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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Magnetoelectric Coupling in a Mn 4 Na–Organic Complex under Pulsed Magnetic Fields up to 73 T

Research on the magnetoelectric (ME) effect (or spin-electric coupling) in molecule-based magnetic materials is a relatively nascent but promising topic. Molecule-based magnetic materials have diverse magnetic functionalities that can be coupled to electrical properties. Here, in this study, we investigate a realization of ME coupling that is fundamental but not heavily studied─the coupling of magnetic spin level crossings to changes in electric polarization. A mixed-valence Mn 4 Na complex with a total ground-state spin S = 5/2 under zero magnetic field and S = 17/2 under high magnetic field undergoes a cascade of ground-state level crossings of the S z states with increasing magnetic field. Magnetization and electrical polarization measurements under pulsed magnetic fields up to 73 T show that each spin level crossing is accompanied by a significant change in electric polarization that is an even function of the applied magnetic field. A molecular Hamiltonian describing antiferromagnetic exchange in a distorted tetrahedron of three Mn III and one Mn II ions matches the data well. We conclude that the ME coupling is caused by magnetostriction within the polar molecule as it distorts to lower its magnetic exchange energy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Anomalous Magnetoelectric Coupling in the Paramagnetic State of a Chiral and Polar Magnet

Abstract Chiral magnets are excellent platforms for studying intertwined spin, charge, orbit, and lattice degrees of freedom in solid‐state materials. In this work, the anomalous magnetoelectric behavior in a chiral magnet K 2 Co 2 (SO 4 ) 3 is demonstrated using comprehensive experimental probes. This material adopts a P 2 1 3 chiral cubic structure at room temperature. Based on the results of high‐resolution synchrotron X‐ray diffraction, this study shows that the low‐temperature (<130 K) crystal structure is a P 2 1 monoclinic phase, both polar and chiral. Magnetic and thermodynamic measurements reveal highly frustrated magnetic interactions and possible non‐collinear antiferromagnetic ordering at an extremely low temperature ≈0.6 K. Critically, anomalous magnetoelectric correlations are experimentally detected in its paramagnetic temperature regime, which can arise from the synergetic interplay between magnetoelastic and piezoelectric effects. These findings thus indicate that K 2 Co 2 (SO 4 ) 3 is a unique material, displaying multiple emergent structural and magnetic phenomena. This is attributed to both its overall crystallographic symmetry and the fact that its magnetic ions are located at low‐symmetry sites.

Xu, Xianghan↗
DOE OSTI2024

Magnetic structure and magnetoelectric coupling in the antiferromagnet Co 5⁢ (Te⁢O 3 ) 4 ⁢Cl 2

The van der Waals (vdW) layered multiferroics, which host simultaneous ferroelectric and magnetic orders, have attracted attention not only for their potentials to be utilized in nanoelectric devices and spintronics, but also offer alternative opportunities for emergent physical phenomena. To date, the vdW layered multiferroic materials are still very rare. In this work, we have investigated the magnetic structure and magnetoelectric (ME) effects in Co 5 ⁢(Te⁢O 3 ) 4 ⁢Cl 2 , a promising multiferroic compound with antiferromagnetic (AFM) Néel point T N ~18 K. The neutron-powder diffraction reveals the noncoplanar AFM state with preferred Néel vector along the c axis, while a spin reorientation occurring between 8 and 15 K is identified, which results from the distinct temperature dependence of the nonequivalent Co site's moment in Co 5 ⁢(Te⁢O 3 ) 4 ⁢Cl 2 . Moreover, it is found that Co 5 ⁢(Te⁢O 3 ) 4 ⁢Cl 2 is one of the best vdW multiferroics studied so far in terms of the multiferroic performance. The measured linear ME coefficient exhibits the emergent oscillation dependence of the angle between magnetic field and electric field, and the maximal value is as big as 45 ps/m. Finally, it is suggested that Co 5 ⁢(Te⁢O 3 ) 4 ⁢Cl 2 is an appreciated platform for exploring the emergent multiferroicity in vdW layered compounds.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Magnetoelectric effect arising from a field-induced pseudo Jahn-Teller distortion in a rare-earth magnet

