Showing papers by "Ivan K. Schuller published in 2021"

Energy-efficient Mott activation neuron for full-hardware implementation of neural networks.

Abstract: To circumvent the von Neumann bottleneck, substantial progress has been made towards in-memory computing with synaptic devices. However, compact nanodevices implementing non-linear activation functions are required for efficient full-hardware implementation of deep neural networks. Here, we present an energy-efficient and compact Mott activation neuron based on vanadium dioxide and its successful integration with a conductive bridge random access memory (CBRAM) crossbar array in hardware. The Mott activation neuron implements the rectified linear unit function in the analogue domain. The neuron devices consume substantially less energy and occupy two orders of magnitude smaller area than those of analogue complementary metal-oxide semiconductor implementations. The LeNet-5 network with Mott activation neurons achieves 98.38% accuracy on the MNIST dataset, close to the ideal software accuracy. We perform large-scale image edge detection using the Mott activation neurons integrated with a CBRAM crossbar array. Our findings provide a solution towards large-scale, highly parallel and energy-efficient in-memory computing systems for neural networks.

Spatiotemporal characterization of the field-induced insulator-to-metal transition.

Abstract: Many correlated systems feature an insulator-to-metal transition that can be triggered by an electric field. Although it is known that metallization takes place through filament formation, the details of how this process initiates and evolves remain elusive. We use in-operando optical reflectivity to capture the growth dynamics of the metallic phase with space and time resolution. We demonstrate that filament formation is triggered by nucleation at hotspots, with a subsequent expansion over several decades in time. By comparing three case studies (VO2, V3O5, and V2O3), we identify the resistivity change across the transition as the crucial parameter governing this process. Our results provide a spatiotemporal characterization of volatile resistive switching in Mott insulators, which is important for emerging technologies, such as optoelectronics and neuromorphic computing.

Controlling Metal-Insulator Transitions in Vanadium Oxide Thin Films by Modifying Oxygen Stoichiometry.

Abstract: Vanadium oxides are strongly correlated materials which display metal-insulator transitions (MITs) 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 concentrations in VOX thin films by carefully tuning the 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 Magneli phases. A variety of annealing routes were found to achieve the desired phases and eventually control the MIT. The pronounced MIT of the transformed films along with the detailed structural investigations based on X-ray diffraction measurements and X-ray photoelectron spectroscopy 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 because of strain and finite size effects. Our study demonstrates new pathways to strategically tune the oxygen stoichiometry in complex oxides and provides a road map for understanding the phase stability of VOX thin films.

Operando characterization of conductive filaments during resistive switching in Mott VO2.

Abstract: Vanadium dioxide (VO2) has attracted much attention owing to its metal-insulator transition near room temperature and the ability to induce volatile resistive switching, a key feature for developing novel hardware for neuromorphic computing. Despite this interest, the mechanisms for nonvolatile switching functioning as synapse in this oxide remain not understood. In this work, we use in situ transmission electron microscopy, electrical transport measurements, and numerical simulations on Au/VO2/Ge vertical devices to study the electroforming process. We have observed the formation of V5O9 conductive filaments with a pronounced metal-insulator transition and that vacancy diffusion can erase the filament, allowing for the system to "forget." Thus, both volatile and nonvolatile switching can be achieved in VO2, useful to emulate neuronal and synaptic behaviors, respectively. Our systematic operando study of the filament provides a more comprehensive understanding of resistive switching, key in the development of resistive switching-based neuromorphic computing.

Switchable Optically Active Schottky Barrier in La0.7Sr0.3MnO3/BaTiO3/ITO Ferroelectric Tunnel Junction

Abstract: One of the most desirable attributes of non-volatile memories and memristors is a fast and non-destructive read out of their resistive state. Prototypical ferroelectric (FE) memories use the bulk photovoltaic response associated to the polarization of FE films to address this requirement by optically sensing binary memory cells. A more advanced type of non-volatile memories is FE tunnel junctions (FTJs). They feature resistive state ratios R_High/R_Low up to 10^6, with a continuum of resistive states accessible, making them promising candidates for neuromorphic computing applications. A novel approach is presented to achieve the optical sensing of the resistive state in a La_(0.7)Sr_(0.3)MnO_3/BaTiO_3/ITO FTJ, by using the Schottky barrier forming in the La_(0.7)Sr_(0.3)MnO_3/BaTiO_3/ITO interface to dramatically enhance the optical response of the 5 nm BaTiO3 (BTO) barrier. Illumination with UV light exceeding the BTO bandgap through the top transparent ITO electrode generates a photovoltaic response in the R_High state, with an open circuit voltage V_oc of 400 mV at 20 K, enabling the optical sensing of the resistive state. In the R_Low state, the Schottky barrier is removed and the photoresponse disappears.

