Memristors with Tunable Volatility for Reconfigurable Neuromorphic Computing.

Neuromorphic computing promises an energy-efficient alternative to traditional digital processors in handling data-heavy tasks, primarily driven by the development of both volatile (neuronal) and nonvolatile (synaptic) resistive switches or memristors. However, despite their energy efficiency, memristor-based technologies presently lack functional tunability, thus limiting their competitiveness with arbitrarily programmable (general purpose) digital computers. This work introduces a two-terminal bilayer memristor, which can be tuned among neuronal, synaptic, and hybrid behaviors. The varying behaviors are accessed via facile control over the filament formed within the memristor, enabled by the interplay between the two active ionic species (oxygen vacancies and metal cations). This solution is unlike single-species ion migration employed in most other memristors, which makes their behavior difficult to control. By reconfiguring a single crossbar array of hybrid memristors, two different applications that usually require distinct types of devices are demonstrated - reprogrammable heterogeneous reservoir computing and arbitrary non-Euclidean graph networks. Thus, this work outlines a potential path toward functionally reconfigurable postdigital computers.

Mott neurons with dual thermal dynamics for spatiotemporal computing.

Heat dissipation is a natural consequence of operating any electronic system. In nearly all computing systems, such heat is usually minimized by design and cooling. Here, we show that the temporal dynamics of internally produced heat in electronic devices can be engineered to both encode information within a single device and process information across multiple devices. In our demonstration, electronic NbOx Mott neurons, integrated on a flexible organic substrate, exhibit 18 biomimetic neuronal behaviours and frequency-based nociception within a single component by exploiting both the thermal dynamics of the Mott transition and the dynamical thermal interactions with the organic substrate. Further, multiple interconnected Mott neurons spatiotemporally communicate purely via heat, which we use for graph optimization by consuming over 106 times less energy when compared with the best digital processors. Thus, exploiting natural thermal processes in computing can lead to functionally dense, energy-efficient and radically novel mixed-physics computing primitives.

Picosecond carrier dynamics in InAs and GaAs revealed by ultrafast electron microscopy.

Understanding the limits of spatiotemporal carrier dynamics, especially in III-V semiconductors, is key to designing ultrafast and ultrasmall optoelectronic components. However, identifying such limits and the properties controlling them has been elusive. Here, using scanning ultrafast electron microscopy, in bulk n-GaAs and p-InAs, we simultaneously measure picosecond carrier dynamics along with three related quantities: subsurface band bending, above-surface vacuum potentials, and surface trap densities. We make two unexpected observations. First, we uncover a negative-time contrast in secondary electrons resulting from an interplay among these quantities. Second, despite dopant concentrations and surface state densities differing by many orders of magnitude between the two materials, their carrier dynamics, measured by photoexcited band bending and filling of surface states, occur at a seemingly common timescale of about 100 ps. This observation may indicate fundamental kinetic limits tied to a multitude of material and surface properties of optoelectronic III-V semiconductors and highlights the need for techniques that simultaneously measure electro-optical kinetic properties.

True random number generation using the spin crossover in LaCoO3.

While digital computers rely on software-generated pseudo-random number generators, hardware-based true random number generators (TRNGs), which employ the natural physics of the underlying hardware, provide true stochasticity, and power and area efficiency. Research into TRNGs has extensively relied on the unpredictability in phase transitions, but such phase transitions are difficult to control given their often abrupt and narrow parameter ranges (e.g., occurring in a small temperature window). Here we demonstrate a TRNG based on self-oscillations in LaCoO3 that is electrically biased within its spin crossover regime. The LaCoO3 TRNG passes all standard tests of true stochasticity and uses only half the number of components compared to prior TRNGs. Assisted by phase field modeling, we show how spin crossovers are fundamentally better in producing true stochasticity compared to traditional phase transitions. As a validation, by probabilistically solving the NP-hard max-cut problem in a memristor crossbar array using our TRNG as a source of the required stochasticity, we demonstrate solution quality exceeding that using software-generated randomness.

Tunable stochastic memristors for energy-efficient encryption and computing.

Information security and computing, two critical technological challenges for post-digital computation, pose opposing requirements - security (encryption) requires a source of unpredictability, while computing generally requires predictability. Each of these contrasting requirements presently necessitates distinct conventional Si-based hardware units with power-hungry overheads. This work demonstrates Cu0.3Te0.7/HfO2 ('CuTeHO') ion-migration-driven memristors that satisfy the contrasting requirements. Under specific operating biases, CuTeHO memristors generate truly random and physically unclonable functions, while under other biases, they perform universal Boolean logic. Using these computing primitives, this work experimentally demonstrates a single system that performs cryptographic key generation, universal Boolean logic operations, and encryption/decryption. Circuit-based calculations reveal the energy and latency advantages of the CuTeHO memristors in these operations. This work illustrates the functional flexibility of memristors in implementing operations with varying component-level requirements.

