Magnons, the quanta of spin waves, have been extensively studied in a range of materials for spintronics, particularly for non-volatile logic-in-memory devices. Controlling magnons in conventional antiferromagnets and harnessing them in practical applications, however, remains a challenge. Here we demonstrate highly efficient magnon transport in a LaFeO3/BiFeO3/LaFeO3 all-antiferromagnetic system, which can be controlled electrically, making it highly desirable for energy-efficient computation. Leveraging spin-orbit-driven spin-charge transduction, we demonstrate that this material architecture permits magnon confinement in ultrathin antiferromagnets, enhancing the output voltage generated by magnon transport by several orders of magnitude, which provides a pathway to enable magnetoelectric memory and logic functionalities. Additionally, the non-volatility of the output voltage enables ultralow-power logic-in-memory processing, where magnonic devices can be efficiently reconfigured via electrically controlled magnon spin currents within magnetoelectric channels.
Nanostructures formed by spontaneously broken symmetry have provided new ways to manipulate quantum states. Specifically, topological structures with periodic spatial ordering, such as polar vortices and skyrmions, can be ideal hosts for creating engineered responses in both spatial and frequency domains. So far, however, only a few examples of such hierarchical engineering have been reported in the literature. Here we demonstrate that the spatially modulated piezoelectric response of a polar vortex structure can create strain waves with a characteristic nanoscale wavefront. Using time-resolved pump-probe resonant X-ray scattering and diffraction measurements, coupled with dynamical phase-field simulations, we show that the piezoelectric modulation of the spontaneously formed polar vortex crystal functions as an acoustic diffraction grating. This system converts incoming laterally uniform strain waves into outgoing waves with a characteristic sub-terahertz frequency, driven by an intrinsic excitation of the polar vortex crystal. Moreover, our phase-field simulations suggest that the dynamic mechanical displacements exhibiting vortex textures are generated from both space- and time-varying piezoelectric responses. Our findings illustrate a new method for generating nanoscale strain waves with unique spatial textures by tuning the hierarchical order of polar topologies to engineer new collective modes, allowing for a wide range of control through the topological lattice.
Resonators are a key component in modern communications and computing. As demand and technological advances push component requirements into the terahertz regime, there is significant research devoted to the search for resonances at these frequencies. While uniform solid-state materials usually do not intrinsically feature resonances in this frequency range, self-assembled periodic arrays of ferroelectric nanodomains may provide an engineering route to design millimeter-wave properties. Here, we utilize prototypical dielectric-ferroelectric SrTiO3/PbTiO3 superlattices to robustly design periodic ferroelectric nano-scale domains. Phase field simulations predict an emergent domain breathing mode in complex polar textures and state-of-the-art millimeter-wave characterization shows evidence for such emergent resonances up to hundreds of GHz. Complex polar textures in these superlattices lead to emergent piezoelectric properties that also result in millimeter-wave resonances, which are predicted by second principles methods and confirmed by direct measurement. The principles investigated in this work suggest a new modality for ferroelectrics in the design of millimeter-wave electronics.
Magnetoelectric multiferroics, materials with intrinsically coupled electric polarization and magnetic order, promise ultralow-power switching, nonvolatile memory, and energy-efficient signal transduction. Yet practical deployment demands ultrathin films down to the atomic limit, where both orders typically degrade. Maintaining both order parameters at the thinnest scales in complex oxides remains a tremendous challenge, as uncompensated bound charge drives nanoscale depolarization in most ferroelectrics, while off-stoichiometry, reduced anisotropy, and charge transfer can produce magnetic dead layers in ultrathin oxides at substrate interfaces. Here, we realize a multiferroic phase of BiFeO3 that not only sustains both order parameters at room temperature with no dead layer but also exhibits signatures of emergent altermagnetism in the four-unit-cell, ultrathin limit. First-principles calculations, spin symmetry analysis, atomic-resolution imaging, and angle-resolved magnetic imaging reveal that short-circuit electrostatic boundary conditions, together with epitaxial strain, drive a continuous second-order, thickness-driven phase transition that enables the formation of multiferroic topological textures. Moreover, the imposed boundary conditions stabilize a d-wave altermagnetic time-reversal symmetry breaking, with corresponding signatures observed in magnetic circular dichroism. Collectively, these results establish a pathway to stabilize unconventional multiferroicity at device-relevant thicknesses, reframing scaling limits for oxide electronics.
