The strong coupling between spin, charge, and lattice degrees of freedom in perovskite oxides leads to an array of exotic phenomena, giving these materials rich phase diagrams that can include coupled orders. This is exemplified by the A-site doped ferrite La_1/3Sr_2/3FeO_3 (LSFO), which exhibits a coupled paramagnetic-antiferromagnetic and charge ordering phase transition at ∼190 K that has been well studied in thin films, bulk, and polycrystalline samples. However, the low temperature behavior of LSFO thin films below ∼100 K has not been thoroughly explored. This work uses several X-ray scattering and spectroscopy techniques to directly probe LSFO's magnetic and charge order down to low temperature. Using resonant X-ray scattering, we observe a complete suppression of LSFO's known antiferromagnetic and charge order below ∼25 K. Further spectroscopy and coherent scattering measurements provide insight into LSFO's electronic structure and domain dynamics in this new low temperature phase, and we propose possible explanations for the observed order suppression based on reduced dimensionality of domains in our thin films. Our findings provide insight into the effects of competing interactions in strongly correlated materials, particularly those with coupled orders.

Realizing innovative composite materials with passive thermal management capabilities and minimal ecological footprints is a challenging but much sought-after goal that would have a transformative effect on renewable energy sciences. We demonstrate an environmentally friendly metasurface utilizing vanadium dioxide (VO _2 ) that offers responsiveness to ambient temperature and potentially long-term stability. The metasurface enables passive thermal management by self-adjusting its absorptivity and emissivity response over a broad bandwidth ranging from visible to mid-infrared (IR) wavelengths. Above the VO _2 phase transition the metasurface exhibits increased mid-IR emissivity and reduced visible/near-IR absorptivity, creating an efficient radiative emission channel in the first atmospheric transparency window with reduced absorption of solar radiation. In contrast, below VO _2 ’s transition temperature, the metasurface increasingly absorbs sun light while minimizing mid-IR radiative heat losses. Moreover, a functional silicon layer eliminates the need for an additional capping layer commonly employed to protect VO _2 from environmental degradation. The additional protective layer often impedes the use and performance of VO _2 based devices in terrestrial as well as spacecraft applications. Therefore, the proposed durable and eco-friendly metasurface will be an excellent candidate for essential passive thermal regulation systems across residential and terrestrial applications.

Quantum materials have tremendous potential for disruptive applications. However, scaling devices down has been challenging due to electronic inhomogeneities in many of these materials. Understanding and controlling these electronic patterns on a local scale has thus become crucial to further new applications. To address this issue, we have developed a new optical microscopy method that allows for the precise quasi-continuous filming of the insulator-to-metal transition in VO­2 with fine temperature steps. This enables us to track metal and insulator domains over thousands of images and quantify, for the first time, the local hysteresis properties of VO­2 thin films. The analysis of the maps has allowed us to quantify cycle-to-cycle reproducibility of the local transitions and reveals a positive correlation between the local insulator–metal transition temperatures T­c and the local hysteresis widths ΔTc. These maps also enable the optical selection of regions of high or low transition temperature in combination with large or nearly absent local hysteresis. These maps pave the way to understand and use stochasticity to advantage in these materials by picking on-demand transition properties, allowing the scaling down of devices such as optical switches, infrared microbolometers and spiking neural networks.

Strongly correlated materials exhibiting phase transitions which can be controlled through external stimuli, such as electric fields, are promising for future computing technologies beyond conventional semiconductor transistors. Devices that take advantage of structural phase transitions have inherent built‐in memory, reminiscent of synapses and neurons, and are thus natural candidates for neuromorphic computing. Of particular interest are phase‐change oxides, which allow for control over the metal‐to‐insulator transition. Here, X‐ray nano‐diffraction structural imaging of micro‐devices fabricated with the archetypal phase‐change material vanadium sesquioxide (V 2 O 3 ) is reported. The devices contain a Ga ion‐irradiated region where the metal‐to‐insulator transition critical temperature is lowered, a useful feature for controlling neuron‐like spiking behavior. Results show that strain, induced by crystal lattice mismatch between the pristine and irradiated material, leads to a suppression of the metal‐to‐insulator‐transition. Suppression occurs within the irradiated region or along its edges, depending on the defect‐distribution and the size of the region. The observed self‐straining effect can extend to other phase‐change oxides and dominate as device dimensions are reduced and become too small to dissipate strain within the irradiated region. The findings are important for phase engineering in phase‐change devices and highlight the necessity to study phase transitions at the nanoscale.

