Abstract

We introduce a multiplex technique for the single-laser-shot determination of S-branch Raman linewidths with high accuracy and precision by implementing hybrid femtosecond (fs)/picosecond (ps) rotational coherent anti-Stokes Raman spectroscopy (CARS) with multiple spatially and temporally separated probe beams derived from a single laser pulse. The probe beams scatter from the rotational coherence driven by the fs pump and Stokes pulses at four different probe pulse delay times spanning 360 ps, thereby mapping collisional coherence dephasing in time for the populated rotational levels. The probe beams scatter at different folded BOXCARS angles, yielding spatially separated CARS signals which are collected simultaneously on the charge coupled device camera. The technique yields a single-shot standard deviation (1σ) of less than 3.5% in the determination of Raman linewidths and the average linewidth values obtained for N2 are within 1% of those previously reported. The presented technique opens the possibility for correcting CARS spectra for time-varying collisional environments in operando.

© 2013 Optical Society of America

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  1. A. C. Eckbreth, Laser Diagnostics for Combustion Temperature and Species (Gordon and Breach, 1996).
  2. S. Roy, J. R. Gord, and A. K. Patnaik, Prog. Energy Combust. Sci. 36, 280 (2010).
    [CrossRef]
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    [CrossRef]
  4. A. Bohlin, F. Vestin, P. Joubert, J. Bonamy, and P. E. Bengtsson, J. Raman Spectrosc. 40, 788 (2009).
    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
  8. C. C. Hayden and D. W. Chandler, J. Chem. Phys. 103, 10465 (1995).
    [CrossRef]
  9. W. D. Kulatilaka, P. S. Hsu, H. U. Stauffer, J. R. Gord, and S. Roy, Appl. Phys. Lett. 97, 081112 (2010).
    [CrossRef]
  10. C. J. Kliewer, Y. Gao, T. Seeger, J. Kiefer, B. D. Patterson, and T. B. Settersten, Proc. Combust. Inst. 33, 831 (2011).
    [CrossRef]
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    [CrossRef]
  13. C. J. Kliewer, A. Bohlin, E. Nordstrom, B. D. Patterson, P. E. Bengtsson, and T. B. Settersten, Appl. Phys. B 108, 419 (2012).
    [CrossRef]
  14. S. Roy, P. S. Hsu, N. Jiang, J. R. Gord, W. D. Kulatilaka, H. U. Stauffer, and J. R. Gord, J. Chem. Phys. 138, 024201 (2013).
    [CrossRef]
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    [CrossRef]
  16. O. Yue, M. T. Bremer, D. Pestov, J. R. Gord, S. Roy, and M. Dantus, J. Phys. Chem. A 116, 8138 (2012).
    [CrossRef]
  17. B. D. Prince, A. Chakraborty, B. M. Prince, and H. U. Stauffer, J. Chem. Phys. 125, 044502 (2006).
    [CrossRef]
  18. R. P. Lucht, P. J. Kinnius, S. Roy, and J. R. Gord, J. Chem. Phys. 127, 044316 (2007).
    [CrossRef]
  19. J. D. Miller, S. Roy, M. N. Slipchenko, J. R. Gord, and T. R. Meyer, Opt. Express 19, 15627 (2011).
    [CrossRef]
  20. A. Bohlin, B. D. Patterson, and C. J. Kliewer, J. Chem. Phys. 138, 081102 (2013).
    [CrossRef]
  21. A. C. Eckbreth, Appl. Phys. Lett. 32, 421 (1978).
    [CrossRef]
  22. J. D. Miller, C. E. Dedic, S. Roy, J. R. Gord, and T. R. Meyer, Opt. Express 20, 5003 (2012).
    [CrossRef]
  23. S. P. Kearney, D. J. Scoglietti, and C. J. Kliewer, Opt. Express 21, 12327 (2013).
    [CrossRef]
  24. A. Bohlin and C. J. Kliewer, J. Chem. Phys. 138, 221101 (2013).
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2013 (6)

A. Bohlin, E. Nordström, H. Carlsson, X.-S. Bai, and P.-E. Bengtsson, Proc. Combust. Inst. 34, 3629 (2013).
[CrossRef]

S. Roy, P. S. Hsu, N. Jiang, J. R. Gord, W. D. Kulatilaka, H. U. Stauffer, and J. R. Gord, J. Chem. Phys. 138, 024201 (2013).
[CrossRef]

