Abstract

We demonstrate a homodyne coherent anti-Stokes Raman scattering (CARS) technique based on femtosecond laser pulse shaping. This technique utilizes fast phase cycling to extract nonlinear Raman signatures with a self-generated reference signal acting as a local oscillator. The local oscillator is generated at the focus and is intrinsically stable relative to the Raman signal even in highly scattering samples. We can therefore retrieve phase information from the Raman signal and can suppress the ubiquitous non-resonant background.

© 2010 OSA

Full Article  |  PDF Article

References

  • View by:
  • |
  • |
  • |

  1. E. B. Hanlon, R. Manoharan, T. W. Koo, K. E. Shafer, J. T. Motz, M. Fitzmaurice, J. R. Kramer, I. Itzkan, R. R. Dasari, and M. S. Feld, “Prospects for in vivo Raman spectroscopy,” Phys. Med. Biol. 45(2), R1–R59 (2000).
    [CrossRef] [PubMed]
  2. M. Cui, B. R. Bachler, and J. P. Ogilvie, “Comparing coherent and spontaneous Raman scattering under biological imaging conditions,” Opt. Lett. 34(6), 773–775 (2009).
    [CrossRef] [PubMed]
  3. J. X. Cheng and X. S. Xie, “Coherent anti-Stokes Raman scattering microscopy: Instrumentation, theory, and applications,” J. Phys. Chem. B 108(3), 827–840 (2004).
    [CrossRef]
  4. 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 χ(3) for vibrational microscopy,” Opt. Lett. 29(24), 2923–2925 (2004).
    [CrossRef]
  5. M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Vibrational phase contrast microscopy by use of coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 103(4), 043905 (2009).
    [CrossRef] [PubMed]
  6. D. Oron, N. Dudovich, and Y. Silberberg, “Single-pulse phase-contrast nonlinear Raman spectroscopy,” Phys. Rev. Lett. 89(27), 273001 (2002).
    [CrossRef]
  7. X. G. Xu, S. O. Konorov, J. W. Hepburn, and V. Milner, “Background-free coherent Raman spectroscopy by detecting the spectral phase of molecular vibrations,” Opt. Lett. 33(11), 1177–1179 (2008).
    [CrossRef] [PubMed]
  8. B. von Vacano, T. Buckup, and M. Motzkus, “Highly sensitive single-beam heterodyne coherent anti-Stokes Raman scattering,” Opt. Lett. 31(16), 2495–2497 (2006).
    [CrossRef] [PubMed]
  9. D. L. Marks and S. A. Boppart, “Nonlinear interferometric vibrational imaging,” Phys. Rev. Lett. 92(12), 123905 (2004).
    [CrossRef] [PubMed]
  10. S. H. Lim, A. G. Caster, and S. R. Leone, “Fourier transform spectral interferometric coherent anti-Stokes Raman scattering (FTSI-CARS) spectroscopy,” Opt. Lett. 32(10), 1332–1334 (2007).
    [CrossRef] [PubMed]
  11. Y. J. Lee and M. T. Cicerone, “Single-shot interferometric approach to background free broadband coherent anti-Stokes Raman scattering spectroscopy,” Opt. Express 17(1), 123–135 (2009).
    [CrossRef] [PubMed]
  12. S. Postma, A. C. W. van Rhijn, J. P. Korterik, P. Gross, J. L. Herek, and H. L. Offerhaus, “Application of spectral phase shaping to high resolution CARS spectroscopy,” Opt. Express 16(11), 7985–7996 (2008).
    [CrossRef] [PubMed]
  13. C. W. Hillegas, J. X. Tull, D. Goswami, D. Strickland, and W. S. Warren, “Femtosecond laser pulse shaping by use of microsecond radio-frequency pulses,” Opt. Lett. 19(10), 737–739 (1994).
    [CrossRef] [PubMed]
  14. M. C. Fischer, H. C. Liu, I. R. Piletic, and W. S. Warren, “Simultaneous self-phase modulation and two-photon absorption measurement by a spectral homodyne Z-scan method,” Opt. Express 16(6), 4192–4205 (2008).
    [CrossRef] [PubMed]
  15. I. R. Piletic, M. C. Fischer, P. Samineni, G. Yurtsever, and W. S. Warren, “Rapid pulse shaping with homodyne detection for measuring nonlinear optical signals,” Opt. Lett. 33(13), 1482–1484 (2008).
    [CrossRef] [PubMed]
  16. D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, “Narrow-band coherent anti-stokes Raman signals from broad-band pulses,” Phys. Rev. Lett. 88(6), 063004 (2002).
    [CrossRef] [PubMed]
  17. 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(12), 3653–3661 (2008).
    [CrossRef] [PubMed]

