Abstract

Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS) offers accurate thermometry at kHz rates for combustion diagnostics. In high-temperature flames, selection of probe-pulse characteristics is key to simultaneously optimizing signal-to-nonresonant-background ratio, signal strength, and spectral resolution. We demonstrate a simple method for enhancing signal-to-nonresonant-background ratio by using a narrowband Lorentzian filter to generate a time-asymmetric probe pulse with full-width-half-maximum (FWHM) pulse width of only 240 fs. This allows detection within just 310 fs after the Raman excitation for eliminating nonresonant background while retaining 45% of the resonant signal at 2000 K. The narrow linewidth is comparable to that of a time-symmetric sinc2 probe pulse with a pulse width of ~2.4 ps generated with a conventional 4-f pulse shaper. This allows nonresonant-background-free, frequency-domain vibrational spectroscopy at high temperature, as verified using comparisons to a time-dependent theoretical fs/ps CARS model.

© 2011 OSA

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    [CrossRef]
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    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef]
  7. L. A. Rahn, L. J. Zych, and P. L. Mattern, “Background-free CARS studies of carbon monoxide in a flame,” Opt. Commun. 30(2), 249–252 (1979).
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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  27. 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(5822), 265–268 (2007).
    [CrossRef] [PubMed]
  28. A. Lagutchev, S. A. Hambir, and D. D. Dlott, “Nonresonant background suppression in broadband vibrational sum-frequency generation spectroscopy,” J. Phys. Chem. C 111(37), 13645–13647 (2007).
    [CrossRef]
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    [CrossRef]

2011 (1)

2010 (5)

2009 (2)

2008 (2)

S. Roy, P. J. Kinnius, R. P. Lucht, and J. R. Gord, “Temperature measurements in reacting flows by time-resolved femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy,” Opt. Commun. 281(2), 319–325 (2008).
[CrossRef]

J. R. Gord, T. R. Meyer, and S. Roy, “Applications of ultrafast lasers for optical measurements in combusting flows,” Ann. Rev. Anal. Chem. (Palo Alto Calif) 1(1), 663–687 (2008).
[CrossRef] [PubMed]

2007 (3)

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(5822), 265–268 (2007).
[CrossRef] [PubMed]

A. Lagutchev, S. A. Hambir, and D. D. Dlott, “Nonresonant background suppression in broadband vibrational sum-frequency generation spectroscopy,” J. Phys. Chem. C 111(37), 13645–13647 (2007).
[CrossRef]

T. R. Meyer, S. Roy, and J. R. Gord, “Improving signal-to-interference ratio in rich hydrocarbon-air flames using picosecond coherent anti-Stokes Raman scattering,” Appl. Spectrosc. 61(11), 1135–1140 (2007).
[CrossRef] [PubMed]

2006 (2)

R. P. Lucht, S. Roy, T. R. Meyer, and J. R. Gord, “Femtosecond coherent anti-Stokes Raman scattering measurement of gas temperatures from frequency-spread dephasing of the Raman coherence,” Appl. Phys. Lett. 89(25), 251112 (2006).
[CrossRef]

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(4), 44502 (2006).
[CrossRef] [PubMed]

2005 (2)

S. Roy, T. R. Meyer, and J. R. Gord, “Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals,” Appl. Phys. Lett. 87(26), 264103 (2005).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, “Broadband coherent anti-Stokes Raman scattering spectroscopy of nitrogen using a picosecond modeless dye laser,” Opt. Lett. 30(23), 3222–3224 (2005).
[CrossRef] [PubMed]

2002 (1)

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(17), 10994–11001 (2002).
[CrossRef] [PubMed]

2001 (2)

P. Beaud, H. M. Frey, T. Lang, and M. Motzkus, “Flame thermometry by femtosecond CARS,” Chem. Phys. Lett. 344(3-4), 407–412 (2001).
[CrossRef]

T. Lang, M. Motzkus, H. M. Frey, and P. Beaud, “High resolution femtosecond coherent anti-Stokes Raman scattering: Determination of rotational constants, molecular anharmonicity, collisional line shifts, and temperature,” J. Chem. Phys. 115(12), 5418–5426 (2001).
[CrossRef]

