Precise analyses of photoelectrochemical reactions on particulate ZnCdSe photoanodes in nonaqueous electrolytes using Ru bipyridyl complexes as a probe.

Recombination of photoexcited carriers at interface states is generally believed to strongly govern the photoelectrochemical (PEC) performance of semiconductors in electrolytes. Sacrificial reagents (, methanol or NaSO) are often used to assess the ideal PEC performance of photoanodes in cases of minimised interfacial recombination kinetics as well as accelerated surface reaction kinetics. However, varying the sacrificial reagents in the electrolyte means simultaneously changing the equilibrium potential and the number of electrons required to perform the sacrificial reaction, and thus the thermodynamic and kinetic aspects of the PEC reactions cannot be distinguished.

The 'after you' gesture in a bird.

Gestures are ubiquitous in human communication, involving movements of body parts produced for a variety of purposes, such as pointing out objects (deictic gestures) or conveying messages (symbolic gestures). While displays of body parts have been described in many animals, their functional similarity to human gestures has primarily been explored in great apes, with little research attention given to other animal groups. To date, only a few studies have provided evidence for deictic gestures in birds and fish, but it is unclear whether non-primate animals can employ symbolic gestures, such as waving to mean 'goodbye', which are, in humans, more cognitively demanding than deictic gestures.

Nanoarchitectonics of highly dispersed polythiophene on paper for accurate quantitative detection of metal ions.

π-Conjugated polymers such as polythiophene provide intramolecular wire effects upon analyte capture, which contribute to sensitive detection in chemical sensing. However, inherent aggregation-induced quenching causes difficulty in fluorescent chemical sensing in the solid state. Herein, we propose a solid-state fluorescent chemosensor array device made of a paper substrate (PCSAD) for the qualitative and quantitative detection of metal ions.

Long and oriented graphene nanoribbon synthesis from well-ordered 10,10'-dibromo-9,9'-bianthracene monolayer on crystalline Au surfaces.

Bottom-up synthesis on metal surfaces has attracted attention for the fabrication of graphene nanoribbons (GNRs) with atomically-precise chemical structures to realize novel electronic devices. However, control of length and orientation on surfaces during GNR synthesis is difficult, thus, achieving longer and aligned GNR growth is a significant challenge. Herein, we report GNR synthesis from a well-ordered dense monolayer on Au crystalline surfaces for long and oriented GNR growth.

Highly active and stable surface structure for oxygen evolution reaction originating from balanced dissolution and strong connectivity in BaIrO solid solutions.

Catalysts for the oxygen evolution reaction (OER) are receiving great interest since OER remains the bottleneck of water electrolyzers for hydrogen production. Especially, OER in acidic solutions is crucial since it produces high current densities and avoids precipitation of carbonates. However, even the acid stable iridates undergo severe dissolution during the OER.

Organic deliquescence: organic vapor-induced dissolution of molecular salts.

This report demonstrates organic vapor-induced dissolution of several molecular salts (, organic deliquescence), like water vapor-induced deliquescence. Systematic experiments indicate that appropriate organic deliquescent responses to volatile organic compounds can be designed according to the principle, "like dissolves like". The phenomena will be useful for developing agents to collect various volatile organic compounds.

Tracking the crystallization behavior of high-silica FAU during AEI-type zeolite synthesis using acid treated FAU-type zeolite.

During AEI zeolite synthesis using acid treated FAU (AcT-FAU), we found the recrystallization of high-silica FAU with high crystallinity and Si/Al ratio of 6.1 using ,-dimethyl-3,5-dimethylpiperidinium hydroxide (DMDMPOH) after 2 h, followed by the crystallization of AEI FAU-to-AEI interzeolite conversion at a longer synthesis time. In order to understand the formation mechanism of high-silica FAU and generalize its direct synthesis, we have investigated this synthesis process.

Iterative synthesis of nitrogen-containing polyketide oxime intermediates.

Typical polyketides consist of C, H, and O atoms, whereas several types of N-containing polyketides are known to show intriguing properties. Because conventional synthetic approaches for such compounds focus on only specific structures, a more general method is desirable. Here, we have developed an iterative synthesis of nitrogen-containing polyketide.

Electrochemical deposition of amorphous cobalt oxides for oxygen evolution catalysis.

