Abstract

We report on mode-selective ultrafast coherent anti-Stokes Raman spectroscopy (CARS) of a powder of sodium dipicolinate. We produce a pair of stretched laser pulses with precisely adjusted matching chirp rates. We use the pulses for frequency-resolved excitation of coherent molecular vibrations in this highly scattering medium. The induced oscillations are probed with the third delayed ultrashort laser pulse. Since the attained spectral width of the pump-Stokes excitation band is on the order of the spacing between the Raman lines, time-resolved CARS measurements reveal single-mode as well as double-mode coherence decay dynamics, depending on the timing between the pump and Stokes pulses. For a fixed probe pulse delay, the sweeping of the arrival time for one of the preparation pulses maps out the CARS spectrum of the analyte.

© 2008 Optical Society of America

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    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef]
  4. R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, “Nonresonant control of multimode molecular wave packets at room temperature,” Phys. Rev. Lett. 88, 033001 (2002).
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  8. D. Oron, N. Dudovich, and Y. Silberberg, “Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy,” Phys. Rev. Lett. 90, 213902 (2003).
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  9. D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, “Narrow-band coherent anti-Stokes Raman signals from broad-band pulses,” Phys. Rev. Lett. 88, 063004 (2002).
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    [CrossRef]
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  13. T. Hellerer, A. M. K. Enejder, and A. Zumbusch, “Spectral focusing: high spectral resolution spectroscopy with broad-bandwidth laser pulses,” Appl. Phys. Lett. 85, 25-27 (2004).
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    [CrossRef]
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    [CrossRef] [PubMed]
  21. D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14976-14981 (2005).
    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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  26. A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, “Wave packet dynamics in different electronic states investigated by femtosecond time-resolved four-wave-mixing spectroscopy,” Appl. Phys. B 71, 299-317 (2000).
    [CrossRef]
  27. A. V. Sokolov and S. E. Harris, “Ultrashort pulse generation by molecular modulation,” J. Opt. B: Quantum Semiclassical Opt. 5, R1-R26 (2003).
    [CrossRef]
  28. A. V. Sokolov, M. Y. Shverdin, D. R. Walker, D. D. Yavuz, A. M. Burzo, G. Y. Yin, and S. E. Harris, “Generation and control of femtosecond pulses by molecular modulation,” J. Mod. Opt. 52, 285-304 (2005).
    [CrossRef]

2007 (2)

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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316, 265-268 (2007).
[CrossRef] [PubMed]

M. C. Zhi, D. Pestov, X. Wang, R. K. Murawski, Y. V. Rostovtsev, Z. E. Sariyanni, V. A. Sautenkov, N. G. Kalugin, and A. V. Sokolov, “Concentration dependence of femtosecond coherent anti-Stokes Raman scattering in the presence of strong absorption,” J. Opt. Soc. Am. B 24, 1181-1186 (2007).
[CrossRef]

2006 (3)

2005 (2)

A. V. Sokolov, M. Y. Shverdin, D. R. Walker, D. D. Yavuz, A. M. Burzo, G. Y. Yin, and S. E. Harris, “Generation and control of femtosecond pulses by molecular modulation,” J. Mod. Opt. 52, 285-304 (2005).
[CrossRef]

D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14976-14981 (2005).
[CrossRef] [PubMed]

2004 (2)

V. V. Lozovoy, I. Pastirk, and M. Dantus, “Multiphoton intrapulse interference. IV. Ultrashort laser pulse spectral phase characterization and compensation,” Opt. Lett. 29, 775-777 (2004).
[CrossRef] [PubMed]

T. Hellerer, A. M. K. Enejder, and A. Zumbusch, “Spectral focusing: high spectral resolution spectroscopy with broad-bandwidth laser pulses,” Appl. Phys. Lett. 85, 25-27 (2004).
[CrossRef]

2003 (3)

E. Gershgoren, R. A. Bartels, J. T. Fourkas, R. Tobey, M. M. Murnane, and H. C. Kapteyn, “Simplified setup for high-resolution spectroscopy that uses ultrashort pulses,” Opt. Lett. 28, 361-363 (2003).
[CrossRef] [PubMed]

D. Oron, N. Dudovich, and Y. Silberberg, “Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy,” Phys. Rev. Lett. 90, 213902 (2003).
[CrossRef] [PubMed]

A. V. Sokolov and S. E. Harris, “Ultrashort pulse generation by molecular modulation,” J. Opt. B: Quantum Semiclassical Opt. 5, R1-R26 (2003).
[CrossRef]

