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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.

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., Comment: 54 pages, 13 figures

There is growing interest in strongly correlated insulator thin films because the intricate interplay of their intrinsic and extrinsic state variables causes memristive behavior that might be used for bio-mimetic devices in the emerging field of neuromorphic computing. In this study we find that laser irradiation tends to drive V$_2$O$_3$ from supercooled/superheated metastable states towards thermodynamic equilibrium, most likely in a non-thermal way. We study thin films of the prototypical Mott-insulator V$_2$O$_3$, which show spontaneous phase separation into metal-insulator herringbone domains during the Mott transition. Here, we use low-temperature microscopy to investigate how these metal-insulator domains can be modified by scanning a focused laser beam across the thin film surface. We find that the response depends on the thermal history: When the thin film is heated from below the Mott transition temperature, the laser beam predominantly induces metallic domains. On the contrary, when the thin film is cooled from a temperature above the transition, the laser beam predominantly induces insulating domains. Very likely, the V$_2$O$_3$ thin film is in a superheated or supercooled state, respectively, during the first-order phase transition, and the perturbation by a laser beam drives these metastable states into stable ones. This way, the thermal history is locally erased. Our findings are supported by a phenomenological model with a laser-induced lowering of the energy barrier between the metastable and equilibrium states., Comment: 14 pages, 10 figures

In the pursuit of scalable and energy-efficient neuromorphic devices, recent research has unveiled a novel category of spiking oscillators, termed "thermal neuristors." These devices function via thermal interactions among neighboring vanadium dioxide resistive memories, emulating biological neuronal behavior. Here, we show that the collective dynamical behavior of networks of these neurons showcases a rich phase structure, tunable by adjusting the thermal coupling and input voltage. Notably, we identify phases exhibiting long-range order that, however, does not arise from criticality, but rather from the time non-local response of the system. In addition, we show that these thermal neuristor arrays achieve high accuracy in image recognition and time series prediction through reservoir computing, without leveraging long-range order. Our findings highlight a crucial aspect of neuromorphic computing with possible implications on the functioning of the brain: criticality may not be necessary for the efficient performance of neuromorphic systems in certain computational tasks., Comment: 20 pages, 14 figures

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.

We present a novel heterostructured approach to disentangle the mechanism of electrical transport of the strongly correlated PrNiO3, by placing the nickelate under the photoconductor CdS. This enables the injection of carriers into PrNiO3 in a controlled way, which can be used to interrogate its intrinsic transport mechanism. We find a non-volatile resistance decrease when illuminating the system at temperatures below the PrNiO3 metal-insulator transition. The photoinduced change becomes more volatile as the temperature increases. These data help understand the intrinsic transport properties of the nickelate-CdS bilayer. Together with data from a bare PrNiO3 film, we find that the transport mechanism includes a combination of mechanisms including both thermal activation and variable range hopping. At low temperatures without photoinduced carriers the transport is governed by hopping, while at higher temperatures and intense illumination the activation mechanism becomes relevant. This work shows a new way to optically control the low-temperature resistance of PrNiO3.

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.

Neuromorphic functionalities in memristive devices are commonly associated with the ability to electrically create local conductive pathways by resistive switching. The archetypal correlated material, VO2, has been intensively studied for its complex electronic and structural phase transition as well as its filament formation under applied voltages. Local structural studies of the filament behavior are often limited due to time-consuming rastering which makes impractical many experiments aimed at investigating large spatial areas or temporal dynamics associated with the electrical triggering of the phase transition. Utilizing Dark Field X-ray Microscopy (DFXM), a novel full-field x-ray imaging technique, we study this complex filament formation process in-operando in VO2 devices from a structural perspective. We show that prior to filament formation, there is a significant gain of the metallic rutile phase beneath the metal electrodes that define the device. We observed that the filament formation follows a preferential path determined by the nucleation sites within the device. These nucleation sites are predisposed to the phase transition and can persistently maintain the high-temperature rutile phase even after returning to room temperature, which can enable a novel training/learning mechanism. Filament formation also appears to follow a preferential path determined by a nucleation site within the device which is predisposed to the rutile transition even after returning to room temperature. Finally, we found that small isolated low-temperature phase clusters can be present inside the high-temperature filaments indicating that the filament structure is not uniform. Our results provide a unique perspective on the electrically induced filament formation in metal-insulator transition materials, which further the basic understanding of this resistive switching., Comment: 29 pages, 10 figures; 19 pages main text, 3 figures; 10 pages Supplementary material, 7 figures

