全文获取类型
收费全文 | 713篇 |
免费 | 23篇 |
国内免费 | 2篇 |
专业分类
化学 | 523篇 |
晶体学 | 9篇 |
力学 | 12篇 |
数学 | 86篇 |
物理学 | 108篇 |
出版年
2023年 | 9篇 |
2022年 | 5篇 |
2021年 | 18篇 |
2020年 | 13篇 |
2019年 | 9篇 |
2018年 | 6篇 |
2017年 | 3篇 |
2016年 | 19篇 |
2015年 | 16篇 |
2014年 | 19篇 |
2013年 | 38篇 |
2012年 | 55篇 |
2011年 | 61篇 |
2010年 | 20篇 |
2009年 | 33篇 |
2008年 | 56篇 |
2007年 | 42篇 |
2006年 | 46篇 |
2005年 | 26篇 |
2004年 | 28篇 |
2003年 | 16篇 |
2002年 | 27篇 |
2001年 | 21篇 |
2000年 | 15篇 |
1999年 | 10篇 |
1998年 | 6篇 |
1997年 | 11篇 |
1996年 | 10篇 |
1995年 | 4篇 |
1994年 | 8篇 |
1993年 | 7篇 |
1992年 | 10篇 |
1991年 | 6篇 |
1990年 | 3篇 |
1989年 | 8篇 |
1988年 | 3篇 |
1985年 | 11篇 |
1984年 | 5篇 |
1983年 | 5篇 |
1982年 | 5篇 |
1981年 | 2篇 |
1980年 | 4篇 |
1979年 | 1篇 |
1978年 | 3篇 |
1977年 | 3篇 |
1976年 | 1篇 |
1975年 | 2篇 |
1973年 | 5篇 |
1971年 | 3篇 |
1967年 | 1篇 |
排序方式: 共有738条查询结果,搜索用时 359 毫秒
721.
Atomic hydrogen has received recent attention because of its potential role in energy devices, silicon devices, artificial photosynthesis, hydrogen storage, and so forth. Here, we propose a highly efficient route for producing atomic hydrogen using semi-clathrate hydrates. Two major hydrogen radical sources, derived from guest/host materials, are closely examined. 相似文献
722.
Jin Ah Seo Jong Kwan Koh Ki Bong Lee Sang Wook Kang Jong Hak Kim 《Journal of Solid State Electrochemistry》2012,16(2):513-520
Poly(oxyethylene methacrylate)–poly(4-vinyl pyridine) (POEM–P4VP) comb-like copolymers with 3:7, 5:5, and 6:4 wt ratio were
synthesized via atom transfer radical polymerization and confirmed by 1H-NMR and FT-IR spectroscopy. The copolymers were quaternized with 1-iodopropane to convert the pyridine groups into pyridinium
ions, i.e., POEM–qP4VP. Transmission electron microscopy showed that strongly segregated microphase separation in POEM–P4VP
was less prominent upon quaternization due to interactions between the ether oxygens of POEM and the quaternized pyridine
groups of qP4VP, as confirmed by FT-IR spectroscopy. The energy conversion efficiencies of dye-sensitized solar cells (DSSCs)
with quaternized polymer electrolytes were always greater than those with pristine electrolytes due to greater ionic conductivity
and concentrations of free iodide ions. The maximum energy conversion efficiency of a DSSC employing POEM–qP4VP electrolyte
reached 3.0% at 100 mW/cm2 when a 6:4 wt.% of POEM–qP4VP was used. 相似文献
723.
Yoo IY Ryu DW Yoon JH Sohn AR Lim KS Cho BK Koh EK Hong CS 《Dalton transactions (Cambridge, England : 2003)》2012,41(6):1776-1785
Five Fe(III)Mn(III) bimetallic compounds [Fe(iqc)(CN)(3)][Mn(5-Xsalen)]·pMeOH·qMeCN·rH(2)O [Hiqc = N-(quinolin-8-yl)isoquinoline-1-carboxamide; salen = N,N'-ethylenebis(salicylideneiminato) dianion; X = H(2), F(3, 3a), Cl(4), Br(5)] were prepared by assembling a newly designed mer-Fe tricyanide (Ph(4)P)[Fe(iqc)(CN)(3)]·0.5H(2)O (1) and the respective Mn Schiff bases Mn(5-Xsalen)(+). Compounds 2-4 show linear chain structures in which trans-positioned cyanides of the Fe precursor bridge neighbouring Mn atoms, while 5 is a zigzag chain coordination polymer where two cyanide groups of the precursor in the cis mode act as bridges. The structural change from linear to zigzag may arise from the size effect of the halogens. The reversible structural transformation occurs between 3 and 3a upon the solvation-desolvation protocol and the corresponding magnetic behaviours are affected. Furthermore, in 4 and 5, the helical chains are established through hydrogen bonding of solvent molecules. From a magnetostructural point of view, within the linear chain system, the ferromagnetic coupling in 2, contrary to antiferromagnetic interactions in 3-4, is associated with the large torsion angle of C(eq)-Fe-Mn-N(O)(eq) (eq = equatorial) as well as almost the linear Mn-N≡C angle. 相似文献
724.
