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At least 559 records · Page 31

Imitation of spin density wave order in Cu 3 Nb 2 O 8

Spin density waves, based on modulated local moments, are usually associated with metallic materials, but have recently been reported in insulators which display coupled magnetic and structural order parameters. Here, we discuss one such example, the multiferroic Cu 3 Nb 2 O 8 , which is reported to undergo two magnetic phase transitions, first to an unknown antiferromagnetic phase at $T_N$ ≈ 26.5 K , and then to a helicoidal structure coupled to an electric polarization below $T_2$ ≈ 24 K which breaks the crystallographic inversion symmetry. By analogy with other complex oxides, one might naturally expect this intermediate phase to be a spin density wave phase. We apply spherical polarimetry to confirm the low-temperature magnetic structure, yet only observe a single magnetic phase transition to helicoidal order. We argue that the reported unknown phase actually supports an imitation spin density wave which originates from a decoupling of the components of the magnetic order parameter, as allowed by symmetry and driven by thermal fluctuations. This provides a mechanism for the magnetic, but not nuclear, structure to break inversion symmetry thereby creating an intermediate phase in the proximity of $T_N$ which imitates a spin density wave. As the temperature is reduced, this intermediate structure destabilizes the crystal such that a structural chirality is induced, as reflected by the emergence of the electric polarization, and the imitation spin density wave relaxes into a generic helicoid. This scenario in which critical fluctuations allow the magnetic structure to break inversion symmetry while the crystal structure remains centrosymmetric might be relevant to other complex multiferroics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Observation of orbital selective charge transfer in a Fe/BaTi⁢O 3 interfacial two-dimensional electron gas

Two-dimensional electron gas (2DEG) states at oxide interfaces between two ferroic materials have been fertile ground to realize controllable multiferroicity. Here, in this work, we investigate the 2DEG states at the interface of ferroelectric BaTi⁢O 3 and a magnetic layer of iron using angle-resolved photoemission spectroscopy. Orbital-selective charge transfer occurs on the surprisingly robust 2DEG. Based on first-principles calculations, we show how the interfacial hybridization can give rise to the unexpected charge transfer in the magnetic 2DEG. Our study reveals a close interplay on a 2DEG between magnetic and ferroelectric interfaces, which sheds light on future design principles of multiferroic 2DEG states.

36 MATERIALS SCIENCE↗

Pinning, rotation, and metastability of BiFeO 3 cycloidal domains in a magnetic field

Earlier models for the room-temperature multiferroic BiFeO 3 implicitly assumed that a very strong anisotropy restricts the domain wave vectors q to the threefold-symmetric axis normal to the static polarization P. However, recent measurements demonstrate that the domain wave vectors q rotate within the hexagonal plane normal to P away from the magnetic field orientation m. In this paper, we show that the previously neglected threefold anisotropy K 3 restricts the wave vectors to lie along the threefold axis in zero field. Taking m to lie along a threefold axis, the domain with q parallel to m remains metastable below B c1 ≈7 T. Due to the pinning of domains by nonmagnetic impurities, the wave vectors of the other two domains start to rotate away from m above 5.6 T, when the component of the torque τ=M×B along P exceeds a threshold value τ pin . Since τ=0 when m⊥q, the wave vectors of those domains never become completely perpendicular to the magnetic field. Our results explain recent measurements of the critical field as a function of field orientation, small-angle neutron scattering measurements of the wave vectors, as well as spectroscopic measurements with m along a threefold axis. Finally, the model developed in this paper also explains how the three multiferroic domains of BiFeO 3 for a fixed P can be manipulated by a magnetic field.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Strain-induced ferroelectricity and spin-lattice coupling in SrMn O 3 thin films