1990 (1)

M. J. Cottereau, F. Grisch, and J. J. Marie, “CARS measurements of temperature and species concentrations in an IC engine,” Appl. Phys. B 51(1), 63–66 (1990).
[CrossRef]

1987 (1)

1984 (1)

1981 (1)

A. C. Eckbreth and R. J. Hall, “CARS concentration sensitivity with and without non-resonant background suppression,” Combust. Sci. Technol. 25(5), 175–192 (1981).
[CrossRef]

1980 (2)

1979 (1)

L. A. Rahn, L. J. Zych, and P. L. Mattern, “Background-free CARS studies of carbon monoxide in a flame,” Opt. Commun. 30(2), 249–252 (1979).
[CrossRef]

1978 (1)

A. C. Eckbreth, “BOXCARS: Crossed-beam phase-matched CARS generation in gases,” Appl. Phys. Lett. 32(7), 421–423 (1978).
[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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Beaud, P.

P. Beaud, H. M. Frey, T. Lang, and M. Motzkus, “Flame thermometry by femtosecond CARS,” Chem. Phys. Lett. 344(3-4), 407–412 (2001).
[CrossRef]

T. Lang, M. Motzkus, H. M. Frey, and P. Beaud, “High resolution femtosecond coherent anti-Stokes Raman scattering: Determination of rotational constants, molecular anharmonicity, collisional line shifts, and temperature,” J. Chem. Phys. 115(12), 5418–5426 (2001).
[CrossRef]

Blades, M. W.

Boedeker, L. R.

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(4), 44502 (2006).
[CrossRef] [PubMed]

Cottereau, M. J.

M. J. Cottereau, F. Grisch, and J. J. Marie, “CARS measurements of temperature and species concentrations in an IC engine,” Appl. Phys. B 51(1), 63–66 (1990).
[CrossRef]

Dlott, D. D.

A. Lagutchev, S. A. Hambir, and D. D. Dlott, “Nonresonant background suppression in broadband vibrational sum-frequency generation spectroscopy,” J. Phys. Chem. C 111(37), 13645–13647 (2007).
[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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Eckbreth, A. C.

A. C. Eckbreth and R. J. Hall, “CARS concentration sensitivity with and without non-resonant background suppression,” Combust. Sci. Technol. 25(5), 175–192 (1981).
[CrossRef]

A. C. Eckbreth, “BOXCARS: Crossed-beam phase-matched CARS generation in gases,” Appl. Phys. Lett. 32(7), 421–423 (1978).
[CrossRef]

Farrow, R. L.

Frey, H. M.

P. Beaud, H. M. Frey, T. Lang, and M. Motzkus, “Flame thermometry by femtosecond CARS,” Chem. Phys. Lett. 344(3-4), 407–412 (2001).
[CrossRef]

T. Lang, M. Motzkus, H. M. Frey, and P. Beaud, “High resolution femtosecond coherent anti-Stokes Raman scattering: Determination of rotational constants, molecular anharmonicity, collisional line shifts, and temperature,” J. Chem. Phys. 115(12), 5418–5426 (2001).
[CrossRef]

Gao, Y.

Gord, J. R.

H. U. Stauffer, W. D. Kulatilaka, P. S. Hsu, J. R. Gord, and S. Roy, “Gas-phase thermometry using delayed-probe-pulse picosecond coherent anti-Stokes Raman scattering spectra of H2.,” Appl. Opt. 50(4), A38–A48 (2011).
[CrossRef] [PubMed]

J. D. Miller, M. N. Slipchenko, T. R. Meyer, H. U. Stauffer, and J. R. Gord, “Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering for high-speed gas-phase thermometry,” Opt. Lett. 35, 2430–2432 (2010).
[CrossRef] [PubMed]

