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排序方式: 共有60条查询结果,搜索用时 15 毫秒
1.
Myron S. Huzan Manuel Fix Matteo Aramini Peter Bencok J. Frederick W. Mosselmans Shusaku Hayama Franziska A. Breitner Leland B. Gee Charles J. Titus Marie-Anne Arrio Anton Jesche Michael L. Baker 《Chemical science》2020,11(43):11801
Large single-ion magnetic anisotropy is observed in lithium nitride doped with iron. The iron sites are two-coordinate, putting iron doped lithium nitride amongst a growing number of two coordinate transition metal single-ion magnets (SIMs). Uniquely, the relaxation times to magnetisation reversal are over two orders of magnitude longer in iron doped lithium nitride than other 3d-metal SIMs, and comparable with high-performance lanthanide-based SIMs. To understand the origin of these enhanced magnetic properties a detailed characterisation of electronic structure is presented. Access to dopant electronic structure calls for atomic specific techniques, hence a combination of detailed single-crystal X-ray absorption and emission spectroscopies are applied. Together K-edge, L2,3-edge and Kβ X-ray spectroscopies probe local geometry and electronic structure, identifying iron doped lithium nitride to be a prototype, solid-state SIM, clean of stoichiometric vacancies where Fe lattice sites are geometrically equivalent. Extended X-ray absorption fine structure and angular dependent single-crystal X-ray absorption near edge spectroscopy measurements determine FeI dopant ions to be linearly coordinated, occupying a D6h symmetry pocket. The dopant engages in strong 3dπ-bonding, resulting in an exceptionally short Fe–N bond length (1.873(7) Å) and rigorous linearity. It is proposed that this structure protects dopant sites from Renner–Teller vibronic coupling and pseudo Jahn–Teller distortions, enhancing magnetic properties with respect to molecular-based linear complexes. The Fe ligand field is quantified by L2,3-edge XAS from which the energy reduction of 3dz2 due to strong 4s mixing is deduced. Quantification of magnetic anisotropy barriers in low concentration dopant sites is inhibited by many established methods, including far-infrared and neutron scattering. We deduce variable temperature L3-edge XAS can be applied to quantify the J = 7/2 magnetic anisotropy barrier, 34.80 meV (∼280 cm−1), that corresponds with Orbach relaxation via the first excited, MJ = ±5/2 doublet. The results demonstrate that dopant sites within solid-state host lattices could offer a viable alternative to rare-earth bulk magnets and high-performance SIMs, where the host matrix can be tailored to impose high symmetry and control lattice induced relaxation effects.Taking advantage of synchrotron light source methods, we present the geometric and electronic structure of iron doped in lithium nitride. 相似文献
2.
Thompson H Wasse JC Skipper NT Hayama S Bowron DT Soper AK 《Journal of the American Chemical Society》2003,125(9):2572-2581
The technique of hydrogen/deuterium isotopic substitution has been used to extract detailed information concerning the solvent structure in pure ammonia and metallic lithium-ammonia solutions. In pure ammonia we find evidence for approximately 2.0 hydrogen bonds around each central nitrogen atom, with an average N-H distance of 2.4 A. On addition of alkali metal, we observe directly significant disruption of this hydrogen bonding. At 8 mol % metal there remains only around 0.7 hydrogen bond per nitrogen atom. This value decreases to 0.0 for the saturated solution of 21 mol % metal, as all ammonia molecules have then become incorporated into the tetrahedral first solvation spheres of the lithium cations. In conjunction with a classical three-dimensional computer modeling technique, we are now able to identify a well-defined second cationic solvation shell. In this secondary shell the nitrogen atoms tend to reside above the faces and edges of the primary tetrahedral shell. Furthermore, the computer-generated models reveal that on addition of alkali metal the solvent molecules form voids of approximate radius 2.5-3.0 A. Our data therefore provide new insight into the structure of the polaronic cavities and tunnels, which have been theoretically predicted for lithium-ammonia solutions. 相似文献
3.
Todoroki K Hayama T Ijiri S Kazuta A Yoshida H Nohta H Yamaguchi M 《Journal of chromatography. A》2004,1038(1-2):113-120
6-Rhodamine B amine functions as a highly sensitive fluorescence derivatization reagent for mono- and oligosaccharides; it reacts with the reducing end of saccharides under acidic conditions. The fluorescent derivatives of five monosaccharides can be separated within 25 min by reversed-phase liquid chromatography with isocratic elution. The detection limits (S/N = 3) for mono-, di-, and oligosaccharides are 7-51, 13, and 9-35 fmol/20 microl injection, which correspond to analyte concentrations of 35-255, 65, 45-175 nM, respectively. We have applied this derivatization method successfully to the analysis of the components of oligosaccharides in glycoproteins (ribonuclease B and fetuin) following their acidic or enzymatic hydrolysis. The results from these analyses are in good agreements with the reported values established previously. 相似文献
4.
