Abstract

We report on the realization of a sensitive microspectroscopy and imaging approach based on a three-color femtosecond coherent anti-Stokes Raman scattering (CARS) technique with high spectral, time, and spatial resolution. Independently tunable, high-repetition rate optical parametric oscillators were used to attain a dynamic range of 5 orders of magnitude for time-domain CARS signal. The attained sensitivity permitted tracing the decay of weak and structurally complex Raman active modes in soft condensed matter. Application of this approach to imaging of the biological specimen shows a great potential in quantitative characterization of live biological media with an ability to access inter- and intra-molecular interactions.

© 2011 Optical Society of America

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  1. N. Uzunbajakava, A. Lenferink, Y. Kraan, E. Volokhina, G. Vrensen, J. Greve, and C. Otto, Biophys. J. 84, 3968(2003).
    [CrossRef] [PubMed]
  2. A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
    [CrossRef]
  3. T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, Proc. Natl. Acad. Sci. USA 104, 14658(2007).
    [CrossRef] [PubMed]
  4. T. W. Kee and M. T. Cicerone, Opt. Lett. 29, 2701 (2004).
    [CrossRef] [PubMed]
  5. E. Ploetz, S. Laimgruber, S. Berner, W. Zinth, and P. Gilch, Appl. Phys. B 87, 389 (2007).
    [CrossRef]
  6. 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, Science 322, 1857(2008).
    [CrossRef] [PubMed]
  7. G. I. Petrov, R. Arora, V. V. Yakovlev, X. Wang, A. V. Sokolov, and M. O. Scully, Proc. Natl. Acad. Sci. USA 104, 7776 (2007).
    [CrossRef] [PubMed]
  8. A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
    [CrossRef]
  9. D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, Phys. Rev. Lett. 88, 63004 (2002).
    [CrossRef]
  10. Y. J. Lee and M. T. Cicerone, Appl. Phys. Lett. 92, 041108(2008).
    [CrossRef]
  11. A. Lauberau and W. Kaiser, Rev. Mod. Phys. 50, 607 (1978).
    [CrossRef]
  12. Y. R. Shen, The Principles of Nonlinear Optics (Wiley, 2003).
  13. N. Abe, M. Wakayama, and M. Ito, J. Raman Spectrosc. 6, 38 (1977).
    [CrossRef]
  14. J. D. Rowley, S. Yang, and F. Ganikhanov, J. Opt. Soc. Am. B 28, 1026 (2011).
    [CrossRef]
  15. A. M. K. Enejder, T. G. Scecin, J. Oh, M. Hunter, W. Shi, S. Sasi, G. L. Horowit, and M. S. Feld, J. Biomed. Opt. 10, 031114 (2005).
    [CrossRef] [PubMed]
  16. R. M. El-Abassy, P. Donfack, and A. Materny, J. Raman Spectrosc. 40, 1284 (2009).
    [CrossRef]

2011 (1)

2009 (1)

R. M. El-Abassy, P. Donfack, and A. Materny, J. Raman Spectrosc. 40, 1284 (2009).
[CrossRef]

2008 (2)

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, Science 322, 1857(2008).
[CrossRef] [PubMed]

Y. J. Lee and M. T. Cicerone, Appl. Phys. Lett. 92, 041108(2008).
[CrossRef]

2007 (3)

G. I. Petrov, R. Arora, V. V. Yakovlev, X. Wang, A. V. Sokolov, and M. O. Scully, Proc. Natl. Acad. Sci. USA 104, 7776 (2007).
[CrossRef] [PubMed]

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, Proc. Natl. Acad. Sci. USA 104, 14658(2007).
[CrossRef] [PubMed]

E. Ploetz, S. Laimgruber, S. Berner, W. Zinth, and P. Gilch, Appl. Phys. B 87, 389 (2007).
[CrossRef]

2005 (1)