Ferroelectric materials exhibit a spontaneous electric polarization that can be reversed byan electric field 1 , a property central to non-volatile memories 2,3 , sensors 4 and actuators 5,6 . In most conventional ferroelectric oxides, the polarization originates from a softening of a polar mode 7 . The amplitude of the mode along a given direction couples with the applied field along the same direction 8 . A long-standing challenge has been to achieve controlled switching of the in-plane polarization component using an out-of-plane electric field. We have discovered that a trilinear coupling between the in-plane and out-of-plane polarization, mediated via the octahedral tilts and rotations in the layered ferroelectric Bi 4 Ti 3 O 12 naturally fulfills these requirements and enables trans-switching of the polarization state. In its monoclinic phase, this material hosts a large in-plane polarization (∼ 50 μC cm -2 ) driven by a proper ferroelectric instability, together with smaller out-of-plane polarization (∼ 5 μC cm -2 ) of improper origin, induced by oxygen-octahedral distortions. We demonstrate that in c-axis-oriented epitaxial films the in-plane polarization switches deterministically under an out-of-plane electric field. This cross-coupling between orthogonal polarization components provides a route to transverse manipulation of ferroic order parameters and establishes layered ferroelectrics as a platform for capacitive computing concepts, analogous to the transconductance of modern CMOS electronics.
Ferroelectric materials exhibit a spontaneous electric polarization that can be reversed by an electric field1, a property central to non-volatile memories2,3, sensors4 and actuators5,6. In most conventional ferroelectrics, the polarization originates from a softening of a polar mode7. The amplitude of the mode along a given direction couples with the applied field along the same direction8. Ferroelectrics with a predominant in-plane polarization are harder to use in standard device geometries and therefore the field has mostly focused on out-of-plane ferroelectrics. Developing approaches that enable manipulation of the in-plane polarization component with an out-of-plane field would therefore provide new opportunities for device design and functionality. Here we have discovered that a trilinear coupling between the in-plane and out-of-plane polarization, mediated by means of the octahedral tilts and rotations in the layered ferroelectric Bi4Ti3O12, naturally fulfils this challenge and enables perpendicular switching of the polarization state. In its bulk monoclinic phase, this material hosts a large in-plane polarization (about 50 μC cm-2) driven by a proper ferroelectric instability, together with smaller out-of-plane polarization (about 5 μC cm-2) of improper origin, induced by oxygen octahedral distortions. We demonstrate that, in c-axis-oriented epitaxial films, the in-plane polarization switches deterministically under an out-of-plane electric field. This cross-coupling between orthogonal polarization components provides a route to transverse manipulation of ferroic order parameters and establishes layered ferroelectrics as a platform for capacitive computing concepts.
A systematic study of the effect of film thickness on the stability of the spin cycloid in BiFeO3 grown epitaxially on TbScO3 (110) substrates reveals a complex evolution of both the crystal and ferroelectric domain structures as well as the magnetic order. For films thicker than ∼5 nm, the structure remains rhombohedral, but the lattice mismatch is accommodated by the formation of 71° ferroelastic-closure domains, rather than misfit dislocations, followed by the formation of 109° domains. For films ≲ 5 nm, a mixed-phase coexistence of a polar, rhombohedral-like (R3c) phase and an antipolar (Pnma) phase is observed. Scanning nitrogen-vacancy magnetometry reveals a change in the propagation vector of the spin cycloid with thickness. It evolves from parallel to the ferroelectric domains for 50 nm thick samples and thicker and reorients to perpendicular to the ferroelectric domains for intermediate thicknesses, and vanishes for films ≲ 5 nm, which is reflected in macroscopic spin transport measurements and supported by the simulations. Ultimately, this work provides a deep understanding of the role of film thickness and electrostatic boundary conditions on the ferroelectric domain configuration and, therefore on the spin cycloid to design the device with electric field control antiferromagnetism.
