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At least 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

High-temperature structural phase transition in the LiCu{sub 2}O{sub 2} multiferroic

The results of thermogravimetric, X-ray diffraction, and electrical studies of LiCu{sub 2}O{sub 2} single crystals in the temperature range 300-1100 K are presented. A reversible first-order phase transition between the orthorhombic and tetragonal phases is found to occur in these single crystals at T = 993 K. A pronounced peak on a differential thermal analysis curve and jumps in the unit cell parameters and the electrical resistivity are detected at the phase-transition temperature. The data on the crystal structure of LiCu{sub 2}O{sub 2} and the phase transition-induced change in the entropy determined in this work are used to conclude that the revealed phase transition is caused by the ordering-disordering of Li{sup +} and Cu{sup 2+} cations in their structural positions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Organic Multiferroics (Final Technical Report)

The research objective of this project is to explore the unusual physical properties of molecular electronic crystal materials, comprised of two chemically and electronically distinct donor and acceptor molecules, which combine two or more properties in the same crystal lattice in a manner that is difficult or impossible to achieve in continuous inorganic crystalline solids.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Realization of Large Electric Polarization and Strong Magnetoelectric Coupling in BiMn 3 Cr 4 O 12

Here, magnetoelectric multiferroics have received much attention in the past decade due to their interesting physics and promising multifunctional performance. For practical applications, simultaneous large ferroelectric polarization and strong magnetoelectric coupling are preferred. However, these two properties have not been found to be compatible in the single–phase multiferroic materials discovered as yet. Here, it is shown that superior multiferroic properties exist in the A–site ordered perovskite BiMn 3 Cr 4 O 12 synthesized under high–pressure and high–temperature conditions. The compound experiences a ferroelectric phase transition ascribed to the 6s 2 lone–pair effects of Bi 3+ at around 135 K, and a long–range antiferromagnetic order related to the Cr 3+ spins around 125 K, leading to the presence of a type–I multiferroic phase with huge electric polarization. On further cooling to 48 K, a type–II multiferroic phase induced by the special spin structure composed of both Mn– and Cr–sublattices emerges, accompanied by considerable magnetoelectric coupling. BiMn 3 Cr 4 O 12 thus provides a rare example of joint multiferroicity, where two different types of multiferroic phases develop subsequently so that both large polarization and significant magnetoelectric effect are achieved in a single–phase multiferroic material.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Using interfaces to: create strongly-coupled magnetic-ferroelectrics

Starting at the level of electrons and atoms our long-term goal is to rationally design complex oxide heterostructures and interface-materials with targeted emergent behaviors. This is not a matter of simply optimizing material parameters, but rather begins with understanding a mechanism to control the interplay between the diverse microscopic degrees of freedom prevalent in complex oxides in order to create targeted macroscopic phenomena and ends with the design of new material realizations. These realizations are in turn created with atomic-layer precision, structurally assessed to see that they are the intended realization, and finally their relevant properties are measured. During this program we have developed the scientific ideas necessary to apply this materials-by-design paradigm to the creation of materials offering electrical control of magnetism. At the heart of our approach lies a partnership between theory, synthesis, and characterization. These are the areas of expertise of the three co-PIs, who have worked closely together since their arrival at Cornell. During this project bold ideas on where to put the atoms to provide electrical control of magnetism were met with the latest methods of synthesis science and electron microscopy in an attempt create targeted new multiferroics. Our work applying this materials-by-design methodology to multiferroics has enjoyed multiple successes. The Co-PIs have invented new mechanisms for multiferroics, which provide strong coupling between polarization and magnetism, and reduced them to practice. Specifically, we pioneered multiferroics based on spin-phonon coupling, rotation-driven multiferroicity, and novel geometric multiferroics. Importantly, the latter two of these mechanisms enable the deterministic switching of magnetism by an applied electric field, which is key to the application of multiferroics to future device technologies. Most recently, we performed detailed theoretical analysis on a system involving the combination of magnetoelectric and colossal magnetoresistance behaviors and predict that electrical control of a metal-insulator transition is possible in appropriately strained SmBaMn2O6. The research enabled by this grant led to 63 publications in leading refereed journals including Nature, Nature Materials, Physical Review Letters, and Advanced Materials demonstrating a materials-by-design paradigm to the creation of materials offering electrical control of magnetism.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Engineering of Ferroic Orders in Thin Films by Anionic Substitution