A. M. K. Enejder, T. G. Scecin, J. Oh, M. Hunter, W. Shi, S. Sasi, G. L. Horowit, and M. S. Feld, J. Biomed. Opt. 10, 031114 (2005).
[CrossRef] [PubMed]

2004 (1)

2003 (1)

N. Uzunbajakava, A. Lenferink, Y. Kraan, E. Volokhina, G. Vrensen, J. Greve, and C. Otto, Biophys. J. 84, 3968(2003).
[CrossRef] [PubMed]

2002 (2)

A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
[CrossRef]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, Phys. Rev. Lett. 88, 63004 (2002).
[CrossRef]

1999 (1)

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

1978 (1)

A. Lauberau and W. Kaiser, Rev. Mod. Phys. 50, 607 (1978).
[CrossRef]

1977 (1)

N. Abe, M. Wakayama, and M. Ito, J. Raman Spectrosc. 6, 38 (1977).
[CrossRef]

Abe, N.

N. Abe, M. Wakayama, and M. Ito, J. Raman Spectrosc. 6, 38 (1977).
[CrossRef]

Arora, R.

G. I. Petrov, R. Arora, V. V. Yakovlev, X. Wang, A. V. Sokolov, and M. O. Scully, Proc. Natl. Acad. Sci. USA 104, 7776 (2007).
[CrossRef] [PubMed]

Axäng, C.

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, Proc. Natl. Acad. Sci. USA 104, 14658(2007).
[CrossRef] [PubMed]

Berner, S.

E. Ploetz, S. Laimgruber, S. Berner, W. Zinth, and P. Gilch, Appl. Phys. B 87, 389 (2007).
[CrossRef]

Book, L. D.

A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
[CrossRef]

Brackmann, C.

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, Proc. Natl. Acad. Sci. USA 104, 14658(2007).
[CrossRef] [PubMed]

Cicerone, M. T.

Y. J. Lee and M. T. Cicerone, Appl. Phys. Lett. 92, 041108(2008).
[CrossRef]

T. W. Kee and M. T. Cicerone, Opt. Lett. 29, 2701 (2004).
[CrossRef] [PubMed]

Donfack, P.

R. M. El-Abassy, P. Donfack, and A. Materny, J. Raman Spectrosc. 40, 1284 (2009).
[CrossRef]

Dudovich, N.

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, Phys. Rev. Lett. 88, 63004 (2002).
[CrossRef]

El-Abassy, R. M.

R. M. El-Abassy, P. Donfack, and A. Materny, J. Raman Spectrosc. 40, 1284 (2009).
[CrossRef]

Enejder, A.

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, Proc. Natl. Acad. Sci. USA 104, 14658(2007).
[CrossRef] [PubMed]

Enejder, A. M. K.

A. M. K. Enejder, T. G. Scecin, J. Oh, M. Hunter, W. Shi, S. Sasi, G. L. Horowit, and M. S. Feld, J. Biomed. Opt. 10, 031114 (2005).
[CrossRef] [PubMed]

Feld, M. S.

A. M. K. Enejder, T. G. Scecin, J. Oh, M. Hunter, W. Shi, S. Sasi, G. L. Horowit, and M. S. Feld, J. Biomed. Opt. 10, 031114 (2005).
[CrossRef] [PubMed]

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, Science 322, 1857(2008).
[CrossRef] [PubMed]

Ganikhanov, F.

Gilch, P.

E. Ploetz, S. Laimgruber, S. Berner, W. Zinth, and P. Gilch, Appl. Phys. B 87, 389 (2007).
[CrossRef]

Greve, J.

N. Uzunbajakava, A. Lenferink, Y. Kraan, E. Volokhina, G. Vrensen, J. Greve, and C. Otto, Biophys. J. 84, 3968(2003).
[CrossRef] [PubMed]

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, Science 322, 1857(2008).
[CrossRef] [PubMed]

Hellerer, T.

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, Proc. Natl. Acad. Sci. USA 104, 14658(2007).
[CrossRef] [PubMed]

Hillertz, P.

