Publications by authors named "Ashby P"

We study the effect of strain on the magnetic properties and magnetization configurations in nanogranular FeGe1-xfilms (x=0.53±0.05) with and without B20 FeGe nanocrystals surrounded by an amorphous structure.

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Magnetic skyrmions have so far been treated as two-dimensional spin structures characterized by a topological winding number. However, in real systems with the finite thickness of the device material being larger than the magnetic exchange length, the skyrmion spin texture extends into the third dimension and cannot be assumed as homogeneous. Using soft x-ray laminography, we reconstruct with about 20-nanometer spatial (voxel) size the full three-dimensional spin texture of a skyrmion in an 800-nanometer-diameter and 95-nanometer-thin disk patterned into a 30× [iridium/cobalt/platinum] multilayered film.

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Covalent chemistry is a versatile approach for expanding the ligandability of the human proteome. Activity-based protein profiling (ABPP) can infer the specific residues modified by electrophilic compounds through competition with broadly reactive probes. However, the extent to which such residue-directed platforms fully assess the protein targets of electrophilic compounds in cells remains unclear.

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We study the temperature dependent elastic properties of BaSrTiO freestanding membranes across the ferroelectric-to-paraelectric phase transition using an atomic force microscope. The bending rigidity of thin membranes can be stiffer compared to stretching due to strain gradient elasticity (SGE). We measure the Young's modulus of freestanding BaSrTiO drumheads in bending and stretching dominated deformation regimes on a variable temperature platform, finding a peak in the difference between the two Young's moduli obtained at the phase transition.

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The conformational dynamics of nucleosome arrays generate a diverse spectrum of microscopic states, posing challenges to their structural determination. Leveraging cryogenic electron tomography (cryo-ET), we determine the three-dimensional (3D) structures of individual mononucleosomes and arrays comprising di-, tri-, and tetranucleosomes. By slowing the rate of condensation through a reduction in ionic strength, we probe the intra-array structural transitions that precede inter-array interactions and liquid droplet formation.

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Assemblies of nanoparticles at liquid interfaces hold promise as dynamic "active" systems when there are convenient methods to drive the system out of equilibrium via crowding. To this end, we show that oversaturated assemblies of charged nanoparticles can be realized and held in that state with an external electric field. Upon removal of the field, strong interparticle repulsive forces cause a high in-plane electrostatic pressure that is released in an explosive emulsification.

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The ability to control and manipulate semiconductor/bio interfaces is essential to enable biological nanofabrication pathways and bioelectronic devices. Traditional surface functionalization methods, such as self-assembled monolayers (SAMs), provide limited customization for these interfaces. Polymer brushes offer a wider range of chemistries, but choices that maintain compatibility with both lithographic patterning and biological systems are scarce.

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An active droplet system, programmed to repeatedly move autonomously at a specific velocity in a well-defined direction, is demonstrated. Coulombic energy is stored in oversaturated interfacial assemblies of charged nanoparticle-surfactants by an applied DC electric field and can be released on demand. Spontaneous emulsification is suppressed by an increase in the stiffness of the oversaturated assemblies.

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Silver cations can mediate base pairing of guanine (G) DNA oligomers, yielding linear parallel G-Ag-G duplexes with enhanced stabilities compared to those of canonical DNA duplexes. To enable their use in programmable DNA nanotechnologies, it is critical to understand solution-state formation and the nanomechanical stiffness of G-Ag-G duplexes. Using temperature-controlled circular dichroism (CD) spectroscopy, we find that heating mixtures of G oligomers and silver salt above 50 °C fully destabilizes G-quadruplex structures and converts oligomers to G-Ag-G duplexes.

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Invading microbes face a myriad of cidal mechanisms of phagocytes that inflict physical damage to microbial structures. How intracellular bacterial pathogens adapt to these stresses is not fully understood. Here, we report the discovery of a virulence mechanism by which changes to the mechanical stiffness of the mycobacterial cell surface confer refraction to killing during infection.

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The in-plane packing of gold (Au), polystyrene (PS), and silica (SiO) spherical nanoparticle (NP) mixtures at a water-oil interface is investigated in situ by UV-vis reflection spectroscopy. All NPs are functionalized with carboxylic acid such that they strongly interact with amine-functionalized ligands dissolved in an immiscible oil phase at the fluid interface. This interaction markedly increases the binding energy of these nanoparticle surfactants (NPSs).

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Metal-organic decomposition epitaxy is an economical wet-chemical approach suitable to synthesize high-quality low-spin-damping films for resonator and oscillator applications. This work reports the temperature dependence of ferromagnetic resonances and associated structural and magnetic quantities of yttrium iron garnet nanofilms that coincide with single-crystal values. Despite imperfections originating from wet-chemical deposition and spin coating, the quality factor for out-of-plane and in-plane resonances approaches 600 and 1000, respectively, at room temperature and 40 GHz.

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Copper compounds have been extensively investigated for diverse applications. However, studies of cuprous hydroxide (CuOH) have been scarce due to structural metastability. Herein, a facile, wet-chemistry procedure is reported for the preparation of stable CuOH nanostructures via deliberate functionalization with select organic ligands, such as acetylene and mercapto derivatives.

