Cryo-Electron Microscopy Reveals Na Infiltration into Separator Pore Free-Volume as a Degradation Mechanism in Na Anode:Liquid Electrolyte Electrochemical Cells.

Batteries utilizing a sodium (Na) metal anode with a liquid electrolyte are promising for affordable large-scale energy storage. However, a deep understanding of the intrinsic degradation mechanisms is limited by challenges in accessing the buried interfaces. Here, cryogenic electron microscopy of intact electrode:separator:electrode stacks is performed and degradation and failure of symmetric Na||Na coin cells occurs through the infiltration of Na metal through the pores of the separator rather than by mechanical puncturing by dendrites is revealed. It is shown the interior structure of the cell (electrode:separator:electrode) must be preserved and deconstructing the cell into different layers for characterization results in artifacts. In intact cell stacks, minimal liquid is found between the electrodes and separator, leading to intimate electrode:separator interfaces. After electrochemical cycling, Na infiltrates into the pore free-volume, growing through the separator to create electrical shorts and degradation. The Na infiltration occurs at interfacial regions devoid of solid-electrolyte interphase (SEI), revealing SEI plays an important role in preventing Na from growing into the separator by being a physical barrier that the plated Na cannot penetrate. These results shed new light on the fundamental failure mechanisms in Na batteries and demonstrate the importance of preserving the cell structure and buried interfaces.

Low-Temperature Synthesis of WSe2 by the Selenization Process under Ultrahigh Vacuum for BEOL Compatible Reconfigurable Neurons.

Low-temperature large-area growth of two-dimensional (2D) transition-metal dichalcogenides (TMDs) is critical for their integration with silicon chips. Especially, if the growth temperatures can be lowered below the back-end-of-line (BEOL) processing temperatures, the Si transistors can interface with 2D devices (in the back end) to enable high-density heterogeneous circuits. Such configurations are particularly useful for neuromorphic computing applications where a dense network of neurons interacts to compute the output. In this work, we present low-temperature synthesis (400 °C) of 2D tungsten diselenide (WSe2) via the selenization of the W film under ultrahigh vacuum (UHV) conditions. This simple yet effective process yields large-area, homogeneous films of 2D TMDs, as confirmed by several characterization techniques, including reflection high-energy electron diffraction, atomic force microscopy, transmission electron microscopy, and different spectroscopy methods. Memristors fabricated using the grown WSe2 film are leveraged to realize a novel compact neuron circuit that can be reconfigured to enable homeostasis.

Ultra-fast switching memristors based on two-dimensional materials.

The ability to scale two-dimensional (2D) material thickness down to a single monolayer presents a promising opportunity to realize high-speed energy-efficient memristors. Here, we report an ultra-fast memristor fabricated using atomically thin sheets of 2D hexagonal Boron Nitride, exhibiting the shortest observed switching speed (120 ps) among 2D memristors and low switching energy (2pJ). Furthermore, we study the switching dynamics of these memristors using ultra-short (120ps-3ns) voltage pulses, a frequency range that is highly relevant in the context of modern complementary metal oxide semiconductor (CMOS) circuits. We employ statistical analysis of transient characteristics to gain insights into the memristor switching mechanism. Cycling endurance data confirms the ultra-fast switching capability of these memristors, making them attractive for next generation computing, storage, and Radio-Frequency (RF) circuit applications.

Precision Synthesis of Bimetallic Nanoparticles via Nanofluidics in Nanopipets.

Bimetallic nanoparticles often show properties superior to their single-component counterparts. However, the large parameter space, including size, structure, composition, and spatial arrangement, impedes the discovery of the best nanoparticles for a given application. High-throughput methods that can control the composition and spatial arrangement of the nanoparticles are desirable for accelerated materials discovery. Herein, we report a methodology for synthesizing bimetallic alloy nanoparticle arrays with precise control over their composition and spatial arrangement. A dual-channel nanopipet is used, and nanofluidic control in the nanopipet further enables precise tuning of the electrodeposition rate of each element, which determines the final composition of the nanoparticle. The composition control is validated by finite element simulation as well as electrochemical and elemental analyses. The scope of the particles demonstrated includes Cu-Ag, Cu-Pt, Au-Pt, Cu-Pb, and Co-Ni. We further demonstrate surface patterning using Cu-Ag alloys with precise control of the location and composition of each pixel. Additionally, combining the nanoparticle alloy synthesis method with scanning electrochemical cell microscopy (SECCM) allows for fast screening of electrocatalysts. The method is generally applicable for synthesizing metal nanoparticles that can be electrodeposited, which is important toward developing automated synthesis and screening systems for accelerated material discovery in electrocatalysis.