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1.
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
2.
Takayuki Nakai Yoshiko Murakami Yoshiaki Sasaki Isamu Fujiwara Shoji Tagashira 《Analytical sciences》2004,20(1):235-237
The extraction and separation of copper(II), zinc(II), cobalt(II), and cadmium(II) were investigated. Both copper(II) and zinc(II) formed ammine-complexes, while cadmium(II) and cobalt(II) formed hydroxide precipitates in an ammonia medium. By the addition of sodium dodecylsulfate (SDS), a copper(II) complex formed an ion-pair (copper-ammine-DS), which was extracted into the SDS phase. However, a zinc(II) complex did not form an ion-pair, and was soluble in water. Copper(II) ion was recovered by stripping (back-extraction) after the addition of hydrochloric acid. This method was applied to the separation of copper(II) in a brass alloy. 相似文献
3.
A large-volume (100 microl) injection-ETAAS with W-treated PG furnace combined with a phosphate modifier was applied to the determination of unpolluted levels of Cd in tap, snow and river-water samples. The limit of detection of 1.1 ng l(-1) was observed for a 4 w/v% NH4H2PO4 modifer. Matrix interference studies were tested for major ion species well found in fresh water. The direct determination of Cd in certified river water (12 +/- 2 ng l(-1)) was carried out and the observed value was in agreement with the certified one. The good recoveries of Cd added to real environmental water samples were also observed. This method was applied to the determination of Cd in unpolluted environmental water samples. 相似文献
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方永得 张玉虎 M.Oshima Y.Toh 周小红 M.Koizumi A.Osa A.Kimura Y.Hatsukawa T.Morikawa M.Nakamura M.Sugawara H.Kusakari 《中国物理 C》2006,30(2):99-104
利用在束γ谱学实验技术, 通过173Yb(19F,4nγ)反应
布居了188Au的高自旋态, 并对其准粒子带结构进行了研究. 基于实验测量结果, 对原有的双奇核188Au能级纲图做了较大的修改. 通过系统性比较, 对15+以上的能级结构进行了讨论. 相似文献
7.
H. Kimura 《Journal of Mathematical Sciences》2004,124(5):5250-5261
We compute explicitly the cohomological intersection numbers for the basis and extend the result of Iwasaki and Matsumoto. To this end, we establish the exterior power structure for the polynomial twisted de Rham cohomology group associated with the generalized Airy functions at a point of extended Veronese variety. Using this structure, we introduce a natural basis of the twisted de Rham cohomology group coming from that of the one-dimensional case, which is considered as an analogue of a flat basis of the Jacobi ring of A-type simple singularity. 相似文献
8.
It is an important challenge to analyze a three-dimensional thermal flow field in engineering, science, and agriculture. For such an analysis, it is essential to measure physical quantities such as temperature and velocity over the entire thermal flow field. This paper presents a measurement system based on color image processing for temperature and velocity vector distributions in a three-dimensional thermal flow field. Flow visualization is accomplished by the use of thermo-sensitive liquid crystal tracers. An algorithm for the color-to-temperature transformation using a multi-layer feed-forward neural network is applied to three-dimensional natural convection in a rotating cylindrical cell. Two-dimensional temperature distributions in a slit plane are obtained by using the algorithm. A three-dimensional temperature distribution is consequently constructed by interpolating the two-dimensional distributions using the B-spline function. In addition, the Spatio-Temporal correlation method is applied to the natural convection to obtain a three-dimensional velocity vector distribution. 相似文献
9.
In this paper, we give a new genus-3 topological recursion relation for Gromov-Witten invariants of compact symplectic manifolds.
This formula also applies to intersection numbers on moduli spaces of spin curves. A by-product of the proof of this formula
is a new relation in the tautological ring of the moduli space of 1-pointed genus-3 stable curves.
Research of the first author was partially supported by NSF grant DMS-0204824
Research of the second author was partially supported by NSF grant DMS-0505835 相似文献
10.