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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.more » « less
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Bimetallic heterostructures, including core–shell and Janus configurations, often offer unique electrocatalytic properties compared to monometallic nanoparticles. However, achieving precise control over both elemental composition and spatial arrangement within these structures remains a challenge. Here, an electrosynthesis method is introduced that enables the fabrication of heterostructured bimetallic nanoparticles with precise, independent control of their elemental distribution. By leveraging dual‐channel scanning electrochemical cell microscopy (SECCM), the local ionic environment is dynamically modulated in situ, adjusting the deposition bias between channels to achieve selective electrodeposition. This approach allows temporal control over the solution conditions within the SECCM droplet, facilitating the synthesis of multi‐layer core–shell nanoparticles with tunable thickness, number, and sequence of layers. This technique is demonstrated with Pt–Cu and Pt–Ni systems, synthesizing arrays of Cu@Pt and Pt@Cu core–shell structures, which are then screened for catalytic activity in hydrogen evolution (HER) and oxygen reduction (ORR) reactions. The high spatial resolution and on‐demand control over the composition and structure make this method well‐suitable for creating arrays of complex, multi‐metallic heterostructures, which is expected to accelerate the discovery of advanced electrocatalytic materials, offering a platform for efficient and scalable electrocatalyst screening.more » « less
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Abstract 2D memristors have demonstrated attractive resistive switching characteristics recently but also suffer from the reliability issue, which limits practical applications. Previous efforts on 2D memristors have primarily focused on exploring new material systems, while damage from the metallization step remains a practical concern for the reliability of 2D memristors. Here, the impact of metallization conditions and the thickness of MoS2films on the reliability and other device metrics of MoS2‐based memristors is carefully studied. The statistical electrical measurements show that the reliability can be improved to 92% for yield and improved by ≈16× for average DC cycling endurance in the devices by reducing the top electrode (TE) deposition rate and increasing the thickness of MoS2films. Intriguing convergence of switching voltages and resistance ratio is revealed by the statistical analysis of experimental switching cycles. An “effective switching layer” model compatible with both monolayer and few‐layer MoS2, is proposed to understand the reliability improvement related to the optimization of fabrication configuration and the convergence of switching metrics. The Monte Carlo simulations help illustrate the underlying physics of endurance failure associated with cluster formation and provide additional insight into endurance improvement with device fabrication optimization.more » « less
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Abstract Single-photon emitters are crucial building blocks for optical quantum technologies. Hexagonal boron nitride (hBN) is a promising two-dimensional material that hosts bright, room-temperature single-photon emitters. However, photo instability is a persistent challenge preventing practical applications of these properties. Here, we reveal the ubiquitous photobleaching of hBN vacancy emitters. Independent of the source or the number of hBN layers, we find that the photobleaching of a common emission at 1.98 ± 0.05 eV can be described by two consistent time constants, namely a first bleaching lifetime of 5 to 10 s, and a second bleaching lifetime in the range of 150 to 220 s. Only the former is environmentally sensitive and can be significantly mitigated by shielding O2, whereas the latter could be the result of carbon-assisted defect migration. Annular dark-field scanning transmission electron microscopy of photobleached hBN allows for visualizing vacancy defects and carbon substitution at single atom resolution, supporting the migration mechanism along with X-ray photoelectron spectroscopy. Thermal annealing at 850 °C of liquid exfoliated hBN eliminates both bleaching processes, leading to persistent photostability. These results represent a significant advance to potentially engineer hBN vacancy emitters with the photostability requisite for quantum applications.more » « less
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Abstract In alignment with the Materials Genome Initiative and as the product of a workshop sponsored by the US National Science Foundation, we define a vision for materials laboratories of the future in alloys, amorphous materials, and composite materials; chart a roadmap for realizing this vision; identify technical bottlenecks and barriers to access; and propose pathways to equitable and democratic access to integrated toolsets in a manner that addresses urgent societal needs, accelerates technological innovation, and enhances manufacturing competitiveness. Spanning three important materials classes, this article summarizes the areas of alignment and unifying themes, distinctive needs of different materials research communities, key science drivers that cannot be accomplished within the capabilities of current materials laboratories, and open questions that need further community input. Here, we provide a broader context for the workshop, synopsize the salient findings, outline a shared vision for democratizing access and accelerating materials discovery, highlight some case studies across the three different materials classes, and identify significant issues that need further discussion. Graphical abstractmore » « less
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