2009

M. Cui, B. R. Bachler, and J. P. Ogilvie, “Comparing coherent and spontaneous Raman scattering under biological imaging conditions,” Opt. Lett. 34(6), 773–775 (2009).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Vibrational phase contrast microscopy by use of coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 103(4), 043905 (2009).
[CrossRef] [PubMed]

Y. J. Lee and M. T. Cicerone, “Single-shot interferometric approach to background free broadband coherent anti-Stokes Raman scattering spectroscopy,” Opt. Express 17(1), 123–135 (2009).
[CrossRef] [PubMed]

2008

S. Postma, A. C. W. van Rhijn, J. P. Korterik, P. Gross, J. L. Herek, and H. L. Offerhaus, “Application of spectral phase shaping to high resolution CARS spectroscopy,” Opt. Express 16(11), 7985–7996 (2008).
[CrossRef] [PubMed]

M. C. Fischer, H. C. Liu, I. R. Piletic, and W. S. Warren, “Simultaneous self-phase modulation and two-photon absorption measurement by a spectral homodyne Z-scan method,” Opt. Express 16(6), 4192–4205 (2008).
[CrossRef] [PubMed]

I. R. Piletic, M. C. Fischer, P. Samineni, G. Yurtsever, and W. S. Warren, “Rapid pulse shaping with homodyne detection for measuring nonlinear optical signals,” Opt. Lett. 33(13), 1482–1484 (2008).
[CrossRef] [PubMed]

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(12), 3653–3661 (2008).
[CrossRef] [PubMed]

X. G. Xu, S. O. Konorov, J. W. Hepburn, and V. Milner, “Background-free coherent Raman spectroscopy by detecting the spectral phase of molecular vibrations,” Opt. Lett. 33(11), 1177–1179 (2008).
[CrossRef] [PubMed]

2007

S. H. Lim, A. G. Caster, and S. R. Leone, “Fourier transform spectral interferometric coherent anti-Stokes Raman scattering (FTSI-CARS) spectroscopy,” Opt. Lett. 32(10), 1332–1334 (2007).
[CrossRef] [PubMed]

2006

B. von Vacano, T. Buckup, and M. Motzkus, “Highly sensitive single-beam heterodyne coherent anti-Stokes Raman scattering,” Opt. Lett. 31(16), 2495–2497 (2006).
[CrossRef] [PubMed]

2004

D. L. Marks and S. A. Boppart, “Nonlinear interferometric vibrational imaging,” Phys. Rev. Lett. 92(12), 123905 (2004).
[CrossRef] [PubMed]

J. X. Cheng and X. S. Xie, “Coherent anti-Stokes Raman scattering microscopy: Instrumentation, theory, and applications,” J. Phys. Chem. B 108(3), 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 χ(3) for vibrational microscopy,” Opt. Lett. 29(24), 2923–2925 (2004).
[CrossRef]

2002

D. Oron, N. Dudovich, and Y. Silberberg, “Single-pulse phase-contrast nonlinear Raman spectroscopy,” Phys. Rev. Lett. 89(27), 273001 (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(6), 063004 (2002).
[CrossRef] [PubMed]

2000

E. B. Hanlon, R. Manoharan, T. W. Koo, K. E. Shafer, J. T. Motz, M. Fitzmaurice, J. R. Kramer, I. Itzkan, R. R. Dasari, and M. S. Feld, “Prospects for in vivo Raman spectroscopy,” Phys. Med. Biol. 45(2), R1–R59 (2000).
[CrossRef] [PubMed]

1994

C. W. Hillegas, J. X. Tull, D. Goswami, D. Strickland, and W. S. Warren, “Femtosecond laser pulse shaping by use of microsecond radio-frequency pulses,” Opt. Lett. 19(10), 737–739 (1994).
[CrossRef] [PubMed]

Bachler, B. R.

