Intrinsic cascading contributions to the fifth- and seventh-order electronically off-resonant Raman spectroscopies

The cascading polarization contributing to the femtosecond fifth- and seventh-order coherent Raman scattering processes is obtained in terms of the third- and fifth-order Raman response functions. It is found that four cascading processes contribute to the fifth-order Raman scattering signal. In the...

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Veröffentlicht in:The Journal of chemical physics 2000-02, Vol.112 (5), p.2082-2094
Hauptverfasser: Cho, Minhaeng, Blank, David A., Sung, Jaeyoung, Park, Kisam, Hahn, Sangjoon, Fleming, Graham R.
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Sprache:eng
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Zusammenfassung:The cascading polarization contributing to the femtosecond fifth- and seventh-order coherent Raman scattering processes is obtained in terms of the third- and fifth-order Raman response functions. It is found that four cascading processes contribute to the fifth-order Raman scattering signal. In the case of the seventh-order Raman scattering, there are 34 possible cascading processes contributing to the seventh-order Raman scattering signal, and they are classified as χ(5)×χ(3)- and χ(3)×χ(3)×χ(3)-types depending on the involved low-order nonlinear optical processes. Due to the complicated interference among these polarization fields, it may not be possible to experimentally measure the pure seventh-order Raman scattering signal without contamination from the cascaded contributions.
ISSN:0021-9606
1089-7690
DOI:10.1063/1.480777