Phase separation naturally occurs in a variety of magnetic materials and it often has a major impact on both electric and magnetotransport properties. In resistive switching systems, phase separation can be created on demand by inducing local switching, which provides an opportunity to tune the electronic and magnetic state of the device by applying voltage. Here we explore the magnetotransport properties in the ferromagnetic oxide (La,Sr)MnO3 (LSMO) during the electrical triggering of an intrinsic metal-insulator transition (MIT) that produces volatile resistive switching. This switching occurs in a characteristic spatial pattern, i.e., the formation of an insulating barrier perpendicular to the current flow, enabling an electrically actuated ferromagnetic-paramagnetic-ferromagnetic phase separation. At the threshold voltage of the MIT triggering, both anisotropic and colossal magnetoresistances exhibit anomalies including a large increase in magnitude and a sign flip. Computational analysis revealed that these anomalies originate from the coupling between the switching-induced phase separation state and the intrinsic magnetoresistance of LSMO. This work demonstrates that driving the MIT material into an out-of-equilibrium resistive switching state provides the means to electrically control of the magnetotransport phenomena.

While the complementary metal-oxide semiconductor (CMOS) technology is the mainstream for the hardware implementation of neural networks, we explore an alternative route based on a new class of spiking oscillators we call thermal neuristors, which operate and interact solely via thermal processes. Utilizing the insulator-to-metal transition in vanadium dioxide, we demonstrate a wide variety of reconfigurable electrical dynamics mirroring biological neurons. Notably, inhibitory functionality is achieved just in a single oxide device, and cascaded information flow is realized exclusively through thermal interactions. To elucidate the underlying mechanisms of the neuristors, a detailed theoretical model is developed, which accurately reflects the experimental results. This study establishes the foundation for scalable and energy-efficient thermal neural networks, fostering progress in brain-inspired computing.

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. Quantitative estimates find a spin Seebeck coefficient comparable in magnitude to that observed in strongly magnetic materials. The microscopic nature of the magnetic excitations in VO2 requires further examination., Comment: 30 pages, 16 figures

The strongly correlated material La0.7Sr0.3MnO3 (LSMO) exhibits metal-to-insulator and magnetic transition near room temperature. Although the physical properties of LSMO can be manipulated by strain, chemical doping, temperature, or magnetic field, they often require large external stimuli. To include additional flexibility and tunability, we developed a hybrid optoelectronic heterostructure that uses photocarrier injection from cadmium sulfide (CdS) to an LSMO layer to change its electrical conductivity. LSMO exhibits no significant optical response, however, the CdS/LSMO heterostructures show an enhanced conductivity, with ~ 37 % resistance drop, at the transition temperature under light stimuli. This enhanced conductivity in response to light is comparable to the effect of a 9 T magnetic field in pure LSMO. Surprisingly, the optical and magnetic responses of CdS/LSMO heterostructures are decoupled and exhibit different effects when both stimuli are applied. This unexpected behavior shows that heterostructuring strongly correlated oxides may require a new understanding of the coupling of physical properties across the transitions and provide the means to implement new functionalities.

Controlling the magnetic ground states at the nanoscale is a long-standing basic research problem and an important issue in magnetic storage technologies. Here, we designed a nanostructured material that exhibits very unusual hysteresis loops due to a transition between vortex and double pole states. Arrays of 700 nm diamond-shape nanodots consisting of Py(30 nm)/Ru(tRu)/Py(30 nm) (Py, permalloy (Ni80Fe20)) trilayers were fabricated by interference lithography and e-beam evaporation. We show that varying the Ru interlayer spacer thickness (tRu) governs the interaction between the Py layers. We found this interaction mainly mediated by two mechanisms: magnetostatic interaction that favors antiparallel (antiferromagnetic, AFM) alignment of the Py layers and exchange interaction that oscillates between ferromagnetic (FM) and AFM couplings. For a certain range of Ru thicknesses, FM coupling dominates and forms magnetic vortices in the upper and lower Py layers. For Ru thicknesses at which AFM coupling dominates, the magnetic state in remanence is a double pole structure. Our results showed that the interlayer exchange coupling interaction remains finite even at 4 nm Ru thickness. The magnetic states in remanence, observed by Magnetic Force Microscopy (MFM), are in good agreement with corresponding hysteresis loops obtained by Magneto-Optic Kerr Effect (MOKE) and micromagnetic simulations., Comment: 16 pages, 4 figures, 1table