Magnetoelectric materials are attractive for several applications, including actuators, switches, and magnetic field sensors. Typical mechanisms for achieving a strong magnetoelectric coupling are rooted in transition metal magnetism. In sharp contrast, here we identify CsEr(MoO 4 ) 2 as a magnetoelectric material without magnetic transition metal ions, thus ensuring that the Er ions play a key role in achieving this interesting property. Our detailed study includes measurements of the structural, magnetic, and magnetoelectric properties of this material. Bulk characterization and neutron powder diffraction show no evidence for structural phase transitions down to 0.3 K and therefore CsEr(MoO 4 ) 2 maintains the room temperature P2/c space group over a wide temperature range without external magnetic field. These same measurements also identify collinear antiferromagnetic ordering of the Er 3+ moments below T N =0.87K. Complementary dielectric constant and pyroelectric current measurements reveal that a ferroelectric phase with a maximum polarization P~0.6 nC/cm 2 emerges when applying a modest external magnetic field, which indicates that this material has a strong magnetoelectric coupling. Finally, we argue that the magnetoelectric coupling in this system arises from a pseudo Jahn-Teller distortion induced by the magnetic field.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Ferroelectric Self-Polarization Controlled Magnetic Stratification and Magnetic Coupling in Ultrathin La 0.67 Sr 0.33 MnO 3 Films

Multiferroic oxide heterostructures consisting of ferromagnetic and ferroelectric components hold the promise for nonvolatile magnetic control via ferroelectric polarization, advantageous for the low-dissipation spintronics. Modern understanding of the magnetoelectric coupling in these systems involves structural, orbital, and magnetic reconstructions at interfaces. Previous works have long proposed polarization-dependent interfacial magnetic structures; however, direct evidence is still missing, which requires advanced characterization tools with near-atomic-scale spatial resolutions. Here, extensive polarized neutron reflectometry (PNR) studies have determined the magnetic depth profiles of PbZr 0.2 Ti 0.8 O 3 /La 0.67 Sr 0.33 MnO 3 (PZT/LSMO) bilayers with opposite self-polarizations. When the LSMO is 2–3 nm thick, the bilayers show two magnetic transitions on cooling. However, temperature-dependent magnetization is different below the lower-temperature transition for opposite polarizations. PNR finds that the LSMO splits into two magnetic sublayers, but the inter-sublayer magnetic couplings are of opposite signs for the two polarizations. Near-edge X-ray absorption spectroscopy further shows contrasts in both the Mn valences and the Mn–O bond anisotropy between the two polarizations. Finally, this work completes the puzzle for the magnetoelectric coupling model at the PZT/LSMO interface, showing a synergic interplay among multiple degrees of freedom toward emergent functionalities at complex oxide interfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Nonvolatile Magnetoelectric Switching of Magnetic Tunnel Junctions with Dipole Interaction

The magnetoelectric effect is technologically appealing because of its ability to manipulate magnetism using an electric field rather than magnetic field or current, thus providing a promising solution for the development of energy-efficient spintronics. Although 180° magnetization switching is vital to spintronic devices, the achievement of 180° magnetization switching via magnetoelectric coupling is still a fundamental challenge. Here, in this work, voltage-driven full resistance switching of a magnetic tunnel junction (MTJ) with dipole interaction on a ferroelectric substrate through switchable parallel/antiparallel magnetization alignment is demonstrated. Parallel magnetization alignment along the y direction is obtained under a bias magnetic field. By rotating the magnetic easy axis via strain-mediated magnetoelectric coupling, the parallel magnetizations in the MTJ reorient to the x axis with opposite paths because of dipole interaction, thus resulting in antiparallel alignment. Moreover, this voltage switching of MTJs is nonvolatile owing to variations in dipole interaction and can be well understood via phase field simulations. The results provide an avenue to realize electrical switching of MTJs and are significant for exploring energy-efficient spintronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Electrical control of magnetism by electric field and current-induced torques

