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981.
982.
983.
Guo YN Xu GF Wernsdorfer W Ungur L Guo Y Tang J Zhang HJ Chibotaru LF Powell AK 《Journal of the American Chemical Society》2011,133(31):11948-11951
The high axiality and Ising exchange interaction efficiently suppress quantum tunneling of magnetization of an asymmetric dinuclear Dy(III) complex, as revealed by combined experimental and theoretical investigations. Two distinct regimes of blockage of magnetization, one originating from the blockage at individual Dy sites and the other due to the exchange interaction between the sites, are separated for the first time. The latter contribution is found to be crucial, allowing an increase of the relaxation time by 3 orders of magnitude. 相似文献
984.
Thielemann DT Klinger M Wolf TJ Lan Y Wernsdorfer W Busse M Roesky PW Unterreiner AN Powell AK Junk PC Deacon GB 《Inorganic chemistry》2011,50(23):11990-12000
Two types of structurally related one-dimensional coordination polymers were prepared by reacting lanthanide trichloride hydrates [LnCl(3)·(H(2)O)(m)] with dibenzoylmethane (Ph(2)acacH) and a base. Using cesium carbonate (Cs(2)CO(3)) and praseodymium, neodymium, samarium, or dysprosium salts yielded [Cs{Ln(Ph(2)acac)(4)}](n) (Ln = Pr (1), Nd (2), Sm (3), Dy (4)) in considerable yields. Reaction of potassium tert-butoxide (KOtBu) and the neodymium salt [NdCl(3)·(H(2)O)(6)] with Ph(2)acacH resulted in [K{Nd(Ph(2)acac)(4)}](n) (5). All polymers exhibit a heterobimetallic backbone composed of alternating lanthanide and alkali metal atoms which are bridged by the Ph(2)acac ligands in a linear fashion. ESI-MS investigations on DMF solutions of 1-5 revealed a dissociation of all the five compounds upon dissolution, irrespective of the individual lanthanide and alkali metal present. Temporal profiles of changes in optical density were acquired performing pump/probe experiments with DMF solutions of 1-5 via femtosecond laser spectroscopy, highlighting a lanthanide-specific relaxation dynamic. The corresponding relaxation times ranging from seven picoseconds to a few hundred picoseconds are strongly dependent on the central lanthanide atom, indicating an intramolecular energy transfer from ligands to lanthanides. This interpretation also demands efficient intersystem crossing within one to two picoseconds from the S(1) to T(1) level of the ligands. Magnetic studies show that [Cs{Dy(Ph(2)acac)(4)}](n) (4) has slow relaxation of the magnetization arising from the single Dy(3+) ions and can be described as a single-ion single molecule magnet (SMM). Below 0.5 K, hysteresis loops of the magnetization are observed, which show weak single chain magnet (SCM) behavior. 相似文献
985.
D.B. Haidvogel H. Arango W.P. Budgell B.D. Cornuelle E. Curchitser E. Di Lorenzo K. Fennel W.R. Geyer A.J. Hermann L. Lanerolle J. Levin J.C. McWilliams A.J. Miller A.M. Moore T.M. Powell A.F. Shchepetkin C.R. Sherwood R.P. Signell J.C. Warner J. Wilkin 《Journal of computational physics》2008,227(7):3595-3624
Systematic improvements in algorithmic design of regional ocean circulation models have led to significant enhancement in simulation ability across a wide range of space/time scales and marine system types. As an example, we briefly review the Regional Ocean Modeling System, a member of a general class of three-dimensional, free-surface, terrain-following numerical models. Noteworthy characteristics of the ROMS computational kernel include: consistent temporal averaging of the barotropic mode to guarantee both exact conservation and constancy preservation properties for tracers; redefined barotropic pressure-gradient terms to account for local variations in the density field; vertical interpolation performed using conservative parabolic splines; and higher-order, quasi-monotone advection algorithms. Examples of quantitative skill assessment are shown for a tidally driven estuary, an ice-covered high-latitude sea, a wind- and buoyancy-forced continental shelf, and a mid-latitude ocean basin. The combination of moderate-order spatial approximations, enhanced conservation properties, and quasi-monotone advection produces both more robust and accurate, and less diffusive, solutions than those produced in earlier terrain-following ocean models. Together with advanced methods of data assimilation and novel observing system technologies, these capabilities constitute the necessary ingredients for multi-purpose regional ocean prediction systems. 相似文献
986.
Anthony V. Powell Rachel J.E. Lees Ann M. Chippindale 《Journal of Physics and Chemistry of Solids》2008,69(4):1000-1006
The chromium(II) antimony(III) sulphide, [Cr((NH2CH2CH2)3N)]Sb4S7, was synthesised under solvothermal conditions from the reaction of Sb2S3, Cr and S dissolved in tris(2-aminoethyl)amine (tren) at 438 K. The products were characterised by single-crystal X-ray diffraction, elemental analysis, SQUID magnetometry and diffuse reflectance spectroscopy. The compound crystallises in the monoclinic space group P21/n with a=7.9756(7), b=10.5191(9), c=25.880(2) Å and β=90.864(5)°. Alternating SbS33− trigonal pyramids and Sb3S63− semi-cubes generate Sb4S72− chains which are directly bonded to Cr(tren)2+ pendant units. The effective magnetic moment of 4.94(6)μB shows a negligible orbital contribution, in agreement with expectations for Cr(II):d4 in a 5A ground state. The measured band gap of 2.14(3) eV is consistent with a correlation between optical band gap and framework density that is established from analysis of a wide range of antimony sulphides. 相似文献
987.