High Thermal Conductivity of Submicrometer Aluminum Nitride Thin Films Sputter-Deposited at Low Temperature.

Aluminum nitride (AlN) is one of the few electrically insulating materials with excellent thermal conductivity, but high-quality films typically require exceedingly hot deposition temperatures (>1000 °C). For thermal management applications in dense or high-power integrated circuits, it is important to deposit heat spreaders at low temperatures (<500 °C), without affecting the underlying electronics. Here, we demonstrate 100 nm to 1.7 µm thick AlN films achieved by low-temperature (<100 °C) sputtering, correlating their thermal properties with their grain size and interfacial quality, which we analyze by X-ray diffraction, transmission X-ray microscopy, as well as Raman and Auger spectroscopy. Controlling the deposition conditions through the partial pressure of reactive N2, we achieve an ∼3× variation in thermal conductivity (∼36-104 W m-1 K-1) of ∼600 nm films, with the upper range representing one of the highest values for such film thicknesses at room temperature, especially at deposition temperatures below 100 °C. Defect densities are also estimated from the thermal conductivity measurements, providing insight into the thermal engineering of AlN that can be optimized for application-specific heat spreading or thermal confinement.

ECRAM Materials, Devices, Circuits and Architectures: A Perspective.

Non-von-Neumann computing using neuromorphic systems based on two-terminal resistive nonvolatile memory elements has emerged as a promising approach, but its full potential has not been realized due to the lack of materials and devices with the appropriate attributes. Unlike memristors, which require large write currents to drive phase transformations or filament growth, electrochemical random access memory (ECRAM) decouples the "write" and "read" operations using a "gate" electrode to tune the conductance state through charge-transfer reactions, and every electron transferred through the external circuit in ECRAM corresponds to the migration of ≈1 ion used to store analogue information. Like static dopants in traditional semiconductors, electrochemically inserted ions modulate the conductivity by locally perturbing a host's electronic structure; however, ECRAM does so in a dynamic and reversible manner. The resulting change in conductance can span orders of magnitude, from gradual increments needed for analog elements, to large, abrupt changes for dynamically reconfigurable adaptive architectures. In this in-depth perspective, the history of ECRAM, the recent progress in devices spanning organic, inorganic, and 2D materials, circuits, architectures, the rich portfolio of challenging, fundamental questions, and how ECRAM can be harnessed to realize a new paradigm for low-power neuromorphic computing are discussed.

Electro-Thermal Characterization of Dynamical VO2 Memristors via Local Activity Modeling.

Translating the surging interest in neuromorphic electronic components, such as those based on nonlinearities near Mott transitions, into large-scale commercial deployment faces steep challenges in the current lack of means to identify and design key material parameters. These issues are exemplified by the difficulties in connecting measurable material properties to device behavior via circuit element models. Here, the principle of local activity is used to build a model of VO2 /SiN Mott threshold switches by sequentially accounting for constraints from a minimal set of quasistatic and dynamic electrical and high-spatial-resolution thermal data obtained via in situ thermoreflectance mapping. By combining independent data sets for devices with varying dimensions, the model is distilled to measurable material properties, and device scaling laws are established. The model can accurately predict electrical and thermal conductivities and capacitances and locally active dynamics (especially persistent spiking self-oscillations). The systematic procedure by which this model is developed has been a missing link in predictively connecting neuromorphic device behavior with their underlying material properties, and should enable rapid screening of material candidates before employing expensive manufacturing processes and testing procedures.

Universal phase dynamics in VO2 switches revealed by ultrafast operando diffraction.

Understanding the pathways and time scales underlying electrically driven insulator-metal transitions is crucial for uncovering the fundamental limits of device operation. Using stroboscopic electron diffraction, we perform synchronized time-resolved measurements of atomic motions and electronic transport in operating vanadium dioxide (VO2) switches. We discover an electrically triggered, isostructural state that forms transiently on microsecond time scales, which is shown by phase-field simulations to be stabilized by local heterogeneities and interfacial interactions between the equilibrium phases. This metastable phase is similar to that formed under photoexcitation within picoseconds, suggesting a universal transformation pathway. Our results establish electrical excitation as a route for uncovering nonequilibrium and metastable phases in correlated materials, opening avenues for engineering dynamical behavior in nanoelectronics.

