Multiferroic Heterostructures Research Articles

Electric field control of 180° magnetization reversal in a spin-valve multiferroic heterostructure

Electrical tuning of magnetism, rather than a spin current or magnetic field, has attracted much attention due to its great potential for designing energy-efficient spintronic devices. However, pure electric field (E-field) control of 180° magnetization reversal is still challenging. Thus, we report an E-field-controlled 180° magnetization reversal in a spin valve (SV)/Pb(Mg1/3Nb2/3)0.7Ti0.3O3 (PMN-PT) multiferroic heterostructure. Via the converse magnetoelectric coupling effect in CoFe/PMN-PT heterostructures, the magnetic anisotropy and coercive field of the CoFe film can be tremendously modulated by an E-field. We fabricated an optimized SV grown on the PMN-PT substrate, in which the magnetic moments of the free and pinned layers are parallel to each other at the initial state. By applying an E-field, the coercive field of the free layer was enhanced, exhibiting an antiparallel configuration between the free and pinned layers. Based on the theoretical and experimental results, a complete 180° magnetization reversal of the free layer can be obtained without a magnetic field. Accordingly, an E-field-controlled giant, reversible and repeatable magnetoresistance modulation can be achieved. This work proposes a feasible strategy to achieve E-field-controlled 180° magnetization reversal, which is critical for exploring ultralow power consumption magnetic memory devices.

Photon-Dipole-Spin Interactions in M(TCNE)x/P(VDF-TrFE) Multiferroic Heterostructure Available for Bimodal Control of Multistate Data-Storage.

Organic multiferroic heterostructure is one of the most promising structures for the future design of high-density flexible energy-efficient data storage. Here, we fabricate organic ferromagnetic M(TCNE)x/ferroelectric P(VDF-TrFE) multiferroic heterostructures, where the excited state in M(TCNE)x interacted with localized dipole in P(VDF-TrFE) provides a key link for the interfacial coupling. Thus, aligned dipoles in P(VDF-TrFE) by external electric field can affect the magnetization of Fe(TCNE)x effectively to result in a pronounced magnetization-voltage (M-V) hysteresis loop. Moreover, light-induced electron-hole pairs in Fe(TCNE)x with long lifetime will effectively interact with the dipoles in P(VDF-TrFE) to lead to an effect in external light control of electric polarization of P(VDF-TrFE). Overall, the organic multiferroic heterostructure provides the possibility of realizing two storage modes, light control of dipole as well as electric field control of spin, which can broaden multifunctional applications of organic multiferroic materials in the area of multistate storage. This article is protected by copyright. All rights reserved.

Interfacial strain induced giant magnetoresistance and magnetodielectric effects in multiferroic BCZT/LSMO thin film heterostructures

Layered thin films of the ferroelectric perovskite Ba0.85Ca0.15Ti0.9Zr0.1O3 (BCZT) and the ferromagnetic half-metal La0.80Sr0.20MnO3 (LSMO) are well-known multiferroic systems that show promise for spintronic applications. In this work, the structure–property relationships are explored in novel BCZT/LSMO thin film heterostructures with optimized ferroic properties. Epitaxial BCZT/LSMO thin film heterostructures are grown by varying the lattice mismatch strains on single crystal LaAlO3 (LAO) (100) and MgO (100) substrates using the pulsed laser deposition technique. The epitaxial strain in the films gives rise to a tetragonal distortion of the BCZT and LSMO unit cells and significantly affects their magnetotransport and magnetodielectric properties. The BCZT/LSMO/LAO heterostructure exhibits a colossal magnetoresistance effect due to a large out-of-plane tensile strain, which induces enhanced carrier hopping in the LSMO layer as compared to the BCZT/LSMO/MgO film. The larger tetragonal distortion of the BCZT unit cell in BCZT/LSMO/MgO contributes to higher dielectric permittivity, with a greater dielectric maxima temperature and freezing temperature. Magnetodielectric measurements reveal a hitherto unobserved giant magnetodielectric effect in the BCZT/LSMO/MgO film, attributed to a large in-plane strain, which induces interfacial polarization distortion at the interfacial layer. Overall, this work elucidates the unique strain and charge-mediated cross-coupled phenomena of magnetic and electric orders in multiferroic thin film heterostructures, which are critical for their technological applications.

