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  • 1
    Electronic Resource
    Electronic Resource
    Direct observation of energy transfer in a photosynthetic membrane: chlorophyll b to chlorophyll a transfer in LHC (1989)
    s.l. : American Chemical Society
    The @journal of physical chemistry 〈Washington, DC〉 93 (1989), S. 8271-8275 
    Details
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/j100363a001
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  • 2
    Electronic Resource
    Electronic Resource
    The dynamics of polar solvation: Inhomogeneous dielectric continuum models (1988)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 89 (1988), S. 3519-3534 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The influence of an inhomogeneous dielectric response on the dynamics of solvation of ions and dipoles is investigated. Solvent models considered include discrete shell models as well as models in which the solvent dielectric constant varies continuously as a function of distance from a spherical solute. The effect of such dielectric inhomogeneity is to introduce additional, slower relaxation times into the solvation response when compared to the homogeneous case. For all models studied, the deviation of the average relaxation time from that predicted for a homogeneous continuum solvent increases as the dielectric constant and the length parameter, which specifies the rapidity of approach to bulk behavior, increase. For a given solvent model the solvation response to a change in a point dipole moment is slower than the response to a charge jump. The continuum results are compared to a recent molecular model based on the mean spherical approximation. The comparison suggests that deviations from homogeneous continuum behavior in the molecular model can be accounted for by inhomogeneity of the solvent dielectric constant extending only over the first solvation shell. Predictions of inhomogeneous continuum models are also compared to experimental data. Both the observed dependence of average relaxation time on dielectric constant, and the detailed time dependence of the relaxation in high dielectric constant solvents can be rationalized on the basis of such models.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.454923
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  • 3
    Electronic Resource
    Electronic Resource
    Femtosecond dynamics of hydrogen-bonding solvents. Formamide and N-methylformamide in acetonitrile, DMF, and water (1993)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 99 (1993), S. 113-125 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We have used optical-heterodyne-detected optical Kerr effect (OHD-OKE) spectroscopy to measure the ultrafast dynamical profile of the amide series formamide (FA), N-methylformamide (NMF), and N,N-dimethylformamide (DMF). We have studied the concentration dependence of binary solutions of FA and NMF using DMF, water, and acetonitrile as cosolvents. Our results show an underdamped librational motion with a period of about 100 cm−1 in both FA and NMF, which also occurs in the binary solutions. The significance of these results for ultrafast chemical reactions in solution is discussed.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.465790
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  • 4
    Electronic Resource
    Electronic Resource
    Fast responses from "slowly relaxing'' liquids: A comparative study of the femtosecond dynamics of triacetin, ethylene glycol, and water (1993)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 99 (1993), S. 7289-7299 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We have measured the ultrafast solvent relaxation of liquid ethylene glycol, triacetin, and water by means of femtosecond polarization spectroscopy, using optical-heterodyne-detected Raman-induced Kerr-effect spectroscopy. In the viscous liquids triacetin and ethylene glycol, femtosecond relaxation processes were resolved. Not surprisingly, the femtosecond nonlinear optical response of ethylene glycol is quite similar to that of water. Using the theory of Maroncelli, Kumar, and Papazyan, we transform the pure-nuclear solvent response into a dipolar-solvation correlation function for comparison with ultrafast electron-transfer reaction rates.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.465710
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  • 5
    Electronic Resource
    Electronic Resource
    Reductive quenching of the emission of trans-dioxo(1,4,8,11-tetramethyl-1,4,8,11-tetraazacyclotetradecane)osmium(VI) in water (1993)
    s.l. : American Chemical Society
    Inorganic chemistry 32 (1993), S. 4200-4208 
    Details
    ISSN: 1520-510X
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/ic00072a009
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  • 6
    Electronic Resource
    Electronic Resource
    Deuterium Isotope Effects on the Ultrafast Solvent Relaxation of Formamide and N,N-Dimethylformamide (1994)
    s.l. : American Chemical Society
    The @journal of physical chemistry 〈Washington, DC〉 98 (1994), S. 9712-9722 
