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141.
142.
We explore whether our models for starbursts, quiescent star-forming galaxies and for active galactic nuclei (AGN) dust tori are able to model the full range of Spitzer Infrared Spectrograph (IRS) spectra measured with Spitzer . The diagnostic plot of 9.7 μm silicate optical depth versus 6.2 μm polycyclic aromatic hydrocarbon (PAH) equivalent width, introduced by Spoon and coworkers in 2007, gives a good indication of the age and optical depth of a starburst, and of the contribution of an AGN dust torus. However, there is aliasing between age and optical depth at later times in the evolution of a starburst, and between age and the presence of an AGN dust torus. Modelling the full IRS spectra and using broad-band 25–850 μm fluxes can help to resolve these aliases. The observed spectral energy distributions require starbursts of a range of ages with initial dust optical depth ranging from 50–200, optically thin dust emission ('cirrus') illuminated by a range of surface brightnesses of the interstellar radiation field, and AGN dust tori with a range of viewing angles.  相似文献   
143.
Abstract— Batch culture experiments were performed to investigate the weathering of meteoritic material by iron‐oxidizing bacteria. The aerobic, acidophilic iron oxidizer (A. ferrooxidans) was capable of oxidizing iron from both carbonaceous chondrites (Murchison and Cold Bokkeveld) and iron meteorites (York and Casas Grandes). Preliminary iron isotope results clearly show contrasted iron pathways during oxidation with and without bacteria suggesting that a biological role in meteorite weathering could be distinguished isotopically. Anaerobic iron‐oxidizers growing under pH‐neutral conditions oxidized iron from iron meteorites. These results show that rapid biologically‐mediated alteration of extraterrestrial materials can occur in both aerobic and anaerobic environments. These results also demonstrate that iron can act as a source of energy for microorganisms from both iron and carbonaceous chondrites in aerobic and anaerobic conditions with implications for life on the early Earth and the possible use of microorganisms to extract minerals from asteroidal material.  相似文献   
144.
In order to better understand the long-term speciation and fractionation of Zn in soils, we investigated three soils naturally enriched in Zn (237–864 mg/kg Zn) from the weathering of Zn-rich limestones (40–207 mg/kg Zn) using extended X-ray absorption fine structure (EXAFS) spectroscopy and sequential extractions. The analysis of bulk EXAFS spectra by linear combination fitting (LCF) indicated that Zn in the oolitic limestones was mainly present as Zn-containing calcite (at site Dornach), Zn-containing goethite (Gurnigel) and Zn-containing goethite and sphalerite (Liestal). Correspondingly, extraction of the powdered rocks with 1 M NH4-acetate at pH 6.0 mobilized only minor fractions of Zn from the Gurnigel and Liestal limestones (<30%), but most Zn from the Dornach rock (81%). In the Dornach soil, part of the Zn released from the dissolving limestone was subsequently incorporated into pedogenic hydroxy-interlayered vermiculite (Zn-HIV, 30%) and Zn-containing kaolinite (30%) and adsorbed or complexed by soil organic and inorganic components (40%). The Gurnigel and Liestal soils contained substantial amounts of Zn-containing goethite (50%) stemming from the parent rock, smaller amounts (20%) of Zn-containing kaolinite (and possibly Zn-HIV), as well as adsorbed or complexed Zn-species (30%). In the soil from Liestal, sphalerite was only found in trace amounts, indicating its dissolution during soil formation. In sequential extractions, large percentages of Zn (55–85%) were extracted in recalcitrant extraction steps, confirming that Zn-HIV, Zn-containing kaolinite and Zn-containing goethite are highly resistant to weathering. These Zn-bearing phases thus represent long-term hosts for Zn in soils over thousands of years. The capability of these phases to immobilize Zn in heavily contaminated soils may however be limited by their uptake capacity (especially HIV and kaolinite) or their abundance in soil.  相似文献   
145.
