Abstract The arrangement of DNA‐based nanostructures into extended higher order assemblies is an important step towards their utilization as functional molecular materials. We herein demonstrate that by electrostatically controlling the adhesion and mobility DNA origami structures on mica surfaces simple addition monovalent cations, large ordered 2D arrays tiles can be generated. lattices formed either close‐packing symmetric, non‐interacting structures, or utilizing blunt‐end stacking...

The hydrophobic effect, i.e., the poor solvation of nonpolar parts molecules, plays a key role in protein folding and more generally for molecular self-assembly aggregation aqueous media. perturbation water structure accounts many aspects hydrophobicity. However, to what extent dispersion interaction between entities themselves contributes has remained unclear. This is so because peptide interactions structural changes occur on all length scales make disentangling various contributions...

Membrane compartmentalization and growth are central aspects of living cells, thus encoded in every cell's genome. For the creation artificial cellular systems, genetic information production membrane building blocks will need to be coupled a similar manner. However, natural biochemical reaction networks notoriously difficult implement vitro. Here, we utilized amphiphilic elastin-like peptides (ELP) create self-assembled vesicular structures about 200 nm diameter. In order genetically encode...

The force-induced desorption of single peptide chains from mixed OH/CH3-terminated self-assembled monolayers is studied in closely matched molecular dynamics simulations and atomic force microscopy experiments with the goal to gain microscopic understanding transition between adsorption resistance as surface contact angle varied. In both experiments, surfaces become resistant against hydrophilic well hydrophobic peptides when their decreases below θ ≈ 50°–60°, thus confirming so-called Berg...

The spring constant of cantilever in atomic force microscopy (AFM) is often calibrated from thermal noise spectra. Essential for accurate implementation this “thermal method” an appropriate fitting function and procedure. Here, we survey the commonly used functions examine their applicability a range environments. We find that viscous liquid environments are extremely problematic due to frequency dependent nature damping coefficient. deviations true were sometimes more than 100% when...

The fabrication of defined polymer objects reduced dimensions such as polymer-coated nanoparticles (zero-dimensional (0D)), cylindrical brushes (1D), and membranes (2D), is currently the subject intense research. In particular, ultrathin with high aspect ratios are being discussed novel materials for miniaturized sensors because they would provide extraordinary sensitivity dynamic range when sufficient mechanical stability can be combined flexibility chemical functionality. Unlike current...

DNA-binding proteins are promising reagents for the sequence-specific modification of DNA-based nanostructures. Here, we investigate utility a series relaxase proteins-TrwC, TraI, and MobA-for nanofunctionalization. Relaxases involved in conjugative transfer plasmids between bacteria, bind to their DNA target sites via covalent phosphotyrosine linkage. We study binding relaxases two standard origami structures-rodlike six-helix bundles flat rectangular sheets. find highly orthogonal with...

Nanoscale plasmonic waveguides composed of metallic nanoparticles are capable guiding electromagnetic energy below the optical diffraction limit. Signal feed-in and readout typically require utilization electronic effects or near-field techniques, whereas for their fabrication mainly lithographic methods employed. Here we developed a switchable waveguide assembled from gold (AuNPs) on DNA origami structure that facilitates simple spectroscopic excitation readout. The is specifically excited...

Fast and efficient transport of molecular cargoes along tracks or on supramolecular platforms is an important prerequisite for the development future nanorobotic systems assembly lines. Here, we study diffusive DNA cargo strands bound to a origami structure via extended tether arm. For short distances (on order few nanometers), from start target site found be less than direct transfer without tether. scale platform itself, however, mediated by rigid arm occurs very fast robust, whereas more...

AFM-based single-molecule force spectroscopy has been used to study the effect of Hofmeister salts and protein hydrophobicity on adhesion recombinant spider silk proteins onto solid substrates. Therefore, a molecular probe consisting an AFM tip developed, which (i) is well-defined, small system that can be simulated by dynamics simulations, (ii) allows access whole soluble concentration range for ions, (iii) provides distribution desorption forces rather than just ensemble-averaged mean...

Compartmentalization and spatial organization of biochemical reactions are essential for the establishment complex metabolic pathways inside synthetic cells. Phospholipid fatty acid membranes most natural candidates this purpose, but also polymers have shown great potential as enclosures artificial cell mimics. Herein, we report on formation giant vesicles in a size range 1 μm-100 μm using amphiphilic elastin-like polypeptides. The peptide can accommodate cell-free gene expression reactions,...

In this paper we probe the influence of surface properties, pH and salt on adhesion recombinant spider silk proteins onto solid substrates with single molecule force spectroscopy. A engineered protein (monomeric C16 or dimeric (QAQ)8NR3) is covalently bound one end to an AFM tip, which assures long-time measurements for hours same protein. The tip brought into contact various at buffer conditions then retracted desorb We observe a linear dependence concentration three selected salts (NaCl,...

