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941.
Wang Z Hagerstrom A Anderson JQ Tong W Wu M Carr LD Eykholt R Kalinikos BA 《Physical review letters》2011,107(11):114102
Chaotic spin-wave solitons in magnetic film active feedback rings were observed for the first time. At some ring gain level, one observes the self-generation of a single spin-wave soliton pulse in the ring. When the pulse circulates in the ring, its amplitude varies chaotically with time. Numerical simulations based on a gain-loss nonlinear Schr?dinger equation reproduce the observed responses. 相似文献
942.
Luo Y de Leon E Castro J Lee J Barton JK Kostuk RK Barbastathis G 《Optics letters》2011,36(7):1290-1292
A phase-contrast volume holographic imaging system for three-dimensional contrast enhancement is presented. The system utilizes a spatial filter placed on a conjugate plane to the volume holographic pupil to simultaneously enhance weak phase information at different depths within an object. The proposed system was validated with experimental image data obtained in mouse colon samples and quantitative measurements of modulation transfer function as well. 相似文献
943.
Fortier S Walensky JR Wu G Hayton TW 《Journal of the American Chemical Society》2011,133(18):6894-6897
Addition of the Wittig reagent Ph(3)P═CH(2) to the U(III) tris(amide) U(NR(2))(3) (R = SiMe(3)) generates a mixture of products from which the U(IV) complex U═CHPPh(3)(NR(2))(3) (2) can be obtained. Complex 2 features a short U═C bond and represents a rare example of a uranium carbene. In solution, 2 exists in equilibrium with the U(IV) metallacycle U(CH(2)SiMe(2)NR)(NR(2))(2) and free Ph(3)P═CH(2). Measurement of this equilibrium as a function of temperature provides ΔH(rxn) = 11 kcal/mol and ΔS(rxn) = 31 eu. Additionally, the electronic structure of the U═C bond was investigated using DFT analysis. 相似文献
944.
Toader M Knupfer M Zahn DR Hietschold M 《Journal of the American Chemical Society》2011,133(14):5538-5544
The adsorption of lutetium(III) bis-phthalocyanine (LuPc(2)) on Ag(111) was investigated using scanning tunneling microscopy and spectroscopy (STM/STS). A comprehensive study was carried out toward understanding the driving mechanism responsible for the formation of the first and second monolayers (MLs). In both MLs, the adsorbed molecules are found to exhibit different in-plane orientations arranged according to a "chess-board" like pattern. Highly resolved STM images allowed an exact determination of the corresponding angle mismatch, which differs for the first and second MLs. The tunneling transport through individual molecules reveals a negative differential resistance (NDR) effect detectable within the current-voltage curves. The corresponding density of states (DOS) representation is consistent with a resonant tunneling mechanism sustained by the valence band (VB) states close to the Fermi energy (E(F)) recorded via highly resolved ultraviolet photoemission spectroscopy (UPS). 相似文献
945.
Kiesewetter MK Edward JA Kim H Waymouth RM 《Journal of the American Chemical Society》2011,133(41):16390-16393
The catalytic condensation of cis-2-butene-1,4-diol with CpRu(MQA)(C(3)H(5)) (Cp = cyclopentadienyl, MQA = 4-methoxyquinoline-2-carboxylate) generates poly(2-butenediol), an unsaturated telechelic polyether diol with molecular weights between 400 and 4600 g/mol. This Ru(IV) allyl catalyst enchains 2-butene-1,4-diol primarily as the linear trans-2-butenyl ether (92%) along with vinyl branches (8%). These telechelic oligomers are useful chain extenders and macromonomers, as demonstrated by their use in the synthesis of poly(lactide)-b-poly(butenediol)-b-poly(lactide) triblock copolymers. Model studies support a proposed mechanism involving the formation of Ru(IV) allyl intermediates from allylic alcohols and chain growth by selective nucleophilic displacement at the terminus of the Ru(IV) allyl to generate trans-2-butenyl ether linkages. 相似文献
946.
The fusion domain of the influenza coat protein hemagglutinin HA2, bound to dodecyl phosphocholine micelles, was recently shown to adopt a structure consisting of two antiparallel α-helices, packed in an exceptionally tight hairpin configuration. Four interhelical H(α) to C═O aliphatic H-bonds were identified as factors stabilizing this fold. Here, we report evidence for an additional stabilizing force: a strong charge-dipole interaction between the N-terminal Gly(1) amino group and the dipole moment of helix 2. pH titration of the amino-terminal (15)N resonance, using a methylene-TROSY-based 3D NMR experiment, and observation of Gly(1 13)C' show a strongly elevated pK = 8.8, considerably higher than expected for an N-terminal amino group in a lipophilic environment. Chemical shifts of three C-terminal carbonyl carbons of helix 2 titrate with the protonation state of Gly(1)-N, indicative of a close proximity between the N-terminal amino group and the axis of helix 2, providing an optimal charge-dipole stabilization of the antiparallel hairpin fold. pK values of the side-chain carboxylate groups of Glu(11) and Asp(19) are higher by about 1 and 0.5 unit, respectively, than commonly seen for solvent-exposed side chains in water-soluble proteins, indicative of dielectric constants of ε = ~30 (Glu(11)) and ~60 (Asp(19)), placing these groups in the headgroup region of the phospholipid micelle. 相似文献
947.