In many river basins, floodplain soils have accumulated a variety of metal contaminants, which might be released during periods of flooding. We investigated the dynamics of copper, cadmium, lead, zinc, and nickel in a contaminated freshwater floodplain soil under a realistic sulfate-limited flooding regime in microcosm experiments. We found that most contaminants were initially mobilized by processes driven by the reductive dissolution of Fe(III) and Mn(IV, III) (hydr)oxides. Subsequently, bacterial sulfate respiration resulted in the transformation of the entire available sulfate (2.3 mmol/kg) into chromous reducible sulfur (CRS). Cu K-edge X-ray absorption fine structure (XAFS) spectroscopy revealed that the soil Cu speciation changed from predominantly Cu(II) bound to soil organic matter (SOM) intermittently to 14% metallic Cu(0) and subsequently to 66% copper sulfide (CuxS). These CuxS precipitates accounted for most of the formed CRS, suggesting that CuxS was the dominant sulfide phase formed in the flooded soil. Sequential metal extractions, in agreement with CRS results, suggested that easily mobilizable Cd was completely and Pb partially sequestered in sulfide precipitates, controlling their dissolved concentrations to below detection limits. In contrast, Zn and Ni (as well as Fe) were hardly sequestered into sulfide phases, so that micromolar levels of dissolved Zn and Ni (and millimolar dissolved Fe(II)) persisted in the reduced soil. The finding that Cu, Cd, and Pb were sequestered (but hardly any Zn, Ni, and Fe) is consistent with the thermodynamically predicted sulfide ladder following the increasing solubility products of the respective metal sulfides. The observation that Cd and Pb were sequestered in sulfides despite the presence of remaining SOM-bound Cu(II) suggested that the kinetics of Cu(II) desorption, diffusion, and/or CuxS precipitation interfered with the sulfide ladder. We conclude that the dynamics of multiple metal contaminants are intimately coupled under sulfate limitation by the relative thermodynamic stabilities and formation kinetics of the respective metal sulfides.  相似文献   
146.
With previous two-dimensional (2D) simulations based on surface-specific feldspar dissolution succeeding in relating the macroscopic feldspar kinetics to the molecular-scale surface reactions of Si and Al atoms ( [Zhang and Lüttge, 2008] and [Zhang and Lüttge, 2009]), we extended our modeling effort to three-dimensional (3D) feldspar particle dissolution simulations. Bearing on the same theoretical basis, the 3D feldspar particle dissolution simulations have verified the anisotropic surface kinetics observed in the 2D surface-specific simulations. The combined effect of saturation state, pH, and temperature on the surface kinetics anisotropy has been subsequently evaluated, found offering diverse options for morphological evolution of dissolving feldspar nanoparticles with varying grain sizes and starting shapes. Among the three primary faces on the simulated feldspar surface, the (1 0 0) face has the biggest dissolution rate across an extensively wide saturation state range and thus acquires a higher percentage of the surface area upon dissolution. The slowest dissolution occurs to either (0 0 1) or (0 1 0) faces depending on the bond energies of Si-(O)-Si (ΦSi-O-Si/kT) and Al-(O)-Si (ΦAl-O-Si/kT). When the ratio of ΦSi-O-Si/kT to ΦAl-O-Si/kT changes from 6:3 to 7:5, the dissolution rates of three primary faces change from the trend of (1 0 0) > (0 1 0) > (0 0 1) to the trend of (1 0 0) > (0 0 1) > (0 1 0). The rate difference between faces becomes more distinct and accordingly edge rounding becomes more significant. Feldspar nanoparticles also experience an increasing degree of edge rounding from far-from-equilibrium to close-to-equilibrium. Furthermore, we assessed the connection between the continuous morphological modification and the variation in the bulk dissolution rate during the dissolution of a single feldspar particle. Different normalization treatments equivalent to the commonly used mass, cube assumption, sphere assumption, geometric surface area, and reactive surface area normalizations have been used to normalize the bulk dissolution rate. For each of the treatments, time consistence and grain size dependence of the normalized dissolution rate have been evaluated and the results revealed significant dependences on the magnitude of surface kinetic anisotropy under differing environmental conditions. In general, the normalized dissolution rates are strongly dependent on grain size. Time-consistent normalization treatment varies with the investigated condition. The modeling results suggest that the sphere-, cube-, and BET-normalized dissolution rates are appropriate under the far-from-equilibrium conditions at low pH where these normalizations are time-consistent and are slightly dependent on grain size.  相似文献   
147.
