Abstract

Detection of molecules using vibrational resonances in the fingerprint region for narrowband coherent anti-Stokes Raman scattering (CARS) is challenging. The spectrum is highly congested resulting in a large background and a reduced specificity. Recently we introduced vibrational phase contrast CARS (VPC-CARS) microscopy as a technique capable of detecting both the amplitude and phase of the CARS signal, providing background-free images and high specificity. In this paper we present a new implementation of VPC-CARS based on a third-order cascaded phase-preserving chain, where the CARS signal is generated at a single (constant) wavelength independent of the vibrational frequency that is addressed. This implementation will simplify the detection side considerably.

© 2011 Optical Society of America

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References

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  1. C. L. Evans and X. S. Xie, “Coherent anti-Stokes Raman scattering microscopy: chemical imaging for biology and medicine,” Annu. Rev. Anal. Chem. 1, 883–909 (2008).
    [CrossRef]
  2. Y. Yoo, D. Lee, and H. Cho, “Differential two-signal picosecond-pulse coherent anti-Stokes Raman scattering imaging microscopy by using a dualmode optical parametric oscillator,” Opt. Lett. 32, 3254–3256 (2007).
    [CrossRef] [PubMed]
  3. F. Ganikhanov, C. Evans, B. Saar, and X. Xie, “High-sensitivity vibrational imaging with frequency modulation coherent anti-Stokes Raman scattering (FM CARS) microscopy,” Opt. Lett. 31, 1872–1874 (2006).
    [CrossRef] [PubMed]
  4. G. Marowsky and G. Lüpke, “CARS-background suppression by phase-controlled nonlinear interferometry,” Appl. Phys. B 51, 49–51 (1990).
    [CrossRef]
  5. E. Potma, C. Evans, and X. Xie, “Heterodyne coherent anti-Stokes Raman scattering (CARS) imaging,” Opt. Lett. 31, 241–243 (2006).
    [CrossRef] [PubMed]
  6. M. Jurna, J. P. Korterik, C. Otto, and H. L. Offerhaus, “Shot noise limited heterodyne detection of CARS signals,” Opt. Express 15, 15207–15213 (2007).
    [CrossRef] [PubMed]
  7. M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Background-free CARS imaging by phase sensitive heterodyne CARS,” Opt. Express 16, 15863–15869(2008).
    [CrossRef] [PubMed]
  8. A. Volkmer, L. Book, and X. Xie, “Time-resolved coherent anti-Stokes Raman scattering microscopy: Imaging based on Raman free induction decay,” Appl. Phys. Lett. 80, 1505–1507 (2002).
    [CrossRef]
  9. A. Voroshilov, C. Otto, and J. Greve, “Secondary structure of bovine albumin as studied by polarization-sensitive multiplex CARS spectroscopy,” Appl. Spectrosc. 50, 78–85 (1996).
    [CrossRef]
  10. J. Cheng, L. Book, and X. Xie, “Polarization coherent anti-Stokes Raman scattering microscopy,” Opt. Lett. 26, 1341–1343 (2001).
    [CrossRef]
  11. M. Jurna, J. Korterik, C. Otto, J. Herek, and H. Offerhaus, “Vibrational phase contrast microscopy by use of coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 103, 043905(2009).
    [CrossRef] [PubMed]
  12. M. Jurna, E. T. Garbacik, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Visualizing resonances in the complex plane with vibrational phase contrast coherent anti-Stokes Raman scattering,” Anal. Chem. 82, 7656–7659 (2010).
    [CrossRef] [PubMed]
  13. P. Chen, “Rejection of background light using single-wavelength detection in nonlinear Raman spectroscopy,” Appl. Spectrosc. 51, 376–379 (1997).
    [CrossRef]
  14. Y. Fu, H. Wang, R. Shi, and J. Cheng, “Characterization of photodamage in coherent anti-Stokes Raman scattering microscopy,” Opt. Express 14, 3942–3951 (2006).
    [CrossRef] [PubMed]
  15. M. Balu, T. Baldacchini, J. Carter, T. Krasieva, R. Zadoyan, and B. Tromberg, “Effect of excitation wavelength on penetration depth in nonlinear optical microscopy of turbid media,” J. Biomed. Opt. 14, 010508 (2009).
    [CrossRef] [PubMed]
  16. C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322, 1857–1861 (2008).
    [CrossRef] [PubMed]

2010 (1)

M. Jurna, E. T. Garbacik, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Visualizing resonances in the complex plane with vibrational phase contrast coherent anti-Stokes Raman scattering,” Anal. Chem. 82, 7656–7659 (2010).
[CrossRef] [PubMed]

2009 (2)

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

M. Balu, T. Baldacchini, J. Carter, T. Krasieva, R. Zadoyan, and B. Tromberg, “Effect of excitation wavelength on penetration depth in nonlinear optical microscopy of turbid media,” J. Biomed. Opt. 14, 010508 (2009).
[CrossRef] [PubMed]

2008 (3)

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322, 1857–1861 (2008).
[CrossRef] [PubMed]

C. L. Evans and X. S. Xie, “Coherent anti-Stokes Raman scattering microscopy: chemical imaging for biology and medicine,” Annu. Rev. Anal. Chem. 1, 883–909 (2008).
[CrossRef]

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Background-free CARS imaging by phase sensitive heterodyne CARS,” Opt. Express 16, 15863–15869(2008).
[CrossRef] [PubMed]

2007 (2)

2006 (3)

2002 (1)

A. Volkmer, L. Book, and X. 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)

1997 (1)

1996 (1)

1990 (1)

G. Marowsky and G. Lüpke, “CARS-background suppression by phase-controlled nonlinear interferometry,” Appl. Phys. B 51, 49–51 (1990).
[CrossRef]

Baldacchini, T.

