Single-shot interferometric approach to background free broadband coherent anti-Stokes Raman scattering spectroscopy

Optics Express
Young Jong Lee, Marcus T Cicerone

Abstract

We introduce a single-shot interferometric approach to suppress the nonresonant background (NRB) contribution to a broadband coherent anti-Stokes Raman scattering (CARS) spectrum; this single-shot approach is conducive to rapid imaging. A pulse shaper prepares a narrowband pulse with two spectral components of differing phase. When the CARS fields generated by these two out-of-phase components are optically mixed, NRB signal is greatly reduced while a resonant CARS signal remains with minimal attenuation. We discuss and demonstrate two model schemes for the interfering pulse components: (1) two pulses with different bandwidths and the same center frequency (ps-fs scheme) and (2) two pulses with the same bandwidth and shifted center frequencies (ps-ps scheme). In both schemes, only the resonant signal from the "3-color" CARS mechanism survives. The resonant signal from "2-color" CARS mechanism vanishes along with the NRB. We discuss optimization conditions for signal intensity and shape of resonant CARS peaks. Experimental CARS spectra of c-hexane and benzonitrile demonstrate feasibility of these approaches.

References

Feb 28, 2002·Physical Review Letters·Dan OronYaron Silberberg
Nov 3, 2005·Proceedings of the National Academy of Sciences of the United States of America·Conor L EvansX Sunney Xie
Jan 31, 2006·Optics Letters·Eric O PotmaX Sunney Xie
Feb 25, 2006·Optics Letters·Jennifer P OgilvieManuel Joffre
Mar 3, 2006·The Journal of Physical Chemistry. B·Hilde A RiniaMichiel Müller
Nov 21, 2007·Optics Letters·Young Jong LeeMarcus T Cicerone
Dec 1, 2007·Optics Letters·J X ChengX S Xie
Feb 29, 2008·The Journal of Physical Chemistry. B·Bi-Chang Chen, Sang-Hyun Lim
Apr 17, 2006·Optics Express·Tak W KeeMarcus T Cicerone
Nov 12, 2007·Optics Express·M JurnaH L Offerhaus

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Citations

Apr 9, 2010·Analytical Chemistry·Praveen D ChowdaryMartin Gruebele
Dec 4, 2009·IEEE Journal of Quantum Electronics·Wladimir A BenalcazarStephen A Boppart
Oct 21, 2010·Biophysical Journal·Sapun H ParekhMarcus T Cicerone
Dec 22, 2015·Applied Spectroscopy·Hai LiuTianxu Zhang
Feb 23, 2010·Optics Express·Alexander C W van RhijnAliakbar Jafarpour
May 6, 2019·Physical Review Letters·V Yu ShishkovA A Lisyansky

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