Designing novel multiferroic materials with simultaneous ferroelectric and magnetic orders has been one of the focal points over the last decade due to the promising applications and rich physics involved. In this study, using epitaxial strain (up to 3.8%) as tuning knob, we successfully introduce multiferroicity with prominent high-temperature ferroelectricity into the paraelectric SrMnO3.More interestingly, the experimental temperature-dependent ferroelectric and magnetic studies suggest that the emergent antiferromagnetic order below 100 K greatly enhances the ferroelectric polarization due to the spin-order-induced ionic displacements. We envision that the strain-mediated spin-phonon coupling can be utilized as a pathway to discover functionalities in a wide range of antiferromagnetic insulators with delicate epitaxial manipulations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Linearly aligned single-chiral vortices in hexagonal manganites by in situ electric arc heating

Nanoscale topological defects, such as vortices and skyrmions in ferroic systems, have been intensively investigated due to their intriguing properties and behaviors. In addition to harnessing and tuning their functionalities, spatial manipulation and control of topological defects as functional elements are important for future nanotechnologies. Here in this paper, we report a linear alignment behavior of single-chiral vortices observed in thin transmission electron microscopy samples of multiferroic hexagonal manganites during an in situ heating experiment. In order to avoid chemical degradation during high-temperature heating in vacuum, we have utilized a rapid heating and quenching by in situ electric arcing. Using atomic resolution electron microscopy and phase-field simulation, we found that vortices and antivortices formed near the phase transition temperature are pulled out in the opposite directions by mechanical strain to leave single-chiral vortices linearly aligned along an isothermal line formed during quenching. In conclusion, Oour study provides important insight into spatial manipulation of the topological defects in oxide multiferroics by investigating far-equilibrium dynamics of symmetry-breaking continuous phase transitions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Interface reconstruction with emerging charge ordering in hexagonal manganite

Multiferroic materials, which simultaneously have multiple orderings, hold promise for use in the next generation of memory devices. We report a novel self-assembled MnO double layer forming at the interface between a multiferroic YMnO 3 film and a c-Al 2 O 3 substrate. The crystal structures and the valence states of this MnO double layer were studied by atomically resolved scanning transmission electron microscopy and spectroscopy, as well as density functional theory (DFT) calculations. A new type of charge ordering has been identified within this MnO layer, which also contributes to a polarization along the [001] direction. DFT calculations further establish the occurrence of multiple couplings between charge and lattice in this novel double layer, in addition to the polarization in nearby YMnO 3 single layer. The interface reconstruction reported here creates a new playground for emergent physics, such as giant ferroelectricity and strong magnetoelectric coupling, in manganite systems.

36 MATERIALS SCIENCE↗

Nanoscale ferroelastic twins formed in strained LaCoO 3 films

The coexistence and coupling of ferroelasticity and magnetic ordering in a single material offers a great opportunity to realize novel devices with multiple tuning knobs. Complex oxides are a particularly promising class of materials to find multiferroic interactions due to their rich phase diagrams, and are sensitive to external perturbations. Still, there are very few examples of these systems. Here, we report the observation of twin domains in ferroelastic LaCoO 3 epitaxial films and their geometric control of structural symmetry intimately linked to the material’s electronic and magnetic states. A unidirectional structural modulation is achieved by selective choice of substrates having twofold rotational symmetry. This modulation perturbs the crystal field–splitting energy, leading to unexpected in-plane anisotropy of orbital configuration and magnetization. These findings demonstrate the use of structural modulation to control multiferroic interactions and may enable a great potential for stimulation of exotic phenomena through artificial domain engineering.

