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31.
Sarma DD Ray S Tanaka K Kobayashi M Fujimori A Sanyal P Krishnamurthy HR Dasgupta C 《Physical review letters》2007,98(15):157205
We present magnetization (M) and magnetoresistance (MR) data for a series of Sr2FeMoO6 samples with independent control on antisite defect and grain-boundary densities, which reveal several unexpected features, including a novel switching-like behavior of MR with M. These, in conjunction with model calculations, establish that the MR in Sr2FeMoO6 is dominantly controlled by a new mechanism, derived from the magnetic polarization of grain-boundary regions acting like spin valves, leading to behavior qualitatively different from that usually encountered in tunneling MR. We show that a simple and useful experimental signature for the presence of this spin-valve-type MR (SVMR) is a wider hysteresis in MR compared to that in M. 相似文献
32.
We synthesized boron containing 2-(4-methoxybenzyl)-4-(4-(4,4,5,5-tetramethyl-1,3,2-dioaborolan-2-yl)phenyl) phthalazin-1(2H)-one 3 and 7-methyl-3-(4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)phenyl)-2H-benzo[b][1,4] oxazine 8. The reaction of compound 2 with B2pin2 using potassium acetate as the base and Pd(PPh3)2Cl2 as the catalyst, produced the corresponding boron-containing derivative 3 as a white solid in 65% yield. Alternatively, we have synthesized compound 8 as a yellow solid in 59% yield using the Miyaura borylation reaction. The potassium trifluoro(4-(-methyl-2H-benzo[b][1,4]oxazine-3-yl)phenylborate 9 was then obtained after treatment of 8 with aqueous solution of KF2H in methanol as white solid product in 60% yield. The biological activities of the synthetic compounds are currently being evaluated. 相似文献
33.
Gurkan Hizal Umit Tunca Amitav Sanyal 《Journal of polymer science. Part A, Polymer chemistry》2011,49(19):4103-4120
Functional polymeric materials with desired properties can be designed by precise control of macromolecular architectures. Over the recent years, click reactions have enabled efficient synthesis of a variety of polymers with different topologies via efficient polymer–polymer conjugations. While the copper catalyzed Huisgen type (3+2) dipolar cycloaddition between azide and alkyne has been widely used toward this goal, the Diels–Alder (DA) reaction offers an alternative click reaction that allow efficient macromolecular conjugations, oftentimes without the need of any additional reagent or catalyst. This article highlights, with illustrative examples, the power of the DA “click” reaction to efficiently synthesize a variety of different well‐defined macromolecular constructs in a modular fashion. © 2011 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2011 相似文献
34.
Agopcan S Çelebi-Ölçüm N Üçışık MN Sanyal A Aviyente V 《Organic & biomolecular chemistry》2011,9(23):8079-8088
In this study, the origins of diastereoselectivity in the hydrogen bonding assisted Diels-Alder reactions of chiral dienes with achiral dienophiles have been investigated with density functional methods. The distortion/interaction model has been applied to shed light on the origins of selectivity. C9-Substituted chiral anthracene templates (R = (CH(3))(OCH(3))(H), R = (CH(3))(OH)(H), R = (CH(3))(CH(2)CH(3))(H) and R = (-CH(2)-C(CH(3))(OCH(3))(H)) are used to rationalize the role of a stereogenic center and H-bonding on the product distribution ratio. Even though hydrogen bonding increases the reactivity of the diene, the stereoselectivity is reduced because of the hydrogen bonding capacity of both diastereomeric transition states. The interaction energies of the studied anthracene templates with N-methyl maleimide at the transition state correlate linearly with an increase in reactivity. The selectivity is determined by both favorable distortion and interaction energies. The π-facial selectivity induced by the presence of a chiral auxiliary in 1-substituted 1,3-pentadienes (R1 = (CH(3))(OCH(3))(H) and R1 = (CH(3))(OH)(H)) has also been modeled in order to rationalize the role of the stereogenic center and H-bonding on the stereoselectivity of an aliphatic diene. In both parts, the product distribution ratios calculated from Boltzmann distributions based on Gibbs free energies are in reasonable agreement with the experimental results. Finally the role of OH-substituted five-membered pyrrolidine on C9 of anthracene is investigated since the successful usage of the conformationally rigid pyrrolidines in asymmetric synthesis is well known. Overall, both in the acyclic system and in anthracene, the facilitation due to H-bonding is reflected in the interaction energies: the higher the difference in interaction energies in the transition structures of the two diastereomers, the more selective the H-bonding assisted Diels-Alder reaction is. 相似文献
35.