Third-order nanocircuit elements for neuromorphic engineering.

Current hardware approaches to biomimetic or neuromorphic artificial intelligence rely on elaborate transistor circuits to simulate biological functions. However, these can instead be more faithfully emulated by higher-order circuit elements that naturally express neuromorphic nonlinear dynamics1-4. Generating neuromorphic action potentials in a circuit element theoretically requires a minimum of third-order complexity (for example, three dynamical electrophysical processes)5, but there have been few examples of second-order neuromorphic elements, and no previous demonstration of any isolated third-order element6-8. Using both experiments and modelling, here we show how multiple electrophysical processes-including Mott transition dynamics-form a nanoscale third-order circuit element. We demonstrate simple transistorless networks of third-order elements that perform Boolean operations and find analogue solutions to a computationally hard graph-partitioning problem. This work paves a way towards very compact and densely functional neuromorphic computing primitives, and energy-efficient validation of neuroscientific models.

Fast Spiking of a Mott VO2-Carbon Nanotube Composite Device.

The recent surge of interest in brain-inspired computing and power-efficient electronics has dramatically bolstered development of computation and communication using neuron-like spiking signals. Devices that can produce rapid and energy-efficient spiking could significantly advance these applications. Here we demonstrate direct current or voltage-driven periodic spiking with sub-20 ns pulse widths from a single device composed of a thin VO2 film with a metallic carbon nanotube as a nanoscale heater, without using an external capacitor. Compared with VO2-only devices, adding the nanotube heater dramatically decreases the transient duration and pulse energy, and increases the spiking frequency, by up to 3 orders of magnitude. This is caused by heating and cooling of the VO2 across its insulator-metal transition being localized to a nanoscale conduction channel in an otherwise bulk medium. This result provides an important component of energy-efficient neuromorphic computing systems and a lithography-free technique for energy-scaling of electronic devices that operate via bulk mechanisms.

Separation of current density and electric field domains caused by nonlinear electronic instabilities.

In 1963 Ridley postulated that under certain bias conditions circuit elements exhibiting a current- or voltage-controlled negative differential resistance will separate into coexisting domains with different current densities or electric fields, respectively, in a process similar to spinodal decomposition of a homogeneous liquid or disproportionation of a metastable chemical compound. The ensuing debate, however, failed to agree on the existence or causes of such electronic decomposition. Using thermal and chemical spectro-microscopy, we directly imaged signatures of current-density and electric-field domains in several metal oxides. The concept of local activity successfully predicts initiation and occurrence of spontaneous electronic decomposition, accompanied by a reduction in internal energy, despite unchanged power input and heat output. This reveals a thermodynamic constraint required to properly model nonlinear circuit elements. Our results explain the electroforming process that initiates information storage via resistance switching in metal oxides and has significant implications for improving neuromorphic computing based on nonlinear dynamical devices.

Physical origins of current and temperature controlled negative differential resistances in NbO2.

Negative differential resistance behavior in oxide memristors, especially those using NbO2, is gaining renewed interest because of its potential utility in neuromorphic computing. However, there has been a decade-long controversy over whether the negative differential resistance is caused by a relatively low-temperature non-linear transport mechanism or a high-temperature Mott transition. Resolving this issue will enable consistent and robust predictive modeling of this phenomenon for different applications. Here we examine NbO2 memristors that exhibit both a current-controlled and a temperature-controlled negative differential resistance. Through thermal and chemical spectromicroscopy and numerical simulations, we confirm that the former is caused by a ~400 K non-linear-transport-driven instability and the latter is caused by the ~1000 K Mott metal-insulator transition, for which the thermal conductance counter-intuitively decreases in the metallic state relative to the insulating state.The development of future computation devices will be aided by a better understanding of the physics underlying material behaviors. Using thermoreflectance and spatially resolved X-ray microscopy, Kumar et al. elucidate the origin of two types of negative differential resistance in NbO2 memristors.

Chaotic dynamics in nanoscale NbO2 Mott memristors for analogue computing.

