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Ivan K. Schuller

Publications and source records attributed to Ivan K. Schuller.

At least 19 recordsLinked to original sources

Phase noise analysis and control of VO$_2$-based relaxation type oscillators

VO$_2$-based relaxation oscillators form a rapidly developing field that finds applications in neuromorphic computing, Ising machines, and numerous signal processing concepts. These oscillators operate in a deeply nonlinear relaxation regime based on rapid phase transitions between insulating and metallic states in the VO$_2$ material. This process is governed by thermal effects, which lead to additional voltage fluctuations and contribute to a considerably wide spectral linewidth in the VO$_2$-based oscillator signal. In this work, we thoroughly study the phase noise in VO$_2$-based relaxation oscillators and demonstrate that the broadening of the generation spectrum linewidth at low oscillation frequencies is caused by an increased susceptibility to thermal fluctuations during the incubation phase. We explore the types of noise affecting oscillator stability and show that synchronization with an external square-wave signal improves the phase noise more effectively than a sinusoidal-shape injection locking signal.

physics.app-ph

Signal amplification in simple metal-insulator transition devices

Signal dissipation in large-scale neural networks can lead to information loss and ultimately to computational failures, necessitating local signal amplification at neuron - synapse connections. In biological nervous systems, axons are responsible for local signal amplification. Translating axon functionality into hardware, i.e., the ability to amplify and transmit signals without loss, is non-trivial because emulating the human brain implies building networks composed of ~10 billion interconnected neurons, each requiring a dedicated compact and scalable amplifier. Here, we demonstrate signal amplification in simple two-terminal devices made of a metal-insulator transition material. By operating the devices on the verge of the phase transition and taking advantage of negative differential resistance, we achieve robust signal amplification up to a factor of ~11.5. We also demonstrate the amplification of spiking sequences generated by a real neuristor, opening new exciting opportunities for the direct integration of artificial neurons and axons. The amplification can be controlled by easily adjustable experimental parameters, including DC bias, AC excitation, series resistance, and temperature. We further propose a model that predicts the gain using readily observable transport characteristics. Our results establish a framework for developing and optimizing axon-like amplification functionalities in nonlinear electronic materials.

cond-mat.mtrl-sci

Understanding Damping Mechanisms via Spin Diffusion Length in Low-damping Li$_{0.5}$Al$_{1.0}$Fe$_{1.5}$O$_4$ Spinel Ferrite Thin Films

The mechanisms underlying magnon damping are of fundamental and technological interest in low-damping materials. We find low-damping ferrimagnetic insulator Li$_{0.5}$Al$_{1.0}$Fe$_{1.5}$O$_4$ (LAFO) thin films to be a promising model system for probing these mechanisms because of its distinct temperature dependent spin diffusion length (SDL) trends for electrically and thermally generated magnons. With increasing temperature, the electrical SDL shows minimal change, while the thermal SDL decreases. We attribute these trends to distinct magnon populations and scattering mechanisms: thermally generated high $k$ magnons are limited by magnon-phonon scattering, whereas electrically generated low $k$ magnons are limited by relaxational scattering from magnetic impurities.

cond-mat.mtrl-sci

Inhibitory neuristor based on metal-to-insulator transition

Mimicking the collective excitatory and inhibitory behaviors of biological neurons remains a critical challenge in the development of neuromorphic computing systems that rival the complexity and performance of the human brain. Volatile high-to-low resistance switching in insulator-to-metal transition (IMT) materials produces an abrupt increase in current flow, resembling neuronal excitation. This electrical excitation enables IMT materials to be driven into a neuron-like spiking self-oscillation regime using simple RC circuits. Here, we report a new type of self-oscillation dynamics that occurs in the opposite class of metal-to-insulator transition (MIT) materials. Electrical triggering of the MIT suppresses current flow, resembling neuronal inhibition. Using a prototypical MIT material, we experimentally demonstrate inhibitory-like self-oscillations in two-terminal switching devices incorporated into a simple RL circuit. Our results show robust ~0.1 - 1 MHz electric current oscillations with minimal cycle-to-cycle variation, which can be controlled by varying the applied DC voltage, temperature, and inductance. This work demonstrates a new type of inhibitory MIT-based artificial neuron that can complement the excitatory functionalities of IMT-based neuristors in biologically plausible neuromorphic systems.

cond-mat.mtrl-sci

Martensitic laminate geometry controls electronic phase transitions in a Mott insulator

