Abstract

We demonstrate that the value of the underlying frequency–frequency correlation function can be retrieved from a two-dimensional optical correlation spectrum through a simple relationship. The proposed method yields both intuitive clues and a quantitative measure of the dynamics of the system. The technique is applied to studying the effects of temperature and phase changes on liquid-glass solvent dynamics.

© 2006 Optical Society of America

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  1. D. M. Jonas, Annu. Rev. Phys. Chem. 54, 425 (2003).
    [CrossRef] [PubMed]
  2. K. Okumura, A. Tokmakoff, and Y. Tanimura, Chem. Phys. Lett. 314, 488 (1999).
    [CrossRef]
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    [CrossRef] [PubMed]
  4. P. Hamm, M. Lim, W. F. DeGrado, and R. M. Hochstrasser, Proc. Natl. Acad. Sci. U.S.A. 96, 2036 (1999).
    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef]
  8. W. P. de Boeij, M. S. Pshenichnikov, and D. A. Wiersma, J. Phys. Chem. 100, 11806 (1996).
    [CrossRef]
  9. S. Yeremenko, M. S. Pshenichnikov, and D. A. Wiersma, Phys. Rev. A 73, 21804 (2006).
    [CrossRef]
  10. Y. Tanimura and S. Mukamel, Phys. Rev. E 47, 118 (1993).
    [CrossRef]
  11. K. Kwac and M. H. Cho, J. Phys. Chem. 119, 2256 (2003).
    [CrossRef]
  12. S. Woutersen, Y. Mu, G. Stock, and P. Hamm, Chem. Phys. 266, 137 (2001).
    [CrossRef]
  13. J. Zheng, K. Kwak, J. Asbury, X. Chen, I. R. Piletic, and M. D. Fayer, Science 309, 1338 (2005).
    [CrossRef] [PubMed]
  14. C. J. Bardeen and C. V. Shank, Chem. Phys. Lett. 203, 535 (1993).
    [CrossRef]
  15. M. Aihara, Phys. Rev. B 25, 53 (1982).
    [CrossRef]

2006 (1)

S. Yeremenko, M. S. Pshenichnikov, and D. A. Wiersma, Phys. Rev. A 73, 21804 (2006).
[CrossRef]

2005 (2)

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, Nature 434, 625 (2005).
[CrossRef] [PubMed]

J. Zheng, K. Kwak, J. Asbury, X. Chen, I. R. Piletic, and M. D. Fayer, Science 309, 1338 (2005).
[CrossRef] [PubMed]

2003 (3)

K. Kwac and M. H. Cho, J. Phys. Chem. 119, 2256 (2003).
[CrossRef]

D. M. Jonas, Annu. Rev. Phys. Chem. 54, 425 (2003).
[CrossRef] [PubMed]

C. J. Fecko, J. D. Eaves, J. J. Loparo, A. Tokmakoff, and P. L. Geissler, Science 301, 1698 (2003).
[CrossRef] [PubMed]

2001 (1)

S. Woutersen, Y. Mu, G. Stock, and P. Hamm, Chem. Phys. 266, 137 (2001).
[CrossRef]

1999 (2)

P. Hamm, M. Lim, W. F. DeGrado, and R. M. Hochstrasser, Proc. Natl. Acad. Sci. U.S.A. 96, 2036 (1999).
[CrossRef] [PubMed]

K. Okumura, A. Tokmakoff, and Y. Tanimura, Chem. Phys. Lett. 314, 488 (1999).
[CrossRef]

1996 (1)

W. P. de Boeij, M. S. Pshenichnikov, and D. A. Wiersma, J. Phys. Chem. 100, 11806 (1996).
[CrossRef]

1993 (2)

C. J. Bardeen and C. V. Shank, Chem. Phys. Lett. 203, 535 (1993).
[CrossRef]

Y. Tanimura and S. Mukamel, Phys. Rev. E 47, 118 (1993).
[CrossRef]

1985 (1)

1982 (1)

M. Aihara, Phys. Rev. B 25, 53 (1982).
[CrossRef]

Aihara, M.

M. Aihara, Phys. Rev. B 25, 53 (1982).
[CrossRef]

Asbury, J.

J. Zheng, K. Kwak, J. Asbury, X. Chen, I. R. Piletic, and M. D. Fayer, Science 309, 1338 (2005).
[CrossRef] [PubMed]

Bardeen, C. J.

C. J. Bardeen and C. V. Shank, Chem. Phys. Lett. 203, 535 (1993).
[CrossRef]

Blankenship, R. E.

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, Nature 434, 625 (2005).
[CrossRef] [PubMed]

Brixner, T.

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, Nature 434, 625 (2005).
[CrossRef] [PubMed]

Chen, X.

J. Zheng, K. Kwak, J. Asbury, X. Chen, I. R. Piletic, and M. D. Fayer, Science 309, 1338 (2005).
[CrossRef] [PubMed]

Cho, M.