Y. Gao, A. Bohlin, T. Seeger, P. E. Bengtsson, and C. J. Kliewer, Proc. Combust. Inst. 34, 3637 (2013).
[CrossRef]

A. Bohlin, B. D. Patterson, and C. J. Kliewer, J. Chem. Phys. 138, 081102 (2013).
[CrossRef]

S. P. Kearney, D. J. Scoglietti, and C. J. Kliewer, Opt. Express 21, 12327 (2013).
[CrossRef]

A. Bohlin and C. J. Kliewer, J. Chem. Phys. 138, 221101 (2013).
[CrossRef]

2012 (4)

J. D. Miller, C. E. Dedic, S. Roy, J. R. Gord, and T. R. Meyer, Opt. Express 20, 5003 (2012).
[CrossRef]

O. Yue, M. T. Bremer, D. Pestov, J. R. Gord, S. Roy, and M. Dantus, J. Phys. Chem. A 116, 8138 (2012).
[CrossRef]

A. Bohlin, E. Nordstrom, B. D. Patterson, P.-E. Bengtsson, and C. J. Kliewer, J. Chem. Phys. 137, 074302 (2012).
[CrossRef]

C. J. Kliewer, A. Bohlin, E. Nordstrom, B. D. Patterson, P. E. Bengtsson, and T. B. Settersten, Appl. Phys. B 108, 419 (2012).
[CrossRef]

2011 (3)

C. J. Kliewer, Y. Gao, T. Seeger, J. Kiefer, B. D. Patterson, and T. B. Settersten, Proc. Combust. Inst. 33, 831 (2011).
[CrossRef]

J. D. Miller, S. Roy, J. R. Gord, and T. R. Meyer, J. Chem. Phys. 135, 201104 (2011).
[CrossRef]

J. D. Miller, S. Roy, M. N. Slipchenko, J. R. Gord, and T. R. Meyer, Opt. Express 19, 15627 (2011).
[CrossRef]

2010 (2)

S. Roy, J. R. Gord, and A. K. Patnaik, Prog. Energy Combust. Sci. 36, 280 (2010).
[CrossRef]

W. D. Kulatilaka, P. S. Hsu, H. U. Stauffer, J. R. Gord, and S. Roy, Appl. Phys. Lett. 97, 081112 (2010).
[CrossRef]

2009 (1)

A. Bohlin, F. Vestin, P. Joubert, J. Bonamy, and P. E. Bengtsson, J. Raman Spectrosc. 40, 788 (2009).
[CrossRef]

2007 (1)

R. P. Lucht, P. J. Kinnius, S. Roy, and J. R. Gord, J. Chem. Phys. 127, 044316 (2007).
[CrossRef]

2006 (1)

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

1995 (1)

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

1991 (1)

L. A. Rahn, R. L. Farrow, and G. J. Rosasco, Phys. Rev. A 43, 6075 (1991).
[CrossRef]

1990 (1)

D. A. Greenhalgh and L. A. Rahn, J. Raman Spectrosc. 21, 847 (1990).
[CrossRef]

1986 (1)

1978 (1)

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

Bai, X.-S.

A. Bohlin, E. Nordström, H. Carlsson, X.-S. Bai, and P.-E. Bengtsson, Proc. Combust. Inst. 34, 3629 (2013).
[CrossRef]

Bengtsson, P. E.

Y. Gao, A. Bohlin, T. Seeger, P. E. Bengtsson, and C. J. Kliewer, Proc. Combust. Inst. 34, 3637 (2013).
[CrossRef]

C. J. Kliewer, A. Bohlin, E. Nordstrom, B. D. Patterson, P. E. Bengtsson, and T. B. Settersten, Appl. Phys. B 108, 419 (2012).
[CrossRef]

A. Bohlin, F. Vestin, P. Joubert, J. Bonamy, and P. E. Bengtsson, J. Raman Spectrosc. 40, 788 (2009).
[CrossRef]

Bengtsson, P.-E.

A. Bohlin, E. Nordström, H. Carlsson, X.-S. Bai, and P.-E. Bengtsson, Proc. Combust. Inst. 34, 3629 (2013).
[CrossRef]

A. Bohlin, E. Nordstrom, B. D. Patterson, P.-E. Bengtsson, and C. J. Kliewer, J. Chem. Phys. 137, 074302 (2012).
[CrossRef]

Bohlin, A.

