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101.
Perovskite solar cells (PSCs) have advanced rapidly with power conversion efficiencies (PCEs) now exceeding 22%. Due to the long diffusion lengths of charge carriers in the photoactive layer, a PSC device architecture comprising an electron‐ transporting layer (ETL) is essential to optimize charge flow and collection for maximum performance. Here, a novel approach is reported to low temperature, solution‐processed ZnO ETLs for PSCs using combustion synthesis. Due to the intrinsic passivation effects, high crystallinity, matched energy levels, ideal surface topography, and good chemical compatibility with the perovskite layer, this combustion‐derived ZnO enables PCEs approaching 17–20% for three types of perovskite materials systems with no need for ETL doping or surface functionalization.  相似文献   
102.
Developing efficient interfacial hole transporting materials (HTMs) is crucial for achieving high‐performance Pb‐free Sn‐based halide perovskite solar cells (PSCs). Here, a new series of benzodithiophene (BDT)‐based organic small molecules containing tetra‐ and di‐triphenyl amine donors prepared via a straightforward and scalable synthetic route is reported. The thermal, optical, and electrochemical properties of two BDT‐based molecules are shown to be structurally and energetically suitable to serve as HTMs for Sn‐based PSCs. It is reported here that ethylenediammonium/formamidinium tin iodide solar cells using BDT‐based HTMs deliver a champion power conversion efficiency up to 7.59%, outperforming analogous reference solar cells using traditional and expensive HTMs. Thus, these BDT‐based molecules are promising candidates as HTMs for the fabrication of high‐performance Sn‐based PSCs.  相似文献   
103.
Bulk‐heterojunction organic photovoltaic materials containing nonfullerene acceptors (NFAs) have seen remarkable advances in the past year, finally surpassing fullerenes in performance. Indeed, acceptors based on indacenodithiophene (IDT) have become synonymous with high power conversion efficiencies (PCEs). Nevertheless, NFAs have yet to achieve fill factors (FFs) comparable to those of the highest‐performing fullerene‐based materials. To address this seeming anomaly, this study examines a high efficiency IDT‐based acceptor, ITIC , paired with three donor polymers known to achieve high FFs with fullerenes, PTPD3T , PBTI3T , and PBTSA3T . Excellent PCEs up to 8.43% are achieved from PTPD3T:ITIC blends, reflecting good charge transport, optimal morphology, and efficient ITIC to PTPD3T hole‐transfer, as observed by femtosecond transient absorption spectroscopy. Hole‐transfer is observed from ITIC to PBTI3T and PBTSA3T , but less efficiently, reflecting measurably inferior morphology and nonoptimal energy level alignment, resulting in PCEs of 5.34% and 4.65%, respectively. This work demonstrates the importance of proper morphology and kinetics of ITIC → donor polymer hole‐transfer in boosting the performance of polymer: ITIC photovoltaic bulk heterojunction blends.  相似文献   
104.
High‐performance solution‐processed metal oxide (MO) thin‐film transistors (TFTs) are realized by fabricating a homojunction of indium oxide (In2O3) and polyethylenimine (PEI)‐doped In2O3 (In2O3:x% PEI, x = 0.5–4.0 wt%) as the channel layer. A two‐dimensional electron gas (2DEG) is thereby achieved by creating a band offset between the In2O3 and PEI‐In2O3 via work function tuning of the In2O3:x% PEI, from 4.00 to 3.62 eV as the PEI content is increased from 0.0 (pristine In2O3) to 4.0 wt%, respectively. The resulting devices achieve electron mobilities greater than 10 cm2 V?1 s?1 on a 300 nm SiO2 gate dielectric. Importantly, these metrics exceed those of the devices composed of the pristine In2O3 materials, which achieve a maximum mobility of ≈4 cm2 V?1 s?1. Furthermore, a mobility as high as 30 cm2 V?1 s?1 is achieved on a high‐k ZrO2 dielectric in the homojunction devices. This is the first demonstration of 2DEG‐based homojunction oxide TFTs via band offset achieved by simple polymer doping of the same MO material.  相似文献   
105.