M. Balu, T. Baldacchini, J. Carter, T. Krasieva, R. Zadoyan, and B. Tromberg, “Effect of excitation wavelength on penetration depth in nonlinear optical microscopy of turbid media,” J. Biomed. Opt. 14, 010508 (2009).
[CrossRef] [PubMed]

Balu, M.

M. Balu, T. Baldacchini, J. Carter, T. Krasieva, R. Zadoyan, and B. Tromberg, “Effect of excitation wavelength on penetration depth in nonlinear optical microscopy of turbid media,” J. Biomed. Opt. 14, 010508 (2009).
[CrossRef] [PubMed]

Book, L.

A. Volkmer, L. Book, and X. 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. Cheng, L. Book, and X. Xie, “Polarization coherent anti-Stokes Raman scattering microscopy,” Opt. Lett. 26, 1341–1343 (2001).
[CrossRef]

Carter, J.

M. Balu, T. Baldacchini, J. Carter, T. Krasieva, R. Zadoyan, and B. Tromberg, “Effect of excitation wavelength on penetration depth in nonlinear optical microscopy of turbid media,” J. Biomed. Opt. 14, 010508 (2009).
[CrossRef] [PubMed]

Chen, P.

Cheng, J.

Cho, H.

Evans, C.

Evans, C. L.

C. L. Evans and X. S. Xie, “Coherent anti-Stokes Raman scattering microscopy: chemical imaging for biology and medicine,” Annu. Rev. Anal. Chem. 1, 883–909 (2008).
[CrossRef]

Freudiger, C. W.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322, 1857–1861 (2008).
[CrossRef] [PubMed]

Fu, Y.

Ganikhanov, F.

Garbacik, E. T.

M. Jurna, E. T. Garbacik, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Visualizing resonances in the complex plane with vibrational phase contrast coherent anti-Stokes Raman scattering,” Anal. Chem. 82, 7656–7659 (2010).
[CrossRef] [PubMed]

Greve, J.

He, C.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322, 1857–1861 (2008).
[CrossRef] [PubMed]

Herek, J.

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

Herek, J. L.

M. Jurna, E. T. Garbacik, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Visualizing resonances in the complex plane with vibrational phase contrast coherent anti-Stokes Raman scattering,” Anal. Chem. 82, 7656–7659 (2010).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Background-free CARS imaging by phase sensitive heterodyne CARS,” Opt. Express 16, 15863–15869(2008).
[CrossRef] [PubMed]

Holtom, G. R.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322, 1857–1861 (2008).
[CrossRef] [PubMed]

Jurna, M.

M. Jurna, E. T. Garbacik, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Visualizing resonances in the complex plane with vibrational phase contrast coherent anti-Stokes Raman scattering,” Anal. Chem. 82, 7656–7659 (2010).
[CrossRef] [PubMed]

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

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Background-free CARS imaging by phase sensitive heterodyne CARS,” Opt. Express 16, 15863–15869(2008).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, C. Otto, and H. L. Offerhaus, “Shot noise limited heterodyne detection of CARS signals,” Opt. Express 15, 15207–15213 (2007).
[CrossRef] [PubMed]

Kang, J. X.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322, 1857–1861 (2008).
[CrossRef] [PubMed]

Korterik, J.

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

Korterik, J. P.

Krasieva, T.

M. Balu, T. Baldacchini, J. Carter, T. Krasieva, R. Zadoyan, and B. Tromberg, “Effect of excitation wavelength on penetration depth in nonlinear optical microscopy of turbid media,” J. Biomed. Opt. 14, 010508 (2009).
[CrossRef] [PubMed]

Lee, D.

Lu, S.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322, 1857–1861 (2008).
[CrossRef] [PubMed]

Lüpke, G.

G. Marowsky and G. Lüpke, “CARS-background suppression by phase-controlled nonlinear interferometry,” Appl. Phys. B 51, 49–51 (1990).
[CrossRef]

Marowsky, G.

G. Marowsky and G. Lüpke, “CARS-background suppression by phase-controlled nonlinear interferometry,” Appl. Phys. B 51, 49–51 (1990).
[CrossRef]

Min, W.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322, 1857–1861 (2008).
[CrossRef] [PubMed]

Offerhaus, H.

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

Offerhaus, H. L.

Otto, C.

