Enhanced Exchange Bias in Epitaxial High-Entropy Oxide Heterostructures.

High-entropy oxides (HEOs) have gained significant interest in recent years due to their unique structural characteristics and potential to tailor functional properties. However, the electronic structure of the HEOs currently remains vastly unknown. In this work, combining magnetometry measurements, scanning transmission electron microscopy, and element-specific X-ray absorption spectroscopy, the electronic structure and magnetic properties of the perovskite-HEO La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 epitaxial thin films are systemically studied. It is found that enhanced magnetic frustration emerges from competing exchange interactions of the five transition-metal cations with energetically favorable half-filled/full-filled electron configurations, resulting in an unprecedented large vertical exchange bias effect in the single-crystalline films. Furthermore, our findings demonstrate that the La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 layer with a thickness down to 1 nm can be used as a pinning layer and strongly coupled with a ferromagnetic La0.7Sr0.3MnO3 layer, leading to a notable exchange bias and coercivity enhancement in a cooling field as small as 5 Oe. Our studies not only provide invaluable insight into the electronic structure of HEOs but also pave the way for a new era of large bias materials for spintronics devices.

Real-space observation of ergodicity transitions in artificial spin ice.

Ever since its introduction by Ludwig Boltzmann, the ergodic hypothesis became a cornerstone analytical concept of equilibrium thermodynamics and complex dynamic processes. Examples of its relevance range from modeling decision-making processes in brain science to economic predictions. In condensed matter physics, ergodicity remains a concept largely investigated via theoretical and computational models. Here, we demonstrate the direct real-space observation of ergodicity transitions in a vertex-frustrated artificial spin ice. Using synchrotron-based photoemission electron microscopy we record thermally-driven moment fluctuations as a function of temperature, allowing us to directly observe transitions between ergodicity-breaking dynamics to system freezing, standing in contrast to simple trends observed for the temperature-dependent vertex populations, all while the entropy features arise as a function of temperature. These results highlight how a geometrically frustrated system, with thermodynamics strictly adhering to local ice-rule constraints, runs back-and-forth through periods of ergodicity-breaking dynamics. Ergodicity breaking and the emergence of memory is important for emergent computation, particularly in physical reservoir computing. Our work serves as further evidence of how fundamental laws of thermodynamics can be experimentally explored via real-space imaging.

Low-energy states, ground states, and variable frustrations of the finite-size dipolar Cairo lattices.

To investigate the influence of geometric frustration on the properties of low-energy configurations of systems of ferromagnetic nanoislands located on the edges of the Cairo lattice, the model of interacting Ising-like magnetic dipoles is used. By the method of complete enumeration, the densities of states of the Cairo pentagonal lattices of a finite number of Ising-like point dipoles are calculated. The calculated ground and low-energy states for systems with a small number of dipoles can be used to solve the problem of searching for the ground states in a system with a relatively large number of dipoles. It is shown that the ground-state energy of the Cairo pentagonal lattices exhibits nonmonotonic behavior on one of the lattice parameters. The lattice parameters can be used to control the degree of geometric frustration. For the studied lattices of a finite number of Ising dipoles on the Cairo lattice in the ground-state configurations, a number of closed pentagons is observed, which are different from the obtained maximum closed pentagons. The magnetic order in the ground-state configurations obeys the ice rule and the quasi-ice rules.

Manipulating magnetoelectric energy landscape in multiferroics.

Magnetoelectric coupling at room temperature in multiferroic materials, such as BiFeO3, is one of the leading candidates to develop low-power spintronics and emerging memory technologies. Although extensive research activity has been devoted recently to exploring the physical properties, especially focusing on ferroelectricity and antiferromagnetism in chemically modified BiFeO3, a concrete understanding of the magnetoelectric coupling is yet to be fulfilled. We have discovered that La substitutions at the Bi-site lead to a progressive increase in the degeneracy of the potential energy landscape of the BiFeO3 system exemplified by a rotation of the polar axis away from the 〈111〉pc towards the 〈112〉pc discretion. This is accompanied by corresponding rotation of the antiferromagnetic axis as well, thus maintaining the right-handed vectorial relationship between ferroelectric polarization, antiferromagnetic vector and the Dzyaloshinskii-Moriya vector. As a consequence, La-BiFeO3 films exhibit a magnetoelectric coupling that is distinctly different from the undoped BiFeO3 films.

Geometrical Frustration and Planar Triangular Antiferromagnetism in Quasi-Three-Dimensional Artificial Spin Architecture.

