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    Floquet–Liouville supermatrix approach. II. Intensity‐dependent generalized nonlinear optical susceptibilities

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    Issue Date
    1987-08-15
    Author
    Chu, Shih-I
    Wang, Kwanghsi
    Publisher
    AIP Publishing
    Type
    Article
    Article Version
    Scholarly/refereed, publisher version
    Metadata
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    Abstract
    We present a practical n o n p e r t u r b a t i v e method for e x a c t treatment of i n t e n s i t y‐d e p e n d e n t generalized nonlinear optical susceptibilities χ(ω) in intense polychromatic fields, valid for arbitrary laser intensities, detunings, and relaxation. By means of the many‐mode Floquet theory, the time‐dependent Liouville equation can be transformed into an equivalent t i m e‐i n d e p e n d e n t infinite‐dimensional Floquet–Liouville supermatrix (FLSM) eigenvalue problem. It is then shown that the nonlinear optical susceptibilities χ(ω) can be completely determined simply from the supereigenvalues and eigenfunctions of the Floquet–Liouvillian  L̂ F . In addition to this exact FLSM approach, we have also presented higher‐order perturbative results, based on the extension of the Salwen’s nearly degenerate perturbation theory, appropriate for somewhat weaker fields and near‐resonant multiphoton processes, but beyond the conventional perturbative or rotating wave approximation (RWA). In the case of two‐level systems, for example, the implementation of Salwen’s method in the time‐independent L̂ F allows the reduction of the infinite‐dimensional FLSM into a 4×4 dimensional effective Hamiltonian, from which essential a n a l y t i c a l formulas for intensity‐dependent χ(ω) can be obtained. These methods are applied to a detailed study of intensity‐dependent spectralline shapes (such as hole burning and extra resonance peaks at the line center, and the effects of saturation, detuning, and radiative and collisional damping, etc.) and subharmonic structures in nonlinear multiple wave mixings χ[(m+1)ω1−mω2] for two‐level systems in intense linearly polarized bichromatic fields.
    Description
    This is the published version, also available here: http://dx.doi.org/10.1063/1.451981
    URI
    http://hdl.handle.net/1808/15839
    DOI
    https://doi.org/10.1063/1.451981
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    • Chemistry Scholarly Works [610]
    Citation
    Wang, Kwanghsi & Chu, Shih-I. "Floquet–Liouville supermatrix approach. II. Intensity‐dependent generalized nonlinear optical susceptibilities." The Journal of Chemical Physics 86, 3225 (1987); http://dx.doi.org/10.1063/1.451981.

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    KU Libraries
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    785-864-8983

    KU Libraries
    1425 Jayhawk Blvd
    Lawrence, KS 66045
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    Contact KU ScholarWorks
    785-864-8983
    KU Libraries
    1425 Jayhawk Blvd
    Lawrence, KS 66045
    785-864-8983

    KU Libraries
    1425 Jayhawk Blvd
    Lawrence, KS 66045
    Image Credits
     

     

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