At present, machine learning systems use simplified neuron models that lack the rich nonlinear phenomena observed in biological systems, which display spatio-temporal cooperative dynamics. There is evidence that neurons operate in a regime called the edge of chaos that may be central to complexity, learning efficiency, adaptability and analogue (non-Boolean) computation in brains. Neural networks have exhibited enhanced computational complexity when operated at the edge of chaos, and networks of chaotic elements have been proposed for solving combinatorial or global optimization problems. Thus, a source of controllable chaotic behaviour that can be incorporated into a neural-inspired circuit may be an essential component of future computational systems. Such chaotic elements have been simulated using elaborate transistor circuits that simulate known equations of chaos, but an experimental realization of chaotic dynamics from a single scalable electronic device has been lacking. Here we describe niobium dioxide (NbO2) Mott memristors each less than 100 nanometres across that exhibit both a nonlinear-transport-driven current-controlled negative differential resistance and a Mott-transition-driven temperature-controlled negative differential resistance. Mott materials have a temperature-dependent metal-insulator transition that acts as an electronic switch, which introduces a history-dependent resistance into the device. We incorporate these memristors into a relaxation oscillator and observe a tunable range of periodic and chaotic self-oscillations. We show that the nonlinear current transport coupled with thermal fluctuations at the nanoscale generates chaotic oscillations. Such memristors could be useful in certain types of neural-inspired computation by introducing a pseudo-random signal that prevents global synchronization and could also assist in finding a global minimum during a constrained search. We specifically demonstrate that incorporating such memristors into the hardware of a Hopfield computing network can greatly improve the efficiency and accuracy of converging to a solution for computationally difficult problems.

Spatially uniform resistance switching of low current, high endurance titanium-niobium-oxide memristors.

We analyzed micrometer-scale titanium-niobium-oxide prototype memristors, which exhibited low write-power (<3 µW) and energy (<200 fJ per bit per µm2), low read-power (∼nW), and high endurance (>millions of cycles). To understand their physico-chemical operating mechanisms, we performed in operando synchrotron X-ray transmission nanoscale spectromicroscopy using an ultra-sensitive time-multiplexed technique. We observed only spatially uniform material changes during cell operation, in sharp contrast to the frequently detected formation of a localized conduction channel in transition-metal-oxide memristors. We also associated the response of assigned spectral features distinctly to non-volatile storage (resistance change) and writing of information (application of voltage and Joule heating). These results provide critical insights into high-performance memristors that will aid in device design, scaling and predictive circuit-modeling, all of which are essential for the widespread deployment of successful memristor applications.

Conduction Channel Formation and Dissolution Due to Oxygen Thermophoresis/Diffusion in Hafnium Oxide Memristors.

Transition-metal-oxide memristors, or resistive random-access memory (RRAM) switches, are under intense development for storage-class memory because of their favorable operating power, endurance, speed, and density. Their commercial deployment critically depends on predictive compact models based on understanding nanoscale physicochemical forces, which remains elusive and controversial owing to the difficulties in directly observing atomic motions during resistive switching, Here, using scanning transmission synchrotron X-ray spectromicroscopy to study in situ switching of hafnium oxide memristors, we directly observed the formation of a localized oxygen-deficiency-derived conductive channel surrounded by a low-conductivity ring of excess oxygen. Subsequent thermal annealing homogenized the segregated oxygen, resetting the cells toward their as-grown resistance state. We show that the formation and dissolution of the conduction channel are successfully modeled by radial thermophoresis and Fick diffusion of oxygen atoms driven by Joule heating. This confirmation and quantification of two opposing nanoscale radial forces that affect bipolar memristor switching are important components for any future physics-based compact model for the electronic switching of these devices.

Direct Observation of Localized Radial Oxygen Migration in Functioning Tantalum Oxide Memristors.

Oxygen migration in tantalum oxide, a promising next-generation storage material, is studied using in operando X-ray absorption spectromicroscopy. This approach allows a physical description of the evolution of conduction channel and eventual device failure. The observed ring-like patterns of oxygen concentration are modeled using thermophoretic forces and Fick diffusion, establishing the critical role of temperature-driven oxygen migration.

Sequential electronic and structural transitions in VO2 observed using X-ray absorption spectromicroscopy.

The popular dual electronic and structural transitions in VO2 are explored using X-ray absorption spectromicroscopy with high spatial and spectral resolutions. It is found that during both heating and cooling, the electronic transition always precedes the structural Peierls transition. Between the two transitions, there are intermediate states that are spectrally isolated here.

Local temperature redistribution and structural transition during joule-heating-driven conductance switching in VO2.

Joule-heating induced conductance-switching is studied in VO2 , a Mott insulator. Complementary in situ techniques including optical characterization, blackbody microscopy, scanning transmission X-ray microscopy (STXM) and numerical simulations are used. Abrupt redistribution in local temperature is shown to occur upon conductance-switching along with a structural phase transition, at the same current.