Fifth-order electronically non-resonant raman scattering: Two-dimensional Fourier deconvolution

Laura J. Kaufman, Jiyoung Heo, Graham R. Fleming, Jaeyoung Sung, Minhaeng Cho

    Research output: Contribution to journalArticlepeer-review

    17 Citations (Scopus)

    Abstract

    This paper presents an analytical Fourier deconvolution procedure for homodyne detected electronically non-resonant fifth-order signal that reveals the bare nuclear response function free from the influence of the electronic (hyperpolarizability) responses generated by the five potentially overlapping finite duration pulses used in the experiment. In developing the fifth-order deconvolution procedure, an analogous procedure for homodyne detected third-order responses is elaborated. The potential implementation problems with the homodyne deconvolution procedure are evaluated through comparison of the third-order homodyne deconvolution result with that of the well-known third-order heterodyne deconvolution. Then, the homodyne deconvolution is extended to fifth-order where it is used on several measured tensor elements of the direct fifth-order signal. Suggestions are given for improving implementation of the procedure in fifth order so that more information on the direct fifth-order nuclear response as well as the hyperpolarizability responses can be recovered via the deconvolution procedure.

    Original languageEnglish
    Pages (from-to)251-271
    Number of pages21
    JournalChemical Physics
    Volume266
    Issue number2-3
    DOIs
    Publication statusPublished - 2001 May 15

    Bibliographical note

    Funding Information:
    This work was supported by the NSF (USA) and the CRI program of KISTEP (MOST, Korea). J. Sung is supported by a postdoctoral fellowship from the Korea Science and Engineering Foundation (KOSEF). The authors gratefully acknowledge Dr. Mino Yang for helpful suggestions and insightful comments.

    Keywords

    • Electronic responses
    • Fourier deconvolution
    • Raman scattering

    ASJC Scopus subject areas

    • General Physics and Astronomy
    • Physical and Theoretical Chemistry

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