Abstract

We demonstrate circularly polarized coherent anti-Stokes Raman scattering (CP-CARS) microscopy that significantly suppresses the nonresonant background for high-contrast vibrational imaging. Circularly polarized pump and Stokes fields with opposite handedness are used to excite CARS signal. In this case, theoretically the nonresonant CARS signal and resonant CARS signal from isotropic media will completely vanish, while the resonant CARS signal from anisotropic structures can still exist. This allows CARS imaging of anisotropic samples with enhanced resonant contrast. Furthermore, we performed CP-CARS imaging on fibroin fibers from silkworm silk, and the results confirmed its effectiveness in background suppression.

© 2013 Optical Society of America

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References

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  1. A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
    [CrossRef]
  2. J. X. Cheng, L. D. Book, and X. S. Xie, Opt. Lett. 26, 1341 (2001).
    [CrossRef]
  3. F. Lu, W. Zheng, and Z. Huang, Opt. Lett. 33, 2842 (2008).
    [CrossRef]
  4. A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
    [CrossRef]
  5. E. O. Potma, C. L. Evans, and X. S. Xie, Opt. Lett. 31, 241 (2006).
    [CrossRef]
  6. F. Lu, W. Zheng, C. Sheppard, and Z. Huang, Opt. Lett. 33, 602 (2008).
    [CrossRef]
  7. N. Dudovich, D. Oron, and Y. Silberberg, Nature 418, 512 (2002).
    [CrossRef]
  8. R. W. Boyd, Nonlinear Optics (Academic, 2003).
  9. M. D. Levenson and S. S. Kano, Introduction to Nonlinear Laser Spectroscopy (Academic, 1988).
  10. X. Hu, D. Kaplan, and P. Cebe, Macromolecules 39, 6161 (2006).
    [CrossRef]
  11. M.-E. Rousseau, T. Lefèvre, L. Beaulieu, T. Asakura, and M. Pézolet, Biomacromolecules 5, 2247 (2004).
    [CrossRef]
  12. M. Dwivedi and S. Krimm, Macromolecules 15, 186 (1982).
    [CrossRef]
  13. Y. Takahashi, M. Gehoh, and K. Yuzuriha, J. Polym. Sci. 29, 889 (1991).

2008 (2)

2006 (2)

X. Hu, D. Kaplan, and P. Cebe, Macromolecules 39, 6161 (2006).
[CrossRef]

E. O. Potma, C. L. Evans, and X. S. Xie, Opt. Lett. 31, 241 (2006).
[CrossRef]

2004 (1)

M.-E. Rousseau, T. Lefèvre, L. Beaulieu, T. Asakura, and M. Pézolet, Biomacromolecules 5, 2247 (2004).
[CrossRef]

2002 (2)

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

N. Dudovich, D. Oron, and Y. Silberberg, Nature 418, 512 (2002).
[CrossRef]

2001 (1)

1999 (1)

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

1991 (1)

Y. Takahashi, M. Gehoh, and K. Yuzuriha, J. Polym. Sci. 29, 889 (1991).

1982 (1)

M. Dwivedi and S. Krimm, Macromolecules 15, 186 (1982).
[CrossRef]

Asakura, T.

M.-E. Rousseau, T. Lefèvre, L. Beaulieu, T. Asakura, and M. Pézolet, Biomacromolecules 5, 2247 (2004).
[CrossRef]

Beaulieu, L.

M.-E. Rousseau, T. Lefèvre, L. Beaulieu, T. Asakura, and M. Pézolet, Biomacromolecules 5, 2247 (2004).
[CrossRef]

Book, L. D.

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

J. X. Cheng, L. D. Book, and X. S. Xie, Opt. Lett. 26, 1341 (2001).
[CrossRef]

Boyd, R. W.

R. W. Boyd, Nonlinear Optics (Academic, 2003).

Cebe, P.

X. Hu, D. Kaplan, and P. Cebe, Macromolecules 39, 6161 (2006).
[CrossRef]

Cheng, J. X.

Dudovich, N.

N. Dudovich, D. Oron, and Y. Silberberg, Nature 418, 512 (2002).
[CrossRef]

Dwivedi, M.

M. Dwivedi and S. Krimm, Macromolecules 15, 186 (1982).
[CrossRef]

Evans, C. L.

Gehoh, M.

Y. Takahashi, M. Gehoh, and K. Yuzuriha, J. Polym. Sci. 29, 889 (1991).

Holtom, G. R.

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

Hu, X.

X. Hu, D. Kaplan, and P. Cebe, Macromolecules 39, 6161 (2006).
[CrossRef]

Huang, Z.

Kano, S. S.

