Guohua Dong

Deterministic Switching of Perpendicular Magnetic Anisotropy by Voltage Control of Spin Reorientation Transition in (Co/Pt)3/Pb(Mg1/3Nb2/3)O3–PbTiO3 Multiferroic Heterostructures

One of the central challenges in realizing multiferroics-based magnetoelectric memories is to switch perpendicular magnetic anisotropy (PMA) with a control voltage. In this study, we demonstrate electrical flipping of magnetization between the out-of-plane and the in-plane directions in (Co/Pt)3/(011) Pb(Mg1/3Nb2/3)O3-PbTiO3 multiferroic heterostructures through a voltage-controllable spin reorientation transition (SRT). The SRT onset temperature can be dramatically suppressed at least 200 K by applying an electric field, accompanied by a giant electric-field-induced effective magnetic anisotropy field (ΔHeff) up to 1100 Oe at 100 K. In comparison with conventional strain-mediated magnetoelastic coupling that provides a ΔHeff of only 110 Oe, that enormous effective field is mainly related to the interface effect of electric field modification of spin-orbit coupling from Co/Pt interfacial hybridization via strain. Moreover, electric field control of SRT is also achieved at room temperature, resulting in a ΔHeff of nearly 550 Oe. In addition, ferroelastically nonvolatile switching of PMA has been demonstrated in this system. E-field control of PMA and SRT in multiferroic heterostructures not only provides a platform to study strain effect and interfacial effect on magnetic anisotropy of the ultrathin ferromagnetic films but also enables the realization of power efficient PMA magnetoelectric and spintronic devices.

Ionic Liquid Gating Control of RKKY Interaction in FeCoB/Ru/FeCoB and (Pt/Co)2/Ru/(Co/Pt)2 Multilayers.

To overcome the fundamental challenge of the weak natural response of antiferromagnetic materials under a magnetic field, voltage manipulation of antiferromagnetic interaction is developed to realize ultrafast, high-density, and power efficient antiferromagnetic spintronics. Here, we report a low voltage modulation of Ruderman–Kittel–Kasuya–Yosida (RKKY) interaction via ionic liquid gating in synthetic antiferromagnetic multilayers of FeCoB/Ru/FeCoB and (Pt/Co)2/Ru/(Co/Pt)2. At room temperature, the distinct voltage control of transition between antiferromagnetic and ferromagnetic ordering is realized and up to 80% of perpendicular magnetic moments manage to switch with a small-applied voltage bias of 2.5 V. We related this ionic liquid gating-induced RKKY interaction modification to the disturbance of itinerant electrons inside synthetic antiferromagnetic heterostructure and the corresponding change of its Fermi level. Voltage tuning of RKKY interaction may enable the next generation of switchable spintronics between antiferromagnetic and ferromagnetic modes with both fundamental and practical perspectives.Energy efficient control of magnetization in antiferromagnetic materials is one of the key ingredients for antiferromagnetic spintronics. Here the authors demonstrate voltage control of RKKY interaction and magnetization switching in synthetic antiferromagnetic multilayers by ionic liquid gating.

Ionic Liquid Gating Control of Spin Reorientation Transition and Switching of Perpendicular Magnetic Anisotropy

Electric field (E-field) modulation of perpendicular magnetic anisotropy (PMA) switching, in an energy-efficient manner, is of great potential to realize magnetoelectric (ME) memories and other ME devices. Voltage control of the spin-reorientation transition (SRT) that allows the magnetic moment rotating between the out-of-plane and the in-plane direction is thereby crucial. In this work, a remarkable magnetic anisotropy field change up to 1572 Oe is achieved under a small operation voltage of 4 V through ionic liquid (IL) gating control of SRT in Au/[DEME]+ [TFSI]- /Pt/(Co/Pt)2 /Ta capacitor heterostructures at room temperature, corresponding to a large ME coefficient of 378 Oe V-1 . As revealed by both ferromagnetic resonance measurements and magnetic domain evolution observation, the magnetization can be switched stably and reversibly between the out-of-plane and in-plane directions via IL gating. The key mechanism, revealed by the first-principles calculation, is that the IL gating process influences the interfacial spin-orbital coupling as well as net Rashba magnetic field between the Co and Pt layers, resulting in the modulation of the SRT and in-plane/out-of-plane magnetization switching. This work demonstrates a unique IL-gated PMA with large ME tunability and paves a way toward IL gating spintronic/electronic devices such as voltage tunable PMA memories.

