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31.
Saibal Bera Kaushik Dey Tapan K. Pal Arjun Halder Srinu Tothadi Suvendu Karak Matthew Addicoat Rahul Banerjee 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(13):4287-4291
Porous solids that can be switched between different forms with distinct physical properties are appealing candidates for separation, catalysis, and host–guest chemistry. In this regard, porous organic cages (POCs) are of profound interest because of their solution‐state accessibility. However, the application of POCs is limited by poor chemical stability. Synthesis of an exceptionally stable imine‐linked (4+6) porous organic cage ( TpOMe‐CDA ) is reported using 2,4,6‐trimethoxy‐1,3,5‐triformyl benzene (TpOMe) as a precursor aldehyde. Introduction of the ‐OMe functional group to the aldehyde creates significant steric and hydrophobic characteristics in the environment around the imine bonds that protects the cage molecules from hydrolysis in the presence of acids or bases. The electronic effect of the ‐OMe group also plays an important role in enhancing the stability of the reported POCs. As a consequence, TpOMe‐CDA reveals exceptional chemical stability in neutral, acidic and basic conditions, even in 12 m NaOH. Interestingly, TpOMe‐CDA exists in three different porous and non‐porous polymorphic forms (α, β, and γ) with respect to differences in crystallographic packing and the orientation of the flexible methoxy groups. All of the polymorphs retain their crystallinity even after treatment with acids and bases. All the polymorphs of TpOMe‐CDA differ significantly in their properties as well as morphology and could be reversibly switched in the presence of an external stimulus. 相似文献
32.
Neville SM Leita BA Halder GJ Kepert CJ Moubaraki B Létard JF Murray KS 《Chemistry (Weinheim an der Bergstrasse, Germany)》2008,14(32):10123-10133
Three analogous one dimensional (1D) polymeric iron(II) spin crossover (SCO) materials containing the new ligand 4,6-bis(2',2'-pyridyl)pyrazine (bdpp) have been comprehensively characterised magnetically (thermal and light-induced) and structurally. Within this series are two polymorphs of the formula [Fe(NCS)(2)(bdpp)], 1 and 2 a, which differ magnetically in that phase 1 undergoes a full two-step SCO (T(1/2(1))=135 K and T(1/2(2))=90 K) whereas phase 2 a remains high spin (HS) over all temperatures. The central distinction between these two materials lies in the presence of intermolecular pi-pi interactions generated by the crystal packing in 1, which are absent in 2 a. The isostructural selenocyanate analogue of 2 a, [Fe(NCSe)(2)(bdpp)], 2 b, undergoes a full two-step SCO (T(1/2(1))=200 K and T(1/2(2))=125 K). Structural analyses of 1 and 2 b at a range of temperatures provide deep insight into their two-step SCO nature. Structural analysis of 1 at 25 K (1(LS-LS)), 123 K (1(LS-HS)) and 250 K (1(HS-HS)) reveals two distinct iron(II) centres at each temperature, with ordered, alternating HS and LS (low spin) sites at the intermediate plateau (IP) temperatures. In contrast, structural analysis of 2 b at 90 K (2 b(LS)), 150 K (2 b(LS/HS)) and 250 K (2 b(HS)) reveals one unique iron(II) centre at each temperature with an "averaged" LS/HS character at the IP temperature. Weak planes of diffuse scattering in the single-crystal X-ray diffraction patterns were observed for this phase at 90 and 150 K, indicating that 1D long range ordering of alternating HS/LS iron(II) centres occurs along the 1D coordination chains, but that there is no correlation between chains. The lack of observable diffuse scattering at 250 K suggests that the onset of the 1D structural ordering in the chain direction corresponds to the first step of the SCO and that this structural transition is electronically driven. The photomagnetic properties of both 1 and 2 b have been investigated and show approximately 62 and 53 % photo-excitation of a HS metastable state at low temperatures and T(LIESST) values of 55 and 49 K, respectively. Relaxation studies on the HS fraction in 2 b fitted well to a stretched exponential model with kinetic parameters indicative of weak cooperativity. 相似文献
33.
