Shinjulactone C,a new quassinoid ith a 1α, 12α:5α, 13α-dicyclo-9βH-picrasane skeleton from ailanthus altissima SWINGLE

A new non-bitter quassinoid, named shinjulactone C ($\text{1}$), was isolated from the root bark of $\text{Ailanthus altissima}$ SWINGLE and shown to be 1α, 12α:5α, 13α-dicyclo-1β, 12β, 20-trihydroxy-9β$\text{H}$-picras-3-ene-2, 11, 16-trione by X-ray diffraction method.     

Boundary trace of reflecting Brownian motions

We establish a uniform dimensional result for normally reflected Brownian motion (RBM) in a large class of non-smooth domains. Hausdorff dimensions for the boundary occupation time and the boundary trace of RBM are determined. Extensions to stable-like jump processes and to symmetric reflecting diffusions are also given.Mathematics Subject Classification (2000):Primary 60G17, 60J60, Secondary 28A80, 30C35, 60G52, 60J50     

The influence of ligand side chain on the enantioselectivity of Lewis acid catalyzed Diels-Alder reactions

The enantioselective Lewis acid-catalyzed Diels-Alder reaction of 3-(2-propenoyl)-1,3-oxazolidin-2-one 8 with cyclopentadiene was examined using a series of chiral mox ligands 2-6, deferring in the side chain at 2-position of the chiral oxazoline and in the nature of the substituent at the chiral center (4-position) of the oxazoline ring, and a combination of N-[(1R)-2-chloro-1-phenylethyl]-2-[(4R)-4-phenyl-4,5-dihydrooxazol-2-yl]butyramide 2-MgI(2)-I(2) was the most efficient catalyst.     

Peliosis hepatis and neoplastic/dysplastic lesions in aged male Long-Evans Cinnamon rats: MR imaging with pathologic correlation

The Long-Evans Cinnamon (LEC) rat, an animal model of Wilson's disease, abnormally accumulates copper in the liver. There have been a lot of reports on preneoplastic and neoplastic hepatic tumors in LEC rats, but few studies have been focused on other lesions. The aim of this study was to describe the MR findings of the liver of LEC rats with pathologic correlation to characterize the hepatic lesions developed in them. We measured MR images of the liver of six aged (over the age of 70 weeks old) male LEC rats. Measurements of T(1), T(2)-weighted images, and the dynamic and delayed studies after i.v. gadolinium injection were performed. The rats were sacrificed immediately after the measurements, and the diagnosis was histologically made. We identified seven lesions of peliosis hepatis, three neoplastic/dysplastic lesions, three cysts and one cholangiofibrosis. Peliosis hepatis was characterized as showing a significantly long T(2) relaxation time of 57.9 +/- 13.3 ms (mean +/- standard deviation) compared with 41.3 +/- 1.7 ms in normal liver, and prolonged enhancement after a gadolinium injection. Neoplastic/dysplastic lesions tended to show prolonged T(2), and they showed isointensity on T(1)-weighted images. They were best characterized by early enhancement followed by a rapid wash-out after a gadolinium injection. In conclusions, the frequent occurrence of peliosis hepatis observed in the present study suggests this can be a characteristic lesion in aged LEC rats. The characteristic MR findings enable us to distinguish between peliosis hepatis and neoplastic/dysplastic lesions.     

Upper bounds on the height difference of the Gaussian random field and the range of random graph homomorphisms into ℤ

Bounds on the range of random graph homomorphism into ℤ, and the maximal height difference of the Gaussian random field, are presented. © 2000 John Wiley & Sons, Inc. Random Struct. Alg., 17: 20–25, 2000     

Chemical-to-mechanical energy conversion in biomacromolecular machines: a plasmon and optimum control theory for directional work. 1. General considerations