M. Cui, B. R. Bachler, and J. P. Ogilvie, “Comparing coherent and spontaneous Raman scattering under biological imaging conditions,” Opt. Lett. 34(6), 773–775 (2009).
[CrossRef] [PubMed]

Boppart, S. A.

D. L. Marks and S. A. Boppart, “Nonlinear interferometric vibrational imaging,” Phys. Rev. Lett. 92(12), 123905 (2004).
[CrossRef] [PubMed]

Buckup, T.

B. von Vacano, T. Buckup, and M. Motzkus, “Highly sensitive single-beam heterodyne coherent anti-Stokes Raman scattering,” Opt. Lett. 31(16), 2495–2497 (2006).
[CrossRef] [PubMed]

Caster, A. G.

S. H. Lim, A. G. Caster, and S. R. Leone, “Fourier transform spectral interferometric coherent anti-Stokes Raman scattering (FTSI-CARS) spectroscopy,” Opt. Lett. 32(10), 1332–1334 (2007).
[CrossRef] [PubMed]

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(12), 3653–3661 (2008).
[CrossRef] [PubMed]

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(3), 827–840 (2004).
[CrossRef]

Cicerone, M. T.

Y. J. Lee and M. T. Cicerone, “Single-shot interferometric approach to background free broadband coherent anti-Stokes Raman scattering spectroscopy,” Opt. Express 17(1), 123–135 (2009).
[CrossRef] [PubMed]

Cui, M.

M. Cui, B. R. Bachler, and J. P. Ogilvie, “Comparing coherent and spontaneous Raman scattering under biological imaging conditions,” Opt. Lett. 34(6), 773–775 (2009).
[CrossRef] [PubMed]

Dasari, R. R.

E. B. Hanlon, R. Manoharan, T. W. Koo, K. E. Shafer, J. T. Motz, M. Fitzmaurice, J. R. Kramer, I. Itzkan, R. R. Dasari, and M. S. Feld, “Prospects for in vivo Raman spectroscopy,” Phys. Med. Biol. 45(2), R1–R59 (2000).
[CrossRef] [PubMed]

Dudovich, N.

D. Oron, N. Dudovich, and Y. Silberberg, “Single-pulse phase-contrast nonlinear Raman spectroscopy,” Phys. Rev. Lett. 89(27), 273001 (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(6), 063004 (2002).
[CrossRef] [PubMed]

Evans, C. L.

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 χ(3) for vibrational microscopy,” Opt. Lett. 29(24), 2923–2925 (2004).
[CrossRef]

Feld, M. S.

E. B. Hanlon, R. Manoharan, T. W. Koo, K. E. Shafer, J. T. Motz, M. Fitzmaurice, J. R. Kramer, I. Itzkan, R. R. Dasari, and M. S. Feld, “Prospects for in vivo Raman spectroscopy,” Phys. Med. Biol. 45(2), R1–R59 (2000).
[CrossRef] [PubMed]

Fischer, M. C.

I. R. Piletic, M. C. Fischer, P. Samineni, G. Yurtsever, and W. S. Warren, “Rapid pulse shaping with homodyne detection for measuring nonlinear optical signals,” Opt. Lett. 33(13), 1482–1484 (2008).
[CrossRef] [PubMed]

M. C. Fischer, H. C. Liu, I. R. Piletic, and W. S. Warren, “Simultaneous self-phase modulation and two-photon absorption measurement by a spectral homodyne Z-scan method,” Opt. Express 16(6), 4192–4205 (2008).
[CrossRef] [PubMed]

Fitzmaurice, M.