We have developed a new optical microscopy technique able to track micron-sized surface clusters as temperature is varied. Potential candidates for study include phase separated metal-insulator materials, ferroelectrics, and porous structures. Several key techniques (including autofocus, step motor/cross correlation alignments, single-pixel thresholding, pair connectivity correlation length and image convolution) were implemented in order to obtain a time series of thresholded images. Here, we apply this new method to probe the archetypal phase separated insulator-metal transition in VO$_2$. A precise time and temperature series of the insulator-metal transition was achieved, allowing us to construct for the first time in this material spatial maps of the transition temperature T$_c$. These maps reveal multiple interesting features such as fractal electronic patterns on micron scales, regions of the sample with an extremely large or nearly absent local hysteresis, a positive correlation between the T$_c$ value and the hysteresis width $\Delta$T$_c$, and high cycle-to-cycle reproducibility of the transition. These maps also allow for the identification of individual pixels with unique transition characteristics. This unprecedented knowledge of the local properties of each spot along with the behavior of the entire network paves the way to novel electronics applications enabled by, {\em e.g.}, addressing specific regions with desired memory and/or switching characteristics, as well as detailed explorations of open questions in the theory of hysteresis.

The low temperature monoclinic, insulating phase of vanadium dioxide is ordinarily considered nonmagnetic, with dimerized vanadium atoms forming spin singlets, though paramagnetic response is seen at low temperatures. We find a nonlocal spin Seebeck signal in VO2 films that appears below 30 K and which increases with decreasing temperature. The spin Seebeck response has a non-hysteretic dependence on in-plane external magnetic field. This paramagnetic spin Seebeck response is discussed in terms of prior findings on paramagnetic spin Seebeck effects and expected magnetic excitations of the monoclinic ground state., Comment: 11 pages, 3 figures, + 11 pages and 10 figures of supplemental material

In solids, strong repulsion between electrons can inhibit their movement and result in a "Mott" metal-to-insulator transition (MIT), a fundamental phenomenon whose understanding has remained a challenge for over 50 years. A key issue is how the wave-like itinerant electrons change into a localized-like state due to increased interactions. However, observing the MIT in terms of the energy- and momentum-resolved electronic structure of the system, the only direct way to probe both itinerant and localized states, has been elusive. Here we show, using angle-resolved photoemission spectroscopy (ARPES), that in V$_2$O$_3$ the temperature-induced MIT is characterized by the progressive disappearance of its itinerant conduction band, without any change in its energy-momentum dispersion, and the simultaneous shift to larger binding energies of a quasi-localized state initially located near the Fermi level., Comment: Main Text (4 figures) and Supplementary Information (12 figures)

Neuromorphic computing approaches become increasingly important as we address future needs for efficiently processing massive amounts of data. The unique attributes of quantum materials can help address these needs by enabling new energy-efficient device concepts that implement neuromorphic ideas at the hardware level. In particular, strong correlations give rise to highly non-linear responses, such as conductive phase transitions that can be harnessed for short and long-term plasticity. Similarly, magnetization dynamics are strongly non-linear and can be utilized for data classification. This paper discusses select examples of these approaches, and provides a perspective for the current opportunities and challenges for assembling quantum-material-based devices for neuromorphic functionalities into larger emergent complex network systems.

Using the extensively studied V2O3 as a prototype system, we investigate the role of percolation in metal-insulator transition (MIT). We apply scanning microwave impedance microscopy to directly determine the metallic phase fraction p and relate it to the macroscopic conductance G, which shows a sudden jump when p reaches the percolation threshold. Interestingly, the conductance G exhibits a hysteretic behavior against p, suggesting two different percolating processes upon cooling and warming. Based on our image analysis and model simulation, we ascribe such hysteretic behavior to different domain nucleation and growth processes between cooling and warming, which is likely caused by the decoupled structural and electronic transitions in V2O3 during MIT. Our work provides a microscopic view of how the interplay of structural and electronic degrees of freedom affects MIT in strongly correlated systems.

