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1.
Feng Cheng Shuqi Wu Wenwei Zheng Shengqun Su Takumi Nakanishi Wenhuang Xu Pritam Sadhukhan Hibiki Sejima Shimon Ikenaga Kaoru Yamamoto Kaige Gao Shinji Kanegawa Prof. Osamu Sato 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(59):e202202161
The crystallization of a complex having electron transfer properties in a polar space group can induce the polarization switching of a crystal in a specific direction, which is attractive for the development of sensors, memory devices, and capacitors. Unfortunately, the probability of crystallization in a polar space group is usually low. Noticing that enantiopure compounds crystallize in Sohncke space groups, this paper reports a strategy for the molecular design of non-ferroelectric polarization switching crystals based on the use of intramolecular electron transfer and chirality. In addition, this paper describes the synthesis of a mononuclear valence tautomeric (VT) cobalt complex bearing an enantiopure ligand. The introduction of enantiomer enables the crystallization of the complex in the polar space group (P21). The polarization of the crystals along the b-axis direction is not canceled out and the VT transition is accompanied by a change in the macroscopic polarization of the polar crystal. Polarization switching via electron transfer is realized at around room temperature. 相似文献
2.
We introduce a quantum key distribution protocol using mean multi-kings’ problem. Using this protocol, a sender can share a bit sequence as a secret key with receivers. We consider a relation between information gain by an eavesdropper and disturbance contained in legitimate users’ information. In BB84 protocol, such relation is known as the so-called information disturbance theorem. We focus on a setting that the sender and two receivers try to share bit sequences and the eavesdropper tries to extract information by interacting legitimate users’ systems and an ancilla system. We derive trade-off inequalities between distinguishability of quantum states corresponding to the bit sequence for the eavesdropper and error probability of the bit sequence shared with the legitimate users. Our inequalities show that eavesdropper’s extracting information regarding the secret keys inevitably induces disturbing the states and increasing the error probability. 相似文献
3.
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
4.
Taishi Nakanishi Dr. Jun Kikuchi Dr. Atsushi Kaga Prof. Dr. Shunsuke Chiba Prof. Dr. Masahiro Terada 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(37):8230-8234
A catalytic enantioselective synthesis of β-amino secondary amides was achieved using vinyl azides as the enamine-type nucleophile and chiral N-Tf phosphoramide as the chiral Brønsted acid catalyst through a five-step sequential transformation in one pot. The established sequential transformation involves an enantioselective [4+2] cycloaddition reaction of vinyl azides with N-acyl imines as the key stereo-determining step that is efficiently accelerated by a chiral N-Tf phosphoramide catalyst in a highly enantioselective manner in most cases. Further generation of the iminodiazonium ion intermediate through ring opening of the cycloaddition product and subsequent skeletal rearrangement involving Schmidt-type 1,2-aryl group migration followed by recyclization of the resulting nitrilium ion were also initiated by the same acid catalyst. Final acid hydrolysis of the recyclized products in the same pot gave rise to enantioenriched β-amino amides through C−C bond formation at the α-position of the secondary amides. 相似文献
5.
Dr. Sudhir Kumar Keshri Dr. Waka Nakanishi Dr. Atsuro Takai Prof. Dr. Tomoya Ishizuka Prof. Dr. Takahiko Kojima Prof. Dr. Masayuki Takeuchi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(58):13288-13294
The design and synthesis of a tweezer-shaped naphthalenediimide (NDI)–anthracene conjugate ( 2NDI ) are reported. In the structure of the closed form (πNDI ⋅⋅⋅ πNDI stack) of 2NDI , which was elucidated by single-crystal XRD, the existence of C−H ⋅⋅⋅ O hydrogen bonding involving the nearest carbonyl oxygen atom of an NDI unit was suggested. The tunability of πNDI ⋅⋅⋅ πNDI interactions was studied by means of UV/Vis absorption, fluorescence and NMR spectroscopy and molecular modelling. This revealed that the πNDI ⋅⋅⋅ πNDI interactions in 2NDI affect the absorption and emission properties depending on the temperature. Furthermore, in polar solvents, 2NDI prefers the stronger πNDI ⋅⋅⋅ πNDI stack, whereas the πNDI ⋅⋅⋅ πNDI interaction is diminished in nonpolar solvents. Importantly, the conformational variations of 2NDI can be reversibly switched by variation in temperature, and this suggests potential application for fluorogenic molecular switches upon temperature changes. 相似文献
6.