ALD preparation of high-k HfO2 thin films with enhanced energy density and efficient electrostatic energy storage

High-k dielectric HfO2 thin films with a predominant monoclinic phase were prepared by atomic layer deposition (ALD). The annealed HfO2 films exhibited a large dielectric constant, of up to er = 26 with a high breakdown field of over 4000 kV cm−1. The best performance with a maximum recoverable energy density of 21.3 J cm−3 and energy efficiency of 75% was obtained with the 63 nm HfO2 films. In addition, a well-defined temperature dependence of the energy storage properties from room temperature to 150 °C was demonstrated, indicating a stable energy density variation between 11.0 and 13.0 J cm−3 with a high energy efficiency of about 80%. These achievements provide a platform for synthesizing high-k dielectric thin films with enhanced energy densities and efficiencies.

Discovery of Enhanced Magnetoelectric Coupling through Electric Field Control of Two-Magnon Scattering within Distorted Nanostructures

Electric field control of dynamic spin interactions is promising to break through the limitation of the magnetostatic interaction based magnetoelectric (ME) effect. In this work, electric field control of the two-magnon scattering (TMS) effect excited by in-plane lattice rotation has been demonstrated in a La0.7Sr0.3MnO3 (LSMO)/Pb(Mn2/3Nb1/3)-PbTiO3 (PMN-PT) (011) multiferroic heterostructure. Compared with the conventional strain-mediated ME effect, a giant enhancement of ME effect up to 950% at the TMS critical angle is precisely determined by angular resolution of the ferromagnetic resonance (FMR) measurement. Particularly, a large electric field modulation of magnetic anisotropy (464 Oe) and FMR line width (401 Oe) is achieved at 173 K. The electric-field-controllable TMS effect and its correlated ME effect have been explained by electric field modulation of the planar spin interactions triggered by spin-lattice coupling. The enhancement of the ME effect at various temperatures and spin dynamics control are promising paradigms for next-generation voltage-tunable spintronic devices.

Recoverable Self-Polarization in Lead-Free Bismuth Sodium Titanate Piezoelectric Thin Films

Bismuth sodium titanate, Bi0.5Na0.5TiO3 (BNT), is a promising lead-free ferroelectric material. However, its potential applications have not been fully explored, mainly because of the complex domain structure arising from its intricate phase transitions. A deep and thorough study of its domain structure and polarization switching behavior will greatly help with understanding the polarization nature and with promoting future applications. In this work, we demonstrate that BNT polycrystalline films possess a highly ordered out-of-plane polarization (self-polarization) and randomly oriented in-plane polarizations. Interestingly, the inherent nature of polarization in the BNT films does not allow for the nonvolatile domain writing, as the switched polarization spontaneously and rapidly reverses to the initial orientation state once the external poling electric field is removed, making the self-polarization recoverable. Such a stable self-polarization vanishes gradually with temperature increasing over 150 °C but starts to recover to its initial state upon cooling down to 250 °C, and entirely recovers once the temperature is reduced to below 200 °C. Such interesting properties of BNT films are attributed to the combined effects of the free charges at the Pt electrode, (detected) cation vacancies at the oxide/Pt interface and the defects in oxide lattices. Our results make a step closer to fully understand the nature of polarization and related piezoelectricity in BNT. Such films with recoverable self-polarization are of great interest for applications as sensors, actuators, and transducers that can operate particularly under high temperatures and high electric field conditions.

Low voltage induced reversible magnetoelectric coupling in Fe3O4 thin films for voltage tunable spintronic devices

The ongoing demand for efficient and low-energy consumption spintronic devices has motivated the idea of manipulating magnetism by ionic liquid (IL) electrolyte gating at low voltages. Although magnetoelectric (ME) coupling has already been realized in some field-effect-transistor (FET) structures, some vital parameters such as giant ME coupling coefficient, excellent reversibility and low gating voltage seldom come at the same time, which greatly suppresses industrialization. Here we demonstrate a large 552 Oe spin dynamics modulation of Fe3O4 thin films induced at a gating voltage of Vg = +1.5 V in an IL-gated Au/[DEME]+[TFSI]−/Fe3O4/MgO heterostructure with good reversibility up to 80 cycles, giving rise to a high ME coefficient of 368 Oe V−1. Such a large ME tunability under low Vg could be attributed to the electric field (E-field) induced ionic transformation between Fe2+ and Fe3+ at the interface. The tiny thickness change (∼2 angstrom) and roughness change of Fe3O4 films under Vg = +1.5 V illustrated by in situ X-ray reflection (XRR) give a reasonable explanation of the outstanding reversible property. Interestingly, it is found that the Verwey transition temperature of Fe3O4 has a strong dependence on Vg, revealing the potential of IL gating control of the intrinsic spin ordering inside magnetic films. This work drives forward the low-voltage induced reversible ME coupling to high-performance spintronic devices.