2002 (5)

M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, “FAST CARS: engineering a laser spectroscopic technique for rapid identification of bacterial spores,” Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002).
[CrossRef] [PubMed]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, “Narrow-band coherent anti-Stokes Raman signals from broad-band pulses,” Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, “Nonresonant control of multimode molecular wave packets at room temperature,” Phys. Rev. Lett. 88, 033001 (2002).
[CrossRef] [PubMed]

N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy,” Nature 418, 512-514 (2002).
[CrossRef] [PubMed]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, “Quantum control of coherent anti-Stokes Raman processes,” Phys. Rev. A 65, 043408 (2002).
[CrossRef]

2000 (3)

A. M. Zheltikov and A. N. Naumov, “High-resolution four-photon spectroscopy with chirped pulses,” Quantum Electron. 30, 606-610 (2000).
[CrossRef]

V. V. Lozovoy, B. I. Grimberg, E. J. Brown, I. Pastirk, and M. Dantus, “Femtosecond spectrally dispersed three-pulse four-wave mixing: the role of sequence and chirp in controlling intramolecular dynamics,” J. Raman Spectrosc. 31, 41-49 (2000).
[CrossRef]

A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, “Wave packet dynamics in different electronic states investigated by femtosecond time-resolved four-wave-mixing spectroscopy,” Appl. Phys. B 71, 299-317 (2000).
[CrossRef]

1999 (1)

D. Meshulach and Y. Silberberg, “Coherent quantum control of multiphoton transitions by shaped ultrashort optical pulses,” Phys. Rev. A 60, 1287-1292 (1999).
[CrossRef]

1998 (1)

A. Assion, T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, “Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses,” Science 282, 919-922 (1998).
[CrossRef] [PubMed]

1994 (1)

A. S. Weling, B. B. Hu, N. M. Froberg, and D. H. Auston, “Generation of tunable narrow-band Thz radiation from large-aperture photoconducting antennas,” Appl. Phys. Lett. 64, 137-139 (1994).
[CrossRef]

1987 (1)

R. Leonhardt, W. Holzapfel, W. Zinth, and W. Kaiser, “Terahertz quantum beats in molecular liquids,” Chem. Phys. Lett. 133, 373-377 (1987).
[CrossRef]

1959 (1)

B. D. Church and H. Halvorson, “Dependence of the heat resistance of bacterial endospores on their dipicolinic acid content,” Nature 183, 124-125 (1959).
[CrossRef] [PubMed]

1953 (1)

J. F. Powell, “Isolation of dipicolinic acid (pyridine-2-6-dicarboxylic acid) from spores of bacillus-megatherium,” Biochem. J. 54, 210-211 (1953).
[PubMed]

Akimov, D. A.

D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14976-14981 (2005).
[CrossRef] [PubMed]

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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316, 265-268 (2007).
[CrossRef] [PubMed]

Assion, A.

A. Assion, T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, “Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses,” Science 282, 919-922 (1998).
[CrossRef] [PubMed]

Auston, D. H.

A. S. Weling, B. B. Hu, N. M. Froberg, and D. H. Auston, “Generation of tunable narrow-band Thz radiation from large-aperture photoconducting antennas,” Appl. Phys. Lett. 64, 137-139 (1994).
[CrossRef]

Bartels, R. A.

E. Gershgoren, R. A. Bartels, J. T. Fourkas, R. Tobey, M. M. Murnane, and H. C. Kapteyn, “Simplified setup for high-resolution spectroscopy that uses ultrashort pulses,” Opt. Lett. 28, 361-363 (2003).
[CrossRef] [PubMed]

R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, “Nonresonant control of multimode molecular wave packets at room temperature,” Phys. Rev. Lett. 88, 033001 (2002).
[CrossRef] [PubMed]

Baumert, T.

A. Assion, T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, “Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses,” Science 282, 919-922 (1998).
[CrossRef] [PubMed]

Bergt, M.

A. Assion, T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, “Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses,” Science 282, 919-922 (1998).
[CrossRef] [PubMed]

Boppart, S. A.

Brixner, T.

A. Assion, T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, “Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses,” Science 282, 919-922 (1998).
[CrossRef] [PubMed]

Brown, E. J.

V. V. Lozovoy, B. I. Grimberg, E. J. Brown, I. Pastirk, and M. Dantus, “Femtosecond spectrally dispersed three-pulse four-wave mixing: the role of sequence and chirp in controlling intramolecular dynamics,” J. Raman Spectrosc. 31, 41-49 (2000).
[CrossRef]

Burzo, A. M.