36 MATERIALS SCIENCE↗

Scaling, rotation, and channeling behavior of helical and skyrmion spin textures in thin films of Te-doped Cu 2 OSeO 3

Topologically nontrivial spin textures such as vortices, skyrmions, and monopoles are promising candidates as information carriers for future quantum information science. Their controlled manipulation including creation and annihilation remains an important challenge toward practical applications and further exploration of their emergent phenomena. Here, we report controlled evolution of the helical and skyrmion phases in thin films of multiferroic Te-doped Cu 2 OSeO 3 as a function of material thickness, dopant, temperature, and magnetic field using in situ Lorentz phase microscopy. We report two previously unknown phenomena in chiral spin textures in multiferroic Cu 2 OSeO 3 : anisotropic scaling and channeling with a fixed-Q state. The skyrmion channeling effectively suppresses the recently reported second skyrmion phase formation at low temperature. Our study provides a viable way toward controlled manipulation of skyrmion lattices, envisaging chirality-controlled skyrmion flow circuits and enabling precise measurement of emergent electromagnetic induction and topological Hall effects in skyrmion lattices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Mössbauer study of the modulated magnetic structure of FeVO{sub 4}

Mössbauer spectroscopy is used to study the FeVO{sub 4} multiferroic, which undergoes two magnetic phase transitions at T{sub N1} ≈ 22 K and T{sub N2} ≈ 15 K. The first transition (T{sub N1}) is related to transformation from a paramagnetic state into a magnetically ordered state of a spin density wave, and the second transition (T{sub N2}) is associated with a change in the type of the spatial magnetic structure of the vanadate. The electric field gradient tensor at {sup 57}Fe nuclei is calculated to perform a crystal-chemical identification of the partial Mössbauer spectra corresponding to various crystallographic positions of Fe{sup 3+} cations. The spectra measured in the range T{sub N2} < T < T{sub N1} are analyzed on the assumption about amplitude modulation of the magnetic moments of iron atoms μ{sub Fe}. The results of model intersection of the spectra recorded at T < T{sub N2} point to a high degree of anharmonicity of the helicoidal magnetic structure of the vanadate and to elliptic polarization of μ{sub Fe}. These features are characteristic of type-II multiferroics. The temperature dependences of the hyperfine interaction parameters of {sup 57}Fe nuclei that were obtained in this work are analyzed in terms of the Weiss molecular field model on the assumption of orbital contribution to the magnetic moments of iron cations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

The Origin and Coupling Mechanism of the Magnetoelectric Effect in TM Cl 2 -4SC(NH 2 ) 2 ( TM = Ni and Co)

Most research on multiferroics and magnetoelectric effects to date has focused on inorganic oxides. Molecule-based materials are a relatively new field in which to search for magnetoelectric multiferroics and to explore new coupling mechanisms between electric and magnetic order. We present magnetoelectric behavior in NiCl 2 -4SC(NH 2 ) 2 (DTN) and CoCl 2 -4SC(NH 2 ) 2 (DTC). These compounds form tetragonal structures where the transition metal ion (Ni or Co) is surrounded by four electrically polar thiourea molecules [SC(NH 2 ) 2 ]. By tracking the magnetic and electric properties of these compounds as a function of magnetic field, we gain insights into the coupling mechanism by observing that, in DTN, the electric polarization tracks the magnetic ordering, whereas in DTC it does not. For DTN, all electrically polar thiourea molecules tilt in the same direction along the c -axis, breaking spatial-inversion symmetry, whereas, for DTC, two thiourea molecules tilt up and two tilt down with respect to c -axis, perfectly canceling the net electrical polarization. Thus, the magnetoelectric coupling mechanism in DTN is likely a magnetostrictive adjustment of the thiourea molecule orientation in response to magnetic order.

Mun, Eundeok↗

Strain-dependence Of The Structure And Ferroic Properties Of Epitaxial NiTiO3 Thin Films Grown On Different Substrates

