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151.
152.
We present a direct calculation by molecular-dynamics computer simulation of the crystal/melt interfacial free energy gamma for a system of hard spheres of diameter sigma. The calculation is performed by thermodynamic integration along a reversible path defined by cleaving, using specially constructed movable hard-sphere walls, separate bulk crystal, and fluid systems, which are then merged to form an interface. We find the interfacial free energy to be slightly anisotropic with gamma = 0.62+/-0.01, 0.64+/-0.01, and 0. 58+/-0.01k(B)T/sigma(2) for the (100), (110), and (111) fcc crystal/fluid interfaces, respectively. These values are consistent with earlier density functional calculations and recent experiments. 相似文献
153.
van Weperen I Armstrong BD Laird EA Medford J Marcus CM Hanson MP Gossard AC 《Physical review letters》2011,107(3):030506
We report coherent operation of a singlet-triplet qubit controlled by the spatial arrangement of two confined electrons in an adjacent double quantum dot that is electrostatically coupled to the qubit. This four-dot system is the specific device geometry needed for two-qubit operations of a two-electron spin qubit. We extract the strength of the capacitive coupling between qubit and adjacent double quantum dot and show that the present geometry allows fast conditional gate operation, opening pathways toward implementation of a universal set of gates for singlet-triplet spin qubits. 相似文献
154.
Understanding Electrogenerated Chemiluminescence Efficiency in Blue‐Shifted Iridium(III)‐Complexes: An Experimental and Theoretical Study
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Dr. Gregory J. Barbante Dr. Egan H. Doeven Emily Kerr Timothy U. Connell Dr. Paul S. Donnelly Prof. Jonathan M. White Thais Lópes Sarah Laird Dr. David J. D. Wilson Dr. Peter J. Barnard Dr. Conor F. Hogan Prof. Paul S. Francis 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(12):3322-3332
Compared to tris(2‐phenylpyridine)iridium(III) ([Ir(ppy)3]), iridium(III) complexes containing difluorophenylpyridine (df‐ppy) and/or an ancillary triazolylpyridine ligand [3‐phenyl‐1,2,4‐triazol‐5‐ylpyridinato (ptp) or 1‐benzyl‐1,2,3‐triazol‐4‐ylpyridine (ptb)] exhibit considerable hypsochromic shifts (ca. 25–60 nm), due to the significant stabilising effect of these ligands on the HOMO energy, whilst having relatively little effect on the LUMO. Despite their lower photoluminescence quantum yields compared with [Ir(ppy)3] and [Ir(df‐ppy)3], the iridium(III) complexes containing triazolylpyridine ligands gave greater electrogenerated chemiluminescence (ECL) intensities (using tri‐n‐propylamine (TPA) as a co‐reactant), which can in part be ascribed to the more energetically favourable reactions of the oxidised complex (M+) with both TPA and its neutral radical oxidation product. The calculated iridium(III) complex LUMO energies were shown to be a good predictor of the corresponding M+ LUMO energies, and both HOMO and LUMO levels are related to ECL efficiency. The theoretical and experimental data together show that the best strategy for the design of efficient new blue‐shifted electrochemiluminophores is to aim to stabilise the HOMO, while only moderately stabilising the LUMO, thereby increasing the energy gap but ensuring favourable thermodynamics and kinetics for the ECL reaction. Of the iridium(III) complexes examined, [Ir(df‐ppy)2(ptb)]+ was most attractive as a blue‐emitter for ECL detection, featuring a large hypsochromic shift (λmax=454 and 484 nm), superior co‐reactant ECL intensity than the archetypal homoleptic green and blue emitters: [Ir(ppy)3] and [Ir(df‐ppy)3] (by over 16‐fold and threefold, respectively), and greater solubility in polar solvents. 相似文献
155.