Recently, evidence for a conducting surface state below 19 K was reported for the correlated d-electron small gap semiconductor FeSi. In the work reported herein, the conducting surface state and the bulk phase of FeSi were probed via electrical resistivity measurements as a function of temperature T, magnetic field B to 60 T and pressure P to 7.6 GPa, and by means of a magnetic field modulated microwave spectroscopy (MFMMS) technique. The properties of FeSi were also compared to those of the Kondo insulator SmB6 to address the question of whether FeSi is a d-electron analogue of an f-electron Kondo insulator and, in addition, a topological Kondo insulator. The overall behavior of the magnetoresistance MR of FeSi at temperatures above and below the onset temperature (T_S) 19 K of the conducting surface state is similar to that of SmB6. The two energy gaps, inferred from the resistivity data in the semiconducting regime, increase with pressure up to about 7 GPa, followed by a drop which coincides with a sharp suppression of T_S. This behavior is similar to that reported for SmB6, except that the two energy gaps in SmB6 decrease with pressure before dropping abruptly at T_S. The MFMMS measurements showed a sharp feature at T_S (19 K) for FeSi, but no such feature was observed at T_S 4.5 K for SmB6. The absence of a feature at T_S for SmB6 may be due to experimental issues and will be the subject of a future investigation.

The emergence of spin-orbit torques as a promising approach to energy-efficient magnetic switching has generated large interest in material systems with easily and fully tunable spin-orbit torques. Here, current-induced spin-orbit torques in VO$_2$/NiFe heterostructures were investigated using spin-torque ferromagnetic resonance, where the VO$_2$ layer undergoes a prominent insulator-metal transition. A roughly two-fold increase in the Gilbert damping parameter, $\alpha$, with temperature was attributed to the change in the VO$_2$/NiFe interface spin absorption across the VO$_2$ phase transition. More remarkably, a large modulation ($\pm$100%) and a sign change of the current-induced spin-orbit torque across the VO$_2$ phase transition suggest two competing spin-orbit torque generating mechanisms. The bulk spin Hall effect in metallic VO$_2$, corroborated by our first-principles calculation of spin Hall conductivity, $\sigma_{SH} \approx 10^4 \frac{\hbar}{e} \Omega^{-1} m^{-1}$, is verified as the main source of the spin-orbit torque in the metallic phase. The self-induced/anomalous torque in NiFe, of the opposite sign and a similar magnitude to the bulk spin Hall effect in metallic VO$_2$, could be the other competing mechanism that dominates as temperature decreases. For applications, the strong tunability of the torque strength and direction opens a new route to tailor spin-orbit torques of materials which undergo phase transitions for new device functionalities., Comment: 16 pages, 5 figures

We report on a temperature-driven reversible change of the in-plane magnetic anisotropy of V$_2$O$_3$/Ni bilayers. This is caused by the rhombohedral to monoclinic structural phase transition of V$_2$O$_3$ at $T_C$ = 160 K. The in-plane magnetic anisotropy is uniaxial above $T_C$, but as the bilayer is cooled through the structural phase transition, a secondary magnetic easy axis emerges. Ferromagnetic resonance measurements show that this change in magnetic anisotropy is reversible with temperature. We identify two structural properties of the V$_2$O$_3$/Ni bilayers affecting the in-plane magnetic anisotropy: (1) a growth-induced uniaxial magnetic anisotropy associated with step-like terraces in the bilayer microstructure and (2) a low-temperature strain-induced biaxial anisotropy associated with the V$_2$O$_3$ structural phase transition. Magnetoresistance measurements corroborate the change in magnetic anisotropy across the structural transition and suggest that the negative magnetostriction of Ni leads to the emergence of a strain-induced easy-axis. This shows that a temperature-dependent structural transition in V$_2$O$_3$ may be used to tune the magnetic anisotropy in an adjacent ferromagnetic thin film., Comment: 9 pages, 8 figures

