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Amit Mondal Biswajit Bhattacharya Susobhan Das Surojit Bhunia Rituparno Chowdhury Somnath Dey C. Malla Reddy 《Angewandte Chemie (International ed. in English)》2020,59(27):10971-10980
Ductility is a common phenomenon in many metals but is difficult to achieve in molecular crystals. Organic crystals bend plastically on one or two face‐specific directions but fracture when stressed in any other arbitrary directions. An exceptional metal‐like ductility and malleability in the isomorphous crystals of two globular molecules, BH3NMe3 and BF3NMe3, is reported, with characteristic tensile stretching, compression, twisting, and thinning. The mechanically deformed samples, which transition to lower symmetry phases, retain good long‐range order amenable to structure determination by single‐crystal X‐ray diffraction. Molecules in these high‐symmetry crystals interact through electrostatic forces (B??N+) to form columnar structures with multiple slip planes and weak dispersive forces between columns. On the other hand, the limited number of facile slip planes and strong dihydrogen bonding in BH3NHMe2 negates ductility. Our study has implications for the design of soft ferroelectrics, solid electrolytes, barocalorics, and soft robotics. 相似文献
123.
Takashi Sagawa Saleh Chowdhury Makoto Takafuji Hirotaka Ihara 《Macromolecular Symposia》2006,237(1):28-38
Summary: This article gives a review on self-assembled nanofibrillar aggregates such as helical, twisted ribbon-like and tubular forms, those are produced in aqueous bilayer membrane and organogel systems. Two common features necessary for the chemical structure that yields special morphology are a chiral carbon atom and moieties feasible for intermolecular interactions although there are some exceptions. In aqueous systems, a hydrophobic effect is also an essential driving force for molecular aggregates in aqueous solution systems but almost disappear in organic media. More positive intermolecular interactions play an important role in molecular aggregation in organic media. Hydrogen bonding interaction is especially effective and many organogelators are classified into this category. Some lipophilic peptides have been investigated not only as organogelators but also with respect to their self-assembling behaviors. This latter property gives them distinct advantages compared with conventional gel systems because the gels include highly-ordered structures supramolecular functions like aqueous lipid membranes through molecular orientation. This article also introduces applicability of the organogel system. 相似文献
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Adam Ashcraft Kaixuan Liu Arindam Mukhopadhyay Victor Paulino Chuan Liu Brianna Bernard Dalia Husainy Tina Phan Jean‐Hubert Olivier 《Angewandte Chemie (International ed. in English)》2020,59(19):7487-7493
Locking‐in the conformation of supramolecular assemblies provides a new avenue to regulate the (opto)electronic properties of robust nanoscale objects. In the present contribution, we show that the covalent tethering of a perylene bisimide (PBI)‐derived supramolecular polymer with a molecular locker enables the formation of a locked superstructure equipped with emergent structure–function relationships. Experiments that exploit variable‐temperature ground‐state electronic absorption spectroscopy unambiguously demonstrate that the excitonic coupling between nearest neighboring units in the tethered superstructure is preserved at a temperature (371 K) where the pristine, non‐covalent assembly exists exclusively in a molecularly dissolved state. A close examination of the solid‐state morphologies reveals that the locked superstructure engenders the formation of hierarchical 1D materials which are not achievable by unlocked assemblies. To complement these structural attributes, we further demonstrate that covalently tethering a supramolecular polymer built from PBI subunits enables the emergence of electronic properties not evidenced in non‐covalent assemblies. Using cyclic voltammetry experiments, the elucidation of the potentiometric properties of the locked superstructure reveals a 100‐mV stabilization of the conduction band energy when compared to that recorded for the non‐covalent assembly. 相似文献
127.
