Abstract

We introduce an interferometric technique for eliminating the non-resonant background of broadband coherent anti-Stokes Raman scattering (CARS) microscopy. CARS microscopy has been used for imaging a number of biological samples and processes, but the studies are mostly limited to detecting lipids in biological systems by probing the C-H stretch. Non-resonant background and incoherent noise sources can easily overwhelm less intense signals from other molecular vibrations. In this study, we demonstrate a one-laser broadband interferometric technique that separates the spontaneous Raman scattering-related component of the CARS signal from the non-resonant background using liquid benzonitrile as a model system.

© 2006 Optical Society of America

Full Article  |  PDF Article

References

  • View by:
  • |
  • |
  • |

  1. M. D. Duncan, J. Reintjes, and T. J. Manuccia, "Scanning coherent anti-Stokes Raman microscope," Opt. Lett. 7,350-352 (1982).
    [CrossRef] [PubMed]
  2. J. X. Cheng and X. S. Xie, "Coherent anti-Stokes Raman scattering microscopy: Instrumentation, theory, and applications," J. Phys. Chem. B 108,827-840 (2004).
    [CrossRef]
  3. 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]
  4. M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," PNAS 99, 10994-11001 (2002).
    [CrossRef] [PubMed]
  5. S. A. Schaertel, A. C. Albrecht, A. Lau, and A. Kummrow, "Interferometric coherent Raman-spectroscopy with incoherent-light - some applications," Appl. Phys. B: Lasers Opt. 59,377-387 (1994).
    [CrossRef]
  6. J. X. Cheng, Y. K. Jia, G. F. Zheng, and X. S. Xie, "Laser-scanning coherent anti-Stokes Raman scattering microscopy and applications to cell biology," Biophys. J. 83,502-509 (2002).
    [CrossRef] [PubMed]
  7. H. F. Wang, Y. Fu, P. Zickmund, R. Y. Shi, and J. X. Cheng, "Coherent anti-Stokes Raman scattering imaging of axonal myelin in live spinal tissues," Biophys. J. 89,581-591 (2005).
    [CrossRef] [PubMed]
  8. E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108,1296-1301 (2004).
    [CrossRef]
  9. 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]
  10. K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, "High spectral resolution multiplex CARS spectroscopy using chirped pulses," Chem. Phys. Lett. 387,436-441 (2004).
    [CrossRef]
  11. M. Muller and J. M. Schins, "Imaging the thermodynamic state of lipid membranes with multiplex CARS microscopy," J. Phys. Chem. B 106,3715-3723 (2002).
    [CrossRef]
  12. H. Kano and H. Hamaguchi, "Femtosecond coherent anti-Stokes Raman scattering spectroscopy using supercontinuum generated from a photonic crystal fiber," Appl. Phys. Lett. 85,4298-4300 (2004).
    [CrossRef]
  13. 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]
  14. 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]
  15. J. L. Oudar, R. W. Smith, and Y. R. Shen, "Polarization-sensitive coherent anti-Stokes Raman-spectroscopy," Appl. Phys. Lett. 34,758-760 (1979).
    [CrossRef]
  16. 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]
  17. 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]
  18. Y. Yacoby, R. Fitzgibbon, and B. Lax, "Coherent cancellation of background in 4-wave mixing spectroscopy," J. Appl. Phys. 51,3072-3077 (1980).
    [CrossRef]
  19. 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," PNAS 102,16807-16812 (2005).
    [CrossRef] [PubMed]
  20. 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]
  21. D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Quantum control of coherent anti-Stokes Raman processes," Phys. Rev. A65, (2002).
    [CrossRef]
  22. S. H. Lim, A. G. Caster, and S. R. Leone, "Single-pulse phase-control interferometric coherent anti-Stokes Raman scattering spectroscopy," Phys. Rev. A 72, (2005).
    [CrossRef]
  23. D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, "Interferometric differentiation between resonant coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85,5787-5789 (2004). http://www.chemistry.ohio-state.edu/~rmccreer/freqcorr/images/benzo.html.
    [CrossRef]
  24. Certain equipment, instruments or materials are identified in this paper in order to adequately specify the experimental details. Such identification does not imply recommendation by the National Institute of Standards and Technology nor does it imply the materials are necessarily the best available for the purpose.