We investigated the structure of uranyl sorption complexes on gibbsite (pH 5.6-9.7) by two independent methods, density functional theory (DFT) calculations and extended X-ray absorption fine structure (EXAFS) spectroscopy at the U-LIII edge. To model the gibbsite surface with DFT, we tested two Al (hydr)oxide clusters, a dimer and a hexamer. Based on polarization, structure, and relaxation energies during geometry optimization, the hexamer cluster was found to be the more appropriate model. An additional advantage of the hexamer model is that it represents both edges and basal faces of gibbsite. The DFT calculations of (monomeric) uranyl sorption complexes show an energetic preference for the corner-sharing versus the edge-sharing configuration on gibbsite edges. The energy difference is so small, however, that possibly both surface species may coexist. In contrast to the edge sites, sorption to basal sites was energetically not favorable. EXAFS spectroscopy revealed in all investigated samples the same interatomic distances of the uranyl coordination environment (RU-Oax ≈ 1.80 Å, RU-Oeq ≈ 2.40 Å), and towards the gibbsite surface (RU-O ≈ 2.87 Å, RU-Al ≈ 3.38 Å). In addition, two U-U distances were observed, 3.92 Å at pH 9.7 and 4.30 Å at pH 5.6, both with coordination numbers of ∼1. The short U-U distance is close to that of the aqueous uranyl hydroxo dimer, UO2(OH)2, reported as 3.875 Å in the literature, but significantly longer than that of aqueous trimers (3.81-3.82 Å), suggesting sorption of uranyl dimers at alkaline pH. The longer U-U distance (4.30 Å) at acidic pH, however, is not in line with known aqueous uranyl polymer complexes. Based on the EXAFS findings we further refined dimeric surface complexes with DFT. We propose two structural models: in the acidic region, the observed long U-U distance can be explained with a distortion of the uranyl dimer to form both a corner-sharing and an edge-sharing linkage to neighboring Al octahedra, leading to RU-U = 4.150 Å. In the alkaline region, a corner-sharing uranyl dimer complex is the most favorable. The U-O path at ∼2.87 Å in the EXAFS spectra arises from the oxygen atom linking two Al cations in corner-sharing arrangement. The adsorption structures obtained by DFT calculations are in good agreement with the structural parameters from EXAFS analysis: U-Al (3.394 Å), U-U (3.949 Å), and U-O (2.823 Å) for the alkaline pH model, and U-Al (3.279 Å), U-U (4.150 Å), and U-O (2.743 Å) for the acidic pH model. This work shows that by combining EXAFS and DFT, consistent structural models for uranyl sorption complexes can be obtained, which are relevant to predict the migration behavior of uranium at nuclear facilities.  相似文献   
148.
This paper reports the results of an investigation of the Weichselian Upper Pleniglacial loess sequences of Nussloch (Rhine Valley, Germany) based on stratigraphy, palaeopedology, sedimentology, palynology, malacology and geochemistry (δ13C), supported by radiocarbon, TL and OSL dating. Grain-size and magnetic susceptibility records are taken at 5 cm intervals from the Upper Pleniglacial (UPG) loess. The data indicate cyclic variations in loess deposition between ca 34 and 17 ka, when the sedimentation rate is especially high (1.0–1.2 m per ka for more than 10 m). The grain-size index (GSI: ratio of coarse silt versus fine silt and clay) shows variations, which are assumed to be an indirect measurement of wind intensity. The sedimentation rate, interpreted from the profiles, indicates high values in loess (Loess events LE-1 to LE-7) and low or negligible values in tundra gley horizons G1 to G8. OSL ages from the loess and 14C dates from organic matter in the loess show that loess deposition was rapid but was interrupted by shorter periods of reduced aeolian sedimentation. Comparison between the data from Nussloch and other European sequences demonstrates a progressive coarsening of the loess deposits between ca 30 and 22 ka. This coarsening trend ends with a short but major grain-size decrease and is followed by an increase to a new maximum at 20 ± 2 ka (“W” shape). Correlation between the loess GSI and the Greenland ice-core dust records, suggests a global connection between North Atlantic and Western European global atmospheric circulation and wind regimes. In addition, the typical Upper Pleniglacial loess deposition begins at ca 30–31 ka, close to Heinrich event (HE) 3, and the main period of loess sedimentation at about 25 ± 2 ka is coeval to HE 2. Correlation of magnetic susceptibility and grain-size records shows that the periods, characterised by high GSI, coincide with an increase in the amount of ferromagnetic minerals reworked from the Rhine alluvial plain. They suggest enhancement in the frequency of the storms from N–NW. These results are integrated within a palaeogeographical model of dust transport and deposition in Western Europe for the Weichselian Upper Pleniglacial (or Late Pleniglacial).  相似文献   
149.