E. B. Hanlon, R. Manoharan, T. W. Koo, K. E. Shafer, J. T. Motz, M. Fitzmaurice, J. R. Kramer, I. Itzkan, R. R. Dasari, and M. S. Feld, “Prospects for in vivo Raman spectroscopy,” Phys. Med. Biol. 45(2), R1–R59 (2000).
[CrossRef] [PubMed]

Goswami, D.

C. W. Hillegas, J. X. Tull, D. Goswami, D. Strickland, and W. S. Warren, “Femtosecond laser pulse shaping by use of microsecond radio-frequency pulses,” Opt. Lett. 19(10), 737–739 (1994).
[CrossRef] [PubMed]

Gross, P.

S. Postma, A. C. W. van Rhijn, J. P. Korterik, P. Gross, J. L. Herek, and H. L. Offerhaus, “Application of spectral phase shaping to high resolution CARS spectroscopy,” Opt. Express 16(11), 7985–7996 (2008).
[CrossRef] [PubMed]

Hanlon, E. B.

E. B. Hanlon, R. Manoharan, T. W. Koo, K. E. Shafer, J. T. Motz, M. Fitzmaurice, J. R. Kramer, I. Itzkan, R. R. Dasari, and M. S. Feld, “Prospects for in vivo Raman spectroscopy,” Phys. Med. Biol. 45(2), R1–R59 (2000).
[CrossRef] [PubMed]

Hepburn, J. W.

X. G. Xu, S. O. Konorov, J. W. Hepburn, and V. Milner, “Background-free coherent Raman spectroscopy by detecting the spectral phase of molecular vibrations,” Opt. Lett. 33(11), 1177–1179 (2008).
[CrossRef] [PubMed]

Herek, J. L.

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Vibrational phase contrast microscopy by use of coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 103(4), 043905 (2009).
[CrossRef] [PubMed]

S. Postma, A. C. W. van Rhijn, J. P. Korterik, P. Gross, J. L. Herek, and H. L. Offerhaus, “Application of spectral phase shaping to high resolution CARS spectroscopy,” Opt. Express 16(11), 7985–7996 (2008).
[CrossRef] [PubMed]

Hillegas, C. W.

C. W. Hillegas, J. X. Tull, D. Goswami, D. Strickland, and W. S. Warren, “Femtosecond laser pulse shaping by use of microsecond radio-frequency pulses,” Opt. Lett. 19(10), 737–739 (1994).
[CrossRef] [PubMed]

Itzkan, I.

E. B. Hanlon, R. Manoharan, T. W. Koo, K. E. Shafer, J. T. Motz, M. Fitzmaurice, J. R. Kramer, I. Itzkan, R. R. Dasari, and M. S. Feld, “Prospects for in vivo Raman spectroscopy,” Phys. Med. Biol. 45(2), R1–R59 (2000).
[CrossRef] [PubMed]

Jurna, M.

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Vibrational phase contrast microscopy by use of coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 103(4), 043905 (2009).
[CrossRef] [PubMed]

Konorov, S. O.

X. G. Xu, S. O. Konorov, J. W. Hepburn, and V. Milner, “Background-free coherent Raman spectroscopy by detecting the spectral phase of molecular vibrations,” Opt. Lett. 33(11), 1177–1179 (2008).
[CrossRef] [PubMed]

Koo, T. W.

E. B. Hanlon, R. Manoharan, T. W. Koo, K. E. Shafer, J. T. Motz, M. Fitzmaurice, J. R. Kramer, I. Itzkan, R. R. Dasari, and M. S. Feld, “Prospects for in vivo Raman spectroscopy,” Phys. Med. Biol. 45(2), R1–R59 (2000).
[CrossRef] [PubMed]

Korterik, J. P.

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Vibrational phase contrast microscopy by use of coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 103(4), 043905 (2009).
[CrossRef] [PubMed]

S. Postma, A. C. W. van Rhijn, J. P. Korterik, P. Gross, J. L. Herek, and H. L. Offerhaus, “Application of spectral phase shaping to high resolution CARS spectroscopy,” Opt. Express 16(11), 7985–7996 (2008).
[CrossRef] [PubMed]

Kramer, J. R.