P. S. Hsu, A. K. Patnaik, J. R. Gord, T. R. Meyer, W. D. Kulatilaka, and S. Roy, “Investigation of optical fibers for coherent anti-Stokes Raman scattering (CARS) spectroscopy in reacting flows,” Exp. Fluids 49(4), 969–984 (2010).
[CrossRef]

S. Roy, J. R. Gord, and A. Patnaik, “Recent advances in coherent anti-Stokes Raman scattering spectroscopy: Fundamental developements and applications in reacting flows,” Pror. Energy Combust. Sci. 36(2), 280–306 (2010).
[CrossRef]

S. Roy, W. D. Kulatilaka, D. R. Richardson, R. P. Lucht, and J. R. Gord, “Gas-phase single-shot thermometry at 1 kHz using fs-CARS spectroscopy,” Opt. Lett. 34(24), 3857–3859 (2009).
[CrossRef] [PubMed]

S. Roy, P. J. Kinnius, R. P. Lucht, and J. R. Gord, “Temperature measurements in reacting flows by time-resolved femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy,” Opt. Commun. 281(2), 319–325 (2008).
[CrossRef]

J. R. Gord, T. R. Meyer, and S. Roy, “Applications of ultrafast lasers for optical measurements in combusting flows,” Ann. Rev. Anal. Chem. (Palo Alto Calif) 1(1), 663–687 (2008).
[CrossRef] [PubMed]

T. R. Meyer, S. Roy, and J. R. Gord, “Improving signal-to-interference ratio in rich hydrocarbon-air flames using picosecond coherent anti-Stokes Raman scattering,” Appl. Spectrosc. 61(11), 1135–1140 (2007).
[CrossRef] [PubMed]

R. P. Lucht, S. Roy, T. R. Meyer, and J. R. Gord, “Femtosecond coherent anti-Stokes Raman scattering measurement of gas temperatures from frequency-spread dephasing of the Raman coherence,” Appl. Phys. Lett. 89(25), 251112 (2006).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, “Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals,” Appl. Phys. Lett. 87(26), 264103 (2005).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, “Broadband coherent anti-Stokes Raman scattering spectroscopy of nitrogen using a picosecond modeless dye laser,” Opt. Lett. 30(23), 3222–3224 (2005).
[CrossRef] [PubMed]

Grisch, F.

M. J. Cottereau, F. Grisch, and J. J. Marie, “CARS measurements of temperature and species concentrations in an IC engine,” Appl. Phys. B 51(1), 63–66 (1990).
[CrossRef]

Hall, R. J.

R. J. Hall and L. R. Boedeker, “CARS thermometry in fuel-rich combustion zones,” Appl. Opt. 23(9), 1340–1346 (1984).
[CrossRef] [PubMed]

A. C. Eckbreth and R. J. Hall, “CARS concentration sensitivity with and without non-resonant background suppression,” Combust. Sci. Technol. 25(5), 175–192 (1981).
[CrossRef]

Hambir, S. A.

A. Lagutchev, S. A. Hambir, and D. D. Dlott, “Nonresonant background suppression in broadband vibrational sum-frequency generation spectroscopy,” J. Phys. Chem. C 111(37), 13645–13647 (2007).
[CrossRef]

Hsu, P. S.

H. U. Stauffer, W. D. Kulatilaka, P. S. Hsu, J. R. Gord, and S. Roy, “Gas-phase thermometry using delayed-probe-pulse picosecond coherent anti-Stokes Raman scattering spectra of H2.,” Appl. Opt. 50(4), A38–A48 (2011).
[CrossRef] [PubMed]

P. S. Hsu, A. K. Patnaik, J. R. Gord, T. R. Meyer, W. D. Kulatilaka, and S. Roy, “Investigation of optical fibers for coherent anti-Stokes Raman scattering (CARS) spectroscopy in reacting flows,” Exp. Fluids 49(4), 969–984 (2010).
[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(5822), 265–268 (2007).
[CrossRef] [PubMed]

Kamga, F. M.

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(17), 10994–11001 (2002).
[CrossRef] [PubMed]

Kiefer, J.

Kinnius, P. J.

