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Title: Mode-dependent dispersion in Raman line shapes: Observation and implications from ultrafast Raman loss spectroscopy

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.3464332· OSTI ID:21559882
; ;  [1]
  1. Department of Inorganic and Physical Chemistry, Indian Institute of Science, Bangalore 560012 (India)

Ultrafast Raman loss spectroscopy (URLS) enables one to obtain the vibrational structural information of molecular systems including fluorescent materials. URLS, a nonlinear process analog to stimulated Raman gain, involves a narrow bandwidth picosecond Raman pump pulse and a femtosecond broadband white light continuum. Under nonresonant condition, the Raman response appears as a negative (loss) signal, whereas, on resonance with the electronic transition the line shape changes from a negative to a positive through a dispersive form. The intensities observed and thus, the Franck-Condon activity (coordinate dependent), are sensitive to the wavelength of the white light corresponding to a particular Raman frequency with respect to the Raman pump pulse wavelength, i.e., there is a mode-dependent response in URLS.

OSTI ID:
21559882
Journal Information:
Journal of Chemical Physics, Vol. 133, Issue 2; Other Information: DOI: 10.1063/1.3464332; (c) 2010 American Institute of Physics; ISSN 0021-9606
Country of Publication:
United States
Language:
English