To rationalize coherence and mechanochemical aspects of proteins acting as molecular machines, a plasmon concept for dealing with protein nonequilibrium dynamics is introduced and tested with respect to thermodynamic consistency. A stochastic optimum-control theory for protein conformational diffusion is developed and the corresponding stochastic Newton's second law derived for optimum-controlled conformational diffusion in proteins. The plasmon concept is shown to be consistent with this theory, in that optical plasmons can pump entropy out of (or into) the protein, decreasing (or increasing) its conformational diffusion and, at the same time, help decrease intra- and intermolecular friction, as well as (potentially) break the symmetry of the latter. Instead, acoustic plasmons may break the spatial symmetry of a protein's "potential of mean force", thus converting it into an effective Brownian ratchet potential by applying quasistatic deformational corrections to the former. These concepts seem to be of rather general applicability and might also be useful when studying, for example, intercalation of cationic dyes into DNA duplexes, positively charged oligopeptide transduction through cell membranes, or even DNA translocation through nanopores.     

Charge-transfer biexciton annihilation in a donor–acceptor co-crystal yields high-energy long-lived charge carriers

Organic donor–acceptor (D–A) co-crystals have attracted much interest due to their important optical and electronic properties. Co-crystals having ⋯DADA⋯ π-stacked morphologies are especially interesting because photoexcitation produces a charge-transfer (CT) exciton, D˙⁺–A˙⁻, between adjacent D–A molecules. Although several studies have reported on the steady-state optical properties of this type of CT exciton, very few have measured the dynamics of its formation and decay in a single D–A co-crystal. We have co-crystallized a peri-xanthenoxanthene (PXX) donor with a N,N-bis(3-pentyl)-2,5,8,11-tetraphenylperylene-3,4:9,10-bis(dicarboximide) (Ph4PDI) acceptor to give an orthorhombic PXX–Ph4PDI ⋯DADA⋯ π-stacked co-crystal with a CT transition dipole moment that is perpendicular to the transition moments for S_n ← S₀ excitation of PXX and Ph4PDI. Using polarized, broadband, femtosecond pump–probe microscopy, we have determined that selective photoexcitation of Ph4PDI in the single co-crystal results in CT exciton formation within the 300 fs instrument response time. At early times (0.3 ≤ t ≤ 500 ps), the CT excitons decay with a t^−1/2 dependence, which is attributed to CT biexciton annihilation within the one-dimensional ⋯DADA⋯ π-stacks producing high-energy, long-lived (>8 ns) electron–hole pairs in the crystal. These energetic charge carriers may prove useful in applications ranging from photovoltaics and opto-electronics to photocatalysis.

Femtosecond transient absorption microscopy of donor–acceptor single co-crystals shows that photogenerated charge transfer excitons in one-dimensional donor–acceptor π stacks annihilate to produce high-energy, long-lived electrons and holes.     

Conceptual thinking and metrology concepts

In introducing the term ‘concept’, the authors of the 2008 International vocabulary of metrology ‘Basic and general concepts and associated terms’ (VIM, 2008) recognize that in order to operationalize a globally accepted set of metrology terms, one requires to deal with a higher level of abstraction. Concepts are obviously not specific to metrology–handling complex tasks in any domain of knowledge that requires conceptual thinking abilities. In this short white paper, we discuss how to assess and develop conceptual thinking of professionals in service, business, and industrial environments. The approach builds on a proven methodology called MERLO that has been developed in the last 15 years by experts in psychology and education with adaptation to new interactive technologies such as clickers and internet-based formative assessments. MERLO pedagogy can be used to assess individuals’ inherent conceptual thinking abilities and train them to enhance their competence in analyzing complex conceptual situations. This is pertinent to the education of metrology, quality, and statistical thinking. We suggest that MERLO can be considered as a complementary enabler to VIM, so that this fundamental work can enhance its impact and applicability.     

NO(2) dissociation on Ag(111) revisited by theory

NO(2) dissociation on Ag(111) is investigated with first-principles calculations. For single NO(2) molecules, a high adsorption potential energy is found to prohibit dissociation. This result is surprising as experiments indicate dissociation at low temperatures. Neither entropy effects nor irregularities in the potential energy surface can remedy the discrepancy. Instead it is proposed that collective Eley-Rideal type of reaction mechanisms can drive the dissociation.