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.

© 2009 Optical Society of America

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  1. A. Zumbusch, G. R. Holtom, and X. S. Xie, "Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering," Phys. Rev. Lett. 82, 4142-4145 (1999).
    [CrossRef]
  2. C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
    [CrossRef] [PubMed]
  3. J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "Multiplex coherent anti-stokes Raman scattering microspectroscopy and study of lipid vesicles," J. Phys. Chem. B 106, 8493-8498 (2002).
    [CrossRef]
  4. T. W. Kee and M. T. Cicerone, "Simple approach to one-laser, broadband coherent anti-Stokes Raman scattering microscopy," Opt. Lett. 29, 2701-2703 (2004).
    [CrossRef] [PubMed]
  5. G. I. Petrov and V. V. Yakovlev, "Enhancing red-shifted white-light continuum generation in optical fibers for applications in nonlinear Raman microscopy," Opt. Express 13, 1299-1306 (2005).
    [CrossRef] [PubMed]
  6. H. A. Rinia, M. Bonn, and M. Muller, "Quantitative multiplex CARS spectroscopy in congested spectral regions," J. Phys. Chem. B 110, 4472-4479 (2006).
    [CrossRef] [PubMed]
  7. Y. J. Lee, Y Liu, and M. T. Cicerone, "Characterization of 3-color CARS in a 2-pulse broadband CARS spectrum," Opt. Lett. 32, 3370-3372 (2007).
    [CrossRef] [PubMed]
  8. F. Ganikhanov, C. L. Evans, B. G. Saar, and X. S. Xie, "High-sensitivity vibrational imaging with frequency modulation coherent anti-Stokes Raman scattering (FM CARS) microscopy," Opt. Lett. 31, 1872-1874 (2006).
    [CrossRef] [PubMed]
  9. J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "An epi-detected coherent anti-stokes raman scattering (E-CARS) microscope with high spectral resolution and high sensitivity," J. Phys. Chem. B 105, 1277-1280 (2001).
    [CrossRef]
  10. J. X. Cheng, L. D. Book, and X. S. Xie, "Polarization coherent anti-Stokes Raman scattering microscopy," Opt. Lett. 26, 1341-1343 (2001).
    [CrossRef]
  11. A. Volkmer, L. D. Book, and X. S. Xie, "Time-resolved coherent anti-Stokes Raman scattering microscopy: Imaging based on Raman free induction decay," Appl. Phys. Lett. 80, 1505-1507 (2002).
    [CrossRef]
  12. C. L. Evans, E. O. Potma, and X. S. N. Xie, "Coherent anti-Stokes Raman scattering spectral interferometry: determination of the real and imaginary components of nonlinear susceptibility ?(3) for vibrational microscopy," Opt. Lett. 29, 2923-2925 (2004).
    [CrossRef]
  13. E. O. Potma, C. L. Evans, and X. S. Xie, "Heterodyne coherent anti-Stokes Raman scattering (CARS) imaging," Opt. Lett. 31, 241-243 (2006).
    [CrossRef] [PubMed]
  14. D. Oron, N. Dudovich, and Y. Silberberg, "Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 90, 213902 (2003).
    [CrossRef] [PubMed]
  15. B. C. Chen and S. H. Lim, "Optimal laser pulse shaping for interferometric multiplex coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 112, 3653-3661 (2008).
    [CrossRef] [PubMed]
  16. T. W. Kee, H. X. Zhao, and M. T. Cicerone, "One-laser interferometric broadband coherent anti-Stokes Raman scattering," Opt. Express 14, 3631-3640 (2006).
    [CrossRef] [PubMed]
  17. J. P. Ogilvie, E. Beaurepaire, A. Alexandrou, and M. Joffre, "Fourier-transform coherent anti-Stokes Raman scattering microscopy," Opt. Lett. 31, 480-482 (2006).
    [CrossRef] [PubMed]
  18. H. Kano and H. Hamaguchi, "Dispersion-compensated supercontinuum generation for ultrabroadband multiplex coherent anti-Stokes Raman scattering spectroscopy," J. Raman Spectrosc. 37, 411-415 (2006).
    [CrossRef]
  19. G. L. Eesley, Coherent Raman Spectroscopy (Pergamon Press, Oxford 1981).
  20. D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Narrow-band coherent anti-stokes Raman signals from broad-band pulses," Phys. Rev. Lett. 88, 063004 (2002).
    [CrossRef] [PubMed]
  21. A. Morresi, L. Mariani, M. R. Distefano, and M. G. Giorgini, "Vibrational-Relaxation Processes in Isotropic Molecular Liquids - A Critical Comparison," J. Raman Spectrosc. 26, 179-216 (1995).
    [CrossRef]
  22. J. M. Dudley, G. Genty, and S. Coen, "Supercontinuum generation in photonic crystal fiber," Rev. Mod. Phys. 78, 1135-1184 (2006).
    [CrossRef]
  23. Y. J. Lee and M. T. Cicerone, "Vibrational dephasing time imaging by time-resolved broadband coherent anti-Stokes Raman scattering microscopy," Appl. Phys. Lett. 92, 041108 (2008).
    [CrossRef]
  24. Certain equipment is identified in this Letter to specify adequately the experimental details. Such identification does not imply recommendation by the National Institute of Standards and Technology, nor does it imply that the equipment is necessarily the best available for this purpose.
  25. B. von Vacano, L. Meyer, and M. Motzkus, "Rapid polymer blend imaging with quantitative broadband multiplex CARS microscopy," J. Raman Spectrosc. 38, 916-926 (2007).
    [CrossRef]
  26. M. Jurna, J. P. Korterik, C. Otto, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Opt. Express 15, 15207-15213 (2007).
    [CrossRef] [PubMed]

