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At least 919 records · Page 51

Modular DNA strand-displacement controllers for directing material expansion

Abstract Soft materials that swell or change shape in response to external stimuli show extensive promise in regenerative medicine, targeted therapeutics, and soft robotics. Generally, a stimulus for shape change must interact directly with the material, limiting the types of stimuli that may be used and necessitating high stimulus concentrations. Here, we show how DNA strand-displacement controllers within hydrogels can mediate size change by interpreting, amplifying, and integrating stimuli and releasing signals that direct the response. These controllers tune the time scale and degree of DNA-crosslinked hydrogel swelling and can actuate dramatic material size change in response to <100 nM of a specific biomolecular input. Controllers can also direct swelling in response to small molecules or perform logic. The integration of these stimuli-responsive materials with biomolecular circuits is a major step towards autonomous soft robotic systems in which sensing and actuation are implemented by biomolecular reaction networks.

59 BASIC BIOLOGICAL SCIENCES↗

Single- and multi-component chiral supraparticles as modular enantioselective catalysts

Nanoscale biological assemblies exemplified by exosomes, endosomes and capsids, play crucial roles in all living systems. Supraparticles (SP) from inorganic nanoparticles (NPs) replicate structural characteristics of these bioassemblies, but it is unknown whether they can mimic their biochemical functions. Here, we show that chiral ZnS NPs self-assemble into 70–100 nm SPs that display sub-nanoscale porosity associated with interstitial spaces between constituent NPs. Similarly to photosynthetic bacterial organelles, these SPs can serve as photocatalysts, enantioselectively converting L- or D-tyrosine (Tyr) into dityrosine (diTyr). Experimental data and molecular dynamic simulations indicate that the chiral bias of the photocatalytic reaction is associated with the chiral environment of interstitial spaces and preferential partitioning of enantiomers into SPs, which can be further enhanced by co-assembling ZnS with Au NPs. Besides replicating a specific function of biological nanoassemblies, these findings establish a path to enantioselective oxidative coupling of phenols for biomedical and other needs.

Science & Technology - Other Topics↗

Toward a modular multi-material nanoparticle synthesis and assembly strategy via bionanocombinatorics: bifunctional peptides for linking Au and Ag nanomaterials

Materials-binding peptides represent a unique avenue towards controlling the shape and size of nanoparticles (NPs) grown under aqueous conditions. Here, employing a bionanocombinatorics approach, two such materials-binding peptides were linked at either end of a photoswitchable spacer, forming a multi-domain materials-binding molecule to control the in situ synthesis and organization of Ag and Au NPs under ambient conditions. These multi-domain molecules retained the peptides’ ability to nucleate, grow, and stabilize Ag and Au NPs in aqueous media. Disordered co-assemblies of the two nanomaterials were observed by TEM imaging of dried samples after sequential growth of the two metals, and showed a clustering behavior that was not observed without both metals and the linker molecules. While TEM evidence indicated the formation of AuNP/AgNP assemblies upon drying, SAXS analysis indicated that no extended assemblies existed in solution, suggesting that sample drying plays an important role in facilitating NP clustering. Molecular simulations and experimental data revealed tunable materials-binding based upon the isomerization state of the photoswitchable unit and metal employed. This work is a first step in generating externally actuated biomolecules with specific material-binding properties that could be used as the building blocks to achieve multi-material switchable NP assemblies.

36 MATERIALS SCIENCE↗

Synthesis, modular composition, and electrochemical properties of lamellar iron sulfides

Transition metal chalcogenides with layered structures are promising materials for energy storage, catalysis, and electronics, among other areas. We have identified a new layered phase of iron sulfide containing interlayer solvated cations. We present an optimized synthesis for the Li + -containing material from an Fe(III) xanthate complex. Structure and composition data indicate the material consists of poorly-ordered iron sulfide layers separated by solvated cations. The lamellar spacing in these materials can be tuned by changing the identity of the cation. Furthermore, the lamellar spacing can also be reversibly tuned by the degree of solvation of the material. The material is electrically conductive and can serve as a pseudocapacitor with comparable performance to commercial materials such as MnO 2 . Finally, these materials also show promise as lithium or sodium ion battery cathodes with good capacity and reversibility.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Towards a modular architecture for science factories

Advances in robotic automation, high-performance computing, and artificial intelligence encourage us to propose large, general-purpose science factories with the scale needed to tackle large discovery problems and to support thousands of scientists.