Sanyal R Cameron SA Brooker S 《Dalton transactions (Cambridge, England : 2003)》2011,40(45):12277-12287
An N(4) tetradentate [1 + 1] Schiff base metal free macrocycle HL was prepared, by 1?:?1 condensation of 2,2'-iminobisbenzaldehyde (1) and diethylenetriamine, and characterised. Seven mononuclear complexes, [Zn(II)L(py)](BF(4)) (2), [Cu(II)L](BF(4))]·H(2)O (3), [Ni(II)L](BF(4))·H(2)O (4), [Co(II)L](BF(4))]·H(2)O (5), Fe(III)L(BF(4))(2)·2H(2)O·MeCN (6), [Co(III)L(NCS)(2)]·0.3py (7) and [Fe(III)L(NCS)(2)] (8), of L(-) are reported. The Cu(II) and Ni(II) complexes were prepared by a template approach whereas the others were accessed by metallation of pre-formed HL. The X-ray crystal structure determinations show that [Cu(II)L](BF(4)) and [Ni(II)L](BF(4)) feature square planar N(4) coordinated Cu(II) and Ni(II) centres, respectively, whereas [Fe(III)L(NCS)(2)]·NO(2)Me features an octahedral N(6) coordinated Fe(III) centre (two NCS anions bound axially) and the Zn(II) complex, which crystallised as 2{[Zn(II)L(py)](BF(4))}·py, features square pyramidal Zn(II) ions (a pyridine molecule bound axially). In all cases the N(4) macrocycle is bound equatorially to the metal ion. Cyclic voltammograms of the soluble BF(4) complexes, 2-5, were carried out in MeCN vs. 0.01 mol L(-1) AgNO(3)/Ag and revealed multiple, mostly irreversible or quasi-reversible, redox processes. The Zn(II) complex 2 exhibited two irreversible oxidation processes and one irreversible reduction process, all of which are ligand-centered. The Ni(II) complex 4 showed a process with a weak return wave at E(m) = +0.57 V (ΔE = 0.05 V). Interestingly, after controlled potential coulometry experiments on 2, 3 and 4 (at +0.48, +0.61 and +0.71 V which transferred 1.2, 1.0 and 1.6 e(-) equiv. per complex, respectively), a new reversible or quasi-reversible process was obtained, with a lower potential than beforehand (E(m) (ΔE)/V = +0.16 (0.08), +0.31 (0.13) and +0.45 (0.11) respectively). 相似文献
36.
We will show that an uniform treatment yields Wiener–Tauberian type results for various Banach algebras and modules consisting of radial sections of some homogenous vector bundles on rank one Riemannian symmetric spaces G/K of noncompact type. One example of such a vector bundle is the spinor bundle. The algebras and modules we consider are natural generalizations of the commutative Banach algebra of integrable radial functions on G/K. The first set of them are Beurling algebras with analytic weights, while the second set arises due to Kunze–Stein phenomenon for noncompact semisimple Lie groups. 相似文献
37.
We present a complete theoretical analysis of the periodic and non-periodic travelling waves in a diatomic chain model, in
the continuum limit by incorporating nonlinear sixth order polarization potential (φ6) at the anion site. We have formulated a nonlinear lattice dynamical theory in which various energy curves are obtained for
different types and magnitudes of the core-shell force constants. For periodic solutions, we have obtained two types of commensurate
wave amplitudes which propagate in the opposite direction with respect to each other. For nonperiodic solutions, we have obtained
various travelling excitations such as kink, antikink, excitons etc. for different values of the mass ratio and velocity parameter.
The dipole moment per unit charge for SrTiO3 has been calculated and it is found that the nonlinear excitations in this model carry large amount of energy as compared
to those obtained from harmonic and anharmonic optical phonons in the φ4-polarizable model. 相似文献
38.
The phonon spectra of unstrained and strained quasiperiodic semiconductor superlattices (QSSL) have been calculated using
one-dimensional linear chain model. We consider two types of quasiperiodic systems, namely cantor triadic bar (CTB) and Fibonacci
sequences (FS), constituting of AlAs, GaAs and GaSb of which the latter two have a lattice mismatch of about 7%. The calculations
have been made using transfer matrix method and also with and without the inclusion of strain. We present the results on phonon
spectra of two component CTB and two as well as three component FS semiconductor superlattices (SSL), thickness and order
dependence on LO mode of GaAs, effect of strain on LO frequency of GaAs. The calculated results show that the strain generated
due to lattice mismatch reduces significantly the magnitudes of the confined optical phonon frequency of GaAs. 相似文献
39.
We have investigated the lattice vibrational properties of a two-component strained layer semiconductor superlattice (GaAs)
n1 (GaSb)
n2 using a one-dimensional linear chain model and transfer matrix method [1]. Effect of strain, arising due to the lattice mismatch
(∼ 7%) has been considered explicitly in the equation of motion. We show for the first time that the optical vibrational frequency
increases (in the case of (GaAs)4 (GaSb)
n
) or decreases (in the case of (GaAs)
n
(GaSb)4) with increase of layer thicknessn, in either type of superlattices. Raman scattering measurements on some other similar systems support our findings. 相似文献
40.
We have calculated the phonon and periodon dispersion relations in IV–VI semi-conducting bulk PbTe and SnTe and their superlattice
structure. The model used here is a one-dimensional lattice which includes harmonic interactions up to second neighbours as
well as on-site nonlinear electron-ion interactions at the anion site. We calculate the phonon and periodon dispersion relations
in bulk and PbTe-SnTe superlattice for the transverse optic and acoustic modes using the transfer matrix method. Our analysis
has predicted correct nature of the folding of acoustic and confinement of optical phonons at various frequency intervals
corresponding to pass and stop bands of the superlattices. 相似文献