Showing 1–6 of 6 results for author: Dietz, H

Mono-exponential Current Attenuation with Distance across 16 nm Thick Bacteriorhodopsin Multilayers

Authors: Domenikos Chryssikos, Jerry A. Fereiro, Jonathan Rojas, Sudipta Bera, Defne Tüzün, Evanthia Kounoupioti, Rui N. Pereira, Christian Pfeiffer, Ali Khoshouei, Hendrik Dietz, Mordechai Sheves, David Cahen, Marc Tornow

Abstract: The remarkable ability of natural proteins to conduct electricity in the dry state over long distances remains largely inexplicable despite intensive research. In some cases, a (weakly) exponential length-attenuation, as in off-resonant tunneling transport, extends to thicknesses even beyond 10 nm. This report deals with such charge transport characteristics observed in self-assembled multilayers… ▽ More The remarkable ability of natural proteins to conduct electricity in the dry state over long distances remains largely inexplicable despite intensive research. In some cases, a (weakly) exponential length-attenuation, as in off-resonant tunneling transport, extends to thicknesses even beyond 10 nm. This report deals with such charge transport characteristics observed in self-assembled multilayers of the protein bacteriorhodopsin (bR). About 7.5 nm to 15.5 nm thick bR layers were prepared on conductive titanium nitride (TiN) substrates using aminohexylphosphonic acid and poly-diallyl-dimethylammonium electrostatic linkers. Using conical EGaIn top contacts, an intriguing, mono-exponential conductance attenuation as a function of the bR layer thickness with a small attenuation coefficient $β\approx 0.8 \space {\rm nm}^{-1}$ is measured at zero bias. Variable-temperature measurements using evaporated Ti/Au top contacts yield effective energy barriers of about 100 meV from fitting the data to tunneling, hopping, and carrier cascade transport models. The observed temperature-dependence is assigned to the protein-electrode interfaces. The transport length and temperature dependence of the current densities are consistent with tunneling through the protein-protein and protein-electrode interfaces, respectively. Importantly, our results call for new theoretical approaches to find the microscopic mechanism behind the remarkably efficient, long-range electron transport within bR. △ Less

Submitted 17 August, 2024; originally announced August 2024.

Journal ref: Adv. Funct. Mater. 2024, 2408110

Hierarchical assembly is more robust than egalitarian assembly in synthetic capsids

Authors: Wei-Shao Wei, Anthony Trubiano, Christian Sigl, Stefan Paquay, Hendrik Dietz, Michael F. Hagan, Seth Fraden

Abstract: Self-assembly of complex and functional materials remains a grand challenge in soft material science. Efficient assembly depends on a delicate balance between thermodynamic and kinetic effects, requiring fine-tuning affinities and concentrations of subunits. By contrast, we introduce an assembly paradigm that allows large error-tolerance in the subunit affinity and helps avoid kinetic traps. Our c… ▽ More Self-assembly of complex and functional materials remains a grand challenge in soft material science. Efficient assembly depends on a delicate balance between thermodynamic and kinetic effects, requiring fine-tuning affinities and concentrations of subunits. By contrast, we introduce an assembly paradigm that allows large error-tolerance in the subunit affinity and helps avoid kinetic traps. Our combined experimental and computational approach uses a model system of triangular subunits programmed to assemble into T=3 icosahedral capsids comprising 60 units. The experimental platform uses DNA origami to create monodisperse colloids whose 3D geometry is controlled to nanometer precision, with two distinct bonds whose affinities are controlled to kBT precision, quantified in situ by static light scattering. The computational model uses a coarse-grained representation of subunits, short-ranged potentials, and Langevin dynamics. Experimental observations and modeling reveal that when the bond affinities are unequal, two distinct hierarchical assembly pathways occur, in which the subunits first form dimers in one case, and pentamers in another. These hierarchical pathways produce complete capsids faster and are more robust against affinity variation than egalitarian pathways, in which all binding sites have equal strengths. This finding suggests that hierarchical assembly may be a general engineering principle for optimizing self-assembly of complex target structures. △ Less

Submitted 28 October, 2023; originally announced October 2023.

Journal ref: Proceedings of the National Academy of Sciences, 121(7), e2312775121 (2024)

Sustained unidirectional rotation of a self-organized DNA rotor on a nanopore

Authors: Xin Shi, Anna-Katharina Pumm, Jonas Isensee, Wenxuan Zhao, Daniel Verschueren, Alejandro Martin-Gonzalez, Ramin Golestanian, Hendrik Dietz, Cees Dekker

Abstract: Flow-driven rotary motors drive functional processes in human society such as windmills and water wheels. Although examples of such rotary motors also feature prominently in cell biology, their synthetic construction at the nanoscale has thus far remained elusive. Here, we demonstrate flow-driven rotary motion of a self-organized DNA nanostructure that is docked onto a nanopore in a thin solid-sta… ▽ More Flow-driven rotary motors drive functional processes in human society such as windmills and water wheels. Although examples of such rotary motors also feature prominently in cell biology, their synthetic construction at the nanoscale has thus far remained elusive. Here, we demonstrate flow-driven rotary motion of a self-organized DNA nanostructure that is docked onto a nanopore in a thin solid-state membrane. An elastic DNA bundle self assembles into a chiral conformation upon phoretic docking onto the solid-state nanopore, and subsequently displays a sustained unidirectional rotary motion of up to 20 revolutions/s. The rotors harness energy from a nanoscale water and ion flow that is generated by a static (electro)chemical potential gradient in the nanopore that is established through a salt gradient or applied voltage. These artificial nanoengines self-organize and operate autonomously in physiological conditions, paving a new direction in constructing energy-transducing motors at nanoscale interfaces. △ Less

Submitted 14 June, 2022; originally announced June 2022.

