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141.
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143.
The absorption spectra and excited state dipole moments of four differently substituted fulvenes have been investigated both experimentally and computationally. The results reveal that the excited state dipole moment of fulvenes reverses in the first excited singlet state when compared to the ground state. The oppositely polarized electron density distributions, which dominate the ground state and the first excited singlet state of fulvenes, respectively, reflect the reversed π-electron counting rules for aromaticity in the two states (4n + 2 vs. 4n, respectively). The results show that substituents indeed influence the polarity of fulvenes in the two states, however, cooperative interactions between the substituents and the fulvene moiety are most pronounced in the ground state. 相似文献
144.
Buschmann H Dölle J Berendts S Kuhn A Bottke P Wilkening M Heitjans P Senyshyn A Ehrenberg H Lotnyk A Duppel V Kienle L Janek J 《Physical chemistry chemical physics : PCCP》2011,13(43):19378-19392
The solid lithium-ion electrolyte "Li(7)La(3)Zr(2)O(12)" (LLZO) with a garnet-type structure has been prepared in the cubic and tetragonal modification following conventional ceramic syntheses routes. Without aluminium doping tetragonal LLZO was obtained, which shows a two orders of magnitude lower room temperature conductivity than the cubic modification. Small concentrations of Al in the order of 1 wt% were sufficient to stabilize the cubic phase, which is known as a fast lithium-ion conductor. The structure and ion dynamics of Al-doped cubic LLZO were studied by impedance spectroscopy, dc conductivity measurements, (6)Li and (7)Li NMR, XRD, neutron powder diffraction, and TEM precession electron diffraction. From the results we conclude that aluminium is incorporated in the garnet lattice on the tetrahedral 24d Li site, thus stabilizing the cubic LLZO modification. Simulations based on diffraction data show that even at the low temperature of 4 K the Li ions are blurred over various crystallographic sites. This strong Li ion disorder in cubic Al-stabilized LLZO contributes to the high conductivity observed. The Li jump rates and the activation energy probed by NMR are in very good agreement with the transport parameters obtained from electrical conductivity measurements. The activation energy E(a) characterizing long-range ion transport in the Al-stabilized cubic LLZO amounts to 0.34 eV. Total electric conductivities determined by ac impedance and a four point dc technique also agree very well and range from 1 × 10(-4) Scm(-1) to 4 × 10(-4) Scm(-1) depending on the Al content of the samples. The room temperature conductivity of Al-free tetragonal LLZO is about two orders of magnitude lower (2 × 10(-6) Scm(-1), E(a) = 0.49 eV activation energy). The electronic partial conductivity of cubic LLZO was measured using the Hebb-Wagner polarization technique. The electronic transference number t(e-) is of the order of 10(-7). Thus, cubic LLZO is an almost exclusive lithium ion conductor at ambient temperature. 相似文献
145.
Crounse JD Paulot F Kjaergaard HG Wennberg PO 《Physical chemistry chemical physics : PCCP》2011,13(30):13607-13613
We report experimental evidence for the formation of C(5)-hydroperoxyaldehydes (HPALDs) from 1,6-H-shift isomerizations in peroxy radicals formed from the hydroxyl radical (OH) oxidation of 2-methyl-1,3-butadiene (isoprene). At 295 K, the isomerization rate of isoprene peroxy radicals (ISO2?) relative to the rate of reaction of ISO2? + HO2 is k(isom)(295)/(k(ISO2?+HO2)(295)) = (1.2 ± 0.6) x 10(8) mol cm(-3), or k(isom)(295) ? 0.002 s(-1). The temperature dependence of this rate was determined through experiments conducted at 295, 310 and 318 K and is well described by k(isom)(T)/(k(ISO2?+HO2)(T)) = 2.0 x 10(21) exp(-9000/T) mol cm(-3). The overall uncertainty in the isomerization rate (relative to k(ISO2?+HO2)) is estimated to be 50%. Peroxy radicals from the oxidation of the fully deuterated isoprene analog isomerize at a rate ~15 times slower than non-deuterated isoprene. The fraction of isoprene peroxy radicals reacting by 1,6-H-shift isomerization is estimated to be 8-11% globally, with values up to 20% in tropical regions. 相似文献
146.
Bruus H 《Lab on a chip》2011,11(22):3742-3751
In Part 1 of the thematic tutorial series "Acoustofluidics--exploiting ultrasonic standing waves forces and acoustic streaming in microfluidic systems for cell and particle manipulation", we establish the governing equations in microfluidics. Examples of basic flow solutions are presented, and equivalent circuit modeling for determining flow rates in microfluidic networks is introduced. 相似文献
147.
Boris Andreianov Kenneth Hvistendahl Karlsen Nils Henrik Risebro 《Archive for Rational Mechanics and Analysis》2011,201(1):27-86
We propose a general framework for the study of L
1 contractive semigroups of solutions to conservation laws with discontinuous flux:
$ u_t + \mathfrak{f}(x,u)_x=0, \qquad \mathfrak{f}(x,u)= \left\{{ll} f^l(u),& x < 0,\\ f^r(u), & x > 0, \right.\quad\quad\quad (\rm CL) $ u_t + \mathfrak{f}(x,u)_x=0, \qquad \mathfrak{f}(x,u)= \left\{\begin{array}{ll} f^l(u),& x < 0,\\ f^r(u), & x > 0, \end{array} \right.\quad\quad\quad (\rm CL) 相似文献
148.
Martin Månsson Oscar Tjernberg Tomas Claesson Henrik S. Karlsson Ulf O. Karlsson 《Applied Surface Science》2006,252(15):5308-5311
Transiently excited electron states at the GaSb(0 0 1) surface have been studied by means of time- and angle-resolved photoemission spectroscopy based on a femtosecond laser system. A normally unpopulated surface electron state has been found at ∼250 meV above the valence band maximum with a strong confinement at the center of the surface Brillouin zone. The lifetime of transiently excited carriers at the intergap surface states has been found to be ∼11 ps, associated with rapid carrier diffusion. 相似文献
149.
Johan Nilsson Hans-Peter Eckle Henrik Johannesson 《Czechoslovak Journal of Physics》2006,56(10-11):1251-1256
We consider the problem of a persistent current in a one-dimensional mesoscopic ring with the electrons coupled by a spin exchange to a magnetic impurity. We show that this problem can be mapped onto an integrable model with a quadratic dispersion (with the latter property allowing for an unambiguous definition of the persistent current). We have solved the model exactly by a Bethe ansatz and found that the current is insensitive to the presence of the impurity. We conjecture that this result holds for any integrable quantum impurity model with an electronic dispersionε(k) that is an even function ofk. 相似文献
150.
We present new numerical methods for constructing approximate solutions to the Cauchy problem for Hamilton–Jacobi equations of the form ut+H(Dxu)=0. The methods are based on dimensional splitting and front tracking for solving the associated (non-strictly hyperbolic) system of conservation laws pt+DxH(p)=0, where p=Dxu. In particular, our methods depend heavily on a front tracking method for one-dimensional scalar conservation laws with discontinuous coefficients. The proposed methods are unconditionally stable in the sense that the time step is not limited by the space discretization and they can be viewed as “large-time-step” Godunov-type (or front tracking) methods. We present several numerical examples illustrating the main features of the proposed methods. We also compare our methods with several methods from the literature. 相似文献
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