Inherent stochasticity during insulator–metal transition in VO2

Abstract: Vanadium dioxide (VO2), which exhibits a near-room-temperature insulator-metal transition, has great potential in applications of neuromorphic computing devices. Although its volatile switching property, which could emulate neuron spiking, has been studied widely, nanoscale studies of the structural stochasticity across the phase transition are still lacking. In this study, using in situ transmission electron microscopy and ex situ resistive switching measurement, we successfully characterized the structural phase transition between monoclinic and rutile VO2 at local areas in planar VO2/TiO2 device configuration under external biasing. After each resistive switching, different VO2 monoclinic crystal orientations are observed, forming different equilibrium states. We have evaluated a statistical cycle-to-cycle variation, demonstrated a stochastic nature of the volatile resistive switching, and presented an approach to study in-plane structural anisotropy. Our microscopic studies move a big step forward toward understanding the volatile switching mechanisms and the related applications of VO2 as the key material of neuromorphic computing.

Metal-insulator transition in V 2 O 3 with intrinsic defects

Abstract: Vanadium sesquioxide (${\mathrm{V}}_{2}{\mathrm{O}}_{3}$) is a Mott insulator exhibiting a temperature-dependent metal-insulator transition (MIT) at 165 K accompanied by both a magnetic and structural transition. Although it is expected to be a metal under conventional band theory, electron interactions at low temperature cause it to behave like an insulator, making it difficult to accurately model its electronic properties with standard ab initio methods. As such, accurate theoretical assessments of the MIT with point defects requires special attention to the type of functionals used. In this study, we conclude that the $\mathrm{PBE}+U$ functional provides the best compromise between accuracy and efficiency in calculating the properties related to the MIT between low-temperature and high-temperature ${\mathrm{V}}_{2}{\mathrm{O}}_{3}$. We use this functional to explore the various influences that intrinsic point defects will have on the MIT in ${\mathrm{V}}_{2}{\mathrm{O}}_{3}$.

Transverse barrier formation by electrical triggering of a metal-to-insulator transition.

Abstract: 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 a conducting filament parallel to the current flow, is a highly active research topic. Using the magneto-optical Kerr imaging, we found that the opposite type of resistive switching, from a metal into an insulator, occurs in a reciprocal characteristic spatial pattern: the formation of an insulating barrier perpendicular to the driving current. This barrier formation leads to an unusual N-type negative differential resistance in the current-voltage characteristics. We further demonstrate that electrically inducing a transverse barrier enables a unique approach to voltage-controlled magnetism. By triggering the metal-to-insulator resistive switching in a magnetic material, local on/off control of ferromagnetism is achieved using a global voltage bias applied to the whole device.

Cation and anion topotactic transformations in cobaltite thin films leading to Ruddlesden-Popper phases

Abstract: Author(s): Chiu, IT; Lee, MH; Cheng, S; Zhang, S; Heki, L; Zhang, Z; Mohtashami, Y; Lapa, PN; Feng, M; Shafer, P; N'Diaye, AT; Mehta, A; Schuller, JA; Galli, G; Ramanathan, S; Zhu, Y; Schuller, IK; Takamura, Y | Abstract: Topotactic transformations involve structural changes between related crystal structures due to a loss or gain of material while retaining a crystallographic relationship. The perovskite oxide La0.7Sr0.3CoO3 (LSCO) is an ideal system for investigating phase transformations due to its high oxygen vacancy conductivity, relatively low oxygen vacancy formation energy, and strong coupling of the magnetic and electronic properties to the oxygen stoichiometry. While the transition between cobaltite perovskite and brownmillerite (BM) phases has been widely reported, further reduction beyond the BM phase lacks systematic studies. In this paper, we study the evolution of the physical properties of LSCO thin films upon exposure to highly reducing environments. We observe the rarely reported crystalline Ruddlesden-Popper phase, which involves the loss of both oxygen anions and cobalt cations upon annealing where the cobalt is found as isolated Co ions or Co nanoparticles. First-principles calculations confirm that the concurrent loss of oxygen and cobalt ions is thermodynamically possible through an intermediary BM phase. The strong correlation of the magnetic and electronic properties to the crystal structure highlights the potential of utilizing ion migration as a basis for emerging applications such as neuromorphic computing.

