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51.
Polymer:fullerene blends have been widely studied as an inexpensive alternative to traditional silicon solar cells. Some polymer:fullerene blends, such as blends of poly(2,5‐bis(3‐tetradecylthiophen‐2‐yl)thieno[3,2‐b]thiophene (pBTTT) with phenyl‐c71‐butyric acid methyl ester (PC71BM), form bimolecular crystals due to fullerene intercalation between the polymer side chains. Here we present the determination of the eutectic pBTTT:PC71BM phase diagram using differential scanning calorimetry (DSC) and two‐dimensional grazing incidence X‐ray scattering (2D GIXS) with in‐situ thermal annealing. The phase diagram explains why the most efficient pBTTT:PC71BM solar cells have 75–80 wt % PC71BM since these blends lie in the center of the only room‐temperature phase region containing both electron‐conducting (PC71BM) and hole‐conducting (bimolecular crystal) phases. We show that intercalation can be suppressed in 50:50 pBTTT:PC71BM blends by using rapid thermal annealing to heat the blends above the eutectic temperature, which forces PC71BM out of the bimolecular crystal, followed by quick cooling to kinetically trap the pure PC71BM phase. © 2011 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2011  相似文献   
52.
Motivated by Khovanov homology and relations between the Jones polynomial and graph polynomials, we construct a homology theory for embedded graphs from which the chromatic polynomial can be recovered as the Euler characteristic. For plane graphs, we show that our chromatic homology can be recovered from the Khovanov homology of an associated link. We apply this connection with Khovanov homology to show that the torsion-free part of our chromatic homology is independent of the choice of planar embedding of a graph. We extend our construction and categorify the Bollobás-Riordan polynomial (a generalization of the Tutte polynomial to embedded graphs). We prove that both our chromatic homology and the Khovanov homology of an associated link can be recovered from this categorification.  相似文献   
53.
We report the development of an enhanced algorithm for the calculation of collision cross‐sections in combination with Travelling‐Wave ion mobility mass spectrometry technology and its optimisation and evaluation through the analysis of an organoruthenium anticancer complex [(η6‐biphenyl)RuII(en)Cl]+. Excellent agreement was obtained between the experimentally determined and theoretically determined collision cross‐sections of the complex and its major product ion formed via collision‐induced dissociation. Collision cross‐sections were also experimentally determined for adducts of this ruthenium complex with the single‐stranded oligonucleotide hexamer d(CACGTG). Ion mobility tandem mass spectrometry measurements have allowed the binding sites for ruthenium on the oligonucleotide to be determined. Copyright © 2009 John Wiley & Sons, Ltd.  相似文献   
54.
A two-step synthesis of 3-(2-chloropyrimidin-4-yl)imidazo[1,2-a]pyridines is presented. The late stage elaboration of the imidazopyridine through a cyclocondensation allows a rapid access to a variety of substitution patterns. The intermediate enol ethers were obtained from inexpensive reagents in a ligand-free Heck coupling. This methodology has been extended to the formation of pyrazolo[1,5-a]pyridines via a formal 1,3-dipolar cycloaddition.  相似文献   
55.
The three-dimensional conformation of a protein is an important property and plays a key role in its biological activity. We show here that ion mobility-mass spectrometry (IM-MS) can be used to detect conformational changes in the protein ubiquitin in the gas phase induced by reaction with the anticancer drug cisplatin. The primary adduct was ubiquitin-{Pt(NH3)2} under denaturing conditions. Up to three different conformations appear to be generated upon platination depending on the charge state. The collision cross-sections (Ω) for each conformation indicate that the conformations of the platinated protein are contracted in size compared with unmodified ubiquitin with generally smaller Ω values. Ion mobility-tandem MS allowed determination of the platinum binding site without a requirement for prior Chromatographic separation. A rapid 30-min digestion of cisplatin-modified ubiquitin with trypsin allowed the platination site to be identified as the N-terminal methionine following low-energy collision-induced dissociation (CID) studies of the modified peptide. The data were generated using a Traveling-Wave based ion mobility-MS approach. Such cisplatin-induced shape changes may have a significant effect on its function in vivo. This work highlights the usefulness of the ion-mobility mass spectrometry technique for shedding new light on such protein interactions.  相似文献   
56.
The analysis of diffusion NMR data in terms of distributions of diffusion coefficients is hampered by the ill-posed nature of the required inverse Laplace transformation. Na?ve approaches such as multiexponential fitting or standard least-squares algorithms are numerically unstable and often fail. This paper updates the CONTIN approach of the application of Tikhonov regularization to stabilise this numerical inversion problem and demonstrates two methods for automatically choosing the optimal value of the regularization parameter. These approaches are computationally efficient and easy to implement using standard matrix algebra techniques. Example analyses are presenting using both synthetic data and experimental results of diffusion NMR studies on the azo-dye sunset yellow and some polymer molecular weight reference standards.  相似文献   
57.
At the LHC and Tevatron strong initial-state radiation (ISR) plays an important role. It can significantly affect the partonic luminosity available to the hard interaction or contaminate a signal with additional jets and soft radiation. An ideal process to study ISR is isolated Drell-Yan production, pp → X?+ ?- without central jets, where the jet veto is provided by the hadronic event shape beam thrust τB. Most hadron collider event shapes are designed to study central jets. In contrast, requiring τ B < 1 provides an inclusive veto of central jets and measures the spectrum of ISR. For τ B < 1 we carry out a resummation of α s(n)ln(m)τ B corrections at next-to-next-to-leading-logarithmic order. This is the first resummation at this order for a hadron-hadron collider event shape. Measurements of τ B at the Tevatron and LHC can provide crucial tests of our understanding of ISR and of τ B's utility as a central jet veto.  相似文献   
58.
59.
Matrix application continues to be a critical step in sample preparation for matrix‐assisted laser desorption/ionization (MALDI) mass spectrometry imaging (MSI). Imaging of small molecules such as drugs and metabolites is particularly problematic because the commonly used washing steps to remove salts are usually omitted as they may also remove the analyte, and analyte spreading is more likely with conventional wet matrix application methods. We have developed a method which uses the application of matrix as a dry, finely divided powder, here referred to as dry matrix application, for the imaging of drug compounds. This appears to offer a complementary method to wet matrix application for the MALDI‐MSI of small molecules, with the alternative matrix application techniques producing different ion profiles, and allows the visualization of compounds not observed using wet matrix application methods. We demonstrate its value in imaging clozapine from rat kidney and 4‐bromophenyl‐1,4‐diazabicyclo(3.2.2)nonane‐4‐carboxylic acid from rat brain. In addition, exposure of the dry matrix coated sample to a saturated moist atmosphere appears to enhance the visualization of a different set of molecules. Copyright © 2010 John Wiley & Sons, Ltd.  相似文献   
60.
We discuss methods for solving medium to large-scale sparse least-squares problems on supercomputers, illustrating our remarks by experiments on the CRAY-2 supercomputer at Harwell. The method we are primarily concerned with is an augmented system approach which has the merit of both robustness and accuracy, in addition to a kernel operation that is just the solution of a symmetric indefinite system. We consider extensions to handle weighted and constrained problems, and include experiments on systems similar to those arising in the Karmarkar algorithm for linear programming. We indicate how recent improvements to the kernel software could greatly improve the performance of the least-squares code.This paper is based on an invited talk by the author at a Workshop on Supercomputers and Large-Scale Optimization held at the Minnesota Supercomputing Center on 16th to 18th May, 1988.  相似文献   
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