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  • 1
    Electronic Resource
    Electronic Resource
    Dynamical theory of statistical unimolecular decay (1986)
    s.l. : American Chemical Society
    The @journal of physical chemistry 〈Washington, DC〉 90 (1986), S. 3509-3516 
    Details
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/j100407a012
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  • 2
    Electronic Resource
    Electronic Resource
    Creation and dynamics of molecular states prepared with coherent vs partially coherent pulsed light (1991)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 94 (1991), S. 5833-5843 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The mixed state of an isolated molecule, which results from one-photon absorption using a pulsed laser of arbitrary coherence, is obtained using a simple model for a partially coherent laser source. The relative effect of the pulse time τ, source coherence time τcoh, and field correlation time τc on the prepared state and on its subsequent molecular dynamics are described. Numerical computations on several properties are provided and support obtained for the analytical result showing that under certain circumstances the falloff of the survival probability of the created molecular state depends primarily on the pulse time τ.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.460467
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  • 3
    Electronic Resource
    Electronic Resource
    Intramolecular vibrational redistribution in alkylbenzenes. I. Normal modes and their energy distribution (1991)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 94 (1991), S. 2848-2861 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Normal modes for the ground and first excited singlet state are computed for ethylbenzene, pentylbenzene, and hexylbenzene and are assigned in terms of zero-order mode descriptors. The energy distribution, i.e., the partitioning of energy between the ring and chain, is computed for the normal modes and the concept of "system modes,'' i.e., modes localized on the ring, is examined. Several of the basic assumptions made in traditional interpretations of intramolecular vibrational redistribution in molecules with a "ring+tail'' structure are examined in light of the computed normal mode characteristics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.459807
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  • 4
    Electronic Resource
    Electronic Resource
    Two-pulse coherent control of electronic states in the photodissociation of IBr: Theory and proposed experiment (1990)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 93 (1990), S. 2493-2498 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: It is shown how the principles of coherent control can be applied to a pulsed experiment aimed at controlling curve-crossing processes. A realistic computational study (incorporating the ground, A, B, and Y electronic states of IBr) of control of atomic states produced in the photodissociation of IBr is presented. The suggested scheme, which consists of applying an excitation pulse followed by a dissociation pulse, is theoretically shown to yield essentially total control over the Br*/Br atomic branching ratio. It is shown that the only external parameters that need to be varied are the central frequency of the excitation pulse and the time delay between the two pulses. A brief description of a proposed experiment is provided.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.459031
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  • 5
    Electronic Resource
    Electronic Resource
    Laser control of unimolecular decay yields in the presence of collisions (1989)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 90 (1989), S. 6179-6186 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We show that coherent light can be used to control the relative product yield in unimolecular photodissociation, even in the presence of collisions. That is, coherence contributions to the photodissociation, which are responsible for control over the reaction, are sufficiently robust to survive inhomogeneous broadening effects over a substantial temperature range. A number of experimental implementations for control in the presence of collisions are proposed.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.456334
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  • 6
    Electronic Resource
    Electronic Resource
    Total N-channel control in the weak field domain (1992)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 97 (1992), S. 6259-6261 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The existence of a complete solution to the problem of controlling molecular photodissociation using weak laser fields is explored from the perspective of the theory of coherent radiative control. Specifically, the usual two-path coherent radiative control theory is extended to the N-path case and the magnitudes and phases of a series of light frequencies which generate a particular distribution of product photofragments are obtained. Results show that complete control over the distribution of product yields is possible if (a) the continuum absorption spectrum is composed of a series of sufficiently narrow resonances, and (b) that the photodissociation process is nonfactorizeable, i.e., it cannot be broken up to the excitation of a "bright'' state and dissociation to a set of "dark'' states.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.463687
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  • 7
    Electronic Resource
    Electronic Resource
    Controlled photon induced symmetry breaking: Chiral molecular products from achiral precursors (1991)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 95 (1991), S. 8658-8661 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.461247
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  • 8
    Electronic Resource
    Electronic Resource
    Intramolecular vibrational redistribution in alkylbenzenes. II. Spectroscopy and dynamics (1991)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 94 (1991), S. 2862-2872 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Dispersed fluorescence spectra from 00, 6b1, and 121 excitation of ethylbenzene, pentylbenzene, and hexylbenzene are computed within the normal mode approximation and compared with experiment. The harmonic model is shown to be capable of describing the appearance of the "new shifted spectrum,'' originally identified as a "relaxed spectrum,'' which becomes increasingly dominant with increasing chain length. Thus, this feature cannot be a consequence of intramolecular vibrational redistribution (IVR). By contrast, the appearance of substantial spectral broadening can only be accounted for through the introduction of anharmonic coupling. An assessment of standard assumptions in the analysis of IVR in "ring+tail'' molecules is also provided. Results show that some crucial assumptions, e.g., that electronic transitions are not accompanied by changes in chain excitation, are unjustified.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.459808
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  • 9
    Electronic Resource
    Electronic Resource
    Coherent control of bimolecular chemical reactions (1990)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 92 (1990), S. 1126-1131 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We show how the method of coherent control can be applied to control product yield in bimolecular chemical reactions. First, a laser pulse prepares a coherent superposition of two bound levels of an electronically excited state of the reactants. Then, after a variable delay, a second laser pulse photodissociates the system to the ground state continuum. By varying the detuning of the excitation pulse and the delay between the two pulses, we show that significant control of the product ratio can be achieved. As a first application of the method we demonstrate, with exact quantum-mechanical calculations, the control of the collinear H+H2 and D+H2 reactions. The pulses and delays used in these calculations are on the order of picoseconds, a range of time scales well within that achievable with conventional laser systems.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.458174
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  • 10
    Electronic Resource
    Electronic Resource
    Three-dimensional quantum-mechanical computations of the control of the H+OD←DOH→D+OH reaction (1993)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 98 (1993), S. 201-205 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A three-dimensional quantum mechanical study of the control of a branching photochemical reaction H+OD←DOH→D+OH is presented. It is shown that with two laser pulses, one pulse used to generate a superposition of the (0,2,0) and the (1,0,0) states, and the other, a VUV pulse, used to dissociate the molecule by exciting it to the B continuum, it is possible to control which of two chemical channels is preferred. The control parameters used are the center frequency of the excitation laser and the time delay between the two pulses. For the above superposition state, a combination of a 200 fs excitation pulse and a 50 fs dissociation pulse is found to yield the widest (10% to 90% yield in the H+OD channel) range of control, essentially irrespective of the photolysis wavelength.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.464655
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