Thermal Driven Giant Spin Dynamics at Three-Dimensional Heteroepitaxial Interface in Ni0.5Zn0.5Fe2O4/BaTiO3-Pillar Nanocomposites

Traditional magnetostrictive/piezoelectric laminated composites rely on the two-dimensional interface that transfers stress/strain to achieve the large magnetoelectric (ME) coupling, nevertheless, they suffer from the theoretical limitation of the strain effect and of the substrate clamping effect in real ME applications. In this work, 3D NZFO/BTO-pillar nanocomposite films were grown on SrTiO3 by template-assisted pulsed laser deposition, where BaTiO3 (BTO) nanopillars appeared in an array with distinct phase transitions as the cores were covered by NiZn ferrite (NZFO) layer. The perfect 3D heteroepitaxial interface between BTO and NZFO phases can be identified without any edge dislocations, which allows effective strain transfer at the 3D interface. The 3D structure nanocomposites enable the strong two magnon scattering (TMS) effect that enhances ME coupling at the interface and reduces the clamping effect by strain relaxation. Thereby, a large FMR field shift of 1866 Oe in NZFO/BTO-pillar nanocomposite was obtained at the TMS critical angle near the BTO nanopillars phase transition of 255 K.

Self-Polarization in Epitaxial Fully Matched Lead-Free Bismuth Sodium Titanate Based Ferroelectric Thin Films

The Bi0.5Na0.5TiO3-based ferroelectric is one of the most promising candidates for environment-friendly lead-free ferroelectric/piezoelectric materials for various applications such as actuators and micro-electromechanical systems. The understanding and tailoring of the ferro-(piezo-)electric properties of thin films, however, are strongly hindered by the formation of the defects such as dislocations, ion vacancies in the film, as well as by the complexity of the interface between the film and the substrate. An ideal system for the study of the polarization behavior in the ferro-(piezo-)electric film would be a fully matched system. In this work, monocrystalline 0.89Bi0.5Na0.5TiO3-0.11BaTiO3 thin films were epitaxially grown on (001)-oriented Nb-doped SrTiO3 substrates using a sol-gel technique. The films were almost fully lattice- and thermally matched with the substrate, thus avoiding the impact of dislocations and thermal stress. The films were self-poled by a built-in electric field, originating from the sedimentation of heavier atoms during the film preparation. As a consequence, an upward self-polarization was introduced into the films, giving rise to asymmetric phase hysteresis loops and domain switching current responses. These results highlight the importance of the interface complexity for the self-polarization of piezoelectric thin films, even for fully matched films, which will therefore facilitate the control of properties of piezoelectric films and their applications for various functional devices.

Ferroelectric Phase Transition Induced a Large FMR Tuning in Self-Assembled BaTiO3:Y3Fe5O12 Multiferroic Composites

Yttrium iron garnet (YIG) is of great importance in RF/microwave devices for its low loss, low intrinsic damping, and high permeability. Nevertheless, tuning of YIG-based multiferroics is still a challenge due to its near-zero magnetostriction and the difficulty of building epitaxial interface between ferromagnetic garnet and ferroelectric perovskite phases. In this work, the vertically aligned heterostructure of YIG:BTO/STO(001) with local epitaxial interface between BTO and YIG is well-constructed, where the single crystal BTO pillars are embedded in YIG matrix. A large magnetoelectric coupling effect that drives YIGs FMR shift up to 512 and 333 Oe (1-2 order greater than those of all state-of-the-art progresses) is obtained through BTO ferroelectric phase changes induced by temperature variation at 295 and 193 K, correspondingly. This record high magnetoelectric tunability of YIG paves a way toward thermal/electrical tunable YIG devices.