S. Roy, P. J. Kinnius, R. P. Lucht, and J. R. Gord, “Temperature measurements in reacting flows by time-resolved femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy,” Opt. Commun. 281(2), 319–325 (2008).
[CrossRef]

Kliewer, C. J.

Konorov, S. O.

Kulatilaka, W. D.

Lagutchev, A.

A. Lagutchev, S. A. Hambir, and D. D. Dlott, “Nonresonant background suppression in broadband vibrational sum-frequency generation spectroscopy,” J. Phys. Chem. C 111(37), 13645–13647 (2007).
[CrossRef]

Lang, T.

P. Beaud, H. M. Frey, T. Lang, and M. Motzkus, “Flame thermometry by femtosecond CARS,” Chem. Phys. Lett. 344(3-4), 407–412 (2001).
[CrossRef]

T. Lang, M. Motzkus, H. M. Frey, and P. Beaud, “High resolution femtosecond coherent anti-Stokes Raman scattering: Determination of rotational constants, molecular anharmonicity, collisional line shifts, and temperature,” J. Chem. Phys. 115(12), 5418–5426 (2001).
[CrossRef]

Leipertz, A.

Lucht, R. P.

S. Roy, W. D. Kulatilaka, D. R. Richardson, R. P. Lucht, and J. R. Gord, “Gas-phase single-shot thermometry at 1 kHz using fs-CARS spectroscopy,” Opt. Lett. 34(24), 3857–3859 (2009).
[CrossRef] [PubMed]

S. Roy, P. J. Kinnius, R. P. Lucht, and J. R. Gord, “Temperature measurements in reacting flows by time-resolved femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy,” Opt. Commun. 281(2), 319–325 (2008).
[CrossRef]

R. P. Lucht, S. Roy, T. R. Meyer, and J. R. Gord, “Femtosecond coherent anti-Stokes Raman scattering measurement of gas temperatures from frequency-spread dephasing of the Raman coherence,” Appl. Phys. Lett. 89(25), 251112 (2006).
[CrossRef]

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(17), 10994–11001 (2002).
[CrossRef] [PubMed]

R. L. Farrow, R. P. Lucht, and L. A. Rahn, “Measurements of the nonresonant 3rd-order susceptibilities of gases using coherent anti-Stokes Raman spectroscopy,” J. Opt. Soc. Am. B 4(8), 1241–1246 (1987).
[CrossRef]

Marie, J. J.

M. J. Cottereau, F. Grisch, and J. J. Marie, “CARS measurements of temperature and species concentrations in an IC engine,” Appl. Phys. B 51(1), 63–66 (1990).
[CrossRef]

Mattern, P. L.

L. A. Rahn, L. J. Zych, and P. L. Mattern, “Background-free CARS studies of carbon monoxide in a flame,” Opt. Commun. 30(2), 249–252 (1979).
[CrossRef]

Meyer, T. R.

P. S. Hsu, A. K. Patnaik, J. R. Gord, T. R. Meyer, W. D. Kulatilaka, and S. Roy, “Investigation of optical fibers for coherent anti-Stokes Raman scattering (CARS) spectroscopy in reacting flows,” Exp. Fluids 49(4), 969–984 (2010).
[CrossRef]

J. D. Miller, M. N. Slipchenko, T. R. Meyer, H. U. Stauffer, and J. R. Gord, “Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering for high-speed gas-phase thermometry,” Opt. Lett. 35, 2430–2432 (2010).
[CrossRef] [PubMed]

J. R. Gord, T. R. Meyer, and S. Roy, “Applications of ultrafast lasers for optical measurements in combusting flows,” Ann. Rev. Anal. Chem. (Palo Alto Calif) 1(1), 663–687 (2008).
[CrossRef] [PubMed]

T. R. Meyer, S. Roy, and J. R. Gord, “Improving signal-to-interference ratio in rich hydrocarbon-air flames using picosecond coherent anti-Stokes Raman scattering,” Appl. Spectrosc. 61(11), 1135–1140 (2007).
[CrossRef] [PubMed]

R. P. Lucht, S. Roy, T. R. Meyer, and J. R. Gord, “Femtosecond coherent anti-Stokes Raman scattering measurement of gas temperatures from frequency-spread dephasing of the Raman coherence,” Appl. Phys. Lett. 89(25), 251112 (2006).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, “Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals,” Appl. Phys. Lett. 87(26), 264103 (2005).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, “Broadband coherent anti-Stokes Raman scattering spectroscopy of nitrogen using a picosecond modeless dye laser,” Opt. Lett. 30(23), 3222–3224 (2005).
[CrossRef] [PubMed]

Miller, J. D.

