Net Magnetization Research Articles

Non-uniform Gd distribution and magnetization profiles within GdCoFe alloy thin films

Rare earth (RE):transition metal (TM) ferrimagnetic alloys continue to attract significant attention for spintronics. This work focuses on the elemental distribution of RE and TM elements throughout the thickness of nominally uniform films and the resulting spatial variations of the magnetization within these layers. Samples of CoFe alloyed with Gd were studied using secondary ion mass spectroscopy, polarized neutron reflectometry, and x-ray resonant magnetic reflectivity. The samples were grown by magnetron co-sputtering to control the RE:TM alloy ratio of the ferrimagnetic layer, which was combined with W and Pt layers as either under or over-layers to create sample structures such as W/Gdx(Co70Fe30)100−x/Pt, where x = 0, 8, and 23 at. %. Results show that uniformly deposited thin-films have a significant variation in the distribution of the TM and RE through the film thickness, and this leads to a spatial distribution in the net magnetization profile and a non-uniform Gd magnetization profile within the layer. These findings have implications for the application RE:TM alloys in spintronics as they may impact the perpendicular magnetic anisotropy, the ferrimagnetic compensation temperature, and interfacial spin transport.

Magnetic and electronic properties of La-doped hexagonal 4H-SrMnO3

As typical strongly correlated electronic materials, manganites show rich magnetic phase diagrams and electronic structures depending on the doped carrier density. Most previous relevant studies of doped manganites rely on the cubic/orthorhombic structures, while the hexagonal structure is much less studied. Here first-principles calculations are employed to investigate the magnetic and electronic structures of La-doped 4H-SrMnO3. By systematically analyzing the two kinds of La-doped positions, our calculations predict that the doped electron with lattice distortion would prefer to form polarons, which contribute to the local magnetic phase transition, nonzero net magnetization, and semiconducting behavior. In addition, the energy gap decreases gradually with increasing doping concentration, indicating a tendency of insulator–metal transition.

Particle size-dependent structural and magnetic properties of Pr0.6-xBixSr0.4MnO3 (x = 0.10 and 0.25)

Nanoparticles of Pr0.6-xBixSr0.4MnO3 (x = 0.10 and 0.25) have been prepared using the swift and cost-effective top-down approach in a high-energy planetary ball mill without any chemical processing and environmental impacts resulting due to pollutants arising from nanoparticle synthesis. The work investigates the role of particle size reduction on the structural and magnetic properties. An increase in milling time from 0 to 240 min results in the drastic reduction of particle size which drops significantly in the initial phase of ball milling i.e., 0–60 min while the microstrain and dislocation densities show nearly monotonic increase. Interestingly the magnetism and size reduction demonstrate a clear one to one correspondence. In both compositions, the paramagnetic (PM) to ferromagnetic (FM) transition, TC decreases and the magnetic transitions broaden both as function Bi and size reduction. The Curie–Weiss analysis of the inverse magnetic susceptibility ({chi }^{-1}) shows a deviation from linearity indicating the presence of the short-range FM interactions above TC which has been understood as Griffith’s phase like singularity. The size reduction can effectively reduce TC, enabling a significant control over tuning of transition temperature and net magnetization. The field dependent magnetization for x = 0.10 demonstrate dominant FM state whereas for x = 0.25, metamagnetic magnetization highlights competitive coexistence of FM and antiferromagnetic (AFM) interactions in the system. With ball milling, the net magnetization decreases, and the metamagnetic behaviour is suppressed. The M–H loops of ball milled nanoparticles are highly unsaturated indicating the enhanced surface disorder in the nanoparticles which can be understood using the core–shell structure.

Double stranded antiferromagnetic helix as an efficient spin filter

We report a large degree of spin filtration in a double stranded (ds) antiferromagnetic helix (AFH) system. Generally spin channel separation is not possible when a magnetic system possesses a vanishing net magnetization. But we show that a highly polarized spin current can be obtained through the ds AFH when it is subjected to a transverse electric field. Describing the physical system within a tight-binding framework, spin-dependent transport phenomena are studied using the well known Green’s function formalism. The effects of chirality (left-handed and right-handed), electric field, electronic hopping (short-range and long-range) in each strand, system temperature, and size of the helix on spin filtration are critically investigated. Two different configurations of magnetic moments in the helix are taken into account, for a more general description. Suitably adjusting the physical parameters, almost cent percent spin polarization can be substantiated and that feature persists even for a broad parameter range. Our analysis may open up a new direction for achieving spin-selective electron transmission and designing of controlled spintronic devices using similar kinds of fascinating helical magnetic systems.