The remanent magnetization of ferromagnets has long been studied and used to store binary information. While early magnetic memory designs relied on magnetization switching by locally generated magnetic fields, key insights in condensed matter physics later suggested the possibility of doing it by electrical means instead. In the 1990s, Slonczewski and Berger formulated the concept of current-induced spin torques in magnetic multilayers through which a spin-polarized current generated by a first ferromagnet may be used to switch the magnetization of a second one. This discovery drove the development of spin-transfer-torque magnetic random-access memories (MRAMs). More recent fundamental research revealed other types of current-induced torques named spin-orbit torques (SOTs) and will lead to a new generation of devices including SOT MRAMs and skyrmion-based devices. Parallel to these advances, multiferroics and their magnetoelectric coupling, first investigated experimentally in the 1960s, experienced a renaissance. Dozens of multiferroic compounds with new magnetoelectric coupling mechanisms were discovered and high-quality multiferroic films were synthesized (notably of BiFeO 3 ), also leading to novel device concepts for information and communication technology such as the magnetoelectric spin-orbit (MESO) transistor. The story of the electrical switching of magnetization, which is discussed in this review, is that of a dance between fundamental research (in spintronics, condensed matter physics, and materials science) and technology (MRAMs, MESO transistors, microwave emitters, spin diodes, skyrmion-based devices, components for neuromorphics, etc.). This pas de deux has led to major scientific and technological breakthroughs in recent decades (such as the conceptualization of pure spin currents, the observation of magnetic skyrmions, and the discovery of spin-charge interconversion effects). As a result, this field has not only propelled MRAMs into consumer electronics products but also fueled discoveries in adjacent research areas such as ferroelectrics or magnonics. Here, in this review, recent advances in the control of magnetism by electric fields and by current-induced torques are covered. Fundamental concepts in these two directions are reviewed first, their combination is then discussed, and finally current various families of devices harnessing the electrical control of magnetic properties for various application fields are addressed. The review concludes by giving perspectives in terms of both emerging fundamental physics concepts and new directions in materials science.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Evidence for a single-layer van der Waals multiferroic

Here we searched for signatures of type-II multiferroic order in ultrathin van der Waals materials, to determine if such a state, comprising coexisting electrical polarization and spin order with strong magnetoelectric effects, could persist down to a single-atomic layer. We reported the first observation of such a state in triangular lattice material NiI 2 . This system has a layered structure and built-in magnetic frustration that promotes a complex magnetic ground state with proper-screw spin helices. The spin helix pattern breaks inversion symmetry and induces electrical polarization via magnetoelectric coupling. We use circular dichroic Raman measurements to directly probe the magneto-chiral ground state and its electromagnon modes originating from dynamic magnetoelectric coupling. Using birefringence and second-harmonic generation measurements, we detect a highly anisotropic electronic state simultaneously breaking three-fold rotational and inversion symmetry. The evolution of the optical signatures as a function of temperature and layer number surprisingly revealed a multiferroic state that persists down to the ultrathin limit of monolayer NiI 2 . These observations establish NiI 2 and transition metal dihalides as a new platform for studying emergent multiferroic phenomena, chiral magnetic textures and ferroelectricity in the 2D limit.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Lattice symmetry breaking transition and critical size limit for ferroic orders in nanophase BiFeO3

Finite size effects on the ferroic orders in BiFeO 3 are studied by atomic pair distribution function analysis and magnetic measurements. While bulk rhombohedral BiFeO 3 exhibits ferroelectricity and antiferromagnetism with a cycloidal magnetic moment arrangement leading to zero magnetization and weak magnetoelectric coupling, BiFeO 3 nanoparticles with a size smaller than the spin cycloid period of 62 nm preserve their polar rhombohedral structure and develop ferromagnetism, thus exhibiting coexisting polarization and nonzero magnetization that enhances the magnetoelectric coupling. When the nanoparticles become smaller than 17 nm, however, their crystal lattice expands and becomes nonpolar cubic. They also become superparamagnetic and thus simultaneously cease exhibiting both ferroelectricity and ferromagnetism. Our findings shed light on the interaction between the lattice structure and ferroic orders in nanophase perovskites and also provide a rare example of a lattice symmetry breaking phase transition that determines their critical size.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Proton switching molecular magnetoelectricity

Abstract The convergence of proton conduction and multiferroics is generating a compelling opportunity to achieve strong magnetoelectric coupling and magneto-ionics, offering a versatile platform to realize molecular magnetoelectrics. Here we describe machine learning coupled with additive manufacturing to accelerate the design strategy for hydrogen-bonded multiferroic macromolecules accompanied by strong proton dependence of magnetic properties. The proton switching magnetoelectricity occurs in three-dimensional molecular heterogeneous solids. It consists of a molecular magnet network as proton reservoir to modulate ferroelectric polarization, while molecular ferroelectrics charging proton transfer to reversibly manipulate magnetism. The magnetoelectric coupling induces a reversible 29% magnetization control at ferroelectric phase transition with a broad thermal hysteresis width of 160 K (192 K to 352 K), while a room-temperature reversible magnetic modulation is realized at a low electric field stimulus of 1 kV cm −1 . The findings of electrostatic proton transfer provide a pathway of proton mediated magnetization control in hierarchical molecular multiferroics.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Magnetic structure of magnetoelectric multiferroic HoFeWO 6