Polarization-induced weak ferromagnetism has been predicted a few years back in perovskite MTiO3 (M = Fe, Mn, Ni) [Fennie, Phys. Rev. Lett. 100, 167203 (2008)]. We set out to stabilize this metastable perovskite structure by growing NiTiO3 epitaxially on different substrates, and to investigate the dependence of polar and magnetic properties on strain. Epitaxial NiTiO3 films were deposited on Al2O3, Fe2O3, and LiNbO3 substrates by pulsed laser deposition, and characterized using several techniques. The effect of substrate choice on lattice strain, film structure, and physical properties was investigated. Our structural data from x-ray diffraction and electron microscopy shows that substrate-induced strain has a marked effect on the structure and crystalline quality of the films. Physical property measurements reveal a dependence of the weak ferromagnetism and lattice polarization on strain, and highlight our ability to control the ferroic properties in NiTiO3 thin films by the choice of substrate. Our results are also consistent with the theoretical prediction that the ferromagnetism in acentric NiTiO3 is polarization-induced. From the substrates studied here, the perovskite substrate LiNbO3 proved to be the most promising one for strong multiferroism.

Environmental Molecular Sciences Laboratory↗

Magnetoelectric Composites: Applications, Coupling Mechanisms, and Future Directions

Multiferroic (MF)-magnetoelectric (ME) composites, which integrate magnetic and ferroelectric materials, exhibit a higher operational temperature (above room temperature) and superior (several orders of magnitude) ME coupling when compared to single-phase multiferroic materials. Room temperature control and the switching of magnetic properties via an electric field and electrical properties by a magnetic field has motivated research towards the goal of realizing ultralow power and multifunctional nano (micro) electronic devices. Here, some of the leading applications for magnetoelectric composites are reviewed, and the mechanisms and nature of ME coupling in artificial composite systems are discussed. Ways to enhance the ME coupling and other physical properties are also demonstrated. Finally, emphasis is given to the important open questions and future directions in this field, where new breakthroughs could have a significant impact in transforming scientific discoveries to practical device applications, which can be well-controlled both magnetically and electrically.

36 MATERIALS SCIENCE↗

Ultralow Voltage Manipulation of Ferromagnetism

Spintronic elements based on spin transfer torque have emerged with potential for on-chip memory, but they suffer from large energy dissipation due to the large current densities required. In contrast, an electric-field-driven magneto-electric storage element can operate with capacitive displacement charge and potentially reach 1-10 µJ cm -2 switching operation. In this paper, magneto-electric switching of a magnetoresistive element is shown, operating at or below 200 mV, with a pathway to get down to 100 mV. A combination of phase detuning is utilized via isovalent La substitution and thickness scaling in multiferroic BiFeO 3 to scale the switching energy density to ≈10 µJ cm -2 . This work provides a template to achieve attojoule-class nonvolatile memories.

36 MATERIALS SCIENCE↗

Strain‐Control of Cycloidal Spin Order in a Metallic Van der Waals Magnet

Abstract The manipulation of magnetism through strain control is a captivating area of research with potential applications for low‐power devices that do not require dissipative currents. Recent investigations of insulating multiferroics have unveiled tunable relationships among polar lattice distortions, Dzyaloshinskii–Moriya interactions (DMI), and cycloidal spin orders that break inversion symmetry. These findings have raised the possibility of utilizing strain or strain gradient to manipulate intricate magnetic states by changing polarization. However, the effectiveness of manipulating cycloidal spin orders in “metallic” materials with screened magnetism‐relevant electric polarization remains uncertain. In this study, the reversible strain control of cycloidal spin textures in a metallic van der Waals magnet, Cr 1/3 TaS 2 , through the modulation of polarization and DMI induced by strain is demonstrated. With thermally‐induced biaxial strains and isothermally‐applied uniaxial strains, systematic manipulation of the sign and wavelength of the cycloidal spin textures is realized, respectively. Additionally, unprecedented reflectivity reduction under strain and domain modification at a record‐low current density are also discovered. These findings establish a connection between polarization and cycloidal spins in metallic materials and present a new avenue for utilizing the remarkable tunability of cycloidal magnetic textures and optical functionality in van der Waals metals with strain.