2006 (1)

2005 (4)

S. H. Lim, A. G. Caster, and S. R. Leone, "Single-pulse phase-control interferometric coherent anti-Stokes Raman scattering spectroscopy," Phys. Rev. A 72, (2005).
[CrossRef]

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," PNAS 102,16807-16812 (2005).
[CrossRef] [PubMed]

H. F. Wang, Y. Fu, P. Zickmund, R. Y. Shi, and J. X. Cheng, "Coherent anti-Stokes Raman scattering imaging of axonal myelin in live spinal tissues," Biophys. J. 89,581-591 (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 (6)

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, "High spectral resolution multiplex CARS spectroscopy using chirped pulses," Chem. Phys. Lett. 387,436-441 (2004).
[CrossRef]

H. Kano and H. Hamaguchi, "Femtosecond coherent anti-Stokes Raman scattering spectroscopy using supercontinuum generated from a photonic crystal fiber," Appl. Phys. Lett. 85,4298-4300 (2004).
[CrossRef]

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]

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108,1296-1301 (2004).
[CrossRef]

J. X. Cheng and X. S. Xie, "Coherent anti-Stokes Raman scattering microscopy: Instrumentation, theory, and applications," J. Phys. Chem. B 108,827-840 (2004).
[CrossRef]

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, "Interferometric differentiation between resonant coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85,5787-5789 (2004). http://www.chemistry.ohio-state.edu/~rmccreer/freqcorr/images/benzo.html.
[CrossRef]

2002 (6)

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Quantum control of coherent anti-Stokes Raman processes," Phys. Rev. A65, (2002).
[CrossRef]

M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," PNAS 99, 10994-11001 (2002).
[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]

J. X. Cheng, Y. K. Jia, G. F. Zheng, and X. S. Xie, "Laser-scanning coherent anti-Stokes Raman scattering microscopy and applications to cell biology," Biophys. J. 83,502-509 (2002).
[CrossRef] [PubMed]

M. Muller and J. M. Schins, "Imaging the thermodynamic state of lipid membranes with multiplex CARS microscopy," J. Phys. Chem. B 106,3715-3723 (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]

2001 (1)

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]

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]

1994 (1)

S. A. Schaertel, A. C. Albrecht, A. Lau, and A. Kummrow, "Interferometric coherent Raman-spectroscopy with incoherent-light - some applications," Appl. Phys. B: Lasers Opt. 59,377-387 (1994).
[CrossRef]

1982 (1)

1980 (1)

Y. Yacoby, R. Fitzgibbon, and B. Lax, "Coherent cancellation of background in 4-wave mixing spectroscopy," J. Appl. Phys. 51,3072-3077 (1980).
[CrossRef]

1979 (1)

J. L. Oudar, R. W. Smith, and Y. R. Shen, "Polarization-sensitive coherent anti-Stokes Raman-spectroscopy," Appl. Phys. Lett. 34,758-760 (1979).
[CrossRef]

Albrecht, A. C.

S. A. Schaertel, A. C. Albrecht, A. Lau, and A. Kummrow, "Interferometric coherent Raman-spectroscopy with incoherent-light - some applications," Appl. Phys. B: Lasers Opt. 59,377-387 (1994).
[CrossRef]

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]

Boppart, S. A.

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, "Interferometric differentiation between resonant coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85,5787-5789 (2004). http://www.chemistry.ohio-state.edu/~rmccreer/freqcorr/images/benzo.html.
[CrossRef]

Bredfeldt, J. S.