A. V. Sokolov, M. Y. Shverdin, D. R. Walker, D. D. Yavuz, A. M. Burzo, G. Y. Yin, and S. E. Harris, “Generation and control of femtosecond pulses by molecular modulation,” J. Mod. Opt. 52, 285-304 (2005).
[CrossRef]

Chakraborty, A.

B. D. Prince, A. Chakraborty, B. M. Prince, and H. U. Stauffer, “Development of simultaneous frequency- and time-resolved coherent anti-Stokes Raman scattering for ultrafast detection of molecular Raman spectra,” J. Chem. Phys. 125, 044502 (2006).
[CrossRef]

Chen, T.

A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, “Wave packet dynamics in different electronic states investigated by femtosecond time-resolved four-wave-mixing spectroscopy,” Appl. Phys. B 71, 299-317 (2000).
[CrossRef]

Church, B. D.

B. D. Church and H. Halvorson, “Dependence of the heat resistance of bacterial endospores on their dipicolinic acid content,” Nature 183, 124-125 (1959).
[CrossRef] [PubMed]

Dantus, M.

Dela Cruz, J. M.

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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316, 265-268 (2007).
[CrossRef] [PubMed]

Dudovich, N.

D. Oron, N. Dudovich, and Y. Silberberg, “Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy,” Phys. Rev. Lett. 90, 213902 (2003).
[CrossRef] [PubMed]

N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy,” Nature 418, 512-514 (2002).
[CrossRef] [PubMed]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, “Quantum control of coherent anti-Stokes Raman processes,” Phys. Rev. A 65, 043408 (2002).
[CrossRef]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, “Narrow-band coherent anti-Stokes Raman signals from broad-band pulses,” Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

Enejder, A. M. K.

T. Hellerer, A. M. K. Enejder, and A. Zumbusch, “Spectral focusing: high spectral resolution spectroscopy with broad-bandwidth laser pulses,” Appl. Phys. Lett. 85, 25-27 (2004).
[CrossRef]

Engel, V.

A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, “Wave packet dynamics in different electronic states investigated by femtosecond time-resolved four-wave-mixing spectroscopy,” Appl. Phys. B 71, 299-317 (2000).
[CrossRef]

Fourkas, J. T.

Froberg, N. M.

A. S. Weling, B. B. Hu, N. M. Froberg, and D. H. Auston, “Generation of tunable narrow-band Thz radiation from large-aperture photoconducting antennas,” Appl. Phys. Lett. 64, 137-139 (1994).
[CrossRef]

Gerber, G.

A. Assion, T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, “Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses,” Science 282, 919-922 (1998).
[CrossRef] [PubMed]

Gershgoren, E.

Graefe, S.

D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14976-14981 (2005).
[CrossRef] [PubMed]

Grimberg, B. I.

V. V. Lozovoy, B. I. Grimberg, E. J. Brown, I. Pastirk, and M. Dantus, “Femtosecond spectrally dispersed three-pulse four-wave mixing: the role of sequence and chirp in controlling intramolecular dynamics,” J. Raman Spectrosc. 31, 41-49 (2000).
[CrossRef]

Gunn, J. M.

Halvorson, H.

B. D. Church and H. Halvorson, “Dependence of the heat resistance of bacterial endospores on their dipicolinic acid content,” Nature 183, 124-125 (1959).
[CrossRef] [PubMed]

Harris, S. E.

A. V. Sokolov, M. Y. Shverdin, D. R. Walker, D. D. Yavuz, A. M. Burzo, G. Y. Yin, and S. E. Harris, “Generation and control of femtosecond pulses by molecular modulation,” J. Mod. Opt. 52, 285-304 (2005).
[CrossRef]

A. V. Sokolov and S. E. Harris, “Ultrashort pulse generation by molecular modulation,” J. Opt. B: Quantum Semiclassical Opt. 5, R1-R26 (2003).
[CrossRef]

Hellerer, T.

T. Hellerer, A. M. K. Enejder, and A. Zumbusch, “Spectral focusing: high spectral resolution spectroscopy with broad-bandwidth laser pulses,” Appl. Phys. Lett. 85, 25-27 (2004).
[CrossRef]

Holzapfel, W.

R. Leonhardt, W. Holzapfel, W. Zinth, and W. Kaiser, “Terahertz quantum beats in molecular liquids,” Chem. Phys. Lett. 133, 373-377 (1987).
[CrossRef]

Hu, B. B.

