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Journal of Chemical Physics / Volume 133 / Issue 2 / ARTICLES / Condensed Phase Dynamics, Structure, and Thermodynamics: Spectroscopy, Reactions, and Relaxation

J. Chem. Phys. 133, 024505 (2010); http://dx.doi.org/10.1063/1.3464332 (6 pages)

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

S. Umapathy, B. Mallick, and A. Lakshmanna

Department of Inorganic and Physical Chemistry, Indian Institute of Science, Bangalore 560012, India

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(Received 31 October 2008; accepted 24 June 2010; published online 13 July 2010)

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.

© 2010 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. EXPERIMENTAL
  3. RESULTS AND DISCUSSION
  4. IMPLICATIONS

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KEYWORDS and PACS

Keywords

fluorescence, Franck-Condon factors, Raman spectroscopy, spectral line breadth, stimulated Raman scattering, vibrational states

PACS

  • 33.20.Fb

    Raman and Rayleigh spectra (including optical scattering)

  • 52.38.Bv

    Rayleigh scattering; stimulated Brillouin and Raman scattering

  • 33.15.Mt

    Rotation, vibration, and vibration-rotation constants

  • 33.50.Dq

    Fluorescence and phosphorescence spectra

  • 07.57.Ty

    Infrared spectrometers, auxiliary equipment, and techniques

  • 33.70.Jg

    Line and band widths, shapes, and shifts

  • 33.70.Ca

    Oscillator and band strengths, lifetimes, transition moments, and Franck-Condon factors

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.3464332

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

For access to fully linked references, you need to log in.
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