E. B. Hanlon, R. Manoharan, T. W. Koo, K. E. Shafer, J. T. Motz, M. Fitzmaurice, J. R. Kramer, I. Itzkan, R. R. Dasari, and M. S. Feld, “Prospects for in vivo Raman spectroscopy,” Phys. Med. Biol. 45(2), R1–R59 (2000).
[CrossRef] [PubMed]

Lee, Y. J.

Y. J. Lee and M. T. Cicerone, “Single-shot interferometric approach to background free broadband coherent anti-Stokes Raman scattering spectroscopy,” Opt. Express 17(1), 123–135 (2009).
[CrossRef] [PubMed]

Leone, S. R.

S. H. Lim, A. G. Caster, and S. R. Leone, “Fourier transform spectral interferometric coherent anti-Stokes Raman scattering (FTSI-CARS) spectroscopy,” Opt. Lett. 32(10), 1332–1334 (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(12), 3653–3661 (2008).
[CrossRef] [PubMed]

S. H. Lim, A. G. Caster, and S. R. Leone, “Fourier transform spectral interferometric coherent anti-Stokes Raman scattering (FTSI-CARS) spectroscopy,” Opt. Lett. 32(10), 1332–1334 (2007).
[CrossRef] [PubMed]

Liu, H. C.

M. C. Fischer, H. C. Liu, I. R. Piletic, and W. S. Warren, “Simultaneous self-phase modulation and two-photon absorption measurement by a spectral homodyne Z-scan method,” Opt. Express 16(6), 4192–4205 (2008).
[CrossRef] [PubMed]

Manoharan, R.

E. B. Hanlon, R. Manoharan, T. W. Koo, K. E. Shafer, J. T. Motz, M. Fitzmaurice, J. R. Kramer, I. Itzkan, R. R. Dasari, and M. S. Feld, “Prospects for in vivo Raman spectroscopy,” Phys. Med. Biol. 45(2), R1–R59 (2000).
[CrossRef] [PubMed]

Marks, D. L.

D. L. Marks and S. A. Boppart, “Nonlinear interferometric vibrational imaging,” Phys. Rev. Lett. 92(12), 123905 (2004).
[CrossRef] [PubMed]

Milner, V.

X. G. Xu, S. O. Konorov, J. W. Hepburn, and V. Milner, “Background-free coherent Raman spectroscopy by detecting the spectral phase of molecular vibrations,” Opt. Lett. 33(11), 1177–1179 (2008).
[CrossRef] [PubMed]

Motz, J. T.

E. B. Hanlon, R. Manoharan, T. W. Koo, K. E. Shafer, J. T. Motz, M. Fitzmaurice, J. R. Kramer, I. Itzkan, R. R. Dasari, and M. S. Feld, “Prospects for in vivo Raman spectroscopy,” Phys. Med. Biol. 45(2), R1–R59 (2000).
[CrossRef] [PubMed]

Motzkus, M.

B. von Vacano, T. Buckup, and M. Motzkus, “Highly sensitive single-beam heterodyne coherent anti-Stokes Raman scattering,” Opt. Lett. 31(16), 2495–2497 (2006).
[CrossRef] [PubMed]

Offerhaus, H. L.

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Vibrational phase contrast microscopy by use of coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 103(4), 043905 (2009).
[CrossRef] [PubMed]

S. Postma, A. C. W. van Rhijn, J. P. Korterik, P. Gross, J. L. Herek, and H. L. Offerhaus, “Application of spectral phase shaping to high resolution CARS spectroscopy,” Opt. Express 16(11), 7985–7996 (2008).
[CrossRef] [PubMed]

Ogilvie, J. P.

M. Cui, B. R. Bachler, and J. P. Ogilvie, “Comparing coherent and spontaneous Raman scattering under biological imaging conditions,” Opt. Lett. 34(6), 773–775 (2009).
[CrossRef] [PubMed]

Oron, D.