2008 (2)

B. C. Chen and S. H. Lim, "Optimal laser pulse shaping for interferometric multiplex coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 112, 3653-3661 (2008).
[CrossRef] [PubMed]

Y. J. Lee and M. T. Cicerone, "Vibrational dephasing time imaging by time-resolved broadband coherent anti-Stokes Raman scattering microscopy," Appl. Phys. Lett. 92, 041108 (2008).
[CrossRef]

2007 (3)

2006 (7)

2005 (2)

C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
[CrossRef] [PubMed]

G. I. Petrov and V. V. Yakovlev, "Enhancing red-shifted white-light continuum generation in optical fibers for applications in nonlinear Raman microscopy," Opt. Express 13, 1299-1306 (2005).
[CrossRef] [PubMed]

2004 (2)

2003 (1)

D. Oron, N. Dudovich, and Y. Silberberg, "Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 90, 213902 (2003).
[CrossRef] [PubMed]

2002 (3)

A. Volkmer, L. D. Book, and X. S. Xie, "Time-resolved coherent anti-Stokes Raman scattering microscopy: Imaging based on Raman free induction decay," Appl. Phys. Lett. 80, 1505-1507 (2002).
[CrossRef]

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "Multiplex coherent anti-stokes Raman scattering microspectroscopy and study of lipid vesicles," J. Phys. Chem. B 106, 8493-8498 (2002).
[CrossRef]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Narrow-band coherent anti-stokes Raman signals from broad-band pulses," Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

2001 (2)

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "An epi-detected coherent anti-stokes raman scattering (E-CARS) microscope with high spectral resolution and high sensitivity," J. Phys. Chem. B 105, 1277-1280 (2001).
[CrossRef]

J. X. Cheng, L. D. Book, and X. S. Xie, "Polarization coherent anti-Stokes Raman scattering microscopy," Opt. Lett. 26, 1341-1343 (2001).
[CrossRef]

1999 (1)

A. Zumbusch, G. R. Holtom, and X. S. Xie, "Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering," Phys. Rev. Lett. 82, 4142-4145 (1999).
[CrossRef]

1995 (1)

A. Morresi, L. Mariani, M. R. Distefano, and M. G. Giorgini, "Vibrational-Relaxation Processes in Isotropic Molecular Liquids - A Critical Comparison," J. Raman Spectrosc. 26, 179-216 (1995).
[CrossRef]

Alexandrou, A.

