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  • 1
    ISSN: 1476-4687
    Source: Nature Archives 1869 - 2009
    Topics: Biology , Chemistry and Pharmacology , Medicine , Natural Sciences in General , Physics
    Notes: [Auszug] The advent of the laser as an intense source of coherent light gave rise to nonlinear optics, which now plays an important role in many areas of science and technology. One of the first applications of nonlinear optics was the multi-wave mixing, of several optical fields in a nonlinear medium ...
    Type of Medium: Electronic Resource
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  • 2
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 97 (1992), S. 9107-9115 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We describe a technique for totally transferring the population of a molecular vibronic level to another optically accessible level by chirped pulse absorption. The method can be applied even for nonvanishing angular momentum states where the Rabi frequencies for the transitions depend on the magnetic quantum number M of the states. The population of a large J initial state can be totally transferred to a J'=J+1 state by R branch transitions with linearly or circularly polarized light pulses with negative or positive frequency chirp if the bandwidth of the chirped pulse is sufficiently small. For an initial state with small J, having P(Q) and R transitions that are closely spaced in energy and within the chirped pulse bandwidth, the situation is complicated by the presence of transitions involving additional nearby J states which can participate in transitions induced by the chirped pulse. For positive frequency chirp, population can be totally transferred to the excited electronic state, whereas for the negative frequency chirp case the population distribution depends on the details of the energy levels and laser pulse. The technique can be employed to align and orient states in which not all the M states of the initial level are transferred to the same branch, but each M state is totally transferred from the initial state. Criteria for this type of population transfer and alignment and orientation are described and the conditions under which adiabatic passage is maintained are discussed.
    Type of Medium: Electronic Resource
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  • 3
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The strong interaction between the B 3sσ 1Σ+ Rydberg state and the D' 1Σ+ valence state of the CO molecule is shown to cause large changes in the vibrational and rotational constants of the B state, as well as predissociation of all rotational levels of B (v'=2) and a breaking off in the emission of B (v'=1) levels at J=36 in 12C 16O and J=37 in 13C 16O. A two-state diabatic model of the Rydberg–valence interaction is constructed and vibrational term values, widths, and intensities are calculated by close coupling in order to account for the strong mixing. The model separates the differences between the spectroscopic constants of the B state and those of the ground state molecular ion into two components, one due to the R-dependent quantum defect of the B state and another due to the strong Rydberg–valence perturbation. The perturbation is characterized by a constant coupling matrix element of 2900 cm−1 inside the crossing point of the two diabatic potentials, decaying to zero at long internuclear distances. Basically good agreement is found between the model and experiment for shifts in vibrational and rotational terms and for predissociation widths and relative band intensities. The second breaking off in emission in the B (v'=1) rotational series is used to estimate the height of the long-range barrier maximum in the D' 1Σ+ state to be about 1048±19 cm−1 above the ground state dissociation limit. Comparison of predicted widths from the two channel close coupled model with those from a single channel adiabatic model shows differences on the order of a factor of 2.
    Type of Medium: Electronic Resource
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  • 4
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 96 (1992), S. 3339-3341 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Some simple schemes for obtaining complete alignment and orientation of atoms and molecules using stimulated Raman scattering with temporally shifted laser fields is proposed. (AIP)
    Type of Medium: Electronic Resource
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  • 5
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We compare the results of full density matrix calculations with recently reported experimental results describing the population transfer in Na2 using Raman scattering with the fundamental laser beam temporally shifted relative to the Stokes laser beam. Our calculations confirm the conclusion that almost total transfer of the population into the terminal level of the Raman transition can be achieved when the laser frequencies are tuned to resonance and the fundamental laser beam is temporally delayed relative to the Stokes shifted laser beam but still partially overlapping it. We analyze our results when the frequencies of the lasers are tuned off-resonance as a function of the Rabi frequencies and the detuning, and compare with experimental and theoretical results. The alignment of the terminal level as a function of time displacement of the Stokes and pump beams is predicted.
    Type of Medium: Electronic Resource
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  • 6
    Electronic Resource
    Electronic Resource
    New York, NY [u.a.] : Wiley-Blackwell
    Journal of Computational Chemistry 3 (1982), S. 372-380 
    ISSN: 0192-8651
    Keywords: Computational Chemistry and Molecular Modeling ; Biochemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology , Computer Science
    Notes: Spin-orbit and dispersion energy contributions to the energy curves of XeF are examined. A rapid variation in the spin-orbit coupling with internuclear separation is found for both the ground and excited states. This result can explain the experimentally observed ordering of the ionic excited states when the spin-orbit perturbation couples 2σ and 2π energy curves obtained by both all-electron and effective core potential (ECP) calculations at the first-order configuration interaction (FOCI) level of accuracy. Damped dispersion energy contributions to the ground-state energy curve are shown to be comparable to the charge transfer contribution. The energy curve for XeF is in reasonable agreement with experimental results and a calculation of the analogous XeCl curve confirms the qualitative correctness of the calculation. The energy curves and transition moments were then applied to two problems related to the efficiency of the XeF laser. Photodissociation of the X state provides a means of removing a bottlenecked vibrational level but a calculation of the radiative transition probability between the X and A states finds the cross section is too small to yield rates competitive with collisional deactivation. The bottlenecked state may also be removed by electron dissociative attachment but the calculated energy curves for the X states of XeF and XeF- do not cross at a low energy indicating a small cross section.
    Additional Material: 4 Ill.
    Type of Medium: Electronic Resource
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  • 7
    Electronic Resource
    Electronic Resource
    Palo Alto, Calif. : Annual Reviews
    Annual Review of Physical Chemistry 46 (1995), S. 423-452 
    ISSN: 0066-426X
    Source: Annual Reviews Electronic Back Volume Collection 1932-2001ff
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
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  • 8
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 95 (1991), S. 5681-5685 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We present results of density matrix calculations describing population transfer in a four level system via stimulated Raman scattering with three laser pulses whose frequencies are in (or nearly in) resonance with the transitions between the levels. A high degree of transfer to the terminal level is possible via transitions through the two intermediate excited levels, despite the large decay rates of both levels compared with the inverse of the laser pulse durations, provided that the pulse timing sequences are correctly adjusted. Hence multiple stimulated Raman scattering can be an efficient method of moving population into a given molecular level.
    Type of Medium: Electronic Resource
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