全文获取类型
收费全文 | 598篇 |
免费 | 8篇 |
专业分类
化学 | 326篇 |
晶体学 | 3篇 |
力学 | 9篇 |
数学 | 77篇 |
物理学 | 191篇 |
出版年
2022年 | 4篇 |
2021年 | 4篇 |
2020年 | 4篇 |
2019年 | 8篇 |
2018年 | 5篇 |
2017年 | 7篇 |
2016年 | 7篇 |
2015年 | 5篇 |
2014年 | 6篇 |
2013年 | 49篇 |
2012年 | 15篇 |
2011年 | 27篇 |
2010年 | 21篇 |
2009年 | 14篇 |
2008年 | 26篇 |
2007年 | 28篇 |
2006年 | 33篇 |
2005年 | 22篇 |
2004年 | 15篇 |
2003年 | 15篇 |
2002年 | 14篇 |
2001年 | 13篇 |
2000年 | 19篇 |
1999年 | 9篇 |
1998年 | 4篇 |
1997年 | 6篇 |
1996年 | 19篇 |
1995年 | 14篇 |
1994年 | 14篇 |
1993年 | 7篇 |
1992年 | 16篇 |
1991年 | 12篇 |
1990年 | 4篇 |
1989年 | 10篇 |
1988年 | 9篇 |
1987年 | 5篇 |
1986年 | 8篇 |
1985年 | 9篇 |
1984年 | 9篇 |
1983年 | 4篇 |
1982年 | 4篇 |
1981年 | 7篇 |
1979年 | 5篇 |
1976年 | 5篇 |
1975年 | 5篇 |
1974年 | 11篇 |
1973年 | 10篇 |
1972年 | 4篇 |
1971年 | 6篇 |
1862年 | 2篇 |
排序方式: 共有606条查询结果,搜索用时 31 毫秒
1.
Yalda Liaghati Mobarhan Ronald Soong Daniel Lane Andre J. Simpson 《Magnetic resonance in chemistry : MRC》2020,58(5):427-444
Traditionally, due to different hardware requirements, nuclear magnetic resonance (NMR) has developed as two separate fields: one dealing with solids, and one with solutions. Comprehensive multiphase (CMP) NMR combines all electronics and hardware (magic angle spinning [MAS], gradients, high power Radio Frequency (RF) handling, lock, susceptibility matching) into a universal probe that permits a comprehensive study of all phases (i.e., liquid, gel-like, semisolid, and solid), in intact samples. When applied in vivo, it provides unique insight into the wide array of bonds in a living system from the most mobile liquids (blood, fluids) through gels (muscle, tissues) to the most rigid (exoskeleton, shell). In this tutorial, the practical aspects of in vivo CMP NMR are discussed including: handling the organisms, rotor preparation, sample spinning, water suppression, editing experiments, and finishes with a brief look at the potential of other heteronuclei (2H, 15N, 19F, 31P) for in vivo research. The tutorial is aimed as a general resource for researchers interested in developing and applying MAS-based approaches to living organisms. Although the focus here is CMP NMR, many of the approaches can be adapted (or directly applied) using conventional high-resolution magic angle spinning, and in some cases, even standard solid-state NMR probes. 相似文献
2.
Anna Arkhireeva John N. Hay Jackie M. Lane Miguel Manzano Helen Masters Wilberforce Oware Steve J. Shaw 《Journal of Sol-Gel Science and Technology》2004,31(1-3):31-36
The synthesis of ORganically MOdified SILica (ORMOSIL) particles has been carried out using both the hydrolytic and non-hydrolytic sol-gel routes. The hybrid (nano)composites are organically modified with an alkyl or aryl group covalently bonded to silicon. Hybrids have been synthesised in an aqueous sol-gel process by a modified Stöber route, producing spherical nanoparticles with diameters in the range 50–300 nm. The size of the particles can be controlled by control of certain reaction parameters. Smaller ormosil nanoparticles can be synthesised by a base-catalysed emulsion polymerisation route, by varying the type and concentration of surfactant and precursor feed rate. In this case, particles in the size range 3.5–10 nm can be obtained. Hybrids have been synthesised from hyperbranched polyesters by encapsulation in a silica matrix using the hydrolytic sol-gel route. Optimisation of the reaction conditions allows the hybrids to be produced as isolated sub-micron spherical particles. Ormosil particles have also been synthesised using the non-hydrolytic sol-gel route, which may lead to products of different morphologies because of the different polarity of the reaction medium. Different reaction conditions were studied in order to optimise the size and shape of the particles, including choice of solvent, use of surfactants and addition of polystyrene. Dimethylsulfoxide acts as a novel oxygen donor for the catalyst-free formation of colourless silsesquioxanes. 相似文献
3.