In order to make neuromorphic functions in memristive devices more efficient, information about the structural properties of filament formation at the micro- and mesoscopic scales is necessary. Despite extensive research on VO2, a key material due to its filament formation, local operando structural measurements remain challenging and often involve destructive specimen preparation and long rastering times, greatly limiting the scope of experimental studies. Utilizing dark-field X-ray microscopy (DFXM), a full-field imaging modality, structural signatures of the filament formation process operando are revealed in VO2 devices. DFXM experiments illustrate that rutile filaments contain isolated monoclinic clusters, indicating structural nonuniformity interior to the filament. The formation of the rutile phase beneath device electrodes was shown to precede filament development, followed by the formation of filament paths guided by nucleation sites within the device. Finally, a medium-term (<30 min) memory mechanism is observed in VO2, mediated by sites within the device gap that tend to switch at significantly lower voltages after electrical cycling, a tendency that persists through a brief thermal reset. High spatial resolution, large field-of-view, structure selectivity, and fast signal acquisition of DFXM provided insight into structural features of the filamentary channel and surrounding regions during voltage cycling.

The metal-insulator transition (MIT) in vanadium dioxide (VO2) thin films is strongly affected by grain size, thickness, and interfacial properties. Typically, a minimum thickness around 50 nm is required for VO2 to exhibit a significant MIT when functional substrates like sapphire and silicon are used. Several works have shown that thin films below 20 nm, with up to 2-3 decades of change in the resistance across the MIT, can be achieved but require complex pre- or postprocessing of the samples. We show that predeposition substrate condition control facilitates the direct growth of VO2 ultrathin 15 nm films, exhibiting a resistance change between 3 and 4 decades across the MIT. Our findings indicate that the interface between the film and the substrate is crucial in determining the initial growth layers and the structural evolution. With appropriate substrate surface treatment, the desired VO2 MIT can be enhanced regardless of the substrate crystallographic orientation. Moreover, we propose a novel approach to obtain large resistance changes across the MIT in ultrathin VO2 films by incorporating a predeposited 1.5 nm vanadium oxide buffer layer, thereby eliminating the need to use different materials or complex pre- or postprocessing of the samples. We also demonstrate that this method improves the transition of 25-50 nm VO2 thin films on silicon substrates. Our study reveals a simple approach for direct growth of ultrathin VO2 films exhibiting a significant MIT, which is commonly accepted unattainable over substrates of technological importance, such as sapphire and silicon.

The same elements can form different compounds with widely different physical properties. Synthesis of a single-phase material is commonly achieved by controlling experimental conditions. Synthesizing materials that incorporate multiple specific spatially distributed chemical phases is often challenging, especially if different phases must be organized into well-defined spatial patterns. Here, we present an efficient solid reaction laser annealing (SRLA) approach to directly write regions of different local chemical compositions. We demonstrate the practical utility of our approach by locally writing microscale patterns of distinct chemical phases in vanadium oxide thin films. Specifically, we achieved the controlled local recrystallization of a uniform V2O3 matrix into VO2, V3O5, and V4O7 regions exhibiting sharp 1st- and 2nd-order metal–insulator phase transitions over a wide range of critical temperatures, i.e., a characteristic feature of select vanadium oxides that is extremely sensitive to even minute structural or compositional imperfections. We utilized the local chemical phase writing to pattern spiking oscillators with distinct electrical behavior directly in the thin film sample without employing elaborate lithography fabrication. Our laser tuning local chemical composition opens a pathway to synthesize a wide range of artificially micropatterned composite materials, with precision and control unattainable in conventional material synthesis methods.

