Abstract

We present a comparative analysis of spontaneous and coherent Raman scattering on pyridine. The instantaneous excitation of the molecular coherence is done by a pair of ultrashort preparation pulses. Then, a long narrowband probe pulse is scattered off the molecular vibrations. The described hybrid technique allows for the single-shot acquisition of a background-free coherent Raman spectrum within the excitation band and its straightforward comparison with the spontaneous Raman measurements, performed in the same setup. We report a 105-fold increase in the efficiency of the Raman scattering process due to the broadband pump–Stokes preparation. The coherence magnitude (0.5×103) is inferred experimentally, without a priori knowledge about the molecular structure.

© 2007 Optical Society of America

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  1. Y. R. Shen, The Principles of Nonlinear Optics (Wiley, 1984).
  2. W. M. Tolles and R. D. Turner, Appl. Spectrosc. 31, 96 (1977).
    [CrossRef]
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    [CrossRef]
  4. R. Leonhardt, W. Holzapfel, W. Zinth, and W. Kaiser, Chem. Phys. Lett. 133, 373 (1987).
    [CrossRef]
  5. A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, Appl. Phys. B 71, 299 (2000).
  6. A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
    [CrossRef]
  7. R. P. Lucht, S. Roy, T. R. Meyer, and J. R. Gord, Appl. Phys. Lett. 89, 251112 (2006).
    [CrossRef]
  8. P. Kukura, D. W. McCamart, S. Yoon, D. B. Wandschneider, and R. A. Mathies, Science 310, 1006 (2005).
    [CrossRef] [PubMed]
  9. G. I. Petrov, R. Arora, V. V. Yakovlev, X. Wang, A. V. Sokolov, and M. O. Scully, Proc. Natl. Acad. Sci. U.S.A. 104, 7776 (2007).
    [CrossRef] [PubMed]
  10. D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
    [CrossRef] [PubMed]
  11. S. Roy, T. R. Meyer, and J. R. Gord, Appl. Phys. Lett. 87, 264103 (2005).
    [CrossRef]
  12. B. D. Prince, A. Chakraborty, B. M. Prince, and H. U. Stauffer, J. Chem. Phys. 125, 044502 (2006).
    [CrossRef]

2007

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

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

2006

B. D. Prince, A. Chakraborty, B. M. Prince, and H. U. Stauffer, J. Chem. Phys. 125, 044502 (2006).
[CrossRef]

R. P. Lucht, S. Roy, T. R. Meyer, and J. R. Gord, Appl. Phys. Lett. 89, 251112 (2006).
[CrossRef]

2005

P. Kukura, D. W. McCamart, S. Yoon, D. B. Wandschneider, and R. A. Mathies, Science 310, 1006 (2005).
[CrossRef] [PubMed]

S. Roy, T. R. Meyer, and J. R. Gord, Appl. Phys. Lett. 87, 264103 (2005).
[CrossRef]

2002

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

2000

A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, Appl. Phys. B 71, 299 (2000).

1987

R. Leonhardt, W. Holzapfel, W. Zinth, and W. Kaiser, Chem. Phys. Lett. 133, 373 (1987).
[CrossRef]

1977

Ariunbold, G. O.

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

Arora, R.

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

Book, L. D.

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

Chakraborty, A.

B. D. Prince, A. Chakraborty, B. M. Prince, and H. U. Stauffer, J. Chem. Phys. 125, 044502 (2006).
[CrossRef]

Chen, T.

A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, Appl. Phys. B 71, 299 (2000).

Dogariu, A.

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

Engel, V.

A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, Appl. Phys. B 71, 299 (2000).

Gord, J. R.

R. P. Lucht, S. Roy, T. R. Meyer, and J. R. Gord, Appl. Phys. Lett. 89, 251112 (2006).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, Appl. Phys. Lett. 87, 264103 (2005).
[CrossRef]

Holzapfel, W.

R. Leonhardt, W. Holzapfel, W. Zinth, and W. Kaiser, Chem. Phys. Lett. 133, 373 (1987).
[CrossRef]

Huang, Y.