Motzkus, M.

T. Lang, M. Motzkus, H. M. Frey, and P. Beaud, “High resolution femtosecond coherent anti-Stokes Raman scattering: Determination of rotational constants, molecular anharmonicity, collisional line shifts, and temperature,” J. Chem. Phys. 115(12), 5418–5426 (2001).
[CrossRef]

P. Beaud, H. M. Frey, T. Lang, and M. Motzkus, “Flame thermometry by femtosecond CARS,” Chem. Phys. Lett. 344(3-4), 407–412 (2001).
[CrossRef]

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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Opatrny, T.

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(17), 10994–11001 (2002).
[CrossRef] [PubMed]

Patnaik, A.

S. Roy, J. R. Gord, and A. Patnaik, “Recent advances in coherent anti-Stokes Raman scattering spectroscopy: Fundamental developements and applications in reacting flows,” Pror. Energy Combust. Sci. 36(2), 280–306 (2010).
[CrossRef]

Patnaik, A. K.

P. S. Hsu, A. K. Patnaik, J. R. Gord, T. R. Meyer, W. D. Kulatilaka, and S. Roy, “Investigation of optical fibers for coherent anti-Stokes Raman scattering (CARS) spectroscopy in reacting flows,” Exp. Fluids 49(4), 969–984 (2010).
[CrossRef]

Patterson, B. D.

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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Pilloff, H.

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(17), 10994–11001 (2002).
[CrossRef] [PubMed]

Prince, B. D.

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(4), 44502 (2006).
[CrossRef] [PubMed]

Prince, B. M.

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(4), 44502 (2006).
[CrossRef] [PubMed]

Rahn, L. A.

Rebane, A.

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(17), 10994–11001 (2002).
[CrossRef] [PubMed]

Richardson, D. R.

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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Roy, S.

H. U. Stauffer, W. D. Kulatilaka, P. S. Hsu, J. R. Gord, and S. Roy, “Gas-phase thermometry using delayed-probe-pulse picosecond coherent anti-Stokes Raman scattering spectra of H2.,” Appl. Opt. 50(4), A38–A48 (2011).
[CrossRef] [PubMed]

S. Roy, J. R. Gord, and A. Patnaik, “Recent advances in coherent anti-Stokes Raman scattering spectroscopy: Fundamental developements and applications in reacting flows,” Pror. Energy Combust. Sci. 36(2), 280–306 (2010).
[CrossRef]

P. S. Hsu, A. K. Patnaik, J. R. Gord, T. R. Meyer, W. D. Kulatilaka, and S. Roy, “Investigation of optical fibers for coherent anti-Stokes Raman scattering (CARS) spectroscopy in reacting flows,” Exp. Fluids 49(4), 969–984 (2010).
[CrossRef]

S. Roy, W. D. Kulatilaka, D. R. Richardson, R. P. Lucht, and J. R. Gord, “Gas-phase single-shot thermometry at 1 kHz using fs-CARS spectroscopy,” Opt. Lett. 34(24), 3857–3859 (2009).
[CrossRef] [PubMed]

J. R. Gord, T. R. Meyer, and S. Roy, “Applications of ultrafast lasers for optical measurements in combusting flows,” Ann. Rev. Anal. Chem. (Palo Alto Calif) 1(1), 663–687 (2008).
[CrossRef] [PubMed]

S. Roy, P. J. Kinnius, R. P. Lucht, and J. R. Gord, “Temperature measurements in reacting flows by time-resolved femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy,” Opt. Commun. 281(2), 319–325 (2008).
[CrossRef]

