The generation of hydrogen from water using sunlight could potentially form the basis of a clean and renewable source of energy. Various water-splitting methods have been investigated previously, but the use of photocatalysts to split water into stoichiometric amounts of H2 and O2 (overall water splitting) without the use of external bias or sacrificial reagents is of particular interest because of its simplicity and potential low cost of operation. However, despite progress in the past decade, semiconductor water-splitting photocatalysts (such as (Ga1-xZnx)(N1-xOx)) do not exhibit good activity beyond 440 nm (refs 1,2,9) and water-splitting devices that can harvest visible light typically have a low solar-to-hydrogen efficiency of around 0.1%. Here we show that cobalt(II) oxide (CoO) nanoparticles can carry out overall water splitting with a solar-to-hydrogen efficiency of around 5%. The photocatalysts were synthesized from non-active CoO micropowders using two distinct methods (femtosecond laser ablation and mechanical ball milling), and the CoO nanoparticles that result can decompose pure water under visible-light irradiation without any co-catalysts or sacrificial reagents. Using electrochemical impedance spectroscopy, we show that the high photocatalytic activity of the nanoparticles arises from a significant shift in the position of the band edge of the material.
Zero dimensional perovskite Cs4PbBr6 has attracted considerable attention recently not only because of its highly efficient green photoluminescence (PL), but also its two highly debated opposing mechanisms of the luminescence: embedded CsPbBr3 nanocrystals versus intrinsic Br vacancy states. After a brief discussion on the root cause of the controversy, we provide sensitive but noninvasive methods that can not only directly correlate luminescence with the underlying structure, but also distinguish point defects from embedded nanostructures. We first synthesized both emissive and non-emissive Cs4PbBr6 crystals, obtained the complete Raman spectrum of Cs4PbBr6 and assigned all Raman bands based on density functional theory simulations. We then used correlated Raman-PL as a passive structure-property method to identify the difference between emissive and non-emissive Cs4PbBr6 crystals and revealed the existence of CsPbBr3 nanocrystals in emissive Cs4PbBr6. We finally employed a diamond anvil cell to probe the response of luminescence centers to hydrostatic pressure. The observations of fast red-shifting, diminishing and eventual disappearance of both green emission and Raman below Cs4PbBr6 phase transition pressure of ~3 GPa is compatible with CsPbBr3 nanocrystal inclusions as green PL emitters and cannot be explained by Br vacancies. The resolution of this long-lasting controversy paves the way for further device applications of low dimensional perovskites, and our comprehensive optical technique integrating structure-property with dynamic pressure response is generic and can be applied to other emerging optical materials to understand the nature of their luminescent centers.
Same-spot Raman-photoluminescence with two lasers in a diamond anvil cell under hydrostatic pressure reveals that CsPbBr 3 nanocrystals, mostly located on the edges of CsPb 2 Br 5 2D platelets, are responsible for CsPb 2 Br 5 's green emission. This sensitive non-invasive technique combining static and dynamic probes establishes a one-toone property-structure relationship and distinguishes light emission from point defects versus nano-inclusions.
A DNA‐origami chip platform for target‐labeling‐free single‐nucleotide polymorphism (SNP) genotyping is presented. DNA capture probes are anchored on an asymmetric map‐shaped DNA‐origami chip and a “toehold”‐mediated strand‐displacement reaction is employed to endow single‐base‐mismatch differentiation specificity. This design leads to a reliable and potentially universal means for SNP genotyping.
The observation of low-energy edge photoluminescence and its beneficial effect on the solar cell efficiency of Ruddlesden−Popper perovskites has unleashed an intensive research effort to reveal its origin. This effort, however, has been met with more challenges as the underlying material structure has still not been identified; new modelings and observations also do not seem to converge. Using twodimensional (2D) (BA) 2 (MA) 2 Pb 3 Br 10 as an example, we show that threedimensional (3D) MAPbBr 3 is formed due to the loss of BA on the edge. This self-formed MAPbBr 3 can explain the reported edge emission under various conditions, while the reported intriguing optoelectronic properties such as fast exciton trapping from the interior 2D perovskite, rapid exciton dissociation, and long carrier lifetime can be understood via the self-formed 2D/3D lateral perovskite heterostructure. The 3D perovskite is identified by submicron infrared spectroscopy, the emergence of X-ray diffraction (XRD) signature from freezer-milled nanometer-sized 2D perovskite, and its photoluminescence response to external hydrostatic pressure. The revelation of this edge emission mystery and the identification of a self-formed 2D/3D heterostructure provide a new approach to engineering 2D perovskites for high-performance optoelectronic devices.
This work presents an aptamer-based, highly sensitive and specific sensor for atto- to femtomolar level detection of bisphenol A (BPA). Because of its widespread use in numerous products, BPA enters surface water from effluent discharges during its manufacture, use, and from waste landfill sites throughout the world. On-site measurement of BPA concentrations in water is important for evaluating compliance with water quality standards or environmental risk levels of the harmful compound in the environment. The sensor in this work is porous, conducting, interdigitated electrodes that are formed by laser-induced carbonization of flexible polyimide sheets. BPA-specific aptamer is immobilized on the electrodes as the probe, and its binding with BPA at the electrode surface is detected by capacitive sensing. The binding process is aided by ac electroosmotic effect that accelerates the transport of BPA molecules to the nanoporous graphene-like structured electrodes. The sensor achieved a limit of detection of 58.28 aM with a response time of 20 s. The sensor is further applied for recovery analysis of BPA spiked in surface water. This work provides an affordable platform for highly sensitive, real time, and field-deployable BPA surveillance critical to the evaluation of the ecological impact of BPA exposure.
We demonstrate the enhanced four-wave mixing of monolayer graphene on slow-light silicon photonic crystal waveguides. 200-μm interaction length, a four-wave mixing conversion efficiency of −23 dB is achieved in the graphene-silicon slow-light hybrid, with an enhanced 3-dB conversion bandwidth of about 17 nm. Our measurements match well with nonlinear coupled-mode theory simulations based on the measured waveguide dispersion, and provide an effective way for all-optical signal processing in chip-scale integrated optics.
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