Abstract

To achieve high-spectral-resolution multiplex coherent anti-Stokes Raman scattering (CARS), one typically uses a narrowband pump pulse and a broadband Stokes pulse. This is to ensure a correspondence between anti-Stokes and vibrational frequencies. We obtain high-resolution CARS spectra of isopropanol, using a broadband chirped pump pulse and a broadband Stokes pulse, by detecting the anti-Stokes pulse with spectral interferometry. With the temporally resolved anti-Stokes signal, we can remove the chirp of the anti-Stokes pulse and restore high spectral resolution while also rejecting nonresonant scattering.

© 2006 Optical Society of America

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2004 (4)

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

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, Chem. Phys. Lett. 387, 436 (2004).
[CrossRef]

C. L. Evans, E. O. Potma, and X. S. Xie, Opt. Lett. 29, 2923 (2004).
[CrossRef]

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, Appl. Phys. Lett. 85, 5787 (2004).
[CrossRef]

2002 (2)

J.-X. Cheng, L. D. Book, and X. S. Xie, J. Phys. Chem. B 106, 8493 (2002).
[CrossRef]

G. W. H. Wurpel, J. M. Schins, and M. Muller, Opt. Lett. 27, 1093 (2002).
[CrossRef]

2001 (1)

C. Otto, A. Voroshilov, S. G. Kruglik, and J. Greve, J. Raman Spectrosc. 32, 495 (2001).
[CrossRef]

1999 (1)

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

1995 (1)

1982 (1)

Book, L. D.

J.-X. Cheng, L. D. Book, and X. S. Xie, J. Phys. Chem. B 106, 8493 (2002).
[CrossRef]

Boppart, S. A.

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

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, Appl. Phys. Lett. 85, 5787 (2004).
[CrossRef]

Bredfeldt, J. S.

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, Appl. Phys. Lett. 85, 5787 (2004).
[CrossRef]

Cheng, J.-X.

J.-X. Cheng, L. D. Book, and X. S. Xie, J. Phys. Chem. B 106, 8493 (2002).
[CrossRef]

Cheriaux, G.

Duncan, M. D.

Evans, C. L.

Greve, J.

C. Otto, A. Voroshilov, S. G. Kruglik, and J. Greve, J. Raman Spectrosc. 32, 495 (2001).
[CrossRef]

Holtom, G. R.

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

Joffre, M.

Johnson, J. C.

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, Chem. Phys. Lett. 387, 436 (2004).
[CrossRef]

Knutsen, K. P.

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, Chem. Phys. Lett. 387, 436 (2004).
[CrossRef]

Kruglik, S. G.

C. Otto, A. Voroshilov, S. G. Kruglik, and J. Greve, J. Raman Spectrosc. 32, 495 (2001).
[CrossRef]

Lepetit, L.

Mandel, L.

L. Mandel and E. Wolf, Optical Coherence and Quantum Optics (Cambridge U. Press, 1995).

Manuccia, T. J.

Marks, D. L.

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

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, Appl. Phys. Lett. 85, 5787 (2004).
[CrossRef]

Miller, A. E.

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, Chem. Phys. Lett. 387, 436 (2004).
[CrossRef]

Muller, M.

Otto, C.

C. Otto, A. Voroshilov, S. G. Kruglik, and J. Greve, J. Raman Spectrosc. 32, 495 (2001).
[CrossRef]

Petersen, P. B.

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, Chem. Phys. Lett. 387, 436 (2004).
[CrossRef]

Potma, E. O.

Reintjes, J.

Saykally, R. J.

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, Chem. Phys. Lett. 387, 436 (2004).
[CrossRef]

Schins, J. M.

Vinegoni, C.

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, Appl. Phys. Lett. 85, 5787 (2004).
[CrossRef]

Voroshilov, A.

C. Otto, A. Voroshilov, S. G. Kruglik, and J. Greve, J. Raman Spectrosc. 32, 495 (2001).
[CrossRef]

Wolf, E.

L. Mandel and E. Wolf, Optical Coherence and Quantum Optics (Cambridge U. Press, 1995).

Wurpel, G. W. H.

Xie, X. S.

C. L. Evans, E. O. Potma, and X. S. Xie, Opt. Lett. 29, 2923 (2004).
[CrossRef]

J.-X. Cheng, L. D. Book, and X. S. Xie, J. Phys. Chem. B 106, 8493 (2002).
[CrossRef]

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

Zumbusch, A.

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

Appl. Phys. Lett. (1)

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, Appl. Phys. Lett. 85, 5787 (2004).
[CrossRef]

Chem. Phys. Lett. (1)

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, Chem. Phys. Lett. 387, 436 (2004).
[CrossRef]

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

J. Phys. Chem. B (1)

J.-X. Cheng, L. D. Book, and X. S. Xie, J. Phys. Chem. B 106, 8493 (2002).
[CrossRef]

J. Raman Spectrosc. (1)

C. Otto, A. Voroshilov, S. G. Kruglik, and J. Greve, J. Raman Spectrosc. 32, 495 (2001).
[CrossRef]

Opt. Lett. (3)

Phys. Rev. Lett. (2)

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

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

Other (1)

L. Mandel and E. Wolf, Optical Coherence and Quantum Optics (Cambridge U. Press, 1995).

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Figures (4)

Fig. 1
Fig. 1

Illustration of multiplex CARS with (a) a narrowband pump pulse and (b) a chirped broadband pump pulse.

Fig. 2
Fig. 2

Schematic of the optical system.

Fig. 3
Fig. 3

(a) Power spectrum of the anti-Stokes pulse from isopropanol. (b) Spectral interferogram of the anti-Stokes pulse.

Fig. 4
Fig. 4

(a) P ( 3 ) ( t ) of isopropanol. (b) Re [ χ ̃ ( 3 ) ( Ω ) ] . The shaded area corresponds to negative values of Re [ χ ̃ ( 3 ) ( Ω ) ] , which otherwise is positive. (c) Im [ χ ̃ ( 3 ) ( Ω ) ] . The sign of Im [ χ ̃ ( 3 ) ( Ω ) ] is negative. The magnitude of the susceptibility is relative to (b). (d) The spontaneous Raman spectrum.

Equations (1)

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P ( 3 ) ( t ) = α 1 2 E ̃ 0 ( α t + ω 0 ) exp [ i ( α t 2 + ω 0 ) t ] ( 2 π ) 1 0 ω 0 d Ω χ ̃ ( 3 ) ( Ω ) E ̃ s ( ω 0 Ω ) E ̃ 0 ( ω 0 ) exp ( i Ω t ) .

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