BiFeO3 is a model multiferroic in which the ferroelectric polarization is coupled to ferroelastic lattice distortions, yet deterministic control of its domain structure remains limited by high switching fields and competing polarization variants. Here, we identify a mechanically assisted polarization switching pathway in epitaxial BiFeO3 thin films that fundamentally alters the switching energetics. Using just out-of-plane electric fields, polarization reversal requires voltages of approximately 4 volts and stabilizes coexisting polarization states. In contrast, when mechanical pressure is applied concurrently, the positive coercive voltage can be substantially reduced, even to 0 volts, resulting in spontaneous switching. Piezoresponse force microscopy measurements reveal that applied mechanical pressure suppresses ferroelastic domain competition, indicating a decrease in the required electrical energy barrier associated with polarization rotation and domain wall motion. This frames the strain field from the AFM tip directly as an effective voltage that assists in ferroelectric switching. By directly coupling lattice distortions to polarization reversal, mechanically assisted switching provides a general framework for controlling coupled order parameters in multiferroic oxides, which can be directly applied in the device-level architecture, where a small mechanical pressure can help in achieving a lower switching energy of ferroelectric polarization. This work advances the fundamental understanding of electromechanical coupling in complex ferroics and establishes mechanical energy as a powerful tool for probing and manipulating ferroelastic-ferroelectric interactions.
Electric field-induced magnetization reversal accompanying polarization switching is promising for low-power consumption, nonvolatile, voltage-write, magnetic-read memory applications. Perovskite BiFe0.9Co0.1O3 is a room-temperature multiferroic material in which both ferroelectric and weakly ferromagnetic orders coexist, with spontaneous magnetization coupled to the ferroelectric polarization. Here, we report electric field-induced ferroelectric and ferromagnetic domain changes in BiFe0.9Co0.1O3 nanodots using a combination of piezoresponse microscopy and scanning nitrogen-vacancy center magnetometry assisted by image analysis techniques to directly observe both ferroic orders on the nanometer scale. The complex ferroelectric domains present in a 190-nanometer structure which can be switched from a net-down to a net-up polarization by scanning with a biased cantilever, accompanied by reversal of both in-plane and out-of-plane components of the magnetization. This directly demonstrates electric field-induced magnetization reversal accompanying 180° polarization switching in a complex structure of a scale relevant to the semiconductor industry, creating a potential path for next generation memory devices.
The coexistence of ferroelectric and antiferromagnetic order in BiFeO3 makes it promising for next-generation magnetoelectric devices. But, single-phase multiferroics with robust room-temperature polarization and magnetization are rare. Here, enhanced, room-temperature ferroelectric polarization (≈ 120 µC cm-2), saturation magnetization (≈ 40 emu cm-3), and strong magnetoelectric coupling (≈ 400 mV cm-1 Oe-1) are observed in epitaxial (1-x)BiFeO3-(x)BaTiO3 thin films. These values of magnetization and magnetoelectric coupling are, respectively, one- and two-orders of magnitude larger than those same properties in the widely studied parent material BiFeO3. This sought after combination of properties is found in a distinct tetragonal phase, which is different from rhombohedral and super-tetragonal variants of BiFeO3, that emerges at x = 0.2 to 0.3 via combined chemical substitution and epitaxial strain. Structural and physical-property characterization, along with first-principles calculations, reveal a transition from monoclinic to tetragonal symmetry and suggest that short-range ordering of the titanium in the tetragonal phase results in ferrimagnetic spin ordering. This work demonstrates a unique single-phase multiferroic combining strong polarization, magnetization, and magnetoelectric coupling achieved through manipulation of the coupled chemical order and spin order; thereby addressing a major challenge in multiferroics research and providing a path toward practical room-temperature, efficient charge-to-spin and spin-to-charge conversion technologies.