Beaurepaire, E.

Bonn, M.

H. A. Rinia, M. Bonn, and M. Muller, "Quantitative multiplex CARS spectroscopy in congested spectral regions," J. Phys. Chem. B 110, 4472-4479 (2006).
[CrossRef] [PubMed]

Book, L. D.

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "Multiplex coherent anti-stokes Raman scattering microspectroscopy and study of lipid vesicles," J. Phys. Chem. B 106, 8493-8498 (2002).
[CrossRef]

A. Volkmer, L. D. Book, and X. S. Xie, "Time-resolved coherent anti-Stokes Raman scattering microscopy: Imaging based on Raman free induction decay," Appl. Phys. Lett. 80, 1505-1507 (2002).
[CrossRef]

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "An epi-detected coherent anti-stokes raman scattering (E-CARS) microscope with high spectral resolution and high sensitivity," J. Phys. Chem. B 105, 1277-1280 (2001).
[CrossRef]

J. X. Cheng, L. D. Book, and X. S. Xie, "Polarization coherent anti-Stokes Raman scattering microscopy," Opt. Lett. 26, 1341-1343 (2001).
[CrossRef]

Chen, B. C.

B. C. Chen and S. H. Lim, "Optimal laser pulse shaping for interferometric multiplex coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 112, 3653-3661 (2008).
[CrossRef] [PubMed]

Cheng, J. X.

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "Multiplex coherent anti-stokes Raman scattering microspectroscopy and study of lipid vesicles," J. Phys. Chem. B 106, 8493-8498 (2002).
[CrossRef]

J. X. Cheng, L. D. Book, and X. S. Xie, "Polarization coherent anti-Stokes Raman scattering microscopy," Opt. Lett. 26, 1341-1343 (2001).
[CrossRef]

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "An epi-detected coherent anti-stokes raman scattering (E-CARS) microscope with high spectral resolution and high sensitivity," J. Phys. Chem. B 105, 1277-1280 (2001).
[CrossRef]

Cicerone, M. T.

Coen, S.

J. M. Dudley, G. Genty, and S. Coen, "Supercontinuum generation in photonic crystal fiber," Rev. Mod. Phys. 78, 1135-1184 (2006).
[CrossRef]

Cote, D.

C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
[CrossRef] [PubMed]

Distefano, M. R.

A. Morresi, L. Mariani, M. R. Distefano, and M. G. Giorgini, "Vibrational-Relaxation Processes in Isotropic Molecular Liquids - A Critical Comparison," J. Raman Spectrosc. 26, 179-216 (1995).
[CrossRef]

Dudley, J. M.

J. M. Dudley, G. Genty, and S. Coen, "Supercontinuum generation in photonic crystal fiber," Rev. Mod. Phys. 78, 1135-1184 (2006).
[CrossRef]

Dudovich, N.

D. Oron, N. Dudovich, and Y. Silberberg, "Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 90, 213902 (2003).
[CrossRef] [PubMed]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Narrow-band coherent anti-stokes Raman signals from broad-band pulses," Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

Evans, C. L.

Ganikhanov, F.

Genty, G.

J. M. Dudley, G. Genty, and S. Coen, "Supercontinuum generation in photonic crystal fiber," Rev. Mod. Phys. 78, 1135-1184 (2006).
[CrossRef]

Giorgini, M. G.

A. Morresi, L. Mariani, M. R. Distefano, and M. G. Giorgini, "Vibrational-Relaxation Processes in Isotropic Molecular Liquids - A Critical Comparison," J. Raman Spectrosc. 26, 179-216 (1995).
[CrossRef]

Hamaguchi, H.

H. Kano and H. Hamaguchi, "Dispersion-compensated supercontinuum generation for ultrabroadband multiplex coherent anti-Stokes Raman scattering spectroscopy," J. Raman Spectrosc. 37, 411-415 (2006).
[CrossRef]

Holtom, G. R.