A. S. Weling, B. B. Hu, N. M. Froberg, and D. H. Auston, “Generation of tunable narrow-band Thz radiation from large-aperture photoconducting antennas,” Appl. Phys. Lett. 64, 137-139 (1994).
[CrossRef]

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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316, 265-268 (2007).
[CrossRef] [PubMed]

Jones, G. W.

Kaiser, W.

R. Leonhardt, W. Holzapfel, W. Zinth, and W. Kaiser, “Terahertz quantum beats in molecular liquids,” Chem. Phys. Lett. 133, 373-377 (1987).
[CrossRef]

Kalugin, N. G.

M. C. Zhi, D. Pestov, X. Wang, R. K. Murawski, Y. V. Rostovtsev, Z. E. Sariyanni, V. A. Sautenkov, N. G. Kalugin, and A. V. Sokolov, “Concentration dependence of femtosecond coherent anti-Stokes Raman scattering in the presence of strong absorption,” J. Opt. Soc. Am. B 24, 1181-1186 (2007).
[CrossRef]

D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14976-14981 (2005).
[CrossRef] [PubMed]

Kapteyn, H. C.

E. Gershgoren, R. A. Bartels, J. T. Fourkas, R. Tobey, M. M. Murnane, and H. C. Kapteyn, “Simplified setup for high-resolution spectroscopy that uses ultrashort pulses,” Opt. Lett. 28, 361-363 (2003).
[CrossRef] [PubMed]

R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, “Nonresonant control of multimode molecular wave packets at room temperature,” Phys. Rev. Lett. 88, 033001 (2002).
[CrossRef] [PubMed]

Kattawar, G. W.

M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, “FAST CARS: engineering a laser spectroscopic technique for rapid identification of bacterial spores,” Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Kiefer, B.

A. Assion, T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, “Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses,” Science 282, 919-922 (1998).
[CrossRef] [PubMed]

Kiefer, W.

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M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, “FAST CARS: engineering a laser spectroscopic technique for rapid identification of bacterial spores,” Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002).
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M. C. Zhi, D. Pestov, X. Wang, R. K. Murawski, Y. V. Rostovtsev, Z. E. Sariyanni, V. A. Sautenkov, N. G. Kalugin, and A. V. Sokolov, “Concentration dependence of femtosecond coherent anti-Stokes Raman scattering in the presence of strong absorption,” J. Opt. Soc. Am. B 24, 1181-1186 (2007).
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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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316, 265-268 (2007).
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D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14976-14981 (2005).
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D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14976-14981 (2005).
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D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14976-14981 (2005).
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D. Oron, N. Dudovich, and Y. Silberberg, “Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy,” Phys. Rev. Lett. 90, 213902 (2003).
[CrossRef] [PubMed]

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[CrossRef]

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[CrossRef] [PubMed]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, “Narrow-band coherent anti-Stokes Raman signals from broad-band pulses,” Phys. Rev. Lett. 88, 063004 (2002).
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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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316, 265-268 (2007).
[CrossRef] [PubMed]

M. C. Zhi, D. Pestov, X. Wang, R. K. Murawski, Y. V. Rostovtsev, Z. E. Sariyanni, V. A. Sautenkov, N. G. Kalugin, and A. V. Sokolov, “Concentration dependence of femtosecond coherent anti-Stokes Raman scattering in the presence of strong absorption,” J. Opt. Soc. Am. B 24, 1181-1186 (2007).
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B. D. Prince, A. Chakraborty, B. M. Prince, and H. U. Stauffer, “Development of simultaneous frequency- and time-resolved coherent anti-Stokes Raman scattering for ultrafast detection of molecular Raman spectra,” J. Chem. Phys. 125, 044502 (2006).
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A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, “Wave packet dynamics in different electronic states investigated by femtosecond time-resolved four-wave-mixing spectroscopy,” Appl. Phys. B 71, 299-317 (2000).
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D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, “Narrow-band coherent anti-Stokes Raman signals from broad-band pulses,” Phys. Rev. Lett. 88, 063004 (2002).
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A. V. Sokolov, M. Y. Shverdin, D. R. Walker, D. D. Yavuz, A. M. Burzo, G. Y. Yin, and S. E. Harris, “Generation and control of femtosecond pulses by molecular modulation,” J. Mod. Opt. 52, 285-304 (2005).
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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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316, 265-268 (2007).
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Figures (5)