T. R. Meyer, S. Roy, and J. R. Gord, “Improving signal-to-interference ratio in rich hydrocarbon-air flames using picosecond coherent anti-Stokes Raman scattering,” Appl. Spectrosc. 61(11), 1135–1140 (2007).
[CrossRef] [PubMed]

R. P. Lucht, S. Roy, T. R. Meyer, and J. R. Gord, “Femtosecond coherent anti-Stokes Raman scattering measurement of gas temperatures from frequency-spread dephasing of the Raman coherence,” Appl. Phys. Lett. 89(25), 251112 (2006).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, “Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals,” Appl. Phys. Lett. 87(26), 264103 (2005).
[CrossRef]

S. Roy, T. R. Meyer, and J. R. Gord, “Broadband coherent anti-Stokes Raman scattering spectroscopy of nitrogen using a picosecond modeless dye laser,” Opt. Lett. 30(23), 3222–3224 (2005).
[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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Sceats, M. G.

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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

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(17), 10994–11001 (2002).
[CrossRef] [PubMed]

Seeger, T.

Settersten, T. B.

Slipchenko, M. N.

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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

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(17), 10994–11001 (2002).
[CrossRef] [PubMed]

Stauffer, H. U.

Turner, R. F. B.

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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Zinth, W.

W. Zinth, “Transient coherent Raman-scattering in the time and frequency domain,” Opt. Commun. 34(3), 479–482 (1980).
[CrossRef]

Zubairy, M. S.

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(17), 10994–11001 (2002).
[CrossRef] [PubMed]

Zych, L. J.

L. A. Rahn, L. J. Zych, and P. L. Mattern, “Background-free CARS studies of carbon monoxide in a flame,” Opt. Commun. 30(2), 249–252 (1979).
[CrossRef]

Ann. Rev. Anal. Chem. (Palo Alto Calif) (1)

J. R. Gord, T. R. Meyer, and S. Roy, “Applications of ultrafast lasers for optical measurements in combusting flows,” Ann. Rev. Anal. Chem. (Palo Alto Calif) 1(1), 663–687 (2008).
[CrossRef] [PubMed]

Appl. Opt. (2)

Appl. Phys. B (1)

M. J. Cottereau, F. Grisch, and J. J. Marie, “CARS measurements of temperature and species concentrations in an IC engine,” Appl. Phys. B 51(1), 63–66 (1990).
[CrossRef]

Appl. Phys. Lett. (3)

S. Roy, T. R. Meyer, and J. R. Gord, “Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals,” Appl. Phys. Lett. 87(26), 264103 (2005).
[CrossRef]

R. P. Lucht, S. Roy, T. R. Meyer, and J. R. Gord, “Femtosecond coherent anti-Stokes Raman scattering measurement of gas temperatures from frequency-spread dephasing of the Raman coherence,” Appl. Phys. Lett. 89(25), 251112 (2006).
[CrossRef]

A. C. Eckbreth, “BOXCARS: Crossed-beam phase-matched CARS generation in gases,” Appl. Phys. Lett. 32(7), 421–423 (1978).
[CrossRef]

Appl. Spectrosc. (2)

Chem. Phys. Lett. (1)

P. Beaud, H. M. Frey, T. Lang, and M. Motzkus, “Flame thermometry by femtosecond CARS,” Chem. Phys. Lett. 344(3-4), 407–412 (2001).
[CrossRef]

Combust. Sci. Technol. (1)

A. C. Eckbreth and R. J. Hall, “CARS concentration sensitivity with and without non-resonant background suppression,” Combust. Sci. Technol. 25(5), 175–192 (1981).
[CrossRef]

Exp. Fluids (1)

P. S. Hsu, A. K. Patnaik, J. R. Gord, T. R. Meyer, W. D. Kulatilaka, and S. Roy, “Investigation of optical fibers for coherent anti-Stokes Raman scattering (CARS) spectroscopy in reacting flows,” Exp. Fluids 49(4), 969–984 (2010).
[CrossRef]