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, "Interferometric differentiation between resonant coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85,5787-5789 (2004). http://www.chemistry.ohio-state.edu/~rmccreer/freqcorr/images/benzo.html.
[CrossRef]

Caster, A. G.

S. H. Lim, A. G. Caster, and S. R. Leone, "Single-pulse phase-control interferometric coherent anti-Stokes Raman scattering spectroscopy," Phys. Rev. A 72, (2005).
[CrossRef]

Cheng, J. X.

H. F. Wang, Y. Fu, P. Zickmund, R. Y. Shi, and J. X. Cheng, "Coherent anti-Stokes Raman scattering imaging of axonal myelin in live spinal tissues," Biophys. J. 89,581-591 (2005).
[CrossRef] [PubMed]

J. X. Cheng and X. S. Xie, "Coherent anti-Stokes Raman scattering microscopy: Instrumentation, theory, and applications," J. Phys. Chem. B 108,827-840 (2004).
[CrossRef]

J. X. Cheng, Y. K. Jia, G. F. Zheng, and X. S. Xie, "Laser-scanning coherent anti-Stokes Raman scattering microscopy and applications to cell biology," Biophys. J. 83,502-509 (2002).
[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]

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.

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," PNAS 102,16807-16812 (2005).
[CrossRef] [PubMed]

Dudovich, N.

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Quantum control of coherent anti-Stokes Raman processes," Phys. Rev. A65, (2002).
[CrossRef]

Duncan, M. D.

Evans, C. L.

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," PNAS 102,16807-16812 (2005).
[CrossRef] [PubMed]

Fitzgibbon, R.

Y. Yacoby, R. Fitzgibbon, and B. Lax, "Coherent cancellation of background in 4-wave mixing spectroscopy," J. Appl. Phys. 51,3072-3077 (1980).
[CrossRef]

Fu, Y.

H. F. Wang, Y. Fu, P. Zickmund, R. Y. Shi, and J. X. Cheng, "Coherent anti-Stokes Raman scattering imaging of axonal myelin in live spinal tissues," Biophys. J. 89,581-591 (2005).
[CrossRef] [PubMed]

Hamaguchi, H.

H. Kano and H. Hamaguchi, "Femtosecond coherent anti-Stokes Raman scattering spectroscopy using supercontinuum generated from a photonic crystal fiber," Appl. Phys. Lett. 85,4298-4300 (2004).
[CrossRef]

Hinsberg, W. D.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108,1296-1301 (2004).
[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]

Jia, Y. K.

J. X. Cheng, Y. K. Jia, G. F. Zheng, and X. S. Xie, "Laser-scanning coherent anti-Stokes Raman scattering microscopy and applications to cell biology," Biophys. J. 83,502-509 (2002).
[CrossRef] [PubMed]

Johnson, J. C.

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, "High spectral resolution multiplex CARS spectroscopy using chirped pulses," Chem. Phys. Lett. 387,436-441 (2004).
[CrossRef]

Jones, D.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108,1296-1301 (2004).
[CrossRef]

Kano, H.

H. Kano and H. Hamaguchi, "Femtosecond coherent anti-Stokes Raman scattering spectroscopy using supercontinuum generated from a photonic crystal fiber," Appl. Phys. Lett. 85,4298-4300 (2004).
[CrossRef]

Kattawar, G. W.

M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," PNAS 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Kee, T. W.

Knutsen, K. P.

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, "High spectral resolution multiplex CARS spectroscopy using chirped pulses," Chem. Phys. Lett. 387,436-441 (2004).
[CrossRef]

Kummrow, A.

S. A. Schaertel, A. C. Albrecht, A. Lau, and A. Kummrow, "Interferometric coherent Raman-spectroscopy with incoherent-light - some applications," Appl. Phys. B: Lasers Opt. 59,377-387 (1994).
[CrossRef]

Lau, A.

