The size of it: Mesoporous silica nanoparticles (MSNs) of controlled size in the range 30 to 280 nm are obtained by adjusting the pH of the reaction solution. The uptake of fluorescein‐labeled MSNs (green, see image) by HeLa cells is size‐dependent, with maximum uptake at a nanoparticle size of 50 nm.
A novel ZnO hierarchical micro/nanoarchitecture is fabricated by a facile solvothermal approach in an aqueous solution of ethylenediamine (EDA). This complex architecture is of a core/shell structure, composed of dense nanosheet‐built networks that stand on a hexagonal‐pyramid‐like microcrystal (core part). The ZnO hexagonal micropyramid has external surfaces that consist of a basal plane (000${\bar 1}$) and lateral planes {0${\bar 1}$11}. The nanosheets are a uniform thickness of about 10 nm and have a single‐crystal structure with sheet‐planar surfaces as {2${\bar 1}\,{\bar 1}$0} planes. These nanosheets interlace and overlap each other with an angle of 60° or 120°, and assemble into a discernible net‐ or grid‐like morphology (about 100 nm in grid‐size) on the micropyramid, which shows a high specific surface area (185.6 m2 g−1). Such a ZnO micro/nanoarchitecture is new in the family of ZnO nanostructures. Its formation depends on the concentration of the EDA solution as well as on the type of zinc source. A two‐step sequential growth model is proposed based on observations from a time‐dependent morphology evolution process. Importantly, such structured ZnO has shown a strong structure‐induced enhancement of photocatalytic performance and has exhibited a much better photocatalytic property and durability for the photodegradation of methyl orange than that of other nanostructured ZnO, such as the powders of nanoparticles, nanosheets, and nanoneedles. This is mainly attributed to its higher surface‐to‐volume ratio and stability against aggregation. This work not only gives insight into understanding the hierarchical growth behaviour of complex ZnO micro/nanoarchitectures in a solution‐phase synthetic system, but also provides an efficient route to enhance the photocatalytic performance of ZnO, which could also be extended to other catalysts, such as the inherently excellent TiO2, if they are of the same hierarchical micro/nanoarchitecture with an open and porous nanostructured surface layer.
Nanoparticles coated with DNA molecules can be programmed to self-assemble into three-dimensional superlattices. Such superlattices can be made from nanoparticles with different functionalities and could potentially exploit the synergetic properties of the nanoscale components. However, the approach has so far been used primarily with single-component systems. Here, we report a general strategy for the creation of heterogeneous nanoparticle superlattices using DNA and carboxylic-based conjugation. We show that nanoparticles with all major types of functionality--plasmonic (gold), magnetic (Fe2O3), catalytic (palladium) and luminescent (CdSe/Te@ZnS and CdSe@ZnS)--can be incorporated into binary systems in a rational manner. We also examine the effect of nanoparticle characteristics (including size, shape, number of DNA per particle and DNA flexibility) on the phase behaviour of the heterosystems, and demonstrate that the assembled materials can have novel optical and field-responsive properties.
One of the most intriguing structural properties, chirality, is often exhibited by organic and bio-organic molecular constructs. Chiral spectral signatures, typically appearing in the UV range for organic materials and known as circular dichroism (CD), are widely used to probe a molecular stereometry. Such probing has an increasingly broad importance for biomedical and pharmacological fields due to synthesis/separation/detection of homochiral species, biological role of chiral organization, and structural response to environmental conditions and enantiomeric drugs. Recent theoretical and experimental works demonstrated that the CD signal from chiral organic molecules could appear in the plasmonic (typically, visible) band when they coupled with plasmonic particles. However, the magnitude of this CD signal, induced by discrete nonchiral plasmonic particles, and its native molecular analog were found to be comparable. Here we show that shaped nonchiral nanoparticles, namely, gold/silver core/shell nanocubes, can act as plasmonic reporters of chirality for attached molecules by providing a giant, 2 orders of magnitude CD enhancement in a near-visible region. Through the experimental and theoretical comparison with nanoparticles of other shapes and materials, we demonstrate a uniqueness of silver nanocube geometry for the CD enhancement. The discovered phenomenon opens novel opportunities in ultrasensitive probing of chiral molecules and for novel optical nanomaterials based on the chiral elements.
Organization of spherical particles into lattices is typically driven by packing considerations. Although the addition of directional binding can significantly broaden structural diversity, nanoscale implementation remains challenging. Here we investigate the assembly of clusters and lattices in which anisotropic polyhedral blocks coordinate isotropic spherical nanoparticles via shape-induced directional interactions facilitated by DNA recognition. We show that these polyhedral blocks—cubes and octahedrons—when mixed with spheres, promote the assembly of clusters with architecture determined by polyhedron symmetry. Moreover, three-dimensional binary superlattices are formed when DNA shells accommodate the shape disparity between nanoparticle interfaces. The crystallographic symmetry of assembled lattices is determined by the spatial symmetry of the block's facets, while structural order depends on DNA-tuned interactions and particle size ratio. The presented lattice assembly strategy, exploiting shape for defining the global structure and DNA-mediation locally, opens novel possibilities for by-design fabrication of binary lattices.
The phase behavior of 3D assemblies of nanocubes in a ligand-rich solution upon solvent evaporation was experimentally investigated using small-angle x-ray scattering and electron microscopy. We observed a continuous transformation of assemblies between simple cubic and rhombohedral phases, where a variable angle of rhombohedral structure is determined by ligand thickness. We established a quantitative relationship between the particle shape evolution from cubes to quasispheres and the lattice distortion during the transformation, with a pathway exhibiting the highest known packing.
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