First-principles study of perpendicular magnetic anisotropy of CrI3/In2Se3 Van der Waals heterostructure

Two-dimensional multiferroic van der Waals (vdW) heterostructures are promising for nanoscale and multifunctional spintronic devices. Controllable perpendicular magnetic anisotropy in vdW heterostructure often plays a central role in stabilizing ferromagnetic order and lowering energy consumption. Here, we carry out first-principles calculations for CrI3/In2Se3 vdW heterostructure and investigate how its magnetic anisotropy is interrelated to the electronic structure. We show that the semiconducting nature of CrI3 is preserved but band gap decreases in monolayer-CrI3/In2Se3 and bilayer-CrI3/In2Se3 vdW heterostructures. The magnetoelectric effect of CrI3/In2Se3 vdW heterostructure enhances the magnetic moment of CrI3, but decreases the perpendicular magnetic anisotropy of CrI3. I-p orbital coupling matrix element is noteworthy in regard to the modulation of magnetic anisotropy. The MAE contribution of Cr atom slightly enhances but is still negligible by the reason of countervailing contribution of d-orbital coupling matrix elements. By reversing the ferroelectric polarization of In2Se3, the easy magnetization axis of monolayer CrI3 can be switched. These results will help to understand the magnetic anisotropy of multiferroic vdW heterostructure and may enable the development of nonvolatile memory devices.

Structural and Morphological Studies of Pt in the As-Grown and Encapsulated States and Dependency on Film Thickness.

The morphology and crystal structure of Pt films grown by pulsed laser deposition (PLD) on yttria-stabilized zirconia (YSZ)at high temperatures Tg = 900 °C was studied for four different film thicknesses varying between 10 and 70 nm. During the subsequent growth of the capping layer, the thermal stability of the Pt was strongly influenced by the Pt film's thickness. Furthermore, these later affected the film morphology, the crystal structure and hillocks size, and distribution during subsequent growth at Tg = 900 °C for a long duration. The modifications in the morphology as well as in the structure of the Pt film without a capping layer, named also as the as-grown and encapsulated layers in the bilayer system, were examined by a combination of microscopic and scattering methods. The increase in the thickness of the deposited Pt film brought three competitive phenomena into occurrence, such as 3D-2D morphological transition, dewetting, and hillock formation. The degree of coverage, film continuity, and the crystal quality of the Pt film were significantly improved by increasing the deposition time. An optimum Pt film thickness of 70 nm was found to be suitable for obtaining a hillock-free Pt bottom electrode which also withstood the dewetting phenomena revealed during the subsequent growth of capping layers. This achievement is crucial for the deposition of functional bottom electrodes in ferroelectric and multiferroic heterostructure systems.

Electric-field control of nonvolatile resistance state of perpendicular magnetic tunnel junction via magnetoelectric coupling.

Magnetic tunnel junctions (MTJs) are the core elements of spintronic devices. Now, the mainstream writing operation of MTJs mainly relies on electric current with high energy dissipation, which can be greatly reduced if an electric field is used instead. In this regard, strain-mediated multiferroic heterostructure composed of MTJ and ferroelectrics are promising with the advantages of room temperature and magnetic field-free as already demonstrated by MTJ with in-plane magnetic anisotropy. However, there is no such report on the perpendicular MTJs (p-MTJs), which have been commercialized. Here, we investigate electric-field control of resistance state of MgO-based p-MTJs in multiferroic heterostructures. A remarkable and nonvolatile manipulation of resistance is demonstrated at room temperature without magnetic field assistance. Through various characterizations and micromagnetic simulation, the manipulation mechanism is uncovered. Our work provides an effective avenue for manipulating p-MTJ resistance by electric fields and is notable for high density and ultralow power spintronic devices.