We present a realization of highly frustrated planar triangular antiferromagnetism achieved in a quasi-three-dimensional artificial spin system consisting of monodomain Ising-type nanomagnets lithographically arranged onto a deep-etched silicon substrate. We demonstrate how the three-dimensional spin architecture results in the first direct observation of long-range ordered planar triangular antiferromagnetism, in addition to a highly disordered phase with short-range correlations, once competing interactions are perfectly tuned. Our work demonstrates how escaping two-dimensional restrictions can lead to new types of magnetically frustrated metamaterials.

Elevated effective dimension in tree-like nanomagnetic Cayley structures.

Using state-of-the-art electron-beam lithography, Ising-type nanomagnets may be defined onto nearly any two-dimensional pattern imaginable. The ability to directly observe magnetic configurations achieved in such artificial spin systems makes them a perfect playground for the realization of artificial spin glasses. However, no experimental realization of a finite-temperature artificial spin glass has been achieved so far. Here, we aim to get a significant step closer in achieving that goal by introducing an artificial spin system with random interactions and increased effective dimension: dipolar Cayley tree. Through synchrotron-based photoemission electron microscopy, we show that an improved balance of ferro- and antiferromagnetic ordering can be achieved in this type of system. This combined with an effective dimension as high as d = 2.72 suggests that future systems generated out of these building blocks can host finite temperature spin glass phases, allowing for real-time observation of glassy dynamics.

Emergent magnetic monopole dynamics in macroscopically degenerate artificial spin ice.

Magnetic monopoles, proposed as elementary particles that act as isolated magnetic south and north poles, have long attracted research interest as magnetic analogs to electric charge. In solid-state physics, a classical analog to these elusive particles has emerged as topological excitations within pyrochlore spin ice systems. We present the first real-time imaging of emergent magnetic monopole motion in a macroscopically degenerate artificial spin ice system consisting of thermally activated Ising-type nanomagnets lithographically arranged onto a pre-etched silicon substrate. A real-space characterization of emergent magnetic monopoles within the framework of Debye-Hückel theory is performed, providing visual evidence that these topological defects act like a plasma of Coulomb-type magnetic charges. In contrast to vertex defects in a purely two-dimensional artificial square ice, magnetic monopoles are free to evolve within a divergence-free vacuum, a magnetic Coulomb phase, for which features in the form of pinch-point singularities in magnetic structure factors are observed.

Complex strain evolution of polar and magnetic order in multiferroic BiFeO3 thin films.

Electric-field control of magnetism requires deterministic control of the magnetic order and understanding of the magnetoelectric coupling in multiferroics like BiFeO3 and EuTiO3. Despite this critical need, there are few studies on the strain evolution of magnetic order in BiFeO3 films. Here, in (110)-oriented BiFeO3 films, we reveal that while the polarization structure remains relatively unaffected, strain can continuously tune the orientation of the antiferromagnetic-spin axis across a wide angular space, resulting in an unexpected deviation of the classical perpendicular relationship between the antiferromagnetic axis and the polarization. Calculations suggest that this evolution arises from a competition between the Dzyaloshinskii-Moriya interaction and single-ion anisotropy wherein the former dominates at small strains and the two are comparable at large strains. Finally, strong coupling between the BiFeO3 and the ferromagnet Co0.9Fe0.1 exists such that the magnetic anisotropy of the ferromagnet can be effectively controlled by engineering the orientation of the antiferromagnetic-spin axis.

Author Correction: Nanoscale control of competing interactions and geometrical frustration in a dipolar trident lattice.

The original version of this article contained an error in the legend to Figure 4. The yellow scale bar should have been defined as '~600 nm', not '~600 µm'. This has now been corrected in both the PDF and HTML versions of the article.

Emergent dynamic chirality in a thermally driven artificial spin ratchet.

Modern nanofabrication techniques have opened the possibility to create novel functional materials, whose properties transcend those of their constituent elements. In particular, tuning the magnetostatic interactions in geometrically frustrated arrangements of nanoelements called artificial spin ice can lead to specific collective behaviour, including emergent magnetic monopoles, charge screening and transport, as well as magnonic response. Here, we demonstrate a spin-ice-based active material in which energy is converted into unidirectional dynamics. Using X-ray photoemission electron microscopy we show that the collective rotation of the average magnetization proceeds in a unique sense during thermal relaxation. Our simulations demonstrate that this emergent chiral behaviour is driven by the topology of the magnetostatic field at the edges of the nanomagnet array, resulting in an asymmetric energy landscape. In addition, a bias field can be used to modify the sense of rotation of the average magnetization. This opens the possibility of implementing a magnetic Brownian ratchet, which may find applications in novel nanoscale devices, such as magnetic nanomotors, actuators, sensors or memory cells.

