Abstract

We present an interferometric time-domain Fourier transform implementation of coherent anti-Stokes Raman scattering (CARS). Based on a single femtosecond laser source, the method provides a straight-forward scheme for obtaining high resolution CARS spectra. We give a theoretical description of the method, and demonstrate good agreement between simulation and experimental CARS spectra. We also discuss the method’s relation to other CARS approaches for microscopy and microspectroscopy applications.

© 2006 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. 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. 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]
  4. M. D. Duncan, J. Reintjes, and T. J. Manuccia, "Scanning coherent anti-Stokes Raman microscope," Opt. Lett. 7, 350-352(1982).
    [CrossRef] [PubMed]
  5. 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]
  6. J. X. Chen, 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]
  7. S. Roy, T. R. Meyer, and J. R. Gord, "Broadband coherent anti-Stokes Raman scattering spectroscopy of nitrogen using a picosecond modeless dye laser," Opt. Lett. 30, 3222-3224 (2005).
    [CrossRef] [PubMed]
  8. N. Dudovich, and D. Oron, Y. Silberberg, "Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy," Nature 418, 512-514 (2002).
    [CrossRef] [PubMed]
  9. N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherent anti-Stokes Raman spectroscopy in the fingerprint spectral region," J. Chem. Phys. 118, 9208-9215 (2003).
    [CrossRef]
  10. 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]
  11. Y. X. Yan, and K. A. Nelson, "Impulsive stimulated light-scattering. 2. Comparison to frequency-domain light-scattering spectroscopy," J. Chem. Phys. 87, 6257-6265 (1987).
    [CrossRef]
  12. A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, and K. A. Nelson, "Femtosecond multi-pulse impulsive stimulated Raman-scattering spectroscopy," J. Opt. Soc. Am. B 8, 1264-1275 (1991).
    [CrossRef]
  13. 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, 041803R (2005).
    [CrossRef]
  14. S. H. Lim, A. G. Caster, O. Nicolet, and S. R. Leone, "Chemical imaging by single pulse interferometric coherent anti-Stokes Raman scattering microscopy," J. Phys. Chem. B 110, 5196-5204 (2006).
    [CrossRef] [PubMed]
  15. 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]
  16. T. Hellerer, A. M. K. Enejder, and A. Zumbusch, "Spectral focusing: High spectral resolution spectroscopy with broad-bandwidth laser pulses," Appl. Phys. Lett. 85, 25-27 (2004).
    [CrossRef]
  17. B. Yellampalle, R. D. Averitt, A. Efimov, and A. J. Taylor, "Spectral interferometric coherent Raman imaging," Optics Express 13, 7672-7682 (2005).
    [CrossRef] [PubMed]
  18. R. Porter, F. Shan, and T. Guo, "Coherent anti-Stokes Raman scattering microscopy with spectrally tailored ultrafast pulses," Rev. Sci. Instrum. 76, 043108 (2005).
    [CrossRef]
  19. H. N. Paulsen, K. M. Hilligsoe, J. Thogersen, S. R. Keiding, and J. J. Larsen, "Coherent anti-Stokes Raman scattering microscopy with a photonic crystal fiber based light source," Opt. Lett. 28, 1123-1125 (2003).
    [CrossRef] [PubMed]
  20. 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]
  21. R. Merlin: "Generating coherent ths phonons with light pulses," Solid State Commun. 102, 207-220 (1997).
    [CrossRef]
  22. 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]
  23. M. Greve, B. Bodermann, H. R. Telle, P. Baum, and E. Riedle, "High-contrast chemical imaging with gated heterodyne coherent anti-Stokes Raman scattering microscopy," Appl. Phys. B 81, 875-879 (2005).
    [CrossRef]
  24. D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, "Interferometric differentiation between resonant and coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85, 5787-5789 (2004).
    [CrossRef]
  25. S. Roy, T. R. Meyer, and J. R. Gord, "Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals," Appl. Phys. Lett. 87, 264103 (2005).
    [CrossRef]
  26. M. D. Levenson, and G. L. Eesley, "Polarization-selective optical heterodyne detection for dramatically improved sensitivity in laser spectroscopy," Appl. Phys. 19, 1(1979).
    [CrossRef]
  27. 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]
  28. D. Oron, N. Dudovich, and Y. Silberberg, "Single-pulse phase-contrast nonlinear Raman spectroscopy," Phys. Rev. Lett. 89,273001 (2002).
    [CrossRef]
  29. G. W. Jones, D. L. Marks, C. Vinegoni, and S. A. Boppart, "High-spectral-resolution coherent anti-Stokes Raman scatterind with interferometrically detected broadband chirped pulses," Opt. Lett. 31, 1543-1545 (2006).
    [CrossRef] [PubMed]
  30. C. L. Evans, E. O. Potma, and X. S. Xie, "Coherent anti-Stokes Raman scattering spectral interferometry: Determination of the real and imaginary components of nonlinear susceptibility chi(3) for vibrational microscopy," Opt. Lett. 29, 2923-2925 (2004).
    [CrossRef]
  31. Sadtler: The Sadtler standard Raman spectra. Philadelphia: Sadtler Research Laboratories, subsidiary of Block Engineering; 1973.
  32. E. Frumker, E. Tal, Y. Silberberg, and D. Majer, "Femtosecond pulse-shape modulation at nanosecond rates," Opt. Lett. 30, 2796-2798 (2005).
    [CrossRef] [PubMed]