The discovery of new mechanisms of controlling magnetic properties by electric fields or currents furthers the fundamental understanding of magnetism and has important implications for practical use. Here, we present a novel approach of utilizing resistive switching to control magnetic anisotropy. We study a ferromagnetic oxide that exhibits an electrically triggered metal-to-insulator phase transition producing a volatile resistive switching. This switching occurs in a characteristic spatial pattern: the formation of a transverse insulating barrier inside a metallic matrix resulting in an unusual ferromagnetic/paramagnetic/ferromagnetic configuration. We found that the formation of this voltage-driven paramagnetic insulating barrier is accompanied by the emergence of a strong uniaxial magnetic anisotropy that overpowers the intrinsic material anisotropy. Our results demonstrate that resistive switching is an effective tool for manipulating magnetic properties. Because resistive switching can be induced in a very broad range of materials, our findings could enable a new class of voltage-controlled magnetism systems.

Resistive switching is one of the key phenomena for applications such as nonvolatile memories or neuromorphic computing. V3O5, a compound of the vanadium oxide Magn\'eli series, is one of the rare materials to exhibit an insulator-metal transition (IMT) above room temperature (Tc ~ 415 K). Here we demonstrate both static dc resistive switching (RS) and fast oscillatory spiking regimes in V3O5 devices at room temperature (120 K below the phase transition temperature) by applying an electric field. We use operando optical imaging to track a reflectivity change during the RS and find that a percolating high temperature metallic phase filament is formed. This demonstrates that the electrically induced RS triggers the phase transition. Furthermore, we optically capture the spiking oscillations that we link to the negative differential resistance regime and find the filament forms and dissolves via a periodic spatio-temporal instability that we describe by numerical simulations.

The coupling of electronic degrees of freedom in materials to create hybridized functionalities is a holy grail of modern condensed matter physics that may produce novel mechanisms of control. Correlated electron systems often exhibit coupled degrees of freedom with a high degree of tunability which sometimes lead to hybridized functionalities based on external stimuli. However, the mechanisms of tunability and the sensitivity to external stimuli are determined by intrinsic material properties which are not always controllable. A Mott metal-insulator transition, which is technologically attractive due to the large changes in resistance, can be tuned by doping, strain, electric fields, and orbital occupancy but cannot be, in and of itself, controlled externally with light. Here we present a new approach to produce hybridized functionalities using a properly engineered photoconductor/strongly-correlated hybrid heterostructure, showing control of the Metal-to-Insulator transition (MIT) using optical means. This approach combines a photoconductor, which does not exhibit an MIT, with a strongly correlated oxide, which is not photoconducting. Due to the close proximity between the two materials, the heterostructure exhibits large volatile and nonvolatile, photoinduced resistivity changes and substantial photoinduced shifts in the MIT transition temperatures. This approach can potentially be extended to other judiciously chosen combinations of strongly correlated materials with systems which exhibit optically, electrically or magnetically controllable behavior.

Resistive-switching -- the current-/voltage-induced electrical resistance change -- is at the core of memristive devices, which play an essential role in the emerging field of neuromorphic computing. This study is about resistive switching in a Mott-insulator, which undergoes a thermally driven metal-to-insulator transition. Two distinct switching mechanisms were reported for such a system: electric-field-driven resistive switching and electrothermal resistive switching. The latter results from an instability caused by Joule heating. Here, we present the visualization of the reversible resistive switching in a planar V$_2$O$_3$ thin-film device using high-resolution wide-field microscopy in combination with electric transport measurements. We investigate the interaction of the electrothermal instability with the strain-induced spontaneous phase-separation in the V$_2$O$_3$ thin film at the Mott-transition. The photomicrographs show the formation of a narrow metallic filament with a minimum width $\lesssim$ 500\,nm. Although the filament formation and the overall shape of the current-voltage characteristics (IVCs) are typical of an electrothermal breakdown, we also observe atypical effects like oblique filaments, filament splitting, and hysteretic IVCs with sawtooth-like jumps at high currents in the low-resistance regime. We were able to reproduce the experimental results in a numerical model based on a two-dimensional resistor network. This model demonstrates that resistive switching, in this case, is indeed electrothermal and that the intrinsic heterogeneity is responsible for the atypical effects. This heterogeneity is strongly influenced by strain, thereby establishing a link between switching dynamics and structural properties., Comment: (18 pages, 12 figures)

