全文获取类型
收费全文 | 265篇 |
免费 | 7篇 |
专业分类
化学 | 233篇 |
晶体学 | 2篇 |
力学 | 6篇 |
物理学 | 31篇 |
出版年
2023年 | 2篇 |
2021年 | 4篇 |
2020年 | 7篇 |
2019年 | 5篇 |
2018年 | 2篇 |
2016年 | 2篇 |
2015年 | 2篇 |
2014年 | 5篇 |
2013年 | 5篇 |
2012年 | 12篇 |
2011年 | 22篇 |
2010年 | 6篇 |
2009年 | 6篇 |
2008年 | 12篇 |
2007年 | 16篇 |
2006年 | 20篇 |
2005年 | 19篇 |
2004年 | 16篇 |
2003年 | 9篇 |
2002年 | 5篇 |
2001年 | 10篇 |
2000年 | 4篇 |
1998年 | 2篇 |
1997年 | 3篇 |
1995年 | 2篇 |
1994年 | 2篇 |
1992年 | 5篇 |
1991年 | 4篇 |
1990年 | 5篇 |
1989年 | 4篇 |
1988年 | 1篇 |
1987年 | 4篇 |
1986年 | 3篇 |
1985年 | 7篇 |
1984年 | 3篇 |
1983年 | 6篇 |
1982年 | 3篇 |
1981年 | 1篇 |
1980年 | 4篇 |
1979年 | 2篇 |
1977年 | 2篇 |
1976年 | 2篇 |
1974年 | 1篇 |
1973年 | 3篇 |
1972年 | 1篇 |
1971年 | 1篇 |
1970年 | 2篇 |
1969年 | 2篇 |
1968年 | 1篇 |
1967年 | 2篇 |
排序方式: 共有272条查询结果,搜索用时 15 毫秒
1.
Yulu Jiang Dr. Taro Ozaki Mei Harada Tadachika Miyasaka Dr. Hajime Sato Dr. Kazunori Miyamoto Dr. Junichiro Kanazawa Dr. Chengwei Liu Prof. Dr. Jun-ichi Maruyama Dr. Masaatsu Adachi Dr. Atsuo Nakazaki Prof. Dr. Toshio Nishikawa Prof. Dr. Masanobu Uchiyama Dr. Atsushi Minami Prof. Dr. Hideaki Oikawa 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(41):18152-18158
Lolitrems are tremorgenic indole diterpenes that exhibit a unique 5/6 bicyclic system of the indole moiety. Although genetic analysis has indicated that the prenyltransferase LtmE and the cytochrome P450 LtmJ are involved in the construction of this unique structure, the detailed mechanism remains to be elucidated. Herein, we report the reconstitution of the biosynthetic pathway for lolitrems employing a recently established genome-editing technique for the expression host Aspergillus oryzae. Heterologous expression and bioconversion of the various intermediates revealed that LtmJ catalyzes multistep oxidation to furnish the lolitrem core. We also isolated the key reaction intermediate with an epoxyalcohol moiety. This observation allowed us to establish the mechanism of radical-induced cyclization, which was firmly supported by density functional theory calculations and a model experiment with a synthetic analogue. 相似文献
2.
Dr. Alessandra Alberti Dr. Ioannis Deretzis Dr. Giovanna Pellegrino Dr. Corrado Bongiorno Dr. Emanuele Smecca Dr. Giovanni Mannino Dr. Filippo Giannazzo Prof. Guglielmo Guido Condorelli Dr. Nobuya Sakai Prof. Tsutomu Miyasaka Dr. Corrado Spinella Dr. Antonino La Magna 《Chemphyschem》2015,16(14):3064-3071
We investigate the degradation path of MAPbI3 (MA=methylammonium) films over flat TiO2 substrates at room temperature by means of X‐ray diffraction, spectroscopic ellipsometry, X‐ray photoelectron spectroscopy, and high‐resolution transmission electron microscopy. The degradation dynamics is found to be similar in air and under vacuum conditions, which leads to the conclusion that the occurrence of intrinsic thermodynamic mechanisms is not necessarily linked to humidity. The process has an early stage, which drives the starting tetragonal lattice in the direction of a cubic atomic arrangement. This early stage is followed by a phase change towards PbI2. We describe how this degradation product is structurally coupled with the original MAPbI3 lattice through the orientation of its constituent PbI6 octahedra. Our results suggest a slight octahedral rearrangement after volatilization of HI+CH3NH2 or MAI, with a relatively low energy cost. Our experiments also clarify why reducing the interfaces and internal defects in the perovskite lattice enhances the stability of the material. 相似文献
3.
Masao Sumita Hibeki Abe Hiroyuki Kayaki Keizo Miyasaka 《Journal of Macromolecular Science: Physics》2013,52(1-2):171-184
The electrical conductivities of carbon-black-filled low-density polyethylene (LDPE), poly(methyl methacrylate) (PMMA), and poly(vinyl chloride)-vinyl acetate (PVC/ VAc) copolymer were measured as functions of carbon content and melt viscosity of the matrix at the temperatures at which the composites were prepared. Sharp breaks in the relationship between the carbon filler content and the conductivity of composites were observed in all specimens at some content of the carbon filler. The conductivity jumps as much as 10 orders of magnitude at the break point. This phenomenon has been known as the “percolation threshold”. The critical carbon content corresponding to the break point 相似文献
4.
