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排序方式: 共有85条查询结果,搜索用时 31 毫秒
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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
3.
We have measured the two-color double resonance enhanced four-photon ionization and the fluorescence de-enhanced spectra of nitric oxide by using two tunable pulsed dye lasers. The spectra show clear structure in the third-photon (8.2 eV) region. Also discussed is the multiphoton ionization mechanism in the resonance state. 相似文献
4.
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
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S. Urabe K. Hayasaka M. Watanabe H. Imajo R. Ohmukai R. Hayashi 《Applied physics. B, Lasers and optics》1993,57(5):367-371
This paper describes trapping and laser cooling of a Ca+ ion in an rf quadrupole ion trap. A single Ca+ ion is laser cooled to below 130 mK and quantum jumps are observed by exciting the ion into the metastable D
5/2 state via the P
3/2 state. The lifetime of the metastable D
5/2 state is estimated from the distribution of the dark periods of the quantum-jump signal. Collision-induced jumps between the metastable D
3/2 state and the D
5/2 state in a background gas are also directly observed. 相似文献
7.
T. Matsui A.S.-C. Cheung K. Yoshino W.H. Parkinson J.E. Murray T. Imajo 《Journal of Molecular Spectroscopy》2003,219(1):45-57
The photoabsorption spectrum of the O2 Schumann-Runge bands was measured with resolution comparable to the Doppler widths by using the VUV Fourier transform spectrometer from Imperial College, London, combined with synchrotron radiation as a continuum light source at the Photon Factory, KEK, Japan. The analysis of the (12,0)-(17,0) bands of the Schumann-Runge system provides accurate rotational line positions as well as the line intensities from 185 to 175 nm. Molecular constants of the levels of the state have been determined. The (v′,0) band oscillator strengths were determined as 2.38, 2.62, 2.70, 2.66, 2.40, and 2.12×10−5 for the bands from v′=12 to 17, respectively. 相似文献
8.
Koji Takagi Takato Isomura Yohei Ito Masanori Sakaida Shusaku Nagano Takahiro Seki 《Journal of polymer science. Part A, Polymer chemistry》2011,49(23):4993-5000
The Suzuki (for O1 – O3 ) and Stille (for O4 ) coupling polymerization of 2‐(phenylazo)imidazole bearing the benzyl protecting group at the 1‐position gave conjugated oligomers. The transformation from the neutral imidazole in the conjugated oligomer O2 , consisted of the alternating 2,5‐didecyl‐1,4‐phenylene unit, to the cationic imidazolium salt O2S was performed. Depending on the chemical structure of coupling partners, the absorption maximum of conjugated oligomers showed red shift or blue shift from that of the model compound M with the benzene ring at the 4,5‐positions. The absorption maximum wavelength of the cationic conjugated oligomer O2S showed a blue shift from that of the neutral conjugated oligomer O2 . The trans‐to‐cis photoisomerization of the azoimidazole unit in conjugated oligomers was observed by irradiating the light at 436 nm, and the conversion degree to the cis structure had a rough correlation with the maximum absorption wavelength of materials. The trans‐to‐cis photoisomerization in the film state was sluggish. On the other hand, the cis‐to‐trans thermal isomerization of the azoimidazole unit was confirmed and the absorbance returned to the initial state before the photoisomerization. The trans‐to‐cis photoisomerization of the cationic conjugated oligomer O2S required large energy, and the prolonged light irradiation might decompose the azoimidazole unit. © 2011 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2011. 相似文献
9.
Hirokazu Sato Shusaku Hamada Roberto M. Sertkawa Tatsuya Nishimura Takashi Usui Hideo Sekino 《高压研究》2013,33(1-6):403-413
Abstract Continuous flames have been observed in Supercritical water oxidation (scWO) of isopropyl alcohol (IPA), using a vertical continuous reactor with sapphire windows and a mixing nozzle. Two types of continuous flame were confirmed: the one was long pale blue colored and the other was red short cone shaped, changing blue to red at around air ratio 2.0. The flame was strongly influenced by IPA concentration, air ratio and design of the mixing nozzle. Results for decomposition of PA are presented for IPA concentrations ranging from 600 up to 28260 ppm as TOC and initial reactor temperatures, were mostly around 490°C, at 25 MPa. Decomposition rate at steady state was over 99.9%. Experimentally measured CO2 and O2 concentrations at the flue gas were in good agreement with theoretically calculated values. Even for low air ratio as 1.1, high decomposition rate without CO, NO, NO2 was achieved. 相似文献
10.
T. Ino Y. ArimotoT. Yoshioka K. MishimaK. Taketani S. MutoH.M. Shimizu H. KiraY. Sakaguchi T. OkuK. Sakai T. ShinoharaJ. Suzuki H. OtonoH. Oide S. YamashitaS. Imajo H. FunahashiM. Yamada Y. IwashitaM. Kitaguchi M. HinoZ. Suzuki T. SanukiT. Seki K. HirotaK. Ikeda H. SatoY. Otake H. OhmoriT. Morishima T. Shima 《Physica B: Condensed Matter》2011,406(12):2424-2428
We measured the neutron beam polarization of the BL05/NOP (Neutron Optics and Physics) beamline at J-PARC with an accuracy of less than 10−3 using polarized 3He gas as a neutron spin analyzer. Precise polarimetry of the neutron beam is necessary to understand the beamline optics as well as for the asymmetry measurements of the neutron beta decay, which are planned in this beamline. 相似文献