Abstract

We propose and demonstrate a new approach to subtracting high nonresonant background in coherent anti-Stokes Raman scattering spectroscopy. The method is based on the retrieval of the spectral phase of molecular vibrations using the technique of frequency-resolved optical gating of Raman scattering. In the presence of high nonresonant background the retrieved phase corresponds directly to the background-free spectrum of the coherent Raman response.

© 2008 Optical Society of America

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2007 (4)

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[Crossref] [PubMed]

S. O. Konorov, R. F. B. Turner, and M. W. Blades, Appl. Spectrosc. 61, 486 (2007).
[Crossref] [PubMed]

X. J. G. Xu, S. O. Konorov, S. Zhdanovich, J. W. Hepburn, and V. Milner, J. Chem. Phys. 126, 091102 (2007).
[Crossref] [PubMed]

S. O. Konorov, X. G. Xu, R. F. Turner, M. W. Blades, J. W. Hepburn, and V. Milner, Opt. Express 15, 7564 (2007).
[Crossref] [PubMed]

2006 (2)

2005 (1)

S. H. Lim, A. G. Caster, and S. R. Leone, Phys. Rev. A 72, 041803 (2005).
[Crossref]

2004 (1)

J. X. Cheng and X. S. Xie, J. Phys. Chem. B 108, 827 (2004).
[Crossref]

2002 (1)

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

2001 (1)

1997 (1)

S. Constantine, Y. Zhou, J. Morais, and L. D. Ziegler, J. Phys. Chem. A 101, 5456 (1997).
[Crossref]

1995 (1)

C. C. Hayden and D. W. Chandler, J. Chem. Phys. 103, 10465 (1995).
[Crossref]

1979 (1)

N. I. Koroteev, M. Endemann, and R. L. Byer, Phys. Rev. Lett. 43, 398 (1979).
[Crossref]

1978 (1)

A. C. Eckbreth, Appl. Phys. Lett. 32, 421 (1978).
[Crossref]

1977 (1)

1965 (1)

P. D. Maker and R. W. Terhune, Phys. Rev. 137, A801 (1965).
[Crossref]

Ariunbold, G. O.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[Crossref] [PubMed]

Blades, M. W.

Book, L. D.

Buckup, T.

Byer, R. L.

N. I. Koroteev, M. Endemann, and R. L. Byer, Phys. Rev. Lett. 43, 398 (1979).
[Crossref]

Caster, A. G.

S. H. Lim, A. G. Caster, and S. R. Leone, Phys. Rev. A 72, 041803 (2005).
[Crossref]

Chandler, D. W.

C. C. Hayden and D. W. Chandler, J. Chem. Phys. 103, 10465 (1995).
[Crossref]

Cheng, J. X.

J. X. Cheng and X. S. Xie, J. Phys. Chem. B 108, 827 (2004).
[Crossref]

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

Constantine, S.

S. Constantine, Y. Zhou, J. Morais, and L. D. Ziegler, J. Phys. Chem. A 101, 5456 (1997).
[Crossref]

Dogariu, A.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[Crossref] [PubMed]

Dudovich, N.

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

Eckbreth, A. C.

A. C. Eckbreth, Appl. Phys. Lett. 32, 421 (1978).
[Crossref]

Endemann, M.

N. I. Koroteev, M. Endemann, and R. L. Byer, Phys. Rev. Lett. 43, 398 (1979).
[Crossref]

Evans, C. L.

Harvey, A. B.

Hayden, C. C.

C. C. Hayden and D. W. Chandler, J. Chem. Phys. 103, 10465 (1995).
[Crossref]

Hepburn, J. W.

X. J. G. Xu, S. O. Konorov, S. Zhdanovich, J. W. Hepburn, and V. Milner, J. Chem. Phys. 126, 091102 (2007).
[Crossref] [PubMed]

S. O. Konorov, X. G. Xu, R. F. Turner, M. W. Blades, J. W. Hepburn, and V. Milner, Opt. Express 15, 7564 (2007).
[Crossref] [PubMed]

Huang, Y.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[Crossref] [PubMed]

Konorov, S. O.

Koroteev, N. I.

N. I. Koroteev, M. Endemann, and R. L. Byer, Phys. Rev. Lett. 43, 398 (1979).
[Crossref]

Leone, S. R.

S. H. Lim, A. G. Caster, and S. R. Leone, Phys. Rev. A 72, 041803 (2005).
[Crossref]

Lim, S. H.

S. H. Lim, A. G. Caster, and S. R. Leone, Phys. Rev. A 72, 041803 (2005).
[Crossref]

Maker, P. D.

P. D. Maker and R. W. Terhune, Phys. Rev. 137, A801 (1965).
[Crossref]

McDonald, J. R.

Milner, V.

X. J. G. Xu, S. O. Konorov, S. Zhdanovich, J. W. Hepburn, and V. Milner, J. Chem. Phys. 126, 091102 (2007).
[Crossref] [PubMed]

S. O. Konorov, X. G. Xu, R. F. Turner, M. W. Blades, J. W. Hepburn, and V. Milner, Opt. Express 15, 7564 (2007).
[Crossref] [PubMed]

Morais, J.