The oxygen evolution reaction (OER) is crucial in water splitting for hydrogen production. However, its high over-potential and sluggish kinetics cause an additional energy loss and hinder its practical application. The cobalt spinel oxide CoO exhibits a high catalytic activity for the OER in alkaline solutions.

Ratchet-like mechanism in a long-life photoproduct of salicylideneaniline enclathrated in a pillared-layer guanidinium disulfonate structure.

Salicylideneaniline (SA) was found to exhibit extraordinary long-life photochromism upon being included in a cavity of guanidinium organosulfonate and exhibited a lifetime of ∼30 times that of a pure SA crystal. Crystal structure analysis suggested that the sulfonate molecule in the apo-host provided a flexible cavity space that kinetically trapped SA in its photo-isomerized form, as if it was locked by a ratchet-like mechanism.

The origin of unidirectional charge separation in photosynthetic reaction centers: nonadiabatic quantum dynamics of exciton and charge in pigment-protein complexes.

Exciton charge separation in photosynthetic reaction centers from purple bacteria (PbRC) and photosystem II (PSII) occurs exclusively along one of the two pseudo-symmetric branches (active branch) of pigment-protein complexes. The microscopic origin of unidirectional charge separation in photosynthesis remains controversial. Here we elucidate the essential factors leading to unidirectional charge separation in PbRC and PSII, using nonadiabatic quantum dynamics calculations in conjunction with time-dependent density functional theory (TDDFT) with the quantum mechanics/molecular mechanics/polarizable continuum model (QM/MM/PCM) method.

Distorted Porphyrins with High Stability: Synthesis and Characteristic Electronic Properties of Mono- and Di-Nuclear Tricarbonyl Rhenium Tetraazaporphyrin Complexes.

Mono- and di-nuclear tricarbonyl Re(I) tetraazaporphyrin complexes (Re TAP and Re TAP) are investigated and compared with Re(I) phthalocyanine complexes (Re Pc and Re Pc). Although Re Pc is unstable in polar solvents, and easily undergoes demetallation reaction, the coordination of the TAP ligand significantly improves the tolerance toward polar solvents, affording more stability to Re TAP. Additionally, the incorporation of [Re(CO) ] unit(s) and the TAP ligand results in remarkable positive shifts in both oxidation and reduction potentials.

Morphological Manipulation of DNA Gel Microbeads with Biomolecular Stimuli.

Hydrogels are essential in many fields ranging from tissue engineering and drug delivery to food sciences or cosmetics. Hydrogels that respond to specific biomolecular stimuli such as DNA, mRNA, miRNA and small molecules are highly desirable from the perspective of medical applications, however interfacing classical hydrogels with nucleic acids is still challenging. Here were demonstrate the generation of microbeads of DNA hydrogels with droplet microfluidic, and their morphological actuation with DNA strands.

Blackening of titanium dioxide nanoparticles by atomic hydrogen and the effect of coexistence of water on the blackening.

A fast blackening process of titanium dioxide nanoparticles by exposing to atomic hydrogen was studied by estimating the color of the nanoparticles. The whiteness of TiO decreased exponentially with time, which suggests a first-order reaction between atomic H and surface oxygen, whose rate constant is proportional to the ambient pressure of H. The rate constant increases as the temperature of nanoparticles at exposing to atomic hydrogen.

Interaction analyses of SARS-CoV-2 spike protein based on fragment molecular orbital calculations.

At the stage of SARS-CoV-2 infection in human cells, the spike protein consisting of three chains, A, B, and C, with a total of 3300 residues plays a key role, and thus its structural properties and the binding nature of receptor proteins to host human cells or neutralizing antibodies has attracted considerable interest. Here, we report on interaction analyses of the spike protein in both closed (PDB-ID: 6VXX) and open (6VYB) structures, based on large-scale fragment molecular orbital (FMO) calculations at the level of up to the fourth-order Møller-Plesset perturbation with singles, doubles, and quadruples (MP4(SDQ)). Inter-chain interaction energies were evaluated for both structures, and a mutual comparison indicated considerable losses of stabilization energies in the open structure, especially in the receptor binding domain (RBD) of chain-B.

Extended gate-type organic transistor functionalized by molecularly imprinted polymer for taurine detection.