M. D. Levenson and S. S. Kano, Introduction to Nonlinear Laser Spectroscopy (Academic, 1988).

Kaplan, D.

X. Hu, D. Kaplan, and P. Cebe, Macromolecules 39, 6161 (2006).
[CrossRef]

Krimm, S.

M. Dwivedi and S. Krimm, Macromolecules 15, 186 (1982).
[CrossRef]

Lefèvre, T.

M.-E. Rousseau, T. Lefèvre, L. Beaulieu, T. Asakura, and M. Pézolet, Biomacromolecules 5, 2247 (2004).
[CrossRef]

Levenson, M. D.

M. D. Levenson and S. S. Kano, Introduction to Nonlinear Laser Spectroscopy (Academic, 1988).

Lu, F.

Oron, D.

N. Dudovich, D. Oron, and Y. Silberberg, Nature 418, 512 (2002).
[CrossRef]

Pézolet, M.

M.-E. Rousseau, T. Lefèvre, L. Beaulieu, T. Asakura, and M. Pézolet, Biomacromolecules 5, 2247 (2004).
[CrossRef]

Potma, E. O.

Rousseau, M.-E.

M.-E. Rousseau, T. Lefèvre, L. Beaulieu, T. Asakura, and M. Pézolet, Biomacromolecules 5, 2247 (2004).
[CrossRef]

Sheppard, C.

Silberberg, Y.

N. Dudovich, D. Oron, and Y. Silberberg, Nature 418, 512 (2002).
[CrossRef]

Takahashi, Y.

Y. Takahashi, M. Gehoh, and K. Yuzuriha, J. Polym. Sci. 29, 889 (1991).

Volkmer, A.

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

Xie, X. S.

E. O. Potma, C. L. Evans, and X. S. Xie, Opt. Lett. 31, 241 (2006).
[CrossRef]

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

J. X. Cheng, L. D. Book, and X. S. Xie, Opt. Lett. 26, 1341 (2001).
[CrossRef]

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

Yuzuriha, K.

Y. Takahashi, M. Gehoh, and K. Yuzuriha, J. Polym. Sci. 29, 889 (1991).

Zheng, W.

Zumbusch, A.

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

Appl. Phys. Lett. (1)

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

Biomacromolecules (1)

M.-E. Rousseau, T. Lefèvre, L. Beaulieu, T. Asakura, and M. Pézolet, Biomacromolecules 5, 2247 (2004).
[CrossRef]

J. Polym. Sci. (1)

Y. Takahashi, M. Gehoh, and K. Yuzuriha, J. Polym. Sci. 29, 889 (1991).

Macromolecules (2)

M. Dwivedi and S. Krimm, Macromolecules 15, 186 (1982).
[CrossRef]

X. Hu, D. Kaplan, and P. Cebe, Macromolecules 39, 6161 (2006).
[CrossRef]

Nature (1)

N. Dudovich, D. Oron, and Y. Silberberg, Nature 418, 512 (2002).
[CrossRef]

Opt. Lett. (4)

Phys. Rev. Lett. (1)

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

Other (2)

R. W. Boyd, Nonlinear Optics (Academic, 2003).

M. D. Levenson and S. S. Kano, Introduction to Nonlinear Laser Spectroscopy (Academic, 1988).

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Figures (3)

Fig. 1.
Fig. 1.

Schematic of the CP-CARS microscope: M, mirror; OPO, optical parametric oscillator; VA, variable attenuator; T, telescope; HWP, half-wave plate; QWP, quarter-wave plate; DL, delay line; DM, dichroic mirror.

Fig. 2.
Fig. 2.

F-CARS images of 3 μm polystyrene beads on a cover glass. (a)–(c) Nonresonant images at 2000cm1. (d)–(f) Resonant images at 3050cm1. AOI, area of interest.

Fig. 3.
Fig. 3.

F-CARS images of a fibroin fiber embedded in a fibroin film. (a)–(c) Nonresonant images at 2000cm1. (d)–(f) Resonant images of symmetric CH3 stretching at 2938cm1. (g)–(i) Line profiles for (d)–(f) after normalization with excitation powers.

Equations (5)

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

Pi(3)(ωout)=jkl(abc)χijkl(3)(ωout;ωa,ωb,ωc)Ej(ωa)Ek(ωb)El(ωc),
Px=3(χ1111(3)χ1122(3)χ1221(3)χ1212(3))Epx2Esx*,
Py=3i(χ2222(3)χ2211(3)χ2112(3)χ2121(3))Epx2Esx*.
χ2222(3)=χ2211(3)+χ2112(3)+χ2121(3),
χ1111(3)=χ1122(3)+χ1221(3)+χ1212(3).

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