Application of an electric stimulus to a material with a metal-insulator transition can trigger a large resistance change. Resistive switching from an insulating into a metallic phase, which typically occurs by the formation of conducting filaments parallel to the current flow, has been an active research topic. Here we present the discovery of an opposite, metal-to-insulator switching that proceeds via nucleation and growth of an insulating barrier perpendicular to the driving current. The barrier formation leads to an unusual N-type negative differential resistance in the current-voltage characteristics. Electrically inducing a transverse barrier enables a novel approach to voltage-controlled magnetism. By triggering a metal-to-insulator resistive switching in a magnetic material, local on/off control of ferromagnetism can be achieved by a global voltage bias applied to the whole device.

Nitrogen vacancy (NV) centers, optically-active atomic defects in diamond, have attracted tremendous interest for quantum sensing, network, and computing applications due to their excellent quantum coherence and remarkable versatility in a real, ambient environment. Taking advantage of these strengths, we report on NV-based local sensing of the electrically driven insulator-to-metal transition (IMT) in a proximal Mott insulator. We studied the resistive switching properties of both pristine and ion-irradiated VO2 thin film devices by performing optically detected NV electron spin resonance measurements. These measurements probe the local temperature and magnetic field in electrically biased VO2 devices, which are in agreement with the global transport measurement results. In pristine devices, the electrically-driven IMT proceeds through Joule heating up to the transition temperature while in ion-irradiated devices, the transition occurs non-thermally, well below the transition temperature. Our results provide the first direct evidence for non-thermal electrically induced IMT in a Mott insulator, highlighting the significant opportunities offered by NV quantum sensors in exploring nanoscale thermal and electrical behaviors in Mott materials.

Vanadium oxides are strongly correlated materials which display metal-insulator transitions as well as various structural and magnetic properties that depend heavily on oxygen stoichiometry. Therefore, it is crucial to precisely control oxygen stoichiometry in these materials, especially in thin films. This work demonstrates a high-vacuum gas evolution technique which allows for the modification of oxygen concentration in VOX thin films by carefully tuning thermodynamic conditions. We were able to control the evolution between VO2, V3O5, and V2O3 phases on sapphire substrates, overcoming the narrow phase stability of adjacent Magn\'eli phases. A variety of annealing routes were found to achieve the desired phases and eventually to control the metal-insulator transition (MIT). The pronounced MIT of the transformed films along with the detailed structural investigations based on x-ray diffraction measurements and reciprocal space mapping show that optimal stoichiometry is obtained and stabilized. Using this technique, we find that the thin film V-O phase diagram differs from that of the bulk material due to strain and finite size effects. Our study demonstrates new pathways to strategically tune the oxygen stoichiometry in complex oxides and provides a roadmap for understanding the phase stability of VOX thin films.

We present a coordinated study of the paramagnetic-to-antiferromagnetic, rhombohedral-to-monoclinic, and metal-to-insulator transitions in thin-film specimens of the classic Mott insulator V$_2$O$_3$ using low-energy muon spin relaxation, x-ray diffraction, and nanoscale-resolved near-field infrared spectroscopic techniques. The measurements provide a detailed characterization of the thermal evolution of the magnetic, structural, and electronic phase transitions occurring in a wide temperature range, including quantitative measurements of the high- and low-temperature phase fractions for each transition. The results reveal a stable coexistence of the high- and low-temperature phases over a broad temperature range throughout the transition. Careful comparison of temperature dependence of the different measurements, calibrated by the resistance of the sample, demonstrates that the electronic, magnetic, and structural degrees of freedom remain tightly coupled to each other during the transition process. We also find evidence for antiferromagnetic fluctuations in the vicinity of the phase transition, highlighting the important role of the magnetic degree of freedom in the metal-insulator transition.

Resistive switching can be achieved in a Mott insulator by applying current/voltage, which triggers an insulator-metal transition (IMT). This phenomenon is key for understanding IMT physics and developing novel memory elements and brain-inspired technology. Despite this, the roles of electric field and Joule heating in the switching process remain controversial. We resolve this issue by studying nanowires of two archetypical Mott insulators - VO2 and V2O3. Our findings show a crossover between two qualitatively different regimes. In one, the IMT is driven by Joule heating to the transition temperature, while in the other, field-assisted carrier generation gives rise to a doping driven IMT which is purely non-thermal. By identifying the key material properties governing these phenomena, we propose a universal mechanism for resistive switching in Mott insulators. This understanding enabled us to control the switching mechanism using focused ion-beam irradiation, thereby facilitating an electrically driven non-thermal IMT. The energy consumption associated with the non-thermal IMT is extremely low, rivaling that of state of the art electronics and biological neurons. These findings pave the way towards highly energy-efficient applications of Mott insulators.

