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111.
Optically heterodyne-detected optical Kerr effect experiments are applied to study the orientational dynamics of the supercooled ionic organic liquids N-propyl-3-methylpyridinium bis(trifluoromethylsulfonyl)imide (PMPIm) and 1-ethyl-3-methylimidazolium tosylate (EMImTOS). The orientational dynamics are complex with relaxation involving several power law decays followed by a final exponential decay. A mode coupling theory (MCT) schematic model, the Sj?gren model, was able to reproduce the PMPIm data very successfully over a wide range of times from 1 ps to hundreds of ns for all temperatures studied. Over the temperature range from room temperature down to the critical temperature Tc of 231 K, the OHD-OKE signal of PMPIm is characterized by the intermediate power law t(-1.00+/-0.04) at short times, a von Schweidler power law t(-0.51+/-0.03) at intermediate times, and a highly temperature-dependent exponential (alpha relaxation) at long times. This form of the decay is identical to the form observed previously for a large number of organic van der Waals liquids. MCT analysis indicates that the theory can explain the experimental data very well for a range of temperatures above Tc, but as might be expected, there are some deviations from the theoretical modeling at temperatures close to Tc. For EMImTOS, the orientational dynamics were studied on the ps time scale in the deeply supercooled region near its glass transition temperature. The orientational relaxation of EMImTOS clearly displays the feature associated with the boson peak at approximately 2 ps, which is the first time domain evidence of the boson peak in ionic organic liquids. Overall, all the dynamical features observed earlier for organic van der Waals liquids using the same experimental technique are also observed for organic ionic liquids. 相似文献
112.
Massari AM McClain BL Finkelstein IJ Lee AP Reynolds HL Bren KL Fayer MD 《The journal of physical chemistry. B》2006,110(38):18803-18810
Spectrally resolved infrared stimulated vibrational echo experiments are used to measure the vibrational dephasing of a CO ligand bound to the heme cofactor in two mutated forms of the cytochrome c552 from Hydrogenobacter thermophilus. The first mutant (Ht-M61A) is characterized by a single mutation of Met61 to an Ala (Ht-M61A), while the second variant is doubly modified to have Gln64 replaced by an Asn in addition to the M61A mutation (Ht-M61A/Q64N). Multidimensional NMR experiments determined that the geometry of residue 64 in the two mutants is consistent with a non-hydrogen-bonding and hydrogen-bonding interaction with the CO ligand for Ht-M61A and Ht-M61A/Q64N, respectively. The vibrational echo experiments reveal that the shortest time scale vibrational dephasing of the CO is faster in the Ht-M61A/Q64N mutant than that in Ht-M61A. Longer time scale dynamics, measured as spectral diffusion, are unchanged by the Q64N modification. Frequency-frequency correlation functions (FFCFs) of the CO are extracted from the vibrational echo data to confirm that the dynamical difference induced by the Q64N mutation is primarily an increase in the fast (hundreds of femtoseconds) frequency fluctuations, while the slower (tens of picoseconds) dynamics are nearly unaffected. We conclude that the faster dynamics in Ht-M61A/Q64N are due to the location of Asn64, which is a hydrogen bond donor, above the heme-bound CO. A similar difference in CO ligand dynamics has been observed in the comparison of the CO derivative of myoglobin (MbCO) and its H64V variant, which is caused by the difference in axial residue interactions with the CO ligand. The results suggest a general trend for rapid ligand vibrational dynamics in the presence of a hydrogen bond donor. 相似文献
113.
Thuy-Kieu Truong Ji Hyun Park MD Asiqur Rahman Martin Urbanski Eun Sung Kim Giusy Scalia Dongseok Suh 《Current Applied Physics》2019,19(2):162-167
The use of a highly aligned carbon nanotube (CNT) sheet as a multifunctional constituent for liquid crystal (LC) displays and electro-optic LC applications is assessed. The CNT sheet can perform a dual function: one is an alignment layer for LCs, replacing the commonly used rubbed polyimide film, and the other is a transparent conductive layer, taking the place of indium tin oxide. The hydrophobic treatment improved the adhesion quality between aligned CNT bundles and the glass substrate, which helps to preserve the inherently aligned nanogroove morphology of transparent CNT sheets. The test LC display cells, comprising 4-cyano-4′-pentylbiphenyl molecules sandwiched between CNT-sheet-on-glass substrates, demonstrate the operation characteristics comparable to that of the conventional cell under temperature variation and ac electric field of 1?kHz. The results offer a possibility of deploying multifunctional CNT-sheet alignment layers in LC-based devices, especially in the future flexible display applications. 相似文献
114.
