Reorganization Energy upon Controlled Intermolecular Charge-Transfer Reactions in Monolithically Integrated Nanodevices.

Intermolecular electron-transfer reactions are key processes in physics, chemistry, and biology. The electron-transfer rates depend primarily on the system reorganization energy, that is, the energetic cost to rearrange each reactant and its surrounding environment when a charge is transferred. Despite the evident impact of electron-transfer reactions on charge-carrier hopping, well-controlled electronic transport measurements using monolithically integrated electrochemical devices have not successfully measured the reorganization energies to this date. Here, it is shown that self-rolling nanomembrane devices with strain-engineered mechanical properties, on-a-chip monolithic integration, and multi-environment operation features can overcome this challenge. The ongoing advances in nanomembrane-origami technology allow to manufacture the nCap, a nanocapacitor platform, to perform molecular-level charge transport characterization. Thereby, employing nCap, the copper-phthalocyanine (CuPc) reorganization energy is probed, ≈0.93 eV, from temperature-dependent measurements of CuPc nanometer-thick films. Supporting the experimental findings, density functional theory calculations provide the atomistic picture of the measured CuPc charge-transfer reaction. The experimental strategy demonstrated here is a consistent route towards determining the reorganization energy of a system formed by molecules monolithically integrated into electrochemical nanodevices.

Advanced Neuromorphic Applications Enabled by Synaptic Ion-Gating Vertical Transistors.

Bioinspired synaptic devices have shown great potential in artificial intelligence and neuromorphic electronics. Low energy consumption, multi-modal sensing and recording, and multifunctional integration are critical aspects limiting their applications. Recently, a new synaptic device architecture, the ion-gating vertical transistor (IGVT), has been successfully realized and timely applied to perform brain-like perception, such as artificial vision, touch, taste, and hearing. In this short time, IGVTs have already achieved faster data processing speeds and more promising memory capabilities than many conventional neuromorphic devices, even while operating at lower voltages and consuming less power. This work focuses on the cutting-edge progress of IGVT technology, from outstanding fabrication strategies to the design and realization of low-voltage multi-sensing IGVTs for artificial-synapse applications. The fundamental concepts of artificial synaptic IGVTs, such as signal processing, transduction, plasticity, and multi-stimulus perception are discussed comprehensively. The contribution draws special attention to the development and optimization of multi-modal flexible sensor technologies and presents a roadmap for future high-end theoretical and experimental advancements in neuromorphic research that are mostly achievable by the synaptic IGVTs.

Bio-Inspired Dynamically Morphing Microelectronics toward High-Density Energy Applications and Intelligent Biomedical Implants.

Choreographing the adaptive shapes of patterned surfaces to exhibit designable mechanical interactions with their environment remains an intricate challenge. Here, a novel category of strain-engineered dynamic-shape materials, empowering diverse multi-dimensional shape modulations that are combined to form fine-grained adaptive microarchitectures is introduced. Using micro-origami tessellation technology, heterogeneous materials are provided with strategic creases featuring stimuli-responsive micro-hinges that morph precisely upon chemical and electrical cues. Freestanding multifaceted foldable packages, auxetic mesosurfaces, and morphable cages are three of the forms demonstrated herein of these complex 4-dimensional (4D) metamaterials. These systems are integrated in dual proof-of-concept bioelectronic demonstrations: a soft foldable supercapacitor enhancing its power density (≈108 mW cm-2), and a bio-adaptive device with a dynamic shape that may enable novel smart-implant technologies. This work demonstrates that intelligent material systems are now ready to support ultra-flexible 4D microelectronics, which can impart autonomy to devices culminating in the tangible realization of microelectronic morphogenesis.