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, Proc. Natl. Acad. Sci. USA 104, 14658(2007).
[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, Science 322, 1857(2008).
[CrossRef] [PubMed]

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

Horowit, G. L.

A. M. K. Enejder, T. G. Scecin, J. Oh, M. Hunter, W. Shi, S. Sasi, G. L. Horowit, and M. S. Feld, J. Biomed. Opt. 10, 031114 (2005).
[CrossRef] [PubMed]

Hunter, M.

A. M. K. Enejder, T. G. Scecin, J. Oh, M. Hunter, W. Shi, S. Sasi, G. L. Horowit, and M. S. Feld, J. Biomed. Opt. 10, 031114 (2005).
[CrossRef] [PubMed]

Ito, M.

N. Abe, M. Wakayama, and M. Ito, J. Raman Spectrosc. 6, 38 (1977).
[CrossRef]

Kaiser, W.

A. Lauberau and W. Kaiser, Rev. Mod. Phys. 50, 607 (1978).
[CrossRef]

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, Science 322, 1857(2008).
[CrossRef] [PubMed]

Kee, T. W.

Kraan, Y.

N. Uzunbajakava, A. Lenferink, Y. Kraan, E. Volokhina, G. Vrensen, J. Greve, and C. Otto, Biophys. J. 84, 3968(2003).
[CrossRef] [PubMed]

Laimgruber, S.

E. Ploetz, S. Laimgruber, S. Berner, W. Zinth, and P. Gilch, Appl. Phys. B 87, 389 (2007).
[CrossRef]

Lauberau, A.

A. Lauberau and W. Kaiser, Rev. Mod. Phys. 50, 607 (1978).
[CrossRef]

Lee, Y. J.

Y. J. Lee and M. T. Cicerone, Appl. Phys. Lett. 92, 041108(2008).
[CrossRef]

Lenferink, A.

N. Uzunbajakava, A. Lenferink, Y. Kraan, E. Volokhina, G. Vrensen, J. Greve, and C. Otto, Biophys. J. 84, 3968(2003).
[CrossRef] [PubMed]

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, Science 322, 1857(2008).
[CrossRef] [PubMed]

Materny, A.

R. M. El-Abassy, P. Donfack, and A. Materny, J. Raman Spectrosc. 40, 1284 (2009).
[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, Science 322, 1857(2008).
[CrossRef] [PubMed]

Oh, J.

A. M. K. Enejder, T. G. Scecin, J. Oh, M. Hunter, W. Shi, S. Sasi, G. L. Horowit, and M. S. Feld, J. Biomed. Opt. 10, 031114 (2005).
[CrossRef] [PubMed]

Oron, D.

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, Phys. Rev. Lett. 88, 63004 (2002).
[CrossRef]

Otto, C.

N. Uzunbajakava, A. Lenferink, Y. Kraan, E. Volokhina, G. Vrensen, J. Greve, and C. Otto, Biophys. J. 84, 3968(2003).
[CrossRef] [PubMed]

Petrov, G. I.

G. I. Petrov, R. Arora, V. V. Yakovlev, X. Wang, A. V. Sokolov, and M. O. Scully, Proc. Natl. Acad. Sci. USA 104, 7776 (2007).
[CrossRef] [PubMed]

Pilon, M.

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, Proc. Natl. Acad. Sci. USA 104, 14658(2007).
[CrossRef] [PubMed]

Ploetz, E.

E. Ploetz, S. Laimgruber, S. Berner, W. Zinth, and P. Gilch, Appl. Phys. B 87, 389 (2007).
[CrossRef]

Rowley, J. D.

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, Science 322, 1857(2008).
[CrossRef] [PubMed]

Sasi, S.

A. M. K. Enejder, T. G. Scecin, J. Oh, M. Hunter, W. Shi, S. Sasi, G. L. Horowit, and M. S. Feld, J. Biomed. Opt. 10, 031114 (2005).
[CrossRef] [PubMed]

Scecin, T. G.