S. A. Schaertel, A. C. Albrecht, A. Lau, and A. Kummrow, "Interferometric coherent Raman-spectroscopy with incoherent-light - some applications," Appl. Phys. B: Lasers Opt. 59,377-387 (1994).
[CrossRef]

Lax, B.

Y. Yacoby, R. Fitzgibbon, and B. Lax, "Coherent cancellation of background in 4-wave mixing spectroscopy," J. Appl. Phys. 51,3072-3077 (1980).
[CrossRef]

Leone, S. R.

S. H. Lim, A. G. Caster, and S. R. Leone, "Single-pulse phase-control interferometric coherent anti-Stokes Raman scattering spectroscopy," Phys. Rev. A 72, (2005).
[CrossRef]

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108,1296-1301 (2004).
[CrossRef]

Lim, S. H.

S. H. Lim, A. G. Caster, and S. R. Leone, "Single-pulse phase-control interferometric coherent anti-Stokes Raman scattering spectroscopy," Phys. Rev. A 72, (2005).
[CrossRef]

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," PNAS 102,16807-16812 (2005).
[CrossRef] [PubMed]

Lucht, R. P.

M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," PNAS 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Manuccia, T. J.

Marks, D. L.

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, "Interferometric differentiation between resonant coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85,5787-5789 (2004). http://www.chemistry.ohio-state.edu/~rmccreer/freqcorr/images/benzo.html.
[CrossRef]

Miller, A. E.

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, "High spectral resolution multiplex CARS spectroscopy using chirped pulses," Chem. Phys. Lett. 387,436-441 (2004).
[CrossRef]

Muller, M.

M. Muller and J. M. Schins, "Imaging the thermodynamic state of lipid membranes with multiplex CARS microscopy," J. Phys. Chem. B 106,3715-3723 (2002).
[CrossRef]

Muntean, L.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108,1296-1301 (2004).
[CrossRef]

Opatrny, T.

M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," PNAS 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Oron, D.

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Quantum control of coherent anti-Stokes Raman processes," Phys. Rev. A65, (2002).
[CrossRef]

Oudar, J. L.

J. L. Oudar, R. W. Smith, and Y. R. Shen, "Polarization-sensitive coherent anti-Stokes Raman-spectroscopy," Appl. Phys. Lett. 34,758-760 (1979).
[CrossRef]

Petersen, P. B.

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, "High spectral resolution multiplex CARS spectroscopy using chirped pulses," Chem. Phys. Lett. 387,436-441 (2004).
[CrossRef]

Petrov, G. I.

Pilloff, H.

M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," PNAS 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Potma, E. O.

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," PNAS 102,16807-16812 (2005).
[CrossRef] [PubMed]

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108,1296-1301 (2004).
[CrossRef]

Preusser, J.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108,1296-1301 (2004).
[CrossRef]

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," PNAS 102,16807-16812 (2005).
[CrossRef] [PubMed]

Rebane, A.

M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," PNAS 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Reintjes, J.

Saykally, R. J.

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, "High spectral resolution multiplex CARS spectroscopy using chirped pulses," Chem. Phys. Lett. 387,436-441 (2004).
[CrossRef]

Schade, W.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108,1296-1301 (2004).
[CrossRef]

Schaertel, S. A.

S. A. Schaertel, A. C. Albrecht, A. Lau, and A. Kummrow, "Interferometric coherent Raman-spectroscopy with incoherent-light - some applications," Appl. Phys. B: Lasers Opt. 59,377-387 (1994).
[CrossRef]

Schins, J. M.

M. Muller and J. M. Schins, "Imaging the thermodynamic state of lipid membranes with multiplex CARS microscopy," J. Phys. Chem. B 106,3715-3723 (2002).
[CrossRef]

Scully, M. O.

M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," PNAS 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Shen, Y. R.

