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Brandon Blue

Publications and source records attributed to Brandon Blue.

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Towards Atom-by-Atom Fabrication: Mechanosynthetic donation and abstraction

Enabled by inverted-mode scanning tunneling microscopy (IM-STM) and the use of functionalized molecular tools, we demonstrate positionally-controlled mechanosynthetic addition (donation) of carbon and subtraction (abstraction) of silicon atoms on a model build site: atomically clean and crystalline Si(100). The resulting structures represent the first demonstrations of an emerging ability to manipulate radical chemistry with positional control of specific atoms and moieties in 3D. Furthermore, by comparing the behavior of molecular tools designed for atomic donation versus abstraction, we highlight general principles governing molecular tool design for selective and reliable mechanosynthetic functionality.

cond-mat.mtrl-sci

Atomically precise mechanosynthesis of carbon structures on hydrogenated Si(100) by inverted-mode STM

The ability to build atomically precise structures on surfaces with complete control over both atomic placement and chemical bonding remains a central challenge in nanoscale fabrication. Here, we demonstrate simultaneous spatial and chemical control over the mechanosynthetic fabrication of carbon structures. Using inverted-mode STM, C$_2$ units are donated from surface-deposited molecules to pre-patterned reactive sites on a hydrogen-passivated Si(100) surface. We demonstrate single-site C$_2$ donation, spatially patterned multi-site C$_2$ donation, and the stepwise assembly of polyyne structures through successive C-C bond formation. Together, these results establish controlled mechanosynthetic donation as a foundational capability for programmable atomically precise fabrication.

cond-mat.mtrl-sci

Inverted-Mode Scanning Tunneling Microscopy for Atomically Precise Fabrication

Scanning Tunneling Microscopy (STM) enables fabrication of atomically precise structures with unique properties and growing technological potential. However, reproducible manipulation of covalently bonded atoms requires control over the atomic configuration of both sample and probe - a longstanding challenge in STM. Here, we introduce inverted-mode STM, an approach that enables mechanically controlled chemical reactions for atomically precise fabrication. Tailored molecules on a Si(100) surface image the probe apex, and the usual challenge of understanding the probe structure is effectively solved. The molecules can also react with the probe, with the two sides of the tunnel junction acting as reagents positioned with sub-angstrom precision. This allows abstraction or donation of atoms from or to the probe apex. We demonstrate this by using a novel alkynyl-terminated molecule to reproducibly abstract hydrogen atoms from the probe. The approach is expected to extend to other elements and moieties, opening a new avenue for scalable atomically precise fabrication.

cond-mat.mes-hall

Molecular Tools for Non-Planar Surface Chemistry

Scanning probe microscopy (SPM) investigations of on-surface chemistry on passivated silicon have only shown in-plane chemical reactions, and studies on bare silicon are limited in facilitating additional reactions post-molecular-attachment. Here, we enable subsequent reactions on Si(100) through selectively adsorbing 3D, silicon-specific "molecular tools". Following an activation step, the molecules present an out-of-plane radical that can function both to donate or accept molecular fragments, thereby enabling applications across multiple scales, e.g., macroscale customizable silicon-carbon coatings or nanoscale tip-mediated mechanosynthesis. Creation of many such molecular tools is enabled by broad molecular design criteria that facilitate reproducibility, surface specificity, and experimental verifiability. These criteria are demonstrated using a model molecular tool tetrakis(iodomethyl)germane ($Ge(CH_{2}I)_{4}$; TIMe-Ge), with experimental validation by SPM and X-ray photoelectron spectroscopy (XPS), and theoretical support by density functional theory (DFT) investigations. With this framework, a broad and diverse range of new molecular engineering capabilities are enabled on silicon.

cond-mat.mtrl-sci

Hydrated Cable Bacteria Exhibit Protonic Conductivity Over Long Distances

This study presents the direct measurement of proton transport along filamentous Desulfobulbaceae, or cable bacteria. Cable bacteria are filamentous multicellular microorganisms that have garnered much interest due to their ability to serve as electrical conduits, transferring electrons over several millimeters. Our results indicate that cable bacteria can also function as protonic conduits because they contain proton wires that transport protons at distances greater than 100 um. We find that protonic conductivity ({\sigma}P) along cable bacteria varies between samples and is measured as high as 114 +/- 28 uS cm^-1 at 25-degrees C and 70-percent relative humidity (RH). For cable bacteria, the protonic conductance (GP) and {\sigma}P are dependent upon the RH, increasing by as much as 26-fold between 60-percent and 80-percent RH. This observation implies that proton transport occurs via the Grotthuss mechanism along water associated with cable bacteria, forming proton wires. In order to determine {\sigma}P and GP along cable bacteria, we implemented a protocol using a modified transfer-printing technique to deposit either palladium interdigitated protodes (IDP), palladium transfer length method (TLM) protodes, or gold interdigitated electrodes(IDE) on top of cable bacteria. Due to the relatively mild nature of the transfer-printing technique, this method should be applicable to a broad array of biological samples and curved materials. The observation of protonic conductivity in cable bacteria presents possibilities for investigating the importance of long-distance proton transport in microbial ecosystems and to potentially build biotic or biomimetic scaffolds to interface with materials via proton-mediated gateways or channels.

physics.bio-ph

Enabling remote quantum emission in 2D semiconductors via porous metallic networks

The interaction between two-dimensional crystals (2DCs) and metals is ubiquitous in 2D material research. Here we report how 2DC overlayers influence the recrystallization of relatively thick metal films and the subsequent synergetic benefits this provides for coupling surface plasmon-polaritons (SPPs) to photon emission in 2D semiconductors. We show that annealing 2DC/Au films on SiO2 results in a 'reverse epitaxial' process where initially nanocrystalline Au films become highly textured and in close crystallographic registry to the 2D crystal overlayer. With continued annealing, the metal underlayer dewets to form an oriented pore enabled network (OPEN) film in which the 2DC overlayer remains suspended above or coats the inside of the metal pores. This OPEN film geometry supports SPPs launched by either direct laser excitation or by light emitted from the TMD semiconductor itself, where energy in-coupling and out-coupling occurs at the metal pore sites such that dielectric spacers between the metal and 2DC layer are unnecessary. At low temperatures a high density of single-photon emitters (SPEs) is present across an OPEN-WSe2 film, and we demonstrate non-local excitation of SPEs at a distance of 17 {\mu}m with minimal loss of photon purity. Our results suggest the OPEN film geometry is a versatile platform that could facilitate the use of layered materials in quantum optics systems.

cond-mat.mes-hall