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  • 1
    Electronic Resource
    Electronic Resource
    Femtosecond real-time probing of reactions. IV. The reactions of alkali halides (1989)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 91 (1989), S. 7415-7436 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The photodissociation dynamics of some alkali halides are explored via the method of femtosecond transition-state spectroscopy (FTS). The alkali halide dissociation reaction is influenced by the interaction between the covalent and the ground state ionic potential energy surfaces (PES), which cross at a certain internuclear separation. Depending upon the adiabaticity of the PES, the dissociating fragments may be trapped in a well formed by the avoided crossing of these surfaces. Here, we detail the FTS results of this class of reactions, with particular focus on the reaction of sodium iodide: NaI*→[Na---I]°* →Na+I. As in our first report [T. S. Rose, M. J. Rosker, and A. H. Zewail, J. Chem. Phys. 88, 6672 (1988)], we observe the dynamical motion of the wave packet along the reaction coordinate and the crossing between the covalent and ionic surfaces. The studies presented here characterize the effects of various experimental parameters, including pump and probe wavelengths, on the dynamics of the dissociation and its detection. Comparisons of the results with classical and quantum mechanical calculations are also presented.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.457266
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  • 2
    Electronic Resource
    Electronic Resource
    Femtosecond real-time probing of reactions. II. The dissociation reaction of ICN (1988)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 89 (1988), S. 6128-6140 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Experimental results obtained for the dissociation reaction ICN*→[I⋅⋅⋅CN]
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.455428
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    Paper (German National Licenses)
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  • 3
    Electronic Resource
    Electronic Resource
    Femtosecond real-time probing of reactions. I. The technique (1988)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 89 (1988), S. 6113-6127 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: When a chemical bond is broken in a direct dissociation reaction, the process is so rapid that it has generally been considered instantaneous and therefore unobservable. But the fragments formed interact with one another for times on the order of 10−13 s after the photon has been absorbed. On this time scale the system passes through intermediate transition configurations; the totality of such configurations have been, in the recent literature, designated as "transition states.'' Femtosecond transition-state spectroscopy (FTS) is a real-time technique for probing chemical reactions. It allows the direct observation of a molecule in the process of falling apart or in the process of formation. In this paper, the first in a series on femtosecond real-time probing of reactions, we examine the technique in detail. The concept of FTS is explored, and the interrelationship between the dynamics of chemical reactions and molecular potential energy surfaces is considered. The experimental method, which requires the generation of spectrally tunable femtosecond optical pulses, is detailed. Illustrative results from FTS experiments for several elementary reactions are presented, and we describe methods for relating these results to the potential energy surface(s).
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.455427
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  • 4
    Electronic Resource
    Electronic Resource
    Time-resolved degenerate four-wave mixing studies of solid-state poly(p-phenylene) oligomers (1994)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 100 (1994), S. 3325-3333 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We have measured χ(3) for a series of solid-state samples of polyphenylene oligomers, (Ph)n, where n=4–8 is the number of phenyl ring units, using optical pulses of 140 fs duration and 650 nm wavelength. A degenerate four-wave mixing (DFWM) signal was only observable for n≥6, and thereafter the measured values of χ(3) increased monotonically with n. Measurements of the linear absorption are also reported. Although the DFWM measurements were performed at wavelengths far from resonance, the figure of merit χ(3)/α was essentially flat beyond n≥6. In contrast to previous studies of oligomers in solution, the principal nonlinear responses were instantaneous within the 140 fs temporal resolution.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.466424
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    Paper (German National Licenses)
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  • 5
    Electronic Resource
    Electronic Resource
    Real-time femtosecond probing of "transition states'' in chemical reactions (1987)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 87 (1987), S. 2395-2397 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.453122
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    Paper (German National Licenses)
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  • 6
    Electronic Resource
    Electronic Resource
    Femtosecond real-time observation of wave packet oscillations (resonance) in dissociation reactions (1988)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 88 (1988), S. 6672-6673 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.454408
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    Paper (German National Licenses)
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