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Dr. Yohei Hattori Tatsuya Maejima Yumi Sawae Jun-ichiro Kitai Prof. Masakazu Morimoto Dr. Ryojun Toyoda Prof. Hiroshi Nishihara Prof. Satoshi Yokojima Dr. Shinichiro Nakamura Prof. Kingo Uchida 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(50):11441-11450
The cyclization reaction of diarylethenes having an azulene ring occurs only via higher excited states. Novel diarylethenes having an azulene ring with a strong donor or acceptor were synthesized and examined in these reactions. A derivative having an electron-donating 1,3-benzodithiol-2-ylidenemethyl group at the 1-position of the azulene ring showed photochromism, whereas neither a derivative having a π-conjugated electron-donating group at the 3-position of the azulene ring nor derivatives having a π-conjugated electron-withdrawing group at the 1- or 3-position of the azulene ring showed any photochromism. The photoreactivities of these compounds were explained by calculating forces and bond orders on the excited states using density functional theory (DFT) and time-dependent (TD)-DFT. 相似文献
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Nobuyuki Ichinose Masahide Hagiri Jun-ichiro Kinugasa Nobuyuki Shichi Toshihiro Nakayama 《Research on Chemical Intermediates》2013,39(1):425-435
A charge-transfer (CT) complex of NOBF4 and hexamethoxybenzene (HMB), which gives out HMB?+ as a “fluorescent radical cation probe,” upon one-electron oxidation, has been designed to explore the excited state dynamics of contact radical ion pairs by laser-induced fluorescence and femtosecond transient absorption spectroscopic techniques. The acetonitrile solution of the CT complex showed weak fluorescence with a similar spectrum to that observed for free excited HMB radical cation (HMB?+*), suggesting the formation of HMB?+* upon the one-photonic excitation of the CT complex. The laser-power dependence of the fluorescence intensity supported the one-photonic excitation event. We have also observed a short-lived transient species but no long-lived species by femtosecond laser flash photolysis of the CT complex. The lifetime (6.5 ps) was in good accordance with its fluorescence quantum yield (2.5 × 10?5) and was able to assign the transient species to the fluorescent state, an excited radical ion pair [HMB ?+*/NO?]. All the events were completed within the inner sphere and the short lifetime of the transient species could be attributed to rapid back-electron transfer. It is concluded that the excited radical cation character in the excited state of the CT complex originates from the radical ion character in the CT complex in the ground state and that a relatively long lifetime of HMB?+* facilitates its observation even in the contact ion pair. 相似文献
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We consider magnetotransport properties in a conducting chiral helimagnet, where the magnetic kink crystal (MKC) is formed under weak magnetic field applied perpendicular to the helical axis. The MKC behaves as a magnetic superlattice potential and results in Bragg scattering of conduction electrons. Tuning of the weak magnetic field enables us to control the size of the superlattice Brillouin zone and gives rise to a series of divergent resistivity anomalies originating from resonant Bragg scatterings. We discuss as well a nontrivial magnetic structure in the resonant states realized in the subsystem of the itinerant electrons. 相似文献
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Michihito Ueda Masahiro Ueda Hiroaki Takagi Masayuki J. Sato Toshio Yanagida Ichiro Yamashita Kentaro Setsune 《Physica A》2008,387(16-17):4475-4481
“End of Moore’s Law” has recently become a topic. Keeping the signal-to-noise ratio (SNR) at the same level in the future will surely increase the energy density of smaller-sized transistors. Lowering the operating voltage will prevent this, but the SNR would inevitably degrade. Meanwhile, biological systems such as cells and brains possess robustness against noise in their information processing in spite of the strong influence of stochastic thermal noise. Inspired by the information processing of organisms, we propose a stochastic computing model to acquire information from noisy signals. Our model is based on vector matching, in which the similarities between the input vector carrying external noisy signals and the reference vectors prepared in advance as memorized templates are evaluated in a stochastic manner. This model exhibited robustness against the noise strength and its performance was improved by addition of noise with an appropriate strength, which is similar to a phenomenon observed in stochastic resonance. Because the stochastic vector matching we propose here has robustness against noise, it is a candidate for noisy information processing that is driven by stochastically-operating devices with low energy consumption in future. Moreover, the stochastic vector matching may be applied to memory-based information processing like that of the brain. 相似文献
