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91.
We study the nature of the smectic–isotropic phase transition using a mobile 6-state Potts model. Each Potts state represents a molecular orientation. We show that with the choice of an appropriate microscopic Hamiltonian describing the interaction between individual molecules modeled by a mobile 6-state Potts spins, we observe the smectic phase dynamically formed when we cool the molecules from the isotropic phase to low temperatures (T). In order to elucidate the order of the transition and the low-T properties, we use the high-performance Wang–Landau flat energy-histogram technique. We show that the smectic phase goes to the liquid (isotropic) phase by melting/evaporating layer by layer starting from the film surface with increasing T. At a higher T, the whole remaining layers become orientationally disordered. The melting of each layer is characterized by a peak of the specific heat. Such a succession of partial transitions cannot be seen by the Metropolis algorithm. The successive layer meltings/evaporations at low T are found to have a first-order character by examining the energy histogram. These results are in agreement with experiments performed on some smectic liquid crystals. 相似文献
92.
The task of reconstructing the system’s state from the measurements results, known as the Pauli problem, usually requires repetition of two successive steps. Preparation in an initial state to be determined is followed by an accurate measurement of one of the several chosen operators in order to provide the necessary “Pauli data”. We consider a similar yet more general problem of recovering Feynman’s transition (path) amplitudes from the results of at least three consecutive measurements. The three-step histories of a pre- and post-selected quantum system are subjected to a type of interference not available to their two-step counterparts. We show that this interference can be exploited, and if the intermediate measurement is “fuzzy”, the path amplitudes can be successfully recovered. The simplest case of a two-level system is analysed in detail. The “weak measurement” limit and the usefulness of the path amplitudes are also discussed. 相似文献
93.
《中国化学快报》2020,31(11):2897-2902
Directly monitoring mitophagy-specific viscosity dynamic in living cells is of great significance but remains challenging. Herein, this study reported a novel mitochondria-targeted fluorescent probe DPAC-DY based on vibration-induced emission (VIE) for monitoring viscosity changes during mitochondrial autophagy. This probe contained N,N'-diphenyl- dihydrodibenzo[a,c]phenazine (DPAC) as the VIE core and two positively charged pyridinium moieties for mitochondria anchoring. As the ambient viscosity increased, the vibration of DPAC-DY could be hindered, and subsequently resulting in the enhancement of fluorescence emission. In vitro and intracellular experiments indicated that the probe DPAC-DY showed highly sensitive response to viscosity due to VIE mechanism. Importantly, by virtue of this probe, in situ and real-time visualization of the specific viscosity dynamics during the mitochondrial autophagy process was achieved. Thus, this work provides a novel strategy for VIE-based viscosity response sensors applied to specific organelles and offers a platform for in-depth study of mitochondrial viscosity-related diseases. 相似文献
94.
Novel highly sensitive chiral organic field-effect transistors(COFET)were developed by directly assembling imidazolium3,5-dimethylphenylcabamoylated-β-cyclodextrin(lm^+-Ph-β-CD)and 3,5-dimethylphenylcarbamoylated-β-CD(Ph-β-CD)respectively onto the semiconductor layer as sensing units.The Im+-Ph-β-CD/COFET afforded better enantioselectivity and a lowest detection concentration of10^-18 L/mol as well as the potentiality in quantitative analysis of commercial medicines. 相似文献
95.
Dr. Victor de Seauve Dr. Marie-Angélique Languille Dr. Mathieu Kociak Dr. Stéphanie Belin Dr. James Ablett Prof. Christine Andraud Prof. Odile Stéphan Dr. Jean-Pascal Rueff Dr. Emiliano Fonda Prof. Bertrand Lavédrine 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(23):9198-9204
The first colour photographs were created by a process introduced by Edmond Becquerel in 1848. The nature of these photochromatic images colours motivated a debate between scientists during the XIXth century, which is still not settled. We present the results of chemical analysis (EDX, HAXPES and EXAFS) and morphology studies (SEM, STEM) aiming at explaining the optical properties of the photochromatic images (UV-visible spectroscopy and low loss EELS). We rule out the two hypotheses (pigment and interferences) that have prevailed since 1848, respectively based on variations in the oxidation degree of the compound forming the sensitized layer and periodically spaced photolytic silver planes. A study of the silver nanoparticles dispersions contained in the coloured layers showed specific localizations and sizes distributions of the nanoparticles for each colour. These results allow us to formulate a plasmonic hypothesis on the origin of the photochromatic images colours. 相似文献
96.
