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91.
Steffen M. Brülls Dr. Valentina Cantatore Zhenping Wang Dr. Pui Lam Tam Dr. Per Malmberg Jessica Stubbe Prof. Dr. Biprajit Sarkar Prof. Dr. Itai Panas Prof. Dr. Jerker Mårtensson Prof. Dr. Siegfried Eigler 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(29):6694-6702
Hybridizing graphene and molecules possess a high potential for developing materials for new applications. However, new methods to characterize such hybrids must be developed. Herein, the wet-chemical non-covalent functionalization of graphene with cationic π-systems is presented and the interaction between graphene and the molecules is characterized in detail. A series of tricationic benzimidazolium salts with various steric demand and counterions was synthesized, characterized and used for the fabrication of graphene hybrids. Subsequently, the doping effects were studied. The molecules are adsorbed onto graphene and studied by Raman spectroscopy, XPS as well as ToF-SIMS. The charged π-systems show a p-doping effect on the underlying graphene. Consequently, the tricationic molecules are reduced through a partial electron transfer process from graphene, a process which is accompanied by the loss of counterions. DFT calculations support this hypothesis and the strong p-doping could be confirmed in fabricated monolayer graphene/hybrid FET devices. The results are the basis to develop sensor applications, which are based on analyte/molecule interactions and effects on doping. 相似文献
92.
Adsorption, desorption, and surface-promoted hydrolysis of glucose-1-phosphate in aqueous goethite (α-FeOOH) suspensions 总被引:2,自引:0,他引:2
Olsson R Giesler R Loring JS Persson P 《Langmuir : the ACS journal of surfaces and colloids》2010,26(24):18760-18770
Adsorption, desorption, and precipitation reactions at environmental interfaces govern the fate of phosphorus in terrestrial and aquatic environments. Typically, a substantial part of the total pool of phosphorus consists of organophosphate, and in this study we have focused on the interactions between glucose-1-phosphate (G1P) and goethite (α-FeOOH) particles. The adsorption and surface-promoted hydrolysis reactions have been studied at room temperature as a function of pH, time, and total concentration of G1P by means of quantitative batch experiments in combination with infrared spectroscopy. A novel simultaneous infrared and potentiometric titration (SIPT) technique has also been used to study the rates and mechanisms of desorption of the surface complexes. The results have shown that G1P adsorption occurs over a wide pH interval and at pH values above the isoelectric point of goethite (IEP(goethite) = 9.4), indicating a comparatively strong interaction with the particle surfaces. As evidenced by IR spectroscopy, G1P formed pH-dependent surface complexes on goethite, and investigations of both adsorption and desorption processes were consistent with a model including three types of surface complexes. These complexes interact monodentately with surface Fe but differ in hydrogen bonding interactions via the auxiliary oxygens of the phosphate group. The apparent desorption rates were shown to be influenced by reaction pathways that include interconversion of surface species, which highlights the difficulty in determining the intrinsic desorption rates of individual surface complexes. Desorption results have also indicated that the molecular structures of surface complexes and the surface charge are two important determinants of G1P desorption rates. Finally, this study has shown that surface-promoted hydrolysis of G1P by goethite is base-catalyzed but that the extent of hydrolysis was small. 相似文献
93.
Per Flodin 《Macromolecular Symposia》1988,17(1):213-220
Chemically crosslinked gels made by polymerization and copolymerization of trimethylolpropane trimethacrylate have been characterized. Bimodal pore size distributions were obtained. The radii of the large pores (100 Å to 1 μm) varied with concentration while the small ones (20 to 30 Å) were largely independent of the concentration of TRIM. A mechanism of formation of the pores is outlined. Physically crosslinked gels of polyacrylonitrile with highly porous structures were made by cooling polymer solutions in DMF containing varying amounts of water. By controlling the thermal treatment the pore sizes could be varied from 0.1 to 1 μm. Finally the surface modification of cellulose fibers with derivatives of dichlorotriazine is described. It is shown that derivatives containing double bonds in the side chain can form covalent bonds across the interface between cellulose and an unsaturated polyester. 相似文献
94.
In this paper we discuss how partial knowledge of the density of states for a model can be used to give good approximations
of the energy distributions in a given temperature range. From these distributions one can then obtain the statistical moments
corresponding to e.g. the internal energy and the specific heat. These questions have gained interest apropos of several recent
methods for estimating the density of states of spin models. As a worked example we finally apply these methods to the 3-state
Potts model for cubic lattices of linear order up to 128. We give estimates of e.g. latent heat and critical temperature,
as well as the micro-canonical properties of interest.
相似文献
95.