β-Sheet forming self assembling cyclic peptides offer a versatile scaffold for the construction and control of hydrogen-bonded nanotube assemblies. These structures have major advantages over other nanoscale tubular structures, including sub-nanometer control over the internal diameter, and the ability to control internal and external chemical functionality. This Tutorial Review presents an overview of nanotubes derived from this class of cyclic peptides. The design rationale for functional nanotubes based on cyclic peptide ring size and chemical functionality is discussed. Additionally, we highlight the recent expansion of the nanotube toolbox through conjugation of (macro)molecules to the cyclic peptides. These provide additional functionality and control nanotube dimensions that could potentially prove beneficial in future applications. 相似文献
725.
B Koh G Kim HK Yoon JB Park R Kopelman W Cheng 《Langmuir : the ACS journal of surfaces and colloids》2012,28(32):11676-11686
DNA short oligo, surfactant, peptides, and polymer-assisted dispersion of single-walled carbon nanotube (SWCNTs) in aqueous solution have been intensively studied. It has been suggested that van der Waals interaction, π-π stacking, and hydrophobic interaction are major factors that account for the SWCNTs dispersion. Fluorophore and dye molecules such as Rhodamine B and fluorescein have both hydrophilic and hydrophobic moieties. These molecules also contain π-conjugated systems that can potentially interact with SWCNTs to induce its dispersion. Through a systematic study, here we show that SWCNTs can be dispersed in aqueous solution in the presence of various fluorophore or dye molecules. However, the ability of a fluorophore or dye molecule to disperse SWCNTs is not correlated with the stability of the fluorophore/dye-SWCNT complex, suggesting that the on-rate of fluorophore/dye binding to SWCNTs may dominate the efficiency of this process. We also examined the uptake of fluorophore molecules by mammalian cells when these molecules formed complexes with SWCNTs. The results can have potential applications in the delivery of poor cell-penetrating fluorophore molecules. 相似文献
726.
Neutral superexcited states in molecular oxygen converging to the O(2)(+) c (4)Σ(u)(-) ion state are excited and probed with femtosecond time-resolved photoelectron spectroscopy to investigate predissociation and autoionization relaxation channels as the superexcited states decay. The c (4)Σ(u)(-) 4sσ(g) v=0, c (4)Σ(u)(-) 4sσ(g) v=1, and c (4)Σ(u)(-) 3dσ(g) v=1 superexcited states are prepared with pulsed high-harmonic radiation centered at 23.10 eV. A time-delayed 805 nm laser pulse is used to probe the excited molecular states and neutral atomic fragments by ionization; the ejected photoelectrons from these states are spectrally resolved with a velocity map imaging spectrometer. Three excited neutral O* atom products are identified in the photoelectron spectrum as 4d(1)?(3)D(J)°, 4p(1) (5)P(J)° and 3d(1) (3)D(J)° fragments. Additionally, several features in the photoelectron spectrum are assigned to photoionization of the transiently populated superexcited states. Using principles of the ion core dissociation model, the atomic fragments measured are correlated with the molecular superexcited states from which they originate. The 4d(1) (3)D(J)° fragment is observed to be formed on a timescale of 65 ± 5 fs and is likely a photoproduct of the 4sσ(g) v = 1 state. The 4p(1) (5)P(J)° fragment is formed on a timescale of 427 ± 75 fs and correlated with the neutral predissociation of the 4sσ(g) v = 0 state. The timescales represent the sum of predissociation and autoionization decay rates for the respective superexcited state. The production of the 3d(1) (3)D(J)° fragment is not unambiguously resolved in time due to an overlapping decay of a v = 1 superexcited state photoelectron signal. The observed 65 fs timescale is in good agreement with previous experiments and theory on the predissociation lifetimes of the v = 1 ion state, suggesting that predissociation may dominate the decay dynamics from the v = 1 superexcited states. An unidentified molecular state is inferred by the detection of a long-lived depletion signal (reduction in autoionization) associated with the B (2)Σ(g)(-) ion state that persists up to time delays of 105 ps. 相似文献
727.
