We demonstrate the uniaxial alignment of a liquid-crystalline conjugated polymer, poly(9,9-dioctylfluorene-co-benzothiadiazole) (F8BT) by means of nanoconfinement during nanoimprinting. The orientation of the conjugated backbones was parallel to the nanolines imprinted into the polymer film. Polarized UV-vis absorption and photoluminescence spectra were measured to quantify the degree of alignment, showing that the polarization ratio and uniaxial molecular order parameter were as high as 66 and 0.97, respectively. The aligned F8BT film was used as the active layer in a PLED, which resulted in polarized electroluminescence with a polarization ratio of 11. Ambipolar PFET in a top-gate configuration with aligned F8BT as the active semiconducting layer showed mobility enhancement when the chains were aligned parallel to the transport direction. Mobility anisotropies for hole and electron transport were 10-15 and 5-7, respectively, for current flow parallel and perpendicular to the alignment direction.
Moth's eye inspired multiscale ommatidial arrays offer multifunctional properties of great significance in optoelectronic devices. However, a major challenge remains in fabricating these arrays on large-area substrates using a simple and scalable technique. Here we present the fabrication of these multiscale ommatidial arrays over large areas by a distinct approach called sacrificial layer mediated nanoimprinting, which involves nanoimprinting aided by a sacrificial layer. The fabricated arrays exhibited excellent pattern uniformity over the entire patterned area. Optimum dimensions of the multiscale ommatidial arrays determined by the finite-difference time domain simulations served as the design parameters for replicating the arrays on glass. A broadband suppression of reflectance to a minimum of ∼1.4% and omnidirectional antireflection for highly oblique angles of incidence up to 70° were achieved. In addition, superhydrophobicity and superior antifogging characteristics enabled the retention of optical properties even in wet and humid conditions, suggesting reliable optical performance in practical outdoor conditions. We anticipate that these properties could potentially enhance the performance of optoelectronic devices and minimize the influence of in-service conditions. Additionally, as our technique is solely nanoimprinting-based, it may enable scalable and high-throughput fabrication of multiscale ommatidial arrays.
We report the self-assembly of single crystals of single-walled carbon nanotubes (SWCNTs) using thermolysis of nano-patterned precursors. The synthesis of these perfectly ordered, single crystals of SWCNTs results in extended structures with dimension on the micrometer scale. Each crystal is composed of an ordered array of tubes with identical diameters and chirality, although these properties vary between crystals. The results show that SWCNTs can be produced as a perfect bulk material on the micrometer scale and point toward the synthesis of bulk macroscopic crystalline material.
Three-dimensional hierarchical patterning of metals is of paramount importance in diverse fields involving photonics, controlling surface wettability and wearable electronics. Conventionally, this type of structuring is tedious and usually involves layer-by-layer lithographic patterning. Here, we describe a simple process of direct nanoimprint lithography using palladium benzylthiolate, a versatile metal-organic ink, which not only leads to the formation of hierarchical patterns but also is amenable to layer-by-layer stacking of the metal over large areas. The key to achieving such multi-faceted patterning is hysteretic melting of ink, enabling its shaping. It undergoes transformation to metallic palladium under gentle thermal conditions without affecting the integrity of the hierarchical patterns on micro- as well as nanoscale. A metallic rice leaf structure showing anisotropic wetting behavior and woodpile-like structures were thus fabricated. Furthermore, this method is extendable for transferring imprinted structures to a flexible substrate to make them robust enough to sustain numerous bending cycles.
Conventional methods for electron beam patterning of TiO2 are based on sputtering and lift-off. This poses significant problems in producing high aspect ratio and stoichiometric structures, especially in the sub-100 nm size range. We describe an alternative approach of preparing spin-coatable TiO2 resists by chemically reacting titanium n-butoxide with benzoylacetone in methyl alcohol. They have an electron beam sensitivity of ∼35 mC cm-2 and are >107 times more sensitive to an electron beam than sputtered TiO x and crystalline TiO2 films. Fourier transform infrared studies suggest that exposure to an electron beam results in the gradual removal of organic material from the resist. This makes the exposed resist insoluble in organic solvents such as acetone, thereby providing high-resolution negative patterns as small as 8 nm wide. Such negative patterns can be written with a pitch as close as 30 nm.
High temperature nanoimprinting of viscous polymers which are glassy at room temperature is usually performed using brittle and expensive molds made of inorganic materials. As a replacement, soft molds made of plastics or elastomers have been used because of their low cost and ease of fabrication. However, the deformation of polymer molds under pressure remains a major issue which limits their resolution in high temperature nanoimprinting. Moreover, the replicated structures are often broken or lack definition due to sticking of the embossed polymer to the mold. We report a method for imprinting fine, densely packed nanostructures down to 12 nm into a wide range of technologically important polymers using a flexible and robust mold made from ethylene(tetrafluoroethylene) (ETFE). The high resolution achieved is due to the mold's mechanical stability and resistance to distortion at high pressures and high temperatures. The flexibility and low surface energy of ETFE provide a clean mold release without fracture or deformation of the embossed structures. Multiple imprinting and patterning on large areas is also made possible because of the good conformal contact and low‐adhesion of the ETFE mold. Finally, this simple and inexpensive method allows reproduction of the stamps from one single master, thus providing an economical alternative to expensive and brittle inorganic materials.
Direct patterning of oxides using thermal nanoimprint lithography is performed using either the sol-gel or methacrylate route. The sol-gel method results in resists with long shelf-life, but with high surface energy and a considerable amount of solvent that affects the quality of imprinting. The methacrylate route, which is limited to certain oxides, produces polymerizable resists, leading to low surface energy, but suffers from the shorter shelf-life of precursors. By combining the benignant elements from both these routes, a universal method of direct thermal nanoimprinting of oxides is demonstrated using precursors produced by reacting an alkoxide with a polymerizable chelating agent such as 2-(methacryloyloxy)ethyl acetoacetate (MAEAA). MAEAA possesses β -ketoester, which results in the formation of environmentally stable, chelated alkoxide with long shelf-life, and methacrylate groups, which provide a reactive monomer pendant for in situ copolymerization with a cross-linker during imprinting. Polymerization leads to trapping of cations, lowering of surface energy, strengthening of imprints, which enables easy and clean demolding over 1 cm × 2 cm patterned area with ≈ 100% yield. Heat-treatment of imprints gives amorphous/crystalline oxide patterns. This alliance between two routes enables the successful imprinting of numerous oxides including
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