Time- and frequency-resolved coherent anti-Stokes Raman scattering spectroscopy with sub-25 fs laser pulses

Download
  1. (PDF, 1 MB)
  2. Get@NRC: Time- and frequency-resolved coherent anti-Stokes Raman scattering spectroscopy with sub-25 fs laser pulses (Opens in a new window)
DOIResolve DOI: http://doi.org/10.1063/1.2932101
AuthorSearch for: ; Search for: ; Search for: ; Search for: ; Search for: ; Search for:
TypeArticle
Journal titleJournal of Chemical Physics
ISSN0021-9606
Volume128
SubjectStimulated Raman scattering; polarization; excited states; molecular dynamics; time resolved spectroscopy
AbstractIn general, many different diagrams can contribute to the signal measured in broadband four-wave mixing experiments. Care must therefore be taken when designing an experiment to be sensitive to only the desired diagram by taking advantage of phase matching, pulse timing, sequence, and the wavelengths employed. We use sub-25fs pulses to create and monitor vibrational wavepackets in gaseous iodine, bromine, and iodine bromide through time- and frequency-resolved femtosecond coherent anti-Stokes Raman scattering (CARS)spectroscopy. We experimentally illustrate this using iodine, where the broad bandwidths of our pulses, and Boltzmann population in the lower three vibrational levels conspire to make a single diagram dominant in one spectral region of the signal spectrum. In another spectral region, however, the signal is the sum of two almost equally contributing diagrams, making it difficult to directly extract information about the molecular dynamics. We derive simple analytical expressions for the time- and frequency-resolved CARS signal to study the interplay of different diagrams. Expressions are given for all five diagrams which can contribute to the CARS signal in our case.
LanguageEnglish
AffiliationNRC Steacie Institute for Molecular Sciences; National Research Council Canada
Peer reviewedYes
NPARC number21277110
Export citationExport as RIS
Report a correctionReport a correction
Record identifier0fe78fea-ca86-40e8-b36e-af39312a8615
Record created2015-12-01
Record modified2016-05-09
Bookmark and share
  • Share this page with Facebook (Opens in a new window)
  • Share this page with Twitter (Opens in a new window)
  • Share this page with Google+ (Opens in a new window)
  • Share this page with Delicious (Opens in a new window)