A. Zumbusch, G. R. Holtom, and X. S. Xie, "Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering," Phys. Rev. Lett. 82, 4142-4145 (1999).
[CrossRef]

Joffre, M.

Jurna, M.

Kano, H.

H. Kano and H. Hamaguchi, "Dispersion-compensated supercontinuum generation for ultrabroadband multiplex coherent anti-Stokes Raman scattering spectroscopy," J. Raman Spectrosc. 37, 411-415 (2006).
[CrossRef]

Kee, T. W.

Korterik, J. P.

Lee, Y. J.

Y. J. Lee and M. T. Cicerone, "Vibrational dephasing time imaging by time-resolved broadband coherent anti-Stokes Raman scattering microscopy," Appl. Phys. Lett. 92, 041108 (2008).
[CrossRef]

Y. J. Lee, Y Liu, and M. T. Cicerone, "Characterization of 3-color CARS in a 2-pulse broadband CARS spectrum," Opt. Lett. 32, 3370-3372 (2007).
[CrossRef] [PubMed]

Lim, S. H.

B. C. Chen and S. H. Lim, "Optimal laser pulse shaping for interferometric multiplex coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 112, 3653-3661 (2008).
[CrossRef] [PubMed]

Lin, C. P.

C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
[CrossRef] [PubMed]

Liu, Y

Mariani, L.

A. Morresi, L. Mariani, M. R. Distefano, and M. G. Giorgini, "Vibrational-Relaxation Processes in Isotropic Molecular Liquids - A Critical Comparison," J. Raman Spectrosc. 26, 179-216 (1995).
[CrossRef]

Meyer, L.

B. von Vacano, L. Meyer, and M. Motzkus, "Rapid polymer blend imaging with quantitative broadband multiplex CARS microscopy," J. Raman Spectrosc. 38, 916-926 (2007).
[CrossRef]

Morresi, A.

A. Morresi, L. Mariani, M. R. Distefano, and M. G. Giorgini, "Vibrational-Relaxation Processes in Isotropic Molecular Liquids - A Critical Comparison," J. Raman Spectrosc. 26, 179-216 (1995).
[CrossRef]

Motzkus, M.

B. von Vacano, L. Meyer, and M. Motzkus, "Rapid polymer blend imaging with quantitative broadband multiplex CARS microscopy," J. Raman Spectrosc. 38, 916-926 (2007).
[CrossRef]

Muller, M.

H. A. Rinia, M. Bonn, and M. Muller, "Quantitative multiplex CARS spectroscopy in congested spectral regions," J. Phys. Chem. B 110, 4472-4479 (2006).
[CrossRef] [PubMed]

Offerhaus, H. L.

Ogilvie, J. P.

Oron, D.

D. Oron, N. Dudovich, and Y. Silberberg, "Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 90, 213902 (2003).
[CrossRef] [PubMed]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Narrow-band coherent anti-stokes Raman signals from broad-band pulses," Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

Otto, C.

Petrov, G. I.

Potma, E. O.

Puoris'haag, M.

C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
[CrossRef] [PubMed]

Rinia, H. A.

H. A. Rinia, M. Bonn, and M. Muller, "Quantitative multiplex CARS spectroscopy in congested spectral regions," J. Phys. Chem. B 110, 4472-4479 (2006).
[CrossRef] [PubMed]

Saar, B. G.

Silberberg, Y.

D. Oron, N. Dudovich, and Y. Silberberg, "Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 90, 213902 (2003).
[CrossRef] [PubMed]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Narrow-band coherent anti-stokes Raman signals from broad-band pulses," Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

Volkmer, A.

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "Multiplex coherent anti-stokes Raman scattering microspectroscopy and study of lipid vesicles," J. Phys. Chem. B 106, 8493-8498 (2002).
[CrossRef]

A. Volkmer, L. D. Book, and X. S. Xie, "Time-resolved coherent anti-Stokes Raman scattering microscopy: Imaging based on Raman free induction decay," Appl. Phys. Lett. 80, 1505-1507 (2002).
[CrossRef]

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "An epi-detected coherent anti-stokes raman scattering (E-CARS) microscope with high spectral resolution and high sensitivity," J. Phys. Chem. B 105, 1277-1280 (2001).
[CrossRef]

von Vacano, B.