Electrocatalytic two-electron reduction of oxygen is a promising method for producing sustainable H2O2 but lacks low-cost and selective electrocatalysts. Here, the Chevrel phase chalcogenide Ni2Mo6S8 is presented as a novel active motif for reducing oxygen to H2O2 in an aqueous electrolyte. Although it has a low surface area, the Ni2Mo6S8 catalyst exhibits exceptional activity for H2O2 synthesis with >90% H2O2 molar selectivity across a wide potential range. Chemical titration verified successful generation of H2O2 and confirmed rates as high as 90 mmol H2O2 gcat−1 h−1. The outstanding activities are attributed to the ligand and ensemble effects of Ni that promote H2O dissociation and proton-coupled reduction of O2 to HOO*, and the spatial effect of the Chevrel phase structure that isolates Ni active sites to inhibit O O cleavage. The synergy of these effects delivers fast and selective production of H2O2 with high turn-over frequencies of ≈30 s−1. In addition, the Ni2Mo6S8 catalyst has a stable crystal structure that is resistive for oxidation and delivers good catalyst stability for continuous H2O2 production. The described Ni-Mo6S8 active motif can unlock new opportunities for designing Earth-abundant electrocatalysts to tune oxygen reduction for practical H2O2 production.  相似文献   
106.
We report on the observability of valence bonding effects in aberration-corrected high resolution electron microscopy (HREM) images along the [0 1 0] projection of the mineral Forsterite (Mg2SiO4). We have also performed exit wave restorations using simulated noisy images and have determined that both the intensities of individual images and the modulus of the restored complex exit wave are most sensitive to bonding effects at a level of 25% for moderately thick samples of 20-25 nm. This relatively large thickness is due to dynamical amplification of bonding contrast arising from partial de-channeling of 1s states. Simulations also suggest that bonding contrast is similarly high for an un-corrected conventional electron microscope, implying an experimental limitation of signal to noise ratio rather than spatial resolution.  相似文献   
107.
Deng B  Marks LD  Rondinelli JM 《Ultramicroscopy》2007,107(4-5):374-381
We investigate the effects of local charge defects in HREM imaging, using electron densities calculated by density functional methods. As a model of a planar interface with a local charge defect we use the polar MgO square root (111)-3 x 3R30 degrees surface, which has an additional hole per surface unit cell. A complimentary example, the non-polar MgO (100) surface that has no local charge defect is simulated for comparison. We show that the contrast due to local charge defects is rather high, and suggest that they should be directly observable.  相似文献   
108.
Results of atmospheric total gaseous mercury (TGM) measurements performed at two Baltic Sea coastal stations, Peninsula Hel (Poland) and Preila (Lithuania), from June 16 to August 11, 1997, are presented. High time-resolution data were obtained by using automated atomic absorption mercury vapor analyzers (Model Gardis-1A). Analysis of TGM concentration data (directional distribution, correlation with meteorological parameters, diurnal variability) detected the Baltic sea, in particular its southern part and Gulf of Gdansk, as the main gaseous mercury source for the region during the summer months. The source seemed to be activated by solar radiation, air temperature, and, probably, wind.  相似文献   
109.
We propose a novel method of measuring the group refractive index of biological tissues at the micrometer scale. The technique utilizes a broadband confocal microscope embedded into a Mach-Zehnder interferometer, with which spectral interferograms are measured as the sample is translated through the focus of the beam. The method does not require phase unwrapping and is insensitive to vibrations in the sample and reference arms. High measurement stability is achieved because a single spectral interferogram contains all the information necessary to compute the optical path delay of the beam transmitted through the sample. Included are a physical framework defining the forward problem, linear solutions to the inverse problem, and simulated images of biologically relevant phantoms.  相似文献   
110.
Full-field optical coherence tomography (OCT) is able to image an entire en face plane of scatterers simultaneously, but typically the focus is scanned through the volume to acquire three-dimensional structure. By solving the inverse scattering problem for full-field OCT, we show it is possible to computationally reconstruct a three-dimensional volume while the focus is fixed at one plane inside the sample. While a low-numerical-aperture (NA) OCT system can tolerate defocus because the depth of field is large, for high NA it is critical to correct for defocus. By deriving a solution to the inverse scattering problem for full-field OCT, we propose and simulate an algorithm that recovers object structure both inside and outside the depth of field, so that even for high NA the focus can be fixed at a particular plane within the sample without compromising resolution away from the focal plane.  相似文献   
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