Won Jun Choi Yun Jung Ko Girish Chandra Hyuk Woo Lee Hea Ok Kim Hyo Jung Koh Hyung Ryong Moon Young Hoon Jung Lak Shin Jeong 《Tetrahedron》2012,68(4):1253-1261
Conformationally restricted 2′-C-azido-, hydroxy- and fluoromethyl-carbanucleosides 4b–f were efficiently synthesized via the stereoselective conversion of ketone 7 to epoxide 14, followed by the stereoselective opening of the epoxide with nucleophiles (OAc, N3, and F), while the corresponding 2′-C-methyl-carbanucleoside 4a was synthesized via the stereoselective Grignard reaction of ketone 7 with methylmagnesium iodide as a key step. All the final nucleosides 4a–f were assayed for anti-HCV activity, but showed neither significant anti-HCV activity nor cytotoxicity in a cell-based replicon assay. 相似文献
728.
Jeremy Chapman M. Burak Erdo?an Derrick Hart Alex Iosevich Doowon Koh 《Mathematische Zeitschrift》2012,271(1-2):63-93
An analog of the Falconer distance problem in vector spaces over finite fields asks for the threshold α?>?0 such that ${|\Delta(E)| \gtrsim q}$ whenever ${|E| \gtrsim q^{\alpha}}$ , where ${E \subset {\mathbb {F}}_q^d}$ , the d-dimensional vector space over a finite field with q elements (not necessarily prime). Here ${\Delta(E)=\{{(x_1-y_1)}^2+\dots+{(x_d-y_d)}^2: x,y \in E\}}$ . Iosevich and Rudnev (Trans Am Math Soc 359(12):6127–6142, 2007) established the threshold ${\frac{d+1}{2}}$ , and in Hart et?al. (Trans Am Math Soc 363:3255–3275, 2011) proved that this exponent is sharp in odd dimensions. In two dimensions we improve the exponent to ${\tfrac{4}{3}}$ , consistent with the corresponding exponent in Euclidean space obtained by Wolff (Int Math Res Not 10:547–567, 1999). The pinned distance set ${\Delta_y(E)=\{{(x_1-y_1)}^2+\dots+{(x_d-y_d)}^2: x\in E\}}$ for a pin ${y\in E}$ has been studied in the Euclidean setting. Peres and Schlag (Duke Math J 102:193–251, 2000) showed that if the Hausdorff dimension of a set E is greater than ${\tfrac{d+1}{2}}$ , then the Lebesgue measure of Δ y (E) is positive for almost every pin y. In this paper, we obtain the analogous result in the finite field setting. In addition, the same result is shown to be true for the pinned dot product set ${\Pi_y(E)=\{x\cdot y: x\in E\}}$ . Under the additional assumption that the set E has Cartesian product structure we improve the pinned threshold for both distances and dot products to ${\frac{d^2}{2d-1}}$ . The pinned dot product result for Cartesian products implies the following sum-product result. Let ${A\subset \mathbb F_q}$ and ${z\in \mathbb F^*_q}$ . If ${|A|\geq q^{\frac{d}{2d-1}}}$ then there exists a subset ${E'\subset A\times \dots \times A=A^{d-1}}$ with ${|E'|\gtrsim |A|^{d-1}}$ such that for any ${(a_1,\dots, a_{d-1}) \in E'}$ , $$ |a_1A+a_2A+\dots +a_{d-1}A+zA| > \frac{q}{2}$$ where ${a_j A=\{a_ja:a \in A\},j=1,\dots,d-1}$ . A generalization of the Falconer distance problem is to determine the minimal α?>?0 such that E contains a congruent copy of a positive proportion of k-simplices whenever ${|E| \gtrsim q^{\alpha}}$ . Here the authors improve on known results (for k?>?3) using Fourier analytic methods, showing that α may be taken to be ${\frac{d+k}{2}}$ . 相似文献
729.
A high-performance liquid chromatography-diode array detection (HPLC-DAD) method and a liquid chromatography-electrospray ionization tandem mass spectrometry (LC-ESI-MS/MS) method were developed to screen for the presence of synthetic phosphodiesterase-5 (PDE-5) inhibitors and their analogues, namely sildenafil, vardenafil, tadalafil, homosildenafil, acetildenafil and hydroxyhomosildenafil. The methods were applied to pre-market samples submitted to the Health Sciences Authority of Singapore (HSA) for testing. One sample was in the form of capsules while six other samples were pre-mixed bulk powder samples for dietary supplements to be repackaged or formulated into the final dosage forms (usually capsules). Identification of PDE-5 inhibitors and their analogues was achieved by comparing individual peak retention times, UV spectra and mass spectra with those of reference standards. The seven samples were found to contain at least one of the following compounds: sildenafil, vardenafil, hydroxyhomosildenafil, homosildenafil and acetildenafil. The five compounds were simultaneously determined by LC-ESI-MS/MS in multiple reactions monitoring (MRM) scan mode. The method has been validated for accuracy, precision, linearity and sensitivity. 相似文献
730.
Sukanta Kamila Benjamin Koh Omair Khan Hongming Zhang Edward R. Biehl 《Journal of heterocyclic chemistry》2006,43(6):1641-1646