2006

2005

E. Frumker, E. Tal, Y. Silberberg, and D. Majer, "Femtosecond pulse-shape modulation at nanosecond rates," Opt. Lett. 30, 2796-2798 (2005).
[CrossRef] [PubMed]

S. Roy, T. R. Meyer, and J. R. Gord, "Broadband coherent anti-Stokes Raman scattering spectroscopy of nitrogen using a picosecond modeless dye laser," Opt. Lett. 30, 3222-3224 (2005).
[CrossRef] [PubMed]

B. Yellampalle, R. D. Averitt, A. Efimov, and A. J. Taylor, "Spectral interferometric coherent Raman imaging," Optics Express 13, 7672-7682 (2005).
[CrossRef] [PubMed]

R. Porter, F. Shan, and T. Guo, "Coherent anti-Stokes Raman scattering microscopy with spectrally tailored ultrafast pulses," Rev. Sci. Instrum. 76, 043108 (2005).
[CrossRef]

M. Greve, B. Bodermann, H. R. Telle, P. Baum, and E. Riedle, "High-contrast chemical imaging with gated heterodyne coherent anti-Stokes Raman scattering microscopy," Appl. Phys. B 81, 875-879 (2005).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, "Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals," Appl. Phys. Lett. 87, 264103 (2005).
[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, 041803R (2005).
[CrossRef]

2004

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 and coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85, 5787-5789 (2004).
[CrossRef]

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]

T. Hellerer, A. M. K. Enejder, and A. Zumbusch, "Spectral focusing: High spectral resolution spectroscopy with broad-bandwidth laser pulses," Appl. Phys. Lett. 85, 25-27 (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]

C. L. Evans, E. O. Potma, and X. S. Xie, "Coherent anti-Stokes Raman scattering spectral interferometry: Determination of the real and imaginary components of nonlinear susceptibility chi(3) for vibrational microscopy," Opt. Lett. 29, 2923-2925 (2004).
[CrossRef]

2003

H. N. Paulsen, K. M. Hilligsoe, J. Thogersen, S. R. Keiding, and J. J. Larsen, "Coherent anti-Stokes Raman scattering microscopy with a photonic crystal fiber based light source," Opt. Lett. 28, 1123-1125 (2003).
[CrossRef] [PubMed]

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherent anti-Stokes Raman spectroscopy in the fingerprint spectral region," J. Chem. Phys. 118, 9208-9215 (2003).
[CrossRef]

2002

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. Chen, 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]

N. Dudovich, and D. Oron, Y. Silberberg, "Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy," Nature 418, 512-514 (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]

D. Oron, N. Dudovich, and Y. Silberberg, "Single-pulse phase-contrast nonlinear Raman spectroscopy," Phys. Rev. Lett. 89,273001 (2002).
[CrossRef]

2001

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

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]

1997

R. Merlin: "Generating coherent ths phonons with light pulses," Solid State Commun. 102, 207-220 (1997).
[CrossRef]

1991

1987

Y. X. Yan, and K. A. Nelson, "Impulsive stimulated light-scattering. 2. Comparison to frequency-domain light-scattering spectroscopy," J. Chem. Phys. 87, 6257-6265 (1987).
[CrossRef]

1982

1979

M. D. Levenson, and G. L. Eesley, "Polarization-selective optical heterodyne detection for dramatically improved sensitivity in laser spectroscopy," Appl. Phys. 19, 1(1979).
[CrossRef]

Alexandrou, A.

