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81.
G.N. Greaves M.C. Wilding F. Kargl L. Hennet J.K.R. Weber Q. Vu Van P.F. McMillan 《Journal of Non》2011,357(2):435-441
By extending recent work on liquid-liquid transitions in supercooled yttria-alumina AYx liquids we draw attention to the compositional dependence of the structure factor of the high density liquid, arguing that this is sufficiently sensitive to discriminate between liquids at the level of a few %. Comparing structure factor differences between liquids of different compositions and in the same liquid AY20 between high and low temperatures straddling the transition at 1788 K between a high density liquid (HDL) and a low density liquid (LDL) enables compositional phase separation to be ruled out. It points instead to kinetic changes in polyhedral configurational order being the drivers for this polyamorphic transformation. Rotor behaviour observed in levitated liquid drops used in the high temperature experiments enables the reversibility of the LLT transition (LLT) and the associated changes in entropy and density to be identified. Evidence for critical-like behaviour in the structural relaxation time and in the fluctuation correlation length is presented. By re-examining recent work which failed to find the structural and thermal signatures for the LLT in liquid AY20 at 1788 K we present evidence for the LLT occurring instead in liquid AY15 at 1940 K, suggesting that the liquid-liquid transition temperature in AYx liquids decreases with increasing yttria content. 相似文献
82.
Rose RA Greaves SJ Abou-Chahine F Glowacki DR Oliver TA Ashfold MN Clark IP Greetham GM Towrie M Orr-Ewing AJ 《Physical chemistry chemical physics : PCCP》2012,14(30):10424-10437
Transient, broadband infra-red absorption spectroscopy with picosecond time resolution has been used to study the dynamics of reactions of CN radicals with tetrahydrofuran (THF) and d(8)-THF in liquid solutions ranging from neat THF to 0.5 M THF in chlorinated solvents (CDCl(3) and CD(2)Cl(2)). HCN and DCN products were monitored via their v(1) (C≡N stretching) and v(3) (C-H(D) stretching) vibrational absorption bands. Transient spectral features indicate formation of vibrationally excited HCN and DCN, and the onsets of absorption via the fundamental bands of HCN and DCN show short (5-15 ps) delays consistent with vibrational relaxation within the nascent reaction products. This interpretation is confirmed by non-equilibrium molecular dynamics simulations employing a newly derived analytic potential energy surface for the reaction in explicit THF solvent. The rate coefficient for reactive formation of HCN (as determined from measurements on both the 1(1)(0) and 3(1)(0) fundamental bands) decreases with increasing dilution of the THF in CDCl(3) or CD(2)Cl(2), showing pseudo-first order kinetic behaviour for THF concentrations in the range 0.5-4.5 M, and a bimolecular rate coefficient of (1.57 ± 0.12) × 10(10) M(-1) s(-1) is derived. Simultaneous analysis of time-dependent HCN 1(1)(0) and 3(1)(0) band intensities following reaction of CN with THF (3.0 M) in CD(2)Cl(2) suggests that C-H stretching mode excitation is favoured, and this deduction is supported by the computer simulations. The results extend our recent demonstration of nascent vibrational excitation of the products of bimolecular reactions in liquid solution to a different, and more strongly interacting class of organic solvents. They serve to reinforce the finding that dynamics (and thus the topology of the reactive potential energy surface) play an important role in determining the nascent product state distributions in condensed phase reactions. 相似文献
83.
Shingled recording on continuous and bit patterned media (BPM) is compared. From a recording viewpoint, continuous media have the advantage due to the lack of a need to synchronise writing with dot position. For BPM the write windows at 4 Tbit/in2 are only a couple of nm across, requiring extremely tight manufacturing tolerances. In readback, BPM have the higher SNR over a wide range of areal densities due to the absence of transition noise and erase bands. Significant increases in areal density could be achieved using BPM, provided dot uniformity could be maintained. 相似文献
84.
85.
86.
T. Krekels O. Milat G. Van Tendeloo J. Van Landuyt S. Amelinckx P.R. Slater C. Greaves 《Physica C: Superconductivity and its Applications》1993,210(3-4):439-446
YBCO-based materials containing SO4-tetrahedra centered on the Cu(1)-sites of the CuO-chain plane have been examined by means of electron diffraction and high resolution electron microscopy. An incommensurate modulation is observed and attributed to the ordering of b-oriented SO4-rich chains in the Cu(1)-S-O-layer, described in terms of an SO4-concentration wave. 相似文献
87.
Chlorinated hydrocarbons bioaccumulate in tissues and may have severe health consequences. These compounds occur individually, in small groups or as complex mixtures; examples of each category include aldrin, hexachlorocyclohexane and the polychlorinated biphenyls. Tissue extraction and purification schemes have been established, although new approaches such as supercritical fluid extraction are promising. Analyses often require the resolving power of capillary gas chromatography, in combination with the sensitivity and selectivity of electron-capture detection, electrolytic conductivity detection and mass spectrometry. Difficulties arise in quantitating chlorinated hydrocarbons in tissues, due to the number of components present and the fact that individual constituents may be reduced or enhanced in concentration in tissues, compared with the original formulation. Congener specific analysis and computer-assisted identification techniques have been applied to the problem. 相似文献
88.
L. Sajo Bohus N. Rozlosnik J. Pálfalvi C. Birattari E. Gadioli E. D. Greaves 《Acta Physica Hungarica A》1996,3(3-4):135-139
The use of the Scanning Probe Microscope for analyzing latent tracks induced in CR-39 by ions of carbon, oxygen and A~110 ions is described. 相似文献
89.
90.
Greaves SJ Rose RA Abou-Chahine F Glowacki DR Troya D Orr-Ewing AJ 《Physical chemistry chemical physics : PCCP》2011,13(23):11438-11445
We present an on-the-fly classical trajectory study of the Cl + CH(4)→ HCl + CH(3) reaction using a specific reaction parameter (SRP) AM1 Hamiltonian that was previously optimized for the Cl + ethane reaction [S. J. Greaves et al., J. Phys Chem A, 2008, 112, 9387]. The SRP-AM1 Hamiltonian is shown to be a good model for the potential energy surface of the title reaction. Calculated differential cross sections, obtained from trajectories propagated with the SRP-AM1 Hamiltonian compare favourably with experimental results for this system. Analysis of the vibrational modes of the methyl radical shows different scattering distributions for ground and vibrationally excited products. 相似文献