97 MATHEMATICS AND COMPUTING↗

Atomate2: modular workflows for materials science

High-throughput density functional theory (DFT) calculations have become a vital element of computational materials science, enabling materials screening, property database generation, and training of “universal” machine learning models. While several software frameworks have emerged to support these computational efforts, new developments such as machine learned force fields have increased demands for more flexible and programmable workflow solutions. This manuscript introduces atomate2, a comprehensive evolution of our original atomate framework, designed to address existing limitations in computational materials research infrastructure. Key features include the support for multiple electronic structure packages and interoperability between them, along with generalizable workflows that can be written in an abstract form irrespective of the DFT package or machine learning force field used within them. Our hope is that atomate2's improved usability and extensibility can reduce technical barriers for high-throughput research workflows and facilitate the rapid adoption of emerging methods in computational material science.

97 MATHEMATICS AND COMPUTING↗

Non-modular lattices generated by the causal structure

A lattice structure approach is used for investigation of the causal structure of space-time. Two lattices are considered: the first one generated by the chronological relation based on a time-like curve, the second one generated by the causal relation based on a causal path.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Effects of a modular two-step ozone-water and annealing process on silicon carbide graphene

By combining ozone and water, the effect of exposing epitaxial graphene on silicon carbide to an aggressive wet-chemical process has been evaluated after high temperature annealing in ultra high vacuum. The decomposition of ozone in water produces a number of oxidizing species, however, despite long exposure times to the aqueous-ozone environment, no graphene oxide was observed after the two-step process. The systems were comprehensively characterized before and after processing using Raman spectroscopy, core level photoemission spectroscopy, and angle resolved photoemission spectroscopy together with low energy electron diffraction, low energy electron microscopy, and atomic force microscopy. In spite of the chemical potential of the aqueous-ozone reaction environment, the graphene domains were largely unaffected raising the prospect of employing such simple chemical and annealing protocols to clean or prepare epitaxial graphene surfaces.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Maze solving automatons for self-healing of open interconnects: Modular add-on for circuit boards

We present the circuit board integration of a self-healing mechanism to repair open faults. The electric field driven mechanism physically restores fractured interconnects in electronic circuits and has the ability to solve mazes. The repair is performed by conductive particles dispersed in an insulating fluid. We demonstrate the integration of the healing module onto printed circuit boards and the ability of maze solving. We model and perform experiments on the influence of the geometry of conductive particles as well as the terminal impedances of the route on the healing efficiency. The typical heal rate is 10 μm/s with healed route having mean resistance of 8 kΩ across a 200 micron gap and depending on the materials and concentrations used.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Modular apparatus for electrostatic actuation of common atomic force microscope cantilevers

Piezoelectric actuation of atomic force microscope (AFM) cantilevers often suffers from spurious mechanical resonances in the loop between the signal driving the cantilever and the actual tip motion. These spurious resonances can reduce the accuracy of AFM measurements and in some cases completely obscure the cantilever response. To address these limitations, we developed a specialized AFM cantilever holder for electrostatic actuation of AFM cantilevers. The holder contains electrical contacts for the AFM cantilever chip, as well as an electrode (or electrodes) that may be precisely positioned with respect to the back of the cantilever. By controlling the voltages on the AFM cantilever and the actuation electrode(s), an electrostatic force is applied directly to the cantilever, providing a near-ideal transfer function from drive signal to tip motion. We demonstrate both static and dynamic actuations, achieved through the application of direct current and alternating current voltage schemes, respectively. As an example application, we explore contact resonance atomic force microscopy, which is a technique for measuring the mechanical properties of surfaces on the sub-micron length scale. Using multiple electrodes, we also show that the torsional resonances of the AFM cantilever may be excited electrostatically, opening the door for advanced dynamic lateral force measurements with improved accuracy and precision.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