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  • 1
    Electronic Resource
    Electronic Resource
    Fifth-order nonlinear Raman processes in molecular liquids using quasi-cw noisy light. II. Experiment (1999)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 111 (1999), S. 272-280 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Fifth-order analogs of coherent Raman scattering generated in a number of molecular liquids using broadband quasi-cw noisy light are presented. It is seen how the signal for the direct fifth-order process, which probes the dynamics of both a fundamental vibration and its overtone, is often contaminated by a sequential process, that is only capable of probing the vibrational dynamics of the fundamental. Although these two processes are virtually indistinguishable when a single Raman resonance is excited, we find that when a second Raman resonance is available within the experimental window governed by the bandwidth of the noisy light, new frequency components in the signal arise and the two competing fifth-order processes become distinguishable. These new frequency components, as well as their decay, are explained in terms of spectral filtering of the noisy light by the Raman resonances. This spectral filter analogy predicts which of the two competing processes dominates in an equimolar mixture of benzene-h6 and benzene-d6, and also in neat pyridine (each providing two available fundamentals). It is found by this new method that the sequential event is present and apparently fully dominates the direct process for all molecular liquids studied here. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.479271
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  • 2
    Electronic Resource
    Electronic Resource
    Electronically nonresonant coherent Raman scattering using incoherent light: Two Brownian oscillator approaches (1998)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 108 (1998), S. 9425-9435 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The theory for electronically nonresonant coherent Raman scattering using incoherent light (I(2)CRS) is presented for a Brownian oscillator material response. The exploration of Raman line shapes is based on two different approaches, both of which incorporate the Brownian oscillator model. The first takes the Raman transition as a two-level system that is indirectly coupled to the bath through "primary" Brownian oscillators. The I(2)CRS signal in the overdamped, high temperature regime is calculated analytically using this approach. The second approach is the standard one in which the Raman transition itself is represented by primary Brownian oscillators that are directly coupled to the bath. This method permits analytic calculation of the I(2)CRS signal for the entire parameter space and also for a distribution of oscillators to account for inhomogeneous linewidth broadening. These two methods allow for different interpretations of Raman line shapes using noisy light spectroscopy. © 1998 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.476393
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  • 3
    Electronic Resource
    Electronic Resource
    Quantitative biphotonic chemistry by a fluorescence loss method. Photodissociation and photoionization of durene in a rigid solution (1973)
    s.l. : American Chemical Society
    The @journal of physical chemistry 〈Washington, DC〉 77 (1973), S. 2808-2822 
    Details
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/j100641a019
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  • 4
    Electronic Resource
    Electronic Resource
    Fifth-order nonlinear Raman processes in molecular liquids using quasi-cw noisy light. I. Theory (1999)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 111 (1999), S. 253-271 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Fifth-order nonlinear Raman processes using broadband, incoherent light are treated for a multiply resonant, multicomponent mixture. In particular, the theoretical development of the direct and the sequential fifth-order analogs of coherent Raman scattering is presented. Of the complete formalism, only the dominant doubly Raman resonant hyperpolarizability contributions to the signal intensity are discussed in this article. Furthermore, application is made to simulate fifth-order signals from a variety of hypothetical molecular liquids. It is seen how the direct and the sequential processes can distinguish themselves in a mixture, in a neat liquid with more than one Raman coherence, and also whenever the Raman active modes are taken to be anharmonic. This theoretical treatment anticipates experimental results presented in the following paper. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.479287
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  • 5
    Electronic Resource
    Electronic Resource
    Theory of coherent Raman scattering with quasi-cw noisy light for a general line shape function (1997)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 107 (1997), S. 7127-7137 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The theory of electronically nonresonant coherent Raman scattering (CRS) with quasi-cw noisy light (I(2) CRS) is developed for a general material response. The (Raman) resonant–resonant and resonant–nonresonant hyperpolarizability contributions to the I(2) CRS signal are interferometrically separable. It is found that, in general, the interferometric decay of each of these terms exposes the Raman line shape function in a different manner. Only for a Lorentzian line is their decay identical. Thus, in principle, I(2) CRS provides a new way to explore the line shape function that is analytically distinct from frequency domain and time domain methods. By way of illustration, the general theory is applied to three common line shapes: Lorentzian (as in the original I(2) CRS theory), Gaussian, and Voigt. The results are shown to be consistent with the principles of factorized time correlation diagram analysis. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.474954
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  • 6
    Electronic Resource
    Electronic Resource