Empowering Control of Antiferromagnets by THz-Induced Spin Coherence.

Finding efficient and ultrafast ways to control antiferromagnets is believed to be instrumental in unlocking their potential for magnetic devices operating at THz frequencies. Still, it is challenged by the absence of net magnetization in the ground state. Here, we show that the magnetization emerging from a state of coherent spin precession in antiferromagnetic iron borate FeBO_{3} can be used to enable the nonlinear coupling of light to another, otherwise weakly susceptible, mode of spin precession. This nonlinear mechanism can facilitate conceptually new ways of controlling antiferromagnetism.

Perspective on imaging antiferromagnetic domains in thin films with the magneto-optical birefringence effect

Antiferromagnets are considered to be a promising host material for the next generation of magnetic storage due to their high stability and stray-field-free property. However, the absence of net magnetization in antiferromagnets renders conventional magnetometry ineffective, posing a great challenge in investigating microscopic antiferromagnetic (AFM) properties under magnetic or electric fields. In this Perspective, we provide an overview of various AFM domain imaging techniques and discuss the most promising optical imaging method based on the magneto-optical birefringence (MOB) effect. Additionally, we highlight recent advances in imaging AFM domains utilizing the MOB technique. This Perspective aims to provide a comprehensive review of the current research and potential future directions based on the MOB imaging technique, which could pave the way for the development of more efficient and reliable magnetic storage devices based on antiferromagnets.

Non-linear GMI decoding in 3D printed magnetic encoded systems

The nonlinear giant magnetoimpedance (GMI) effect was explored as a highly sensitive sensing technology in 3D-printed magnetic encoded systems. Magnetic nanoparticles with low (magnetite, Fe3O4) and high (Co ferrite, Co0.7Fe2.3O4) magnetic remanence were embedded (10 wt.%) in a polymeric matrix of Polylactic Acid (PLA) and Poly-ε-caprolactone (PCL) and extruded in magnetic filaments to be 3D printed by the Fused Deposition Modelling technique (FDM). Two different geometries were constructed namely, individual magnetic strips and fixed barcoded pieces. The stray magnetic fields generated by the magnetic nanoparticles were detected through the non-linear (second harmonic) GMI voltage using a soft magnetic CoFeSiB wire as the nucleus sensor. The decoding response was analyzed as a function of the magnetization remanence of the nanoparticles, the distance between the individual magnetic strips, and the position (height) of the GMI decoding sensor. It has been shown that modification of the net magnetization direction of each individual fixed strip within the barcode geometry is possible through the application of local external magnetic fields. This possibility improves the versatility of the 3D binary encoding system by adding an additional state (0 without nanoparticles, 1 or -1 depending on the relative orientation of the net magnetization along the strips) during the codifying procedure.

Optically controlled single-valley exciton doublet states with tunable internal spin structures and spin magnetization generation

Manipulating quantum states through light-matter interactions has been actively pursued in two-dimensional materials research. Significant progress has been made toward the optical control of the valley degrees of freedom in semiconducting monolayer transition-metal dichalcogenides, based on doubly degenerate excitons from their two distinct valleys in reciprocal space. Here, we introduce a type of optically controllable doubly degenerate exciton states that come from a single valley, dubbed as single-valley exciton doublet (SVXD) states. They are unique in that their constituent holes originate from the same valence band, making possible the direct optical control of the spin structure of the excited constituent electrons. Combining ab initio GW plus Bethe-Salpeter equation (GW-BSE) calculations and a theoretical analysis method, we demonstrate such SVXD in substrate-supported monolayer bismuthene-which has been successfully grown using molecular beam epitaxy. In each of the two distinct valleys in the Brillouin zone, strong spin-orbit coupling and [Formula: see text] symmetry lead to a pair of degenerate 1s exciton states (the SVXD states) with opposite spin configurations. Any coherent linear combinations of the SVXD in a single valley can be excited by light with a specific polarization, enabling full manipulation of their internal spin configurations. In particular, a controllable net spin magnetization can be generated through light excitation. Our findings open routes to control quantum degrees of freedom, paving the way for applications in spintronics and quantum information science.

