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  • 1
    Electronic Resource
    Electronic Resource
    Solvent-electronic state interactions measured from the glassy to the liquid state. I. Ultrafast transient and permanent hole burning in glycerol (1992)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 96 (1992), S. 8741-8749 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Picosecond transient and permanent hole burning spectroscopies are used to study the interaction between glycerol and the electronic states of the nonpolar solute dimethyl-s-tetrazine. Variable temperature measurements from the low temperature glass into the fluid region have identified a phonon-modulated interaction in agreement with a previous hypothesis [J. Chem. Phys. 94, 5787 (1991)]. However, this mechanism alone cannot account for the magnitude of the subpicosecond line broadening seen at room temperature. A second relaxation mechanism is identified, which is connected to the structural coordinates involved in the glass transition and reaches subpicosecond relaxation times at room temperature.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.462280
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  • 2
    Electronic Resource
    Electronic Resource
    Solvent-electronic state interactions measured from the glassy to the liquid state. II. Fluorescence line narrowing spectroscopy in glycerol (1992)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 96 (1992), S. 8750-8756 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Fluorescence line narrowing spectroscopy is extended to the study of liquid state dynamics. Measurements are made on solutions of dimethyl-s-tetrazine in glycerol from room temperature to below the glass transition. The structural broadening identified in the preceding paper is related to a relaxation function by the use of a simple configuration coordinate model. This relaxation function is ∼150 times faster than the structural relaxation function measured by other experiments, showing that electronic state solvation is sensitive to a unique aspect of the structural dynamics of the liquid.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.462281
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  • 3
    Electronic Resource
    Electronic Resource
    Subpicosecond relaxation of solvent perturbations of nonpolar electronic states measured by transient hole burning (1991)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 94 (1991), S. 5787-5795 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The results of transient hole burning of the nonpolar solute dimethyl-s-tetrazine (DMST) in glycerol, glycerol triacetate, sorbitol hexaacetate, squalane, and hexane solutions are reported. Despite the high viscosity and diversity of chemical types of the solvents, the solvent-induced perturbations of the electronic states of DMST relax in less than 1 ps in all cases. This contrasts strongly with the relaxation of polar electronic states, which are typically slow in viscous solvents. A new type of solvent-interaction mechanism appears to be important. We suggest that short-range repulsions modulated by phonon-like solvent modes are responsible.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.460463
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  • 4
    Electronic Resource
    Electronic Resource
    Limitations on measuring solvent motion with ultrafast transient hole burning (1991)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 94 (1991), S. 2413-2424 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A number of limitations to hole burning in the liquid phase are identified. As spectral diffusion becomes more rapid, a point is reached where the narrowest hole width no longer measures the homogeneous linewidth. Spectral congestion of the solute is also shown to limit the fastest detectable spectral diffusion rate. An optimal pulse length is found which allows observation of the most rapid spectral diffusion. In addition, the coherence effect observed when the pulses overlap is shown to have resonances at both the excited and ground state vibrational spacings. The coherence effect greatly resembles the hole burning spectrum, but contains no dynamical information. Because of these limitations, hole burning may not be observed even when the homogeneous spectrum is well resolved and spectral diffusion is slow. Experimental confirmation is found in the hole burning spectrum of iodine in hexane, which shows no hole burning despite having a narrow homogeneous linewidth.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.459865
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  • 5
    Electronic Resource
    Electronic Resource
    Broadening of vibrational lines by attractive forces: Ultrafast Raman echo experiments in a CH3I:CDCl3 mixture (1993)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 99 (1993), S. 810-819 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A definitive demonstration of inhomogeneous vibrational line broadening in a liquid is made from Raman echo measurements of the sym-methyl stretching vibration of CH3I in a 50% mixture with CDCl3. The lifetime of the inhomogeneity is found to be 4–7 ps. The source of the inhomogeneity is identified as concentration fluctuations within the first solvation shell. The range and time scale of the interaction are consistent with the predictions of Schweizer and Chandler [J. Chem. Phys. 76, 2296 (1982)] for an attractive force interaction.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.465344
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  • 6
    Electronic Resource
    Electronic Resource
    Time-resolved nonpolar solvation dynamics in supercooled and low viscosity n-butylbenzene (1993)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 99 (1993), S. 8552-8558 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We have measured the time-resolved dynamics of the structural solvation of dimethyl-s-tetrazine in n-butylbenzene, a completely nonpolar system. A combination of transient hole burning and time-resolved fluorescence has been used to measure Stokes shift dynamics from 155–250 K, spanning a viscosity range of 6.6×105–2.5 cP. The decays have a nonexponential shape that is well described by a stretched exponential with β∼0.5. The time constants for solvation are equal to the shear relaxation times derived from viscosity and ultrasound measurements, suggesting that mechanical relaxation of the solvent is of prime importance in the structural solvation of nonpolar electronic states. A potential correlation with solute rotational dynamics is argued to be less plausible, based on the small size of the implied hydrodynamic volume.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.465578
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  • 7
    Electronic Resource
    Electronic Resource
    Reactions of vinylcyclopropane induced by multiphoton absorption of infrared radiation (1979)
    s.l. : American Chemical Society
    Journal of the American Chemical Society 101 (1979), S. 6468-6470 
    Details
    ISSN: 1520-5126
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/ja00515a071
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  • 8
    Electronic Resource
    Electronic Resource
    Probing intermolecular interactions with picosecond photon echo experiments (1987)
    s.l. : American Chemical Society
    Accounts of chemical research 20 (1987), S. 120-126 
    Details
    ISSN: 1520-4898
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/ar00135a007
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  • 9
    Electronic Resource
    Electronic Resource
    The influence of solvent dynamics on the lifetime of solute–solvent hydrogen bonds (1996)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 104 (1996), S. 7382-7394 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The lifetimes of the hydrogen bonds formed between resorufin and the solvents ethanol, ethylene glycol, and 1,3-butanediol are measured as a function of temperature. The results show that the hydrogen-bond breaking reaction is strongly influenced by the dynamics of the solvent, in violation of traditional transition-state theory. The relevant solvent dynamics are not well described by the viscosity of the solvent, but do correlate with the dielectric relaxation time. We propose a model in which the hydrogen bond initially breaks to form a poorly solvated, "dangling'' hydrogen bond, which has a high probability of geminate recombination. The product is not stabilized until the solvent hydrogen-bond structure can reorganize to incorporate the "dangling'' bond. The same reorganization determines the dielectric relaxation time. © 1996 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.471454
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  • 10
    Electronic Resource
    Electronic Resource
    Transient hole burning of s-tetrazine in propylene carbonate: A comparison of mechanical and dielectric theories of solvation (1995)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 103 (1995), S. 9146-9160 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The solvation dynamics of s-tetrazine, a nonpolar solute, in propylene carbonate, a polar solvent, have been measured in the temperature range of 190–300 K and the time range of 1.5–300 ps by transient hole burning. A detailed model of the gas-phase spectrum of s-tetrazine is used to extract purely solvent-induced effects from steady-state and ultrafast spectra. Absolute measurements of the solvation response function are extracted from these spectra and are compared to dielectric and mechanical theories of solvation. Although the theories postulate very different solute–solvent interactions mechanisms, either theory can account for the available data. © 1995 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.470026
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