Fig. 1
Fig. 1

Technique and experiment schematics: (a) CARS energy level diagram. The two broadband but shaped preparation pulses, pump ( ω 1 ) and Stokes ( ω 2 ) , excite Raman-active vibrational modes of the sampled molecules. The third pulse ( ω 3 ) probes the initiated coherent molecular vibrations. Inset: spontaneous Raman spectrum of NaDPA powder in the range of interest, acquired with a CW laser operating at 532 nm . (b) Time-frequency diagram of the selective Raman excitation with linearly chirped laser pulses. The difference frequency Δ ω ω 1 ω 2 depends on the relative timing τ 12 between the preparation pulses. (c) Experimental setup layout. The pump and Stokes pulses are sent through 4 cm pieces of SF-11 glass. The Stokes pulse also passes through a commercially available pulse shaper (Silhouette, Coherent), where a parabolic phase mask is added to compensate for the difference in the chirp, produced by the glass slabs. The pump and probe time delays are adjusted relative to the Stokes pulse. The three beams are focused (with 40 to 50 cm focal length lenses) on the sample, a pellet of NaDPA powder. The generated and scattered CARS photons are collected with a 2 in. spherical mirror ( f = 20 cm ) in the backward direction, at an angle of 30 ° to the main axis. The collected light is filtered and refocused on the entrance slit of an imaging spectrometer (Chromex-250is) with a LN2-cooled CCD; CCD - charge coupled device.

Fig. 2
Fig. 2

Pulse shaping characterization: (a) Cross-correlation spectrogram between the chirped pump and transform-limited probe pulses. The spectrum of FWM signal ( 2 ω 3 ω 1 process), generated on a cover glass slide, is recorded as a function of the probe pulse delay; (b) Cross-correlation spectrogram between the linearly chirped pump, Stokes, and ultrashort probe pulses. Again, the spectrum of the FWM signal ( ω 1 ω 2 + ω 3 process) from a cover glass slide is acquired as a function of the probe pulse delay.

Fig. 3
Fig. 3

Selective excitation of Raman modes in NaDPA powder, 1442 cm 1 and 1395 cm 1 . The relative timing τ 12 t 1 t 2 between the two linearly chirped preparation pulses, pump ( λ 1 = 722.5 nm ) and ( λ 2 = 804 nm ) , is set as (a) 333 , (b) 133 , (c) 100 , (d) 67 , (e) 0, (f) + 67 , (g) + 100 , and (h) + 300 fs . The induced molecular vibrations are probed with an ultrashort pulse at λ 3 = 579 nm . CARS spectrum as a function of the probe pulse delay is recorded. Timing of the pump-Stokes pulses leads to consecutive excitation of a single Raman mode at 1442 cm 1 ; both Raman modes, as it can be inferred from the beating; a single Raman mode at 1395 cm 1 . The pump, Stokes, and probe pulse energies are 2.8, 1.1, and 0.39 μ J , respectively. The integration time is 0.2 s per step.

Fig. 4
Fig. 4

Cross section of the spectrogram in Fig. 3e at λ = 535 nm . The beat frequency at positive probe delays corresponds to the frequency difference between the two excited Raman modes, 47 cm 1 . Inset: FFT of the recorded modulation, corrected for the exponential decay.

Fig. 5
Fig. 5

Spectrally-integrated CARS signal as a function of the pump pulse timing, τ 12 . The probe pulse delay is set as (a) 1.4, (b) 2.2, and (c) 2.9 ps , i.e., close to the peaks of the quantum beat profile in Fig. 4, when the two Raman modes are excited. The pump, Stokes, and probe pulse energies are 3.3, 1.2, and 0.37 μ J , respectively. The integration time is 0.2 s per step. Inset: CARS spectrogram recorded in case (b).

Equations (4)

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τ = 2 ln ( 2 ) a 0 , Δ ω = 2 2 ln ( 2 ) a 0 ( 1 + b 0 2 a 0 2 ) .
k ( ω ) ω n ( ω ) c k ( ω 0 ) + k ( ω 0 ) ( ω ω 0 ) + k ( ω 0 ) ( ω ω 0 ) 2 2 ,
E ( t ) = E 0 exp { i ω 0 [ t L V ϕ ( ω 0 ) ] } exp { Γ ( L ) [ t L V g ( ω 0 ) ] 2 } ,
1 Γ ( L ) 1 a i b = 1 Γ 0 + 2 i k ( ω 0 ) L .

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