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941.
Yanai T Kurashige Y Neuscamman E Chan GK 《Physical chemistry chemical physics : PCCP》2012,14(21):7809-7820
The canonical transformation (CT) theory has been developed as a multireference electronic structure method to compute high-level dynamic correlation on top of a large active space reference treated with the ab initio density matrix renormalization group method. This article describes a parallelized algorithm and implementation of the CT theory to handle large computational demands of the CT calculation, which has the same scaling as the coupled cluster singles and doubles theory. To stabilize the iterative solution of the CT method, a modification to the CT amplitude equation is introduced with the inclusion of a level shift parameter. The level-shifted condition has been found to effectively remove a type of intruder state that arises in the linear equations of CT and to address the discontinuity problems in the potential energy curves observed in the previous CT studies. 相似文献
942.
Wobma HM Blades ML Grekova E McGuire DL Chen K Chan WC Cramb DT 《Physical chemistry chemical physics : PCCP》2012,14(10):3290-3294
Direct three-colour fluorescence cross-correlation spectroscopy can reveal interactions between three fluorescently labelled biomolecules, giving insight toward the complex events that constitute signal transduction pathways. Here we provide the optical and theoretical basis for this technology and demonstrate its ability to detect specific biological associations between nanoparticle-labelled DNA molecules. 相似文献
943.
Mohammad A Hossain Sereyrath Ngeth Teddy Chan Michael N Oda Gordon A Francis 《BMC biochemistry》2012,13(1):1
Background
ATP-binding cassette transporter A1 (ABCA1) mediates the lipidation of exchangeable apolipoproteins, the rate-limiting step in the formation of high density lipoproteins (HDL). We previously demonstrated that HDL oxidized ex vivo by peroxidase-generated tyrosyl radical (tyrosylated HDL, tyrHDL) increases the availability of cellular cholesterol for efflux and reduces the development of atherosclerosis when administered to apolipoprotein E-deficient mice as compared to treatment with control HDL. 相似文献944.
Kim MS Sim TS Kim YJ Kim SS Jeong H Park JM Moon HS Kim SI Gurel O Lee SS Lee JG Park JC 《Lab on a chip》2012,12(16):2874-2880
Circulating tumor cells (CTCs) have gained increasing attention as physicians and scientists learn more about the role these extraordinarily rare cells play in metastatic cancer. In developing CTC technology, the critical criteria are high recovery rates and high purity. Current isolation methods suffer from an inherent trade-off between these two goals. Moreover, ensuring minimal cell stress and robust reproducibility is also important for the clinical application of CTCs. In this paper, we introduce a novel CTC isolation technology using selective size amplification (SSA) for target cells and a multi-obstacle architecture (MOA) filter to overcome this trade-off, improving both recovery rate and purity. We also demonstrate SSA-MOA's advantages in minimizing cell deformation during filter transit, resulting in more stable and robust CTC isolation. In this technique, polymer microbeads conjugated with anti-epithelial cell adhesion molecules (anti-EpCAM) were used to selectively size-amplify MCF-7 breast cancer cells, definitively differentiating from the white blood cells (WBCs) by avoiding the size overlap that compromises other size selection methods. 3 μm was determined to be the optimal microbead diameter, not only for size discrimination but also in maximizing CTC surface coverage. A multi-obstacle architecture filter was fabricated using silicon-on-glass (SOG) technology-a first such application of this fabrication technique-to create a precise microfilter structure with a high aspect ratio. The filter was designed to minimize cell deformation as simulation results predicted that cells captured via this MOA filter would experience 22% less moving force than with a single-obstacle architecture. This was verified by experiments, as we observed reliable cell capture and reduced cell deformation, with a 92% average recovery rate and 351 peripheral blood leukocytes (PBL) per millilitre (average). We expect the SSA-MOA platform to optimize CTC recovery rates, purity, and stability, increasing the sensitivity and reliability of such tests, thereby potentially expanding the utilization of CTC technologies in the clinic. 相似文献
945.
We present a novel blood filter unit that is designed to separate blood plasma from whole blood by simple magnetic actuation. A non-diluted blood sample is dropped into the filter unit and magnetic attraction is applied to squeeze out only blood plasma while blood particles are filtered by membranes stacked in the filter unit. The new filter device yields good filtering performance with nearly perfect filtering efficiency (~99.999%), high plasma recovery (~30%), low blood consumption (<50 μl), and fast operation (~1 min). Because it is simple to operate and is attachable to any kind of pre-made biochip, it has commercial potential in various lab-on-a-chip applications for blood tests. 相似文献
946.
