In frustrated magnetic systems, long-range ordering is forbidden and degeneracy of energy states persists, even at extremely low temperatures. Under certain conditions, these systems form an exotic quantum spin-liquid ground state, in which strongly correlated spins fluctuate in the spin lattices. Here we investigate the thermodynamic properties of an anion radical spin liquid of EtMe3Sb[Pd(dmit)2]2, where dmit represents 1,3-dithiole-2-thione-4,5-dithiolate. This compound is an organic dimer-based Mott insulator with a two-dimensional triangular lattice structure. We present distinct evidence for the formation of a gapless spin liquid by examining the T-linear heat capacity coefficient, γ , in the low-temperature heat capacity. Using comparative analyses with κ-(BEDT-TTF)2Cu2(CN)3, a generalized picture of the new spin liquid in dimer-based organic systems is discussed. We also report anomalous enhancement of γ, produced by a kind of criticality inherent to the Pd(dmit)2 phase diagram.
We developed a new method for Pd(II)-catalyzed direct aromatic carbonylation in a phosphine-free catalytic system using Pd(OAc)2 and Cu(OAc)2 in an atmosphere of CO gas containing air. The carbonylation proceeded with ortho-palladation, inducing a remarkable site selectivity to afford a variety of five- or six-membered benzolactams from secondary omega-arylalkylamines, such as N-alkylbenzylamines or N-alkylphenethylamines.
This report summarizes the results of international parallel test on the measurement of the elastic shear modulus at very small strains, Gmax, using bender elements which was carried out from 2003 to 2005 by technical committee, TC29 (Stress-strain and Strength Testing of Geomaterials) of the International Society of Soil Mechanics and Geotechnical Engineering. The purpose was to evaluate the consistency of the bender element test results obtained by applying the exactly similar test material as well as the test method besides identifying the various existing hardware and software being used in this test. It was decided that the domestic TC29 group of Japanese Geotechnical Society (TC29-JGS) was expected to lead this international co-operation. By 2005, reports of the test results were obtained from 23 institutions from 11 countries. This report has been prepared by TC29-JGS taking a leading role from the beginning. A standard test method is proposed here in order to obtain more accurate data from the bender element test by examining various test methods adopted at diŠerent institutions worldwide and the eŠects of various factors on the test results.
[1] We report the field observation of hydrate deposits of different crystal structures in the same cores of a mud volcano in the Kukuy Canyon. We link those deposits to chemical fractionation during gas hydrate crystallization. Gas composition and crystallographic analyses of hydrate samples reveal involvement of two distinct gas source types in gas hydrate formation at present or in the past: microbial (methane) and thermogenic (methane and ethane) gas types. The clathrate structure II, observed for the first time in fresh water sediments, is believed to be formed by higher mixing of thermogenic gas. Citation: Kida, M., et al. (2006), Coexistence of structure I and II gas hydrates in Lake Baikal suggesting gas sources from microbial and thermogenic origin,
A phosphine-free catalytic system [Pd(OAc)2-Cu(OAc)2-air] induced a substrate-specific carbonylation of amines in boiling toluene under CO gas (1 atm). Symmetrical N,N'-dialkylureas were obtained by the carbonylation of primary amines. N,N,N'-Trialkylureas were selectively formed by addition of a secondary amine to the above reaction vessel. Secondary amines did not give tetraalkylureas. However, dialkylamines with a phenyl group on their alkyl chains, such as N-monoalkylated benzylic amine or phenethylamine derivatives, underwent a direct aromatic carbonylation to afford five- or six-membered benzolactams. In the carbonylation, the chelation effect or steric repulsion between Pd(II) and the meta-substituent in the ortho-palladation and the ring sizes of cyclopalladation products that were formed prior to carbonylation were found to generate good site selectivity and increase the reaction rate. In contrast, carbonylation of omega-arylalkylamines with a hydroxyl group gave neither ureas nor benzolactams but instead produced 1,3-oxazolidinones smoothly. Hydrochlorides of amines also underwent carbonylation to afford the corresponding amides under the conditions used. This procedure made it possible to prepare ureas of amino acid esters and N-alkylcarbamates in practical yields.
Magnetic dipole interactions are dominate in quasi one-dimensional (1D) molecular magnetic materials, in which TbNcPc units (Tb =terbium(III) ion, Nc =naphthalocyaninato, Pc =phthalocyaninato) adopt a structure similar to TbPc single-molecule magnets (SMMs). The magnetic properties of the [TbNcPc] (neutral 1 and cationic 2) with 1D structures are significantly different from those of a magnetically diluted sample (3). In particular, the magnetic relaxation time (τ) of 2 in the low-temperature region is five orders of magnitude slower than that of 3. Furthermore, the coercivity (H ) of 2 remained up to about 20 K. The single-ion anisotropy of Tb ions in a 1D structure and the magnetic dipole interactions acting among molecules determines the direction of the magnetic properties. These results show that the spin dynamics can be improved by manipulating the arrangement of SMMs in the solid state.
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