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81.
We have studied the motion of charge carriers along isolated phenylene-vinylene (PV) chains using a combination of experimental and theoretical methods. The conductive properties of positive charges along PV chains in dilute solution were studied by using the pulse-radiolysis time-resolved microwave conductivity (TRMC) technique. This technique enables the measurement of high-frequency (tens of GHz) charge carrier mobilities along isolated PV chains without the use of electrodes. The charge carrier mobility along PV chains with finite and infinite length was studied theoretically by charge transport simulations with parameters from density functional theory (DFT) calculations. The high-frequency charge carrier mobility is found to depend strongly on the conjugation length of the PV chains and is found to increase both with increasing length of the PV chain and with increasing conjugation fraction. The experimental results are in good agreement with the calculated results. On the basis of this combined experimental and theoretical study an intrachain charge carrier mobility of a few tens of cm2/Vs is expected for an infinitely long PV chain without conjugation breaks. 相似文献
82.
Dr. Lydia M. Peschel Carina Vidovič Dr. Ferdinand Belaj Dr. Dmytro Neshchadin Prof. Nadia C. Mösch-Zanetti 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(15):3893-3902
The synthesis and structural determination of four tungsten alkyne complexes coordinated by the bio-inspired S,N-donor ligand 2-(4′,4′-dimethyloxazoline-2′-yl)thiophenolate (S-Phoz) is presented. A previously established protocol that involved the reaction of the respective alkyne with the bis-carbonyl precursor [W(CO)2(S-Phoz)2] was used for the complexes [W(CO)(C2R2)(S-Phoz)2] (R=H, 1 a ; Me, 1 b ; Ph, 1 c ). Oxidation with pyridine-N-oxide gave the corresponding W-oxo species [WO(C2R2)(S-Phoz)2] (R=H, 2 a ; Me, 2 b ; Ph, 2 c ). All W-oxo-alkyne complexes ( 2 a , b , c ) were found to be capable of alkyne release upon light irradiation to afford five-coordinate [WO(S-Phoz)2] ( 3 ). The photoinduced release of the alkyne ligand was studied in detail by in situ 1H NMR measurements, which revealed correlation of the photodissociation rate constant ( 2 b>2 a>2 c ) with the elongation of the alkyne C≡C bond in the molecular structures. Oxidation of [WO(S-Phoz)2] ( 3 ) with pyridine-N-oxide yielded [WO2(S-Phoz)2] ( 4 ), which shows highly fluxional behavior in solution. Variable-temperature 1H NMR spectroscopy revealed three isomeric forms with respect to the ligand arrangement versus each other. Furthermore, compound 4 rearranges to tetranuclear oxo compound [W4O4(μ-O)6(S-Phoz)4] ( 5 ) and dinuclear [{WO(μ-O)(S-Phoz)}2] ( 6 ) over time. The latter two were identified by single-crystal X-ray diffraction analyses. 相似文献
83.
One of the challenges of cellular automaton research is finding models with a low complexity and at the same time a rich dynamics. A measure of low complexity is the number of states in the model and the number of transition rules to switch between those states. In this paper, we propose a 2-dimensional 2-state cellular automaton that-though governed by a single simple transition rule-has a sufficiently rich dynamics to be computationally universal. According to the transition rule, a cell’s state is determined by the sum of the states of the cells at orthogonal or diagonal distances one or two from the cell (distance-2 Moore neighbourhood), but not by the previous state of the cell itself. Notwithstanding its simplicity, this model is able to generate a great variety of patterns, including several types of stable configurations, oscillators and patterns that move over cellular space (gliders). We prove the computational universality of the model by constructing a universal set of logic gates (NOT and AND) from these patterns. A key element in this proof is the shifting of phases and positions of signals such that they meet the input requirements of the logic gates. Similarities of the model with classical spin systems are also discussed. 相似文献
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Kendall A. Smith Deanna L. Pickel Kevin Yager Kim Kisslinger Rafael Verduzco 《Journal of polymer science. Part A, Polymer chemistry》2014,52(2):154-163
Conjugated block copolymers are potentially useful for organic electronic applications and the study of interfacial charge and energy transfer processes; yet few synthetic methods are available to prepare polymers with well‐defined conjugated blocks. Here, we report the synthesis and thin film morphology of a series of conjugated poly(3‐hexylthiophene)‐block‐poly(9,9‐dioctylfluorene) (P3HT‐b‐PF) and poly(3‐dodecylthiophene)‐block‐poly(9,9‐dioctylfluorene) (P3DDT‐b‐PF) block copolymers prepared by functional external initiators and click chemistry. Functional group control is quantified by proton nuclear magnetic resonance spectroscopy, size‐exclusion chromatography, and matrix‐assisted laser desorption/ionization time‐of‐flight mass spectrometry. The thin film morphology of the resulting all‐conjugated block copolymers is analyzed by a combination of grazing‐incidence X‐ray scattering, atomic force microscopy, and transmission electron microscopy. Crystallization of the P3HT or P3DDT blocks is present in thin films for all materials studied, and P3DDT‐b‐PF films exhibit significant PF/P3DDT co‐crystallization. Processing conditions are found to impact thin film crystallinity and orientation of the π–π stacking direction of polymer crystallites. © 2013 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2014 , 52, 154–163 相似文献
89.
Michael Tüchler Lisa Gärtner Susanne Fischer Prof. A. Daniel Boese Prof. Ferdinand Belaj Prof. Nadia C. Mösch‐Zanetti 《Angewandte Chemie (International ed. in English)》2018,57(23):6906-6909
The terminal zinc hydride complex [Tntm]ZnH ( 2 ; Tntm=tris(6‐tert‐butyl‐3‐thiopyridazinyl)methanide) is an efficient hydrosilylation catalyst of CO2 at room temperature without the need of Lewis acidic additives. The inherent electrophilicity of the system leads to selective formation of the monosilylated product (MeO)3SiO2CH (at room temperature with a TOF of 22.2 h?1 and at 45 °C with a TOF of 66.7 h?1). In absence of silanes, the intermediate formate complex [Tntm]Zn(O2CH) ( 3 ) is quantitatively formed within 5 min. All complexes were fully characterized by 1H and 13C NMR spectroscopy and single‐crystal X‐ray diffraction analyses. Density functional theory (DFT) calculations reveal a high positive charge on zinc and the increased preference of the ligand to adopt a κ3‐coordination mode. 相似文献
90.
Kornauth Wilh Bersch A. Philips Christ. Kob und Co. Donner Louise H. Weller C. Schweitzer Ch. L. Penny Ed. van Melckebeke H. J. Wheeler B. Hartwell Knorr W. Büttner Barthé W. Jerwitz C. F. Parker Gust Christ Ferdinand Kryz J. Katz H. Göckel R. Jabota J. J. L. von Rijn F. Baum Joseph Nerking A. E. Taylor J. Gadamer C. Th. L. Hagemann und C. A. Neufeld 《Fresenius' Journal of Analytical Chemistry》1902,41(11):686-695
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