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ABSTRACTQM(UB3LYP)/MM(AMBER) calculations were performed for the locations of the transition structure (TS) of the oxygen–oxygen (O–O) bond formation in the S4 state of the oxygen-evolving complex (OEC) of photosystem II (PSII). The natural orbital (NO) analysis of the broken-symmetry (BS) solutions was also performed to elucidate the nature of the chemical bonds at TS on the basis of several chemical indices defined by the occupation numbers of NO. The computational results revealed a concerted bond switching (CBS) mechanism for the oxygen–oxygen bond formation coupled with the one-electron transfer (OET) for water oxidation in OEC of PSII. The orbital interaction between the σ-HOMO of the Mn(IV)4–O(5) bond and the π*-LUMO of the Mn(V)1=O(6) bond plays an important role for the concerted O–O bond formation for water oxidation in the CaMn4O6 cluster of OEC of PSII. One electron transfer (OET) from the π-HOMO of the Mn(V)1=O(6) bond to the σ*-LUMO of the Mn(IV)4–O(5) bond occurs for the formation of electron transfer diradical, where the generated anion radical [Mn(IV)4–O(5)]-? part is relaxed to the ?Mn(III)4?…?O(5)- structure and the cation radical [O(6)=Mn(V)1]+ ? part is relaxed to the +O(6)–Mn(IV)1? structure because of the charge-spin separation for the electron-and hole-doped Mn–oxo bonds. Therefore, the local spins are responsible for the one-electron reductions of Mn(IV)4->Mn(III)4 and Mn(V)1->Mn(IV)1. On the other hand, the O(5)- and O(6)+ sites generated undergo the O–O bond formation in the CaMn4O6 cluster. The Ca(II) ion in the cubane- skeleton of the CaMn4O6 cluster assists the above orbital interactions by the lowering of the orbital energy levels of π*-LUMO of Mn(V)1=O(6) and σ*-LUMO of Mn(IV)4–O(5), indicating an important role of its Lewis acidity. Present CBS mechanism for the O–O bond formation coupled with one electron reductions of the high-valent Mn ions is different from the conventional radical coupling (RC) and acid-base (AB) mechanisms for water oxidation in artificial and native photosynthesis systems. The proton-coupled electron transfer (PC-OET) mechanism for the O–O bond formation is also touched in relation to the CBS-OET mechanism. 相似文献
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A diagnostic study q (energy transfer processes in a He-N2 flowing discharge and afterglow has been performed in a radiofrequency-produced plasma cooled in a liquid nitrogen hath. Optical emission spectroscopy in the visible and infrared spectral range as well as Langrnuir probe diagnostics were used. The vibrational kinetics of CO injected in such an afterglow has been examined. It shows a slow cooling of the electrons in the afterglow regime. The electron kinetics responsible joy CO vibrahonal excitation is turned off when N2 is added to the He discharge, while that for vibrationally excited N2 molecules is turned on. The results are discussed on the basis of previous theorerical calculations and experiments on the He-N2 system. 相似文献
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聚变等离子体中的快离子压强 总被引:2,自引:2,他引:0
本文运用Fokker-Planck方程的慢化近似,考虑存在多种离子成份(包括杂质),假定它们具有共同的温度,我们得到了聚变产生的快离子压强的简单封闭形式表示式。表明在典型的工作温度下(~60keV),D-~3He等离子体中聚变产生的快离子压强约为本底热压强的20%,这与D-T等离子体工作在20keV时的比值几乎相同。因此,D-~3He和D-T在它们相应的预期工作温度下,它们各自的快离子压强对总压强的影响是类似的,然而在更高的温度下,这个比值将变得更大。 相似文献
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D—^3He聚变动力可行性研究 总被引:9,自引:3,他引:6
本文首先简要地讨论D-3He聚变的物理要求并与D-T聚变作相应的比较,然后运用目前的约束定律和第一稳定区β极限,对计划的近期ETR规模装置(如CIT,TIBER,FER,NET)进行D-3He得失相当和点火实验的可行性研究,并对高径比第二稳定区D-3He托卡马克堆进行参数学研究,最后指出潜在的缩短商用化进程可能性。 相似文献
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S. De Nicola A. E. Kaplan S. Martellucci P. Mormile G. Pierattini J. Quartieri 《Applied physics. B, Lasers and optics》1989,49(5):441-444
We have observed a hysteretic (bistable) reflection of a Gaussian laser beam at the interface between glass and a liquid solution of polystyrene microspheres as nonlinear medium with both branches of the hysteretic curve being stable, in contrast to the results of previous experiments. 相似文献
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双折射双频激光器偏振特性的分析 总被引:6,自引:1,他引:5
用激光原理和晶体光学原理分析了腔内加旋光晶体的激光器输出光的偏振特性,实验和分析表明,激光器输出两束不同频率的垂直线偏振光,激光器两端输出光的偏振面有一夹角a,且此夹角与晶轴和传光方向的夹角θ有关。理论计算结果在双折射双频激光器的实验结果符合很好。 相似文献
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A. Torrisi P. Horák J. Vacík A. Cannavò G. Ceccio J. Vaniš 《Phosphorus, sulfur, and silicon and the related elements》2020,195(11):932-935
AbstractOn the perspective to develop CuO–TiO2 MOS, multilayered Cu and Ti thin layers were alternatively deposited on silicon wafers using 25?keV Ar?+?ion beam sputtering and, subsequently, oxidized by thermal annealing in air at 400?°C for 24?h. The deposited films have variable ratios of the Cu and Ti % at. One of the main goal is to obtain such multilayers avoiding the presence of Cu–Ti–O compounds. The samples were characterized in terms of composition (by RBS and SIMS analyses) and morphology (by AFM and SEM investigations). In particular, SIMS maps allows to observe the spatial distribution and thickness of each phase of the Cu/Ti multilayers, and further to observe Cu diffusion and mixing with Ti, as well as phase separation of CuO and TiO2 in the samples. The reasons of this effect represent an open issue that has to investigated, in order to improve the MOS fabrication. 相似文献
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A new reaction of organolithium compounds with phosphonium salts is described; reaction of t-butyllithium with dibenzylaminophosphonium or tetraphenylphosphonium bromides takes place through addition of the t-butyl group on a benzene ring at the position para to the phosphorus atom, the ylid formed reacts in a characteristic Wittig reaction with p-tolylaldehyde. 相似文献