Averitt, R. D.

B. Yellampalle, R. D. Averitt, A. Efimov, and A. J. Taylor, "Spectral interferometric coherent Raman imaging," Optics Express 13, 7672-7682 (2005).
[CrossRef] [PubMed]

Baum, P.

M. Greve, B. Bodermann, H. R. Telle, P. Baum, and E. Riedle, "High-contrast chemical imaging with gated heterodyne coherent anti-Stokes Raman scattering microscopy," Appl. Phys. B 81, 875-879 (2005).
[CrossRef]

Beaurepaire, E.

Bodermann, B.

M. Greve, B. Bodermann, H. R. Telle, P. Baum, and E. Riedle, "High-contrast chemical imaging with gated heterodyne coherent anti-Stokes Raman scattering microscopy," Appl. Phys. B 81, 875-879 (2005).
[CrossRef]

Book, L. D.

J. X. Chen, 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.

G. W. Jones, D. L. Marks, C. Vinegoni, and S. A. Boppart, "High-spectral-resolution coherent anti-Stokes Raman scatterind with interferometrically detected broadband chirped pulses," Opt. Lett. 31, 1543-1545 (2006).
[CrossRef] [PubMed]

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, "Interferometric differentiation between resonant and coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85, 5787-5789 (2004).
[CrossRef]

Bredfeldt, J. S.

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, "Interferometric differentiation between resonant and coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85, 5787-5789 (2004).
[CrossRef]

Caster, A. G.

S. H. Lim, A. G. Caster, O. Nicolet, and S. R. Leone, "Chemical imaging by single pulse interferometric coherent anti-Stokes Raman scattering microscopy," J. Phys. Chem. B 110, 5196-5204 (2006).
[CrossRef] [PubMed]

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, 041803R (2005).
[CrossRef]

Chen, J. X.

J. X. Chen, 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]

Cheng, J. X.

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, 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.

Dudovich, N.

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherent anti-Stokes Raman spectroscopy in the fingerprint spectral region," J. Chem. Phys. 118, 9208-9215 (2003).
[CrossRef]

D. Oron, N. Dudovich, and Y. Silberberg, "Single-pulse phase-contrast nonlinear Raman spectroscopy," Phys. Rev. Lett. 89,273001 (2002).
[CrossRef]

N. Dudovich, and D. Oron, Y. Silberberg, "Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy," Nature 418, 512-514 (2002).
[CrossRef] [PubMed]

Duncan, M. D.

Eesley, G. L.

M. D. Levenson, and G. L. Eesley, "Polarization-selective optical heterodyne detection for dramatically improved sensitivity in laser spectroscopy," Appl. Phys. 19, 1(1979).
[CrossRef]

Efimov, A.

B. Yellampalle, R. D. Averitt, A. Efimov, and A. J. Taylor, "Spectral interferometric coherent Raman imaging," Optics Express 13, 7672-7682 (2005).
[CrossRef] [PubMed]

Enejder, A. M. K.

T. Hellerer, A. M. K. Enejder, and A. Zumbusch, "Spectral focusing: High spectral resolution spectroscopy with broad-bandwidth laser pulses," Appl. Phys. Lett. 85, 25-27 (2004).
[CrossRef]

Evans, C. L.

Frumker, E.

Gord, J. R.

S. Roy, T. R. Meyer, and J. R. Gord, "Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals," Appl. Phys. Lett. 87, 264103 (2005).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, "Broadband coherent anti-Stokes Raman scattering spectroscopy of nitrogen using a picosecond modeless dye laser," Opt. Lett. 30, 3222-3224 (2005).
[CrossRef] [PubMed]

Greve, M.

M. Greve, B. Bodermann, H. R. Telle, P. Baum, and E. Riedle, "High-contrast chemical imaging with gated heterodyne coherent anti-Stokes Raman scattering microscopy," Appl. Phys. B 81, 875-879 (2005).
[CrossRef]

Guo, T.

