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31.
Schiller A Frank N Baumann T Bazin D Brown BA Brown J DeYoung PA Finck JE Gade A Hinnefeld J Howes R Lecouey JL Luther B Peters WA Scheit H Thoennessen M Tostevin JA 《Physical review letters》2007,99(11):112501
We have observed a resonance in neutron-fragment coincidence measurements that is presumably the first excited state of 23O at 2.8(1) MeV excitation energy which decays into the ground state of 22O. This interpretation is consistent with theory. The reaction mechanism supports the assignment of the observed state as the 5/2+ hole state. This assignment and the recently observed 3/2+ particle state advance the understanding of 23O. 相似文献
32.
Howes AP Vedishcheva NM Samoson A Hanna JV Smith ME Holland D Dupree R 《Physical chemistry chemical physics : PCCP》2011,13(25):11919-11928
It is shown, using the important technological glass Pyrex? as an example, that 1D and 2D (11)B Double-Rotation (DOR) NMR experiments, in combination with thermodynamic modelling, are able to provide unique structural information about complex glasses. (11)B DOR NMR has been applied to Pyrex? glass in order to remove both dipolar and quadrupolar broadening of the NMR lines, leading to high resolution spectra that allow unambiguous, accurate peak fitting to be carried out, of particular importance in the case of the 3-coordinated [BO(3)] (B3) trigonal planar environments. The data obtained are of sufficient quality that they can be used to test the distributions of borate and borosilicate superstructural units predicted by the thermodynamics-based Model of Associated Solutions. The model predicts the dominant boron-containing chemical groupings in Pyrex? glass to be those associated with B(2)O(3) and sodium tetraborate (with smaller amounts of sodium triborate, sodium diborate, sodium pentaborate, danburite and reedmergnerite). Excellent agreement is found between model and experiment provided the (11)B peaks with isotropic chemical shifts of -1.4 ppm and 0.5 ppm are assigned to B4 species from borosilicate units ([B(OSi)(4)] and [B(OSi)(3)(OB)]) and borate superstructural units (mainly triborate rings with some pentaborate and diborate) respectively. The peaks with isotropic shifts of 14 ppm and 18.1 ppm are then assigned to B3 in borate superstructural units (mainly triborate and pentaborate along with connecting B3) and boroxol rings respectively. The assignments of the DOR NMR peaks, are supported by the presence of cross-peaks in (11)B spin-diffusion DOR NMR spectra which can be used to develop a structural model in which B(2)O(3)-like regions are linked, via borate and borosilicate superstructural units, to the majority silica network. Pyrex? is thus shown to have a heterogeneous structure, with distinct molecular groupings that are far removed from a random distribution of network polyhedra with only short-range order. 相似文献
33.
In a traditional analysis of surface x-ray diffraction
data, the surface unit cell can be defined by a small set of
parameters, and fitting of experimental data is accomplished using
well-established procedures. A quantum dot (QD), however, may contain
as many as 20,000 atoms, so a different approach to data analysis is
required. A method for modelling a quantum dot and relaxing the
structure by minimising the Keating energy is presented, and the
simulation of x-ray scattering from such models is described. A method
is then developed for simulating the alloying of InAs and GaAs inside
the QDs using intermediate Keating parameters. This removes the need
to relax and average multiple models with randomly distributed atoms,
which would increase the computation time significantly. 相似文献
34.
Separation of isotropic chemical and second-order quadrupolar shifts by multiple-quantum double rotation NMR 总被引:1,自引:1,他引:0
Ivan Hung Alan Wong Andy P. Howes Tiit Anupld Ago Samoson Mark E. Smith Diane Holland Steven P. Brown Ray Dupree 《Journal of magnetic resonance (San Diego, Calif. : 1997)》2009,197(2):229-236
Using a two-dimensional multiple-quantum (MQ) double rotation (DOR) experiment the contributions of the chemical shift and quadrupolar interaction to isotropic resonance shifts can be completely separated. Spectra were acquired using a three-pulse triple-quantum z-filtered pulse sequence and subsequently sheared along both the ν1 and ν2 dimensions. The application of this method is demonstrated for both crystalline (RbNO3) and amorphous samples (vitreous B2O3). The existence of the two rubidium isotopes (85Rb and 87Rb) allows comparison of results for two nuclei with different spins (I = 3/2 and 5/2), as well as different dipole and quadrupole moments in a single chemical compound. Being only limited by homogeneous line broadening and sample crystallinity, linewidths of approximately 0.1 and 0.2 ppm can be measured for 87Rb in the quadrupolar and chemical shift dimensions, enabling highly accurate determination of the isotropic chemical shift and the quadrupolar product, PQ. For vitreous B2O3, the use of MQDOR allows the chemical shift and electric field gradient distributions to be directly determined—information that is difficult to obtain otherwise due to the presence of second-order quadrupolar broadening. 相似文献
35.