M. Jurna, E. T. Garbacik, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Visualizing resonances in the complex plane with vibrational phase contrast coherent anti-Stokes Raman scattering,” Anal. Chem. 82, 7656–7659 (2010).
[CrossRef] [PubMed]

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

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Background-free CARS imaging by phase sensitive heterodyne CARS,” Opt. Express 16, 15863–15869(2008).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, C. Otto, and H. L. Offerhaus, “Shot noise limited heterodyne detection of CARS signals,” Opt. Express 15, 15207–15213 (2007).
[CrossRef] [PubMed]

A. Voroshilov, C. Otto, and J. Greve, “Secondary structure of bovine albumin as studied by polarization-sensitive multiplex CARS spectroscopy,” Appl. Spectrosc. 50, 78–85 (1996).
[CrossRef]

Potma, E.

Saar, B.

Saar, B. G.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322, 1857–1861 (2008).
[CrossRef] [PubMed]

Shi, R.

Tromberg, B.

M. Balu, T. Baldacchini, J. Carter, T. Krasieva, R. Zadoyan, and B. Tromberg, “Effect of excitation wavelength on penetration depth in nonlinear optical microscopy of turbid media,” J. Biomed. Opt. 14, 010508 (2009).
[CrossRef] [PubMed]

Tsai, J. C.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322, 1857–1861 (2008).
[CrossRef] [PubMed]

Volkmer, A.

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

Voroshilov, A.

Wang, H.

Xie, X.

Xie, X. S.

C. L. Evans and X. S. Xie, “Coherent anti-Stokes Raman scattering microscopy: chemical imaging for biology and medicine,” Annu. Rev. Anal. Chem. 1, 883–909 (2008).
[CrossRef]

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322, 1857–1861 (2008).
[CrossRef] [PubMed]

Yoo, Y.

Zadoyan, R.

M. Balu, T. Baldacchini, J. Carter, T. Krasieva, R. Zadoyan, and B. Tromberg, “Effect of excitation wavelength on penetration depth in nonlinear optical microscopy of turbid media,” J. Biomed. Opt. 14, 010508 (2009).
[CrossRef] [PubMed]

Anal. Chem. (1)

M. Jurna, E. T. Garbacik, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, “Visualizing resonances in the complex plane with vibrational phase contrast coherent anti-Stokes Raman scattering,” Anal. Chem. 82, 7656–7659 (2010).
[CrossRef] [PubMed]

Annu. Rev. Anal. Chem. (1)

C. L. Evans and X. S. Xie, “Coherent anti-Stokes Raman scattering microscopy: chemical imaging for biology and medicine,” Annu. Rev. Anal. Chem. 1, 883–909 (2008).
[CrossRef]

Appl. Phys. B (1)

G. Marowsky and G. Lüpke, “CARS-background suppression by phase-controlled nonlinear interferometry,” Appl. Phys. B 51, 49–51 (1990).
[CrossRef]

Appl. Phys. Lett. (1)

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

Appl. Spectrosc. (2)

J. Biomed. Opt. (1)

M. Balu, T. Baldacchini, J. Carter, T. Krasieva, R. Zadoyan, and B. Tromberg, “Effect of excitation wavelength on penetration depth in nonlinear optical microscopy of turbid media,” J. Biomed. Opt. 14, 010508 (2009).
[CrossRef] [PubMed]

Opt. Express (3)

Opt. Lett. (4)

Phys. Rev. Lett. (1)

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

Science (1)

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322, 1857–1861 (2008).
[CrossRef] [PubMed]

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Figures (3)

Fig. 1
Fig. 1

Schematic of the second-order cascaded phase-preserving chain showing the laser, OPO, and CARS process, where (a) shows the heterodyne phase detection scheme and (b) shows the local excitation phase detection scheme. F, fundamental laser; F*, modulated fundamental laser; I, OPO idler; S, OPO signal; C, CARS signal; HP, heterodyne phase; and EP, excitation phase. The table shows the wavelength and phase relations within the heterodyne detection scheme.

Fig. 2
Fig. 2

Schematic of the third-order cascaded phase-preserving chain showing the laser, OPO, and CARS process, where (a) shows the heterodyne phase detection scheme and (b) shows the local excitation phase detection scheme. F, fundamental laser; F*, modulated fundamental laser; 2F, second harmonic of the laser; I, OPO idler; S, OPO signal; C, CARS signal; HP, heterodyne phase; and EP, excitation phase. The table shows the wavelength and phase relations within the heterodyne detection scheme.

Fig. 3
Fig. 3

OPO tuning curves. The OPO signal and idler wavelengths (left axis) are plotted as a function of crystal temperature. Also shown in the resulting H-CARS and local EP-CARS signals. The addressed Raman shift as a function of crystal temperature is plotted on the right axis. (a) Second-order chain and (b) third-order chain. F, 2F, and 3F are the fundamental, second harmonic, and third harmonic wavelength of the laser, respectively.

Equations (1)

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λ F > λ OPO idler > λ OPO signal > λ H - CARS > λ EP - CARS .

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