The polar magnetic oxide, HoFeWO6, is synthesized, and its crystal structure, magnetic structure, and thermodynamic properties are investigated. HoFeWO 6 forms the polar crystal structure (space group Pna2 1 (#33)) due to the cation ordering of W 6+ and Fe 3+ . An antiferromagnetic transition at T N = 17 K is accompanied by a significant change in magnetic entropy with a value of ≈ 5 J kg -1 K-1 in a 70 kOe applied field. Temperature dependent neutron diffraction and magnetization data indicate that the Fe sublattice orders in a strongly non-collinear and non-coplanar arrangement below T N . The Fe ordering initially leads to induced ordering of the Ho spins such that the Ho spins also show behavior of long-range ordering that is evident from the neutron diffraction measurements. Below T ≈ 4 K, the Ho spins order independently and pull the Fe spins toward the direction of Ho spins. A comparison with the magnetic structures and corresponding ferroelectric properties of other members of RMWO 6 (R = Y, Sm-Tm, M = Cr, Fe, V) family indicate that the spontaneous polarization is due to the magnetic structure specific to the Fe sublattice through magnetoelectric coupling whereas the polarization is independent of the Ho sublattice.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Heterogeneous Integration of Freestanding Bilayer Oxide Membrane for Multiferroicity

Transition metal oxides exhibit a plethora of electrical and magnetic properties described by their order parameters. In particular, ferroic orderings offer access to a rich spectrum of fundamental physics phenomena, in addition to a range of technological applications. The heterogeneous integration of ferroelectric and ferromagnetic materials is a fruitful way to design multiferroic oxides. The realization of freestanding heterogeneous membranes of multiferroic oxides is highly desirable. In this study, epitaxial BaTiO 3 /La 0.7 Sr 0.3 MnO 3 freestanding bilayer membranes are fabricated using pulsed laser epitaxy. The membrane displays ferroelectricity and ferromagnetism above room temperature accompanying the finite magnetoelectric coupling constant. Further, this study reveals that a freestanding heterostructure can be used to manipulate the structural and emergent properties of the membrane. In the absence of the strain caused by the substrate, the change in orbital occupancy of the magnetic layer leads to the reorientation of the magnetic easy-axis, that is, perpendicular magnetic anisotropy. These results of designing multiferroic oxide membranes open new avenues to integrate such flexible membranes for electronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Non-volatile electric control of magnetic and topological properties of MnBi 2 Te 4 thin films

In this letter, we propose a mechanism to control the magnetic properties of topological quantum material (TQM) by using magnetoelectric coupling: this mechanism uses a heterostructure of TQM with two-dimensional (2D) ferroelectric material, which can dynamically control the magnetic order by changing the polarization of the ferroelectric material and induce possible topological phase transitions. This concept is demonstrated using the example of the bilayer MnBi 2 Te 4 on ferroelectric In 2 Se 3 or In 2 Te 3 , where the polarization direction of the 2D ferroelectrics determines the interfacial band alignment and consequently the direction of the charge transfer. This charge transfer, in turn, enhances the stability of the ferromagnetic state of MnBi 2 Te 4 and leads to a possible topological phase transition between the quantum anomalous Hall (QAH) effect and the zero plateau QAH. Our work provides a route to dynamically alter the magnetic ordering of TQMs and could lead to the discovery of new multifunctional topological heterostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Lithiation bridged molecular conducting magnets

Combining ferromagnetism and metallic conductivity has been extensively studied in contemporary materials science. However, building such multifunctionalities in molecular chemistry is particularly challenging, on which two collective properties are long considered as mutually exclusive. Here, we report molecular conducting magnet consisting of two-dimensional graphene and molecular planar magnetic networks bridged by electrochemical lithiation, exhibiting the co-existence of distinct magnetism and conductivity and magneto-electric coupling effects. Here, the room temperature magnetoresistance and magnetoelectric coupling coefficient of such complex solid reach 10.7% and 1.77 V/Oe cm, respectively, which can be further tailored by modulating the interaction between graphene and molecular magnetic network. In addition, the graphene passivation simultaneously introduces environmental stability of molecular mag-nets. The electrochemical lithiation offers a pathway towards coupling magnetism and conductivity in molecular complexes.

2D organic complexes↗