Howes GG Dorland W Cowley SC Hammett GW Quataert E Schekochihin AA Tatsuno T 《Physical review letters》2008,100(6):065004
This Letter presents the first ab initio, fully electromagnetic, kinetic simulations of magnetized turbulence in a homogeneous, weakly collisional plasma at the scale of the ion Larmor radius (ion gyroscale). Magnetic- and electric-field energy spectra show a break at the ion gyroscale; the spectral slopes are consistent with scaling predictions for critically balanced turbulence of Alfvén waves above the ion gyroscale (spectral index -5/3) and of kinetic Alfvén waves below the ion gyroscale (spectral indices of -7/3 for magnetic and -1/3 for electric fluctuations). This behavior is also qualitatively consistent with in situ measurements of turbulence in the solar wind. Our findings support the hypothesis that the frequencies of turbulent fluctuations in the solar wind remain well below the ion cyclotron frequency both above and below the ion gyroscale. 相似文献
36.
37.
Trade and historic oils from 'sandalwoods', labelled as Amyris balsamifera, Eremophila mitchelli, Fusanus acuminatus (= Santalum acuminatum), Santalum album, S. austrocaledonicum, S. latifolium, S. spicatum and S. yasi, were assessed using gas chromatography-mass spectrometry (GC-MS). Using GC-MS, none of the oils assessed complied with the internationally recognised standard of a 90% santalol content, and only about half of the trade sandalwood oils met with recent International Organisation for Standardisation standards. The majority of trade oils, reportedly from S. album, contained approximately 50-70% santalols (Z-alpha and Z-beta). Thus, the internationally recognised specification (90% santalols) for S. album requires re-evaluation by more efficient analysis methods. In view of the issues associated with the quality of sandalwood oils being traded, specifications of > or = 43% Z-alpha-santalol and > or = 18% Z-beta-santalol for S. album oil estimated by GC-MS are suggested. GC-MS are recommended as it assists with authentication and quality control issues associated with sandalwood oils. 相似文献
38.
Measurements of solar ultraviolet radiation (<320 nm) have been made with polysulphone film at a temperate and a tropical site and compared mean monthly values of the fraction of ultraviolet in solar radiation are calculated which allow an estimate of ultraviolet dose to be made from a knowledge of total solar radiation.While the data demonstrate the marked effect of sun elevation on the ultraviolet fraction of solar radiation they also indicate the effect of seasonal variation in the thickness of the ozone layer above the temperate site.It is also shown that whereas sunlight makes by far the major contribution to total solar radiation, skylight is of prime importance as regards ultraviolet radiation. 相似文献
39.
Agbodjan AA Cooley BE Copley RC Corfield JA Flanagan RC Glover BN Guidetti R Haigh D Howes PD Jackson MM Matsuoka RT Medhurst KJ Millar A Sharp MJ Slater MJ Toczko JF Xie S 《The Journal of organic chemistry》2008,73(8):3094-3102
A practical asymmetric synthesis of a highly substituted N-acylpyrrolidine on multi-kilogram scale is described. The key step in the construction of the three stereocenters is a [3+2] cycloaddition of methyl acrylate and an imino ester prepared from l-leucine t-butyl ester hydrochloride and 2-thiazolecarboxaldehyde. The cycloaddition features novel asymmetric catalysis via a complex of silver acetate and a cinchona alkaloid, particularly hydroquinine, with complete diastereomeric control and up to 87% enantiomeric control. The alkaloid serves as a ligand as well as a base for the formation of the azomethine ylide or 1,3-dipole. Experiments have shown that the hydroxyl group of hydroquinine is a critical element for the enantioselectivities observed. The cycloaddition methodology is also applicable to methylvinyl ketone, providing access to either alpha- or beta-epimers of 4-acetylpyrrolidine depending on the reaction conditions utilized. The synthesis also highlights an efficient N-acylation, selective O- versus N-methylation, and a unique ester reduction with NaBH4-MeOH catalyzed by NaB(OAc)3H that not only achieves excellent chemoselectivity but also avoids formation of the undesired but thermodynamically favored epimer. The highly functionalized target is synthesized in seven linear steps from l-leucine t-butyl ester hydrochloride with all three isolated intermediates being highly crystalline. 相似文献
40.
Wong A Howes AP Pike KJ Lemaître V Watts A Anupõld T Past J Samoson A Dupree R Smith ME 《Journal of the American Chemical Society》2006,128(24):7744-7745
A solid-state 17O NMR 1H-decoupled double angle rotation (DOR) study of monosodium l-glutamate monohydrate (l-MSG) is reported. It is shown that all eight inequivalent sites can be resolved with DOR line widths ( approximately 65 Hz) approximately 120 times narrower than those in the MAS spectrum. The lines are tentatively assigned on the basis of their behavior under proton decoupling and the isotropic chemical shift and the quadrupole interaction parameter for each extracted by a combination of DOR and 3Q MAS at variable magnetic fields. With a shift range of approximately 45 ppm for these similar oxygen sites and spectral resolution under DOR comparable to that for spin-1/2 nuclei, solid-state 17O NMR should have tremendous potential in the study of biomolecules. 相似文献