R. Porter, F. Shan, and T. Guo, "Coherent anti-Stokes Raman scattering microscopy with spectrally tailored ultrafast pulses," Rev. Sci. Instrum. 76, 043108 (2005).
[CrossRef]

Hellerer, T.

T. Hellerer, A. M. K. Enejder, and A. Zumbusch, "Spectral focusing: High spectral resolution spectroscopy with broad-bandwidth laser pulses," Appl. Phys. Lett. 85, 25-27 (2004).
[CrossRef]

Hilligsoe, K. M.

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.

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, G. W.

Kee, T. W.

Keiding, S. R.

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]

Larsen, J. J.

Leaird, D. E.

Leone, S. R.

S. H. Lim, A. G. Caster, O. Nicolet, and S. R. Leone, "Chemical imaging by single pulse interferometric coherent anti-Stokes Raman scattering microscopy," J. Phys. Chem. B 110, 5196-5204 (2006).
[CrossRef] [PubMed]

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, 041803R (2005).
[CrossRef]

Levenson, M. D.

M. D. Levenson, and G. L. Eesley, "Polarization-selective optical heterodyne detection for dramatically improved sensitivity in laser spectroscopy," Appl. Phys. 19, 1(1979).
[CrossRef]

Lim, S. H.

S. H. Lim, A. G. Caster, O. Nicolet, and S. R. Leone, "Chemical imaging by single pulse interferometric coherent anti-Stokes Raman scattering microscopy," J. Phys. Chem. B 110, 5196-5204 (2006).
[CrossRef] [PubMed]

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, 041803R (2005).
[CrossRef]

Majer, D.

Manuccia, T. J.

Marks, D. L.

G. W. Jones, D. L. Marks, C. Vinegoni, and S. A. Boppart, "High-spectral-resolution coherent anti-Stokes Raman scatterind with interferometrically detected broadband chirped pulses," Opt. Lett. 31, 1543-1545 (2006).
[CrossRef] [PubMed]

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, "Interferometric differentiation between resonant and coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85, 5787-5789 (2004).
[CrossRef]

Merlin, R.

R. Merlin: "Generating coherent ths phonons with light pulses," Solid State Commun. 102, 207-220 (1997).
[CrossRef]

Meyer, T. R.

S. Roy, T. R. Meyer, and J. R. Gord, "Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals," Appl. Phys. Lett. 87, 264103 (2005).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, "Broadband coherent anti-Stokes Raman scattering spectroscopy of nitrogen using a picosecond modeless dye laser," Opt. Lett. 30, 3222-3224 (2005).
[CrossRef] [PubMed]

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]

Nelson, K. A.

A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, and K. A. Nelson, "Femtosecond multi-pulse impulsive stimulated Raman-scattering spectroscopy," J. Opt. Soc. Am. B 8, 1264-1275 (1991).
[CrossRef]

Y. X. Yan, and K. A. Nelson, "Impulsive stimulated light-scattering. 2. Comparison to frequency-domain light-scattering spectroscopy," J. Chem. Phys. 87, 6257-6265 (1987).
[CrossRef]

Nicolet, O.

S. H. Lim, A. G. Caster, O. Nicolet, and S. R. Leone, "Chemical imaging by single pulse interferometric coherent anti-Stokes Raman scattering microscopy," J. Phys. Chem. B 110, 5196-5204 (2006).
[CrossRef] [PubMed]

Ogilvie, J. P.

Oron, D.

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherent anti-Stokes Raman spectroscopy in the fingerprint spectral region," J. Chem. Phys. 118, 9208-9215 (2003).
[CrossRef]

D. Oron, N. Dudovich, and Y. Silberberg, "Single-pulse phase-contrast nonlinear Raman spectroscopy," Phys. Rev. Lett. 89,273001 (2002).
[CrossRef]

N. Dudovich, and D. Oron, Y. Silberberg, "Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy," Nature 418, 512-514 (2002).
[CrossRef] [PubMed]

Paulsen, H. N.

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]

Porter, R.