Volatile resistive switching in neuromorphic computing can be tuned by external stimuli such as temperature or electric-field. However, this type of switching is generally coupled to structural changes, resulting in slower reaction speed and higher energy consumption when incorporated into an electronic device. The vanadium dioxide (VO2), which has near room temperature metal-insulator transition (MIT), is an archetypical volatile resistive switching system. Here, we demonstrate an isostructural MIT in an ultrathin VO2 film capped with a photoconductive cadmium sulfide (CdS) layer. Transmission electron microscopy, resistivity experiments, and first-principles calculations show that the hole carriers induced by CdS photovoltaic effect are driving the MIT in rutile VO2. The insulating-rutile VO2 phase has been proved and can remain stable for hours. Our finding provides a new approach to produce purely electronically driven MIT in VO2, and widens its applications in fast-response, low-energy neuromorphic devices.

The spin Seebeck effect (SSE) is sensitive to thermally driven magnetic excitations in magnetic insulators. Vanadium dioxide in its insulating low temperature phase is expected to lack magnetic degrees of freedom, as vanadium atoms are thought to form singlets upon dimerization of the vanadium chains. Instead, we find a paramagnetic SSE response in VO2 films that grows as the temperature decreases below 50 K. The field and temperature dependent SSE voltage is qualitatively consistent with a general model of paramagnetic SSE response and inconsistent with triplet spin transport. The microscopic nature of the magnetic excitations in VO2 requires further examination.

Electrical triggering of a metal-insulator transition (MIT) often results in the formation of characteristic spatial patterns such as a metallic filament percolating through an insulating matrix or an insulating barrier splitting a conducting matrix. When the MIT triggering is driven by electrothermal effects, the temperature of the filament or barrier can be substantially higher than the rest of material. Using x-ray microdiffraction and dark-field x-ray microscopy, we show that electrothermal MIT triggering leads to the development of an inhomogeneous strain profile across the switching device, even when the material does not undergo a 1st order structural phase transition coinciding with the MIT. Diffraction measurements further reveal evidence of lattice distortions and twinning occurring within the MIT switching device, highlighting a qualitative distinction between the electrothermal process and equilibrium thermal lattice expansion in nonlinear electrical systems. Electrically induced strain development, lattice distortions, and twinning could have important contributions in the MIT triggering process and could drive the material into non-equilibrium states, providing an unconventional pathway to explore the phase space of strongly correlated electronic systems.

Resistive memory-based reconfigurable systems constructed by CMOS-RRAM integration hold great promise for low energy and high throughput neuromorphic computing. However, most RRAM technologies relying on filamentary switching suffer from variations and noise leading to computational accuracy loss, increased energy consumption, and overhead by expensive program and verify schemes. Low ON-state resistance of filamentary RRAM devices further increases the energy consumption due to high-current read and write operations, and limits the array size and parallel multiply & accumulate operations. High-forming voltages needed for filamentary RRAM are not compatible with advanced CMOS technology nodes. To address all these challenges, we developed a forming-free and bulk switching RRAM technology based on a trilayer metal-oxide stack. We systematically engineered a trilayer metal-oxide RRAM stack and investigated the switching characteristics of RRAM devices with varying thicknesses and oxygen vacancy distributions across the trilayer to achieve reliable bulk switching without any filament formation. We demonstrated bulk switching operation at megaohm regime with high current nonlinearity and programmed up to 100 levels without compliance current. We developed a neuromorphic compute-in-memory platform based on trilayer bulk RRAM crossbars by combining energy-efficient switched-capacitor voltage sensing circuits with differential encoding of weights to experimentally demonstrate high-accuracy matrix-vector multiplication. We showcased the computational capability of bulk RRAM crossbars by implementing a spiking neural network model for an autonomous navigation/racing task. Our work addresses challenges posed by existing RRAM technologies and paves the way for neuromorphic computing at the edge under strict size, weight, and power constraints.