Chan J Lewis AR Indurugalla D Schur M Wakarchuk W Bennet AJ 《Journal of the American Chemical Society》2012,134(8):3748-3757
A series of isotopically labeled natural substrate analogues (phenyl 5-N-acetyl-α-d-neuraminyl-(2→3)-β-d-galactopyranosyl-(1→4)-1-thio-β-d-glucopyranoside; Neu5Acα2,3LacβSPh, and the corresponding 2→6 isomer) were prepared chemoenzymatically in order to characterize, by use of multiple kinetic isotope effect (KIE) measurements, the glycosylation transition states for Vibrio cholerae sialidase-catalyzed hydrolysis reactions. The derived KIEs for Neu5Acα2,3LacβSPh for the ring oxygen ((18)V/K), leaving group oxygen ((18)V/K), C3-S deuterium ((D)V/K(S)) and C3-R deuterium ((D)V/K(R)) are 1.029 ± 0.002, 0.983 ± 0.001, 1.034 ± 0.002, and 1.043 ± 0.002, respectively. In addition, the KIEs for Neu5Acα2,6βSPh for C3-S deuterium ((D)V/K(S)) and C3-R deuterium ((D)V/K(R)) are 1.021 ± 0.001 and 1.049 ± 0.001, respectively. The glycosylation transition state structures for both Neu5Acα2,3LacβSPh and Neu5Acα2,6LacβSPh were modeled computationally using the experimental KIE values as goodness of fit criteria. Both transition states are late with largely cleaved glycosidic bonds coupled to pyranosyl ring flattening ((4)H(5) half-chair conformation) with little or no nucleophilic involvement of the enzymatic tyrosine residue. Notably, the transition state for the catalyzed hydrolysis of Neu5Acα2,6βSPh appears to incorporate a lesser degree of general-acid catalysis, relative to the 2,3-isomer. 相似文献
947.
S Monari G Battistuzzi CA Bortolotti S Yanagisawa K Sato C Li I Salard D Kostrz M Borsari A Ranieri C Dennison M Sola 《Journal of the American Chemical Society》2012,134(29):11848-11851
The hydrophobic patch of azurin (AZ) from Pseudomonas aeruginosa is an important recognition surface for electron transfer (ET) reactions. The influence of changing the size of this region, by mutating the C-terminal copper-binding loop, on the ET reactivity of AZ adsorbed on gold electrodes modified with alkanethiol self-assembled monolayers (SAMs) has been studied. The distance-dependence of ET kinetics measured by cyclic voltammetry using SAMs of variable chain length, demonstrates that the activation barrier for short-range ET is dominated by the dynamics of molecular rearrangements accompanying ET at the AZ-SAM interface. These include internal electric field-dependent low-amplitude protein motions and the reorganization of interfacial water molecules, but not protein reorientation. Interfacial molecular dynamics also control the kinetics of short-range ET for electrostatically and covalently immobilized cytochrome c. This mechanism therefore may be utilized for short-distance ET irrespective of the type of metal center, the surface electrostatic potential, and the nature of the protein-SAM interaction. 相似文献
948.
Prof. Barry M. Trost Mark J. Bartlett Dr. Andrew H. Weiss Dr. Axel Jacobi von Wangelin Dr. Vincent S. Chan 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(51):16498-16509
The development of a general and practical zinc‐catalyzed enantioselective alkyne addition methodology is reported. The commercially available ProPhenol ligand ( 1 ) has facilitated the addition of a wide range of zinc alkynylides to aryl, aliphatic, and α,β‐unsaturated aldehydes in high yield and enantioselectivity. New insights into the mechanism of this reaction have resulted in a significant reduction in reagent stoichiometry, enabling the use of precious alkynes and avoiding the use of excess dimethylzinc. The enantioenriched propargylic alcohols from this reaction serve as versatile synthetic intermediates and have enabled efficient syntheses of several complex natural products. 相似文献
949.
Hyun Ook SeoChae Won Sim Kwang-Dae KimYoung Dok Kim Ji Hyun ParkByung Cheol Lee Kyu Hwan LeeDong Chan Lim 《Radiation Physics and Chemistry》2012,81(3):290-294
High-energy electron-beam with energy of 1 MeV was used for modifying surface structure of TiO2 thin films on carbon fiber prepared by using atomic layer deposition under atmospheric pressure. TiO2 nanoparticles (∼20 nm) on carbon fiber underwent structural modification of the surface upon electron-beam treatment, resulting in enhanced photocatalytic activity. In contrast, a thicker film of TiO2 did not show such changes in surface structure and photocatalytic activity by electron-beam treatment. We demonstrate that electron-beam can be used for modifying surface structure of photocatalysts consisting of nanoparticles for improvement of their activity. 相似文献
950.
The Stokes multipliers in the matrix models are invariants in the string-theory moduli space and related to the D-instanton chemical potentials. They not only represent non-perturbative information but also play an important role in connecting various perturbative string theories in the moduli space. They are a key concept to the non-perturbative completion of string theory and also expected to imply some remnant of strong coupling dynamics in M theory. In this paper, we investigate the non-perturbative completion problem consisting of two constraints on the Stokes multipliers. As the first constraint, Stokes phenomena which realize the multi-cut geometry are studied in the Zk symmetric critical points of the multi-cut two-matrix models. Sequence of solutions to the constraints are obtained in general k-cut critical points. A discrete set of solutions and a continuum set of solutions are explicitly shown, and they can be classified by several constrained configurations of the Young diagram. As the second constraint, we discuss non-perturbative stability of backgrounds in terms of the Riemann-Hilbert problem. In particular, our procedure in the 2-cut (1,2) case (pure-supergravity case) completely fixes the D-instanton chemical potentials and results in the Hastings-McLeod solution to the Painlevé II equation. It is also stressed that the Riemann-Hilbert approach realizes an off-shell background independent formulation of non-critical string theory. 相似文献