Podder Soumik Halder Suman Roychowdhury Anirban Das Dipankar Ghosh Chandan Kr. 《Journal of nanoparticle research》2016,18(10):1-13
Journal of Nanoparticle Research - With the widespread use of titanium dioxide (TiO2) human exposure is inevitable, but the exposure data on TiO2 are still limited. This study adopted off-line... 相似文献
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J. Suseendran N. Halder S. Chakrabarti T.D. Mishima C.R. Stanley 《Superlattices and Microstructures》2009
We are reporting the growth of multilayer stacks of quantum dots (10 periods) with a combination capping of In0.21Al0.21Ga0.58As (30 Å) and GaAs (70–180 Å) grown by solid source molecular beam epitaxy (MBE). Reflection high energy electron diffraction (RHEED) has been used for the insitu monitoring of quantum dot (QD) formation in heterostructure samples. The samples were also characterized by other exsitu techniques like cross sectional transmission electron microscopy (XTEM) and photoluminescence measurements (PL). For a heterostructure sample with thin barrier thickness (<100 Å), an XTEM image showed the stacking of QDs only up to the 5th layer and in the upper layers there was hardly any formation of dots. We presume the stoppage of dot formation is due to the uneven surface of the InAlGaAs alloy overgrown on the InAs QDs, as a result of the local compositional deviations of the Group-III atoms. Samples grown with thicker barriers (>100 Å of GaAs) showed good stacking of islands until the tenth layer. The thick GaAs layer overgrown on the InAlGaAs at 590 °C is believed to remove the surface modifications of the quaternary layer thereby creating a smoother surface front for the growth of subsequent QD layers. 相似文献
36.
Martin B. Duriska Dr. Suzanne M. Neville Dr. Boujemaa Moubaraki Dr. John D. Cashion Assoc. Prof Gregory J. Halder Dr. Karena W. Chapman Dr. Chérif Balde Jean‐François Létard Dr. Keith S. Murray Prof. Cameron J. Kepert Prof. Stuart R. Batten Assoc. Prof. 《Angewandte Chemie (International ed. in English)》2009,48(14):2549-2552
Bottoms up! A discrete metallo‐supramolecular nanoball (see picture), synthesized by using “bottom‐up” methodologies, uniquely undergoes a solvent‐sensitive, physically addressable electronic spin switching. The switching occurs by thermal, light, or solvent perturbation, where importantly it can be switched “on” or “off” by green or red laser irradiation, respectively.
37.
Martin B. Duriska Dr. Suzanne M. Neville Dr. Boujemaa Moubaraki Dr. John D. Cashion Assoc. Prof Gregory J. Halder Dr. Karena W. Chapman Dr. Chérif Balde Jean‐François Létard Dr. Keith S. Murray Prof. Cameron J. Kepert Prof. Stuart R. Batten Assoc. Prof. 《Angewandte Chemie (International ed. in English)》2009,48(14):2428-2428
Continuous switching between high‐spin and low‐spin magnetic states can be accomplished by irradiation with red and green laser light, respectively. In their Communication on page 2549 ff., S. R. Batten and co‐workers report a metallo‐supramolecule that undergoes spin crossover (SCO) switching induced by temperature change or light irradiation. The SCO behavior is also dependent on the presence and nature of intercalated solvent molecules within the porous crystal structure.
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Papia Datta Dibakar Sardar Uttam Panda Ajanta Halder Nabin Baran Manik Chun‐Jung Chen Chittaranjan Sinha 《应用有机金属化学》2016,30(5):323-334
Os(II) hydridocarbonyl complexes of coumarinyl azoimidazoles, [Osh(CO)(PPh3)2(CZ‐4R‐R′)]0/+ ( 3 , 4 ) (CZ‐R‐H = 2‐(coumarinyl‐6‐azo)‐4‐substituted imidazole or 1‐alkyl‐2‐(coumarinyl‐6‐azo)‐4‐substituted imidazole), were characterized from spectroscopic data and the single‐crystal X‐ray data for one of the complexes, [Osh(CO)(PPh3)2(CZ‐4‐Ph)] ( 3c ) (CZ‐4‐Ph = 2‐(coumarinyl‐6‐azo)‐4‐phenylimidazolate), confirmed the structure. The complexes show higher emission (quantum yield ? = 0.0163–0.16) and longer lifetime (τ = 1.4–10.3 ns) than free ligands (? = 0.0012–0.0185 and τ = 0.685–1.306 ns). Cyclic voltammetry shows quasi‐reversible metal oxidation at 0.67–0.94 V for [Os(III)/Os(II)] and 1.21–1.36 V for [Os(IV)/Os(III)] and subsequent azo reductions (?0.68 to ?0.95 V for [? N?N? ]/[? N N? ]? and irreversible < ?1.2 V for [? N N? ]?/[? N? N? ]2?) of the chelated coumarinyl azoimidazole. The complexes are photostable and show better photovoltaic power conversion efficiency than free ligands. Also, the complexes were used as catalysts for the oxidation of primary/secondary alcohols to aldehydes/ketones using oxidizing agents like N‐methylmorpholine N‐oxide, t‐BuOOH and H2O2. Density functional theory computation was carried out from the optimized structures and the data obtained were used to interpret the electronic and photovoltaic properties. Copyright © 2016 John Wiley & Sons, Ltd. 相似文献