Selected area deposition of high purity gold films onto nanoscale 3D architectures is highly desirable as gold is conductive, inert, plasmonically active, and can be functionalized with thiol chemistries, which are useful in many biological applications. Here, we show that high-purity gold coatings can be selectively grown with the Me2Au (acac) precursor onto nanoscale 3D architectures via a pulsed laser pyrolytic chemical vapor deposition process. The selected area of deposition is achieved due to the high thermal resistance of the nanoscale geometries. Focused electron beam induced deposits (FEBID) and carbon nanofibers are functionalized with gold coatings, and we demonstrate the effects that laser irradiance, pulse width, and precursor pressure have on the growth rate. Furthermore, we demonstrate selected area deposition with a feature-targeting resolutions of ~100 and 5 µm, using diode lasers coupled to a multimode (915 nm) and single mode (785 nm) fiber optic, respectively. The experimental results are rationalized via finite element thermal modeling.
12 February 2024 in ACS Applied Materials & Interfaces
High-throughput synthesis and characterization of novel ceramic materials with improved thermomechanical properties and phase stability are needed to accelerate the discovery of next-generation thermal barrier materials. A combinatorial thin film material library of (GdDyHoEr)2Zr2O7 were created via combinatorial magnetron reactive sputtering with rare-earth/zirconium alloy targets. Structural, chemical, and thermal property characterization mapping across the four component composition space was performed and correlated with thermal transport measurements. X-ray diffraction confirms the formation of a single-phase defect fluorite structure, while energy-dispersive X-ray spectroscopy verifies a rare-earth-to-zirconium ratio of 1:1 across the library. X-ray absorption near edge structure and extended X-ray absorption fine structure measurements reveal minimal variation in cation valence states, local coordination environments, and nearest-neighbor bond distances, consistent with the EXAFS confirm the defect fluorite structure and trends in the associated ionic radii. Steady state thermoreflectance mapping identifies a pronounced minimum in thermal conductivity within the Dy/Gd-rich quadrant. This minimum does not coincide with either the equiatomic composition or the region predicted to exhibit maximum cation size disorder. Instead, it corresponds to the largest experimentally observed lattice parameter, despite deviating from Vegard-like chemical averaging, and is independent of grain size and whole-pattern microstrain. These observations suggest that the way the fluorite lattice accommodates compositional complexity, rather than cation size disorder alone, provides a more informative descriptor of thermal transport. Overall, this work establishes a high-throughput workflow for combinatorial thin-film synthesis and multimodal characterization, enabling the rapid identification of previously inaccessible structure-property relationships in compositionally complex ceramics.
Magnetic materials that combine strong spin-orbit coupling with ferromagnetism enable interconversion between charge and spin currents as well as stabilization of exotic spin textures, properties that are critical for advancing next-generation spintronic technologies. The metallic delafossite ${\mathrm{PdCoO}}_{2}$ is a highly conductive, nonmagnetic oxide that resides near a magnetic instability, making it a unique and promising monolithic platform for spin phenomena. Here, we investigate how helium implantation drives ${\mathrm{PdCoO}}_{2}$ into a magnetic state. Through depth-resolved low-energy muon spin relaxation (LE-\ensuremath{\mu}SR) measurements, ion implantation simulations, and first-principles calculations, the defects responsible for the emergent magnetism are identified. While oxygen Frenkel pairs, palladium Frenkel pairs, and interstitial helium contribute weakly, cobalt Frenkel pairs play the dominant role in generating magnetism. In addition, postimplantation annealing reveals distinct thermal windows for defect recombination, confirming the elemental specificity of cation-related defects. These findings establish defect engineering via ion implantation as a powerful route to controllably induce magnetism in ${\mathrm{PdCoO}}_{2}$. The combination of strong spin-orbit coupling, selectively tunable magnetism, and ultrahigh conductivity positions helium-implanted ${\mathrm{PdCoO}}_{2}$ as a unique platform for monolithic spintronic device integration, with implications for low-power magnetic memory and unconventional logic applications.
Large electron microscopy datasets require extensive annotation and review before they can be converted into reliable measurements. ACORN is an open-source, locally executable application that offers image preparation, reviewed annotation, task-specific model training, batch inference, calibrated measurement, and statistical analysis in a single format. Users can create and correct annotations manually or with promptable segmentation and use the reviewed annotations to train models directly within ACORN. Its Cryo-EM Lab Utility (CLU) assistant also allows users to request any analysis or training operations in plain language. To show its use cases, we evaluated ACORN using low-dose cryogenic TEM images of polymeric nanoparticles and SEM images of bacterial spores. YOLO models trained in ACORN produced validation F1 scores of \(0.906\pm0.013\) and \(0.624\pm0.016\), respectively. Controlled simulations built in ACORN provided 25,983 exact object annotations for further model development and a controlled evaluation of software performance. On held-out simulation images, equivalent-circular-diameter mean absolute error was 3.60~nm (10.1\%) for TEM particles and 31.48~nm (3.7\%) for SEM spores among matched detections. The software logs every interaction, training step, and annotation in a sample history for provenance tracking. ACORN provides an environment where annotations, image calibration, model checkpoints, object measurements, and statistical records are easily accessible and traceable. This software provides a traceable path from electron microscopy images to quantitative results in multiple user-friendly formats.