Tensor-Optimized Few-Body Model for s-Shell Nuclei

We propose a tensor-optimized few-body model (TOFM) in the few-body framework with bare nucleon–nucleon interaction. The physical concept of TOFM comes from the tensor-optimized shell-model (TOSM), which is applicable for the study of medium and heavy nuclei. The TOSM wave function describes the deuteron-like tensor correlation and provides a good reproduction of the binding energy with the bare nucleon–nucleon interaction. Using the spirit of the TOSM approximation, we show the performance of TOFM for s-shell nuclei. It is found that the TOFM can account for the contribution of the tensor interaction very well and almost reproduces the total energy and various energy components as compared with rigorous few-body calculations. The relative correlation function is also provided to improve the performance of TOSM for the study of heavy nuclei.     

Facile Synthesis of Azahelicenes and Diaza[8]circulenes through the Intramolecular Scholl Reaction

Carbazole-based aza[7]helicenes and hetero[9]helicenes were successfully obtained via the intramolecular Scholl reaction of 3,6-bis(biphenyl-2-yl)carbazole congeners, while the reaction of 3,6-bis(naphthylphenyl)-appended carbazole gave a triple helicene via an unexpected simultaneous double aryl rearrangement. DFT calculations suggested that the rearrangement proceeded via an arenium cation intermediate. In addition, the reaction of methoxy-appended substrate gave an azahepta[8]circulene via the concurrent C−C bond formation. These helical dyes showed circularly polarized luminescence. The azahepta[8]circulene was further transformed into deeply saddle-distorted dibenzodiaza[8]circulenes as the first example of its solution-based synthesis and unambiguous structural determination.     

Production of a NiO/Al primary battery employing powder-based electrodes

This paper describes the use of aluminum and zinc as anodic materials for a battery employing nickel (II) oxide (NiO) as cathode. Comparison of both materials resulted in the development of a compact, cost effective, and easy to use primary NiO/Al battery employing an alkaline electrolyte. The system features electrodes composed of powder forms of the active materials on modified paper substrates that are contained in a simple multilayer design utilizing thin laminated plastic materials to provide structure and flexibility to the battery as well as a paper separator. Various concentrations of potassium hydroxide (KOH) electrolyte were examined and maximum performance was observed at 6 M KOH. A maximum current density and power density of 1.94 mA/cm² and 1 mW/cm², respectively was achieved. This user-friendly device was able to produce a maximum capacity of 2.33 mAh/g when 2 mA/g was applied. This work demonstrates the viability of a paper-based battery featuring powder electrodes as a possible power source for microelectronic devices.     

Thermally Responsive Poly(ethylene oxide)-Based Polyrotaxanes Bearing Hydrogen-Bonding Pillar[5]arene Rings**

Poly(ethylene oxide)s (PEOs) are useful polymers with good water solubility, biological compatibility, and commercial availability. PEOs with various end groups were threaded into pillar[5]arene rings in a mixture of water and methanol to afford pseudopolyrotaxanes. Corresponding polyrotaxanes were also constructed by capping COOH-terminated pseudopolyrotaxanes with bulky amines, in which multiple hydrogen bonds involving the pillar[5]arene OH groups were critically important to prevent dethreading. The number of threaded ring components could be rationally controlled in these materials, providing a simple and versatile method to tune the mechanical and thermal properties. Specifically, a polyrotaxane with a high-molecular-weight axle became elastic upon heating above the melting point of PEOs and exhibited temperature-dependent shape memory property because of the topological confinement and crosslinked hydrogen bonds.     

Tetramethylammonium hydroxide (TMAH) thermochemolysis of 2-arylcoumaran lignin model compounds

Phenolic 2-arylcoumarans 1–6 were used to examine the behaviors of β-5 subunits in lignin during tetramethylammonium hydroxide (TMAH) thermochemolysis. Products were monitored by gas chromatography/mass spectrometry. The process predominantly provided dimeric products with the opened hydrofuran ring. Substituent changes at the γ-position of ring A and at the 5-position of ring B had a large effect on the product compositions. 2-Arylcoumarans 1 and 6 with the γ-CH₂OH substituent predominantly gave 2,3,3′,4′-tetramethoxystilbenes involving the elimination of the γ-CH₂OH substituent, while 2–5 with the γ-CH₃ substituent gave a mixture of 2,3,3′,4′-tetramethoxy-α-methylstilbenes and α-methoxy-α-(3′,4′-dimethoxyphenyl)-β-(2,3-dimethoxyphenyl)propanes. Substituent –CHCHCH₃ on ring B remained unaffected. Substituents –CHCHCH₂OH and –COOH on ring B produced the corresponding methyl ether and ester, respectively, by methylation. The –CHCHCHO substituent on ring B was converted to the –CHO substituent.     