A. M. K. Enejder, T. G. Scecin, J. Oh, M. Hunter, W. Shi, S. Sasi, G. L. Horowit, and M. S. Feld, J. Biomed. Opt. 10, 031114 (2005).
[CrossRef] [PubMed]

Scully, M. O.

G. I. Petrov, R. Arora, V. V. Yakovlev, X. Wang, A. V. Sokolov, and M. O. Scully, Proc. Natl. Acad. Sci. USA 104, 7776 (2007).
[CrossRef] [PubMed]

Shen, Y. R.

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, 2003).

Shi, W.

A. M. K. Enejder, T. G. Scecin, J. Oh, M. Hunter, W. Shi, S. Sasi, G. L. Horowit, and M. S. Feld, J. Biomed. Opt. 10, 031114 (2005).
[CrossRef] [PubMed]

Silberberg, Y.

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, Phys. Rev. Lett. 88, 63004 (2002).
[CrossRef]

Sokolov, A. V.

G. I. Petrov, R. Arora, V. V. Yakovlev, X. Wang, A. V. Sokolov, and M. O. Scully, Proc. Natl. Acad. Sci. USA 104, 7776 (2007).
[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, Science 322, 1857(2008).
[CrossRef] [PubMed]

Uzunbajakava, N.

N. Uzunbajakava, A. Lenferink, Y. Kraan, E. Volokhina, G. Vrensen, J. Greve, and C. Otto, Biophys. J. 84, 3968(2003).
[CrossRef] [PubMed]

Volkmer, A.

A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
[CrossRef]

Volokhina, E.

N. Uzunbajakava, A. Lenferink, Y. Kraan, E. Volokhina, G. Vrensen, J. Greve, and C. Otto, Biophys. J. 84, 3968(2003).
[CrossRef] [PubMed]

Vrensen, G.

N. Uzunbajakava, A. Lenferink, Y. Kraan, E. Volokhina, G. Vrensen, J. Greve, and C. Otto, Biophys. J. 84, 3968(2003).
[CrossRef] [PubMed]

Wakayama, M.

N. Abe, M. Wakayama, and M. Ito, J. Raman Spectrosc. 6, 38 (1977).
[CrossRef]

Wang, X.

G. I. Petrov, R. Arora, V. V. Yakovlev, X. Wang, A. V. Sokolov, and M. O. Scully, Proc. Natl. Acad. Sci. USA 104, 7776 (2007).
[CrossRef] [PubMed]

Xie, X. 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, Science 322, 1857(2008).
[CrossRef] [PubMed]

A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
[CrossRef]

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

Yakovlev, V. V.

G. I. Petrov, R. Arora, V. V. Yakovlev, X. Wang, A. V. Sokolov, and M. O. Scully, Proc. Natl. Acad. Sci. USA 104, 7776 (2007).
[CrossRef] [PubMed]

Yang, S.

Yelin, D.

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, Phys. Rev. Lett. 88, 63004 (2002).
[CrossRef]

Zinth, W.

E. Ploetz, S. Laimgruber, S. Berner, W. Zinth, and P. Gilch, Appl. Phys. B 87, 389 (2007).
[CrossRef]

Zumbusch, A.

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

Appl. Phys. B (1)

E. Ploetz, S. Laimgruber, S. Berner, W. Zinth, and P. Gilch, Appl. Phys. B 87, 389 (2007).
[CrossRef]

Appl. Phys. Lett. (2)

A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
[CrossRef]

Y. J. Lee and M. T. Cicerone, Appl. Phys. Lett. 92, 041108(2008).
[CrossRef]

Biophys. J. (1)

N. Uzunbajakava, A. Lenferink, Y. Kraan, E. Volokhina, G. Vrensen, J. Greve, and C. Otto, Biophys. J. 84, 3968(2003).
[CrossRef] [PubMed]