Jianxin Guan Rong Wei Antonio Prlj Jie Peng Kun-Han Lin Jitian Liu Han Han Prof. Clémence Corminboeuf Prof. Dahui Zhao Prof. Zhihao Yu Prof. Junrong Zheng 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(35):15013-15019
The mechanism of aggregation-induced emission, which overcomes the common aggregation-caused quenching problem in organic optoelectronics, is revealed by monitoring the real time structural evolution and dynamics of electronic excited state with frequency and polarization resolved ultrafast UV/IR spectroscopy and theoretical calculations. The formation of Woodward–Hoffmann cyclic intermediates upon ultraviolet excitation is observed in dilute solutions of tetraphenylethylene and its derivatives but not in their respective solid. The ultrafast cyclization provides an efficient nonradiative relaxation pathway through crossing a conical intersection. Without such a reaction mechanism, the electronic excitation is preserved in the molecular solids and the molecule fluoresces efficiently, aided by the very slow intermolecular charge and energy transfers due to the well separated molecular packing arrangement. The mechanisms can be general for tuning the properties of chromophores in different phases for various important applications. 相似文献
97.
Lei Xu Chao Wang Yan-Xiang Li Xun-Hui Xu Dr. Li Zhou Dr. Na Liu Prof. Dr. Zong-Quan Wu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(38):16818-16825
Controlling the self-assembly morphology of π-conjugated block copolymer is of great interesting. Herein, amphiphilic poly(3-hexylthiophene)-block-poly(phenyl isocyanide)s (P3HT-b-PPI) copolymers composed of π-conjugated P3HT and optically active helical PPI segments were readily prepared. Taking advantage of the crystallizable nature of P3HT and the chirality of the helical PPI segment, crystallization-driven asymmetric self-assembly (CDASA) of the block copolymers lead to the formation of single-handed helical nanofibers with controlled length, narrow dispersity, and well-defined helicity. During the self-assembly process, the chirality of helical PPI was transferred to the supramolecular assemblies, giving the helical assemblies large optical activity. The single-handed helical assemblies of the block copolymers exhibited interesting white-light emission and circularly polarized luminescence (CPL). The handedness and dissymmetric factor of the induced CPL can be finely tuned through the variation on the helicity and length of the helical nanofibers. 相似文献
98.
Dr. Haoxuan Li Haifei Wen Dr. Zhijun Zhang Dr. Nan Song Prof. Ryan T. K. Kwok Prof. Jacky W. Y. Lam Prof. Lei Wang Prof. Dong Wang Prof. Ben Zhong Tang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(46):20551-20555
Using reverse thinking of the aggregation-induced emission (AIE) principle, we demonstrate an ingenious and universal protocol for amplifying molecular motions to boost photothermal efficiency of fibers. Core–shell nanofibers having the olive oil solution of AIE-active molecules as the core surrounded by PVDF-HFP shell were constructed by coaxial electrospinning. The molecularly dissolved state of AIE-active molecules allows them to freely rotate and/or vibrate in nanofibers upon photoexcitation and thus significantly elevates the proportion of non-radiative energy dissipation, affording impressive heat-generating efficiency. Photothermal evaluation shows that the core–shell nanofibers with excellent durability can reach up to 22.36 % of photothermal conversion efficiency, which is 26-fold as the non-core–shell counterpart. Such a core–shell fiber can be used for photothermal textiles and solar steam generation induced by natural sunlight with green and carbon-zero emission. 相似文献
99.
The electronic (energy gap and work function) as well as electrical properties (dipole moment, polarizability, and first hyperpolarizabilities) of the first-row transition metals decorated C24N24 cavernous nitride fullerene were explored using DFT calculations. The transition metals are decorated at N4 cavity of C24N24 fullerene. According to our spin polarized computations, the most stable spin state monotonically increases to sextet for Mn@C24N24 and thereafter dropped off gradually to singlet state for Zn@C24N24 system. The findings demonstrate that transition metals can remarkably decrease the HOMO-LUMO energy gap and work function values up to 63% and 21% of bare C24N24, respectively. As can be seen, when the Sc and Ti metals are located above the N4 cavity of fullerene, systems of enhanced static hyperpolarizabilities (β0) are delivered. These findings might provide an effective strategy to design high performance eletcro-optical materials based on carbon- nitride fullerene. 相似文献