D. Oron, N. Dudovich, and Y. Silberberg, “Single-pulse phase-contrast nonlinear Raman spectroscopy,” Phys. Rev. Lett. 89(27), 273001 (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(6), 063004 (2002).
[CrossRef] [PubMed]

Otto, C.

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Vibrational phase contrast microscopy by use of coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 103(4), 043905 (2009).
[CrossRef] [PubMed]

Piletic, I. R.

M. C. Fischer, H. C. Liu, I. R. Piletic, and W. S. Warren, “Simultaneous self-phase modulation and two-photon absorption measurement by a spectral homodyne Z-scan method,” Opt. Express 16(6), 4192–4205 (2008).
[CrossRef] [PubMed]

I. R. Piletic, M. C. Fischer, P. Samineni, G. Yurtsever, and W. S. Warren, “Rapid pulse shaping with homodyne detection for measuring nonlinear optical signals,” Opt. Lett. 33(13), 1482–1484 (2008).
[CrossRef] [PubMed]

Postma, S.

S. Postma, A. C. W. van Rhijn, J. P. Korterik, P. Gross, J. L. Herek, and H. L. Offerhaus, “Application of spectral phase shaping to high resolution CARS spectroscopy,” Opt. Express 16(11), 7985–7996 (2008).
[CrossRef] [PubMed]

Potma, E. O.

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 χ(3) for vibrational microscopy,” Opt. Lett. 29(24), 2923–2925 (2004).
[CrossRef]

Samineni, P.

I. R. Piletic, M. C. Fischer, P. Samineni, G. Yurtsever, and W. S. Warren, “Rapid pulse shaping with homodyne detection for measuring nonlinear optical signals,” Opt. Lett. 33(13), 1482–1484 (2008).
[CrossRef] [PubMed]

Shafer, K. E.

E. B. Hanlon, R. Manoharan, T. W. Koo, K. E. Shafer, J. T. Motz, M. Fitzmaurice, J. R. Kramer, I. Itzkan, R. R. Dasari, and M. S. Feld, “Prospects for in vivo Raman spectroscopy,” Phys. Med. Biol. 45(2), R1–R59 (2000).
[CrossRef] [PubMed]

Silberberg, Y.

D. Oron, N. Dudovich, and Y. Silberberg, “Single-pulse phase-contrast nonlinear Raman spectroscopy,” Phys. Rev. Lett. 89(27), 273001 (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(6), 063004 (2002).
[CrossRef] [PubMed]

Strickland, D.

C. W. Hillegas, J. X. Tull, D. Goswami, D. Strickland, and W. S. Warren, “Femtosecond laser pulse shaping by use of microsecond radio-frequency pulses,” Opt. Lett. 19(10), 737–739 (1994).
[CrossRef] [PubMed]

Tull, J. X.

C. W. Hillegas, J. X. Tull, D. Goswami, D. Strickland, and W. S. Warren, “Femtosecond laser pulse shaping by use of microsecond radio-frequency pulses,” Opt. Lett. 19(10), 737–739 (1994).
[CrossRef] [PubMed]

van Rhijn, A. C. W.

S. Postma, A. C. W. van Rhijn, J. P. Korterik, P. Gross, J. L. Herek, and H. L. Offerhaus, “Application of spectral phase shaping to high resolution CARS spectroscopy,” Opt. Express 16(11), 7985–7996 (2008).
[CrossRef] [PubMed]

von Vacano, B.

B. von Vacano, T. Buckup, and M. Motzkus, “Highly sensitive single-beam heterodyne coherent anti-Stokes Raman scattering,” Opt. Lett. 31(16), 2495–2497 (2006).
[CrossRef] [PubMed]

Warren, W. S.