J. Biomed. Opt. (1)

A. M. K. Enejder, T. G. Scecin, J. Oh, M. Hunter, W. Shi, S. Sasi, G. L. Horowit, and M. S. Feld, J. Biomed. Opt. 10, 031114 (2005).
[CrossRef] [PubMed]

J. Opt. Soc. Am. B (1)

J. Raman Spectrosc. (2)

R. M. El-Abassy, P. Donfack, and A. Materny, J. Raman Spectrosc. 40, 1284 (2009).
[CrossRef]

N. Abe, M. Wakayama, and M. Ito, J. Raman Spectrosc. 6, 38 (1977).
[CrossRef]

Opt. Lett. (1)

Phys. Rev. Lett. (2)

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, Phys. Rev. Lett. 88, 63004 (2002).
[CrossRef]

Proc. Natl. Acad. Sci. USA (2)

G. I. Petrov, R. Arora, V. V. Yakovlev, X. Wang, A. V. Sokolov, and M. O. Scully, Proc. Natl. Acad. Sci. USA 104, 7776 (2007).
[CrossRef] [PubMed]

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, Proc. Natl. Acad. Sci. USA 104, 14658(2007).
[CrossRef] [PubMed]

Rev. Mod. Phys. (1)

A. Lauberau and W. Kaiser, Rev. Mod. Phys. 50, 607 (1978).
[CrossRef]

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, Science 322, 1857(2008).
[CrossRef] [PubMed]

Other (1)

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, 2003).

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Figures (4)

Fig. 1
Fig. 1

Schematic of the experimental setup. Time-domain CARS process involved two OPO pulses at tunable ω 1 and ω 2 optical frequencies used to coherently excite Raman active vibrations while a delayed replica of Ti:sapphire pulse at ω pr was used to probe the coherence in the focal plane of the objective lens (OBJ). BS: beamsplitter mirrors. P1 and P2: external dispersive prisms used for pulse precompensation. DM: dichroic mirrors. SM: galvo scanner mirrors, CL: condenser lens. GR: diffraction grating.

Fig. 2
Fig. 2

(a) Time-domain CARS signal generated in microscope coverglass taken at a condition when the OPO wavelengths were set to 965 nm and 1098 nm , respectively (i.e., ω 1 ω 2 1250 cm 1 ). Transients shown in lines were calculated using convolution integral for time-domain CARS signal [11] assuming T 2 = 100 fs (solid line) and 150 fs (dotted line). (b) Time-domain CARS signal obtained from a glucose solution. The measured dephasing time of 660 fs corresponds to 16.1 cm 1 wide homogeneously broadened line in frequency domain. (c) A more complex case of probing fairly weak vibrational resonances in oil near Ω R 1280 cm 1 is shown.

Fig. 3
Fig. 3

(a) CARS image ( 3.5 × 2.5 μm 2 ) of 1 μm diameter polystyrene beads is shown when a cluster of weak Raman lines near 880 cm 1 is excited and probed at 0 fs delay time. (b) The same image is shown for time delay of 380 fs . (c) Image ( 8.5 × 6.5 μm 2 ) of Escherichia coli cells at a time delay of 400 fs with greatly reduced background at OPO wavelengths setting when ω 1 ω 2 1007 cm 1 . At this setting Raman active vibration near Ω R = 1004 cm 1 (phenylalanine line) was efficiently excited and probed. Distance between successive pixels on the images is 210 nm .

Fig. 4
Fig. 4

(a) Image ( 50 × 70 μm 2 ) of a human blood sample at 1180 cm 1 and t d = 200 fs showing densely packed red blood cells with noticeably high resonant CARS signal areas. (b) CARS transient taken on the sample (see text).

Equations (2)

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I CARS max = ( 16 π 2 c 2 ω as 3 n 2 h Γ N L σ R ) 2 I 1 I 2 I pr ,
I CARS ( t d ) e 2 t d T 2 | j A j e i ( ω 1 ω 2 Ω R j ) t d | 2 ,

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