J. L. Oudar, R. W. Smith, and Y. R. Shen, "Polarization-sensitive coherent anti-Stokes Raman-spectroscopy," Appl. Phys. Lett. 34,758-760 (1979).
[CrossRef]

Shi, R. Y.

H. F. Wang, Y. Fu, P. Zickmund, R. Y. Shi, and J. X. Cheng, "Coherent anti-Stokes Raman scattering imaging of axonal myelin in live spinal tissues," Biophys. J. 89,581-591 (2005).
[CrossRef] [PubMed]

Silberberg, Y.

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Quantum control of coherent anti-Stokes Raman processes," Phys. Rev. A65, (2002).
[CrossRef]

Smith, R. W.

J. L. Oudar, R. W. Smith, and Y. R. Shen, "Polarization-sensitive coherent anti-Stokes Raman-spectroscopy," Appl. Phys. Lett. 34,758-760 (1979).
[CrossRef]

Sokolov, A. V.

M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," PNAS 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Vinegoni, C.

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, "Interferometric differentiation between resonant coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85,5787-5789 (2004). http://www.chemistry.ohio-state.edu/~rmccreer/freqcorr/images/benzo.html.
[CrossRef]

Volkmer, A.

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, 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]

Wang, H. F.

H. F. Wang, Y. Fu, P. Zickmund, R. Y. Shi, and J. X. Cheng, "Coherent anti-Stokes Raman scattering imaging of axonal myelin in live spinal tissues," Biophys. J. 89,581-591 (2005).
[CrossRef] [PubMed]

Xie, X. S.

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," PNAS 102,16807-16812 (2005).
[CrossRef] [PubMed]

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108,1296-1301 (2004).
[CrossRef]

J. X. Cheng and X. S. Xie, "Coherent anti-Stokes Raman scattering microscopy: Instrumentation, theory, and applications," J. Phys. Chem. B 108,827-840 (2004).
[CrossRef]

J. X. Cheng, Y. K. Jia, G. F. Zheng, and X. S. Xie, "Laser-scanning coherent anti-Stokes Raman scattering microscopy and applications to cell biology," Biophys. J. 83,502-509 (2002).
[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, 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]

Yacoby, Y.

Y. Yacoby, R. Fitzgibbon, and B. Lax, "Coherent cancellation of background in 4-wave mixing spectroscopy," J. Appl. Phys. 51,3072-3077 (1980).
[CrossRef]

Yakovlev, V. V.

Ye, J.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108,1296-1301 (2004).
[CrossRef]

Yelin, D.

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Quantum control of coherent anti-Stokes Raman processes," Phys. Rev. A65, (2002).
[CrossRef]

Zheng, G. F.

J. X. Cheng, Y. K. Jia, G. F. Zheng, and X. S. Xie, "Laser-scanning coherent anti-Stokes Raman scattering microscopy and applications to cell biology," Biophys. J. 83,502-509 (2002).
[CrossRef] [PubMed]

Zickmund, P.

H. F. Wang, Y. Fu, P. Zickmund, R. Y. Shi, and J. X. Cheng, "Coherent anti-Stokes Raman scattering imaging of axonal myelin in live spinal tissues," Biophys. J. 89,581-591 (2005).
[CrossRef] [PubMed]

Zubairy, M. S.

M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," PNAS 99, 10994-11001 (2002).
[CrossRef] [PubMed]

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. B: Lasers Opt. (1)

S. A. Schaertel, A. C. Albrecht, A. Lau, and A. Kummrow, "Interferometric coherent Raman-spectroscopy with incoherent-light - some applications," Appl. Phys. B: Lasers Opt. 59,377-387 (1994).
[CrossRef]

Appl. Phys. Lett. (4)

H. Kano and H. Hamaguchi, "Femtosecond coherent anti-Stokes Raman scattering spectroscopy using supercontinuum generated from a photonic crystal fiber," Appl. Phys. Lett. 85,4298-4300 (2004).
[CrossRef]

