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991.
Dr. Dennis Svatunek Nicole Houszka Dr. Trevor A. Hamlin Prof. Dr. F. Matthias Bickelhaupt Dr. Hannes Mikula 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(3):754-758
The strain-promoted alkyne-azide cycloaddition (SPAAC) is the most commonly employed bioorthogonal reaction with applications in a broad range of fields. Over the years, several different cyclooctyne derivatives have been developed and investigated in regard to their reactivity in SPAAC reactions with azides. However, only a few studies examined the influence of structurally diverse azides on reaction kinetics. Herein, we report our investigations of the reactivity of primary, secondary, and tertiary azides with the cyclooctynes BCN and ADIBO applying experimental and computational methods. All azides show similar reaction rates with the sterically non-demanding cyclooctyne BCN. However, due to the increased steric demand of the dibenzocyclooctyne ADIBO, the reactivity of tertiary azides drops by several orders of magnitude in comparison to primary and secondary azides. We show that this chemoselective behavior of tertiary azides can be exploited to achieve semiorthogonal dual-labeling without the need for any catalyst using SPAAC exclusively. 相似文献
992.
Alex van der Ham Thomas Hansen Dr. Gerrit Lodder Dr. Jeroen D. C. Codée Dr. Trevor A. Hamlin Dr. Dmitri V. Filippov 《Chemphyschem》2019,20(16):2103-2109
Lithium ion selective crown ethers have been the subject of much research for a multitude of applications. Current research is aimed at structurally rigidifying crown ethers, as restructuring of the crown ether ring upon ion binding is energetically unfavorable. In this work, the lithium ion binding ability of the relatively rigid 8-crown-4 was investigated both computationally by density functional theory calculations and experimentally by 1H and 7Li NMR spectroscopy. Although both computational and experimental results showed 8-crown-4 to bind lithium ion, this binding was found to be weak compared to larger crown ethers. The computational analysis revealed that the complexation is driven by enthalpy rather than entropy, illustrating that rigidity is only of nominal importance. To elucidate the origin of the favorable interaction of lithium ion with crown ethers, activation strain analyses and energy decomposition analyses were performed pointing to the favorable interaction being mainly electrostatic in nature. 8-crown-4 presents the smallest crown ether reported to date capable of binding lithium ion, possessing two distinct conformations from which it is able to do so. 相似文献
993.
We present an all-fiber sensor for simultaneous measurement of temperature and strain. The sensing head is formed by introducing a fiber Bragg grating into a high-birefringence fiber loop mirror that acts as a Mach-Zehnder interferometer for temperature and strain discrimination. A sensing resolution of ±1 °C in temperature and ±21 με in strain has been experimentally achieved over a temperature range of 60 °C and strain range of 600 με. 相似文献
994.
995.
Radiofrequency ablation is the most common minimally invasive therapy used in the United States to treat hepatocellular carcinoma and liver metastases. The ability to perform real-time temperature imaging while a patient is undergoing ablation therapy may help reduce the high recurrence rates following ablation therapy. Ultrasound echo signals undergo time shifts with increasing temperature due to sound speed and thermal expansion, which are tracked using both 1D cross correlation and 2D block matching based speckle tracking methods. In this paper, we present a quantitative evaluation of the accuracy and precision of temperature estimation using the above algorithms on both simulated and experimental data.A finite element analysis simulation of radiofrequency ablation of hepatic tissue was developed. Finite element analysis provides a method to obtain the exact temperature distribution along with a mapping of the tissue displacement due to thermal expansion. These local displacement maps were combined with the displacement due to speed of sound changes and utilized to generate ultrasound radiofrequency frames at specified time increments over the entire ablation procedure. These echo signals provide an ideal test-bed to evaluate the performance of both speckle tracking methods, since the estimated temperature results can be compared directly to the exact finite element solution. Our results indicate that the 1D cross-correlation (CC) method underestimates the cumulative displacement by 0.20 mm, while the underestimation with 2D block matching (BM) is about 0.14 mm after 360 s of ablation. The 1D method also overestimates the size of the ablated region by 5.4% when compared to 2.4% with the 2D method after 720 s of ablation. Hence 2D block matching provides better tracking of temperature variations when compared to the 1D cross-correlation method over the entire duration of the ablation procedure. In addition, results obtained using 1D cross-correlation diverge from the ideal finite element results after 7 min of ablation and for temperatures greater than 65 °C.In a similar manner, experimental results presented using a tissue-mimicking phantom also demonstrate that the maximum percent difference with 2D block matching was 5%, when compared to 31% with the 1D method over the 700 s heating duration on the phantom. 相似文献
996.