Molecularly imprinted polymers (MIPs) are a fascinating technology for the sensitive and selective detection of target molecules. However, in most situations, the need for complicated and expensive analytical devices for reading the responses of MIPs greatly limits their applications. For exploring low-cost and easy-to-use applications of MIPs, herein we have developed a MIP-modified extended-gate type organic field-effect transistor (MIP-OFET).

Plasmonic linear nanomotor using lateral optical forces.

Optical force is a powerful tool to actuate micromachines. Conventional approaches often require focusing and steering an incident laser beam, resulting in a bottleneck for the integration of the optically actuated machines. Here, we propose a linear nanomotor based on a plasmonic particle that generates, even when illuminated with a plane wave, a lateral optical force due to its directional side scattering.

Monitoring intracellular metal ion complexation with an acetylene-tagged ligand by Raman spectroscopy.

We propose to monitor molecular vibrations to identify metal ion-ligand complexation by means of Raman spectroscopy, which has been applied to track vibrational modes of molecules and to obtain a structural fingerprint. We prepared ligand molecules for Zn ion complexation with a dipycolylaminoethyl aniline (DPEA) skeleton and phenylacetylene unit as the Raman tag which showed a typical band around 2200 cm. Among the labeled ligands synthesized in this study, A-DPEA showed a strong band attributed to the acetylene unit at 2212 cm, while the addition of Zn ion resulted in a band shift to 2220 cm due to complex formation.

Controlling the oxidation state of molybdenum oxide nanoparticles prepared by ionic liquid/metal sputtering to enhance plasmon-induced charge separation.

Nanoparticles composed of molybdenum oxide, MoO , were successfully prepared by room-temperature ionic liquid (RTIL)/metal sputtering followed by heat treatment. Hydroxyl groups in RTIL molecules retarded the coalescence between MoO NPs during heat treatment at 473 K in air, while the oxidation state of Mo species in MoO nanoparticles (NPs) could be modified by changing the heat treatment time. An LSPR peak was observed at 840 nm in the near-IR region for MoO NPs of 55 nm or larger in size that were annealed in a hydroxyl-functionalized RTIL.

Protein Assays on Organic Electronics: Rational Device and Material Designs for Organic Transistor-Based Sensors.

Artificial receptor-based protein assays have various attractive features such as a long-term stability, a low-cost production process, and the ease of tuning the target specificity. However, such protein sensors are still immature compared with conventional immunoassays. To enhance the application potential of synthetic sensing materials, organic field-effect transistors (OFETs) are some of the suitable platforms for protein assays because of their solution processability, durability, and compact integration.

Atomic-scale investigation of the heterogeneous structure and ionic distribution in an ionic liquid using scanning transmission electron microscopy.

Ionic liquids show characteristic properties derived from them being composed of only molecular ions, and have recently been used as solvents for chemical reactions and as electrolytes for electrochemical devices. The liquid structures, , ionic distributions, form when solutes are dissolved in ionic liquids and fundamentally affect the reactions and transfer efficiency in such solutions. In this study, we directly observe the liquid structure in a solution of the long-chain ionic liquid 1-octyl-3-methylimidazolium bromide (Cmim Br) and barium stearate (Ba(CHCOO)) using the annular dark-field method of scanning transmission electron microscopy (ADF-STEM).

Author Correction: Thermal transport crossover from crystalline to partial-crystalline partial-liquid state.

The original version of this Article incorrectly omitted an affiliation of Sebastian Volz: 'LIMMS/CNRS-IIS(UMI2820) Institute of Industrial Science, University of Tokyo 4-6-1 Komaba, Meguro-ku Tokyo 153-8505 JAPAN'. This has now been corrected in both the PDF and HTML versions of the Article.

Thermal transport crossover from crystalline to partial-crystalline partial-liquid state.

Phase-change materials (crystalline at low temperatures and partial-crystalline partial-liquid state at high temperatures) are widely used as thermoelectric converters and battery electrodes. Here, we report the underlying mechanisms driving the thermal transport of the liquid component, and the thermal conductivity contributions from phonons, vibrations with extremely short mean free path, liquid and lattice-liquid interactions in phase-changed LiS. In the crystalline state (T ≤ 1000 K), the temperature dependent thermal conductivity manifests two different behaviors, i.