Multiferroics are a unique class of materials where magnetic and ferroelectric orders coexist. The research on multiferroics contributes significantly to the fundamental understanding of the strong correlations between different material degrees of freedom and provides an energy-efficient route toward the electrical control of magnetism. While multiple ABO 3 oxide perovskites are identified as being multiferroic, their magnetoelectric coupling strength is often weak, necessitating the material search in different compounds. Here, the observation of room-temperature multiferroic orders in multi-anion SrNbO 3-x N x thin films is reported. In these samples, the multi-anion state enables the room-temperature ferromagnetic ordering of the Nb d-electrons. Simultaneously, ferroelectric responses that originate from the structural symmetry breaking associated are found with both the off-center displacements of Nb and the geometric displacements of Sr, depending on the relative O-N arrangements within the Nb-centered octahedra. So findings not only diversify the available multiferroic material pool but also demonstrate a new multiferroism design strategy via multi-anion engineering.

thin-films↗
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 OSTI2013

Challenges and opportunities for multi-functional oxide thin films for voltage tunable radio frequency/microwave components

There has been significant progress on the fundamental science and technological applications of complex oxides and multiferroics. Among complex oxide thin films, barium strontium titanate (BST) has become the material of choice for room-temperature-based voltage-tunable dielectric thin films, due to its large dielectric tunability and low microwave loss at room temperature. BST thin film varactor technology based reconfigurable radio frequency (RF)/microwave components have been demonstrated with the potential to lower the size, weight, and power needs of a future generation of communication and radar systems. Low-power multiferroic devices have also been recently demonstrated. Strong magneto-electric coupling has also been demonstrated in different multiferroic heterostructures, which show giant voltage control of the ferromagnetic resonance frequency of more than two octaves. This manuscript reviews recent advances in the processing, and application development for the complex oxides and multiferroics, with the focus on voltage tunable RF/microwave components. The over-arching goal of this review is to provide a synopsis of the current state-of the-art of complex oxide and multiferroic thin film materials and devices, identify technical issues and technical challenges that need to be overcome for successful insertion of the technology for both military and commercial applications, and provide mitigation strategies to address these technical challenges.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Long-range magnetic order and relaxor ferroelectricity in a hexagonal high-entropy ferrite

Multiferroics that combine ferroelectricity and magnetic order are attractive for electronic and spintronic technologies, yet chemical disorder that promotes relaxor ferroelectricity usually suppresses long-range magnetic order. Here, we report entropy-stabilized relaxor multiferroicity in epitaxial hexagonal (Tb0.2Dy0.2Ho0.2Lu0.2Yb0.2)FeO3 thin films. Structural, magnetic, dielectric, and synchrotron spectroscopic measurements show the coexistence of relaxor ferroelectricity and long-range ferromagnetic order. We find that improper ferroelectricity remains robust against A-site configurational disorder, while the Fe sublattice preserves magnetic exchange. This separation of the microscopic origins of the polar and magnetic responses enables chemically disordered multiferroicity. Our results establish entropy engineering in hexagonal ferrites as a route toward multifunctional oxide thin films and provide a general design strategy for high-entropy multiferroics.

Miertschin, Duncan [Baylor University]↗
DOE OSTI2022

Interfacial antiferromagnetic phase induced two-step magnetization reversal in PbZr 0.52 Ti 0.48 O3/La 0.67 Sr 0.33 MnO 3 superlattices

Artificial multiferroic heterostructures have recently attracted much interests due to the demonstrated magnetoelectric coupling (MEC) and unique functionalities, promising a tantalizing perspective of novel applications in next-generation electronic, memory, sensor, and energy harvesting technologies. Herein, we report a two-step magnetization reversal in PbZr 0.52 Ti 0.48 O 3 /La 0.67 Sr 0.33 MnO 3 (PZT/LSMO) superlattices, which originates from the strongly entangled strain-, ferroelectric (FE)-polarization-, and exchange-dependent effects. Specifically, the preferential occupancy of the in-plane Mn d x 2 -y 2 orbitals is triggered via the collective effects of the large tensile strain and FE polarization, giving rise to an interfacial antiferromagnetic (AFM) layer with strong AFM anisotropy. The strong spin exchange coupling between the AFM layer and the adjacent ferromagnetic (FM) layer facilitates the magnetic stratification of the FM layer, leading to two coercivities, i.e., two-step magnetization reversal. Meanwhile, a sizeable exchange bias (EB) field is induced. The emerged two-step magnetization reversal concomitant with the pronounced EB phenomenon should be a signature of an enhanced MEC in PZT/LSMO superlattices. Finally, our results will stimulate further interests in multiferroic superlattices in applications of multiferroic-based devices.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Giant magnetoelectric effects achieved by tuning spin cone symmetry in Y-type hexaferrites