R. Porter, F. Shan, and T. Guo, "Coherent anti-Stokes Raman scattering microscopy with spectrally tailored ultrafast pulses," Rev. Sci. Instrum. 76, 043108 (2005).
[CrossRef]

Potma, E. O.

Reintjes, J.

Riedle, E.

M. Greve, B. Bodermann, H. R. Telle, P. Baum, and E. Riedle, "High-contrast chemical imaging with gated heterodyne coherent anti-Stokes Raman scattering microscopy," Appl. Phys. B 81, 875-879 (2005).
[CrossRef]

Roy, S.

S. Roy, T. R. Meyer, and J. R. Gord, "Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals," Appl. Phys. Lett. 87, 264103 (2005).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, "Broadband coherent anti-Stokes Raman scattering spectroscopy of nitrogen using a picosecond modeless dye laser," Opt. Lett. 30, 3222-3224 (2005).
[CrossRef] [PubMed]

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]

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]

Shan, F.

R. Porter, F. Shan, and T. Guo, "Coherent anti-Stokes Raman scattering microscopy with spectrally tailored ultrafast pulses," Rev. Sci. Instrum. 76, 043108 (2005).
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[CrossRef] [PubMed]

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherent anti-Stokes Raman spectroscopy in the fingerprint spectral region," J. Chem. Phys. 118, 9208-9215 (2003).
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D. Oron, N. Dudovich, and Y. Silberberg, "Single-pulse phase-contrast nonlinear Raman spectroscopy," Phys. Rev. Lett. 89,273001 (2002).
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[CrossRef] [PubMed]

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Taylor, A. J.

B. Yellampalle, R. D. Averitt, A. Efimov, and A. J. Taylor, "Spectral interferometric coherent Raman imaging," Optics Express 13, 7672-7682 (2005).
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M. Greve, B. Bodermann, H. R. Telle, P. Baum, and E. Riedle, "High-contrast chemical imaging with gated heterodyne coherent anti-Stokes Raman scattering microscopy," Appl. Phys. B 81, 875-879 (2005).
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Vinegoni, C.

G. W. Jones, D. L. Marks, C. Vinegoni, and S. A. Boppart, "High-spectral-resolution coherent anti-Stokes Raman scatterind with interferometrically detected broadband chirped pulses," Opt. Lett. 31, 1543-1545 (2006).
[CrossRef] [PubMed]

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, "Interferometric differentiation between resonant and coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85, 5787-5789 (2004).
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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).
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J. X. Chen, 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]

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Wiederrecht, G. P.

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]

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]

C. L. Evans, E. O. Potma, and X. S. Xie, "Coherent anti-Stokes Raman scattering spectral interferometry: Determination of the real and imaginary components of nonlinear susceptibility chi(3) for vibrational microscopy," Opt. Lett. 29, 2923-2925 (2004).
[CrossRef]

J. X. Chen, 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).
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B. Yellampalle, R. D. Averitt, A. Efimov, and A. J. Taylor, "Spectral interferometric coherent Raman imaging," Optics Express 13, 7672-7682 (2005).
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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).
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M. Greve, B. Bodermann, H. R. Telle, P. Baum, and E. Riedle, "High-contrast chemical imaging with gated heterodyne coherent anti-Stokes Raman scattering microscopy," Appl. Phys. B 81, 875-879 (2005).
[CrossRef]

Appl. Phys. Lett.

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, "Interferometric differentiation between resonant and coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes," Appl. Phys. Lett. 85, 5787-5789 (2004).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, "Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals," Appl. Phys. Lett. 87, 264103 (2005).
[CrossRef]

T. Hellerer, A. M. K. Enejder, and A. Zumbusch, "Spectral focusing: High spectral resolution spectroscopy with broad-bandwidth laser pulses," Appl. Phys. Lett. 85, 25-27 (2004).
[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]

Chem. Phys. Lett.

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. Chem. Phys.