Multiple modulation of magnetism in two-dimensional FeCl2/In2Se3 van der Waals heterostructure

The effective modulation of magnetism for two-dimensional (2D) materials not only has potential applications in nanoscale spintronic devices but also has urgent demands in modern industries. In this work, we report the discovery of ferroelectrically (FE) tunable orbital reconstruction in FeCl2/In2Se3 2D van der Waals (vdWs) heterostructures (HSs), which leads to a transition from ferromagnetic (FM) order to ferrimagnetic order (intra-layer magnetic coupling is AFM3 arrangement). The reversible FE polarization not only enables the easy magnetization axis to be tuned from the out-of-plane to in-plane direction but also reduces the net magnetization strength from 31.87 to −0.18 μB/f.u. Based on the charge density differences and the density of states analysis, the preference of FM and AFM3 arrangement can be reasonably explained by the Goodenough–Kanamori–Anderson rule. The ferroelectric switching enables nonvolatile electric control of magnetic order and anisotropy, offering significant potential for high-efficiency nanodevices and nonvolatile information storage. Moreover, modulation of magnetism (magnetic moment from −0.18 to 0.18 μB/f.u.) can also be achieved through interlayer sliding in the −P case, providing a way to control magnetism in 2D vdWs HSs.

Direct observation of antiferromagnetic domains and field-induced reversal in Pt/Cr2O3/Pt epitaxial trilayers

Antiferromagnet does not show the net magnetization, whereas the finite uncompensated moment can residue at the surface. On the surface of the magnetoelectric antiferromagnet, the finite boundary magnetization can acquire the magnetic response. In this paper, we address the magnetic response of the boundary magnetization in the Pt/magnetoelectric Cr2O3/Pt epitaxial trilayer based on the anomalous Hall effect (AHE) and the soft x-ray magnetic circular dichroism (XMCD). Decreasing the Cr2O3 thickness down to 15 nm, the film acquired the magnetic responsiveness, which manifested as the rectangular hysteresis in the magnetic field dependence of the AHE. The sizable XMCD intensity and the rectangular magnetic field dependence of the XMCD intensity revealed that the magnetic response was attributed to the interfacial Cr moment. The detailed investigation of AHE and XMCD revealed that the domain wall motion dominated the reversal process of the boundary magnetization, which was directly visualized by the scanning XMCD microscope.

Ultrafast activation of the double-exchange interaction in antiferromagnetic manganites

In doped manganite systems, strong electronic correlations result in rich phase diagrams where electron delocalization strongly affects the magnetic order. Here, we employ a femtosecond all-optical pump-probe scheme to impulsively photodope the antiferromagnetic parent manganite system CaMnO3 and unveil the formation dynamics of a long-range ferromagnetic state. We resonantly target intense charge transfer electronic transitions in CaMnO3 to photodope the system and probe the subsequent dynamics of both charges and spins using a unique combination of time-resolved terahertz spectroscopy and time-resolved magneto-optical Faraday measurements. We demonstrate that photodoping promotes a long-lived population of delocalized electrons and induces a net magnetization, effectively promoting ferromagnetism resulting from light-induced carrier-mediated short-range double-exchange interactions. The picosecond set time of the magnetization, much longer than the electron timescale, and the presence of an excitation threshold are consistent with the formation of ferromagnetic patches in an antiferromagnetic background.

Novel anomalous Hall effect mechanism in ferrimagnetic GdCo alloy

In this work, we shed light on the mechanism behind the complexity of the anomalous Hall effect (AHE) in the rare earth-transition metal (RE-TM) compound. To achieve a comprehensive picture, we first theoretically investigate the pure elemental metals and observe that the AHE of RE Gd is negative while that of TM Co is positive. We then investigate magnetic properties and AHE behavior for two typical cases of TM-rich and RE-rich compositions that correspond to GdCo5 and GdCo3 alloys, respectively. The observation that net magnetization is not a decisive factor in assessing the AHE value is consistent with recent claims. Besides, our investigations reveal a significant role of the Gd sublattice to the AHE. The reduction AHE signal under a high-applied field is attributed to the counteraction between the positive and negative AHC contributions when the TM and RE sub-moments are aligned parallel. On a bright note, our new findings can be successfully employed to unravel two types of aberrant humps of AHE signals near compensation temperature.

Probing the Néel-Type Antiferromagnetic Order and Coherent Magnon-Exciton Coupling in Van Der Waals VPS3.

2D van der Waals (vdW) antiferromagnets have received intensive attention due to their terahertz resonance, multilevel magnetic-order states, and ultrafast spin dynamics. However, accurately identifying their magnetic configuration still remains a challenge owing to the lack of net magnetization and insensitivity to external fields. In this work, the Néel-type antiferromagnetic (AFM) order in 2D antiferromagnet VPS3 with the out-of-plane anisotropy, which is demonstrated by the temperature-dependent spin-phonon coupling and second-harmonic generation (SHG), is experimentally probed. This long-range AFM order even persists at the ultrathin limit. Furthermore, strong interlayer exciton-magnon coupling (EMC) upon the Néel-type AFM order is detected based on the monolayer WSe2 /VPS3 heterostructure, which induces an enhanced excitonic state and further certifies the Néel-type AFM order of VPS3 . The discovery provides optical routes as the novel platform to study 2D antiferromagnets and promotes their potential applications in magneto-optics and opto-spintronic devices.

