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A first-passage problem for a cumulative process is investigated. The cumulative process is assumed to be generated by a Poisson process, and the amplitude generated by an event is assumed to decay exponentially. An integral equation for the probability density of the first-passage time until the total amplitude exceeds a pre-specified threshold level is derived. The Laplace transform of the probability density of the first-passage time is obtained explicity when each amplitude generated by an event is distributed exponentially. The mean first-passage times are given in a closed form and plotted versus the threshold level. 相似文献
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Numata M Tamesue S Fujisawa T Haraguchi S Hasegawa T Bae AH Li C Sakurai K Shinkai S 《Organic letters》2006,8(24):5533-5536
We have demonstrated that one-dimensional supramolecular dye assemblies with a uniform diameter can be created by utilizing schizophyllan (SPG) as a one-dimensional host. In the supramolecular nanofibers, the dye molecules are assembled into the different aggregation modes depending on the preparation procedures. The findings establish that SPG is useful for creating the supramolecular nanofibers, where temporal superstructures can be stabilized by the SPG-specific helical higher-order structure. [structure: see text]. 相似文献
37.
Novel alpha-beta chimeric oligonucleotides bearing a propionic acid derivative of an anthraquinone-polyamine conjugate in the "linker" region sequence-specifically formed a substantially stable alternate-stranded triplex with dsDNA almost regardless of the stereochemistry of the derivative. 相似文献
38.
Masaya Kobayashi Takeo Tomita Kazuo Shin‐ya Makoto Nishiyama Tomohisa Kuzuyama 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(38):13483-13487
Carquinostatin A (CQS), a potent neuroprotective substance, is a unique carbazole alkaloid with both an ortho‐quinone function and an isoprenoid moiety. We identified the entire gene cluster responsible for CQS biosynthesis in Streptomyces exfoliatus through heterologous production of CQS and gene deletion. Biochemical characterization of seven CQS biosynthetic gene products (CqsB1–7) established the total biosynthetic pathway of CQS. Reconstitution of CqsB1 and CqsB2 showed that the synthesis of the carbazole skeleton involves CqsB1‐catalyzed decarboxylative condensation of an α‐hydroxyl‐β‐keto acid intermediate with 3‐hydroxybutyryl‐ACP followed by CqsB2‐catalyzed oxidative cyclization. Based on crystal structures and mutagenesis‐based biochemical assays, a detailed mechanism for the unique deprotonation‐initiated cyclization catalyzed by CqsB2 is proposed. Finally, analysis of the substrate specificity of the biosynthetic enzymes led to the production of novel carbazoles. 相似文献
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Keiichi Murai Lukas Lauterbach Kazuya Teramoto Zhiyang Quan Lena Barra Tsuyoshi Yamamoto Kenichi Nonaka Kazuro Shiomi Makoto Nishiyama Tomohisa Kuzuyama Jeroen S. Dickschat 《Angewandte Chemie (International ed. in English)》2019,58(42):15046-15050
The skeletons of some classes of terpenoids are unusual in that they contain a larger number of Me groups (or their biosynthetic equivalents such as olefinic methylene groups, hydroxymethyl groups, aldehydes, or carboxylic acids and their derivatives) than provided by their oligoprenyl diphosphate precursor. This is sometimes the result of an oxidative ring‐opening reaction at a terpene‐cyclase‐derived molecule containing the regular number of Me group equivalents, as observed for picrotoxan sesquiterpenes. In this study a sesquiterpene cyclase from Trichoderma spp. is described that can convert farnesyl diphosphate (FPP) directly via a remarkable skeletal rearrangement into trichobrasilenol, a new brasilane sesquiterpene with one additional Me group equivalent compared to FPP. A mechanistic hypothesis for the formation of the brasilane skeleton is supported by extensive isotopic labelling studies. 相似文献
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Ami Saito Dr. Tomohisa Sawada Prof. Dr. Makoto Fujita 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(46):20547-20550
Porous metal complexes enable single-crystal X-ray crystallographic observation of included guests or reaction intermediates through simple soaking with the guests/substrates. Previous studies on this technique have often encountered difficulties in the observation of chiral structures because the host frameworks had no chirality. We synthesized a new metal–peptide porous complex through a folding-and-assembly strategy and utilized the chiral pore for trapping chiral guests. Chiral alcohols and ketones were successfully included within the pore. Crystallographic analyses clearly revealed not only their chemical structures but also chiral transformation events within the pore such as fixed conformations or an unstable hemiacetal formation. 相似文献