correlated with the 4f electrons of rare‐earth atoms, enriching and stimulating alternative generation mechanisms of topological spin textures from emerging rare‐earth magnets, and further applications in spintronics.

Spin reorientation, spin switching, and magnetic compensation in Er1−xSmxFeO3 single crystals

We investigated spin reorientation, magnetic compensation and spin switching transitions in a series of high-quality single crystals of Er1−xSmxFeO3 (x = 0, 0.2, 0.4, 0.6, 0.8) prepared using the optical floating zone method. Structural and other preliminary characterizations confirmed the quality and phase purity of the crystals. Rietveld refinement of powder XRD data indicates that lattice parameters a and c increase linearly with increasing Sm concentration, whereas b remained constant. Field-cooled cooling (FCC) measurements revealed a temperature-induced spin reorientation transition (SRT) from Γ4 (Gx, Ay, Fz) to Γ2 (Fx, Cy, Gz) for all the samples. SRT temperature increased with Sm concentration and spread widely above and below room temperature. Moreover, magnetic compensation is common to all the compositions but decreases as Sm doping increases. We also observe type-I spin switching in samples with x = 0, 0.2, and 0.4 at an applied field of 60 Oe under FCC protocol, with a reduction in spin switching temperature as Sm content increased. For Sm-rich samples (x = 0.6, 0.8), spin switching was absent at 60 Oe.

Transfer of magnetic anisotropy in epitaxial Co/NiO/Fe trilayers

The magnetic properties of Co(10 Å)/NiO(40 Å)/Fe trilayer epitaxially grown on W(110) substrate were investigated with use of x-ray magnetic linear dichroism (XMLD) and x-ray magnetic circular dichroism (XMCD). We showed that magnetic anisotropy of Fe film that can be controlled by a thickness-driven spin reorientation transition is transferred via interfacial exchange coupling not only to NiO layer but further to ferromagnetic Co overlayer as well. Similarly, a temperature driven spin reorientation of Fe sublayer induces a reorientation of NiO spin orientation and simultaneous switching of the Co magnetization direction. Finally, by element specific XMCD and XMLD magnetic hysteresis loop measurements we proved that external magnetic field driven reorientation of Fe and Co magnetizations as well as NiO Néel vector are strictly correlated and magnetic anisotropy fields of Fe and Co sublayers are identical despite the different crystal structures.

Tailoring Magnetic Anisotropy in Ultrathin Cobalt by Surface Carbon Chemistry

AbstractThe ability to manipulate magnetic anisotropy is essential for magnetic sensing and storage tools. Surface carbon species offer cost‐effective alternatives to metal‐oxide and noble metal capping layers, inducing perpendicular magnetic anisotropy in ultrathin ferromagnetic films. Here, the different mechanisms by which the magnetism in a few‐layer‐thick Co thin film is modified upon adsorption of carbon monoxide (CO), dispersed carbon, and graphene are elucidated. Using X‐ray microscopy with chemical and magnetic sensitivity, the in‐plane to out‐of‐plane spin reorientation transition in cobalt is monitored during the accumulation of surface carbon up to the formation of graphene. Complementary magneto‐optical measurements show weak perpendicular magnetic anisotropy (PMA) at room temperature for dispersed carbon on Co, while graphene‐covered cobalt exhibits a significant out‐of‐plane coercive field. Density‐functional theory (DFT) calculations show that going from CO/Co to C/Co and to graphene/Co, the magnetocrystalline and magnetostatic anisotropies combined promote out‐of‐plane magnetization. Anisotropy energies weakly depend on carbidic species coverage. Instead, the evolution of the carbon chemical state from carbidic to graphitic is accompanied by an exponential increase in the characteristic domain size, controlled by the magnetic anisotropy energy. Beyond providing a basic understanding of the carbon‐ferromagnet interfaces, this study presents a sustainable approach to tailor magnetic anisotropy in ultrathin ferromagnetic films.