Phase angle and temperature are two important parameters that affect the photometric and spectral behavior of planetary surfaces in telescopic and spacecraft data. We have derived photometric and spectral phase functions for the Asteroid 4 Vesta, the first target of the Dawn mission, using ground-based telescopes operating at visible and near-infrared wavelengths (0.4–2.5 μm). Photometric lightcurve observations of Vesta were conducted on 15 nights at a phase angle range of 3.8–25.7° using duplicates of the seven narrowband Dawn Framing Camera filters (0.4–1.0 μm). Rotationally resolved visible (0.4–0.7 μm) and near-IR spectral observations (0.7–2.5 μm) were obtained on four nights over a similar phase angle range. Our Vesta photometric observations suggest the phase slope is between 0.019 and 0.029 mag/deg. The G parameter ranges from 0.22 to 0.37 consistent with previous results (e.g., Lagerkvist, C.-I., Magnusson, P., Williams, I.P., Buontempo, M.E., Argyle, R.W., Morrison, L.V. [1992]. Astron. Astrophys. Suppl. Ser. 94, 43–71; Piironen, J., Magnusson, P., Lagerkvist, C.-I., Williams, I.P., Buontempo, M.E., Morrison, L.V. [1997]. Astron. Astrophys. Suppl. Ser. 121, 489–497; Hasegawa, S. et al. [2009]. Lunar Planet. Sci. 40. ID 1503) within the uncertainty. We found that in the phase angle range of 0° < α ? 25° for every 10° increase in phase angle Vesta’s visible slope (0.5–0.7 μm) increases 20%, Band I and Band II depths increase 2.35% and 1.5% respectively, and the BAR value increase 0.30. Phase angle spectral measurements of the eucrite Moama in the lab show a decrease in Band I and Band II depths and BAR from the lowest phase angle 13° to 30°, followed by possible small increases up to 90°, and then a dramatic drop between 90° and 120° phase angle. Temperature-induced spectral effects shift the Band I and II centers of the pyroxene bands to longer wavelengths with increasing temperature. We have derived new correction equations using a temperature series (80–400 K) of HED meteorite spectra that will enable interpretation of telescopic and spacecraft spectral data using laboratory calibrations at room temperature (300 K).  相似文献   
150.
GETEMME (Gravity, Einstein??s Theory, and Exploration of the Martian Moons?? Environment), a mission which is being proposed in ESA??s Cosmic Vision program, shall be launched for Mars on a Soyuz Fregat in 2020. The spacecraft will initially rendezvous with Phobos and Deimos in order to carry out a comprehensive mapping and characterization of the two satellites and to deploy passive Laser retro-reflectors on their surfaces. In the second stage of the mission, the spacecraft will be transferred into a lower 1500-km Mars orbit, to carry out routine Laser range measurements to the reflectors on Phobos and Deimos. Also, asynchronous two-way Laser ranging measurements between the spacecraft and stations of the ILRS (International Laser Ranging Service) on Earth are foreseen. An onboard accelerometer will ensure a high accuracy for the spacecraft orbit determination. The inversion of all range and accelerometer data will allow us to determine or improve dramatically on a host of dynamic parameters of the Martian satellite system. From the complex motion and rotation of Phobos and Deimos we will obtain clues on internal structures and the origins of the satellites. Also, crucial data on the time-varying gravity field of Mars related to climate variation and internal structure will be obtained. Ranging measurements will also be essential to improve on several parameters in fundamental physics, such as the Post-Newtonian parameter ?? as well as time-rate changes of the gravitational constant and the Lense-Thirring effect. Measurements by GETEMME will firmly embed Mars and its satellites into the Solar System reference frame.  相似文献   
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