B. von Vacano, L. Meyer, and M. Motzkus, "Rapid polymer blend imaging with quantitative broadband multiplex CARS microscopy," J. Raman Spectrosc. 38, 916-926 (2007).
[CrossRef]

Xie, X. S.

F. Ganikhanov, C. L. Evans, B. G. Saar, and X. S. Xie, "High-sensitivity vibrational imaging with frequency modulation coherent anti-Stokes Raman scattering (FM CARS) microscopy," Opt. Lett. 31, 1872-1874 (2006).
[CrossRef] [PubMed]

E. O. Potma, C. L. Evans, and X. S. Xie, "Heterodyne coherent anti-Stokes Raman scattering (CARS) imaging," Opt. Lett. 31, 241-243 (2006).
[CrossRef] [PubMed]

C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
[CrossRef] [PubMed]

A. Volkmer, L. D. Book, and X. S. Xie, "Time-resolved coherent anti-Stokes Raman scattering microscopy: Imaging based on Raman free induction decay," Appl. Phys. Lett. 80, 1505-1507 (2002).
[CrossRef]

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "Multiplex coherent anti-stokes Raman scattering microspectroscopy and study of lipid vesicles," J. Phys. Chem. B 106, 8493-8498 (2002).
[CrossRef]

J. X. Cheng, L. D. Book, and X. S. Xie, "Polarization coherent anti-Stokes Raman scattering microscopy," Opt. Lett. 26, 1341-1343 (2001).
[CrossRef]

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "An epi-detected coherent anti-stokes raman scattering (E-CARS) microscope with high spectral resolution and high sensitivity," J. Phys. Chem. B 105, 1277-1280 (2001).
[CrossRef]

A. Zumbusch, G. R. Holtom, and X. S. Xie, "Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering," Phys. Rev. Lett. 82, 4142-4145 (1999).
[CrossRef]

Xie, X. S. N.

Yakovlev, V. V.

Yelin, D.

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Narrow-band coherent anti-stokes Raman signals from broad-band pulses," Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

Zhao, H. X.

Zumbusch, A.

A. Zumbusch, G. R. Holtom, and X. S. Xie, "Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering," Phys. Rev. Lett. 82, 4142-4145 (1999).
[CrossRef]

Appl. Phys. Lett. (2)

Y. J. Lee and M. T. Cicerone, "Vibrational dephasing time imaging by time-resolved broadband coherent anti-Stokes Raman scattering microscopy," Appl. Phys. Lett. 92, 041108 (2008).
[CrossRef]

A. Volkmer, L. D. Book, and X. S. Xie, "Time-resolved coherent anti-Stokes Raman scattering microscopy: Imaging based on Raman free induction decay," Appl. Phys. Lett. 80, 1505-1507 (2002).
[CrossRef]

J. Phys. Chem. B (4)

B. C. Chen and S. H. Lim, "Optimal laser pulse shaping for interferometric multiplex coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 112, 3653-3661 (2008).
[CrossRef] [PubMed]

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "Multiplex coherent anti-stokes Raman scattering microspectroscopy and study of lipid vesicles," J. Phys. Chem. B 106, 8493-8498 (2002).
[CrossRef]

H. A. Rinia, M. Bonn, and M. Muller, "Quantitative multiplex CARS spectroscopy in congested spectral regions," J. Phys. Chem. B 110, 4472-4479 (2006).
[CrossRef] [PubMed]

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, "An epi-detected coherent anti-stokes raman scattering (E-CARS) microscope with high spectral resolution and high sensitivity," J. Phys. Chem. B 105, 1277-1280 (2001).
[CrossRef]

J. Raman Spectrosc. (3)

H. Kano and H. Hamaguchi, "Dispersion-compensated supercontinuum generation for ultrabroadband multiplex coherent anti-Stokes Raman scattering spectroscopy," J. Raman Spectrosc. 37, 411-415 (2006).
[CrossRef]

