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51.
A Novel Bismuth‐Based Metal–Organic Framework for High Volumetric Methane and Carbon Dioxide Adsorption 下载免费PDF全文
Mathew Savage Dr. Sihai Yang Dr. Mikhail Suyetin Prof. Dr. Elena Bichoutskaia Dr. William Lewis Prof. Dr. Alexander J. Blake Sarah A. Barnett Prof. Dr. Martin Schröder 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(26):8024-8029
Solvothermal reaction of H4L (L=biphenyl‐3,3′,5,5′‐tetracarboxylate) and Bi(NO3)3 ? (H2O)5 in a mixture of DMF/MeCN/H2O in the presence of piperazine and nitric acid at 100 °C for 10 h affords the solvated metal–organic polymer [Bi2(L)1.5(H2O)2] ? (DMF)3.5 ? (H2O)3 (NOTT‐220‐solv). A single crystal X‐ray structure determination confirms that it crystallises in space group P2/c and has a neutral and non‐interpenetrated structure comprising binuclear {Bi2} centres bridged by tetracarboxylate ligands. NOTT‐220‐solv shows a 3,6‐connected network having a framework topology with a {4 ? 62}2{42 ? 65 ? 88}{62 ? 8} point symbol. The desolvated material NOTT‐220a shows exceptionally high adsorption uptakes for CH4 and CO2 on a volumetric basis at moderate pressures and temperatures with a CO2 uptake of 553 g L?1 (20 bar, 293 K) with a saturation uptake of 688 g L?1 (1 bar, 195 K). The corresponding CH4 uptake was measured as 165 V(STP)/V (20 bar, 293 K) and 189 V(STP/V) (35 bar, 293 K) with a maximum CH4 uptake for NOTT‐220a recorded at 20 bar and 195 K to be 287 V(STP)/V, while H2 uptake of NOTT‐220a at 20 bar, 77 K is 42 g L?1. These gas uptakes have been modelled by grand canonical Monte Carlo (GCMC) and density functional theory (DFT) calculations, which confirm the experimental data and give insights into the nature of the binding sites of CH4 and CO2 in this porous hybrid material. 相似文献
52.
Dr. Christopher G. P. Taylor Dr. Stephen P. Argent Michael D. Ludden Jerico R. Piper Cristina Mozaceanu Dr. Sarah A. Barnett Prof. Michael D. Ward 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(14):3054-3064
A crystallographic investigation of a series of host–guest complexes in which small-molecule organic guests occupy the central cavity of an approximately cubic M8L12 coordination cage has revealed some unexpected behaviour. Whilst some guests form 1:1 H⋅G complexes as we have seen before, an extensive family of bicyclic guests—including some substituted coumarins and various saturated analogues—form 1:2 H⋅G2 complexes in the solid state, despite the fact that solution titrations are consistent with 1:1 complex formation, and the combined volume of the pair of guests significantly exceeds the Rebek 55±9 % packing for optimal guest binding, with packing coefficients of up to 87 %. Re-examination of solution titration data for guest binding in two cases showed that, although conventional fluorescence titrations are consistent with 1:1 binding model, alternative forms of analysis—Job plot and an NMR titration—at higher concentrations do provide evidence for 1:2 H⋅G2 complex formation. The observation of guests binding in pairs in some cases opens new possibilities for altered reactivity of bound guests, and also highlights the recently articulated difficulties associated with determining stoichiometry of supramolecular complexes in solution. 相似文献
53.