Nanoscale topological polar textures promise new functionalities for ferroelectric memories and logic, yet their three-dimensional structure and mesoscale organization remain experimentally inaccessible. Here we introduce depth-resolved electron diffraction imaging (DREDI), a fast, non-destructive, method that maps polarization with <50 nm lateral and <10 nm depth sensitivity within fraction of a second. Its high acquisition speed enables the first continuous polarization mapping across six orders of magnitude in length scale, from nanometers to millimeters. Using epitaxial BiFeO3 films, DREDI reveals a hidden depth evolution of polar textures: surface 71˚ stripes evolve into subsurface flux-closure vortices that bifurcate into three-fold vertices near the bottom interface. Cross-sectional multi-slice electron ptychography and phase-field modeling confirm these buried configurations and attribute them to strain heterogeneity and ferroelastic twinning in the SrRuO3 electrode. Large-area analysis further shows that vertex-like frustration forms a mesoscale percolating network above a critical length scale of 4 µm. DREDI enables real-time, volumetric studies of buried topological textures in ferroic nanomaterials.
Spin pumping, a central phenomenon in spintronics used to source pure spin currents, is best understood in collinear magnetic multilayers. There is not yet a unified Landau-Lifshitz-Gilbert (LLG) theory that captures the fieldlike and dampinglike torques in a generic noncollinear magnetic multilayer. Here, we theoretically expand the LLG phenomenology to incorporate both dynamic fieldlike and dampinglike torques arising from spin pumping within noncollinear magnetic materials. We find that often overlooked dynamic fieldlike torques are capable of unveiling inversion asymmetries present in magnetic multilayers. Consequently, spin pumping can be used to lift the spectral degeneracy between various magnon modes in noncollinear antiferromagnets. We experimentally confirm this magnon-magnon interaction in a synthetic antiferromagnetic tetralayer, which has highly noncollinear magnetization configurations when under the influence of an external field. Thus, we demonstrate how spin pumping can facilitate a magnon-magnon interaction, significantly expanding how magnonic interactions can be engineered into antiferromagnets and magnetic metamaterials.
Pulsed-laser deposition (PLD) is a powerful technique for growing complex oxides with controlled stoichiometry. To understand growth dynamics therein, it is common to leverage in situ spectroscopies, such as reflection high-energy electron diffraction (RHEED), to monitor surface crystallinity. Most commercial systems rely on video-rate cameras operating at 60-120 Hz that lack sufficient temporal resolution to capture growth dynamics at practical deposition frequencies. Here, a high-speed platform to record in situ dynamics via RHEED at >500 Hz is implemented. An open-source analysis package is designed to fit diffraction spots to 2D Gaussians, allowing single-pulse surface reconstruction kinetics extraction. Using homoepitaxially deposited (001)-oriented SrTiO3 as a model system, we demonstrate how high-speed RHEED can provide real-time insight into growth processes obscured by slower acquisition systems. By fitting the single-pulse intensity to a set of exponential functions, we observe changes in the characteristic decay time and mechanism correlated to the substrate step width and surface termination. We observe distinct surface effects, with diffraction intensity decaying on lower-energy TiO2-terminated surfaces and stabilizing on SrO- or mixed-terminated surfaces. Similarly, using an exponential model, the extracted characteristic time of adatom deposition decreases with increased density of bonding sites associated with mixed termination and narrower step widths. Ultimately, this work shows how increasing RHEED temporal resolution can uncover new insights into growth processes, with practical implications for the design and control of PLD processes. This experimental platform provides new capabilities to enable data-driven machine learning analysis and autonomous control systems to enhance the complexity and fecundity of PLD.
