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Memristive devices based on two-dimensional (2D) materials have emerged as potential synaptic candidates for next-generation neuromorphic computing hardware. Here, we introduce a numerical modeling framework that facilitates efficient exploration of the large parameter space for 2D memristive synaptic devices. High-throughput charge-transport simulations are performed to investigate the voltage pulse characteristics for lateral 2D memristors and synaptic device metrics are studied for different weight-update schemes. We show that the same switching mechanism can lead to fundamentally different pulse characteristics influencing not only the device metrics but also the weight-update direction. A thorough analysis of the parameter space allows simultaneous optimization of the linearity, symmetry, and drift in the synaptic behavior that are related through tradeoffs. The presented modeling framework can serve as a tool for designing 2D memristive devices in practical neuromorphic circuits by providing guidelines for materials properties, device functionality, and system performance for target applications. 

Recent breakthroughs in brain-inspired computing promise to address a wide range of problems from security to healthcare. However, the current strategy of implementing artificial intelligence algorithms using conventional silicon hardware is leading to unsustainable energy consumption. Neuromorphic hardware based on electronic devices mimicking biological systems is emerging as a low-energy alternative, although further progress requires materials that can mimic biological function while maintaining scalability and speed. As a result of their diverse unique properties, atomically thin two-dimensional (2D) materials are promising building blocks for next-generation electronics including nonvolatile memory, in-memory and neuromorphic computing, and flexible edge-computing systems. Furthermore, 2D materials achieve biorealistic synaptic and neuronal responses that extend beyond conventional logic and memory systems. Here, we provide a comprehensive review of the growth, fabrication, and integration of 2D materials and van der Waals heterojunctions for neuromorphic electronic and optoelectronic devices, circuits, and systems. For each case, the relationship between physical properties and device responses is emphasized followed by a critical comparison of technologies for different applications. We conclude with a forward-looking perspective on the key remaining challenges and opportunities for neuromorphic applications that leverage the fundamental properties of 2D materials and heterojunctions. 

We discuss how a dual-gated memtransistor crossbar can accelerate the extraction of the Transformer’s attention scores. A memtransistor is a novel two-dimensional material-based device that offers non-volatile programmability and gate tunability. Leveraging these attributes, we demonstrate the extraction of quadratic-order products on a single memtransistor and the single-step extraction of attention scores without inferring intermediate query/key vectors. The query/key-free processing of memtransistor-based attention scoring results in 2.37× lower energy with less than half crossbar cells. 

Neuromorphic hardware promises to revolutionize information technology with brain-inspired parallel processing, in-memory computing, and energy-efficient implementation of artificial intelligence and machine learning. In particular, two-dimensional (2D) memtransistors enable gate-tunable non-volatile memory, bio-realistic synaptic phenomena, and atomically thin scaling. However, previously reported 2D memtransistors have not achieved low operating voltages without compromising gate-tunability. Here, we overcome this limitation by demonstrating MoS2 memtransistors with short channel lengths < 400 nm, low operating voltages < 1 V, and high field-effect switching ratios > 10,000 while concurrently achieving strong memristive responses. This functionality is realized by fabricating back-gated memtransistors using highly polycrystalline monolayer MoS2 channels on high-κ Al2O3 dielectric layers. Finite-element simulations confirm enhanced electrostatic modulation near the channel contacts, which reduces operating voltages without compromising memristive or field-effect switching. Overall, this work demonstrates a pathway for reducing the size and power consumption of 2D memtransistors as is required for ultrahigh-density integration. 

Van der Waals materials with long-range magnetic order show a range of correlated phenomena that could be of use in the development of optoelectronic and spintronic applications. Magnetically ordered van der Waals semiconductors with spin-polarized currents are, in particular, sensitive to external stimuli such as strain, electrostatic fields, magnetic fields and electromagnetic radiation. Their combination of two-dimensional magnetic order, semiconducting band structure and weak dielectric screening means that these materials could be used to create novel atomically thin opto-spintronic devices. Here we explore the development of van der Waals opto-spintronics. We examine the interplay between optical, magnetic and electronic excitations in van der Waals magnetic semiconductors, and explore the control of their magnetization via external stimuli. We consider fabrication and passivation strategies for the practical handling and design of opto-spintronic devices. We also explore potential opto-spintronic device architectures and applications, which include magnonics, quantum transduction, neuromorphic computing and non-volatile memory. 

Unlike the well-studied and technologically advanced Group III-V and Group II-VI compound semiconductor alloys, alloys of ternary metal oxide semiconductors have only recently begun to receive widespread attention. Here, we describe the effect of alkaline earth metal substitution on the optical, electronic, and photoelectrochemical (PEC) properties of copper metavanadate (CuV₂O₆). As a host, the Cu-V-O compound family presents a versatile framework to develop such composition-property correlations. Alloy compositions of A_0.1Cu_0.9V₂O₆(A = Mg, Ca) photoanodes were synthesized via a time and energy-efficient solution combustion synthesis (SCS) method. The effect of introducing alkaline earth metals (Mg, Ca) on the crystal structure, microstructure, electronic, and optical properties of copper metavanadates was investigated by powder X-ray diffraction (PXRD), scanning electron microscopy (SEM), diffuse reflectance spectroscopy (DRS), transmission electron microscopy (TEM), and Raman spectroscopy. The PXRD, TEM, and Raman spectroscopy data demonstrated the polycrystalline powder samples to be mutually soluble, solid solutions of copper and alkaline earth metal metavanadates and not simple mixtures of these compounds. The DRS data showed a systematic decrease in the optical bandgap with Cu incorporation. These trends were corroborated by electronic band structure calculations. Finally, the PEC properties exhibited a strong dependence on the alloy composition, pointing to possible applicability in solar water splitting, heterogeneous photocatalysis, phosphor lighting/displays, and photovoltaic devices. 

Organic solar cells (OSCs) using non-fullerene acceptors (NFAs) afford exceptional photovoltaic performance metrics, however, their stability remains a significant challenge. Existing OSC stability studies focus on understanding degradation rate-performance relationships, improving interfacial layers, and suppressing degradative chemical reaction pathways. Nevertheless, there is a knowledge gap concerning how such degradation affects crystal structure, electronic states, and recombination dynamics that ultimately impact NFA performance. Here we seek a quantitative relationship between OSC metrics and blend morphology, trap density of states, charge carrier mobility, and recombination processes during the UV-light-induced degradation of PBDB-TF:Y6 inverted solar cells as the PCE (power conversion efficiency) falls from 17.3 to 5.0%. Temperature-dependent electrical and impedance measurements reveal deep traps at 0.48 eV below the conduction band that are unaffected by Y6 degradation, and shallow traps at 0.15 eV below the conduction band that undergo a three-fold density of states increase at the PCE degradation onset. Computational analysis correlates vinyl oxidation with a new trap state at 0.25 eV below the conduction band, likely involving charge transfer from the UV-absorbing ZnO electron transport layer. In-situ integrated photocurrent analysis and transient absorption spectroscopy reveal that these traps lower electron mobility and increase recombination rates during degradation. Grazing-incidence wide-angle x-ray scattering and computational analysis reveal that the degraded Y6 crystallite morphology is largely preserved but that <1% of degraded Y6 molecules cause OSC PCE performance degradation by ≈50%. Together the detailed electrical, impedance, morphological, ultrafast spectroscopic, matrix-assisted laser desorption/ionization time-of-flight (MALDI-ToF) spectroscopy, and computational data reveal that the trap state energies and densities accompanying Y6 vinyl oxidation are primarily responsible for the PCE degradation in these operating NFA-OSCs.