Journal ref: Nat. Phys. 18 (2022) 1105-1111

A DNA turbine powered by a transmembrane potential across a nanopore

Authors: Xin Shi, Anna-Katharina Pumm, Christopher Maffeo, Fabian Kohler, Elija Feigl, Wenxuan Zhao, Daniel Verschueren, Ramin Golestanian, Aleksei Aksimentiev, Hendrik Dietz, Cees Dekker

Abstract: Rotary motors play key roles in energy transduction, from macroscale windmills to nanoscale turbines such as ATP synthase in cells. Despite our capabilities to construct engines at many scales, developing functional synthetic turbines at the nanoscale has remained challenging. Here, we experimentally demonstrate rationally designed nanoscale DNA-origami turbines with three chiral blades. These DNA… ▽ More Rotary motors play key roles in energy transduction, from macroscale windmills to nanoscale turbines such as ATP synthase in cells. Despite our capabilities to construct engines at many scales, developing functional synthetic turbines at the nanoscale has remained challenging. Here, we experimentally demonstrate rationally designed nanoscale DNA-origami turbines with three chiral blades. These DNA nanoturbines are 24-27 nm in height and diameter and can utilise transmembrane electrochemical potentials across nanopores to drive DNA bundles into sustained unidirectional rotations of up to 10 revolutions/s. The rotation direction is set by the designed chirality of the turbine. All-atom molecular dynamics simulations show how hydrodynamic flows drive this turbine. At high salt concentrations, the rotation direction of turbines with the same chirality is reversed, which is explained by a change in the anisotropy of the electrophoretic mobility. Our artificial turbines operate autonomously in physiological conditions, converting energy from naturally abundant electrochemical potentials into mechanical work. The results open new possibilities for engineering active robotics at the nanoscale. △ Less

Submitted 24 October, 2023; v1 submitted 14 June, 2022; originally announced June 2022.

Geometrically programmed self-limited assembly of tubules using DNA origami colloids

Authors: Daichi Hayakawa, Thomas E. Videbæk, Douglas M. Hall, Huang Fang, Christian Sigl, Elija Feigl, Hendrik Dietz, Seth Fraden, Michael F. Hagan, Gregory M. Grason, W. Benjamin Rogers

Abstract: Self-assembly is one of the most promising strategies for making functional materials at the nanoscale, yet new design principles for making self-limiting architectures, rather than spatially unlimited periodic lattice structures, are needed. To address this challenge, we explore the trade-offs between addressable assembly and self-closing assembly of a specific class of self-limiting structures:… ▽ More Self-assembly is one of the most promising strategies for making functional materials at the nanoscale, yet new design principles for making self-limiting architectures, rather than spatially unlimited periodic lattice structures, are needed. To address this challenge, we explore the trade-offs between addressable assembly and self-closing assembly of a specific class of self-limiting structures: cylindrical tubules. We make triangular subunits using DNA origami that have specific, valence-limited interactions and designed binding angles, and study their assembly into tubules that have a self-limited width that is much larger than the size of an individual subunit. In the simplest case, the tubules are assembled from a single component by geometrically programming the dihedral angles between neighboring subunits. We show that the tubules can reach many micrometers in length and that their average width can be prescribed through the dihedral angles. We find that there is a distribution in the width and the chirality of the tubules, which we rationalize by developing a model that considers the finite bending rigidity of the assembled structure as well as the mechanism of self-closure. Finally, we demonstrate that the distributions of tubules can be further sculpted by increasing the number of subunit species, thereby increasing the assembly complexity, and demonstrate that using two subunit species successfully reduces the number of available end states by half. These results help to shed light on the roles of assembly complexity and geometry in self-limited assembly and could be extended to other self-limiting architectures, such as shells, toroids, or triply-periodic frameworks. △ Less

Submitted 2 March, 2022; originally announced March 2022.

Comments: Main text 11 pages and 4 figures; SI 44 pages, 19 figures, 9 tables

Journal ref: PNAS 119 (43) e2207902119 (2022)

Molecular engineering of chiral colloidal liquid crystals using DNA origami

Authors: Mahsa Siavashpouri, Christian H. Wachauf, Mark J. Zakhary, Florian Praetorius, Hendrik Dietz, Zvonimir Dogic

Abstract: Establishing precise control over the shape and the interactions of the microscopic building blocks is essential for design of macroscopic soft materials with novel structural, optical and mechanical properties. Here, we demonstrate robust assembly of DNA origami filaments into cholesteric liquid crystals, 1D supramolecular twisted ribbons and 2D colloidal membranes. The exquisite control afforded… ▽ More Establishing precise control over the shape and the interactions of the microscopic building blocks is essential for design of macroscopic soft materials with novel structural, optical and mechanical properties. Here, we demonstrate robust assembly of DNA origami filaments into cholesteric liquid crystals, 1D supramolecular twisted ribbons and 2D colloidal membranes. The exquisite control afforded by the DNA origami technology establishes a quantitative relationship between the microscopic filament structure and the macroscopic cholesteric pitch. Furthermore, it also enables robust assembly of 1D twisted ribbons, which behave as effective supramolecular polymers whose structure and elastic properties can be precisely tuned by controlling the geometry of the elemental building blocks. Our results demonstrate the potential synergy between DNA origami technology and colloidal science, in which the former allows for rapid and robust synthesis of complex particles, and the latter can be used to assemble such particles into bulk materials. △ Less

Submitted 24 May, 2017; originally announced May 2017.

Journal ref: Nature Materials (2017)