Symmetry-lowering structural phase transitions result in multiple degenerate structures whose coexistence is determined by macroscopic strain compatibility. In quantum materials, these structural transformations often couple to electronic degrees of freedom, yet how the structural arrangements influence electronic phase transitions remains poorly understood. By analyzing hundreds of diffraction peaks from X-ray reciprocal space mapping, we determine the lattice basis vectors and mutual orientations of all coexisting phases in epitaxial V2O3 thin films after a symmetry-lowering transformation coincident with a metal-insulator transition. We identify the orientations of interfaces between all coexisting structures using the theory of martensitic phase transformations and find that the low temperature structure comprises finely tuned layered mixtures of alternating twin variants, akin to metal alloys. By comparing films grown on various substrate orientations, we show that the metal-insulator transition temperature increases monotonically with the degree to which these layered mixtures satisfy macroscopic strain compatibility imposed by the substrate.

cond-mat.mtrl-sci

Disorder-driven stochastic dynamics in Mott resistive-switching systems

Controlled disorder in correlated materials provides a new route to emergent stochastic dynamics in neuromorphic hardware. Here we show that focused ion beam irradiation in VO$_{2}$- and V$_{2}$O$_{3}$-based resistive-switching oscillators induces a transition from regular periodic oscillations to strongly irregular stochastic firing, while simultaneously reducing the required switching energy by orders of magnitude. Under an applied electric field, these materials undergo a volatile insulator-to-metal transition characterized by the formation of percolating metallic filaments within an insulating bulk. Using numerical simulations based on the Mott resistor network, we demonstrate that defect-induced modifications to filament nucleation and stability drive these devices into stochastic oscillatory regimes. These results are validated by experimental measurements on irradiated VO$_{2}$ and V$_{2}$O$_{3}$ devices.

cond-mat.str-el

Jamming-controlled stochasticity in metal-insulator switching

Understanding and controlling phase transitions is a fundamental part of physics and has been central to many technological revolutions, from steam engines to field-effect transistors. At present, there is strong interest in materials with strongly coupled structural and electronic phase transitions, which hold promise for energy-efficient technologies. Utilizing a structural phase transition and controlling its plasticity naturally leads to built-in memory, a key feature for emulating neurons and synapses in neuromorphic technologies. Here, $\textit{operando}$ Bragg X-ray photon correlation spectroscopy is used to study the evolution of the nano-domain distribution at the micron-scale in neuromorphic devices made from the archetypal Mott insulator vanadium dioxide. It is found that after electrical switching, slow nano-domain reconfiguration occurs on timescales of thousands of seconds and that the domains undergo a jamming transition, offering control over switching stochasticity at the micron scale. More precisely, repetitive above-threshold currents plastically drive the system into a jammed/glassy state where switching becomes deterministic, while sub-threshold currents erase the short-term memory contained in the nano-domain distribution, recovering stochastic switching, thus offering a path for in-device learning. The results illustrate the importance of studying the nanoscale physics associated with phase transitions in strongly correlated materials, even for macroscopic devices, and offer guidance for future device operation schemes.

cond-mat.mes-hall

Electrically induced ferromagnetism in an irradiated complex oxide

In metal-insulator transition materials, a small perturbation can shift the delicate balance between competing or coexisting electronic phases, leading to dramatic changes of the material's properties. Using La0.7Sr0.3MnO3, a prototypical metal-insulator transition manganite, we show that local low-dose focused ion beam irradiation increases resistivity by several orders of magnitude, converting the ferromagnetic-metal ground state into a paramagnetic-insulator. Surprisingly, we found that applying electric stimuli to the irradiated material induces a non-thermal insulator-to-metal transition, which results in low-power, repeatable volatile resistive switching. Magnetotransport measurements revealed that this voltage-induced metallic phase in the irradiated material is ferromagnetic, exhibiting clear anisotropic magnetoresistance. This work, thus, reports the discovery of a unique material in which the electrical triggering of the electronic phase transition results in the onset of magnetism, in stark contrast to the magnetic order suppression commonly observed in other metal-insulator transition switching materials. We demonstrate that local focused ion beam irradiation provides new and exciting opportunities to engineer electronic and magnetic functionalities that can find practical applications ranging from spintronics to neuromorphic hardware.

cond-mat.str-el

Effects of Interactions and Defect Motion on Ramp Reversal Memory in Locally Phase Separated Materials