Y. Gao, A. Bohlin, T. Seeger, P. E. Bengtsson, and C. J. Kliewer, Proc. Combust. Inst. 34, 3637 (2013).
[CrossRef]

A. Bohlin, E. Nordström, H. Carlsson, X.-S. Bai, and P.-E. Bengtsson, Proc. Combust. Inst. 34, 3629 (2013).
[CrossRef]

A. Bohlin, B. D. Patterson, and C. J. Kliewer, J. Chem. Phys. 138, 081102 (2013).
[CrossRef]

A. Bohlin and C. J. Kliewer, J. Chem. Phys. 138, 221101 (2013).
[CrossRef]

A. Bohlin, E. Nordstrom, B. D. Patterson, P.-E. Bengtsson, and C. J. Kliewer, J. Chem. Phys. 137, 074302 (2012).
[CrossRef]

C. J. Kliewer, A. Bohlin, E. Nordstrom, B. D. Patterson, P. E. Bengtsson, and T. B. Settersten, Appl. Phys. B 108, 419 (2012).
[CrossRef]

A. Bohlin, F. Vestin, P. Joubert, J. Bonamy, and P. E. Bengtsson, J. Raman Spectrosc. 40, 788 (2009).
[CrossRef]

Bonamy, J.

A. Bohlin, F. Vestin, P. Joubert, J. Bonamy, and P. E. Bengtsson, J. Raman Spectrosc. 40, 788 (2009).
[CrossRef]

Bremer, M. T.

O. Yue, M. T. Bremer, D. Pestov, J. R. Gord, S. Roy, and M. Dantus, J. Phys. Chem. A 116, 8138 (2012).
[CrossRef]

Carlsson, H.

A. Bohlin, E. Nordström, H. Carlsson, X.-S. Bai, and P.-E. Bengtsson, Proc. Combust. Inst. 34, 3629 (2013).
[CrossRef]

Chakraborty, A.

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

Chandler, D. W.

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

Dantus, M.

O. Yue, M. T. Bremer, D. Pestov, J. R. Gord, S. Roy, and M. Dantus, J. Phys. Chem. A 116, 8138 (2012).
[CrossRef]

Dedic, C. E.

Eckbreth, A. C.

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

A. C. Eckbreth, Laser Diagnostics for Combustion Temperature and Species (Gordon and Breach, 1996).

Farrow, R. L.

L. A. Rahn, R. L. Farrow, and G. J. Rosasco, Phys. Rev. A 43, 6075 (1991).
[CrossRef]

Gao, Y.

Y. Gao, A. Bohlin, T. Seeger, P. E. Bengtsson, and C. J. Kliewer, Proc. Combust. Inst. 34, 3637 (2013).
[CrossRef]

C. J. Kliewer, Y. Gao, T. Seeger, J. Kiefer, B. D. Patterson, and T. B. Settersten, Proc. Combust. Inst. 33, 831 (2011).
[CrossRef]

Gord, J. R.

S. Roy, P. S. Hsu, N. Jiang, J. R. Gord, W. D. Kulatilaka, H. U. Stauffer, and J. R. Gord, J. Chem. Phys. 138, 024201 (2013).
[CrossRef]

S. Roy, P. S. Hsu, N. Jiang, J. R. Gord, W. D. Kulatilaka, H. U. Stauffer, and J. R. Gord, J. Chem. Phys. 138, 024201 (2013).
[CrossRef]

O. Yue, M. T. Bremer, D. Pestov, J. R. Gord, S. Roy, and M. Dantus, J. Phys. Chem. A 116, 8138 (2012).
[CrossRef]

J. D. Miller, C. E. Dedic, S. Roy, J. R. Gord, and T. R. Meyer, Opt. Express 20, 5003 (2012).
[CrossRef]

J. D. Miller, S. Roy, M. N. Slipchenko, J. R. Gord, and T. R. Meyer, Opt. Express 19, 15627 (2011).
[CrossRef]

J. D. Miller, S. Roy, J. R. Gord, and T. R. Meyer, J. Chem. Phys. 135, 201104 (2011).
[CrossRef]

W. D. Kulatilaka, P. S. Hsu, H. U. Stauffer, J. R. Gord, and S. Roy, Appl. Phys. Lett. 97, 081112 (2010).
[CrossRef]

S. Roy, J. R. Gord, and A. K. Patnaik, Prog. Energy Combust. Sci. 36, 280 (2010).
[CrossRef]

R. P. Lucht, P. J. Kinnius, S. Roy, and J. R. Gord, J. Chem. Phys. 127, 044316 (2007).
[CrossRef]

Greenhalgh, D. A.

