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301.
Yoshimasa Matsumura Hiroki Nishiyama Shinsuke Inagi Ikuyoshi Tomita 《Journal of polymer science. Part A, Polymer chemistry》2019,57(24):2519-2525
The synthesis and unique optoelectronic features of a π‐conjugated polymer containing both thiophene and 1‐phenylphosphole sulfide units (multiple heteroles) in the main chain by the post‐element transformation of a regioregular organometallic polymer possessing titanacyclopentadiene‐2,5‐diyl unit are described. The π‐conjugated polymer containing multiple heteroles was obtained in 73% yield by the simultaneous reaction of the organotitanium polymer with sulfur monochloride and dichlorophenylphosphine (0.6 equiv each), whose number‐average molecular weight (Mn) and the molecular‐weight distribution (Mw/Mn) were estimated to be 11,000 and 3.4, respectively, by the size exclusion chromatography (SEC). The π‐conjugated polymer thus obtained was found to have the high HOMO and the low LUMO energy levels due to the electron‐rich thiophene and electron‐deficient phosphole sulfide units, respectively, as supported by its cyclic voltammetry (CV) analysis. Compared to a mixture of a polymer containing sole thiophene‐unit and that containing sole phosphole sulfide units, the π‐conjugated polymer‐containing multiple heteroles proved to exhibit interesting optical properties. For example, a specific emission peak was observed at 608 nm in the photoluminescence spectrum, which was not observed in the case of the thiophene‐containing polymer, the phosphole‐containing polymer, and their mixture. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019 , 57, 2519–2525 相似文献
302.
In this work, the EDIP potential is employed for representing silicon and the shuffle-set 60° perfect dislocation motion is investigated by reaction pathway analysis. There are three possible shuffle-set 60° perfect dislocation core structures named as S1, S2 and S3. The activation energy barriers of the kink migration and nucleation in S1and S2 types are calculated by CI-NEB method. The simulation results show that the critical resolved shear strain of the shuffle-set dislocation in S1 type is around 5%, and the S1 type is the dominate one in the shear strain region of 0 to 5%. During the shear strain from 5to 11.81%, the dislocation moves as the S1 core kink nucleation and migration, meanwhile the S1 dislocation core is in process of transforming into S2. More interestingly, both S1 and S2 dislocation core structures is observed along the dislocation line in this shear strain regime, which could response to the missing observation of long segment dislocation line in the experiment. 相似文献
303.
Shinsuke Koyama Uri T. Eden Emery N. Brown Robert E. Kass 《Annals of the Institute of Statistical Mathematics》2010,62(1):37-59
Perception, memory, learning, and decision making are processes carried out in the brain. The performance of such intelligent
tasks is made possible by the communication of neurons through sequences of voltage pulses called spike trains. It is of great
interest to have methods of extracting information from spike trains in order to learn about their relationship to behavior.
In this article, we review a Bayesian approach to this problem based on state-space representations of point processes. We
discuss some of the theory and we describe the way these methods are used in decoding motor cortical activity, in which the
hand motion is reconstructed from neural spike trains. 相似文献
304.
Luca C. Greiner Prof. Dr. Shinsuke Inuki Dr. Norihito Arichi Prof. Dr. Shinya Oishi Rikito Suzuki Dr. Tomohiro Iwai Prof. Dr. Masaya Sawamura Prof. Dr. A. Stephen K. Hashmi Prof. Dr. Hiroaki Ohno 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(51):12992-12997
Because benzannulated and indole-fused medium-sized rings are found in many bioactive compounds, combining these fragments might lead to unexplored areas of biologically relevant and uncovered chemical space. Herein is shown that α-imino gold carbene chemistry can play an important role in solving the difficulty in the formation of medium-sized rings. Namely, phenylene-tethered azido-alkynes undergo arylative cyclization through the formation of a gold carbene intermediate to afford benzannulated indole-fused medium-sized tetracycles. The reactions allow a range of different aryl substitution patterns and efficient access to these otherwise difficult-to-obtain medium-sized rings. This study also demonstrates the feasibility of the semihollow-shaped C-dtbm ligand for the construction of a nine-membered ring. 相似文献
305.
Synthesis of polymers possessing tetraphenylethylene units by three‐component coupling reactions of poly(p‐phenylene ethynylene) derivative with aryl halides and phenylboronic acid 下载免费PDF全文
Takeru Suto Hiroki Nishiyama Shinsuke Inagi Ikuyoshi Tomita 《Journal of polymer science. Part A, Polymer chemistry》2015,53(6):787-791
A derivative of poly(p‐phenylene ethynylene) was subjected to the palladium‐catalyzed three‐component coupling reactions with aryl halides and phenylboronic acid to obtain polymers having tetrasubstituted cis‐vinylene units. For example, 69% of the acetylene units in the prepolymer were converted to cis‐vinylene (i.e., tetrasubstituted cis‐vinylene) units using iodobenzene and phenylboronic acid (5 equiv each with respect to acetylene units). In the UV–vis absorption spectra of the resulting polymers, clear hypsochromic shifts of the absorption maxima were observed, while bathochromic shifts and suppression of the efficiency were observed in their photoluminescence spectra. © 2015 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2015 , 53, 787–791 相似文献
306.