4.
W.P. RDZANEK JR 《Journal of sound and vibration》2002,249(2):307-323
The standardized mutual active and reactive sound power of a clamped plate, representing the energy aspect of the reciprocal interactions of two different in vacuo modes, has been computed. It was assumed that the vibrations are axisymmetric, elastic and time harmonic, the plate's transverse deflection is small as compared with the plate's size, and that the vibration velocity is small as compared with the acoustic wavenumber generated. The Kirchhoff-Love theory of a perfectly elastic plate was used. The integral formulae for the mutual sound power were transformed into their Hankel representations which made possible their subsequent computation. A closed path integral was used to express the integral in its Hankel representation to compute the mutual active sound power. The asymptotic stationary phase method was used to compute the two magnitudes, i.e., the mutual active and reactive sound power. The results obtained are the asymptotic formulae valid for the acoustically fast waves. The oscillating as well as the non-oscillating terms have been identified in the formulae to make possible their further separate analysis. The availability of the asymptotic formulae makes possible some fast numerical computations of the mutual sound power. Moreover, the formulae presented herein, together with those for the individual modes known from the literature, make a complete basis for further computations of the total sound power of the plate's damped and forced vibrations in fluid. 相似文献
5.
Speech deterioration in postlingually deafened adults 总被引:1,自引:0,他引:1
Postlinngually deafened adults reading the Rainbow Passage differed from hearing-control subjects in producing greater pitch variability and mean pitch on stressed and unstressed vowels, greater fluctuations in pitch within sentences, less correlation of intrinsic pitch with vowel height and slower temporal parameters. When reading the Phonetic Inventory Sentences, they revealed less differentiation of place of articulation in fricative and plosive consonants. The present findings, taken together with those of longitudinal and implant studies, are applied to constraining models of the role of self hearing in the elaboration of speech. 相似文献
6.
J Perkell H Lane M Svirsky J Webster 《The Journal of the Acoustical Society of America》1992,91(5):2961-2978
Acoustic parameters were measured for vowels spoken in /hVd/ context by four postlingually deafened recipients of multichannel (Ineraid) cochlear implants. Three of the subjects became totally deaf in adulthood after varying periods of partial hearing loss; the fourth became totally deaf at age four. The subjects received different degrees of perceptual benefit from the prosthesis. Recordings were made before, and at intervals following speech processor activation. The measured parameters included F1, F2, F0, SPL, duration, and amplitude difference between the first two harmonic peaks in the log magnitude spectrum (H 1-H2). Numerous changes in parameter values were observed from pre- to post-implant, with differences among subjects. Many changes, but not all, were in the direction of normative data, and most changes were consistent with hypotheses about relations among the parameters. Some of the changes tended to enhance phonemic contrasts; others had the opposite effect. For three subjects, H 1-H2 changed in a direction consistent with measurements of their average air flow when reading; that relation was more complex for the fourth subject. The results are interpreted with respect to: characteristics of the individual subjects, including vowel identification scores; mechanical interactions among glottal and supraglottal articulations; and hypotheses about the role of auditory feedback in the control of speech production. Almost all the observed differences could be attributed to changes in the average settings of speaking rate, F0 and SPL, which presumably can be perceived without the need for spectral place information. Some observed F2 realignment may be attributable to the reception of spectral cues. 相似文献
7.