M. C. Fischer, H. C. Liu, I. R. Piletic, and W. S. Warren, “Simultaneous self-phase modulation and two-photon absorption measurement by a spectral homodyne Z-scan method,” Opt. Express 16(6), 4192–4205 (2008).
[CrossRef] [PubMed]

I. R. Piletic, M. C. Fischer, P. Samineni, G. Yurtsever, and W. S. Warren, “Rapid pulse shaping with homodyne detection for measuring nonlinear optical signals,” Opt. Lett. 33(13), 1482–1484 (2008).
[CrossRef] [PubMed]

C. W. Hillegas, J. X. Tull, D. Goswami, D. Strickland, and W. S. Warren, “Femtosecond laser pulse shaping by use of microsecond radio-frequency pulses,” Opt. Lett. 19(10), 737–739 (1994).
[CrossRef] [PubMed]

Xie, X. S.

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 χ(3) for vibrational microscopy,” Opt. Lett. 29(24), 2923–2925 (2004).
[CrossRef]

J. X. Cheng and X. S. Xie, “Coherent anti-Stokes Raman scattering microscopy: Instrumentation, theory, and applications,” J. Phys. Chem. B 108(3), 827–840 (2004).
[CrossRef]

Xu, X. G.

X. G. Xu, S. O. Konorov, J. W. Hepburn, and V. Milner, “Background-free coherent Raman spectroscopy by detecting the spectral phase of molecular vibrations,” Opt. Lett. 33(11), 1177–1179 (2008).
[CrossRef] [PubMed]

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(6), 063004 (2002).
[CrossRef] [PubMed]

Yurtsever, G.

I. R. Piletic, M. C. Fischer, P. Samineni, G. Yurtsever, and W. S. Warren, “Rapid pulse shaping with homodyne detection for measuring nonlinear optical signals,” Opt. Lett. 33(13), 1482–1484 (2008).
[CrossRef] [PubMed]

J. Phys. Chem. B

J. X. Cheng and X. S. Xie, “Coherent anti-Stokes Raman scattering microscopy: Instrumentation, theory, and applications,” J. Phys. Chem. B 108(3), 827–840 (2004).
[CrossRef]

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(12), 3653–3661 (2008).
[CrossRef] [PubMed]

Opt. Express

Y. J. Lee and M. T. Cicerone, “Single-shot interferometric approach to background free broadband coherent anti-Stokes Raman scattering spectroscopy,” Opt. Express 17(1), 123–135 (2009).
[CrossRef] [PubMed]

S. Postma, A. C. W. van Rhijn, J. P. Korterik, P. Gross, J. L. Herek, and H. L. Offerhaus, “Application of spectral phase shaping to high resolution CARS spectroscopy,” Opt. Express 16(11), 7985–7996 (2008).
[CrossRef] [PubMed]

M. C. Fischer, H. C. Liu, I. R. Piletic, and W. S. Warren, “Simultaneous self-phase modulation and two-photon absorption measurement by a spectral homodyne Z-scan method,” Opt. Express 16(6), 4192–4205 (2008).
[CrossRef] [PubMed]

Opt. Lett.

I. R. Piletic, M. C. Fischer, P. Samineni, G. Yurtsever, and W. S. Warren, “Rapid pulse shaping with homodyne detection for measuring nonlinear optical signals,” Opt. Lett. 33(13), 1482–1484 (2008).
[CrossRef] [PubMed]

C. W. Hillegas, J. X. Tull, D. Goswami, D. Strickland, and W. S. Warren, “Femtosecond laser pulse shaping by use of microsecond radio-frequency pulses,” Opt. Lett. 19(10), 737–739 (1994).
[CrossRef] [PubMed]

S. H. Lim, A. G. Caster, and S. R. Leone, “Fourier transform spectral interferometric coherent anti-Stokes Raman scattering (FTSI-CARS) spectroscopy,” Opt. Lett. 32(10), 1332–1334 (2007).
[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 χ(3) for vibrational microscopy,” Opt. Lett. 29(24), 2923–2925 (2004).
[CrossRef]

M. Cui, B. R. Bachler, and J. P. Ogilvie, “Comparing coherent and spontaneous Raman scattering under biological imaging conditions,” Opt. Lett. 34(6), 773–775 (2009).
[CrossRef] [PubMed]

X. G. Xu, S. O. Konorov, J. W. Hepburn, and V. Milner, “Background-free coherent Raman spectroscopy by detecting the spectral phase of molecular vibrations,” Opt. Lett. 33(11), 1177–1179 (2008).
[CrossRef] [PubMed]

B. von Vacano, T. Buckup, and M. Motzkus, “Highly sensitive single-beam heterodyne coherent anti-Stokes Raman scattering,” Opt. Lett. 31(16), 2495–2497 (2006).
[CrossRef] [PubMed]

Phys. Med. Biol.