J. Chem. Phys. (2)

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(4), 44502 (2006).
[CrossRef] [PubMed]

T. Lang, M. Motzkus, H. M. Frey, and P. Beaud, “High resolution femtosecond coherent anti-Stokes Raman scattering: Determination of rotational constants, molecular anharmonicity, collisional line shifts, and temperature,” J. Chem. Phys. 115(12), 5418–5426 (2001).
[CrossRef]

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

J. Phys. Chem. C (1)

A. Lagutchev, S. A. Hambir, and D. D. Dlott, “Nonresonant background suppression in broadband vibrational sum-frequency generation spectroscopy,” J. Phys. Chem. C 111(37), 13645–13647 (2007).
[CrossRef]

Opt. Commun. (3)

L. A. Rahn, L. J. Zych, and P. L. Mattern, “Background-free CARS studies of carbon monoxide in a flame,” Opt. Commun. 30(2), 249–252 (1979).
[CrossRef]

W. Zinth, “Transient coherent Raman-scattering in the time and frequency domain,” Opt. Commun. 34(3), 479–482 (1980).
[CrossRef]

S. Roy, P. J. Kinnius, R. P. Lucht, and J. R. Gord, “Temperature measurements in reacting flows by time-resolved femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy,” Opt. Commun. 281(2), 319–325 (2008).
[CrossRef]

Opt. Lett. (6)

Proc. Natl. Acad. Sci. U.S.A. (1)

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(17), 10994–11001 (2002).
[CrossRef] [PubMed]

Pror. Energy Combust. Sci. (1)

S. Roy, J. R. Gord, and A. Patnaik, “Recent advances in coherent anti-Stokes Raman scattering spectroscopy: Fundamental developements and applications in reacting flows,” Pror. Energy Combust. Sci. 36(2), 280–306 (2010).
[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, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Other (2)

D. Pestov, X. Wang, D. Cristancho, K. R. Hall, A. V. Sokolov, and M. O. Scully, “Real-time sensing of gas phase mixtures via coherent Raman spectroscopy,” in 2008 Conference on Lasers and Electro-Optics & Quantum Electronics and Laser Science Conference, Vols 1–9, 1471–1472 (2008).

A. C. Eckbreth, Laser Diagnostics for Combustion Temperature and Species (Abacus Press, 1988).

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Figures (5)

Fig. 1
Fig. 1

(a) Energy diagram for hybrid fs/ps CARS illustrating spectral characteristics of pump (ω1), Stokes (ω2), probe (ω3), and CARS (ωCARS) beams, and (b) timing diagram illustrating temporal lineshapes generated with 4-f pulse shaper and Lorentzian filter with respective delays of τ4f and τL.

Fig. 2
Fig. 2

Schematic diagram of (a) folded 4-f pulse shaper utilizing square slit, and (b) drop-in filter producing Lorentzian lineshape.

Fig. 3
Fig. 3

(a) Experimentally measured spectral lineshape and (b) normalized nonresonant background decay for 850-μm slit, 400-μm slit, and Lorentzian filter. Solid lines in (b) represent fits to the sinc2 and exponential pulse profiles.

Fig. 4
Fig. 4

Comparison of resonant (ν0 → ν1) and nonresonant CARS intensity for 4-f pulse shaper with (a) 850-μm slit, (b) 400-μm slit, and (c) Lorentzian filter. Dashed lines are fit to experimental data (open symbols). Data are normalized to unity.

Fig. 5
Fig. 5

Comparison of spectrally resolved CARS signal for different probe pulse shapes. Left column represents experimental data collected at τ = 0 using (a) the 850-μm slit, (b) the 400-μm slit, and (c) the Lorentzian filter. Right column represents experimental data and simulations (2000 K) at (a) τ = 2.77 ps for the 850-μm slit, (b) τ = 5.5 ps for the 400-μm slit, and (c) τ = 0.31 ps for the Lorentzian filter. Data in (a-c) are normalized to unity and the nonresonant contribution of (a), while data and simulations in (d-f) are normalized to unity.

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