M A Svirsky H Lane J S Perkell J Wozniak 《The Journal of the Acoustical Society of America》1992,92(3):1284-1300
Speech production parameters of three postlingually deafened adults who use cochlear implants were measured: after 24 h of auditory deprivation (which was achieved by turning the subject's speech processor off); after turning the speech processor back on; and after turning the speech processor off again. The measured parameters included vowel acoustics [F1, F2, F0, sound-pressure level (SPL), duration and H1-H2, the amplitude difference between the first two spectral harmonics, a correlate of breathiness] while reading word lists, and average airflow during the reading of passages. Changes in speech processor state (on-to-off or vice versa) were accompanied by numerous changes in speech production parameters. Many changes were in the direction of normalcy, and most were consistent with long-term speech production changes in the same subjects following activation of the processors of their cochlear implants [Perkell et al., J. Acoust. Soc. Am. 91, 2961-2978 (1992)]. Changes in mean airflow were always accompanied by H1-H2 (breathiness) changes in the same direction, probably due to underlying changes in laryngeal posture. Some parameters (different combinations of SPL, F0, H1-H2 and formants for different subjects) showed very rapid changes when turning the speech processor on or off. Parameter changes were faster and more pronounced, however, when the speech processor was turned on than when it was turned off. The picture that emerges from the present study is consistent with a dual role for auditory feedback in speech production: long-term calibration of articulatory parameters as well as feedback mechanisms with relatively short time constants. 相似文献
8.
A. Hempel B. G. Lane N. Camerman 《Acta Crystallographica. Section C, Structural Chemistry》1997,53(11):1707-1709
9.
C. A. Rinaldi J. C. Ferrero S. I. Lane E. V. Oexler 《Journal of Chemical Sciences》1991,103(3):465-469
The IR multiphoton dissociation of CF3I has been studied in the presence of isobutane and with isobutane and Ar and CO2 as inert gases. The dependence of the reaction probability P(Φ) with fluence (ϕ) is confirmed. Modeling of the experimental results shows that for the energy transfer processes the average energy transferred
per collision 〈†E〉d varies with (ϕ). 相似文献
10.
Spikmans V Lane SJ Leavens B Manz A Smith NW 《Rapid communications in mass spectrometry : RCM》2002,16(14):1377-1388
A system is presented that demonstrates the principle of on-line and on-chip post-column derivatisation reactions in micro-high-performance liquid chromatography (micro-HPLC) hyphenated to electrospray time-of-flight mass spectrometry (ESI-TOFMS). In this micro-HPLC-chip-MS set-up, the analytes are separated using gradient micro-HPLC and subsequently derivatised on-chip and detected. One of the major limitations of MS detection is its dependency on the degree of ionisation, which is widely variable and compound-specific. Optimising and controlling the degree of ionisation in a simple manner would allow MS detection to be truly generic. One way of achieving this is by pre-ionisation of analytes using simple derivatisation procedures that are both rapid and quantitative. Performing this in situ on the system described here overcomes issues of sample handling and efficiency losses when time-consuming "bench chemistry" is necessary prior to analysis. The power of the system is demonstrated by the separation of primary and secondary amines, which are subsequently derivatised with a positively charged phosphonium complex and detected in an enhanced manner. Typically, molecular cations (M(+)) are detected showing that the ionisation process is dominated by the phosphonium species, leading to more constant ionisation for a variety of compounds. In addition, stable isotopically labelled ((12)C/(13)C)-phosphonium reagent is used for the reactions, allowing for inherent signal/noise (S/N) improvement and automated data processing using cluster analysis. A similar reaction scheme is used for the derivatisation of ketones and aldehydes, also demonstrating dramatic increases in sensitivity, especially with increasing temperature. Minimal loss in chromatographic fidelity in terms of retention times is observed by the introduction of the micromixer chip into the system. Optimal flow rates in micro-HPLC and ESI-MS are compatible with flow rates for the chip as well as a multitude of in-line optical detectors including UV and fluorescence. In addition, the micromixer chip can be positioned pre-column if preferred. The system is robust, easily fully automated and applicable to a wide variety of reactions. The system has a major advantage in its simple robust connection to the "normal scale" outside world. 相似文献