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

Kaiser, W.

R. Leonhardt, W. Holzapfel, W. Zinth, and W. Kaiser, Chem. Phys. Lett. 133, 373 (1987).
[CrossRef]

Kiefer, W.

A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, Appl. Phys. B 71, 299 (2000).

Knighten, G. V.

J. W. Nibler and G. V. Knighten, in Raman Spectroscopy of Gases and Liquids, A.Weber, ed. (Springer-Verlag, 1979), pp. 253-299.
[CrossRef]

Kukura, P.

P. Kukura, D. W. McCamart, S. Yoon, D. B. Wandschneider, and R. A. Mathies, Science 310, 1006 (2005).
[CrossRef] [PubMed]

Leonhardt, R.

R. Leonhardt, W. Holzapfel, W. Zinth, and W. Kaiser, Chem. Phys. Lett. 133, 373 (1987).
[CrossRef]

Lucht, R. P.

R. P. Lucht, S. Roy, T. R. Meyer, and J. R. Gord, Appl. Phys. Lett. 89, 251112 (2006).
[CrossRef]

Materny, A.

A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, Appl. Phys. B 71, 299 (2000).

Mathies, R. A.

P. Kukura, D. W. McCamart, S. Yoon, D. B. Wandschneider, and R. A. Mathies, Science 310, 1006 (2005).
[CrossRef] [PubMed]

McCamart, D. W.

P. Kukura, D. W. McCamart, S. Yoon, D. B. Wandschneider, and R. A. Mathies, Science 310, 1006 (2005).
[CrossRef] [PubMed]

Meyer, T. R.

R. P. Lucht, S. Roy, T. R. Meyer, and J. R. Gord, Appl. Phys. Lett. 89, 251112 (2006).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, Appl. Phys. Lett. 87, 264103 (2005).
[CrossRef]

Murawski, R. K.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. 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.

J. W. Nibler and G. V. Knighten, in Raman Spectroscopy of Gases and Liquids, A.Weber, ed. (Springer-Verlag, 1979), pp. 253-299.
[CrossRef]

Pestov, D.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[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. U.S.A. 104, 7776 (2007).
[CrossRef] [PubMed]

Prince, B. D.

B. D. Prince, A. Chakraborty, B. M. Prince, and H. U. Stauffer, J. Chem. Phys. 125, 044502 (2006).
[CrossRef]

Prince, B. M.

B. D. Prince, A. Chakraborty, B. M. Prince, and H. U. Stauffer, J. Chem. Phys. 125, 044502 (2006).
[CrossRef]

Rostovtsev, Y. V.

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

Roy, S.

R. P. Lucht, S. Roy, T. R. Meyer, and J. R. Gord, Appl. Phys. Lett. 89, 251112 (2006).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, Appl. Phys. Lett. 87, 264103 (2005).
[CrossRef]

Sautenkov, V. A.

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

Schmitt, M.

A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, Appl. Phys. B 71, 299 (2000).

Scully, M. O.

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

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

Shen, Y. R.

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, 1984).

Siebert, T.

A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, Appl. Phys. B 71, 299 (2000).

Sokolov, A. V.

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

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

Stauffer, H. U.

B. D. Prince, A. Chakraborty, B. M. Prince, and H. U. Stauffer, J. Chem. Phys. 125, 044502 (2006).
[CrossRef]

Tolles, W. M.

Turner, R. D.

Vierheilig, A.

A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, Appl. Phys. B 71, 299 (2000).

Volkmer, A.

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

Wandschneider, D. B.

P. Kukura, D. W. McCamart, S. Yoon, D. B. Wandschneider, and R. A. Mathies, Science 310, 1006 (2005).
[CrossRef] [PubMed]

Wang, X.

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

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. 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.

A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
[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. U.S.A. 104, 7776 (2007).
[CrossRef] [PubMed]

Yoon, S.