D. A. Greenhalgh and L. A. Rahn, J. Raman Spectrosc. 21, 847 (1990).
[CrossRef]

Hayden, C. C.

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

Hsu, P. S.

S. Roy, P. S. Hsu, N. Jiang, J. R. Gord, W. D. Kulatilaka, H. U. Stauffer, and J. R. Gord, J. Chem. Phys. 138, 024201 (2013).
[CrossRef]

W. D. Kulatilaka, P. S. Hsu, H. U. Stauffer, J. R. Gord, and S. Roy, Appl. Phys. Lett. 97, 081112 (2010).
[CrossRef]

Jiang, N.

S. Roy, P. S. Hsu, N. Jiang, J. R. Gord, W. D. Kulatilaka, H. U. Stauffer, and J. R. Gord, J. Chem. Phys. 138, 024201 (2013).
[CrossRef]

Joubert, P.

A. Bohlin, F. Vestin, P. Joubert, J. Bonamy, and P. E. Bengtsson, J. Raman Spectrosc. 40, 788 (2009).
[CrossRef]

Kearney, S. P.

Kiefer, J.

C. J. Kliewer, Y. Gao, T. Seeger, J. Kiefer, B. D. Patterson, and T. B. Settersten, Proc. Combust. Inst. 33, 831 (2011).
[CrossRef]

Kinnius, P. J.

R. P. Lucht, P. J. Kinnius, S. Roy, and J. R. Gord, J. Chem. Phys. 127, 044316 (2007).
[CrossRef]

Kliewer, C. J.

A. Bohlin, B. D. Patterson, and C. J. Kliewer, J. Chem. Phys. 138, 081102 (2013).
[CrossRef]

S. P. Kearney, D. J. Scoglietti, and C. J. Kliewer, Opt. Express 21, 12327 (2013).
[CrossRef]

A. Bohlin and C. J. Kliewer, J. Chem. Phys. 138, 221101 (2013).
[CrossRef]

Y. Gao, A. Bohlin, T. Seeger, P. E. Bengtsson, and C. J. Kliewer, Proc. Combust. Inst. 34, 3637 (2013).
[CrossRef]

A. Bohlin, E. Nordstrom, B. D. Patterson, P.-E. Bengtsson, and C. J. Kliewer, J. Chem. Phys. 137, 074302 (2012).
[CrossRef]

C. J. Kliewer, A. Bohlin, E. Nordstrom, B. D. Patterson, P. E. Bengtsson, and T. B. Settersten, Appl. Phys. B 108, 419 (2012).
[CrossRef]

C. J. Kliewer, Y. Gao, T. Seeger, J. Kiefer, B. D. Patterson, and T. B. Settersten, Proc. Combust. Inst. 33, 831 (2011).
[CrossRef]

Kulatilaka, W. D.

S. Roy, P. S. Hsu, N. Jiang, J. R. Gord, W. D. Kulatilaka, H. U. Stauffer, and J. R. Gord, J. Chem. Phys. 138, 024201 (2013).
[CrossRef]

W. D. Kulatilaka, P. S. Hsu, H. U. Stauffer, J. R. Gord, and S. Roy, Appl. Phys. Lett. 97, 081112 (2010).
[CrossRef]

Lucht, R. P.

R. P. Lucht, P. J. Kinnius, S. Roy, and J. R. Gord, J. Chem. Phys. 127, 044316 (2007).
[CrossRef]

Meyer, T. R.

Miller, J. D.

Nordstrom, E.

A. Bohlin, E. Nordstrom, B. D. Patterson, P.-E. Bengtsson, and C. J. Kliewer, J. Chem. Phys. 137, 074302 (2012).
[CrossRef]

C. J. Kliewer, A. Bohlin, E. Nordstrom, B. D. Patterson, P. E. Bengtsson, and T. B. Settersten, Appl. Phys. B 108, 419 (2012).
[CrossRef]

Nordström, E.

A. Bohlin, E. Nordström, H. Carlsson, X.-S. Bai, and P.-E. Bengtsson, Proc. Combust. Inst. 34, 3629 (2013).
[CrossRef]

Palmer, R. E.