Data‐Driven Materials Exploration for Li‐Ion Conductive Ceramics by Exhaustive and Informatics‐Aided Computations

Interest in all‐solid‐state Li‐ion batteries (LIBs) using non‐flammable Li‐conducting ceramics as solid electrolytes has increased, as safe and robust batteries are urgently desired as power sources for (hybrid) electric vehicles. However, the low Li‐ion conductivities of ceramics have hindered all‐solid‐state LIB commercialization; many researchers have attempted to develop fast Li‐ion conductors. We introduce two efficient high‐throughput computational approaches for materials exploration: (i) exhaustive search and (ii) informatics‐aided prediction. For demonstration, ～400 Li‐ and Zn‐containing oxide (Li?Zn?X?O) compounds of varied crystal structures are extracted from Materials Project datasets. We calculate the migration energies for Li‐ion conduction and the phase stabilities (decomposition energies) of these materials by simulation and apply Bayesian optimization to determine the material with the highest ionic conductivity. The results show much greater efficiency than a random search algorithm.     

Chiral copper-catalyzed enantioselective Michael difluoromethylation of arylidene meldrum's acids with (difluoromethyl)zinc reagents

The catalytic enantioselective difluoromethylation of arylidene Meldrum's acids with (difluoromethyl)zinc reagent, easily prepared through zinc/iodide exchange reaction of difluoroiodomethane and diethylzinc with co-solvent such as pyridines, by a chiral phosphoramidite-Cu catalyst is shown to provide highly enantioselective sp [3]-difluoromethyl Michael addition product in good yields and high levels of enantioselectivity.     

Charge freezing in the zigzag chain PrBa2Cu4O8 cuprate

We report nuclear quadrupole resonance (NQR) studies on the chain Cu sites of PrBa2Cu4O8, a quasi-one-dimensional conductor with a nearly quarter-filled band. The nuclear spin-lattice relaxation rate 1/T1 shows a pronounced peak near 100 K caused by fluctuations of electric field gradient. Similar peak was observed for the spin-echo decay rate 1/T2, however, at a different temperature near 50 K. These results and broadening of the NQR spectrum at low temperatures indicate that slow charge fluctuations of either electronic or ionic origin freeze gradually at low temperatures.     

Solid-state 13C and 1H spin diffusion NMR analyses of the microfibril structure for bacterial cellulose

To obtain further information about the cause for the rather large splitting of the C4 resonance line into the downfield (C4D) and upfield (C4U) lines in CP/MAS ¹³C NMR spectra for native cellulose, ¹³C and ¹H spin diffusion measurements have been conducted by using different types of bacterial cellulose samples. In ¹³C spin diffusion measurements, the C4D resonance line is selectively inverted by the Dante π pulse sequence and the ¹³C spin diffusion is allowed to proceed from the C4D carbons to other carbons including the C4U carbons with use of the ¹³C4-enriched bacterial cellulose sample. The analysis based on the simple spin diffusion theory for the process experimentally observed reveals that the C4U carbons may be located at distances less than about 1 nm from the C4D carbons. In ¹H spin diffusion measurements, poly(vinyl alcohol) (PVA) films in which ribbon assemblies of bacterial cellulose are dispersed are employed and the ¹H spin diffusion process is examined from the water-swollen PVA continuous phase to the dispersed ribbon assemblies by the ¹³C detection through the ¹H–¹³C CP technique. As a result, it is found that the C4D and C4U carbons are almost equally subjected to the ¹H spin diffusion from the PVA phase, indicating that the C4U carbons are not localized in some limited area, e.g. in the surfacial region, but are distributed in the whole area in the microfibrils. These experimental results suggest that the C4U carbons may exist as structural defects probably due to conformational irregularity associated with disordered hydrogen bonding of the CH₂OH groups in the microfibrils.