The Combined Effect of Spin-Transfer Torque and Voltage-Controlled Strain Gradient on Magnetic Domain-Wall Dynamics: Toward Tunable Spintronic Neuron

Magnetic domain wall (DW), as one of the promising information carriers in spintronic devices, have been widely investigated owing to its nonlinear dynamics and tunable properties. Here, we theoretically and numerically demonstrate the DW dynamics driven by the synergistic interaction between current-induced spin-transfer torque (STT) and voltage-controlled strain gradient (VCSG) in multiferroic heterostructures. Through electromechanical and micromagnetic simulations, we show that a desirable strain gradient can be created and it further modulates the equilibrium position and velocity of the current-driven DW motion. Meanwhile, an analytical Thiele’s model is developed to describe the steady motion of DW and the analytical results are quite consistent with the simulation data. Finally, we find that this combination effect can be leveraged to design DW-based biological neurons where the synergistic interaction between STT and VCSG-driven DW motion as integrating and leaking motivates mimicking leaky-integrate-and-fire (LIF) and self-reset function. Importantly, the firing response of the LIF neuron can be efficiently modulated, facilitating the exploration of tunable activation function generators, which can further help improve the computational capability of the neuromorphic system.

Electric field control of perpendicular magnetic tunnel junctions with easy-cone magnetic anisotropic free layers.

Magnetic tunnel junctions (MTJs) are the core element of spintronic devices. Currently, the mainstream writing operation of MTJs is based on electric current with high energy dissipation, and it can be notably reduced if an electric field is used instead. In this regard, it is promising for electric field control of MTJ in the multiferroic heterostructure composed of MTJ and ferroelectrics via strain-mediated magnetoelectric coupling. However, there are only reports on MTJs with in-plane anisotropy so far. Here, we investigate electric field control of the resistance state of MgO-based perpendicular MTJs with easy-cone anisotropic free layers through strain-mediated magnetoelectric coupling in multiferroic heterostructures. A remarkable, nonvolatile, and reversible modulation of resistance at room temperature is demonstrated. Through local reciprocal space mapping under different electric fields for Pb(Mg1/3Nb2/3)0.7Ti0.3O3 beneath the MTJ pillar, the modulation mechanism is deduced. Our work represents a crucial step toward electric field control of spintronic devices with non-in-plane magnetic anisotropy.

Computational study on ferroelectric control over spin polarization in the bipolar magnetic semiconductor

Multiferroic van der Waals (vdW) heterostructures offer an exciting route toward the nanoelectronics and spintronics device technology. How to realize the mutual regulation between ferroelectric and magnetic materials has attracted extensive research. In this work, based on the density functional theory, we simulate a vdW multiferroic heterostructure based on the bipolar magnetic semiconductor material graphone and ferroelectric monolayer In2Te3 and further investigate its electronic properties. We find that direct contact between In2Te3 and graphone induces a transition in graphone from a ferromagnetic state to a non-magnetic state. Fortunately, the magnetic properties of graphone are preserved by using graphene as an intercalation layer, and the graphone monolayer changes from its original semiconductor to a half-metal in the graphone/graphene/In2Te3 vdW heterostructure for P↓ state. Furthermore, by adjusting the layer spacing of the heterostructure, the spin polarization states of graphone at the Fermi level (EF) are regulated between spin-up (S↑) and spin-down (S↓) with the reversal of ferroelectric polarization states. Our results not only provide a promising way to realize the half-metallicity in 2D magnetic materials but also computationally predict the ferroelectric control of the spin polarization state, which has great application potential in the next-generation nonvolatile electrically controlled spintronic devices.

Switching Intrinsic Magnetic Skyrmions with Controllable Magnetic Anisotropy in van der Waals Multiferroic Heterostructures.