Dr. Yoji Horii Dr. Keiichi Katoh Dr. Kunihisa Sugimoto Dr. Ryo Nakanishi Dr. Brian K. Breedlove Prof. Dr. Masahiro Yamashita 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(12):3098-3104
In the research field of single-molecule magnets (SMMs), lanthanoid–lanthanoid interactions, so-called f–f interactions, are known to affect the SMM properties, although their magnitudes are small. In this article, an SMM with very weak f–f interactions is reported, and the effects of the interactions on the SMM properties are discussed. X-ray structural analysis of the DyIII-CdII-phthalocyaninato sextuple-decker complex (Dy2Cd3) reveals that the intramolecular Dy−Dy length in Dy2Cd3 is more than 13 Å, which is longer than the intermolecular Dy−Dy length. Even though the two DyIII ions are far apart, intermolecular ferromagnetic dipole–dipole interactions are observed in Dy2Cd3. From detailed analysis of ac magnetic susceptibilities, quantum tunneling of the magnetization (QTM) in Dy2Cd3 is partially suppressed owing to the existence of very weak Dy−Dy interactions. Our results show that even very weak Dy−Dy interactions act as a dipolar bias, suppressing QTM. 相似文献
7.
Prof. Dr. Yasuchika Hasegawa Takafumi Matsui Dr. Yuichi Kitagawa Dr. Takayuki Nakanishi Dr. Tomohiro Seki Prof. Dr. Hajime Ito Prof. Dr. Yuta Nakasaka Prof. Dr. Takao Masuda Prof. Dr. Koji Fushimi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(53):12308-12315
Oxygen-sensitive and near-infrared (NIR) luminescent YbIII coordination polymers incorporating ligands based on pyrene derivatives were synthesized: YbIII–TBAPy and YbIII–TIAPy (TBAPy: 1,3,6,8-tetrakis(p-benzoate)pyrene; TIAPy: 1,3,6,8-tetrakis(3,5-isophthalic acid)pyrene). The coordination structures of these materials have been characterized by means of electrospray ionization mass spectrometry, X-ray diffraction analysis, and thermogravimetric analysis. Moreover, the porous structure of YbIII–TIAPy has been evaluated by measuring its N2 adsorption isotherm. The NIR luminescence properties of YbIII–TBAPy and YbIII–TIAPy have been examined by acquiring emission spectra and determining emission lifetimes under air or argon and in vacuo. YbIII–TIAPy exhibited high thermal stability (with a decomposition temperature of 400 °C), intense luminescence (with an emission quantum yield under argon of 6.6 %), and effective oxygen-sensing characteristics. These results suggest that NIR luminescent YbIII coordination polymers prepared using pyrene derivatives could have applications in novel thermo-stable oxygen sensors. 相似文献
8.
9.
High‐performance liquid chromatography separation of unsaturated organic compounds by a monolithic silica column embedded with silver nanoparticles 下载免费PDF全文
Yang Zhu Kei Morisato George Hasegawa Nirmalya Moitra Tsutomu Kiyomura Hiroki Kurata Kazuyoshi Kanamori Kazuki Nakanishi 《Journal of separation science》2015,38(16):2841-2847
The optimization of a porous structure to ensure good separation performances is always a significant issue in high‐performance liquid chromatography column design. Recently we reported the homogeneous embedment of Ag nanoparticles in periodic mesoporous silica monolith and the application of such Ag nanoparticles embedded silica monolith for the high‐performance liquid chromatography separation of polyaromatic hydrocarbons. However, the separation performance remains to be improved and the retention mechanism as compared with the Ag ion high‐performance liquid chromatography technique still needs to be clarified. In this research, Ag nanoparticles were introduced into a macro/mesoporous silica monolith with optimized pore parameters for high‐performance liquid chromatography separations. Baseline separation of benzene, naphthalene, anthracene, and pyrene was achieved with the theoretical plate number for analyte naphthalene as 36 000 m?1. Its separation function was further extended to cis/trans isomers of aromatic compounds where cis/trans stilbenes were chosen as a benchmark. Good separation of cis/trans‐stilbene with separation factor as 7 and theoretical plate number as 76 000 m?1 for cis‐stilbene was obtained. The trans isomer, however, is retained more strongly, which contradicts the long‐ established retention rule of Ag ion chromatography. Such behavior of Ag nanoparticles embedded in a silica column can be attributed to the differences in the molecular geometric configuration of cis/trans stilbenes. 相似文献