Diamond-lattice photonic crystals assembled from DNA origami.

Colloidal self-assembly allows rational design of structures on the micrometer and submicrometer scale. One architecture that can generate complete three-dimensional photonic bandgaps is the diamond cubic lattice, which has remained difficult to realize at length scales comparable with the wavelength of visible or ultraviolet light. In this work, we demonstrate three-dimensional photonic crystals self-assembled from DNA origami that act as precisely programmable patchy colloids. Our DNA-based nanoscale tetrapods crystallize into a rod-connected diamond cubic lattice with a periodicity of 170 nanometers. This structure serves as a scaffold for atomic-layer deposition of high-refractive index materials such as titanium dioxide, yielding a tunable photonic bandgap in the near-ultraviolet.

Site-directed placement of three-dimensional DNA origami.

The combination of lithographic methods with two-dimensional DNA origami self-assembly has led, among others, to the development of photonic crystal cavity arrays and the exploration of sensing nanoarrays where molecular devices are patterned on the sub-micrometre scale. Here we extend this concept to the third dimension by mounting three-dimensional DNA origami onto nanopatterned substrates, followed by silicification to provide hybrid DNA-silica structures exhibiting mechanical and chemical stability and achieving feature sizes in the sub-10-nm regime. Our versatile and scalable method relying on self-assembly at ambient temperatures offers the potential to three-dimensionally position any inorganic and organic components compatible with DNA origami nanoarchitecture, demonstrated here with gold nanoparticles. This way of nanotexturing could provide a route for the low-cost production of complex and three-dimensionally patterned surfaces and integrated devices designed on the molecular level and reaching macroscopic dimensions.

Visible wavelength spectral tuning of absorption and circular dichroism of DNA-assembled Au/Ag core-shell nanorod assemblies.

Plasmonic nanoparticles have unique properties which can be harnessed to manipulate light at the nanoscale. With recent advances in synthesis protocols that increase their stability, gold-silver core-shell nanoparticles have become suitable building blocks for plasmonic nanostructures to expand the range of attainable optical properties. Here we tune the plasmonic response of gold-silver core-shell nanorods over the visible spectrum by varying the thickness of the silver shell. Through the chiral arrangement of the nanorods with the help of various DNA origami designs, the spectral tunability of the plasmon resonance frequencies is transferred into circular dichroism signals covering the spectrum from 400 nm to 700 nm. Our approach could aid in the construction of better sensors as well as metamaterials with a tunable optical response in the visible region.

A label-free light-scattering method to resolve assembly and disassembly of DNA nanostructures.

DNA self-assembly, and in particular DNA origami, has evolved into a reliable workhorse for organizing organic and inorganic materials with nanometer precision and with exactly controlled stoichiometry. To ensure the intended performance of a given DNA structure, it is beneficial to determine its folding temperature, which in turn yields the best possible assembly of all DNA strands. Here, we show that temperature-controlled sample holders and standard fluorescence spectrometers or dynamic light-scattering setups in a static light-scattering configuration allow for monitoring the assembly progress in real time. With this robust label-free technique, we determine the folding and melting temperatures of a set of different DNA origami structures without the need for more tedious protocols. In addition, we use the method to follow digestion of DNA structures in the presence of DNase I and find strikingly different resistances toward enzymatic degradation depending on the structural design of the DNA object.

Self-assembled toron-like structures in inverse nematic gels.

A novel form of nematic gel (N-gel) wherein bright flower-like domains (BFDs) rich in gelator fibres are embedded in a matrix of liquid crystal (LC) molecules has been reported. These gels which we denote as inverse N-gels are unlike typical N-gels in which the LC is encapsulated within an aggregated network of gelator molecules. The self-organization of the helical gelator fibres within the BFDs leads to the creation of localized toron-like structures that are topologically protected due to their skyrmion director profile. Optical and confocal microscopy have been used to deduce the LC director configuration, in order to understand possible intermolecular interactions that can lead to the formation of the twisted structures and the inverse N-gels.

Surfaces Affect Screening Reliability in Formulation Development of Biologics.

PURPOSE: The ability to predict an antibody's propensity for aggregation is particularly important during product development to ensure the quality and safety of therapeutic antibodies. We demonstrate the role of container surfaces on the aggregation process of three mAbs under elevated temperature and long-term storage conditions in the absence of mechanical stress. METHODS: A systematic study of aggregation is performed for different proteins, vial material, storage temperature, and presence of surfactant. We use size exclusion chromatography and micro-flow imaging to determine the bulk concentration of aggregates, which we combine with optical and atomic force microscopy of vial surfaces to determine the effect of solid-liquid interfaces on the bulk aggregate concentration under different conditions. RESULTS: We show that protein particles under elevated temperature conditions adhere to the vial surfaces, causing a substantial underestimation of aggregation propensity as determined by common methods used in development of biologics. Under actual long-term storage conditions at 5°C, aggregate particles do not adhere to the surface, causing an increase in bulk concentration of particles, which cannot be predicted from elevated temperature screening tests by common methods alone. We also identify specific protein - surface interactions which promote oligomer formation in the nanometre range. CONCLUSIONS: Special care should be taken when interpreting size exclusion and particle count data from stability studies if different temperatures and vial types are involved. We propose a novel combination of methods to characterise vial surfaces and bulk solution for a full understanding of protein aggregation processes in a sample.

Topology-commanded optical properties of bistable electric-field-induced torons in cholesteric bubble domains.

Nowadays, complicated topological defects enable many experimental manipulations and configurational simulations of active soft matter for optical and photonic applications. Investigation of topological defects in soft anisotropic materials enables one to better understand three-dimensional orientation fields in cholesteric liquid crystals. Here, we describe optical properties of bistable bubble domain (BD) texture torons in a thin layer of cholesteric liquid crystal (CLC), frustrated by homeotropic anchoring conditions, and reliably switchable by a random process. The control of macroscopic optical density and diffraction efficiency of the BD texture is demonstrated by a selection of a confinement ratio of the CLC. Experimentally reconstructed CLC director profile reveals the topology of BD torons allowing consideration of naturally occurring BD texture for applications in optical and photonic devices, which are bistably switchable between active and transparent optical states.

Hidden topological constellations and polyvalent charges in chiral nematic droplets.

Topology has an increasingly important role in the physics of condensed matter, quantum systems, material science, photonics and biology, with spectacular realizations of topological concepts in liquid crystals. Here we report on long-lived hidden topological states in thermally quenched, chiral nematic droplets, formed from string-like, triangular and polyhedral constellations of monovalent and polyvalent singular point defects. These topological defects are regularly packed into a spherical liquid volume and stabilized by the elastic energy barrier due to the helical structure and confinement of the liquid crystal in the micro-sphere. We observe, for the first time, topological three-dimensional point defects of the quantized hedgehog charge q=-2, -3. These higher-charge defects act as ideal polyvalent artificial atoms, binding the defects into polyhedral constellations representing topological molecules.

Points, skyrmions and torons in chiral nematic droplets.

Chiral nematic droplets with perpendicular surface alignment of liquid crystalline molecules frustrate the helical structure into convoluted 3D textures with complex topology. We observe the droplets with fluorescent confocal polarising microscopy (FCPM), and reconstruct and analyse for the first time the topology of the 3D director field using a novel method of director reconstruction from raw data. We always find an odd number of topological defects, which preserve the total topological charge of the droplet of +1 regardless of chirality. At higher chirality, we observe up to 5 point hedgehog defects, which are elastically stabilized with convoluted twisted structures, reminiscent of 2D skyrmions and toron-like structure, nested into a sphere.