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, Nature 434, 625 (2005).
[CrossRef] [PubMed]

Cho, M. H.

K. Kwac and M. H. Cho, J. Phys. Chem. 119, 2256 (2003).
[CrossRef]

de Boeij, W. P.

W. P. de Boeij, M. S. Pshenichnikov, and D. A. Wiersma, J. Phys. Chem. 100, 11806 (1996).
[CrossRef]

de Silvestri, S.

DeGrado, W. F.

P. Hamm, M. Lim, W. F. DeGrado, and R. M. Hochstrasser, Proc. Natl. Acad. Sci. U.S.A. 96, 2036 (1999).
[CrossRef] [PubMed]

Eaves, J. D.

C. J. Fecko, J. D. Eaves, J. J. Loparo, A. Tokmakoff, and P. L. Geissler, Science 301, 1698 (2003).
[CrossRef] [PubMed]

Fayer, M. D.

J. Zheng, K. Kwak, J. Asbury, X. Chen, I. R. Piletic, and M. D. Fayer, Science 309, 1338 (2005).
[CrossRef] [PubMed]

Fecko, C. J.

C. J. Fecko, J. D. Eaves, J. J. Loparo, A. Tokmakoff, and P. L. Geissler, Science 301, 1698 (2003).
[CrossRef] [PubMed]

Fleming, G. R.

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, Nature 434, 625 (2005).
[CrossRef] [PubMed]

Geissler, P. L.

C. J. Fecko, J. D. Eaves, J. J. Loparo, A. Tokmakoff, and P. L. Geissler, Science 301, 1698 (2003).
[CrossRef] [PubMed]

Hamm, P.

S. Woutersen, Y. Mu, G. Stock, and P. Hamm, Chem. Phys. 266, 137 (2001).
[CrossRef]

P. Hamm, M. Lim, W. F. DeGrado, and R. M. Hochstrasser, Proc. Natl. Acad. Sci. U.S.A. 96, 2036 (1999).
[CrossRef] [PubMed]

Hochstrasser, R. M.

P. Hamm, M. Lim, W. F. DeGrado, and R. M. Hochstrasser, Proc. Natl. Acad. Sci. U.S.A. 96, 2036 (1999).
[CrossRef] [PubMed]

Ippen, E. P.

Jonas, D. M.

D. M. Jonas, Annu. Rev. Phys. Chem. 54, 425 (2003).
[CrossRef] [PubMed]

Kwac, K.

K. Kwac and M. H. Cho, J. Phys. Chem. 119, 2256 (2003).
[CrossRef]

Kwak, K.

J. Zheng, K. Kwak, J. Asbury, X. Chen, I. R. Piletic, and M. D. Fayer, Science 309, 1338 (2005).
[CrossRef] [PubMed]

Lim, M.

P. Hamm, M. Lim, W. F. DeGrado, and R. M. Hochstrasser, Proc. Natl. Acad. Sci. U.S.A. 96, 2036 (1999).
[CrossRef] [PubMed]

Loparo, J. J.

C. J. Fecko, J. D. Eaves, J. J. Loparo, A. Tokmakoff, and P. L. Geissler, Science 301, 1698 (2003).
[CrossRef] [PubMed]

Mu, Y.

S. Woutersen, Y. Mu, G. Stock, and P. Hamm, Chem. Phys. 266, 137 (2001).
[CrossRef]

Mukamel, S.

Y. Tanimura and S. Mukamel, Phys. Rev. E 47, 118 (1993).
[CrossRef]

S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford U. Press, 1995), pp. 209-233.

Okumura, K.

K. Okumura, A. Tokmakoff, and Y. Tanimura, Chem. Phys. Lett. 314, 488 (1999).
[CrossRef]

Piletic, I. R.

J. Zheng, K. Kwak, J. Asbury, X. Chen, I. R. Piletic, and M. D. Fayer, Science 309, 1338 (2005).
[CrossRef] [PubMed]

Pshenichnikov, M. S.

S. Yeremenko, M. S. Pshenichnikov, and D. A. Wiersma, Phys. Rev. A 73, 21804 (2006).
[CrossRef]

W. P. de Boeij, M. S. Pshenichnikov, and D. A. Wiersma, J. Phys. Chem. 100, 11806 (1996).
[CrossRef]

Shank, C. V.

C. J. Bardeen and C. V. Shank, Chem. Phys. Lett. 203, 535 (1993).
[CrossRef]

Stenger, J.

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, Nature 434, 625 (2005).
[CrossRef] [PubMed]

Stock, G.

S. Woutersen, Y. Mu, G. Stock, and P. Hamm, Chem. Phys. 266, 137 (2001).
[CrossRef]

Tanimura, Y.

K. Okumura, A. Tokmakoff, and Y. Tanimura, Chem. Phys. Lett. 314, 488 (1999).
[CrossRef]

Y. Tanimura and S. Mukamel, Phys. Rev. E 47, 118 (1993).
[CrossRef]

Tokmakoff, A.