Pattern formation in spin systems with continuous-rotational symmetry (CRS) provides a powerful platform to study emergent complex magnetic phases and topological defects in condensed-matter physics. However, its understanding and correlation with unconventional magnetic order along with high-resolution nanoscale imaging are challenging. Here, we employ scanning nitrogen vacancy (NV) magnetometry to unveil the morphogenesis of spin cycloids at both the local and global scales within a single ferroelectric domain of (111)-oriented BiFeO 3 , which is a noncollinear antiferromagnet, resulting in formation of a glassy labyrinthine pattern. We find that the domains of locally oriented cycloids are interconnected by an array of topological defects and exhibit isotropic energy landscape predicted by first-principles calculations. We propose that the CRS of spin-cycloid propagation directions within the (111) drives the formation of the labyrinthine pattern and the associated topological defects such as antiferromagnetic skyrmions. Unexpectedly, reversing the as-grown ferroelectric polarization from [ 1 ¯ 1 ¯ 1 ¯ ] to [111] produces a noncycloidal NV image contrast which could be attributed to either the emergence of a uniformly magnetized state or a reversal of the cycloid polarity. These findings highlight that (111)-oriented BiFeO 3 is not only important for studying the fascinating subject of pattern formation but could also be utilized as an ideal platform for integrating novel topological defects in the field of antiferromagnetic spintronics.
Conventional racetrack memories move information by pushing magnetic domain walls or other spin textures with spin-polarized currents, but the accompanying Joule heating inflates their energy budget and can hamper scaling. Here we present a voltage-controlled, magnetoelectric racetrack in which transverse electric fields translate coupled ferroelectric-antiferromagnetic walls along BiFeO3 nanostrips at room temperature. Because no charge traverses the track, the switching dissipates orders of magnitude less energy than the most efficient spin-torque devices with more favourable scaling, making the scheme significantly more attractive at the nanoscale. We further uncover noncollinear topological magnetoelectric textures that emerge at domain walls in BiFeO3, where the nature of these topologies influences their stability upon translation. Among these are polar bi-merons and polar vertices magnetoelectrically coupled with magnetic cycloid disclinations and previously unobserved, topological magnetic cycloid twist topologies. We observe domain wall velocities of at least kilometres per second - matching or surpassing the fastest ferrimagnetic and antiferromagnetic racetracks and approaching the acoustic-phonon limit of BiFeO3 - while preserving these topologies over tens of micrometres. The resulting high velocity, low-energy racetrack delivers nanosecond access times without the thermal overhead of current-driven schemes, charting a path toward dense, ultralow-power racetrack devices which rely on spin texture translation.
Er3+ color centers are promising candidates for quantum science and technology due to their long electron and nuclear spin coherence times, as well as their desirable emission wavelength. By selecting host materials with suitable, controllable properties, we introduce new parameters that can be used to tailor the Er3+ emission spectrum. PbTiO3 is a well-studied ferroelectric material with known methods of engineering different domain configurations through epitaxial strain. By distorting the structure of Er3+-doped PbTiO3 thin films, we can manipulate the crystal fields around the Er3+ dopant. This is resolved through changes in the Er3+ resonant fluorescence spectra, tying the optical properties of the defect directly to the domain configurations of the ferroelectic matrix. Additionally, we are able to resolve a second set of peaks for films with in-plane ferroelectric polarization. We hypothesize these results to be due to either the Er3+ substituting different sites of the PbTiO3 crystal, differences in charges between the Er3+ dopant and the original substituent ion, or selection rules. Systematically studying the relationship between the Er3+ emission and the epitaxial strain of the ferroelectric matrix lays the pathway for future optical studies of spin manipulation by altering ferroelectric order parameters
Since Felix Bloch's introduction of the concept of spin waves in 1930, magnons (the quanta of spin waves) have been extensively studied in a range of materials for spintronics, particularly for non-volatile logic-in-memory devices. Controlling magnons in conventional antiferromagnets and harnessing them in practical applications, however, remains a challenge. In this letter, we demonstrate highly efficient magnon transport in an LaFeO$_3$/BiFeO$_3$/LaFeO$_3$ all-antiferromagnetic system which can be controlled electrically, making it highly desirable for energy-efficient computation. Leveraging spin-orbit-driven spin-charge transduction, we demonstrate that this material architecture permits magnon confinement in ultrathin antiferromagnets, enhancing the output voltage generated by magnon transport by several orders of magnitude, which provides a pathway to enable magnetoelectric memory and logic functionalities. Additionally, its non-volatility enables ultralow-power logic-in-memory processing, where magnonic devices can be efficiently reconfigured via electrically controlled magnon spin currents within magnetoelectric channels.