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Rigid, solid-state components represent the current paradigm for electronic systems, but they lack post-production reconfigurability and pose ever-increasing challenges to efficient end-of-life recycling. Liquid electronics may overcome these limitations by offering flexible in-the-field redesign and separation at end-of-life via simple liquid phase chemistries. Up to now, preliminary work on liquid electronics has focused on liquid metal components, but these devices still require an encapsulating polymer and typically use alloys of rare elements like indium.

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Engineered living materials (ELMs) embed living cells in a biopolymer matrix to create materials with tailored functions. While bottom-up assembly of macroscopic ELMs with a de novo matrix would offer the greatest control over material properties, we lack the ability to genetically encode a protein matrix that leads to collective self-organization. Here we report growth of ELMs from Caulobacter crescentus cells that display and secrete a self-interacting protein.

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The nanoscale structure and dynamics of proteins on surfaces has been extensively studied using various imaging techniques, such as transmission electron microscopy and atomic force microscopy (AFM) in liquid environments. These powerful imaging techniques, however, can potentially damage or perturb delicate biological material and do not provide chemical information, which prevents a fundamental understanding of the dynamic processes underlying their evolution under physiological conditions. Here, we use a platform developed in our laboratory that enables acquisition of infrared (IR) spectroscopy and AFM images of biological material in physiological liquids with nanometer resolution in a cell closed by atomically thin graphene membranes transparent to IR photons.

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Article Synopsis
  • * The intersection of synthetic biology and biomaterials holds great potential for addressing major challenges in health, biotechnology, and sustainability, yet both fields have largely developed independently.
  • * This review discusses recent breakthroughs in both areas and proposes a collaborative approach to advance the creation of complex biomaterials, including bioinspired and responsive "living" materials.
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To better exploit all-liquid 3D architectures, it is essential to understand dynamic processes that occur during printing one liquid in a second immiscible liquid. Here, the interfacial assembly and transition of 5,10,15,20-tetrakis(4-sulfonatophenyl) porphyrin (H TPPS) over time provides an opportunity to monitor the interfacial behavior of nanoparticle surfactants (NPSs) during all-liquid printing. The formation of J-aggregates of H TPPS at the interface and the interfacial conversion of the J-aggregates of H TPPS to H-aggregates of H TPPS is demonstrated by interfacial rheology and in situ atomic force microscopy.

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Rare-earth elements, which include the lanthanide series, are key components of many clean energy technologies, including wind turbines and photovoltaics. Because most of these 4f metals are at high risk of supply chain disruption, the development of new recovery technologies is necessary to avoid future shortages, which may impact renewable energy production. This paper reports the synthesis of a non-natural biogenic material as a potential platform for bioinspired lanthanide extraction.

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Water-walking insects can harness capillary forces by changing their body posture to climb or descend the meniscus between the surface of water and a solid object. Controlling surface tension in this manner is necessary for predation, escape and survival. Inspired by this behaviour, we demonstrate autonomous, aqueous-based synthetic systems that overcome the meniscus barrier and shuttle cargo subsurface to and from a landing site and a targeted drop-off site.

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We present a study of the effect of gold nanoparticles (Au NPs) on TiO on charge generation and trapping during illumination with photons of energy larger than the substrate band gap. We used a novel characterization technique, photoassisted Kelvin probe force microscopy, to study the process at the single Au NP level. We found that the photoinduced electron transfer from TiO to the Au NP increases logarithmically with light intensity due to the combined contribution of electron-hole pair generation in the space charge region in the TiO-air interface and in the metal-semiconductor junction.

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Fine control over the mechanical properties of thin sheets underpins transcytosis, cell shape, and morphogenesis. Applying these principles to artificial, liquid-based systems has led to reconfigurable materials for soft robotics, actuation, and chemical synthesis. However, progress is limited by a lack of synthetic two-dimensional membranes that exhibit tunable mechanical properties over a comparable range to that seen in nature.

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The bacterial extracellular matrix forms autonomously, giving rise to complex material properties and multicellular behaviors. Synthetic matrix analogues can replicate these functions but require exogenously added material or have limited programmability. Here, we design a two-strain bacterial system that self-synthesizes and structures a synthetic extracellular matrix of proteins.

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Microemulsions, mixtures of oil, water, and surfactant, are thermodynamically stable. Unlike conventional emulsions, microemulsions form spontaneously, have a monodisperse droplet size that can be controlled by adjusting the surfactant concentration, and do not degrade with time. To make microemulsions, a judicious choice of surfactant molecules must be made, which significantly limits their potential use.

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Two-dimensional heterostructures composed of layers with slightly different lattice vectors exhibit new periodic structure known as moiré lattices, which, in turn, can support novel correlated and topological phenomena. Moreover, moiré superstructures can emerge from multiple misaligned moiré lattices or inhomogeneous strain distributions, offering additional degrees of freedom in tailoring electronic structure. High-resolution imaging of the moiré lattices and superstructures is critical for understanding the emerging physics.

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