A major challenge in nanoparticle self-assembly is programming the large-area organization of a single type of anisotropic nanoparticle into distinct superlattices with tunable packing efficiencies. Here we utilize nanoscale surface chemistry to direct the self-assembly of silver octahedra into three distinct two-dimensional plasmonic superlattices at a liquid/liquid interface. Systematically tuning the surface wettability of silver octahedra leads to a continuous superlattice structural evolution, from close-packed to progressively open structures. Notably, silver octahedra standing on vertices arranged in a square lattice is observed using hydrophobic particles. Simulations reveal that this structural evolution arises from competing interfacial forces between the particles and both liquid phases. Structure-to-function characterizations reveal that the standing octahedra array generates plasmonic ‘hotstrips', leading to nearly 10-fold more efficient surface-enhanced Raman scattering compared with the other more densely packed configurations. The ability to assemble these superlattices on the wafer scale over various platforms further widens their potential applications.
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Information on the physicochemical variability in rapeseed oil from different varieties during each refining process is lacking. Our purpose was to investigate the physicochemical properties, micronutrients and oxidative stability of the oil extracted from the five varieties of rapeseeds during their different stages of refining process. Increase in the acid value, peroxide value and p -anisidine value were detected in the refining, while content of tocopherols, sterols, β-carotene and phenols, which are regarded as important nutritional compounds diminished. Moreover, the loss rate of total phytosterols of all oils during neutralization (9.23–7.3%) and deodorization (9.97–8.27%) were higher than that of degumming (3.01–0.87%) and bleaching (2.75–1.18%). Deodorization affected total tocopherols contents the most, followed by bleaching, neutralization and degumming. There was a remarkable reduction in total content of phenol, β-carotene and oxygen radical absorbance of all oils during refining. The accumulated information can be used in looking for the optimum condition to meet the basic requirements for oil and minimize micronutrients losses so as to increase their market value.
Current plasmonic metasurfaces of nanocubes are limited to planar configurations, restricting the ability to create tailored local electromagnetic fields. Here, we report a new chemical strategy to achieve tunable metasurfaces with nonplanar nanocube orientations, creating novel lattice-dependent field localization patterns. We manipulate the interfacial behaviors of Ag nanocubes by controlling the ratio of hydrophilic/hydrophobic molecules added in a binary thiol mixture during the surface functionalization step. The nanocube orientation at an oil/water interface can consequently be continuously tuned from planar to tilted and standing configurations, leading to the organization of Ag nanocubes into three unique large-area metacrystals, including square close-packed, linear, and hexagonal lattices. In particular, the linear and hexagonal metacrystals are unusual open lattices comprising nonplanar nanocubes, creating unique local electromagnetic field distribution patterns. Large-area "hot hexagons" with significant delocalization of hot spots form in the hexagonal metacrystal. With a lowest packing density of 24%, the hexagonal metacrystal generates nearly 350-fold stronger surface-enhanced Raman scattering as compared to the other denser-packing metacrystals, demonstrating the importance of achieving control over the geometrical and spatial orientation of the nanocubes in the metacrystals.
The application of aluminum (Al)-based nanostructures for visible-range plasmonics, especially for surface-enhanced Raman scattering (SERS), currently suffers from inconsistent local electromagnetic field distributions and/or inhomogeneous distribution of probe molecules. Herein, we lithographically fabricate structurally uniform Al nanostructures which enable homogeneous adsorption of various probe molecules. Individual Al nanostructures exhibit strong local electromagnetic field enhancements, in turn leading to intense SERS activity. The average SERS enhancement factor (EF) for individual nanostructures exceeds 10 for non-resonant probe molecules in the visible spectrum. These Al nanostructures also retain more than 70% of their original SERS intensities after one-month storage, displaying superb stability under ambient conditions. We further achieve tunable polarization-dependent SERS responses using anisotropic Al nanostructures, facilitating the design of sophisticated SERS-based security labels. Our micron-sized security label comprises two-tier security features, including a machine-readable hybrid quick-response (QR) code overlaid with a set of ciphertexts. Our work demonstrates the versatility of Al-based structures in low-cost modern chemical nano-analytics and forgery protection.
Current surface-enhanced Raman scattering (SERS)-based anticounterfeiting strategies primarily encode molecular information in single two-dimensional (2D) planes and under-utilize the three-dimensionality (3D) of plasmonic hot spots. Here, we demonstrate a 3D SERS anticounterfeiting platform, extending “layered security” capabilities from 2D to 3D. We achieve this capability by combining 3D candlestick microstructures with 3D hyperspectral SERS imaging to fully resolve at least three layers of encoded information within the same 2D area along the z-axis, notably using only a single probe molecule. Specific predesigned covert images can only be fully recovered via SERS imaging at predetermined z values. Furthermore, our 3D SERS anticounterfeiting security labels can be fabricated on both rigid and flexible substrates, widening their potential usages to curved product surfaces and banknotes.
This paper presents a tunable optofluidic waveguide dye laser utilizing two centrifugal Dean flows. The centrifugal Dean flow increases the light confinement of the dye laser by shaping a three-dimensional (3D) liquid waveguide from curved microchannels. The active medium with the laser dye is dissolved in the liquid core and pumped with an external pump laser to produce stimulated emission. The laser's Fabry-Pérot microcavity is formed with a pair of aligned gold-coated fiber facets to amplify the fluorescent emission. The advantage of the 3D optofluidic waveguide dye laser is its higher efficiency, thus to obtain lasing at a reduced threshold (60%) with higher output energy. The demonstrated slope efficiency is at least 3-fold higher than its traditional two-dimensional equivalent. In addition, the laser output energy can be varied on demand by tuning the flow rates of the two flows. This technique provides a versatile platform for high potential applications microfluidic biosensor and bioanalysis.
A dithienobenzodithiophene‐based π‐conjugated polymer consisting of fluorinated benzotriazole and benzothiadiazole is successfully applied through anti‐solvent method to passivate the defects of perovskite crystals. The fluorinated polymer interacts with under coordinated Pb2+ ions in the perovskite crystals to form Pb‐F bond which effectively passivates the defects. The trap density is reduced and the charge carrier transfer between the perovskite film and Spiro‐OMeTAD is also improved after passivation with the polymer. As a result, a power conversion efficiency (PCE) of 18.03% is achieved in the champion cell. After storing in an ambient environment with 60% relative humidity for 1000 h, the device still retains 90% of the original PCE. These results demonstrate that dithienobenzodithiophene‐based π‐conjugated polymers are promising materials for passivation of perovskite films to further improve the performance and stability of perovskite solar cells.
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