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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. 

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.