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308.
Shinsuke Mizumoto Siqi Xi Yusuke Fujiwara Shigehiro A. Kawashima Kenzo Yamatsugu Motomu Kanai 《化学:亚洲杂志》2020,15(6):833-839
Lysine acylation of proteins is an essential chemical reaction for posttranslational modification and as a means of protein modification in various applications. N,N‐Dimethyl‐4‐aminopyridine (DMAP) derivatives are widely‐used catalysts for lysine acylation of proteins; however, the DMAP moiety mostly exists in a protonated, and thus deactivated, form under physiological conditions due to its basicity. An alternative catalytic motif furnishing higher acylation activity would further broaden the possible applications of chemical lysine acylation. We herein report that the hydroxamic acid‐piperidine conjugate Ph‐HXA is a more active catalytic motif for lysine acetylation than DMAP under physiological conditions. In contrast to DMAP, the hydroxamic acid moiety is mostly deprotonated under aqueous neutral pH, resulting in a higher concentration of the activated form. The Ph‐HXA catalyst is also more tolerant of deactivation by a high concentration of glutathione than DMAP. Therefore, Ph‐HXA might be a suitable catalytic motif for target protein‐selective and site‐selective acetylation in cells. 相似文献
309.
Shunpei Suzuki Daichi Tatsumi Takamasa Tsukamoto Ryou Honna Tetsuya Shimada Haruo Inoue Shinsuke Takagi 《Tetrahedron letters》2018,59(6):528-531
A novel light harvesting system that captures long-wavelength light of sunlight by the use of hole transfer was newly investigated. Ga phthalocyanine(GaIIITMAPc4+(D)) and Ru porphyrin(RuIIDMPyMP2+(A)) co-adsorbed reaction system on the synthetic nanosheet was examined as an artificial light harvesting system. By irradiating 660?nm light, where GaIIITMAPc4+(D) absorbs, to the system under a presence of PtCl62? as an electron acceptor, cation radical of RuIIDMPyMP2+(A) was produced despite that Ru porphyrin adsorbs only 413 and 533?nm light. The efficient hole transfer reaction from GaIIITMAPc4+(D)+, that is generated from its excited state, to RuIIDMPyMP2+(A) takes place on the nanosheet. 相似文献
310.
Anti-Stokes Raman scattering is used to monitor vibrational energy redistribution in the ambient temperature liquids nitromethane (NM-h3) and perdeuterated nitromethane (NM-d3) after ultrafast IR excitation of either the symmetric or asymmetric CH- or CD-stretch transitions. The instantaneous populations of most of the fifteen NM vibrations are determined with good accuracy, and a global fitting procedure with a master equation is used to fit all the data. The pump pulses excite not only CH- or CD-stretches but also certain combinations of bending and nitro stretching fundamentals. The coupled vibrations that comprise the initial state are revealed via the instantaneous rise of the anti-Stokes transients associated with each vibrational fundamental. In contrast to many other polyatomic liquids studied previously, there is little energy exchange among the CH-stretch (or CD-stretch) excitations, which is attributed to the nearly free rotation of the methyl group in NM. The vibrational cooling process, which is the multistep return to a thermalized state, occurs in three stages in both NM-h3 and NM-d3. In the first stage, the parent CH- or CD-stretch decays in a few picoseconds, exciting all lower-energy vibrations. In the second stage, the midrange vibrations decay in 10-15 ps, exciting the lower-energy vibrations. In the third stage, these lower-energy vibrations decay into the bath in tens of picoseconds. The initial excitations are thermalized in approximately 150 ps in NM-h3 and there is little dependence on which CH-stretch is excited. VC is somewhat faster in NM-d3 with more dependence on the initial CD-stretch, taking approximately 100 ps with symmetric CD-stretch excitation and approximately 120 ps with asymmetric CD-stretch excitation. Comparison is made with earlier nonequilibrium molecular dynamics simulations of VC [Kabadi, V. N.; Rice, B. M. Molecular dynamics simulations of normal mode vibrational energy transfer in liquid nitromethane. J. Phys. Chem. A 2004, 108, 532-540]. The simulations do a good job of reproducing the observed VC process and in addition they predicted the slow interconversion among CH-stretch excitations and the slower relaxation of the asymmetric CH-stretch now observed here. 相似文献