Extraction of mobile charge carrier photogeneration yield spectrum of ultrathin-film metal oxide photoanodes for solar water splitting.

Light absorption in strongly correlated electron materials can excite electrons and holes into a variety of different states. Some of these excitations yield mobile charge carriers, whereas others result in localized states that cannot contribute to photocurrent. The photogeneration yield spectrum, ξ(λ), represents the wavelength-dependent ratio between the contributing absorption that ultimately generates mobile charge carriers and the overall absorption. Despite being a vital material property, it is not trivial to characterize. Here, we present an empirical method to extract ξ(λ) through optical and external quantum efficiency measurements of ultrathin films. We applied this method to haematite photoanodes for water photo-oxidation, and observed that it is self-consistent for different illumination conditions and applied potentials. We found agreement between the extracted ξ(λ) spectrum and the photoconductivity spectrum measured by time-resolved microwave conductivity. These measurements revealed that mobile charge carrier generation increases with increasing energy across haematite's absorption spectrum. Low-energy non-contributing absorption fundamentally limits the photoconversion efficiency of haematite photoanodes and provides an upper limit to the achievable photocurrent that is substantially lower than that predicted based solely on absorption above the bandgap. We extended our analysis to TiO2 and BiVO4 photoanodes, demonstrating the broader utility of the method for determining ξ(λ).

Excipient-Free Pure Drug Nanoparticles Fabricated by Microfluidic Hydrodynamic Focusing.

Nanoprecipitation is one of the most versatile methods to produce pure drug nanoparticles (PDNPs) owing to the ability to optimize the properties of the product. Nevertheless, nanoprecipitation may result in broad particle size distribution, low physical stability, and batch-to-batch variability. Microfluidics has emerged as a powerful tool to produce PDNPs in a simple, reproducible, and cost-effective manner with excellent control over the nanoparticle size. In this work, we designed and fabricated T- and Y-shaped Si-made microfluidic devices and used them to produce PDNPs of three kinase inhibitors of different lipophilicity and water-solubility, namely imatinib, dasatinib and tofacitinib, without the use of colloidal stabilizers. PDNPs display hydrodynamic diameter in the 90-350 nm range as measured by dynamic light scattering and a rounded shape as visualized by high-resolution scanning electron microscopy. Powder X-ray diffraction and differential scanning calorimetry confirmed that this method results in highly amorphous nanoparticles. In addition, we show that the flow rate of solvent, the anti-solvent, and the channel geometry of the device play a key role governing the nanoparticle size.

Propagation Length of Antiferromagnetic Magnons Governed by Domain Configurations.

The compensated magnetic order and characteristic terahertz frequencies of antiferromagnetic materials make them promising candidates to develop a new class of robust, ultrafast spintronic devices. The manipulation of antiferromagnetic spin-waves in thin films is anticipated to lead to new exotic phenomena such as spin-superfluidity, requiring an efficient propagation of spin-waves in thin films. However, the reported decay length in thin films has so far been limited to a few nanometers. In this work, we achieve efficient spin-wave propagation over micrometer distances in thin films of the insulating antiferromagnet hematite with large magnetic domains while evidencing much shorter attenuation lengths in multidomain thin films. Through transport and magnetic imaging, we determine the role of the magnetic domain structure and spin-wave scattering at domain walls to govern the transport. We manipulate the spin transport by tailoring the domain configuration through field cycle training. For the appropriate crystalline orientation, zero-field spin transport is achieved across micrometers, as required for device integration.

Film Flip and Transfer Process to Enhance Light Harvesting in Ultrathin Absorber Films on Specular Back-Reflectors.

Optical interference is used to enhance light-matter interaction and harvest broadband light in ultrathin semiconductor absorber films on specular back-reflectors. However, the high-temperature processing in oxygen atmosphere required for oxide absorbers often degrades metallic back-reflectors and their specular reflectance. In order to overcome this problem, a newly developed film flip and transfer process is presented that enables high-temperature processing without degradation of the metallic back-reflector and without the need of passivation interlayers. The film flip and transfer process improves the performance of photoanodes for photoelectrochemical water splitting comprising ultrathin (<20 nm) hematite (α-Fe2 O3 ) films on silver-gold alloy (90 at% Ag-10 at% Au) back-reflectors. Specular back-reflectors are obtained with high reflectance below hematite films, which is necessary for maximizing the productive light absorption in the hematite film and minimizing nonproductive absorption in the back-reflector. Furthermore, the film flip and transfer process opens up a new route to attach thin film stacks onto a wide range of substrates including flexible or temperature sensitive materials.

Hybrid bio-photo-electro-chemical cells for solar water splitting.

Photoelectrochemical water splitting uses solar power to decompose water to hydrogen and oxygen. Here we show how the photocatalytic activity of thylakoid membranes leads to overall water splitting in a bio-photo-electro-chemical (BPEC) cell via a simple process. Thylakoids extracted from spinach are introduced into a BPEC cell containing buffer solution with ferricyanide. Upon solar-simulated illumination, water oxidation takes place and electrons are shuttled by the ferri/ferrocyanide redox couple from the thylakoids to a transparent electrode serving as the anode, yielding a photocurrent density of 0.5 mA cm(-2). Hydrogen evolution occurs at the cathode at a bias as low as 0.8 V. A tandem cell comprising the BPEC cell and a Si photovoltaic module achieves overall water splitting with solar to hydrogen efficiency of 0.3%. These results demonstrate the promise of combining natural photosynthetic membranes and man-made photovoltaic cells in order to convert solar power into hydrogen fuel.