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121.
Franklin-Mergarejo R Rubayo-Soneira J Halberstadt N Ayed T Bernal-Uruchurtu MI Hernández-Lamoneda R Janda KC 《The journal of physical chemistry. A》2011,115(23):5983-5991
Valence electronic excitation spectra are calculated for the H(2)O···Br(2) complex using highly correlated ab initio potentials for both the ground and the valence electronic excited states and a 2-D approximation for vibrational motion. Due to the strong interaction between the O-Br and the Br-Br stretching motions, inclusion of these vibrations is the minimum necessary for the spectrum calculation. A basis set calculation is performed to determine the vibrational wave functions for the ground electronic state and a wave packet simulation is conducted for the nuclear dynamics on the excited state surfaces. The effects of both the spin-orbit interaction and temperature on the spectra are explored. The interaction of Br(2) with a single water molecule induces nearly as large a shift in the spectrum as is observed for an aqueous solution. In contrast, complex formation has a remarkably small effect on the T = 0 K width of the valence bands due to the fast dissociation of the dihalogen bond upon excitation. We therefore conclude that the widths of the spectra in aqueous solution are mostly due to inhomogeneous broadening. 相似文献
122.
Dr. Amber Janda Prof. Li-Chiang Lin Prof. Bess Vlaisavljevich Dr. Jeroen Van der Mynsbrugge Prof. Alexis T. Bell 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(29):7225-7226
This is a response to the paper published by S. A. Kadam, H. Li, R. F. Wormsbacher, A. Travert, Chem. Eur. J. 2018 , 24, 5489. Key consistencies between our reported results and those reported in this work are also highlighted. 相似文献
123.
We study positive bilinear forms on a Hilbert space which are not necessarily bounded nor induced by some positive operator. We show when different families of bilinear forms can be described as a generalized effect algebra. In addition, we present families which are or are not monotone downwards (Dedekind upwards) σ-complete generalized effect algebras. 相似文献
124.
Jiří Janda 《Quaestiones Mathematicae》2019,42(3):319-345
Group coextensions of monoids, which generalise Schreier-type extensions of groups, have originally been defined by P.A. Grillet and J. Leech. The present paper deals with pomonoids, that is, monoids that are endowed with a compatible partial order. Following the lines of the unordered case, we define pogroup coextensions of pomonoids. We furthermore generalise the construction to the case that pomonoids instead of pogroups are used as the extending structures.
The intended application lies in fuzzy logic, where triangular norms are those binary operations that are commonly used to interpret the conjunction. We present conditions under which the coextension of a finite totally ordered monoid leads to a triangular norm. Triangular norms of a certain type can therefore be classified on the basis of the presented results. 相似文献
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Antibody 38C2 catalyzed a retro-aldol process upon dendritic modified aliphatic polyesters. This catalytic system was studied in detail and displayed rate enhancements, k(cat)/k(uncat), of greater than 10(6). These antibody-catalyzed reactions took place in a stepwise manner yielding partially modified aldol-dendrimers until a fully substituted aldehyde dendrimer was formed. The catalytic antibody 38C2 only reacted with surface-exposed aldol moieties and did not significantly interact with the core groups for dendrons 4 and 8. For a higher generation dendron 8 the rate of unmasking slightly decreased presumably due to steric crowding of the aldol functionalities. In addition, catalytic antibody 38C2 was able to selectively differentiate block-hybrid dendrons and was regiospecific in the retro-aldol reaction of dendron 21. This is an inaugural report of a catalytic antibody utilizing dendrimers as substrates and suggests that antibodies could be used as selective catalysts for the controlled release and activation of specific molecules attached to biodegradable polymeric materials. Furthermore, this is the first example of catalytic antibody 38C2 displaying regioselectivity on a multifunctional aldol substrate. Important for synthetic applications is the antibody's ability to selectively differentiate regions on dendritic substrates and produce partly aldol functionalized dendrons under conditions mild enough to avoid beta-elimination. 相似文献
128.
Chen DW Beuscher AE Stevens RC Wirsching P Lerner RA Janda KD 《The Journal of organic chemistry》2001,66(5):1725-1732
The synthesis of the first examples of stilbene-tethered hydrophobic C-nucleosides is described. Compounds of this type are targeted for use with our recently reported "blue-fluorescent antibodies" with the aim of probing native and nonnatural DNA. The nucleophilic addition of aryl Grignard reagents to either a protected 2'-deoxy-1'-chloro-ribofuranose or a protected 2'-deoxy-ribonolactone was the key synthetic step and afforded C-nucleosides in good yields. Both routes resulted in a final product that was >/=90% of the beta-anomer. Amide- and ether-based linkers for attachment of trans-stilbene to the nucleobase were assessed for utility during synthesis and in binding of the ligands to a blue-fluorescent monoclonal antibody. X-ray structures of each complex were obtained and serve as a guideline for second-generation stilbene-tethered C-nucleosides. The development of these hydrophobic nucleosides will be useful in current native and nonnatural DNA studies and invaluable for investigations regarding novel, nonnatural genomes in the future. 相似文献
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130.
Dickerson TJ Yamamoto N Ruiz DI Janda KD 《Journal of the American Chemical Society》2004,126(37):11446-11447
The drug of abuse methamphetamine has been found to participate in the aberrant glycation of proteins. The importance of this chemical process has been shown wherein mouse albumin was readily modified with methamphetamine, and injection of this protein into mice yields a significant immune response, even in the absence of adjuvants. Competition experiments revealed that although methamphetamine binds weakly to the elicited antibodies, the primary epitope is composed of both the methamphetamine moiety and glucose-derived cross-linking region. Implications of this phenonomenon in the context of drug addiction are discussed. 相似文献