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Bustillo, Karen C

Publications and source records attributed to Bustillo, Karen C.

Memsensing by surface ion migration within Debye length

Integration between electronics and biology is often facilitated by iontronics, where ion migration in aqueous media governs sensing and memory. However, the Debye screening effect limits electric fields to the Debye length, the distance over which mobile ions screen electrostatic interactions, necessitating external voltages that constrain the operation speed and device design. Here we report a high-speed in-memory sensor based on vanadium dioxide (VO2) that operates without an external voltage by leveraging built-in electric fields within the Debye length. When VO2 contacts a low-work-function metal (for example, indium) in a salt solution, electrochemical reactions generate indium ions that migrate into the VO2 surface under the native electric field, inducing a surface insulator-to-metal phase transition of VO2. The VO2 conductance increase rate reflects the salt concentration, enabling in-memory sensing, or memsensing of the solution. The memsensor mimics Caenorhabditis elegans chemosensory plasticity to guide a miniature boat for adaptive chemotaxis, illustrating low-power aquatic neurorobotics with fewer memory units.

Guo, Ruihan

Multi-angle Precession Electron Diffraction (MAPED): A Versatile Approach to 4D-STEM Precession

Precession of a converged beam during acquisition of a 4D-STEM dataset improves strain, orientation, and phase mapping accuracy by averaging over continuous angles of illumination. Precession experiments usually rely on integrated systems, where automatic alignments lead to fast, high-quality results. The dependence of these experiments on specific hardware and software is evident even when switching to nonintegrated detectors on a precession tool, as experimental set-up becomes challenging and time-consuming. Here, we introduce multi-angle precession electron diffraction (MAPED): a method to perform electron diffraction by collecting sequential 4D-STEM scans at different incident beam tilts. The multiple diffraction datasets are averaged together postacquisition, resulting in a single dataset that minimizes the impact of the curvature and orientation of the Ewald sphere relative to the crystal under study. Our results demonstrate that even four additional tilts improved measurement of material properties, namely strain and orientation, as compared to single-tilt 4D-STEM experiments. We show the versatility and flexibility of our MAPED approach with data collected on a number of microscopes with different hardware configurations and a variety of detectors.

4D-STEM

Reuniting crystallography with real space: Ab initio structure elucidation with 4D-STEM

Structure elucidation via single-crystal methods has historically lacked experimental access to real-space information, instead relying exclusively on diffraction-space measurements of Bragg reflections. Here we exploit the dual-space imaging power of 4D scanning transmission electron microscopy to meaningfully integrate real-space information into the crystallographic workflow. We show that virtual apertures assembled by segmentation of high-angle annular dark-field images enable i) pixel-by-pixel separation of coherent Bragg signal from clusters of closely spaced nanocrystals and ii) selective extraction of integrated intensities from thinner subregions of individual specimens, facilitating retroactive tuning of multiple scattering artifacts. This strategy empowers us to simply pick and choose whichever nanoscale regions of interest generate the highest-quality diffraction patterns, allowing us to solve several independent structures of the metal-organic framework UiO-66 from specimens whose agglomerated morphology proved intractable for conventional microcrystal electron diffraction. Our method is compatible with both rotational and serial approaches to data processing, ultimately divulging the first scanning nanobeam electron diffraction structures determined by direct methods at subangstrom resolution.

Saha, Ambarneil

Local Interface Effects Modulate Global Charge Order and Optical Properties of 1T–TaS2/1H–WSe2 Heterostructures

1T-TaS2 is a layered charge density wave (CDW) crystal exhibiting sharp phase transitions and associated resistance changes. These resistance steps could be exploited for information storage, underscoring the importance of controlling and tuning the CDW states. Given the importance of out-of-plane interactions in 1T-TaS2, modulating interlayer interactions by heterostructuring is a promising method for tailoring CDW phase transitions. In this work, we investigate the optical and electronic properties of heterostructures comprising 1T-TaS2 and monolayer 1H-WSe2. By systematically varying the thickness of 1T-TaS2 and its azimuthal alignment with 1H-WSe2, we find that intrinsic moiré strain and interfacial charge transfer introduce CDW disorder in 1T-TaS2 and modify the CDW ordering temperature. Furthermore, our studies reveal that the interlayer alignment impacts the exciton dynamics in 1H-WSe2, indicating that heterostructuring can concurrently tailor the electronic phases in 1T-TaS2 and the optical properties of 1H-WSe2. This work presents a promising approach for engineering the optoelectronic behavior of heterostructures that integrate CDW materials and semiconductors.

charge density wave

Neutral but Impactful: Gallium Cluster-Induced Nanopores from Beam-Blanked Gallium Ion Sources

Neutral atoms originating from liquid metal ion sources are an often-overlooked source of contamination and damage in focused ion beam microscopy. Beyond ions and single atoms, these sources also generate atom clusters. While most studies have investigated charged clusters, here we demonstrate that neutral clusters are also formed. These neutral clusters bypass the electrostatic beam blanking system, allowing them to impinge on samples even when the ion beam is blanked. We investigate this phenomenon using thin (≤20 nm) freestanding membranes of hexagonal boron nitride, silicon, and silicon nitride as targets. Randomly dispersed nanopores that form upon neutral cluster exposure are revealed. The average nanopore diameter is ∼2 nm with a narrow size distribution, suggesting that the atom clusters have a preferred size. Various electron microscopy techniques are used to characterize the nanopores, including high-resolution transmission electron microscopy, multislice ptychography, and electron energy-loss spectroscopy. Finally, we show how electron irradiation in the transmission electron microscope can be used to both remove any amorphous material that may clog the pores and to controllably grow the pores to specific sizes. Tunable nanopores such as these are interesting for nanofluidic applications requiring size-selective membranes.

Byrne, Dana O

Modulating the Electronic Transport of 2D Sb2Te3 Nanoplates by Coinage Metal Intercalation

Thermoelectric materials are particularly relevant to the current energy infrastructure and demands of the 21st century, converting waste heat into usable electricity. The solution intercalation of zerovalent copper into Sb2Te3 nanoplates, a well-established thermoelectric material, is reported. The copper intercalant is homogeneously distributed throughout the nanoplates, confirmed by scanning transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy. The copper composition was shown to be 6 at. % by X-ray photoelectron spectroscopy. Copper ordering within the van der Waals gaps of the nanoplates is confirmed by selected area electron diffraction. Fabrication and thermoelectric property measurements of single-crystal Sb2Te3 and Cu-Sb2Te3 nanoplate devices show effective modulation of electrical conductivity and Seebeck coefficient with Cu intercalation. X-ray photoelectron spectroscopic studies in the valence-band region reveal additional electronic states from copper that appear near the Fermi energy, postulated to act as electron acceptors, leading to modulation of the electronic transport properties.

2D nanoplates