Erik Allard Rikard Åslund Tröger Björn Arvidsson Per Johan Ragnar Sjöberg 《Rapid communications in mass spectrometry : RCM》2010,24(4):429-435
Precision, reproducibility and lower limit of quantitation (LLOQ) are important characteristics of a quantitative method. We have investigated these properties for Ximelagatran (Xi), which has a high tendency to form doubly charged ions in electrospray ionization (ESI), by studying the percentage of doubly charged species formed when varying the formic acid (FA) concentration, analyte concentration, amount of organic modifier and flow rate. It was found that the percentage of [Xi + 2H]2+ can be controlled to be more than 90% or less than 10% by varying the amount of FA present, and that the change between these values is dramatic. Furthermore, the percentage of [Xi + 2H]2+ formed decreases with increased analyte concentration and increased flow rate. No apparent relationship with the amount of organic modifier was found. The results have the implication that, by carefully controlling the selected parameters, the LLOQ, precision and reproducibility can be improved. We have compared the fragmentation of the singly and doubly charged species and concluded that the [Xi + 2H]2+ ion is more inclined to undergo fragmentation than [Xi + H]+. As a consequence, unusual instrumental settings had to be used for the experiments. The fragmentation patterns are to a great extent similar, but the doubly charged species is more inclined to generate low‐mass product ions. Copyright © 2010 John Wiley & Sons, Ltd. 相似文献
96.
Reversible addition–fragmentation chain transfer polymerization of alkyl‐2‐cyanoacrylates: An assessment of livingness 下载免费PDF全文
Cormac Duffy Marisa Phelan Per B. Zetterlund Fawaz Aldabbagh 《Journal of polymer science. Part A, Polymer chemistry》2017,55(8):1397-1408
Alkyl 2‐cyanoacrylates (CAs) are primarily used as instant adhesives, including those sold under the Loctite brand. The adhesive action can be inhibited with acid stabilizers allowing radical polymerization to be employed. The following article details the first attempted controlled/living radical polymerization of alkyl CAs: Reversible addition fragmentation chain transfer (RAFT) polymerization mediated by a poly(methyl methacrylate) dithiobenzoate macroRAFT agent for three different CA monomers (ethyl 2‐cyanoacrylate, n‐butyl 2‐cyanoacrylate, and 2‐phenylethyl cyanoacrylate) allowed the preparation of the first block copolymers of this challenging but commercially important monomer class. Nevertheless, GPC with UV detection indicated significant loss of the RAFT end‐group for all three CAs limiting control/living character. © 2016 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2017 , 55, 1397–1408 相似文献
97.
Per JensenSteven S. Wesolowski Nicole R. BrinkmannNancy A. Richardson Yukio YamaguchiHenry F. Schaefer III P.R. Bunker 《Journal of Molecular Spectroscopy》2002,211(2):254-261
The potential energy surface and dipole moment surfaces of the ã4A2 electronic state of CH2+ are calculated ab initio using an augmented correlation-consistent polarized valence quadruple-ζ (aug-cc-pVQZ) basis set, with the incorporation of dynamical correlation using the coupled cluster method with single and double excitations and perturbatively connected triple excitations [CCSD(T)]. We use these surfaces in the MORBID program system to calculate rotation and rotation-vibration term values for ã-state CH2+, CD+2, and CHD+ and to simulate the rotation and rotation-vibration absorption spectrum of CH2+ in the ã4A2 electronic state. Our work is motivated by studies of CH2+ that use the Coulomb explosion imaging technique and by the goal of predicting spectra that may be obtained from discharge sources. Although the ã state is the lowest-lying excited state above the X?/Ã ground state pair, it turns out to be relatively high-lying, and we determine that Te(ã)=30447.5 cm−1. The equilibrium bond angle for ã-state CH2+ is only 77.1°; as a result the asymmetric top κ value is close to 0, and the molecule is equally far from the oblate and prolate symmetric top limits in this electronic state. 相似文献
98.
Jensen P Odaka TE Kraemer WP Hirano T Bunker PR 《Spectrochimica acta. Part A, Molecular and biomolecular spectroscopy》2002,58(4):763-794
We have developed a computational procedure, based on the variational method, for the calculation of the rovibronic energies of a triatomic molecule in an electronic state that become degenerate at the linear nuclear configuration. In such an electronic state the coupling caused by the electronic orbital angular momentum is very significant and it is called the Renner effect. We include it, and the effect of spin-orbit coupling, in our program. We have developed the procedure to the point where spectral line intensities can be calculated so that absorption and emission spectra can be simulated. In order to gain insight into the nature of the eigenfunctions, we have introduced and calculated the overall bending probability density function f(p) of the states. By projecting the eigenfunctions onto the Born-Oppenheimer basis, we have determined the probability density functions f+(rho) and f-(rho) associated with the individual Born-Oppenheimer states phi(-)elec and phi(+)elec. At a given temperature the Boltzmann averaged value of the f(p) over all the eigenstates gives the bending probability distribution function F(rho), and this can be related to the result of a Coulomb Explosion Imaging (CEI) experiment. We review our work and apply it to the molecules CH2+, MgNC and NH2, all of which are of astrophysical interest. 相似文献
99.
100.
Kristiansen PE Mitchell DJ Evans JN 《Journal of magnetic resonance (San Diego, Calif. : 1997)》2002,157(2):253-266
A full investigation of the possible homonuclear double-quantum recoupling sequences, based on the RN family of sequences with N < or = 20, is given. Several new RN sequences, R16(6)(5), R18(8)(5), and R18(10)(5), were applied at high magic-angle spinning rates and compared with theory. The R18(10)(5) technique can be used to recouple dipolar couplings at spinning rates up to 39 kHz, and the application of the sequence in an INADEQUATE experiment is shown for a spinning rate of 30 kHz. 相似文献