Machine learning imitates the basic features of biological neural networks to efficiently perform tasks such as pattern recognition. This has been mostly achieved at a software level, and a strong effort is currently being made to mimic neurons and synapses with hardware components, an approach known as neuromorphic computing. CMOS-based circuits have been used for this purpose, but they are non-scalable, limiting the device density and motivating the search for neuromorphic materials. While recent advances in resistive switching have provided a path to emulate synapses at the 10 nm scale, a scalable neuron analogue is yet to be found. Here, we show how heat transfer can be utilized to mimic neuron functionalities in Mott nanodevices. We use the Joule heating created by current spikes to trigger the insulator-to-metal transition in a biased VO2 nanogap. We show that thermal dynamics allow the implementation of the basic neuron functionalities: activity, leaky integrate-and-fire, volatility and rate coding. By using local temperature as the internal variable, we avoid the need of external capacitors, which reduces neuristor size by several orders of magnitude. This approach could enable neuromorphic hardware to take full advantage of the rapid advances in memristive synapses, allowing for much denser and complex neural networks. More generally, we show that heat dissipation is not always an undesirable effect: it can perform computing tasks if properly engineered.

We performed measurements of Py/Cu and Py/Ag lateral spin valves as function of injection current direction and magnitude. Above a 'critical' current, there is an unexpected dependence of spin injection on current direction. Positive currents show higher polarization of spin injection than negative. This implies that in addition to current-induced spin injection, there is a thermally induced injection from a spin-dependent Seebeck effect. A temperature gradient in the Py electrode, caused by Joule heating, is responsible for injecting excess spins into the non-magnetic channel. This effect has important consequences for understanding high-current spin-based devices, such as spin transfer torque devices., Comment: 10 pages, 4 figures

This tutorial describes challenges and possible avenues for the implementation of the components of a solid-state system, which emulates a biological brain. The tutorial is devoted mostly to a charge-based (i.e. electric controlled) implementation using transition metal oxides materials, which exhibit unique properties that emulate key functionalities needed for this application. In the Introduction, we compare the main differences between a conventional computational machine, based on the Turing-von Neumann paradigm, to a Neuromorphic machine, which tries to emulate important functionalities of a biological brain. We also describe the main electrical properties of biological systems, which would be useful to implement in a charge-based system. In Chapter II, we describe the main components of a possible solid-state implementation. In Chapter III, we describe a variety of Resistive Switching phenomena, which may serve as the functional basis for the implementation of key devices for Neuromorphic computing. In Chapter IV we describe why transition metal oxides, are promising materials for future Neuromorphic machines. Theoretical models describing different resistive switching mechanisms are discussed in Chapter V while existing implementations are described in Chapter VI. Chapter VII presents applications to practical problems. We list in Chapter VIII important basic research challenges and open issues. We discuss issues related to specific implementations, novel materials, devices and phenomena. The development of reliable, fault tolerant, energy efficient devices, their scaling and integration into a Neuromorphic computer may bring us closer to the development of a machine that rivals the brain., Comment: To appear in Journal of Applied Physics. 43 pages

Despite decades of experimental and theoretical efforts, the origin of metal-insulator transitions (MIT) in strongly-correlated materials is one of the main longstanding problems in condensed matter physics. An archetypal example is V2O3, where electronic, structural and magnetic phase transitions occur simultaneously. This remarkable concomitance makes the understanding of the origin of the MIT a challenge due to the many degrees of freedom at play. In this work, we demonstrate that magnetism plays the key dominant role. By acting on the magnetic degree of freedom, we reveal an anomalous behaviour of the magnetoresistance of V2O3, which provides strong evidence that the origin of the MIT in V2O3 is the opening of an antiferromagnetic gap in the presence of strong electronic correlations., Comment: 7 pages, 4 figures