Magnetic skyrmions, topologically nontrivial whirling spin textures at nanometer scales, have emerged as potential information carriers for spintronic devices. The ability to efficiently create and erase magnetic skyrmions is vital yet challenging for such applications. Based on first-principles studies, we find that switching between intrinsic magnetic skyrmion and high-temperature ferromagnetic states can be achieved in the two-dimensional van der Waals (vdW) multiferroic heterostructure CrSeI/In2Te3 by reversing the ferroelectric polarization of In2Te3. The core mechanism of this switching is traced to the controllable magnetic anisotropy of CrSeI influenced by the ferroelectric polarization of In2Te3. We propose a useful descriptor linking the presence of magnetic skyrmions to magnetic parameters and validate this connection through studies of a variety of similar vdW multiferroic heterostructures. Our work demonstrates that manipulating magnetic skyrmions via tunable magnetic anisotropies in vdW multiferroic heterostructures represents a highly promising and energy-efficient strategy for the future development of spintronics.

Multifunctionality in Electrically Poled PMN–PT/Ni–Mn–In Multiferroic Heterostructure for Flexible Magnetic Field Sensing and Nonvolatile Memory Applications

Multifunctionality in Electrically Poled PMN–PT/Ni–Mn–In Multiferroic Heterostructure for Flexible Magnetic Field Sensing and Nonvolatile Memory Applications

In-situ electric field-tailored exchange bias in the manganite/ferroelectric multiferroic heterostructures

The application of electric field-induced magnetic structure changes has significantly advanced nonvolatile data storage with ultralow energy consumption, as well as spintronics and quantum computing processes. In artificial perovskite oxide multiferroic structures composed of ferromagnetic and ferroelectric layers, the evolution of magnetic phases and ferroelectric domains often contribute to the magnetoelectric coupling. To fully understand the mechanisms behind electric field-induced changes in magnetic structures and enable the miniaturization of magnetoelectric devices, it is crucial to achieve local ferroelectric domain-triggered ferromagnetic evolution. In this study, we have fabricated La0.7Ca0.3MnO3/Pb(Zr0.52Ti0.48)O3 (LCMO/PZT) heterostructures, where the magnetic phase separation of LCMO and the ferroelectric domain of PZT can be modulated by substrates and piezoelectric force microscopy, respectively. Our experiments demonstrate that by switching the polarization states of PZT, we can observe electric field control of the magnetic exchange bias effect through changes in the phase separation of the LCMO layer. These results contribute to the development of magnetoelectric devices with enhanced properties and offer valuable insights for future design strategies.

Robust Magnetoelectric Coupling in FeTiO3/Ga2O3 Non-van der Waals Heterostructures.

Magnetoelectric coupling represents a significant breakthrough for next-generation electronics, offering the ability to achieve nonvolatile magnetic control via electrical means. In this comprehensive investigation, leveraging first-principles calculations, we unveil a robust magnetoelectric coupling within multiferroic heterostructures (HSs) by ingeniously integrating a non-van der Waals (non-vdW) magnetic FeTiO3 monolayer with the ferroelectric (FE) Ga2O3. Diverging from conventional van der Waals (vdW) multiferroic HSs, the magnetic states of the FeTiO3 monolayer can be efficiently toggled between ferromagnetic (FM) and antiferromagnetic (AFM) configurations by reversing the polarization of the Ga2O3 monolayer. This intriguing phenomenon arises from polarization-dependent substantial interlayer electron transfers and the interplay between superexchange and direct-exchange magnetic couplings of the iron atoms. The carrier-mediated interfacial interactions induce crucial shifts in Fermi level positions, decisively imparting distinct electronic characteristics near the Fermi level of composite systems. These novel findings offer exciting prospects for the future of magnetoelectric technology.