A. Morresi, L. Mariani, M. R. Distefano, and M. G. Giorgini, "Vibrational-Relaxation Processes in Isotropic Molecular Liquids - A Critical Comparison," J. Raman Spectrosc. 26, 179-216 (1995).
[CrossRef]

B. von Vacano, L. Meyer, and M. Motzkus, "Rapid polymer blend imaging with quantitative broadband multiplex CARS microscopy," J. Raman Spectrosc. 38, 916-926 (2007).
[CrossRef]

Opt. Express (3)

Opt. Lett. (7)

Phys. Rev. Lett. (3)

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Narrow-band coherent anti-stokes Raman signals from broad-band pulses," Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

A. Zumbusch, G. R. Holtom, and X. S. Xie, "Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering," Phys. Rev. Lett. 82, 4142-4145 (1999).
[CrossRef]

D. Oron, N. Dudovich, and Y. Silberberg, "Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 90, 213902 (2003).
[CrossRef] [PubMed]

Proc. Natl. Acad. Sci. USA (1)

C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
[CrossRef] [PubMed]

Rev. Mod. Phys. (1)

J. M. Dudley, G. Genty, and S. Coen, "Supercontinuum generation in photonic crystal fiber," Rev. Mod. Phys. 78, 1135-1184 (2006).
[CrossRef]

Other (2)

G. L. Eesley, Coherent Raman Spectroscopy (Pergamon Press, Oxford 1981).

Certain equipment is identified in this Letter to specify adequately the experimental details. Such identification does not imply recommendation by the National Institute of Standards and Technology, nor does it imply that the equipment is necessarily the best available for this purpose.

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Figures (7)

Fig. 1.
Fig. 1.

(a) Schematic diagrams of 2- and 3-color CARS generation mechanisms in two-pulse broadband CARS spectroscopy. ωnarr and ωcont represent photons from narrowband and continuum pulses respectively. CARS spectra are simulated via (b) 2-color and (c) 3-color mechanisms. The dashed lines indicate NRB contribution. See the text for the simulation parameters.

Fig. 2.
Fig. 2.

(a) The electric fields E ps(ω) and E fs(ω) used in the ps-fs scheme, where Δω ps = 5 cm-1 and Δω fs = 50 cm-1, respectively. NRB intensity is calculated as a function of (b) Δϕ and (c) E 0 fs/E 0 ps. The inset of Fig. 2(c) shows the symmetry in NRB amplitude around the region of E 0 fs/E 0 ps=0.1.

Fig. 3.
Fig. 3.

(a) NRB suppressed 3-color CARS spectra in the ps-fs scheme for two Δω fs values of 50 cm-1 (blue) and 500 cm-1 (red) when Δω ps = 5 cm-1. The dotted line is the 3-color CARS spectrum calculated only with resonant signal [χNR (3) = 0] generated with a single ps pulse. (b) Semi-log plot of calculated peak intensity of the Raman mode at 1000 cm-1 as a function of Δω fs while Δϕ=π and E 0 fs/E 0 ps = Δω psω fs.

Fig. 4.
Fig. 4.

(a) Electric field amplitudes E ps1(ω) and E ps2(ω) used in the ps-ps scheme, where Δω ps = 5 cm-1. (b) Simulated 3-color CARS spectra for various Δω c. As a reference (the dotted line), a 3-color CARS spectrum is calculated for χNR (3) = 0 by a single ps pulse for E n(ω) when the pulse energy is assumed to be equal to the sum of those of E ps1(ω) and E ps2(ω) for the other ps-ps simulations.

Fig. 5.
Fig. 5.