Multiferroics materials, which exhibit coupled magnetic and ferroelectric properties, have attracted tremendous research interest because of their potential in constructing next-generation multifunctional devices. The application of single-phase multiferroics is currently limited by their usually small magnetoelectric effects. Here, we report the realization of giant magnetoelectric effects in a Y-type hexaferrite Ba 0.4 Sr 1.6 Mg 2 Fe 12 O 22 single crystal, which exhibits record-breaking direct and converse magnetoelectric coefficients and a large electric-field-reversed magnetization. We have uncovered the origin of the giant magnetoelectric effects by a systematic study in the Ba 2-x Sr x Mg 2 Fe 12 O 22 family with magnetization, ferroelectricity and neutron diffraction measurements. With the transverse spin cone symmetry restricted to be two-fold, the one-step sharp magnetization reversal is realized and giant magnetoelectric coefficients are achieved. Our study reveals that tuning magnetic symmetry is an effective route to enhance the magnetoelectric effects also in multiferroic hexaferrites.

36 MATERIALS SCIENCE↗
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 OSTI2025

Electrical switching of a p-wave magnet

Magnetic states with zero magnetization but non-relativistic spin splitting are outstanding candidates for the next generation of spintronic devices. Their electronvolt (eV)-scale spin splitting, ultrafast spin dynamics and nearly vanishing stray fields make them particularly promising for several applications. A variety of such magnetic states with non-trivial spin textures have been identified recently, including even-parity d-wave, g-wave or i-wave altermagnets and odd-parity p-wave magnets. Achieving voltage-based control of the non-uniform spin polarization of these magnetic states is of great interest for realizing energy-efficient and compact devices for information storage and processing. Spin-spiral type II multiferroics are optimal candidates for such voltage-based control, as they exhibit an inversion-symmetry-breaking magnetic order that directly induces ferroelectric polarization, allowing for symmetry-protected cross-control between spin chirality and polar order. Here we combine photocurrent measurements, first-principles calculations and group-theory analysis to provide direct evidence that the spin polarization of the spin-spiral type II multiferroic NiI 2 exhibits odd-parity character connected to the spiral chirality. The symmetry-protected coupling between chirality and polar order enables electrical control of a primarily non-relativistic spin polarization. Our findings represent an observation of p-wave magnetism in a spin-spiral type II multiferroic, which may lead to the development of voltage-based switching of non-relativistic spin polarization in compensated magnets.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Room-temperature large magnetoelectricity in a transition metal doped ferroelectric perovskite

There is increasing interest in novel magnetoelectric (ME) materials that exhibit robust ME coupling at room-temperature (RT) for advanced memory, energy, spintronics, and other multifunctional device applications, by making use of the ability to control polarization with a magnetic field and/or magnetization via an electric field. Obtaining ME materials with strong ME coupling, understanding the origin, and manipulating its processing along with composition to realize large ME coefficients at RT constitute an important step in multiferroic research. To address this, we have investigated the multiferroic and ME properties of Ni-doped Pb(Zr 0.20 Ti 0.80 )O 3 (PZT). We find that the ferroelectric (T C ~ 700 K) and weak ferromagnetic (~ 602 K) phase transitions of Ni-doped PZT are well above RT, leading to a strong ME coupling coefficient (α E,31 ) of 11.7 mVcm -1 Oe -1 (H ac = 1 Oe and f = 1 kHz). While X-ray diffraction suggests a single-phase material, high resolution transmission electron microscopy reveals regions with and without Ni present; thus magnetoelectric coupling between two phases is possible. First-principle calculations suggest the (Ni Pb ) × defect is likely to be responsible for the experimental observed magnetism and ME coupling in Ni-doped PZT. Furthermore, we demonstrate that Ni-doped PZT exhibits low loss tangent, low leakage current, large saturation polarization and weak ferromagnetism. Ultimately, our work demonstrates that Ni-doped PZT is a cost-effective RT multiferroic with strong ME coupling.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Revealing the Effects of Trace Oxygen Vacancies on Improper Ferroelectric Manganite with In Situ Biasing

Abstract Multiferroic materials, which exhibit multiple orderings, are promising for next generation data‐storage device applications. YMnO 3 , in particular, because of the coexistence of the ferroelectricity and (anti)ferromagnetism within one single material, has drawn special attentions to application‐based research. However, the role of defect chemistry related to the behaviors of the ferroelectric polarization has been seldomly studied due to its complexity. In this work, a novel switching behavior of multiferroic YMnO 3 single crystal is reported using in situ biasing and Landau based numerical calculation. It is revealed that the domain switching only happens at the topmost surface, which can be well explained by the electric field redistribution due to the trace amount of oxygen vacancies. These in situ observations demonstrate that defect chemistry plays an important role in domain switching and can be utilized as an additional parameter for controlling the distribution of electric field within the multiferroic materials.

Cheng, Shaobo↗