P. Kukura, D. W. McCamart, S. Yoon, D. B. Wandschneider, and R. A. Mathies, Science 310, 1006 (2005).
[CrossRef] [PubMed]

Zhi, M.

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

Zinth, W.

R. Leonhardt, W. Holzapfel, W. Zinth, and W. Kaiser, Chem. Phys. Lett. 133, 373 (1987).
[CrossRef]

Appl. Phys. B

A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, Appl. Phys. B 71, 299 (2000).

Appl. Phys. Lett.

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

R. P. Lucht, S. Roy, T. R. Meyer, and J. R. Gord, Appl. Phys. Lett. 89, 251112 (2006).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, Appl. Phys. Lett. 87, 264103 (2005).
[CrossRef]

Appl. Spectrosc.

Chem. Phys. Lett.

R. Leonhardt, W. Holzapfel, W. Zinth, and W. Kaiser, Chem. Phys. Lett. 133, 373 (1987).
[CrossRef]

J. Chem. Phys.

B. D. Prince, A. Chakraborty, B. M. Prince, and H. U. Stauffer, J. Chem. Phys. 125, 044502 (2006).
[CrossRef]

Proc. Natl. Acad. Sci. U.S.A.

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

Science

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

P. Kukura, D. W. McCamart, S. Yoon, D. B. Wandschneider, and R. A. Mathies, Science 310, 1006 (2005).
[CrossRef] [PubMed]

Other

J. W. Nibler and G. V. Knighten, in Raman Spectroscopy of Gases and Liquids, A.Weber, ed. (Springer-Verlag, 1979), pp. 253-299.
[CrossRef]

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, 1984).

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Figures (3)

Fig. 1
Fig. 1

Schematics of the experimental setup for the spontaneous Raman and CSRS measurements. BS, beam splitter; G1,2, DS1,2 computer-controlled delay stages; I1,2, irises; BPF, bandpass and neutral density filters; FM, flip mirror; CCD, imaging charge-coupled device (Spec-10, Princeton Instruments) attached to Chromex Spectrograph 250is.

Fig. 2
Fig. 2

Transition from time-resolved to hybrid CSRS. CSRS spectrograms for different spectral bandwidths of the probe pulse: (a) 300 cm 1 , (b) 100 cm 1 , (c) 40 cm 1 , (d) 15 cm 1 . Two Raman lines of pyridine, 992 and 1031 cm 1 , are excited via a pair of ultrashort laser pulses. Pump: λ p = 737 nm , FWHM 260 cm 1 , 0.5 μ J pulse . Stokes: λ s = 801 nm , FWHM 480 cm 1 , 0.9 μ J pulse . Probe: λ pr = 577.9 nm , 0.15 μ J pulse .

Fig. 3
Fig. 3

Spontaneous Raman and CSRS measurements on pyridine: (a) spontaneous Raman spectrum. Probe pulse: λ p r = 577.9 nm , FWHM 19 cm 1 , the average power is 0.13 mW ( 0.13 μ J pulse , 1 kHz rep rate). The integration time is 3 min . The estimated collection angle Ω e f f 0.004 × 4 π . The cuvette path length is 200 μ m . (b) CSRS spectrum. The probe delay relative to the preparation pulses is fixed and equal to 1.8 ps . At this delay, the nonresonant background is suppressed, since the preparation pulses are overlapped at the node of the probe pulse profile [see the spectrograms in Fig. 2d]. Pump: λ p = 738 nm , FWHM 260 cm 1 , 0.72 μ J pulse ; Stokes: λ s = 802 nm , FWHM 480 cm 1 , 1.36 μ J pulse . Probe parameters and the sample are the same as in part (a). Integration time is 1 s after 10 4 -fold attenuation by a set of neutral density filters.

Equations (2)

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

P C S R S P S p R a m a n λ p r 2 N V ρ b c 2 ρ c c Δ L ,
P C S R S P S p R a m a n = P C S R S P S p R a m a n c × ( 4 π Ω e f f ) 10 5 .

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