(a) and (b), electric field amplitudes of probe pulses in the frequency domain for the ps-fs and the ps-ps schemes, respectively. (c) and (d), electric field amplitudes for probe and broadband pulses under NRB suppression conditions in the time domain for the ps-fs and the ps-ps schemes, respectively. The red lines in (c) and (d) represent resonant vibrational population decay, corresponding to Γ= 10 cm-1. For the ps-fs scheme, Δω ps = 5 cm-1 and Δω fs = 50 cm-1. For the ps-ps scheme, Δω ps = 5 cm-1 and Δω c = 20 cm-1. In the panel (d), the time-domain electric field amplitudes in the ps-ps scheme are compared between Δω c = 20 cm-1 (black solid line) and Δω c = 5 cm-1 (green dashed line). The latter is similar to the time-domain electric field amplitude of a single (frequency-domain) Gaussian probe pulse with a π phase step at the center frequency for Δω ps = 10 cm-1 (blue dashed line).

Fig. 6.
Fig. 6.

(a) The original single narrowband pulse (dotted line) is decomposed into two Gaussian pulses with Δω ps = 10 cm-1 and Δω fs = 97 cm-1 for the ps-fs scheme (red and blue respectively). (b) and (c) - Measured broadband CARS spectra of benzonitrile at Δϕ = 0 and Δϕ = π respectively. The laser power of the narrowband and the continuum pulse are 5.8 mW and 2.4 mW at the sample position. The CCD exposure time is 50 ms. Uncertainty in the wavelength calibration is ± 2 cm-1.

Fig. 7.
Fig. 7.

(a) The measured spectrum of the narrowband pulse for the ps-ps scheme. Fitting the spectrum leads to two Gaussian pulses with ΔΩ ps of 11 cm-1 and ΔΩ c of 13 cm-1. Measured broadband CARS spectra of c-hexane as a result of (b) in-phase and (c) out-of-phase interference between the two ps pulses. The vertical lines in the lower plot indicate spontaneous Raman resonant frequencies. The laser powers of the narrowband pulse and the continuum pulse are 7 mW and 6 mW at the sample position.

Equations (18)

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P(3)(ωaS)=χ(3)(ωp,ωS,ωpr;ωaS)E(ωp)E*(ωS)E(ωpr)
×δ(ωpωS+ωprωaS)dωpdωSdωpr
P2color(3)(ωaS)=χ(3)En(ωp)Ec*(ωp+ωprωaS)En(ωpr)dωpdωpr
P3color(3)(ωaS)=χ(3)Ec(ωp)Ec*(ωp+ωprωaS)En(ωpr)dωpdωpr
χ(3)(ωp,ωS)=χNR(3)+χR(3)(ωp,ωS)=χNR(3)+iAi[(ωpωS)ΩR,i]+iΓi
χ(3)(ωaS,ωpr)=χNR(3)+iAi[(ωaSωpr)ΩR,i]+iΓi
P2color(3)(ωaS)=En(ωp)Ec*(ωp+ωprωaS)dωpχ(3)(ωaS,ωpr)En(ωpr)dωpr
P3color(3)(ωaS)=Ec(ωp)Ec*(ωp+ωprωaS)dωpχ(3)(ωaS,ωpr)En(ωpr)dωpr
En(ω)=Eps(ω)eiΔϕ+Efs(ω)
Ipsfs2color(ωaS,Δϕ)[Eps(ωp)eiΔϕ+Efs(ωp)]Ec*(ωp+ωprωaS)dωp
×χ(3)(ωaS,ωpr)[Eps(ωpr)eiΔϕ+Efs(ωpr)]dωpr2
Ipsfs3color(ωaS,Δϕ)Ec(ωp)Ec*(ωp+ωprωaS)dωp
×χ(3)(ωaS,ωpr)[Eps(ωpr)eiΔϕ+Efs(ωpr)]dωpr2
En(ω)=Epsl(ω)eiΔφ+Eps2(ω)
Ipsps2color(ωaS,Δϕ)[Eps1(ωp)eiΔϕ+Eps2(ωp)]Ec*(ωp+ωprωaS)dωp
×χ(3)(ωaS,ωpr)[Eps1(ωpr)eiΔϕ+Eps2(ωpr)]dωpr2
Ipsps3color(ωaS,Δϕ)Ec(ωp)Ec(ωp+ωprωaS)*dωp
×χ(3)(ωaS,ωpr)[Eps1(ωpr)eiΔϕ+Eps2(ωpr)]dωpr2

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