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Bis(azafulvene) was isolated in 55% yield by the reaction of 4 equivalents of phenyllithium with 5,5'-diformyl-3,3',4,4'-tetraethyl-2,2'-bipyrrole followed by quenching with acetic anhydride. Unstable bis(azafulvene)s were obtained in much higher yields by dehydrating 5,5'-bis(hydroxymethyl) derivatives of 2,2'-bipyrrole and gem-dimethyl-2,2'-dipyrrylmethane with (Boc)2O-DMAP at room temperature. X-Ray crystallography of two bis(azafulvene)s is reported. 相似文献
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Seiichiro Onari Tetsuya Hata Yukio Tanaka Jun-ichiro Inoue 《Journal of Physics and Chemistry of Solids》2008,69(12):3307-3309
In order to clarify the tunneling spectroscopy in high-Tc cuprates, we study electronic state of the surface in the strongly correlated electron systems. First, we obtain Green's function of strongly correlated normal bulk system using the fluctuation exchange (FLEX) approximation. Next, we insert infinite potential into the bulk system and obtain Green's function of surface. We find that the density of states (DOS) in strongly correlated bulk systems are different from that on the surface, and the difference decreases as the magnitude of Coulomb interaction (U) increases. 相似文献
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One‐Handed Single Helicates of Dinickel(II) Benzenehexapyrrole‐α,ω‐diimine with an Amine Chiral Source 下载免费PDF全文
Dr. Chaolu Eerdun Satoshi Hisanaga Prof. Dr. Jun‐ichiro Setsune 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(1):239-246
Benzenehexapyrrole‐α,ω‐dialdehyde, composed of a pair of formyltripyrrole units with a 1,3‐phenylene linker, was metallated to give dinuclear single‐stranded helicates. X‐ray studies of the bis‐nickel(II) complex showed a helical C2 form with a pair of helical–metal coordination planes of a 3N+O donor set. The terminal aldehyde was readily converted into the imine by optically active amines, whereby helix‐sense bias was induced. Bis‐nickel(II) and bis‐palladium(II) complexes of the benzenehexapyrrole‐α,ω‐diimines were studied to show that an enantiomer pair of the helical C2 form are interchanged by slow flipping of each coordination plane and fast rotation around the C(benzene)?C(pyrrole) bond. The helical screw in the bis‐nickel(II) complexes was biased to one side in more than 95 % diastereoselectivity, which was achieved by using a variety of optically active amines, such as (R)‐1‐cyclohexylethylamine, (S)‐1‐ phenylethylamine, L ‐Phe(OEt) (Phe=phenylalanine), and (R)‐valinol. The nickel complexes showed much better diastereoselectivity than the corresponding palladium complexes. 相似文献
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Dr. Chaolu Eerdun Thi Hien Thuy Nguyen Takuya Okayama Satoshi Hisanaga Prof. Dr. Jun-ichiro Setsune 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(22):5777-5786
The hexapyrrole-α,ω-dicarbaldehydes 1 a and 1 b were metallated with CuII, NiII, and PdII to give bimetallic complexes where a pair of 3 N+O four-coordinate metal planes are helically distorted and the central 2,2′-bipyrrole subunit adopts a cis or trans conformation. X-ray crystallographic analysis of the bisCu complex revealed a closed form with a cis-2,2′-bipyrrole subunit and an open form with a trans-2,2′-bipyrrole subunit. The bisPd complexes took a closed form both in the solid state and in solution. They are regarded as single helicates of two turns and the energy barrier for the interchange between an M helix and a P helix was remarkably influenced by the bulky 3,3′-substituent of the central 2,2′-bipyrrole subunit. Although the bisNi complexes adopt a closed form in the solid state, they exist as a homohelical open C2-symmetric form or a heterohelical open Ci-symmetric form in solution. A theoretical study suggested that the closed form of 1 a Pd was stabilized by the Pd–Pd interaction. Compound 1 a Pd was reversibly oxidized by one electron at 0.14 V versus ferrocene/ferrocenium (Fc/Fc+) and this oxidized species showed Vis/NIR absorption bands at λ=767 and 1408 nm. 相似文献