Kenichiro Todoroki Hiroki Hashimoto Kazuyuki Machida Miki Itoyama Tadashi Hayama Hideyuki Yoshida Hitoshi Nohta Manabu Nakashima Masatoshi Yamaguchi 《Journal of separation science》2013,36(2):232-238
In this study, we combined a column‐switching system with a fluorous scavenging derivatization method to develop a fully automated reagent peak‐free LC fluorescence detection protocol for the analysis of highly polar carboxylic acids. In this method, highly polar carboxylic acids were derivatized with fluorescent 1‐pyrenemethylamine in the presence of 1‐ethyl‐3‐(3‐dimethylaminopropyl)carbodiimide and 1‐hydroxy‐1H‐benzotriazole. Residual excess of the unreacted reagent was tagged with 2‐(perfluorooctyl)ethyl isocyanate and then removed selectively using a fluorous column‐switching system placed in front of an analytical reversed‐phase column. The signal of the fluorous‐tagged unreacted reagent was completely absent in the resulting chromatograms; therefore, it did not interfere with the quantification of each acid especially those eluted before 20 min. The detection limits (S/N = 3) for the examined acids were in the range from 4.0 to 22 fmol per injection. We have applied this method to comparative analysis of highly polar carboxylic acids in urine samples obtained from diabetes mellitus type‐II model mice and their control. 相似文献
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6.
Kenji Sumiya Tsunetaka Matsumoto Seiji Watatani Fumttada Hayama 《Journal of Physics and Chemistry of Solids》1979,40(12):1097-1102
Highly coercive magnetic powder was obtained by growing cobalt ferrite on the surface of γ-Fe2O3 particles in highly alkaline suspensions containing cobalt and ferrous ions in a Co/Fe molar ratio = . The mechanism of the growth and the structure of cobalt ferrite on γ-Fe2O3 were studied by X-ray diffraction and electron diffraction techniques. Results show that crystals of cobalt ferrite CoFe2O4 with a spinel type crystal structure of lattice constant 8.415 Å grew epitaxially on γ-Fe2O3. The acicular direction of the epitaxially grown Co-γ-Fe2O3 as well as γ-Fe2O3 was in the [01] direction. It was found that from the lattice constant value and the half width of X-ray diffraction peaks, the lattice constant epitaxially grown Co γ-Fe2O3 may be attributed to two kinds of crystals, viz., seed γ-Fe2O3 () which was partly reduced to Fe3O4, and surface layer CoFe2O4 (). The crystal growth in the interface between the seed crystals and the growth layer was affected by the crystal structure of the seed crystals. The lattice constant of CoFe2O4 which was located in the vicinity of the interface was almost equal to that of the seed crystals. 相似文献
7.
Furihata K Hayama A Asano DK Yanagisawa T 《The Journal of the Acoustical Society of America》2003,114(1):174-184
In this paper, an electrodynamic planar loudspeaker driven by a digital signal is experimentally discussed. The digital loudspeaker consists of 22 voice coils, 11 permanent magnets, a diaphragm with streamlined sections molded in plastic, and a suspension made of handmade Japanese paper between the diaphragm and the frame. First, the acoustic responses are affected by the arrangement of the voice coils, so an asymmetric arrangement is studied. This asymmetric arrangement is designed to obtain as flat a frequency response to an analog signal as possible. This arrangement is compared with a symmetric one and results show that the flatness of the frequency response around 1 kHz and 4 kHz is improved and that the sound reproduction band is from 40 Hz to 10 kHz. Second, to evaluate the acoustic responses to a digital signal, the digital loudspeaker is driven with a pulse code modulation signal. Results show that the digital loudspeaker can reproduce pure sound with a total harmonic distortion of less than 5% from 40 Hz to 10 kHz, exceeding this value only in a narrow frequency band near 4 kHz. This digital loudspeaker was demonstrated to have good linearity over its dynamic range of 84 dB. 相似文献
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10.
T. Hirayama A. Hayama T. Koike T. Kuninobu I. Arakawa K. Mitsuke M. Sakurai E. V. Savchenko 《Surface science》1997,390(1-3):266-271
Absolute yields of the metastable excited atoms desorbed from the surfaces of solid Ne and Ar by the creation of surface and bulk excitons have been measured using monochromated synchrotron radiation as a selective excitation source. We have obtained the absolute yields of (2.3 ± 0.7) × 10−3, (1.4 ± 0.4) × 10−3, and (7.8 ± 2.3) × 10−4 atoms/photon at the excitation of S1, B1 and S′ exciton for Ne, respectively, and 1 × 10−5 atoms/photon at S1 excitation for Ar. The probability for metastable atom desorption is found to be about 2 to 10% at the excitation of S1 exciton on the surface of solid Ne. 相似文献