Quantum Sensing of Insulator-to-Metal Transitions in a Mott Insulator

Abstract: 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.

Quantum Sensing of Insulator‐to‐Metal Transitions in a Mott Insulator

Abstract: 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.

A hybrid optoelectronic Mott insulator

Abstract: 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 versatile 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 (MIT) is technologically attractive due to the large changes in resistance, tunable by doping, strain, electric fields, and orbital occupancy but not, in and of itself, controllable with light. Here, an alternate approach is presented to produce optical functionalities using a properly engineered photoconductor/strongly correlated hybrid heterostructure. This approach combines a photoconductor, which does not exhibit an MIT, with a strongly correlated oxide, which is not photoconducting. Due to the intimate proximity between the two materials, the heterostructure exhibits giant volatile and nonvolatile, photoinduced resistivity changes with substantial shifts in the MIT transition temperatures. This approach can be extended to other judicious combinations of strongly correlated materials.

Imaging the itinerant-to-localized transmutation of electrons across the metal-to-insulator transition in V2O3

Abstract: 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 V2O3, 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.

A quantum material spintronic resonator

Abstract: In a spintronic resonator a radio-frequency signal excites spin dynamics that can be detected by the spin-diode effect. Such resonators are generally based on ferromagnetic metals and their responses to spin torques. New and richer functionalities can potentially be achieved with quantum materials, specifically with transition metal oxides that have phase transitions that can endow a spintronic resonator with hysteresis and memory. Here we present the spin torque ferromagnetic resonance characteristics of a hybrid metal-insulator-transition oxide/ ferromagnetic metal nanoconstriction. Our samples incorporate $${\mathrm {V}}_2{\mathrm {O}}_3$$ , with Ni, Permalloy ( $${\hbox {Ni}}_{80}{\hbox {Fe}}_{20}$$ ) and Pt layers patterned into a nanoconstriction geometry. The first order phase transition in $${\mathrm {V}}_2{\mathrm {O}}_3$$ is shown to lead to systematic changes in the resonance response and hysteretic current control of the ferromagnetic resonance frequency. Further, the output signal can be systematically varied by locally changing the state of the $${\mathrm {V}}_2{\mathrm {O}}_3$$ with a dc current. These results demonstrate new spintronic resonator functionalities of interest for neuromorphic computing.

Driving magnetic domains at the nanoscale by interfacial strain-induced proximity

Abstract: We investigate the local nanoscale changes of the magnetic anisotropy of a Ni film subject to an inverse magnetostrictive effect by proximity to a V2O3 layer. Using temperature-dependent photoemission electron microscopy (PEEM) combined with X-ray magnetic circular dichroism (XMCD), direct images of the Ni spin alignment across the first-order structural phase transition (SPT) of V2O3 were obtained. We find an abrupt temperature-driven reorientation of the Ni magnetic domains across the SPT, which is associated with a large increase of the coercive field. Moreover, angular dependent ferromagnetic resonance (FMR) shows a remarkable change in the magnetic anisotropy of the Ni film across the SPT of V2O3. Micromagnetic simulations based on these results are in quantitative agreement with the PEEM data. Direct measurements of the lateral correlation length of the Ni domains from XMCD images show an increase of almost one order of magnitude at the SPT compared to room temperature, as well as a broad spatial distribution of the local transition temperatures, thus corroborating the phase coexistence of Ni anisotropies caused by the V2O3 SPT. We show that the rearrangement of the Ni domains is due to strain induced by the oxide layers’ structural domains across the SPT. Our results illustrate the use of alternative hybrid systems to manipulate magnetic domains at the nanoscale, which allows for engineering of coercive fields for novel data storage architectures.

Imaging of Electrothermal Filament Formation in a Mott Insulator

Abstract: Resistive switching---the current- and voltage-induced change of electrical resistance---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 are 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 $\mathrm{V}$${}_{2}$$\mathrm{O}$${}_{3}$ thin-film device using high-resolution wide-field microscopy in combination with electric transport measurements. We investigate the interaction of the electrothermal instability with the strain-induced spontaneous phase separation in the $\mathrm{V}$${}_{2}$$\mathrm{O}$${}_{3}$ thin film at the Mott transition. The photomicrographs show the formation of a narrow metallic filament with a minimum width $\ensuremath{\lesssim}500$ 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 such as oblique filaments, filament splitting, and hysteretic IVCs with sawtoothlike jumps at high currents in the low-resistance regime. We are 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.

Voltage-controlled magnetism enabled by resistive switching

Abstract: 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.