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51.
52.
Mingfei Xiao Aditya Sadhanala Mojtaba Abdi-Jalebi Tudor H. Thomas Xinglong Ren Tao Zhang Hu Chen Remington L. Carey Qijing Wang Satyaprasad P. Senanayak Cameron Jellett Ada Onwubiko Maximilian Moser Hailiang Liao Wan Yue Iain McCulloch Mark Nikolka Henning Sirringhaus 《Advanced functional materials》2021,31(7):2007359
The measurement of the mechanical properties of conjugated polymers can reveal highly relevant information linking optoelectronic properties to underlying microstructures and the knowledge of the glass transition temperature (Tg) is paramount for informing the choice of processing conditions and for interpreting the thermal stability of devices. In this work, we use dynamical mechanical analysis to determine the Tg of a range of state-of-the-art conjugated polymers with different degrees of crystallinity that are widely studied for applications in organic field-effect transistors. We compare our measured values for Tg to the theoretical value predicted by a recent work based on the concept of effective mobility ζ. The comparison shows that for conjugated polymers with a modest length of the monomer units, the Tg values agree well with theoretically predictions. However, for the near-amorphous, indacenodithiophene–benzothiadiazole family of polymers with more extended backbone units, values for Tg appear to be significantly higher, predicted by theory. However, values for Tg are correlated with the sub-bandgap optical absorption suggesting the possible role of the interchain short contacts within materials’ amorphous domains. 相似文献
53.
Aditya Mishra Masoud Alahbakhshi Ross Haroldson Qing Gu Anvar A. Zakhidov Jason D. Slinker 《Advanced functional materials》2021,31(31):2102006
Blue electroluminescence is highly desired for emerging light-emitting devices for display applications and optoelectronics in general. However, saturated, efficient, and stable blue emission has been challenging to achieve, particularly in mixed-halide perovskites, where intrinsic ion motion and halide segregation compromises spectral purity. Here, CsPbBr3−xClx perovskites, polyelectrolytes, and a salt additive are leveraged to demonstrate pure blue emission from single-layer light-emitting electrochemical cells (LECs). The electrolytes transport the ions from salt additives, enhancing charge injection and stabilizing the inherent perovskite emissive lattice for highly pure and sustained blue emission. Substituting Cl into CsPbBr3 tunes the perovskite luminescence from green through blue. Sky blue and saturated blue devices produce International Commission on Illumination coordinates of (0.105, 0.129) and (0.136, 0.068), respectively, with the latter meeting the US National Television Committee standard for the blue primary. Likewise, maximum luminances of 2900 and 1000 cd m−2, external quantum efficiencies (EQEs) of 4.3% and 3.9%, and luminance half-lives of 5.7 and 4.9 h are obtained for sky blue and saturated blue devices, respectively. Polymer and LiPF6 inclusion increases photoluminescence efficiency, suppresses halide segregation, induces thin-film smoothness and uniformity, and reduces crystallite size. Overall, these devices show superior performance among blue perovskite light-emitting diodes (PeLEDs) and general LECs. 相似文献
54.
Aditya Kaushik 《Journal of Difference Equations and Applications》2016,22(9):1307-1324
The convection dominated diffusion problems are studied. Higher order accurate numerical methods are presented for problems in one and two dimensions. The underlying technique utilizes a superposition of given problem into two independent problems. The first one is the reduced problem that refers to the outer or smooth solution. Stretching transformation is used to obtain the second problem for inner layer solution. The method considered for outer or degenerate problems are based on higher order Runge–Kutta methods and upwind finite differences. However, inner problem is solved analytically or asymptotically. The schemes presented are proved to be consistent and stable. Possible extensions to delay differential equations and to nonlinear problems are outlined. Numerical results for several test examples are illustrated and a comparative analysis is presented. It is observed that the method presented is highly accurate and easy to implement. Moreover, the numerical results obtained are not only comparable with the exact solution but also in agreement with the theoretical estimates. 相似文献
55.
Hogenauer TJ Wang Q Sanki AK Gammon AJ Chu CH Kaneshiro CM Kajihara Y Michael K 《Organic & biomolecular chemistry》2007,5(5):759-762
Under slightly basic or neutral reaction conditions peptide-alpha-thioesters are photochemically synthesized from peptide-alpha-nitroindoline precursors, either in solution, or by direct photorelease from a solid support. 相似文献
56.