Ahmad Kiani Karanji Maryssa Beasley Daud Sharif Ali Ranjbaran Justin Legleiter Stephen J. Valentine 《Journal of mass spectrometry : JMS》2020,55(1)
The first 17 amino acid residues of Huntingtin protein (Nt17 of htt) are thought to play an important role in the protein's function; Nt17 is one of two membrane binding domains in htt. In this study the binding ability of Nt17 peptide with vesicles comprised of two subclasses of phospholipids is studied using electrospray ionization ‐ mass spectrometry (ESI‐MS) and molecular dynamics (MD) simulations. Overall, the peptide is shown to have a greater propensity to interact with vesicles of phosphatidylcholine (PC) rather than phosphatidylethanolamine (PE) lipids. Mass spectra show an increase in lipid‐bound peptide adducts where the ordering of the number of such specie is 1,2‐dioleoyl‐sn‐glycero‐3‐phosphocholine (DOPC) > 1‐palmitoyl‐2‐oleoyl‐glycero‐3‐phosphocholine (POPC) > 1‐palmitoyl‐2‐oleoyl‐sn‐glycero‐3 phosphoethanolamine (POPE). MD simulations suggest that the compactness of the bilayer plays a role in governing peptide interactions. The peptide shows greater disruption of the DOPC bilayer order at the surface and interacts with the hydrophobic tails of lipid molecules via hydrophobic residues. Conversely, the POPE vesicle remains ordered and lipids display transient interactions with the peptide through the formation of hydrogen bonds with hydrophilic residues. The POPC system displays intermediate behavior with regard to the degree of peptide‐membrane interaction. Finally, the simulations suggest a helix stabilizing effect resulting from the interactions between hydrophobic residues and the lipid tails of the DOPC bilayer. 相似文献
948.
Daniel W. Armstrong Mohsen Talebi Nimisha Thakur M. Farooq Wahab Alexander V. Mikhonin Matt T. Muckle Justin L. Neill 《Angewandte Chemie (International ed. in English)》2020,59(1):192-196
We designed and demonstrated the unique abilities of the first gas chromatography–molecular rotational resonance spectrometer (GC‐MRR). While broadly and routinely applicable, its capabilities can exceed those of high‐resolution MS and NMR spectroscopy in terms of selectivity, resolution, and compound identification. A series of 24 isotopologues and isotopomers of five organic compounds are separated, identified, and quantified in a single run. Natural isotopic abundances of mixtures of compounds containing chlorine, bromine, and sulfur heteroatoms are easily determined. MRR detection provides the added high specificity for these selective gas‐phase separations. GC‐MRR is shown to be ideal for compound‐specific isotope analysis (CSIA). Different bacterial cultures and groundwater were shown to have contrasting isotopic selectivities for common organic compounds. The ease of such GC‐MRR measurements may initiate a new era in biosynthetic/degradation and geochemical isotopic compound studies. 相似文献
949.
Joseph V. Handy Yuting Luo Justin L. Andrews Nattamai Bhuvanesh Sarbajit Banerjee 《Angewandte Chemie (International ed. in English)》2020,59(38):16385-16392
The diffusion pathways of Li‐ions as they traverse cathode structures in the course of insertion reactions underpin many questions fundamental to the functionality of Li‐ion batteries. Much current knowledge derives from computational models or the imaging of lithiation behavior at larger length scales; however, it remains difficult to experimentally image Li‐ion diffusion at the atomistic level. Here, by using topochemical Li‐ion insertion and extraction to induce single‐crystal‐to‐single‐crystal transformations in a tunnel‐structured V2O5 polymorph, coupled with operando powder X‐ray diffraction, we leverage single‐crystal X‐ray diffraction to identify the sequence of lattice interstitial sites preferred by Li‐ions to high depths of discharge, and use electron density maps to create a snapshot of ion diffusion in a metastable phase. Our methods enable the atomistic imaging of Li‐ions in this cathode material in kinetic states and provide an experimentally validated angstrom‐level 3D picture of atomic pathways thus far only conjectured through DFT calculations. 相似文献
950.
Zijie Luo Taoyuze Lv Kangning Zhu Yi Li Lei Wang J. Justin Gooding Guozhen Liu Bin Liu 《Angewandte Chemie (International ed. in English)》2020,59(8):3131-3136
Monitoring of human serum albumin (HSA) in a point‐of‐care fashion is urgently needed in particular for elderly or chronically ill patients. Herein, a dual‐state emissive chalcone probe having the feature of aggregation‐induced emission was designed and synthesized. The concentration of HSA can be evaluated by the ratios of emission from probes in aggregated and monomeric state, which gives a visually discernible red‐to‐green color change. A simple, portable paper‐based analytical device have been fabricated by integration of the recognition probe in the detection pad and employed for HSA test using the whole blood samples. This paper‐based assay shows the analytical capability comparable to the standard testing methods but is in a point‐of‐care fashion, providing a promising tool for at‐home HSA detection and HSA‐related disease diagnosis. 相似文献