In nature, compartmentalized and spatially organized enzyme cascades are utilized to increase the efficiency of enzymatic reactions. From a technologically relevant perspective, synthetic systems have be optimized with emphasis on activity, productivity, scalability, ease use. But underlying principles parameters that lead an enhancement activity through spatial organization still under debate. Here, we report 10-fold GOx-HRP cascade for oxidation luminol, when enzymes colocalized...

Abstract Die großflächige Anordnung von DNA‐basierten Nanostrukturen in geordnete Überstrukturen ist ein wichtiger Schritt auf dem Weg zu deren Nutzung als funktionale molekulare Materialien. In dieser Arbeit zeigen wir, dass durch elektrostatische Kontrolle der Adhäsion und Mobilität DNA‐Origami‐Strukturen Glimmeroberflächen mittels einfacher Zugabe monovalenten Kationen große 2D‐Gitterstrukturen aus Origami‐Kacheln erzeugt werden können. Gitter können entweder dichtes Packen symmetrischer,...

Abstract Dynamic DNA nanodevices are designed to perform structure‐encoded motion actuated by a variety of different physicochemical stimuli. In this context, hybrid devices utilizing other components than have the potential considerably expand library functionalities. Here, reversible reconfiguration origami structure using stimulus sensitivity elastin‐like polypeptides is reported. To end, rectangular sheet made technique functionalized with these peptides and applying changes in salt...

The adhesion of polypeptides and proteins at interfaces is important for a wide variety systems--from the onto vessels during their production process over functional coatings to protein-membrane interactions in single cells. Herein, we apply an atomic-force-microscopy-based single-molecule method poly-D-tyrosine determine strength location interfaces. Surprisingly, support (solid, liquid or gas) hardly influences aqueous environment, while addition ethanol solvent cuts half. These findings...

Abstract Implant-associated infections are a challenging problem in surgery. Bacteria biofilms difficult to treat as they less susceptible antibiotics or antiseptics which require high drug concentrations at the site of infection. We present novel strategy concentrate antibiotic doses systemically target using newly developed antibiotic-functionalized nanoparticles directed by magnetic drug-targeting system. The important and effective gentamicin served antimicrobial substance was ionically...

Abstract The creation of self‐replicating cell‐mimicking systems – artificial cells is one the major goals bottom‐up synthetic biology. An essential aspect such realization membranous compartments which can grow and divide in synchrony with internal dynamics cells. Amphiphiles capable forming membranes may be either externally provided to feed growing compartments, or generated situ through chemical processes. In context autonomously systems, genetically encoded are particular interest....

We analyze the polymer filling mechanism in composites containing highly ordered and vertically aligned carbon nanotube (CNT) arrays. CNTs are obtained by a template assisted chemical vapor deposition (CVD) method. Different forms of arrays studied with one or two layers on top bottom surface array, freestanding CNTs. Investigation is done small-angle X-ray scattering (SAXS) combination electron microscopy (TEM SEM) atomic force microscopy. Tubes 40 μm length 40/90 nm diameter. The original...

Cell-free systems allow interference with gene expression processes without requiring elaborate genetic engineering procedures. This makes it ideally suited for rapid prototyping of synthetic biological parts. Inspired by nature's strategies the control via short antisense RNA molecules, we here investigated use small DNA (sDNA) translational inhibition in context cell-free protein expression. We designed sDNA molecules to be complementary ribosome binding site (RBS) and downstream coding...

Atomic force microscopy (AFM) based single polymer spectroscopy allows to detect the interaction (energy) between polymers and interfaces in aqueous environment. We use this method delineate effect of ions, pH, co-solutes temperature on adhesion biopolymers onto solid substrates.

Abstract DNA‐bindende Proteine erlauben die sequenzspezifische Modifikation von DNA‐basierten Nanostrukturen. Hier untersuchen wir Eignung Relaxaseproteinen – speziell TrwC, TraI und MobA für Nanofabrikation. Relaxasen sind Komponenten des bakteriellen Konjugationsmechanismus, bei dem Plasmide zwischen Bakterien ausgetauscht werden, wobei sie an DNA durch eine kovalente Phosphotyrosinbindung binden. Wir Anbindung der zwei prototypische DNA‐Origamistrukturen stabförmige Sechs‐Helix‐Bündel...

Can we scale down robots to small scales and realize them with self-organizing molecules? As biological cells already act a little like – they sense, compute, move, respond their environment the answer is probably “yes”. But wide range of interesting physical challenges have be tackled.

Compartmentalization of biochemical reactions is a central aspect synthetic cells. For this purpose, peptide-based reaction compartments serve as an attractive alternative to liposomes or fatty acid-based vesicles. Externally within the vesicles, peptides can be easily expressed and simplify synthesis membrane precursors. Provided here protocol for creation vesicles with diameters ~200 nm based on amphiphilic elastin-like polypeptides (ELP) utilizing dehydration-rehydration from glass beads....

Abstract The front cover artwork is provided by Marisa A. Goetzfried, Technical University of Munich. image illustrates dynamic peptide vesicles investigated in our group. background displays a fluorescence‐bright‐field overlay micrograph giant vesicles. Read the full text Concept article at 10.1002/syst.201900016 .