Probing the structural, mechanical, phonon, thermal, and transport properties of magnetic halide perovskites XTiBr3 (X = Rb, Cs) through ab-initio results

Herein, we have first reported the intrinsic properties, including structural, mechanical, electronic, magnetic, thermal, and transport properties of XTiBr3 (X = Rb, Cs) halide perovskites within the simulation scheme of density functional theory as integrated into Wien2k. First and foremost, the structural stability in terms of their ground state energies has been keenly evaluated from their corresponding structural optimizations, which advocate that XTiBr3 (X = Rb, Cs) has a stable ferromagnetic rather than the competing non-magnetic phase. Later on, the electronic properties have been computed within the mix of two applied potential schemes like Generalized Gradient Approximation (GGA) along with Trans-Bhala modified Becke Johnson (TB-mBJ), which thoroughly addresses the half-metallic behaviour with spin-up as metallic and in contrast to opposite spin-down channel signatures the semiconducting behaviour. Furthermore, the spin-splitting seen from their corresponding spin-polarised band structures offers a net magnetism of 2 µB which lends their opportunities to unlock the application branch of spintronics. In addition, these alloys have been characterised to show their mechanical stability describing the ductile feature. Moreover, phonon dispersions decisively certify the dynamical stability within the density functional perturbation theory (DFPT) context. Finally, the transport and thermal properties predicted within their specified packages have also been forwarded in this report.

Ultrafast antiferromagnet rearrangement in Co/IrMn/CoGd trilayers

Antiferromagnets offer great potential for high-speed data processing applications, as they can expend spintronic devices from a static storage and gigahertz frequency range to the terahertz range. However, their zero net magnetization makes them difficult to manipulate and detect. In recent years, there has been a lot of attention given to the ultrafast manipulation of magnetic order using ultra-short single laser pulses, but it remains unknown whether a similar scenario can be observed in antiferromagnets. In this work, we demonstrate the manipulation of antiferromagnets with a single femtosecond laser pulse in perpendicular exchange-biased Co/IrMn/CoGd trilayers. We study the dual exchange bias interlayer interaction in quasi-static conditions and competition in ultrafast antiferromagnet rearrangement. Our results show that, compared to conventional ferromagnetic/antiferromagnetic systems, the IrMn antiferromagnet can be ultrafast and efficiently manipulated by the coupled CoGd ferrimagnetic layer, which paves the way for potential energy-efficient spintronic devices.

Ferromagnetism induced by hybridization of Fe 3d orbitals with ligand InSb bands in the n -type ferromagnetic semiconductor (In,Fe)Sb

Fe-doped III-V ferromagnetic semiconductor (FMS) (In,Fe)Sb is a promising material for spintronic device applications because of the n-type carrier conduction and the ferromagnetism with high Curie temperature (TC > 300 K). To clarify the mechanism of the high-TC ferromagnetism, we have investigated the electronic structure and magnetic properties of an (In,Fe)Sb thin film by performing x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) measurements at the Fe L2,3 edges. The magnetic-field dependence of the XMCD spectra reveals that there are ferromagnetic-like Fe and paramagnetic-like Fe components in the (In,Fe)Sb thin film. The XAS and XMCD spectra of the ferromagnetic-like and paramagnetic-like Fe components resemble those of other Fe-doped FMSs and extrinsic oxides, respectively. The finite value of the ratio between the orbital and spin magnetic moments estimated by applying the XMCD sum rules indicates that the valence state of the Fe ions substituting for the In sites in (In,Fe)Sb is not purely ionic Fe3+, but intermediate between Fe3+ and Fe2+. The qualitative correspondence between the magnetic-field dependence of the visible-light magnetic circular dichroism intensity and that of the XMCD intensity demonstrates that the Zeeman splitting of the InSb band is proportional to the net magnetization of the doped Fe. These results suggest that the ferromagnetism of (In,Fe)Sb originates from the Fe 3d orbitals hybridized with the host InSb bands.

Solution-Processed NiPS3 Thin Films from Liquid Exfoliated Inks with Long-Lived Spin-Entangled Excitons.

