Over several billion years, cyanobacteria and plants have evolved highly organized photosynthetic systems to shuttle both electronic and chemical species for the efficient oxidation of water. In a similar manner to reaction centres in natural photosystems, molecular and metal oxide catalysts have been used to photochemically oxidize water. However, the various approaches involving the molecular design of ligands, surface modification and immobilization still have limitations in terms of catalytic efficiency and sustainability. Here, we demonstrate a biologically templated nanostructure for visible light-driven water oxidation that uses a genetically engineered M13 virus scaffold to mediate the co-assembly of zinc porphyrins (photosensitizer) and iridium oxide hydrosol clusters (catalyst). Porous polymer microgels are used as an immobilization matrix to improve the structural durability of the assembled nanostructures and to allow the materials to be recycled. Our results suggest that the biotemplated nanoscale assembly of functional components is a promising route to significantly improved photocatalytic water-splitting systems.
Biological molecules can be used as versatile templates for assembling nanoscale materials because of their unique structures and chemical diversities. Supramolecular organization of molecular pigments, as is found in the natural light-harvesting antenna, has drawn attention for its potential applications to sensors, photocatalytic systems, and photonic devices. Here we show the arrangement of molecular pigments into a one-dimensional light-harvesting antenna using M13 viruses as scaffolds. Chemical grafting of zinc porphyrins to M13 viruses induces distinctive spectroscopic changes, including fluorescence quenching, the extensive band broadening and small red shift of their absorption spectrum, and the shortened lifetime of the excited states. Based on these optical signatures we suggest a hypothetical model to explain the energy transfer occurring in the supramolecular porphyrin structures templated with the virus. We expect that further genetic engineering of M13 viruses can allow us to coassemble other functional materials (e.g., catalysts and electron transfer mediators) with pigments, implying potential applications to photochemical devices.
Long-term onabotulinumtoxinA treatment consistently decreased overactive bladder symptoms and improved quality of life with no new safety signals.
Cuttlefish, Sepia officinalis, possess neurally controlled, pigmented chromatophore organs that allow rapid changes in skin patterning and coloration in response to visual cues. This process of adaptive coloration is enabled by the 500% change in chromatophore surface area during actuation. We report two adaptations that help to explain how colour intensity is maintained in a fully expanded chromatophore when the pigment granules are distributed maximally: (i) pigment layers as thin as three granules that maintain optical effectiveness and (ii) the presence of high-refractive-index proteins-reflectin and crystallin-in granules. The latter discovery, combined with our finding that isolated chromatophore pigment granules fluoresce between 650 and 720 nm, refutes the prevailing hypothesis that cephalopod chromatophores are exclusively pigmentary organs composed solely of ommochromes. Perturbations to granular architecture alter optical properties, illustrating a role for nanostructure in the agile, optical responses of chromatophores. Our results suggest that cephalopod chromatophore pigment granules are more complex than homogeneous clusters of chromogenic pigments. They are luminescent protein nanostructures that facilitate the rapid and sophisticated changes exhibited in dermal pigmentation.
The negatively-charged nitrogen vacancy center (NV) in diamond has generated significant interest as a platform for quantum information processing and sensing in the solid state. For most applications, high quality optical cavities are required to enhance the NV zero-phonon line (ZPL) emission. An outstanding challenge in maximizing the degree of NV-cavity coupling is the deterministic placement of NVs within the cavity. Here, we report photonic crystal nanobeam cavities coupled to NVs incorporated by a delta-doping technique that allows nanometer-scale vertical positioning of the emitters. We demonstrate cavities with Q up to ~24,000 and mode volume V ~ 0.47(λ/n) 3 as well as resonant enhancement of the ZPL of an NV ensemble with Purcell factor of ~20. Our fabrication technique provides a first step towards deterministic NV-cavity coupling using spatial control of the emitters.A diamond-based emitter-cavity system provides an important platform for the realization of quantum information processing and sensing in the solid state 1-4 . The long electron spin coherence of the negatively-charged nitrogen vacancy center (subsequently referred to as NV) in
Lanthanides are vital components in lighting, imaging technologies and future quantum memory applications owing to their narrow optical transitions and long spin coherence times. Recently, diamond has become a pre-eminent platform for the realisation of many experiments in quantum information science. Here we demonstrate a promising approach to incorporate Eu ions into diamond, providing a means to harness the exceptional characteristics of both lanthanides and diamond in a single material. Polyelectrolytes are used to electrostatically assemble Eu(III) chelate molecules on diamond and subsequently chemical vapour deposition is employed for the diamond growth. Fluorescence measurements show that the Eu atoms retain the characteristic optical signature of Eu(III) upon incorporation into the diamond lattice. Computational modelling supports the experimental findings, corroborating that Eu(III) in diamond is a stable configuration. The formed defects demonstrate the outstanding chemical control over the incorporation of impurities into diamond enabled by the electrostatic assembly together with chemical vapour deposition growth.
Wireless neural stimulators are being developed to address problems associated with traditional lead-based implants. However, designing wireless stimulators on the sub-millimeter scale (<1 mm3) is challenging. As device size shrinks, it becomes difficult to deliver sufficient wireless power to operate the device. Here, we present a sub-millimeter, inductively powered neural stimulator consisting only of a coil to receive power, a capacitor to tune the resonant frequency of the receiver, and a diode to rectify the radio-frequency signal to produce neural excitation. By replacing any complex receiver circuitry with a simple rectifier, we have reduced the required voltage levels that are needed to operate the device from 0.5 to 1 V (e.g., for CMOS) to ~0.25–0.5 V. This reduced voltage allows the use of smaller receive antennas for power, resulting in a device volume of 0.3–0.5 mm3. The device was encapsulated in epoxy, and successfully passed accelerated lifetime tests in 80°C saline for 2 weeks. We demonstrate a basic proof-of-concept using stimulation with tens of microamps of current delivered to the sciatic nerve in rat to produce a motor response.
Optical coupling of an ensemble of silicon-vacancy (SiV) centers to single-crystal diamond microdisk cavities is demonstrated. The cavities are fabricated from a single-crystal diamond membrane generated by ion implantation and, electrochemical liftoff followed by homo-epitaxial overgrowth. Whispering gallery modes which spectrally overlap with the zero-phonon line (ZPL) of the SiV centers and exhibit quality factors ~2200 are measured. Lifetime reduction from 1.8 ns to 1.48 ns is observed from SiV centers in the cavity compared to those in the membrane outside the cavity. These results are pivotal in developing diamond integrated photonics networks
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