Search for: All records

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 abstract 

Short-range atomic order in semiconductor alloys is a relatively unexplored topic that may promote design of new materials with unexpected properties. Here, local atomic ordering is investigated in Ge–Sn alloys, a group-IV system that is attractive for its enhanced optoelectronic properties achievable via a direct gap for Sn concentrations exceeding ≈10 at. %. The substantial misfit strain imposed on Ge–Sn thin films during growth on bulk Si or Ge substrates can induce defect formation; however, misfit strain can be accommodated by growing Ge–Sn alloy films on Ge nanowires, which effectively act as elastically compliant substrates. In this work, Ge core/Ge 1−x Sn x ( x ≈  0.1) shell nanowires were characterized with extended x-ray absorption fine structure (EXAFS) to elucidate their local atomic environment. Simultaneous fitting of high-quality EXAFS data collected at both the Ge K-edge and the Sn K-edge reveals a large (≈ 40%) deficiency of Sn in the first coordination shell around a Sn atom relative to a random alloy, thereby providing the first direct experimental evidence of significant short-range order in this semiconductor alloy system. Comparison of path length data from the EXAFS measurements with density functional theory simulations provides alloy atomic structures consistent with this conclusion. 

Magnetic properties and interfacial phenomena of epitaxial perovskite oxides depend sensitively on parameters such as film thickness and strain state. In this work, epitaxial La 0.67 Sr 0.33 CoO 3 (LSCO)/La 0.67 Sr 0.33 MnO 3 (LSMO) bilayers were grown on NdGaO 3 (NGO) and LaAlO 3 (LAO) substrates with a fixed LSMO thickness of 6 nm, and LSCO thickness (t LSCO ) varying from 2 to 10 nm. Soft x-ray magnetic spectroscopy revealed that magnetically active Co 2+ ions that strongly coupled to the LSMO layer were observed below a critical t LSCO for bilayers grown on both substrates. On LAO substrates, this critical thickness was 2 nm, above which the formation of Co 2+ ions was quickly suppressed leaving only a soft LSCO layer with mixed valence Co 3+ /Co 4+ ions. The magnetic properties of both LSCO and LSMO layers displayed strong t LSCO dependence. This critical t LSCO increased to 4 nm on NGO substrates, and the magnetic properties of only the LSCO layer displayed t LSCO dependence. A non-magnetic layer characterized by Co 3+ ions and with a thickness below 2 nm exists at the LSCO/substrate interface for both substrates. The results contribute to the understanding of interfacial exchange spring behavior needed for applications in next generation spintronic and magnetic memory devices. 

Abstract Electrochemical two-electron water oxidation reaction (2e-WOR) has drawn significant attention as a promising process to achieve the continuous on-site production of hydrogen peroxide (H₂O₂). However, compared to the cathodic H₂O₂generation, the anodic 2e-WOR is more challenging to establish catalysts due to the severe oxidizing environment. In this study, we combine density functional theory (DFT) calculations with experiments to discover a stable and efficient perovskite catalyst for the anodic 2e-WOR. Our theoretical screening efforts identify LaAlO₃perovskite as a stable, active, and selective candidate for catalyzing 2e-WOR. Our experimental results verify that LaAlO₃achieves an overpotential of 510 mV at 10 mA cm⁻²in 4 M K₂CO₃/KHCO₃, lower than those of many reported metal oxide catalysts. In addition, LaAlO₃maintains a stable H₂O₂Faradaic efficiency with only a 3% decrease after 3 h at 2.7 V vs. RHE. This computation-experiment synergistic approach introduces another effective direction to discover promising catalysts for the harsh anodic 2e-WOR towards H₂O₂.