J. L. Oudar, R. W. Smith, and Y. R. Shen, "Polarization-sensitive coherent anti-Stokes Raman-spectroscopy," Appl. Phys. Lett. 34,758-760 (1979).
[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]

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, "Interferometric differentiation between resonant coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85,5787-5789 (2004). http://www.chemistry.ohio-state.edu/~rmccreer/freqcorr/images/benzo.html.
[CrossRef]

Biophys. J. (2)

J. X. Cheng, Y. K. Jia, G. F. Zheng, and X. S. Xie, "Laser-scanning coherent anti-Stokes Raman scattering microscopy and applications to cell biology," Biophys. J. 83,502-509 (2002).
[CrossRef] [PubMed]

H. F. Wang, Y. Fu, P. Zickmund, R. Y. Shi, and J. X. Cheng, "Coherent anti-Stokes Raman scattering imaging of axonal myelin in live spinal tissues," Biophys. J. 89,581-591 (2005).
[CrossRef] [PubMed]

Chem. Phys. Lett. (1)

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, "High spectral resolution multiplex CARS spectroscopy using chirped pulses," Chem. Phys. Lett. 387,436-441 (2004).
[CrossRef]

J. Appl. Phys. (1)

Y. Yacoby, R. Fitzgibbon, and B. Lax, "Coherent cancellation of background in 4-wave mixing spectroscopy," J. Appl. Phys. 51,3072-3077 (1980).
[CrossRef]

J. Phys. Chem. B (5)

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]

M. Muller and J. M. Schins, "Imaging the thermodynamic state of lipid membranes with multiplex CARS microscopy," J. Phys. Chem. B 106,3715-3723 (2002).
[CrossRef]

J. X. Cheng and X. S. Xie, "Coherent anti-Stokes Raman scattering microscopy: Instrumentation, theory, and applications," J. Phys. Chem. B 108,827-840 (2004).
[CrossRef]

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108,1296-1301 (2004).
[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]

Opt. Express (1)

Opt. Lett. (3)

Phys. Rev. A (2)

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Quantum control of coherent anti-Stokes Raman processes," Phys. Rev. A65, (2002).
[CrossRef]

S. H. Lim, A. G. Caster, and S. R. Leone, "Single-pulse phase-control interferometric coherent anti-Stokes Raman scattering spectroscopy," Phys. Rev. A 72, (2005).
[CrossRef]

Phys. Rev. Lett. (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]

PNAS (2)

M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," PNAS 99, 10994-11001 (2002).
[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," PNAS 102,16807-16812 (2005).
[CrossRef] [PubMed]

Other (1)

Certain equipment, instruments or materials are identified in this paper in order to adequately specify the experimental details. Such identification does not imply recommendation by the National Institute of Standards and Technology nor does it imply the materials are necessarily the best available for the purpose.

Cited By

OSA participates in CrossRef's Cited-By Linking service. Citing articles from OSA journals and other participating publishers are listed here.

Alert me when this article is cited.


Figures (5)

Fig. 1.
Fig. 1.

Energy-level diagram for narrow-band CARS: solid vertical arrows; broadband CARS: solid and dashed vertical arrows. Symbols: ωp , pump; ωS Stokes; ωpr , probe; ωaS , anti-Stokes light. (b) Energy-level diagrams for a non-resonant process generating light at the same wavelength as is produced in the process depicted in (a).

Fig. 2.
Fig. 2.

Experimental configuration: BC, beamsplitter cube; DG, diffraction grating; PBC, polarizing beamsplitter cube; PZT, piezo-electric transducer; PCF, photonic crystal fiber; LP, long wave pass edge filter; Obj, microscope objective; SP, shortpass filter; Pol, polarizer. The inset spectra are (from top) the 750 fs, and 100 fs outputs of Mira 900, output of PCF, and polarization scheme of the input beams. The PCF feed light is arbitrarily scaled and superimposed on the PCF output spectrum.