Bhan A Allian AD Sunley GJ Law DJ Iglesia E 《Journal of the American Chemical Society》2007,129(16):4919-4924
The acid-catalyzed formation of carbon-carbon bonds from C1 precursors via CO insertion into chemisorbed methyl groups occurs selectively within eight-membered ring (8-MR) zeolite channels. This elementary step controls catalytic carbonylation rates of dimethyl ether (DME) to methyl acetate. The number of O-H groups within 8-MR channels was measured by rigorous deconvolution of the infrared bands for O-H groups in cation-exchanged and acid forms of mordenite (M,H-MOR) and ferrierite (H-FER) after adsorption of basic probe molecules of varying size. DME carbonylation rates are proportional to the number of O-H groups within 8-MR channels. Na+ cations selectively replaced protons within 8-MR channels and led to a disproportionate decrease in carbonylation turnover rates (per total H+). These conclusions are consistent with the low or undetectable rates of carbonylation on zeolites without 8-MR channels (H-BEA, H-FAU, H-MFI). Such specificity of methyl reactivity upon confinement within small channels appears to be unprecedented in catalysis by microporous solids, which typically select reactions by size exclusion of bulkier transition states. 相似文献
57.
We experimentally probe molecular ionization and dissociation of methane molecules in the gas phase upon their irradiation by intense pulses of white light that spans the wavelength range 500-850 nm. White light pulses are generated upon irradiation of BK7 glass by 36-fs-long pulses of intense 820 nm laser light. Comparison is made of the molecular fragmentation patterns obtained using white light that is depolarized with those obtained using single-color (820 nm) light that is highly chirped. On the basis of such comparison, we make hitherto-unavailable estimates of the in situ intensity of white light pulses. Results obtained using white light also indicate that resonances apparently do not play any role in the ionization dynamics that ensue upon irradiation by intense, broadband light; neither are the dynamics affected by the polarization properties of the 820 nm light that is used to generate the white light. 相似文献
58.
59.
Electroviscous stresses arise as hydrodynamic flows disturb the ionic (Debye) clouds that screen charged surfaces in electrolyte solutions. The contribution thereof to the effective bulk viscosity (also known as the second or volume viscosity) of two-phase suspensions is quantified here. Specifically, the bulk viscosity of two model suspensions is calculated: (1) a dilute dispersion of rigid charged spherical particles immersed in a compressible electrolyte that undergoes uniform dilatation and (2) a dilute suspension of charged gas bubbles expanding uniformly in an incompressible electrolyte. In both cases, it is assumed that the fluid flow only slightly drives the Debye cloud out of equilibrium, which formally requires that the ratio of the ion diffusion to flow time scales—a Péclet number—is small. For a suspension of rigid particles, the electroviscous contribution to the effective bulk viscosity is proportional to the particle volume fraction and decreases monotonically as the ratio of the particle radius to the Debye length increases. Similar behavior is well known for the electroviscous contribution to the effective shear viscosity of a dilute hard-sphere suspension; a quantitative comparison between the bulk and shear viscosities is made. In contrast, the electroviscous contribution to the bulk viscosity of a dilute suspension of bubbles is independent of the bubble volume fraction and attains a finite value in the limit of vanishing Debye length. 相似文献
60.
Kulkarni A DeFrees K Hyun SH Thompson DH 《Journal of the American Chemical Society》2012,134(18):7596-7599
A novel siRNA delivery vector has been developed, based on the self-assembly of monosubstituted cationic β-CD derivatives with a poly(vinyl alcohol)MW27kD (PVA) main-chain polymer bearing poly(ethylene glycol)MW2000 (PEG) and acid-labile cholesterol-modified (Chol) grafts through an acid-sensitive benzylidene acetal linkage. These components were investigated for their ability to form nanoparticles with siRNA using two different assembly schemes, involving either precomplexation of the pendant Chol-PVA-PEG polymer with the cationic β-CD derivatives before siRNA condensation or siRNA condensation with the cationic β-CD derivatives prior to addition of Chol-PVA-PEG to engage host:guest complexation. The pendant polymer:amino-β-CD:siRNA complexes were shown to form nanoparticles in the size range of 120-170 nm, with a slightly negative zeta potential. Cell viability studies in CHO-GFP cells shows that these materials have 10(3)-fold lower cytotoxicities than 25 kD bPEI, while maintaining gene-silencing efficiencies that are comparable to those of benchmark transfection reagents such as bPEI and Lipofectamine 2000. These results suggest that the degradable Chol-PVA-PEG polymer is able to self-assemble in the presence of siRNA and cationic-β-CD to form nanoparticles that are an effective and low-toxicity vehicle for delivering siRNA cargo to target cells. 相似文献