Athar SB Patel R Yelton J Rubin P Eisenstein BI Karliner I Mehrabyan S Lowrey N Selen M White EJ Wiss J Mitchell RE Shepherd MR Besson D Pedlar TK Cronin-Hennessy D Gao KY Hietala J Kubota Y Klein T Lang BW Poling R Scott AW Zweber P Dobbs S Metreveli Z Seth KK Tomaradze A Libby J Powell A Wilkinson G Ecklund KM Love W Savinov V Lopez A Mendez H Ramirez J Ge JY Miller DH Shipsey IP Xin B Adams GS Anderson M Cummings JP Danko I Hu D Moziak B Napolitano J He Q Insler J Muramatsu H Park CS 《Physical review letters》2008,100(18):181802
Using e+e--->Ds*-Ds+ data collected near the peak Ds production energy, Ecm=4170 MeV, with the CLEO-c detector, we present the first observation of the decay Ds+-->pn. We measure a branching fraction B(Ds+-->pn)=(1.30+/-0.36(-0.16)+0.12)x10(-3). This is the first observation of a charmed meson decaying into a baryon-antibaryon final state. 相似文献
988.
Dobbs S Metreveli Z Seth KK Tomaradze A Libby J Powell A Wilkinson G Ecklund KM Love W Savinov V Lopez A Mendez H Ramirez J Ge JY Miller DH Shipsey IP Xin B Adams GS Anderson M Cummings JP Danko I Hu D Moziak B Napolitano J He Q Insler J Muramatsu H Park CS Thorndike EH Yang F Artuso M Blusk S Khalil S Li J Mountain R Nisar S Randrianarivony K Sultana N Skwarnicki T Stone S Wang JC Zhang LM Bonvicini G Cinabro D Dubrovin M Lincoln A Naik P Rademacker J Asner DM Edwards KW Reed J Briere RA 《Physical review letters》2008,101(18):182003
A precision measurement of the mass of the h_{c}(1P1) state of charmonium has been made using a sample of 24.5x10;{6} psi(2S) events produced in e;{+}e;{-} annihilation at the Cornell Electron Storage Ring (CESR). The reaction used was psi(2S)-->pi;{0}h_{c}, pi;{0}-->gammagamma, h_{c}-->gammaeta_{c}, and the reaction products were detected in the CLEO-c detector. Data have been analyzed both for the inclusive reaction and for the exclusive reactions in which eta_{c} decays are reconstructed in 15 hadronic decay channels. Consistent results are obtained in the two analyses. The averaged results of the present measurements are M(h_{c})=3525.28+/-0.19(stat.)+/-0.12(syst.) MeV, and B(psi(2S)-->pi;{0}h_{c})xB(h_{c}-->gammaeta_{c})=(4.19+/-0.32+/-0.45)x10;{-4}. Using the ;{3}P_{J} centroid mass, DeltaM_{hf}(1P) identical withM(chi_{cJ})-M(h_{c})=+0.02+/-0.19+/-0.13 MeV. 相似文献
989.
990.
John L. Shibley Robert West Douglas R. Powell Claire A. Tessier 《Heteroatom Chemistry》1994,5(3):205-214
The addition of n equiv of MesNHLi (n = 1, 2, 3, 4) and m equiv of 12-crown-4 (m = 0.1, 1, 2, 3, 4) to (RsiCl2)2 (R = Mesityl; t-Butyl) in THF at −78°C resulted in higher yields and improved selectivities of cyclodisilazanes and azadisilacyclopropanes. The reaction of 2 equiv of MesNDLi with (MesSiCl2)2 ( I ) yielded cis-2-chloro-1,2,3,4-tetramestylcyclodisilazane ( 2a ) with 95% Si H deuteration. 2a was quantitatively chlorinated with retention of stereochemistry by N-chlorosuccinimide to give the cis dichlorocyclodisilazane ( 3 ). Variable-temperature 1H NMR studies from −70°C to 25°C in d8-THF were performed on 1 , 2a , 2b , and 3 . 1 exhibited little variation throughout the temperature range, whereas 2a , 2b , and 3 showed several rotational isomers. trans-2,3-Bis(mesitylamino)-1,2,3-trimesitylazadisilacyclopropane was shown to isomerize to the cis isomer in the presence of n-BuLi or MesNHLi. The molecular structures of 1 and 3 were determined by X-ray crystallography. Compound 1 crystallized in the monoclinic space group P21/c, with cell parameters a = 16.599(2) Å b = 14.633(2) Å, c = 16.945(2) Å, β = 92.044(13)°, V = 4113.1(8) Å3, Z = 8, d (calcd) = 1.409 g/cm3, and R = 6.88%. Compound 3 ° C6H6 crystallized in the orthorhombic space group Pbca, with cell parameters a = 17.906(4) Å, b = 13.918(3) Å, c = 31.700(6) Å, V = 7900(3) Å3, Z = 8, d (calcd) = 1.194 g/cm3, and R = 7.52%. 相似文献