    Details
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/j100090a003
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  • 7
    Electronic Resource
    Electronic Resource
    Subpicosecond resolution studies of solvation dynamics in polar aprotic and alcohol solvents (1987)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 86 (1987), S. 1090-1097 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Subpicosecond resolution measurements of the kinetics of dipolar solvation have been made. The time resolved Stokes shift of a dye molecule, LDS-750 was measured using the fluorescence upconversion technique in the solvents acetonitrile, DMSO, nitrobenzene, methanol, and n-butanol. The solvation dynamics in both aprotic and alcohol solvents occur on a time scale roughly given by the longitudinal relaxation time as predicted by simple continuum theories. The relaxation in nitrobenzene and butanol is nonexponential and the relaxation in methanol is significantly faster than the calculated time. These deviations from simple theory are discussed in the context of (i) the significance of high frequency dispersions in the dielectric response, (ii) translational contributions to the solvent relaxation, and (iii) molecular aspects of the solvation not accounted in the continuum description.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.452249
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  • 8
    Electronic Resource
    Electronic Resource
    Solvation in highly nonideal solutions: A study of aqueous 1-propanol using the coumarin 153 probe (2000)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 112 (2000), S. 2367-2376 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We have investigated the anomalous behavior of aqueous 1-propanol binary solutions using a typical fluorescence probe molecule, coumarin 153. We present data on the fluorescence lifetimes, fluorescence anisotropies, and solvent reorganization dynamics, as well as the steady-state absorption and emission spectra of coumarin 153 in the binary solutions. The rotational diffusion and solvation time constants depend strongly on the content of 1-propanol, especially at low 1-propanol mole fractions. Spectroscopic results presented here are consistent with prior light scattering [G. H. Großmann and K. H. Ebert, Ber. Bunsenges. Phys. Chem. 85, 1026 (1981)], small angle x-ray scattering [H. Hayashi, K. Nishikawa, and T. Iijima, J. Phys. Chem. 94, 8334 (1990)], and dielectric relaxation [S. Mashimo, T. Umehara, and H. Redlin, J. Chem. Phys. 95, 6257 (1991)] data. The anomalous dynamics features likely arise from the effect of the preferential solvation due to the 1-propanol clustering. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.480803
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  • 9
    Electronic Resource
    Electronic Resource
    Aqueous dimethyl sulfoxide solutions: Inter- and intra-molecular dynamics (2002)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 116 (2002), S. 4643-4654 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The inter- and intra-molecular dynamics of aqueous dimethyl sulfoxide (DMSO) solutions have been measured using optical heterodyne-detected Raman-induced Kerr effect spectroscopy. Solutions were studied over the entire range of composition at 294 K. The Kerr transients characterize both the underdamped inter- and intra-molecular vibrational motions, as well as the overdamped, diffusive orientational motions. The longer diffusive relaxation time constant τ2 is assigned to DMSO reorientation, and varies strongly with mole fraction of DMSO. The shorter time constant τ1 is assigned to water reorientation, and the value of 1.0 ps is nearly invariant across the range of solution composition. The solutions deviate substantially from hydrodynamic scaling behavior, since the ratio of DMSO reorientation time constant normalized by shear viscosity τ2/η is not a linear function of mole fraction. The peak frequencies for three of five low frequency intramolecular vibrations decrease with increasing water content. Both anisotropic and isotropic Kerr transients are recorded. The isotropic Kerr transient is dominated by the partially depolarized ν10 symmetric C–S–C stretching vibration at 670 cm−1. Electronic structure calculations for isolated DMSO, perdeuterated DMSO (d6-DMSO), and water are carried out using semi-empirical (PM3), density functional (B3LYP), and MP2 methods. Basis sets up to 6-311++G(d,p) are used and vibrational frequencies are calculated within the harmonic approximation. An unusual hemispherical shape is obtained for the electrostatic potential (ESP) about the DMSO oxygen. This hemispherical ESP was consistently observed for all levels of electronic structure theory and all basis sets that were used. Calculated polarizabilities permit us to estimate the anisotropic Kerr signal for an isolated DMSO molecule to be 79 times greater than for an isolated water molecule. © 2002 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.1449864
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