E. B. Hanlon, R. Manoharan, T. W. Koo, K. E. Shafer, J. T. Motz, M. Fitzmaurice, J. R. Kramer, I. Itzkan, R. R. Dasari, and M. S. Feld, “Prospects for in vivo Raman spectroscopy,” Phys. Med. Biol. 45(2), R1–R59 (2000).
[CrossRef] [PubMed]

Phys. Rev. Lett.

D. L. Marks and S. A. Boppart, “Nonlinear interferometric vibrational imaging,” Phys. Rev. Lett. 92(12), 123905 (2004).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Vibrational phase contrast microscopy by use of coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 103(4), 043905 (2009).
[CrossRef] [PubMed]

D. Oron, N. Dudovich, and Y. Silberberg, “Single-pulse phase-contrast nonlinear Raman spectroscopy,” Phys. Rev. Lett. 89(27), 273001 (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(6), 063004 (2002).
[CrossRef] [PubMed]

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 (6)

Fig. 1
Fig. 1

(a) Our approach uses a broadband pump/probe pulse with a narrowband region rotated rapidly in phase, and a narrowband Stokes pulse as discussed in the text. (b) Experimental setup for phase-cycling CARS. PS denotes the pulse shaper, F the tunable spectral filter, OPA the optical parametric amplifier, DC the dichroic mirror, and APD the avalanche photo diode.

Fig. 2
Fig. 2

(a) Narrow-band CARS spectrum obtained for 3 different benzene concentrations (15 μW pump power and 48 μW Stokes power). The signal was normalized by the signal of pure CS2. (b) The real and (c) the imaginary channel signal from phase-cycling CARS (50 μW pump power and 15 μW Stokes power). The signals were normalized by the real channel signal of pure CS2. Two absorptive peaks at 800 cm−1 and 1200 cm−1 are due to weak Raman transitions of CS2 and Benzene, respectively. In all cases the width of the peaks are determined by the spectral width of the pulses, not by the width of the Raman line (~1.5 cm−1).

Fig. 3
Fig. 3

(a) Dependence of the strength of the imaginary signal component at 1000 cm−1 (absorptive peak value) of phase-cycling CARS on the input Stokes and pump power. (b) Absorptive peak value of phase-cycling CARS as a function of benzene concentration in CS2. Linear fitting on a log-log scale results in a slope value of 1.05 ± 0.05.

Fig. 4
Fig. 4

Simulation (a) and experimental (b) data for a uniform rotating phase component. Simulation (c) and experimental (d) data for a rotating phase component that contains a π phase step. Insets in (a) and (c) show the phase profile of the rotating component. The sample was 20 vol-% benzene in CS2. For the simulation, only one Raman transition was considered.

Fig. 5
Fig. 5

Simulation of the phase-cycling CARS signal with a single (a) and multiple (b) Raman lines within the broad bandwidth of the pump/probe pulse.

Fig. 6
Fig. 6

Simulation of narrow-band and phase cycling CARS signal amplitudes. The spectral width (Stokes and pump in the narrow-band case, Stokes and phase rotating portion in the phase-cycling case) are relative to the width of the Raman line. The signal amplitudes are normalized by the factor E p 2 E s. The variations for low spectral widths for phase-cycling CARS are caused by the discrete values for the width of the local oscillator slice.

Equations (1)

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

S φ χ n r ( 3 ) A p 3 A φ A s 2 { [ 2 χ n r ( 3 ) + Re ( χ r ( 3 ) ( ω φ ω s ) ) ] cos ( φ ) + Im ( χ r ( 3 ) ( ω φ ω s ) ) sin ( φ ) }

Metrics