Direct imaging of the magnetoelectric coupling in multiferroic BaTiO3/La0.9Ba0.1MnO3

We report the direct imaging of the magnetic response of a 4.8 nm La0.9Ba0.1MnO3 film to the voltage applied across a 5 nm BaTiO3 film in a BaTiO3/La0.9Ba0.1MnO3 multiferroic heterostructure using x-ray photoemission electron microscopy (XPEEM). Specifically, we have written square ferroelectric domains on the BaTiO3 layer with an atomic force microscope in contact mode and imaged the corresponding magnetic contrast through the x-ray circular dichroic effect at the Mn L-edge with high spatial lateral resolution using XPEEM. We find a sudden decrease in the magnetic contrast for positive writing voltages above +6 V associated with the switching of the ferroelectric polarization of the BaTiO3, consistent with the presence of a magnetoelectric effect through changes in the hole carrier density at the BaTiO3/La0.9Ba0.1MnO3 interface. Temperature-dependent measurements show a decrease in the Curie temperature and magnetic moment in the areas where a positive voltage above +6 V was applied, corresponding to the hole depletion state and suggesting the onset of a spin-canted state of bulk La0.9Ba0.1MnO3. Our results are the first direct imaging of magnetoelectric coupling in such multiferroic heterostructure.

Polarization Vector Canting in Croconic Acid Ferroelectric Nanoscopic Regions

AbstractCroconic acid is reported to be the organic ferroelectric with the highest above‐room‐temperature saturation polarization in its crystal form, at a value on par with that of commonly used inorganic ferroelectrics. Owing to its organic nature, high polarization value, and small coercive field, Croconic acid is considered as a potential candidate in energy‐efficient and environmentally benign composite multiferroic heterostructures. However, understanding the magnetoelectric mechanism at the ferroelectric/ferromagnetic interface in these structures requires a detailed understanding of the orientation of the polarization vector in its thin film form. To maximize the magnetoelectric effect, the polarization vector should point out of the film plane, yet the polarization in ultra‐thin Croconic acid films is predicted to lie in the film plane. Nevertheless, polycrystalline films show some promise in this direction. In this article, by combining in situ piezoreponse force microscopy imaging with nanoscopic polarization reversal spectroscopy, the authors qualitatively analyze the polarization switching and its orientation in polycrystalline Croconic acid films and show that it is canted with respect to the film plane, with a component along the out‐of‐plane direction.

Nanoscopic spin-wave channeling along programmable magnetic domain walls in a CoFeB/BaTiO3 multiferroic heterostructure

We report a micromagnetic study on spin-wave propagation along magnetic domain walls in a ferromagnetic/ferroelectric bilayer. In our system, strain coupling between the two ferroic materials and inverse magnetostriction produce a fully correlated domain pattern wherein straight and narrow ferroelectric domain walls pin the magnetic domain walls. Consequently, an external magnetic field does tailor the spin structure of the magnetic domain walls instead of moving them. We use experimental parameters from a previously studied CoFeB/BaTiO3 material system to investigate the potential of artificial multiferroics for programmable nanoscopic spin-wave channeling. We show that spin waves are transported along the pinned magnetic domain walls at zero magnetic field and low frequency due to a local demagnetizing field. Further, switching of the domain wall spin structure from a head-to-tail to a head-to-head configuration abruptly changes the propagating spin-wave mode. We study the effect of magnetic field strength on the localized modes and discuss reversible control of spin-wave channeling via electric-field-driven magnetic domain wall motion. Nanoscopic guiding of propagating spin waves by an electric field, in combination with positional robustness to and mode programming by an external magnetic field, offers prospects for low-power and reconfigurable domain-wall-based magnonic devices.

Effects of electric field and light on resistivity switching of Eu0.7Sr0.3MnO3 thin films.