    Raman scattering from a Brownian oscillator with nonohmic Drude dissipation: Applications to continuous wave, impulsive, and noisy excitation (1998)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 109 (1998), S. 4478-4486 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: An extension of the Brownian oscillator model in nonlinear optical spectroscopy to include frictional memory is treated. Although we have obtained analytic expressions for this model, their unwieldiness makes the understanding of the effect of nonzero frictional memory difficult. However, by focusing on the behavior of the analytically continued oscillator coordinate correlation function in the complex frequency plane, qualitative insight is obtained. Applications to spontaneous Raman scattering and two time-resolved coherent Raman scattering spectroscopies are briefly explored. © 1998 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.477051
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  • 7
    Electronic Resource
    Electronic Resource
    Competitive events in fifth order time resolved coherent Raman scattering: Direct versus sequential processes (1998)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 108 (1998), S. 3897-3902 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Higher order time resolved nonlinear optical processes can often be obscured by sequential lower order processes that compete with the direct event and give similar time domain behavior though they probe different dynamics. This is true for a certain fifth order coherent anti-Stokes Raman scattering (CARS) spectroscopy designed to probe overtone vibrational dynamics. The homodyned intensity from the two competing processes is calculated and it is shown how only the direct fifth order polarization probes overtone dephasing. © 1998 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.475837
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  • 8
    Electronic Resource
    Electronic Resource
    Overtone resonance Raman scattering beyond the Condon approximation: Transform theory and vibronic properties (1994)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 101 (1994), S. 1890-1903 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The time correlator formalism is used to develop the expression for nth order (overtone) resonance Raman scattering (RRS) to include both Raman frequency shifts upon electronic excitation as well as non-Condon vibronic coupling. In particular the compact operator formalism recently introduced by Hizhnyakov and Tehver [J. Raman Spectrosc. 19, 383 (1988)] to obtain several RRS correlators (including overtone scattering with frequency shift, but in the Condon approximation) is used to extend the theory. At the same time a formal advantage is achieved by the limited introduction of the Born–Oppenheimer approximation. Also transform relationships including non-Condon effects are given that link the Raman excitation profile of nth order scattering to the absorption spectrum. Finally, it is emphasized how all three vibronic parameters—potential energy surface displacement, Raman mode frequency changes, and the linear non-Condon coupling parameter—can be quantitatively determined without the need for absolute Raman cross-section measurements. The relative scattering intensity of the fundamental and three (or more) overtones suffices to fix the three. By way of application, the vibronic parameters are determined from published single wavelength overtone RRS in six molecules.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.468434
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  • 9
    Electronic Resource
    Electronic Resource
    Theory of three-photon photoselection with application to the hexagonal point groups (1986)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 85 (1986), S. 3145-3154 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The general problem of the polarization dependence of an orientationally averaged four-photon process in a rigid isotropic medium is examined. The theory is then reduced to the special case of three-photon photoselection (3PP) in which an excited state is first created by the simultaneous absorption of three identical photons and then the system is interrogated by a one-photon probe step (absorption or emission). When the probe signal is measured as a function of both excitation and probing polarizations, five unique transition tensor invariants can be determined. These five invariants provide a characteristic signature of the symmetry of the initial three-photon absorption (3PA). A symmetry analysis is illustrated within the hexagonal point groups where it is demonstrated how the measurement of a single photoselection polarization ratio formally allows, with one exception, a unique symmetry assignment to be made for any three-photon allowed transition. This measurement makes use of circularly polarized excitation with variably polarized probing. The polarized probe step in a 3PP experiment provides information concerning the three-photon transition beyond that available from a simple polarized 3PA study.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.450981
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  • 10
    Electronic Resource
    Electronic Resource
    A condensed phase study of the benzene B2u←A1g three-photon transition (1986)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 85 (1986), S. 3155-3164 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Although group theoretically allowed, the benzene B2u←A1g three-photon transition appears to derive intensity exclusively through a vibronic coupling route. The ν6 (e2g) vibration is dominant in providing e1u vibronic symmetry, just as it is in the one-photon transition. Several experiments are presented that provide further insight into the lack of allowed vibronic b2u activity in the three-photon spectrum. Pseudoparity, applicable to even alternate hydrocarbons in the PPP formalism, and offering selection rules beyond those based on symmetry alone, is examined as a possible explanation by looking for effects from the inductive perturbation in a fluorine substituted benzene. The possibility of nonresonant third harmonic generation in the condensed phase sample, which may lead to a viable one-photon absorption route to the excited B2u state, is also explored in both a three-photon photoselection study as well as in an experiment comparing the relative three-photon to one-photon cross sections for benzene and biphenyl. The results obtained for the benzene B2u transition and the corresponding A′2 transition in the symmetrically substituted trifluorobenzene appear to confirm the importance of pseudoparity selection rules and suggest that the third harmonic generation pathway is of minor importance.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.450982
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