Fig. 3.
Fig. 3.

Broadband CARS spectra of benzonitrile from each of the two arms of the interferometer. The spectra are generated by using (a) 100 fs pulses (spectral width 150 cm-1) and (b) 750 fs pulses (20 cm-1) as pump and probe.

Fig. 4.
Fig. 4.

(a) CARS interferograms of benzonitrile – at 3070 cm-1, (resonant, bold solid curve), 2500 cm-1, (non-resonant, dash) and the difference between the interferograms (thin solid). (b) Differential chirp between the local oscillator and signal as a function of wavenumbers, see text for details.

Fig. 5.
Fig. 5.

(a) Real and (b) imaginary components of χ (3) of benzonitrile determined by Fourier analysis of the ϕ 1 dependent interferometric signals (see text for details). The inset in (b) is the imaginary component of χ (3) determined from the interferometric signals oscillating at 2ϕ 1.

Equations (13)

Equations on this page are rendered with MathJax. Learn more.

P i ( 3 ) = j , k , l χ i , j , k , l ( 3 ) ( ω p + ω pr ω S ) : E p j ( ω p ) E pr k ( ω pr ) E S l ( ω S ) *
χ ( 3 ) = χ NR ( 3 ) + χ R ' ( 3 ) + R '' ( 3 )
E m x = E m x exp [ i ( ω m t + ϕ m ) ]
P i ( 3 ) = j , k , l χ i , j , k , l ( 3 ) ( ω p + ω pr ω S ) × E p j E pr k E S l exp ( i [ ( ω p + ω pr ω S ) t + ( ϕ p + ϕ pr ϕ S ) ]
P i ( 3 ) = p = 1 2 pr = 1 2 [ j , k , l χ i , j , k , l ( 3 ) ( ω aS ) E p j E pr k E 3 l exp [ i ( ω aS t + ϕ p + ϕ pr ) ] ]
I i ( ϕ 1 ) = 0 2 π [ C 1,1 NR cos ( t ' + 2 ϕ 1 ) C 1,2 NR cos ( t ' + ϕ 1 ) + C 2,1 NR cos ( t ' + ϕ 1 ) + C 2,2 NR cos ( t ' )
+ C 1,1 R ' cos ( t ' + 2 ϕ 1 ) C 1,2 R ' cos ( t ' + ϕ 1 ) + C 2,1 R ' cos ( t ' + ϕ 1 ) + C 2,2 R ' cos ( t ' )
+ C 1,1 R ' ' sin ( t ' + 2 ϕ 1 ) C 1,2 R ' ' sin ( t ' + ϕ 1 ) + C 2,1 R ' ' sin ( t ' + ϕ 1 ) + C 2,2 R ' ' sin ( t ' ) ] 2 dt '
I i ( ϕ 1 ) = 2 π cos ( ϕ 1 ) α = 1 2 β = 1 2 γ = 1 γ β 2 [ C α , α r ' ' C β , γ r ' ' + ( C α , α nr + C α , α r ' ) ( C β , γ nr + C β , γ r ' ) ]
+ 2 π sin ( ϕ 1 ) α = 1 2 β = 1 2 γ = 1 γ β 2 ( 1 ) α [ C α , α r ' ' + ( C β , γ nr + C β , γ r ' ) C β , γ r ' ' ( C α , α r ' + C α , α nr ) ]
+ 2 π cos ( 1 ) [ C 1 , 1 r ' ' C 2,2 ' ' ( C 1 , 1 nr + C 1 , 1 r ' ) ( C 2 , 2 nr + C 2 , 2 r ' ) ]
+ 2 π sin ( 1 ) [ C 1 , 1 r ' ' ( C 2 , 2 nr + C 2 , 2 r ' ) C 2,2 r ' ' ( C 1 , 1 nr + C 1 , 1 r ' ) ]
+ const .

Metrics