由于探测光脉冲宽度受到限制,布里渊光时域反射仪(BOTDR)在对光纤上的应变进行分布式测量时,空间分辨力只能达到1 m。针对布里渊光时域反射仪单次采样接收背向布里渊散射信号(BBS)需要一定的时间,提出了基于等效脉冲光的多洛仑兹拟合法以提高其应变测量的空间分辨力。该方法将探测光脉冲在布里渊光时域反射仪完成单次采样所需的时间上进行积分,将积分函数作为等效脉冲光的表达式,再根据等效脉冲光的形状将布里渊光时域反射仪接收到的背向布里渊散射谱(BBS)细分,并对它进行多洛仑兹迭代拟合,准确求得每个细分布里渊散射谱的中心频率,进而利用光纤中布里渊频移与应变的对应关系,得到光纤中与细分布里渊散射谱对应的细分光纤单元上的应变情况。实验结果表明,利用这种方法,可使布里渊光时域反射仪应变测量的空间分辨力提高至0.05 m。 相似文献
997.
The EPR g factors gi (i = x, y, z) for the interstitial Ti3+ in rutile are theoretically studied from the perturbation formulas of these parameters for a 3d1 ion in rhombically compressed octahedra. The ligand octahedron in the impurity center is found to be less compressed than
that on the host interstitial site due to the Jahn-Teller effect. The local compression parameter (≈0.026) and the rhombic
distortion angle δϕ′ (≈0.7°) around the impurity Ti3+ are smaller than the host values (≈0.091 and 3.5°). The theoretical g factors based on the above local structural parameters are in good agreement with the experimental data. In addition, the
g factors for a tetragonal interstitial Ti3+ center are also reasonably interpreted.
相似文献
998.
We present an analytic study of the physics of the glasma which is a strong classical gluon field created at early stage of high-energy heavy-ion collisions. Our analysis is based on the picture that the glasma just after the collision is made of color electric and magnetic flux tubes extending in the longitudinal direction with their diameters of the order of 1/Qs (Qs is the saturation scale of the colliding nuclei). We find that both the electric and magnetic flux tubes expand outwards and the field strength inside the flux tube decays rapidly in time. Next we investigate whether there exist instabilities against small rapidity-dependent perturbations for a fixed color configuration. We find that the magnetic background field exhibits an instability induced by the fluctuations in the lowest Landau level, and it grows exponentially in the time scale of 1/Qs. For the electric background field we find no apparent instability while the possible relation to the Schwinger mechanism for particle pair creations is suggested. 相似文献
999.
We examine the time evolution of a quantized field in external backgrounds that violate the stability of vacuum (particle-creating backgrounds). Our purpose is to study the exact form of the final quantum state (the density operator at the final instant of time) that has emerged from a given arbitrary initial state (from a given arbitrary density operator at the initial time instant) in the course of evolution. We find a generating functional that allows one to obtain density operators for an arbitrary initial state. Averaging over states of the subsystem of antiparticles (particles), we obtain explicit forms of reduced density operators for the subsystem of particles (antiparticles). Analyzing one-particle correlation functions, we establish a one-to-one correspondence between these functions and the reduced density operators. It is shown that in the general case a presence of bosons (e.g., gluons) in the initial state increases the creation rate of the same type of bosons. We discuss the question (and its relation to the initial stage of quark–gluon plasma formation) whether a thermal form of one-particle distribution can appear even if the final state of the complete system is not in thermal equilibrium. In this respect, we discuss some cases when pair-creation by an electric-like field can mimic the one-particle thermal distribution. We apply our technics to some QFT problems in slowly varying electric-like backgrounds: electric, SU(3) chromoelectric, and metric. In particular, we analyze the time and temperature behavior of the mean numbers of created particles, provided that the effects of switching the external field on and off are negligible. It is demonstrated that at high temperatures and in slowly varying electric fields the rate of particle-creation is essentially time-dependent. 相似文献
1000.