Mukherjee S Chowdhury P Bunagan MR Gai F 《The journal of physical chemistry. B》2008,112(30):9146-9150
The folding mechanism and dynamics of a helical protein may strongly depend on how quickly its constituent alpha-helices can fold independently. Thus, our understanding of the protein folding problem may be greatly enhanced by a systematic survey of the folding rates of individual alpha-helical segments derived from their parent proteins. As a first step, we have studied the relaxation kinetics of the central helix (L9:41-74) of the ribosomal protein L9 from the bacterium Bacillus stearothermophilus , in response to a temperature-jump ( T-jump) using infrared spectroscopy. L9:41-74 has been shown to exhibit unusually high helicity in aqueous solution due to a series of side chain-side chain interactions, most of which are electrostatic in nature, while still remaining monomeric over a wide concentration range. Thus, this peptide represents an excellent model system not only for examining how the folding rate of naturally occurring helices differs from that of the widely studied alanine-based peptides, but also for estimating the folding speed limit of (small) helical proteins. Our results show that the T-jump induced relaxation rate of L9:41-74 is significantly slower than that of alanine-based peptides. For example, at 11 degrees C its relaxation time constant is about 2 micros, roughly seven times slower than that of SPE(5), an alanine-rich peptide of similar chain length. In addition, our results show that the folding rate of a truncated version of L9:41-74 is even slower. Taken together, these results suggest that individual alpha-helical segments in proteins may fold on a time scale that is significantly slower than the folding time of alanine-based peptides. Furthermore, we argue that the relaxation rate of L9:41-74 measured between 8 and 45 degrees C provides a realistic estimate of the ultimate folding rate of (small) helical proteins over this temperature range. 相似文献
128.
Efficient sunlight-responsive BiOBr–CoWO4 heterostructured nanocomposite photocatalysts were prepared via a chemical precipitation route at 100°C in 4 hours. The prepared BiOBr–CoWO4 heterostructures were characterized for phase identification, chemical composition, surface morphology, optical properties and surface area using various techniques. The X-ray diffraction pattern of the BiOBr–CoWO4 nanocomposite was composed of diffraction peaks equivalent to both the tetragonal phase of BiOBr and the monoclinic phase of CoWO4 nanoparticles. X-ray photoelectron spectral study of the BiOBr–CoWO4 nanocomposite revealed orbitals of both BiOBr and CoWO4 compounds. Transmission electron microscopy images revealed that spherical particles of CoWO4 (20–25 nm) were dispersed on the surface of BiOBr. UV–visible–near-infrared spectral study of the BiOBr–CoWO4 nanocomposite showed good visible-light absorption. Among the manufactured materials, BiOBr–CoWO4-2 nanocomposite showed better charge carrier separation efficiency, as demonstrated by photoluminescence and time-resolved fluorescence. To study the practical utility of the prepared materials, their photocatalytic capability was examined for the degradation of rhodamine B (RhB) aqueous solution under sunlight irradiation. The photodegradation results showed that BiOBr–CoWO4-2 nanocomposite degraded 98.69% RhB solution and the degradation constant was 0.067 min−1, which was 5.6 and 22.5 times larger than that of pure BiOBr and CoWO4 nanoparticles, respectively, after 60 minutes of sunlight irradiation. The superior photoactivity was facilitated by electron–hole pair separation and transfer driven by the heterostructure interface between BiOBr particles and CoWO4 nanoparticles. The removal of RhB was initiated by photogenerated h+, O2• − and •OH reactive species based on the scavenger effect. 相似文献
129.
Swapan K. Chowdhury Stephen D. Cameron Donald M. Cox Krzysztof Kniaz Robert A. Strongin Maria A. Cichy John E. Fischer Amos B. Smith 《Journal of mass spectrometry : JMS》1993,28(8):860-866
Electron-capture negative ion chemical ionization (EC-NICI) and field desorption (FD) mass spectrometric techniques were utilized to examine polyfluorinated C60. Two different samples from the same preparation, one prior to sublimation and the other sublimed material, were investigated. From the raw non-sublimed product in EC-NCI six series of ions corresponding to different numbers of attached oxygen atoms were obtained, which are represented by the formula [C60F2nOm]?, where n ranged from 0 to 30 and m from 0 to 5. The sublimed material in EC-NICI produced the same six series of ions with up to 48 fluorine atoms attached to C60. The field desorption of the same sample produced similar results, but the signal-to-noise ratios of the spectra were low. Both samples, in the two different techniques examined, yielded C60F60 ions with only an even number of fluorine atoms attached. The present investigation, for the first time, provides direct experimental evidence for the existence of higher fluorinated C60 up to C60F60 and multiple oxides of polyfluoro-C60 with up to five oxygen atoms attached. 相似文献
130.