115.
The dynamics of water, confined on a nanometer length scale (1.7 to 4.0 nm) in sodium bis-(2-ethylhexyl) sulfosuccinate reverse micelles, is directly investigated using frequency resolved infrared vibrational echo experiments. The data are compared to bulk water and salt solution data. The experimentally determined frequency-frequency correlation functions show that the confined water dynamics is substantially slower than bulk water dynamics and is size dependent. The fastest dynamics (approximately 50 fs) is more similar to bulk water, while the slowest time scale dynamics is much slower than water, and, in analogy to bulk water, reflects the making and breaking of hydrogen bonds. 相似文献
116.
A nearlattice S is a meet semilattice together with the property that any two elements possessing a common upper bound have a supremum. Here the authors have introduced the notion of sectionally semicomplemented distributive nearlattices and given several characterizations of them. The skeleton SCon(S) of Con(S), the congruence lattice, consists of all those nearlattice congruences which are the pseudocomplements of members of Con(S). The relationship between skeletal congruences and kernel of skeletal congruences leads to numerous characterizations of sectionally semicomplemented distributive nearlattices and semiboolean algebras. For example we prove, for a distributive nearlattice S with 0, the following conditions are equivalent:
AMS Subject Classifications (1991): 06A12, 06A99, 06B10. 相似文献
(i) | S is sectionally semicomplemented |
(ii) | The map Θ Θ ̸ker Θ of SCon(S) onto KSCon(S) is one-to-one. |
(iii) | The map Θ Θ ̸ker Θ of SCon(S) onto KSCon(S) preserves finite joins. |
(iv) | The map Θ Θ ker ̸Θ is a lattice isomorphism of SCon(S) onto KSCon(S), whose inverse is the map J ̸ Θ(J)**. |
117.
Dynamics of five supercooled molecular liquids have been studied using optical heterodyne detected optical Kerr effect experiments. "Intermediate" time scale power law decays (approximately 2 ps to 1-10 ns) with temperature independent exponents close to -1 have been observed in all five samples from high temperature to approximately T(c), the mode-coupling theory (MCT) critical temperature. The amplitude of the intermediate power law increases with temperature as [(T-T(c))/T(c)](1/2). The results cannot be explained by standard MCT, and one possible explanation within MCT would require the higher order singularity scenario, thought to be highly improbable, to be virtually universal. 相似文献
118.
A magnetized Iron CALorimeter (ICAL) detector at the India-based neutrino observatory (INO) is used to study neutrino oscillation sensitivity using atmospheric muon neutrino source. The ICAL detector will be able to detect muon tracks and hadron showers produced by neutrino interactions with the iron target. We have performed precision measurement analysis for the atmospheric neutrino oscillation parameters with the muon neutrino events, generated by Monte Carlo NUANCE event generator. A marginalized χ2 analysis based on reconstructed neutrino energy and muon zenith angle binning scheme has been performed to determine the sensitivity for the atmospheric neutrino mixing parameters, \(\sin ^{2}\theta _{23}\) and \(| {\Delta } m^{2}_{23}|\). 相似文献
119.
H.W.H. Lee F.G. Patterson R.W. Olson D.A. Wiersma M.D. Fayer 《Chemical physics letters》1982,90(3):172-177
Optical dephasing of pentacene dimers in p-terphenyl is studied. Dimer statesR3 and R4 exhibit an exponential temperature activation of T′2 which is inconsistent with a mechanism involving scattering between delocalized dimer states. Other dephasing mechanisms are discussed. An upper limit is placed on the relaxation rate from the upper dimer state, R1, to R3 相似文献
120.
Corcelli SA Lawrence CP Asbury JB Steinel T Fayer MD Skinner JL 《The Journal of chemical physics》2004,121(18):8897-8900
We apply the combined electronic structure/molecular dynamics approach of Corcelli, Lawrence, and Skinner [J. Chem. Phys. 120, 8107 (2004)] to the fluctuating charge (SPC-FQ) model of liquid water developed by Rick, Stuart, and Berne [J. Chem. Phys. 101, 6141 (1994)]. For HOD in H(2)O the time scale for the long-time decay of the OD stretch frequency time-correlation function, which corresponds to the time scale for hydrogen-bond rearrangement in the liquid, is about 1.5 ps. This result is significantly longer than the 0.9 ps decay previously calculated for the nonpolarizable SPC/E water model. Our results for the SPC-FQ model are in better agreement with recent vibrational echo experiments. 相似文献