Applying voltage to metal-insulator transition (MIT) materials allows electrical actuation of the local electronic phase state. In MIT systems that have the electronic order coupled with the magnetic order, voltage switching of the electronic phase state can also enable the electrical manipulation of magnetic properties. In this work, we utilized x-ray magnetic circular dichroism photoemission electron microscopy (XMCD-PEEM) to investigate the control of magnetic domain configurations in ferromagnetic MIT electrical switches. For applied voltages above a threshold value, the XMCD-PEEM images show that the magnetic domains separate into two distinct regions: one with a high contrast (white/black), indicating well-defined micrometer-scale magnetic domains with a component of their magnetization aligned parallel/antiparallel to the x-ray helicity, and the other with different shades of intermediate contrast (gray). Significant changes in magnetic domain configurations upon voltage biasing were only observed in these gray regions. Furthermore, the voltage-induced magnetic domain separation was found to be bias polarity-dependent, with the gray regions expanding from the opposite sample edge when the applied voltage polarity was reversed. This polarity-dependent electrical control of magnetic domain configurations during the MIT switching opens alternative opportunities in memory applications for magnetic MIT switching materials.

Manipulating physical properties through ion migration in complex oxide thin films is an emerging research direction to achieve tunable materials for advanced applications. While the reduction of complex oxides has been widely reported, few reports exist on the modulation of physical properties through a direct hydrogenation process. Here, we report an unusual mechanism for hydrogen-induced topotactic phase transitions in perovskite La0.7Sr0.3CoO3 thin films. Hydrogenation is performed upon annealing in a pure hydrogen gas environment, offering a direct understanding of the role that hydrogen plays at the atomic scale in these transitions. Topotactic phase transformations from the perovskite (P) to hydrogenated-brownmillerite (H-BM) phase can be induced at temperatures as low as 220 °C, while at higher hydrogenation temperatures (320-400 °C), the progression toward more reduced phases is hindered. Density functional theory calculations suggest that hydroxyl bonds are formed with the introduction of hydrogen ions, which lower the formation energy of oxygen vacancies of the neighboring oxygen, enabling the transition from the P to H-BM phase at low temperatures. Furthermore, the impact on the magnetic and electronic properties of the hydrogenation temperature is investigated. Our research provides a potential pathway for utilizing hydrogen as a basis for low-temperature modulation of complex oxide thin films, with potential applications in neuromorphic computing.

Interfacial effects between antiferromagnetic (AFM) and ferromagnetic (FM) materials have long been a center of magnetism studies. Aside from the exchange bias occurring at the AFM/FM interface, controlling the coercivity is another significant topic in magnetic recordings. The coercivity of FM materials is often determined through varying grain size, alloy composition, density of defects, etc., which is set during material growth and offers limited room for modification after growth. Hematite (α-Fe2O3) is an AFM material that undergoes a temperature-controlled spin-flip transition, the so-called Morin transition. This transition gives an extra degree of freedom making hematite an intriguing component to study the exchange coupling when interfaced with an FM material. In this work, changes in the magnetic properties of soft magnetic permalloy (Ni81Fe19, or Py) thin films grown on hematite were studied across the Morin transition. Surprisingly, these samples showed a remarkable change in coercivity during the Morin transition. We attribute this effect to the magnetic domain mixture of hematite during the Morin transition. Our findings present a novel method of controlling the coercivity of plain ferromagnetic thin films.

Vanadium sesquioxide (V2O3) is a strongly correlated electronic material that famously undergoes a triple coupled first-order transition where it transitions from a paramagnetic metal with a rhombohedral structure at high temperature to an antiferromagnetic insulator with a monoclinic structure. While several studies have used one of both electronic and structural transitions to control the properties of a heterostructure, evidence of magnetic coupling has notoriously yet to be found. In this paper, we report on a robust magnetic coupling between the antiferromagnetic (AFM) V2O3 and ferromagnetic (FM) Permalloy (Py) layers that results in a significant exchange bias and strain-induced coercivity enhancement. We provide a temperature and angle-dependent study of magnetic properties, which clearly indicates exchange bias at the AFM/FM interface that appears at the onset of the metal-insulator transition. The magnitude of the exchange bias is strongest when the field is applied along the [001] V2O3 crystallographic orientation which corresponds to an AFM spin configuration on the [110] surface. This opens the door to designing and implementing novel functionalities in transition metal oxide-based computing using the connection between magnetism and the metal-insulator transition.

