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A short and convenient synthesis of metallochlorin-C-60 dyads based on a Heck-type hetero coupling at the 3(2) position of a chlorin is described. p-Bromobenzaldehyde was treated with Zn-metalated 13(2)- demethoxycarbonylmethylpheophorbide a, using a palladium acetate/LiCl catalyst mixture under phase-transfer conditions in DMF at 70 degrees C. The resulting asymmetric olefin was obtained in a high trans/cis ratio. The desired trans isomer was separated and subsequently transformed into a donor-acceptor dyad by a 1,3-dipolar cycloaddition to C-60 in the presence of sarcosine in refluxing toluene. The resulting dyads are expected to undergo efficient photoinduced electron transfer and can potentially be utilized in solar energy conversion devices.
A 741-cm-long laminated sediment core, covering the last 10,800 years was collected from Lake Zigetang, central Tibetan Plateau (90.9 degrees E, 32.0 degrees N, 4560m a.s.l.), and analysed palynologically at 69 horizons. Biome reconstruction suggests a dominance of temperate steppe vegetation (mainly Artemisia and Poaceae) on the central Tibetan Plateau during the first half of the Holocene (10.8-4.4 cal. ka BP), while alpine steppes with desert elements (mainly Cyperaceae, Poaceae, Chenopodiaceae, and characteristic high-alpine herb families) tend to dominate the second half (4.4-0 cal. ka BP). The Artemisia/Cyperaceae ratio-a semi-quantitative measure for summer temperature-indicates a general cooling trend throughout the Holocene. Dense temperate steppe vegetation and maximum desert plant withdrawal, however, indicate that a suitable balance of wet and warm conditions for optimum vegetation growth likely occurred during the middle Holocene (7.3-4.4 cal. ka BP). Severe Early Holocene cold events have been reconstructed for 8.7-8.3 and similar to 7.4 cal. ka BP. (c) 2006 Elsevier Ltd and INQUA. All rights reserved.
A mathematical model of working-memory capacity limits is proposed on the key assumption of mutual interference between items in working memory. Interference is assumed to arise from overwriting of features shared by these items. The model was fit to time-accuracy data of memory-updating tasks from four experiments using nonlinear mixed effect (NLME) models as a framework. The model gave a good account of the data from a numerical and a spatial task version. The performance pattern in a combination of numerical and spatial updating could be explained by variations in the interference parameter: assuming less feature overlap between contents from different domains than between contents from the same domain, the model can account for double dissociations of content domains in dual-task experiments. Experiment 3 extended this idea to similarity within the verbal domain. The decline of memory accuracy with increasing memory load was steeper with phonologically similar than with dissimilar material, although processing speed was faster for the similar material. The model captured the similarity effects with a higher estimated interference parameter for the similar than for the dissimilar condition. The results are difficult to explain with alternative models, in particular models incorporating time-based decay and models assuming limited resource pools.
The paper presents a novel approach to explaining word order variation in the early Germanic languages. Initial observations about verb placement as a device marking types of rhetorical relations made on data from Old High German (cf. Hinterhölzl & Petrova 2005) are now reconsidered on a larger scale and compared with evidence from other early Germanic languages. The paper claims that the identification of information-structural domains in a sentence is best achieved by taking into account the interaction between the pragmatic features of discourse referents and properties of discourse organization.
A successful assignment for the fundamental bands observed in the experimental IR spectra of mn-12S(2)O(2) and fn-12S(2)O(2) dithiacrown ethers was achieved by the aid of the density functional theory (DFT) based quantum mechanical calculations carried out at the 133LYP/6-31G(d) and B3LYP/6-31 + G(d) level of theory. Two different scaling approaches, '(i) scaled quantum mechanics force field (SQM FF) methodology', and (ii) the 'scaling frequencies with dual empirical scale factors', were used in order to fit the calculated harmonic frequencies to the experimental ones. Potential energy distribution (PED) calculations were carried out to define the internal coordinate contributions to each normal mode and to define the corresponding normal modes of the molecules. The effects of the conformational differences onto the IR active normal modes of the two isomeric molecules and their corresponding experimental frequencies were discussed in the light of the calculated spectral data.
Objective Pre-eclampsia is a serious complication of pregnancy with high morbidity and mortality and an incidence of 3-5% in all pregnancies. Early prediction is still insufficient in clinical practice. Although most pre- eclamptic patients have pathological uterine perfusion in the second trimester, perfusion disturbance has a positive predictive accuracy (PPA) only of approximately 30%. Methods Non-invasive continuous blood pressure recordings were taken simultaneously via a finger cuff for 30 min. Time series of systolic as well as diastolic beat-to-beat pressure values were extracted to analyse heart rate and blood pressure variability and baroreflex sensitivity in 102 second- trimester pregnancies, to assess predictability for pre-eclampsia (n = 16). All women underwent Doppler investigations of the uterine arteries. Results We identified a combination of three variability and baroreflex parameters to best predict pre-eclampsia several weeks before clinical manifestation. The discriminant function of these three parameters classified patients with later pre-eclampsia with a sensitivity of 87.5%, a specificity of 83.7%, and a PPA of 50.0%. Combined with Doppler investigations of uterine arteries, PPA increased to 71.4%. Conclusions This technique of incorporating one-stop clinical assessment of uterine perfusion and variability parameters in the second trimester produces the most effective prediction of pre-eclampsia to date
Binding or catalysis? Both can be distinguished with a molecularly imprinted polymer (MIP) by the different patterns of heat generation. The catalytically active sites, like in the corresponding enzyme, generate a steady-state temperature increase. Thus, enzyme-like catalysis and antibody-analogue binding are analyzed simultaneously in a bifunctional MIP for the first time (see scheme).
(Near-)inverses of sequences
(2006)
We introduce the notion of a near-inverse of a non-decreasing sequence of positive integers; near-inverses are intended to assume the role of inverses in cases when the latter cannot exist. We prove that the near-inverse of such a sequence is unique; moreover, the relation of being near-inverses of each other is symmetric, i.e. if sequence g is the near-inverse of sequence f, then f is the near-inverse of g. There is a connection, by approximations, between near- inverses of sequences and inverses of continuous strictly increasing real-valued functions which can be exploited to derive simple expressions for near-inverses