Based on the excellent piezoelectric properties of 0.7Pb(Mg1/3Nb2/3)O3-0.3PbTiO3 (PMN-PT) single crystals, a hole-doped manganite film/PMN-PT heterostructure has been constructed to achieve electric-field and light co-control of physical properties. Here, we report the resistivity switching behavior of Eu0.7Sr0.3MnO3/PMN-PT(111) multiferroic heterostructures under different in-plane reading currents, temperatures, light stimuli and electric fields, and discuss the underlying coupling mechanisms of resistivity change. The transition from the electric-field induced lattice strain effect to polarization current effect can be controlled effectively by decreasing the in-plane reading current at room temperature. With the decrease of temperature, the interfacial charge effect dominates over the lattice strain effect due to the reduced charge carrier density. In addition, light stimulus can lead to the delocalization of eg carriers, and thus enhance the lattice strain effect and suppress the interfacial charge effect. This work helps to understand essential physics of magnetoelectric coupling and also provides a potential method to realize energy-efficient multi-field control of manganite thin films.

Electric field control of magnetization reversal in FeGa/PMN-PT thin films

Abstract Artificial magnetoelectric materials possess huge potential to be utilized in the development of energy efficient spintronic devices. In the past decade, the search for a good ferromagnetic/ferroelectric combination having the ability to create high magnetoelectric coupling, created new insights and also new challenges. In this report, the magnetoelectric effect is studied in the FeGa/PMN-PT(001) multiferroic heterostructures in the presence of electric fields via strain-mediated effects. The formation of magnetic anisotropy in FeGa is observed after changing the polarization of PMN-PT to out-of-plane orientations. The magnetic domain structures forming during the magnetization reversal were studied in compressive, tensile and remanent strained states. The changes in the magnetic properties were reversible after each cycling of the electric field polarity, hence creating a non-volatile system. The control of magnetization switching sustained by an ON–OFF electric field makes our multiferroic heterostructure suitable for application in low-power magnetoelectric based memory applications.

Nonvolatile switchable half-metallicity and magnetism in the MXene Hf2MnC2O2/Sc2CO2 multiferroic heterostructure.

Nonvolatile electrical control of two-dimensional (2D) van der Waals (vdW) magnetism is important for spintronic devices. Here, using first-principles calculations, we systematically investigated the magnetic properties of the MXene Hf2MnC2O2 combined with the ferroelectric MXene Sc2CO2. When flipping the electric polarization of Sc2CO2, a transition between a semiconductor and a half-metal occurs in the Hf2MnC2O2 monolayer. Moreover, the ferromagnetic exchange parameter J1 can be enhanced to 9.67 meV under polarized P↑ of Sc2CO2, much larger than those of the pristine Hf2MnC2O2 monolayer and Hf2MnC2O2/Sc2CO2-P↓. In addition, the easy magnetization axis of the Hf2MnC2O2 monolayer is also dependent on the polarization orientation of Sc2CO2. Our results indicate a multiferroic heterostructure based on MXenes, offering an effective way for obtaining nonvolatile electrical control of electronic and magnetic properties.

Magneto-electric coupling beyond van der Waals interaction in two-dimensional multiferroic heterostructures

Exploring two-dimensional (2D) multiferroic systems with strong magneto-electric coupling properties holds significant application value in nanoscale spintronics devices. However, due to the weak interlayer van der Waals interactions, strong magneto-electric coupling in 2D heterostructures is relatively rare. By using first-principles simulations, we demonstrate that in the NiPS3/Sc2CO2 heterostructure, the ferroelectric polarization switching of the Sc2CO2 layer induces a transition in the magnetic ground state of the NiPS3 layer from the ferromagnetic state to antiferromagnetic ordering, accompanied by a transformation from a semiconductor to a half-metallic state. This magnetic phase transition is caused by a novel magneto-electric coupling mechanism: the polarization switching changes the band alignment between the two materials and then induces a significant interlayer charge transfer, leading to the emergence of Stoner itinerant ferromagnetism. In addition, the polarization switching can also change the magnetic anisotropy from an easy magnetization plane to an easy magnetization axis. These results not only offer a promising multiferroic heterostructure for nonvolatile memory devices and magnetic sensors but also provide a feasible approach for designing multiferroic system with strong magneto-electric coupling.