Despite its amazing quantitative successes and contributions to revolutionary technologies, physics currently faces many unsolved mysteries ranging from the meaning of quantum mechanics to the nature of the dark energy that will determine the future of the Universe. It is clearly prohibitive for the general reader, and even the best informed physicists, to follow the vast number of technical papers published in the thousands of specialized journals. For this reason, we have asked the leading experts across many of the most important areas of physics to summarise their global assessment of some of the most important issues. In lieu of an extremely long abstract summarising the contents, we invite the reader to look at the section headings and their authors, and then to indulge in a feast of stimulating topics spanning the current frontiers of fundamental physics from 'The Future of Physics' by William D Phillips and 'What characterises topological effects in physics?' by Gerard 't Hooft through the contributions of the widest imaginable range of world leaders in their respective areas. This paper is presented as a preface to exciting developments by senior and young scientists in the years that lie ahead, and a complement to the less authoritative popular accounts by journalists.

While the connection between colossal magnetoresistance and phase separation in praseodymium-doped rareearth manganites has been well established, the underlying mechanisms enabling this connection still need to be fully understood. This paper thoroughly examines the phase separation in La5/8-xPrxCa3/8MnO3 (x = 0.40) using an integrated approach including magnetotransport, electron spin resonance, and magnetic susceptibility. We observed that the initially fluidlike magnetic phase separation at intermediate temperatures transforms into the solidlike phase separation via a glass transition at low temperatures. Magnetization dynamics measurements revealed that this transition is concurrent with the reentrance of the paramagnetic phase. Our findings offer a perspective on the freezing of phase separation fluidlike behavior resulting in the advent of the low-temperature solidlike state, contributing to a deeper understanding of the temperature-dependent behaviors of praseodymiumdoped rare-earth manganites.

Bulk V2O3 features concomitant metal-insulator (MIT) and structural (SPT) phase transitions at TC ~ 160 K. In thin films, where the substrate clamping can impose geometrical restrictions on the SPT, the epitaxial relation between the V2O3 film and substrate can have a profound effect on the MIT. Here we present a detailed characterization of domain nucleation and growth across the MIT in (001)-oriented V2O3 films grown on sapphire. By combining scanning electron transmission microscopy (STEM) and photoelectron emission microscopy (PEEM), we imaged the MIT with planar and vertical resolution. We observed that upon cooling, insulating domains nucleate at the top of the film, where strain is lowest, and expand downwards and laterally. This growth is arrested at a critical thickness of 50 nm from the substrate interface, leaving a persistent bottom metallic layer. As a result, the MIT cannot take place in the interior of films below this critical thickness. However, PEEM measurements revealed that insulating domains can still form on a very thin superficial layer at the top interface. Our results demonstrate the intricate spatial complexity of the MIT in clamped V2O3, especially the strain-induced large variations along the c-axis. Engineering the thickness-dependent MIT can provide an unconventional way to build out-of-plane geometry devices by using the persistent bottom metal layer as a native electrode.

Metal-insulator transitions (MITs) in resistive switching materials can be triggered by an electric stimulus that produces significant changes in the electrical response. When these phases have distinct magnetic characteristics, dramatic changes in spin excitations are also expected. The transition metal oxide La0.7Sr0.3MnO3 (LSMO) is a ferromagnetic metal at low temperatures and a paramagnetic insulator above room temperature. When LSMO is in its metallic phase a critical electrical bias has been shown to lead to an MIT that results in the formation of a paramagnetic resistive barrier transverse to the applied electric field. Using spin-transfer ferromagnetic resonance spectroscopy, we show that even for electrical biases less than the critical value that triggers the MIT, there is magnetic phase separation with the spin-excitation resonances varying systematically with applied bias. Thus, applied voltages provide a means to alter spin resonance characteristics of interest for neuromorphic circuits.