The ramp-reversal memory (RRM) effect in metal-insulator transition metal oxides (TMOs), a non-volatile resistance change induced by repeated temperature cycling, has attracted considerable interest in neuromorphic computing and non-volatile memory devices. Our previously introduced defect motion model successfully explained RRM in vanadium dioxide (VO$_2$), capturing observed critical temperature shifts and memory accumulation throughout the sample. However, this approach lacked interactions between metallic and insulating domains, whereas the RRM only appears when TMOs are brought into the metal-insulator coexistence regime. Here, we extend our model by combining the Random Field Ising Model with defect diffusion-segregation, thereby enabling accurate hysteresis modeling while predicting the relationship between RRM and domain interactions. Our simulations demonstrate that maximum RRM occurs when the turnaround temperature approaches the warming branch inflection point, consistent with experimental observations on VO$_2$. Most significantly, we find that increasing nearest-neighbor interactions enhances the maximum memory effect, thus providing a clear mechanism for optimizing RRM performance. Since our model employs minimal assumptions, we predict that RRM should be a widespread phenomenon in materials exhibiting patterned phase coexistence of electronic domains. This work not only advances fundamental understanding of memory behavior in TMOs but also establishes a much-needed theoretical framework for optimizing device applications.

cond-mat.mtrl-sci

Enhanced stochasticity in irradiated vanadium oxide oscillators

Insulator-to-metal transition materials are highly sensitive to even minute deviations of stoichiometry, lattice defects, and disorder, which provides opportunities to engineer their electrical switching characteristics. Using V2O3 as a prototypical metal-insulator transition resistive switching material, we demonstrate that localized focused ion beam irradiation can induce stochastic oscillatory dynamics in simple two-terminal switching devices. After irradiating the material, we observed an unusual dynamic regime where the voltage induced metallic state momentarily collapses into an insulating state, which results in a rapid current flickering that is qualitatively different from the conventional current spiking in a Pearson-Anson type oscillatory circuit implemented using the pristine material. Furthermore, the current flickering timing in the irradiated devices becomes progressively more random and more sparse with increasing input voltage, resulting in nonlinear and nondeterministic oscillatory behavior. The irradiation also leads to a dramatic reduction in switching power required to induce the current oscillations. These results are elucidated through random resistor network simulations which indicate that a small number of local sites can control the electrical metal-insulator transition switching properties in large devices with high defect concentration. Our results show that selective focused ion beam irradiation provides exciting prospects for engineering and tuning novel stochastic behaviors in emergent technologies that rely on the intrinsic randomness of physical processes.

cond-mat.dis-nn

Spin Seebeck Effect in Correlated Antiferromagnetic V2O3

The spin Seebeck effect is useful for probing the spin correlations and magnetic order in magnetic insulators. Here, we report a strong longitudinal spin Seebeck effect (LSSE) in antiferromagnetic V2O3 thin films. The LSSE response at cryogenic temperatures increases as a function of the external magnetic field until it approaches saturation. The response at given power and field exhibits a non-monotonic temperature dependence, with a pronounced peak that shifts toward higher temperatures as the field increases. Furthermore, the magnitude of the LSSE signal decreases consistently with increasing thickness, implying that the bulk SSE dominates any interfacial contribution. This negative correlation between the SSE and the thickness implies that the magnon energy relaxation length in V2O3 is shorter than the thickness of our thinnest film, 50 nm, consistent with the strong spin-lattice coupling in this material.

cond-mat.mes-hall

Self-strain suppression of the metal-to-insulator transition in phase-change oxide devices

Quantum 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, we report X-ray nano-diffraction structural imaging of micro-devices fabricated with the archetypal phase-change material vanadium sesquioxide (V$_2$O$_3$). 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 could 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.

cond-mat.mes-hall

Collective dynamics and long-range order in thermal neuristor networks

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.

cond-mat.dis-nn

Low temperature spin Seebeck effect in non-magnetic vanadium dioxide

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.

cond-mat.str-el

Voltage control of spin resonance in phase change materials

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.

physics.app-ph

Laser-induced quenching of metastability at the Mott-insulator to metal transition

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.

cond-mat.str-el

Domain nucleation across the metal-insulator transition of self-strained V2O3 films

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.

cond-mat.mtrl-sci

Disentangling transport mechanisms in a correlated oxide by photoinduced charge injection

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.

cond-mat.str-el