Matei C Buchmann L Hannes WR Hutcheon DA Ruiz C Brune CR Caggiano J Chen AA D'Auria J Laird A Lamey M Li ZH Liu WP Olin A Ottewell D Pearson J Ruprecht G Trinczek M Vockenhuber C Wrede C 《Physical review letters》2006,97(24):242503
Radiative alpha-particle capture into the first excited, J(pi)=0+ state of 16O at 6.049 MeV excitation energy has rarely been discussed as contributing to the 12C(alpha,gamma)16O reaction cross section due to experimental difficulties in observing this transition. We report here measurements of this radiative capture in 12C(alpha,gamma)16O for center-of-mass energies of E=2.22 MeV to 5.42 MeV at the DRAGON recoil separator. To determine cross sections, the acceptance of the recoil separator has been simulated in GEANT as well as measured directly. The transition strength between resonances has been identified in R-matrix fits as resulting both from E2 contributions as well as E1 radiative capture. Details of the extrapolation of the total cross section to low energies are then discussed [S6.0(300)=25(-15)(+16) keV b] showing that this transition is likely the most important cascade contribution for 12C(alpha,gamma)16O. 相似文献
156.
Laird EA Petta JR Johnson AC Marcus CM Yacoby A Hanson MP Gossard AC 《Physical review letters》2006,97(5):056801
We measure singlet-triplet dephasing in a two-electron double quantum dot in the presence of an exchange interaction which can be electrically tuned from much smaller to much larger than the hyperfine energy. Saturation of dephasing and damped oscillations of the spin correlator as a function of time are observed when the two interaction strengths are comparable. Both features of the data are compared with predictions from a quasistatic model of the hyperfine field. 相似文献
157.
An experimental study into calcium phosphate (CP) nucleation and growth on cholesterol and cholestanol surfaces from a supersaturated simulated body fluid (SBF) is presented with the overall aim of gaining some fundamental insights into the pathological calcifications associated with atherosclerosis. Soaking of pressed cholesterol disks at physiological temperature in SBF solutions was found to lead to CP nucleation and growth if the disks were surface roughened and if an SBF with concentrations of the calcium and hydrogen phosphate ions at 2.25x physiological concentrations was used. The CP phase deposited was shown via SEM micrographs to possess a florette type morphology akin to that observed in earlier reported studies. The use of recrystallised cholesterol and cholestanol microcrystals as substrates for soaking in SBF facilitated the observation of CP deposition. In general, cholesterol recrystallised from polar solvents like 95% ethanol as a cholesterol monohydrate phase which was a better substrate for CP growth than cholesterol recrystallised from more non-polar solvents (e.g., benzene) which produced anhydrous cholesterol phases. CP was also observed to form on recrystallised cholestanol microcrystals, a molecule closely related to cholesterol. Inductively coupled plasma optical emission spectrometry (ICP-OES) data gave confirmation that Ca:P mole ratios of the grown CP were 1.3-1.5 suggesting a mixed phase of octacalcium phosphate (OCP) and Ca-deficient HAp and that the CP coating grows (with time of soaking) on the substrates after nucleation in the SBF growth medium. Infrared (IR) spectra of the extracted coatings from the cholesterol substrates confirmed that the CP phase deposited is a semi crystalline HAp with either carbonate substituted into its structure or else co-deposited as calcium carbonate. Soaking experiments involving modified cholesterol substrates in which the OH group in the molecule was replaced with the oleiyl or phosphonate group showed no CP nucleation and growth. This observation illustrates the importance of the known epitaxial relationship between cholesterol and HAp (which theoretically predicts favourable deposition of one phase upon the other) and the consequences of its destruction (by chemical modification of the cholesterol). In the case of the phosphorylated cholesterol, failure of this substrate to nucleate CP phases may have also been caused by the reduction in concentration of free solution Ca2+ in the SBF medium by complexation with the phosphonate groups on the phosphorylated cholesterol. This would have reduced the ion product of Ca2+ and inorganic phosphate and lowered the degree of supersaturation in the SBF medium. 相似文献