Dr. Hikaru Sotome Dr. Hajime Okajima Tatsuhiro Nagasaka Yuka Tachii Prof. Akira Sakamoto Prof. Seiya Kobatake Prof. Masahiro Irie Prof. Hiroshi Miyasaka 《Chemphyschem》2020,21(14):1524-1530
The geometrical evolution of the reactant and formation of the photoproduct in the cycloreversion reaction of a diarylethene derivative were probed using time-resolved absorption spectroscopies in the visible to near-infrared and mid-infrared regions. The time-domain vibrational data in the visible region show that the initially formed Franck-Condon state is geometrically relaxed into the minimum in the excited state potential energy surface, concomitantly with the low-frequency coherent vibrations. Theoretical calculations indicate that the nuclear displacement in this coherent vibration is nearly parallel to that in the geometrical relaxation. Time-resolved mid-infrared spectroscopy directly detected the formation of the open-ring isomer with the same time constant as the decrease of the closed-ring isomer in the excited state minimum. This observation reveals that no detectable intermediate, in which the population is accumulated, is present between the excited closed-ring isomer and the open-ring isomer in the ground state. 相似文献
5.
Yulu Jiang Taro Ozaki Mei Harada Tadachika Miyasaka Hajime Sato Kazunori Miyamoto Junichiro Kanazawa Chengwei Liu Jun‐ichi Maruyama Masaatsu Adachi Atsuo Nakazaki Toshio Nishikawa Masanobu Uchiyama Atsushi Minami Hideaki Oikawa 《Angewandte Chemie (International ed. in English)》2020,59(41):17996-18002
Lolitrems are tremorgenic indole diterpenes that exhibit a unique 5/6 bicyclic system of the indole moiety. Although genetic analysis has indicated that the prenyltransferase LtmE and the cytochrome P450 LtmJ are involved in the construction of this unique structure, the detailed mechanism remains to be elucidated. Herein, we report the reconstitution of the biosynthetic pathway for lolitrems employing a recently established genome‐editing technique for the expression host Aspergillus oryzae. Heterologous expression and bioconversion of the various intermediates revealed that LtmJ catalyzes multistep oxidation to furnish the lolitrem core. We also isolated the key reaction intermediate with an epoxyalcohol moiety. This observation allowed us to establish the mechanism of radical‐induced cyclization, which was firmly supported by density functional theory calculations and a model experiment with a synthetic analogue. 相似文献
6.
Systematic Tuning and Switching of Neutral and Ionic Phases in a Donor–Acceptor Chain Compound by Doping with Less‐Active Donors and by Pressure Application 下载免费PDF全文
Keita Nakabayashi Prof. Dr. Hitoshi Miyasaka 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(17):5121-5131
The temperature‐induced stepwise neutral–ionic (N–I) phase transition in the covalently bonded donor–acceptor chain compound [Ru2(2,3,5,6‐F4PhCO2)4DMDCNQI] ? 2(p‐xylene) (2,3,5,6‐F4PhCO2?=2,3,5,6‐tetrafluorobenzoate; DMDCNQI=2,5‐dimethyl‐N,N′‐dicyanoquinodiimine) was systematically tuned over a wide temperature range using two techniques: 1) A chemical technique based on doping with a less‐active donor unit [Ru2II,II(F5PhCO2)4] (F5PhCO2?=pentafluorobenzoate), thereby providing an isostructural doped series [{Ru2II,II(2,3,5,6‐F4PhCO2)4}1?x{Ru2II,II(F5PhCO2)4}xDMDCNQI] ? 2(p‐xylene), with x=0.06, 0.10, 0.21, and 0.24; and 2) a physical technique, which was the application of hydrostatic pressure to the doped compounds. The stepwise N–I transition observed in the original compound was systematically varied in terms of the viewpoints of both transition temperature and transition features (stepwise or monotonic) dependent on the amount of dopants x. Application of pressure efficiently tuned the N–I transitions, with the oxidation phases being dramatically modified by applying only weak pressure up to 4 kbar. Even in cases that led to N–I transitions in small domains of the chains at ambient pressure, the application of pressure caused an expansion of the domains that enabled N–I transitions, finally leading to a complete change in the oxidation state of the chains, from neutral to ionic, accompanied by a change from a paramagnetic state to a ferrimagnetically ordered state. 相似文献
7.
Masahiro Yamashita Daisuke Kawakami Satoshi Matsunaga Yoshio Nakayama Mari Sasaki Shinya Takaishi Fumiyasu Iwahori Hitoshi Miyasaka Ken‐ichi Sugiura Yoshiki Wada Hiroshi Miyamae Hiroyuki Matsuzaki Hiroshi Okamoto Hisaaki Tanaka Kazuhiro Marumoto Shin‐ichi Kuroda 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2004,116(36):4867-4871
8.
9.
10.