S. Constantine, Y. Zhou, J. Morais, and L. D. Ziegler, J. Phys. Chem. A 101, 5456 (1997).
[Crossref]

Motzkus, M.

Murawski, R. K.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[Crossref] [PubMed]

Nibler, J. W.

Oron, D.

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

Pestov, D.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[Crossref] [PubMed]

Potma, E. O.

Rostovtsev, Y. V.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[Crossref] [PubMed]

Sautenkov, V. A.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[Crossref] [PubMed]

Scully, M. O.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[Crossref] [PubMed]

Silberberg, Y.

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

Sokolov, A. V.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[Crossref] [PubMed]

Terhune, R. W.

P. D. Maker and R. W. Terhune, Phys. Rev. 137, A801 (1965).
[Crossref]

Tolles, W. M.

Turner, R. F.

Turner, R. F. B.

Vacano, B. von

Wang, X.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[Crossref] [PubMed]

Xie, X. S.

Xu, X. G.

Xu, X. J. G.

X. J. G. Xu, S. O. Konorov, S. Zhdanovich, J. W. Hepburn, and V. Milner, J. Chem. Phys. 126, 091102 (2007).
[Crossref] [PubMed]

Zhdanovich, S.

X. J. G. Xu, S. O. Konorov, S. Zhdanovich, J. W. Hepburn, and V. Milner, J. Chem. Phys. 126, 091102 (2007).
[Crossref] [PubMed]

Zhi, M. C.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[Crossref] [PubMed]

Zhou, Y.

S. Constantine, Y. Zhou, J. Morais, and L. D. Ziegler, J. Phys. Chem. A 101, 5456 (1997).
[Crossref]

Ziegler, L. D.

S. Constantine, Y. Zhou, J. Morais, and L. D. Ziegler, J. Phys. Chem. A 101, 5456 (1997).
[Crossref]

Appl. Phys. Lett. (1)

A. C. Eckbreth, Appl. Phys. Lett. 32, 421 (1978).
[Crossref]

Appl. Spectrosc. (2)

J. Chem. Phys. (2)

X. J. G. Xu, S. O. Konorov, S. Zhdanovich, J. W. Hepburn, and V. Milner, J. Chem. Phys. 126, 091102 (2007).
[Crossref] [PubMed]

C. C. Hayden and D. W. Chandler, J. Chem. Phys. 103, 10465 (1995).
[Crossref]

J. Phys. Chem. A (1)

S. Constantine, Y. Zhou, J. Morais, and L. D. Ziegler, J. Phys. Chem. A 101, 5456 (1997).
[Crossref]

J. Phys. Chem. B (1)

J. X. Cheng and X. S. Xie, J. Phys. Chem. B 108, 827 (2004).
[Crossref]

Nature (1)

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

Opt. Express (1)

Opt. Lett. (3)

Phys. Rev. (1)

P. D. Maker and R. W. Terhune, Phys. Rev. 137, A801 (1965).
[Crossref]

Phys. Rev. A (1)

S. H. Lim, A. G. Caster, and S. R. Leone, Phys. Rev. A 72, 041803 (2005).
[Crossref]

Phys. Rev. Lett. (1)

N. I. Koroteev, M. Endemann, and R. L. Byer, Phys. Rev. Lett. 43, 398 (1979).
[Crossref]

Science (1)

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[Crossref] [PubMed]

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Figures (3)

Fig. 1
Fig. 1

Numerical simulation of the squared amplitude (solid curve) and phase (dashed curve) of coherent vibrational response of azobenzene (a) with and (b) without high nonresonant background excited by the pump and Stokes pulses of 130 fs duration (FWHM). The similarity between the phase in (a) and amplitude in (b) is the key point exploited in our approach to background subtraction.

Fig. 2
Fig. 2

Experimentally observed time-frequency CARS spectrogram of azobenzene.

Fig. 3
Fig. 3

(a) XFROG retrieval of the squared amplitude, R ( Ω ) 2 (solid curve), and phase, Φ ( Ω ) (dashed curve), of the coherent Raman response of azobenzene. Sharp dips in the spectral phase correspond to the Raman resonances. The smooth parabolic baseline indicates the residual frequency chirp of the pump-Stokes pulses. (b) The retrieved spectral phase (upper curve) in comparison with the spontaneous Raman spectrum (middle curve) and the squared amplitude of the vibrational response R ( Ω ) (lower curve). The background-free spectral phase better reflects the small peaks at 1317 and 1591 cm 1 (dashed lines), whereas R ( Ω ) 2 shows dispersive profiles on top of the strong nonresonant background.

Equations (5)

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R ( Ω ) = [ k C k Ω Ω k i Γ k + C NR ] A ( Ω ) ,
A ( Ω ) = E p ( ω ) E S * ( ω Ω ) d ω .
E CARS ( ω ) R ( Ω ) E p r ( ω Ω ) d Ω .
Φ ( Ω ) = arctan Im ( R ( Ω ) ) Re ( R ( Ω ) ) Im ( R ( Ω ) ) Re ( R ( Ω ) ) ,
Φ ( Ω ) [ k C k Γ k ( Ω Ω k ) 2 + Γ 2 ] C NR .

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