36 MATERIALS SCIENCE↗

Designed Spin‐Texture‐Lattice to Control Anisotropic Magnon Transport in Antiferromagnets

Abstract Spin waves in magnetic materials are promising information carriers for future computing technologies due to their ultra‐low energy dissipation and long coherence length. Antiferromagnets are strong candidate materials due, in part, to their stability to external fields and larger group velocities. Multiferroic antiferromagnets, such as BiFeO 3 (BFO), have an additional degree of freedom stemming from magnetoelectric coupling, allowing for control of the magnetic structure, and thus spin waves, with the electric field. Unfortunately, spin‐wave propagation in BFO is not well understood due to the complexity of the magnetic structure. In this work, long‐range spin transport is explored within an epitaxially engineered, electrically tunable, 1D magnonic crystal. A striking anisotropy is discovered in the spin transport parallel and perpendicular to the 1D crystal axis. Multiscale theory and simulation suggest that this preferential magnon conduction emerges from a combination of a population imbalance in its dispersion, as well as anisotropic structural scattering. This work provides a pathway to electrically reconfigurable magnonic crystals in antiferromagnets.

36 MATERIALS SCIENCE↗

Asymmetric Character of the Ferroelectric Phase Transition and Charged Domain Walls in a Hybrid Improper Ferroelectric

Abstract In improper ferroelectrics, the spontaneous ordering is typically driven by a structural distortion or a magnetic spin alignment. The induced electric polarization is only a secondary effect. This dependence is a rich source for unusual phenomena and ferroelectric domain configurations for proper, polarization‐driven ferroelectrics. This study focuses on the polar domain structure and the hysteretic behavior at the ferroelectric phase transition in Ca 3 Mn 1.9 Ti 0.1 O 7 as a representative of the recently discovered hybrid improper ferroelectric class of multiferroics. Combining optical second harmonic generation and Raman spectroscopy gives access to the spontaneous structural distortion and the resulting improper electric polarization. This study shows that hybrid improper ferroelectrics contrast proper and improper ferroelectrics in several ways. Most intriguingly, adjacent ferroelectric domains favor head‐to‐head and tail‐to‐tail domain walls over charge‐neutral configurations. Furthermore, the phase transition occurs in an asymmetric fashion. The regime of phase coexistence of the nonpolar and polar phases shows a clear and abrupt upper temperature limit. In contrast, the coexistence toward low temperatures is best described as a fade‐out process, where 100‐nm‐sized islands of the nonpolar phase expand deep into the polar phase.

36 MATERIALS SCIENCE↗

Applications of Strain-Coupled Magnetoelectric Composites

This article deals with research, development and future directions of magnetoelectric composites for practical devices applications. In the past 20 years there has been a surge of research in the area of multiferroics (MF) and magnetoelectrics (ME) due to their potential to replace existing technologies based only on ferroelectric or ferromagnetic materials. Some of the magnetoelectric composites show exceptionally high potential in the area of magnetic field sensors, however, work remains before commercialization can be realized. The cross coupling among various ferroic parameters in magnetoelectric composites is several orders higher than single phase magetoelectrics, which make its favorable for low detection (nT or pT) magnetic field sensors. Advances in both layered structures or controlled three-dimensional matrix composites for applications as magnetoelectric nonvolatile memory elements are both required. Robust cross-coupling among various parameters with more than four logic states and its compatibility with complementary-symmetry metal–oxide–semiconductor (CMOS) technology are the main requirements for heterostructure magnetoelectric thin films. The major hurdles in the area of magnetoelectric nonvolatile memory elements are poor interfacial properties and weak magnetoelectric coupling for high density fast read and write processes. Another potential area is strained coupled magneto-electric composites where magnetostriction mediated dimensional change in the magnetic layer effectively modulate the change in the dimension of piezoelectric layers via piezostriction, which leads to a strong ME coupling where their coupling magnitude is sufficient for magnetic field sensors. Energy harvesters based on magnetoelectric composites are also intriguing concepts to capture various types of waste energy, in the form mechanical vibration, pressure, wind energy, hydrothermal and waste temperature.

36 MATERIALS SCIENCE↗