Patnaik, A. K.

S. Roy, J. R. Gord, and A. K. Patnaik, Prog. Energy Combust. Sci. 36, 280 (2010).
[CrossRef]

Patterson, B. D.

A. Bohlin, B. D. Patterson, and C. J. Kliewer, J. Chem. Phys. 138, 081102 (2013).
[CrossRef]

C. J. Kliewer, A. Bohlin, E. Nordstrom, B. D. Patterson, P. E. Bengtsson, and T. B. Settersten, Appl. Phys. B 108, 419 (2012).
[CrossRef]

A. Bohlin, E. Nordstrom, B. D. Patterson, P.-E. Bengtsson, and C. J. Kliewer, J. Chem. Phys. 137, 074302 (2012).
[CrossRef]

C. J. Kliewer, Y. Gao, T. Seeger, J. Kiefer, B. D. Patterson, and T. B. Settersten, Proc. Combust. Inst. 33, 831 (2011).
[CrossRef]

Pestov, D.

O. Yue, M. T. Bremer, D. Pestov, J. R. Gord, S. Roy, and M. Dantus, J. Phys. Chem. A 116, 8138 (2012).
[CrossRef]

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]

Rahn, L. A.

L. A. Rahn, R. L. Farrow, and G. J. Rosasco, Phys. Rev. A 43, 6075 (1991).
[CrossRef]

D. A. Greenhalgh and L. A. Rahn, J. Raman Spectrosc. 21, 847 (1990).
[CrossRef]

L. A. Rahn and R. E. Palmer, J. Opt. Soc. Am. B 3, 1164 (1986).
[CrossRef]

Rosasco, G. J.

L. A. Rahn, R. L. Farrow, and G. J. Rosasco, Phys. Rev. A 43, 6075 (1991).
[CrossRef]

Roy, S.

S. Roy, P. S. Hsu, N. Jiang, J. R. Gord, W. D. Kulatilaka, H. U. Stauffer, and J. R. Gord, J. Chem. Phys. 138, 024201 (2013).
[CrossRef]

O. Yue, M. T. Bremer, D. Pestov, J. R. Gord, S. Roy, and M. Dantus, J. Phys. Chem. A 116, 8138 (2012).
[CrossRef]

J. D. Miller, C. E. Dedic, S. Roy, J. R. Gord, and T. R. Meyer, Opt. Express 20, 5003 (2012).
[CrossRef]

J. D. Miller, S. Roy, M. N. Slipchenko, J. R. Gord, and T. R. Meyer, Opt. Express 19, 15627 (2011).
[CrossRef]

J. D. Miller, S. Roy, J. R. Gord, and T. R. Meyer, J. Chem. Phys. 135, 201104 (2011).
[CrossRef]

W. D. Kulatilaka, P. S. Hsu, H. U. Stauffer, J. R. Gord, and S. Roy, Appl. Phys. Lett. 97, 081112 (2010).
[CrossRef]

S. Roy, J. R. Gord, and A. K. Patnaik, Prog. Energy Combust. Sci. 36, 280 (2010).
[CrossRef]

R. P. Lucht, P. J. Kinnius, S. Roy, and J. R. Gord, J. Chem. Phys. 127, 044316 (2007).
[CrossRef]

Scoglietti, D. J.

Seeger, T.

Y. Gao, A. Bohlin, T. Seeger, P. E. Bengtsson, and C. J. Kliewer, Proc. Combust. Inst. 34, 3637 (2013).
[CrossRef]

C. J. Kliewer, Y. Gao, T. Seeger, J. Kiefer, B. D. Patterson, and T. B. Settersten, Proc. Combust. Inst. 33, 831 (2011).
[CrossRef]

Settersten, T. B.

C. J. Kliewer, A. Bohlin, E. Nordstrom, B. D. Patterson, P. E. Bengtsson, and T. B. Settersten, Appl. Phys. B 108, 419 (2012).
[CrossRef]

C. J. Kliewer, Y. Gao, T. Seeger, J. Kiefer, B. D. Patterson, and T. B. Settersten, Proc. Combust. Inst. 33, 831 (2011).
[CrossRef]

Slipchenko, M. N.

Stauffer, H. U.