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherent anti-Stokes Raman spectroscopy in the fingerprint spectral region," J. Chem. Phys. 118, 9208-9215 (2003).
[CrossRef]

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[CrossRef]

J. Opt. Soc. Am. B

J. Phys. Chem. B

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

S. H. Lim, A. G. Caster, O. Nicolet, and S. R. Leone, "Chemical imaging by single pulse interferometric coherent anti-Stokes Raman scattering microscopy," J. Phys. Chem. B 110, 5196-5204 (2006).
[CrossRef] [PubMed]

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[CrossRef]

E. Frumker, E. Tal, Y. Silberberg, and D. Majer, "Femtosecond pulse-shape modulation at nanosecond rates," Opt. Lett. 30, 2796-2798 (2005).
[CrossRef] [PubMed]

S. Roy, T. R. Meyer, and J. R. Gord, "Broadband coherent anti-Stokes Raman scattering spectroscopy of nitrogen using a picosecond modeless dye laser," Opt. Lett. 30, 3222-3224 (2005).
[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]

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[CrossRef] [PubMed]

Optics Express

B. Yellampalle, R. D. Averitt, A. Efimov, and A. J. Taylor, "Spectral interferometric coherent Raman imaging," Optics Express 13, 7672-7682 (2005).
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[CrossRef]

D. Oron, N. Dudovich, and Y. Silberberg, "Single-pulse phase-contrast nonlinear Raman spectroscopy," Phys. Rev. Lett. 89,273001 (2002).
[CrossRef]

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R. Porter, F. Shan, and T. Guo, "Coherent anti-Stokes Raman scattering microscopy with spectrally tailored ultrafast pulses," Rev. Sci. Instrum. 76, 043108 (2005).
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Figures (5)

Fig. 1.
Fig. 1.

(a). Resonant CARS process. (b) Nonresonant CARS process. (c) Multiplex CARS – multiple Raman coherences can be generated when broadband Stokes light is available. (d) (i) Experimental implementation of standard FTCARS. BS: beamsplitter, DC: dispersion compensation (chirped mirrors), LPF: long pass filter, SPF: short pass filter, PMT: photomultiplier tube. (ii) Experimental setup for Homodyne CARS. Gr: 600 lines/mm grating, ND: neutral density filter, CG: compensating glass, M: mirror, SM: spherical mirror (f=30 cm).

Fig. 2.
Fig. 2.

Simulated (left) and experimental (right) FTCARS results. a) Spectrum of the pump and probe pulse. The locations of the long pass (dashed) and short pass (solid) filters are also indicated. b) Time domain FTCARS signal for pyridine including the dominant CARS modes at 990 cm-1 and 1030 cm-1, with smaller peaks at 983 cm-1 and 1070 cm-1. The actual scan length was 12 ps, providing ~3 cm-1 resolution. c) CARS

Fig. 3.
Fig. 3.

Dependence of resonant CARS signal on the pump (dashed line) and probe (solid line) pulse power. Slopes of 1.18 and 2.16 indicate linear and quadratic dependence on the pump and probe power respectively. The resonant signal amplitude was measured from the CARS power spectrum. Simulations give slopes of 1 and 2 respectively.

Fig. 4.
Fig. 4.

(a). FTCARS power spectra obtained 2-propanol, exhibiting a single dominant peak near 820 cm-1. The weak signal from regular detection (dashed line/circles) has been multiplied by 100 to appear visible on the same scale as the homodyne signal (solid line/triangles). b) Oscillation amplitude as a function of relative phase between the LO and the resonant and nonresonant FTCARS signals, demonstrating control over the homodyne amplification.

Fig. 5.
Fig. 5.

Controlled homodyne (solid) and standard FTCARS (dashed) spectra of pyridine using 5mW pump and 5 mW probe power.

Equations (8)

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P R ( 3 ) ( ω ) 0 d Ω 1 Ω Ω R i Γ R E ( ω Ω ) A ( Ω )
A ( Ω ) = 0 d ω ' E * ( ω ' ) E ( Ω + ω ' )
P N R ( 3 ) ( ω ) 0 d Ω Ω E ( ω Ω ) A ( Ω )
S FTCARS ( τ ) 0 P FTCARS ( τ , t ) 2 d t
P FTCARS ( τ , t ) = P R ( 3 ) ( τ , t ) + P N R ( 3 ) ( τ , t )
P FTCARS ( τ ) P R both ( τ ) + P N R both ( τ ) + P R probe + P N R probe
P FTCARS χ R ( 3 ) I pump E probe + χ R ( 3 ) I probe E probe + χ N R ( 3 ) I probe E probe
S FTCARS χ R ( 3 ) I pump I probe 2

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