Back to Search Start Over

Development of simultaneous frequency- and time-resolved coherent anti-Stokes Raman scattering for ultrafast detection of molecular Raman spectra.

Authors :
Prince, Benjamin D.
Chakraborty, Abhijit
Prince, Beth M.
Stauffer, Hans U.
Source :
Journal of Chemical Physics. 7/28/2006, Vol. 125 Issue 4, p044502. 8p. 1 Diagram, 7 Graphs.
Publication Year :
2006

Abstract

The development of a time-resolved coherent anti-Stokes Raman scattering (CARS) variant for use as a probe of excited electronic state Raman-active modes following excitation with an ultrafast pump pulse is detailed. Application of this technique involves a combination of broadband fs-time scale pulses and a narrowband pulse of ps duration that allows multiplexed detection of the CARS signal, permitting direct observation of molecular Raman frequencies and intensities with time resolution dictated by the broadband pulses. Thus, this nonlinear optical probe, designated fs/ps CARS, is suitable for observation of Raman spectral evolution following excitation with a pump pulse. Because of the spatial separation of the CARS output signal relative to the three input beams inherent in a folded BOXCARS arrangement, this technique is particularly amenable to probing low-frequency vibrational modes, which play a significant role in accepting vibrational energy during intramolecular vibrational energy redistribution within electronically excited states. Additionally, this spatial separation allows discrimination against strong fluorescence signal, as demonstrated in the case of rhodamine 6G. [ABSTRACT FROM AUTHOR]

Details

Language :
English
ISSN :
00219606
Volume :
125
Issue :
4
Database :
Academic Search Index
Journal :
Journal of Chemical Physics
Publication Type :
Academic Journal
Accession number :
21845397
Full Text :
https://doi.org/10.1063/1.2219439