Monomeric Chini‐Type Triplatinum Clusters Featuring Dianionic and Radical‐Anionic π*‐Systems 下载免费PDF全文
Brandon R. Barnett Prof. Arnold L. Rheingold Prof. Joshua S. Figueroa 《Angewandte Chemie (International ed. in English)》2016,55(32):9253-9258
Owing to their unique topologies and abilities to self‐assemble into a variety of extended and aggregated structures, the binary platinum carbonyl clusters [Pt3(CO)6]n2? (“Chini clusters”) continue to draw significant interest. Herein, we report the isolation and structural characterization of the trinuclear electron‐transfer series [Pt3(μ‐CO)3(CNArDipp2)3]n? (n=0, 1, 2), which represents a unique set of monomeric Pt3 clusters supported by π‐acidic ligands. Spectroscopic, computational, and synthetic investigations demonstrate that the highest‐occupied molecular orbitals of the mono‐ and dianionic clusters consist of a combined π*‐framework of the CO and CNArDipp2 ligands, with negligible Pt character. Accordingly, this study provides precedent for an ensemble of carbonyl and isocyanide ligands to function in a redox non‐innocent manner. 相似文献
54.
A. J. T. Colin S. M. Barnett J. Jeffers 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2011,63(3):463-472
We investigate some properties of programmed quantum-state discriminators with simple programs. Bergou et al. [Phys. Rev.
A 73, 062334 (2006)] have considered programmable devices which are supplied with two distinct but unknown program qbits and one data qbit which is certain to be identical to one or other of the program qbits. The task is to discriminate between the first
and the second possibility. In this paper, we consider this state-discrimination problem when there is some additional classical
information available. We find that in the minimum error discrimination mode, the probability of correct discrimination is
increased by each type of classical information. The same is broadly true of unambiguous discrimination, with the chance of
success improving when the overlap between the program qbits is reduced. 相似文献
55.
56.
Affolder T Akimoto H Akopian A Albrow MG Amaral P Amidei D Anikeev K Antos J Apollinari G Arisawa T Artikov A Asakawa T Ashmanskas W Azfar F Azzi-Bacchetta P Bacchetta N Bachacou H Bailey S de Barbaro P Barbaro-Galtieri A Barnes VE Barnett BA Baroiant S Barone M Battle C Bauer G Bedeschi F Belforte S Bell WH Bellettini G Bellinger J Benjamin D Bensinger J Beretvas A Berge JP Berryhill J Bhatti A Binkley M Bisello D Bishai M Blair RE Blocker C Bloom K Blumenfeld B Blusk SR Bocci A Bodek A 《Physical review letters》2002,88(7):071806
We present the first general search for new heavy particles, X, which decay via X --> WZ0 --> e(nu)+jj as a function of M(X) and Gamma(X) in pp collisions at square root[s] = 1.8 TeV. No evidence is found for production of X in 110 pb(-1) of data collected by the Collider Detector at Fermilab. General cross section limits are set at the 95% C.L. as a function of mass and width of the new particle. The results are further interpreted as mass limits on the production of new heavy charged vector bosons which decay via W' --> WZ0 in an extended gauge model as a function of the width, Gamma(W'), and mixing factor between the W' and the standard model W bosons. 相似文献
57.
An optimal control problem for a single bulk-service queue is considered. Theorems that characterize the optimal control strategy in some circumstances are proved; they complement earlier results by Deb and Serfozo for a comparable problem. Most of the analysis uses direct probabilistic reasoning rather than specialized methods such as dynamic programming. Some illustrative examples are presented. 相似文献
58.
59.
According to general theory, a semi-infinite piezoelectric crystal with mechanically free surface and an adjoining medium with zero dielectric constant, may or may not allow a surface wave solution. Examples where surface wave solutions are not allowed, are not known, and one might think that solutions actually always exist. In the present paper this problem is put to rest by an explicit example of non-existence. 相似文献
60.
B. Barnett D. Blockus M. Burka C. Y. Chien D. Christian W. Koska L. Madansky C. May Y. T. Oh A. Pevsner S. Wagner C. Woody N. C. Yang 《Physics letters. [Part B]》1983,120(4-6)
Results are presented from a search for a ρ0ρ0 enhancement in antiproton annihilations. A ρ0ρ0 resonance was recently observed in radiative ψ decays, and its existence has been supported by the results of an antiproton experiment at 5.7 GeV/c. No indication of this ρ0ρ0 enhancement is seen is our data, in direct contradiction with the earlier, lower statistics experiment. 相似文献