Nanoscale control of competing interactions and geometrical frustration in a dipolar trident lattice.

Geometrical frustration occurs when entities in a system, subject to given lattice constraints, are hindered to simultaneously minimize their local interactions. In magnetism, systems incorporating geometrical frustration are fascinating, as their behavior is not only hard to predict, but also leads to the emergence of exotic states of matter. Here, we provide a first look into an artificial frustrated system, the dipolar trident lattice, where the balance of competing interactions between nearest-neighbor magnetic moments can be directly controlled, thus allowing versatile tuning of geometrical frustration and manipulation of ground state configurations. Our findings not only provide the basis for future studies on the low-temperature physics of the dipolar trident lattice, but also demonstrate how this frustration-by-design concept can deliver magnetically frustrated metamaterials.Artificial magnetic nanostructures enable the study of competing frustrated interactions with more control over the system parameters than is possible in magnetic materials. Farhan et al. present a two-dimensional lattice geometry where the frustration can be controlled by tuning the unit cell parameters.

Thermodynamics of emergent magnetic charge screening in artificial spin ice.

Electric charge screening is a fundamental principle governing the behaviour in a variety of systems in nature. Through reconfiguration of the local environment, the Coulomb attraction between electric charges is decreased, leading, for example, to the creation of polaron states in solids or hydration shells around proteins in water. Here, we directly visualize the real-time creation and decay of screened magnetic charge configurations in a two-dimensional artificial spin ice system, the dipolar dice lattice. By comparing the temperature dependent occurrence of screened and unscreened emergent magnetic charge defects, we determine that screened magnetic charges are indeed a result of local energy reduction and appear as a transient minimum energy state before the system relaxes towards the predicted ground state. These results highlight the important role of emergent magnetic charges in artificial spin ice, giving rise to screened charge excitations and the emergence of exotic low-temperature configurations.

Atomically engineered ferroic layers yield a room-temperature magnetoelectric multiferroic.

Materials that exhibit simultaneous order in their electric and magnetic ground states hold promise for use in next-generation memory devices in which electric fields control magnetism. Such materials are exceedingly rare, however, owing to competing requirements for displacive ferroelectricity and magnetism. Despite the recent identification of several new multiferroic materials and magnetoelectric coupling mechanisms, known single-phase multiferroics remain limited by antiferromagnetic or weak ferromagnetic alignments, by a lack of coupling between the order parameters, or by having properties that emerge only well below room temperature, precluding device applications. Here we present a methodology for constructing single-phase multiferroic materials in which ferroelectricity and strong magnetic ordering are coupled near room temperature. Starting with hexagonal LuFeO3-the geometric ferroelectric with the greatest known planar rumpling-we introduce individual monolayers of FeO during growth to construct formula-unit-thick syntactic layers of ferrimagnetic LuFe2O4 (refs 17, 18) within the LuFeO3 matrix, that is, (LuFeO3)m/(LuFe2O4)1 superlattices. The severe rumpling imposed by the neighbouring LuFeO3 drives the ferrimagnetic LuFe2O4 into a simultaneously ferroelectric state, while also reducing the LuFe2O4 spin frustration. This increases the magnetic transition temperature substantially-from 240 kelvin for LuFe2O4 (ref. 18) to 281 kelvin for (LuFeO3)9/(LuFe2O4)1. Moreover, the ferroelectric order couples to the ferrimagnetism, enabling direct electric-field control of magnetism at 200 kelvin. Our results demonstrate a design methodology for creating higher-temperature magnetoelectric multiferroics by exploiting a combination of geometric frustration, lattice distortions and epitaxial engineering.

Thermal fluctuations in artificial spin ice.

Artificial spin ice systems have been proposed as a playground for the study of monopole-like magnetic excitations, similar to those observed in pyrochlore spin ice materials. Currents of magnetic monopole excitations have been observed, demonstrating the possibility for the realization of magnetic-charge-based circuitry. Artificial spin ice systems that support thermal fluctuations can serve as an ideal setting for observing dynamical effects such as monopole propagation and as a potential medium for magnetricity investigations. Here, we report on the transition from a frozen to a dynamic state in artificial spin ice with a square lattice. Magnetic imaging is used to determine the magnetic state of the islands in thermal equilibrium. The temperature-induced onset of magnetic fluctuations and excitation populations are shown to depend on the lattice spacing and related interaction strength between islands. The excitations are described by Boltzmann distributions with their factors in the frozen state relating to the blocking temperatures of the array. Our results provide insight into the design of thermal artificial spin ice arrays where the magnetic charge density and response to external fields can be studied in thermal equilibrium.