C. J. Fecko, J. D. Eaves, J. J. Loparo, A. Tokmakoff, and P. L. Geissler, Science 301, 1698 (2003).
[CrossRef] [PubMed]

K. Okumura, A. Tokmakoff, and Y. Tanimura, Chem. Phys. Lett. 314, 488 (1999).
[CrossRef]

Vaswani, H. M.

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, Nature 434, 625 (2005).
[CrossRef] [PubMed]

Weiner, A. M.

Wiersma, D. A.

S. Yeremenko, M. S. Pshenichnikov, and D. A. Wiersma, Phys. Rev. A 73, 21804 (2006).
[CrossRef]

W. P. de Boeij, M. S. Pshenichnikov, and D. A. Wiersma, J. Phys. Chem. 100, 11806 (1996).
[CrossRef]

Woutersen, S.

S. Woutersen, Y. Mu, G. Stock, and P. Hamm, Chem. Phys. 266, 137 (2001).
[CrossRef]

Yeremenko, S.

S. Yeremenko, M. S. Pshenichnikov, and D. A. Wiersma, Phys. Rev. A 73, 21804 (2006).
[CrossRef]

Zheng, J.

J. Zheng, K. Kwak, J. Asbury, X. Chen, I. R. Piletic, and M. D. Fayer, Science 309, 1338 (2005).
[CrossRef] [PubMed]

Annu. Rev. Phys. Chem. (1)

D. M. Jonas, Annu. Rev. Phys. Chem. 54, 425 (2003).
[CrossRef] [PubMed]

Chem. Phys. (1)

S. Woutersen, Y. Mu, G. Stock, and P. Hamm, Chem. Phys. 266, 137 (2001).
[CrossRef]

Chem. Phys. Lett. (2)

C. J. Bardeen and C. V. Shank, Chem. Phys. Lett. 203, 535 (1993).
[CrossRef]

K. Okumura, A. Tokmakoff, and Y. Tanimura, Chem. Phys. Lett. 314, 488 (1999).
[CrossRef]

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

J. Phys. Chem. (2)

W. P. de Boeij, M. S. Pshenichnikov, and D. A. Wiersma, J. Phys. Chem. 100, 11806 (1996).
[CrossRef]

K. Kwac and M. H. Cho, J. Phys. Chem. 119, 2256 (2003).
[CrossRef]

Nature (1)

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, Nature 434, 625 (2005).
[CrossRef] [PubMed]

Phys. Rev. A (1)

S. Yeremenko, M. S. Pshenichnikov, and D. A. Wiersma, Phys. Rev. A 73, 21804 (2006).
[CrossRef]

Phys. Rev. B (1)

M. Aihara, Phys. Rev. B 25, 53 (1982).
[CrossRef]

Phys. Rev. E (1)

Y. Tanimura and S. Mukamel, Phys. Rev. E 47, 118 (1993).
[CrossRef]

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

P. Hamm, M. Lim, W. F. DeGrado, and R. M. Hochstrasser, Proc. Natl. Acad. Sci. U.S.A. 96, 2036 (1999).
[CrossRef] [PubMed]

Science (2)

J. Zheng, K. Kwak, J. Asbury, X. Chen, I. R. Piletic, and M. D. Fayer, Science 309, 1338 (2005).
[CrossRef] [PubMed]

C. J. Fecko, J. D. Eaves, J. J. Loparo, A. Tokmakoff, and P. L. Geissler, Science 301, 1698 (2003).
[CrossRef] [PubMed]

Other (1)

S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford U. Press, 1995), pp. 209-233.

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Figures (4)

Fig. 1
Fig. 1

Schematics of the 2D experiment.

Fig. 2
Fig. 2

Retrieval of the CF from CS using Eq. (3), with no Stokes shift (solid circles), with Stokes shift (open symbols), for finite pulses before (squares) and after normalization (crosses).

Fig. 3
Fig. 3

Experimental (left) and calculated (right) 2D CS. Δ ω 1 ( 3 ) indicates the detuning from the transition frequency. Solid contours are drawn with the 10% increments of the maximum value.

Fig. 4
Fig. 4

The CF derived from full-scale simulations (solid line) and from the CS in Fig. 3 using Eq. (3) (symbols).

Equations (3)

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

g ( t 12 ( 34 ) + t 23 ) g ( t 23 ) + Δ 2 t 12 ( 34 ) 0 t 23 M ( t ) d t + Δ 2 2 t 12 ( 34 ) 2 M ( t 23 ) .
Re [ S ( ω 1 , t 23 , ω 3 ) ] exp { ω 1 2 + ω 3 2 2 M ( t 23 ) ω 1 ω 3 2 Δ 2 [ 1 M 2 ( t 23 ) ] } .
M ( t 23 ) = a 2 b 2 a 2 + b 2 .

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