S. Roy, P. S. Hsu, N. Jiang, J. R. Gord, W. D. Kulatilaka, H. U. Stauffer, and J. R. Gord, J. Chem. Phys. 138, 024201 (2013).
[CrossRef]

W. D. Kulatilaka, P. S. Hsu, H. U. Stauffer, J. R. Gord, and S. Roy, Appl. Phys. Lett. 97, 081112 (2010).
[CrossRef]

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

Vestin, F.

A. Bohlin, F. Vestin, P. Joubert, J. Bonamy, and P. E. Bengtsson, J. Raman Spectrosc. 40, 788 (2009).
[CrossRef]

Yue, O.

O. Yue, M. T. Bremer, D. Pestov, J. R. Gord, S. Roy, and M. Dantus, J. Phys. Chem. A 116, 8138 (2012).
[CrossRef]

Appl. Phys. B (1)

C. J. Kliewer, A. Bohlin, E. Nordstrom, B. D. Patterson, P. E. Bengtsson, and T. B. Settersten, Appl. Phys. B 108, 419 (2012).
[CrossRef]

Appl. Phys. Lett. (2)

W. D. Kulatilaka, P. S. Hsu, H. U. Stauffer, J. R. Gord, and S. Roy, Appl. Phys. Lett. 97, 081112 (2010).
[CrossRef]

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

J. Chem. Phys. (8)

A. Bohlin, B. D. Patterson, and C. J. Kliewer, J. Chem. Phys. 138, 081102 (2013).
[CrossRef]

A. Bohlin and C. J. Kliewer, J. Chem. Phys. 138, 221101 (2013).
[CrossRef]

S. Roy, P. S. Hsu, N. Jiang, J. R. Gord, W. D. Kulatilaka, H. U. Stauffer, and J. R. Gord, J. Chem. Phys. 138, 024201 (2013).
[CrossRef]

J. D. Miller, S. Roy, J. R. Gord, and T. R. Meyer, J. Chem. Phys. 135, 201104 (2011).
[CrossRef]

A. Bohlin, E. Nordstrom, B. D. Patterson, P.-E. Bengtsson, and C. J. Kliewer, J. Chem. Phys. 137, 074302 (2012).
[CrossRef]

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

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

R. P. Lucht, P. J. Kinnius, S. Roy, and J. R. Gord, J. Chem. Phys. 127, 044316 (2007).
[CrossRef]

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

J. Phys. Chem. A (1)

O. Yue, M. T. Bremer, D. Pestov, J. R. Gord, S. Roy, and M. Dantus, J. Phys. Chem. A 116, 8138 (2012).
[CrossRef]

J. Raman Spectrosc. (2)

A. Bohlin, F. Vestin, P. Joubert, J. Bonamy, and P. E. Bengtsson, J. Raman Spectrosc. 40, 788 (2009).
[CrossRef]

D. A. Greenhalgh and L. A. Rahn, J. Raman Spectrosc. 21, 847 (1990).
[CrossRef]

Opt. Express (3)

Phys. Rev. A (1)

L. A. Rahn, R. L. Farrow, and G. J. Rosasco, Phys. Rev. A 43, 6075 (1991).
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Figures (4)

Fig. 1.
Fig. 1.

Experimental arrangement for split-probe fs/ps CARS. (a) BD, beam dump; BS, nonpolarizing beam splitter; DM, dichroic mirror; HP, half-wave plate; L, lens; M, mirror; P, prism; PBS, polarizing beam splitter; SPF, short-pass filter; TS, translation stage. The red beams are the time-coincident fs pump/Stokes pulses, and the green beams are the time-delayed probe pulses. (b) The region near the beam crossing. The interaction generates four signal beams emitted from the probe region at different angles.

Fig. 2.
Fig. 2.

Single-shot, split-probe CARS signal on the CCD. The differing folded BOXCARS angles yield spatially isolated signals corresponding to different probe delay times.

Fig. 3.
Fig. 3.

Single shot analysis of a single rotational transition. Four data points from the four spatially separated probes (red circles) map the state-specific coherence decay. The inverse slope of the line fitted through the data yields the exponential decay constant, τ.

Fig. 4.
Fig. 4.

Single laser shot measurements of N2 Raman broadening coefficients. Shown are 3 of the 20 such coefficients measured at 295 K. The standard deviation (1σ) is <3.5% for all measured coefficients.

Equations (1)

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ΓJ=(2πcτCARS,J)1,

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