Antiferromagnets are promising materials for future opto-spintronic applications since they show spin dynamics in the THz range and no net magnetization. Recently, layered van der Waals (vdW) antiferromagnets have been reported, which combine low-dimensional excitonic properties with complex spin-structure. While various methods for the fabrication of vdW 2D crystals exist, formation of large area and continuous thin films is challenging because of either limited scalability, synthetic complexity, or low opto-spintronic quality of the final material. Here, we fabricate centimeter-scale thin films of the van der Waals 2D antiferromagnetic material NiPS3, which we prepare using a crystal ink made from liquid phase exfoliation (LPE). We perform statistical atomic force microscopy (AFM) and scanning electron microscopy (SEM) to characterize and control the lateral size and number of layers through this ink-based fabrication. Using ultrafast optical spectroscopy at cryogenic temperatures, we resolve the dynamics of photoexcited excitons. We find antiferromagnetic spin arrangement and spin-entangled Zhang-Rice multiplet excitons with lifetimes in the nanosecond range, as well as ultranarrow emission line widths, despite the disordered nature of our films. Thus, our findings demonstrate scalable thin-film fabrication of high-quality NiPS3, which is crucial for translating this 2D antiferromagnetic material into spintronic and nanoscale memory devices and further exploring its complex spin-light coupled states.

Nanoscale Magnetic Domains in Polycrystalline Mn3Sn Films Imaged by a Scanning Single-Spin Magnetometer.

Noncollinear antiferromagnets with novel magnetic orders, vanishingly small net magnetization, and exotic spin related properties hold enormous promise for developing next-generation, transformative spintronic applications. A major ongoing research focus of this community is to explore, control, and harness unconventional magnetic phases of this emergent material system to deliver state-of-the-art functionalities for modern microelectronics. Here we report direct imaging of magnetic domains of polycrystalline Mn3Sn films, a prototypical noncollinear antiferromagnet, using nitrogen-vacancy-based single-spin scanning microscopy. Nanoscale evolution of local stray field patterns of Mn3Sn samples are systematically investigated in response to external driving forces, revealing the characteristic "heterogeneous" magnetic switching behaviors in polycrystalline textured Mn3Sn films. Our results contribute to a comprehensive understanding of inhomogeneous magnetic orders of noncollinear antiferromagnets, highlighting the potential of nitrogen-vacancy centers to study microscopic spin properties of a broad range of emergent condensed matter systems.

Evidence of non-collinear spin texture in magnetic moiré superlattices

Moir\'e magnetism, parallel with moir\'e electronics that has led to novel correlated and topological electronic states, emerges as a new venue to design and control exotic magnetic phases in twisted magnetic two-dimensional(2D) crystals. Here, we report direct evidence of noncollinear spin texture in 2D twisted double bilayer (tDB) magnet chromium triiodide (CrI$_3$). Using magneto-optical spectroscopy in tDB CrI$_3$, we revealed the presence of a net magnetization, unexpected from the composing antiferromagnetic bilayers with compensated magnetizations, and the emergence of noncollinear spins, originated from the moir\'e exchange coupling-induced spin frustrations. Exploring the twist angle dependence, we demonstrated that both features are present in tDB CrI$_3$ with twist angles from 0.5$^o$ to 5$^o$, but are most prominent in the 1.1$^o$ tDB CrI$_3$. Focusing on the temperature dependence of the 1.1$^o$ tDB CrI$_3$, we resolved the dramatic suppression in the net magnetization onset temperature and the significant softening of noncollinear spins, as a result of the moir\'e induced frustration. Our results demonstrate the power of moir\'e superlattices in introducing novel magnetic phenomena that are absent in natural 2D magnets.

Tuning crystal orientation and chiral spin order in Mn3Ge by annealing process and ion implantation

The non-collinear antiferromagnetic Weyl semimetal Mn3X (X = Ga, Ge, Sn) system has attracted a lot of attentions owing to its robust anomalous Hall effect (AHE), large spin Hall angle and small net magnetization at room temperature. The high spin-charge interconversion efficiency makes it a super candidate in topological antiferromagnetic spintronic devices, which could facilitate ultra-fast operation of high-density devices with low energy consumption. In this work, we have realized to obtain different chiral spin structures in Heusler alloy Mn3Ge thin films, which originate from different crystalline orientations. The high-quality (0002)- and (200)-oriented single phase hexagonal Mn3Ge films are achieved by controllable growth, annealing process and ion implantation. The various magnetic properties and AHE behaviors are observed along a and c crystal axes, equivalent to magnetic field in and out of the inverse triangular spin plane. The observation demonstrates the manipulation of crystal structure accompanied with chiral spin order in a non-collinear antiferromagnetic Mn3Ge film, which is induced by energy conversion and defect introduction. The in situ thermal treatment induces crystal phase rotation up to 90° and robust AHE modulation, which is significantly important and highly desirable for flexible spin memory device applications.