Abstract

We present a polarization method that significantly improves the signal-to-noise ratio in two-dimensional (2D) spectra collected in a “pump–probe” phase-matching geometry by improving the signal strength and eliminating unwanted background signals. This beam geometry is particularly useful when collecting 2D spectra using a pulse shaper.

© 2008 Optical Society of America

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  1. S. Mukamel and R. M. Hochstrasser, eds., special issue, Chem. Phys. 266, 135 (2001).
    [CrossRef]
  2. R. M. Hochstrasser, ed., special issue, Proc. Natl. Acad. Sci. U.S.A. 104, 14189 (2007).
    [CrossRef] [PubMed]
  3. S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford U. Press, 1995).
  4. F. Ding, P. Mukherjee, and M. T. Zanni, Opt. Lett. 31, 2918 (2006).
    [CrossRef] [PubMed]
  5. M. Khalil, N. Demirdoven, and A. Tokmakoff, Phys. Rev. Lett. 90, 047401 (2003).
    [CrossRef] [PubMed]
  6. S. H. Shim, D. B. Strasfeld, Y. L. Ling, and M. T. Zanni, Proc. Natl. Acad. Sci. U.S.A. 104, 14197 (2007).
    [CrossRef] [PubMed]
  7. E. M. Grumstrup, S. H. Shim, M. A. Montgomery, N. H. Damrauer, and M. T. Zanni, Opt. Express 15, 16681 (2007).
    [CrossRef] [PubMed]
  8. P. F. Tian, D. Keusters, Y. Suzaki, and W. S. Warren, Science 300, 1553 (2003).
    [CrossRef] [PubMed]
  9. J. C. Vaughan, T. Hornung, K. W. Stone, and K. A. Nelson, J. Phys. Chem. A 111, 4873 (2007).
    [CrossRef] [PubMed]
  10. L. P. DeFlores, R. A. Nicodemus, and A. Tokmakoff, Opt. Lett. 32, 2966 (2007).
    [CrossRef] [PubMed]
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    [CrossRef]
  12. R. M. Hochstrasser, Chem. Phys. 266, 273 (2001).
    [CrossRef]
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    [CrossRef] [PubMed]
  14. M. Lim and R. M. Hochstrasser, J. Chem. Phys. 115, 7629 (2001).
    [CrossRef]
  15. O. Golonzka, M. Khalil, N. Demirdoven, and A. Tokmakoff, J. Chem. Phys. 115, 10814 (2001).
    [CrossRef]
  16. M. T. Zanni, S. Gnanakaran, J. Stenger, and R. M. Hochstrasser, J. Phys. Chem. B 105, 6520 (2001).
    [CrossRef]
  17. M. Ninck, A. Galler, T. Feurer, and T. Brixner, Opt. Lett. 32, 3379 (2007).
    [CrossRef] [PubMed]
  18. O. Masihzadeh, P. Schlup, and R. A. Bartels, Opt. Express 15, 18025 (2007).
    [CrossRef] [PubMed]

2007

2006

F. Ding, P. Mukherjee, and M. T. Zanni, Opt. Lett. 31, 2918 (2006).
[CrossRef] [PubMed]

W. Zhuang, D. Abramavicius, and S. Mukamel, Proc. Natl. Acad. Sci. U.S.A. 103, 18934 (2006).
[CrossRef] [PubMed]

2003

M. Khalil, N. Demirdoven, and A. Tokmakoff, Phys. Rev. Lett. 90, 047401 (2003).
[CrossRef] [PubMed]

P. F. Tian, D. Keusters, Y. Suzaki, and W. S. Warren, Science 300, 1553 (2003).
[CrossRef] [PubMed]

2001

R. M. Hochstrasser, Chem. Phys. 266, 273 (2001).
[CrossRef]

M. Lim and R. M. Hochstrasser, J. Chem. Phys. 115, 7629 (2001).
[CrossRef]

O. Golonzka, M. Khalil, N. Demirdoven, and A. Tokmakoff, J. Chem. Phys. 115, 10814 (2001).
[CrossRef]

M. T. Zanni, S. Gnanakaran, J. Stenger, and R. M. Hochstrasser, J. Phys. Chem. B 105, 6520 (2001).
[CrossRef]

S. Mukamel and R. M. Hochstrasser, eds., special issue, Chem. Phys. 266, 135 (2001).
[CrossRef]

1999

S. M. G. Faeder and D. M. Jonas, J. Phys. Chem. A 103, 10489 (1999).
[CrossRef]

Abramavicius, D.

W. Zhuang, D. Abramavicius, and S. Mukamel, Proc. Natl. Acad. Sci. U.S.A. 103, 18934 (2006).
[CrossRef] [PubMed]

Bartels, R. A.

Brixner, T.

Damrauer, N. H.

DeFlores, L. P.

Demirdoven, N.

M. Khalil, N. Demirdoven, and A. Tokmakoff, Phys. Rev. Lett. 90, 047401 (2003).
[CrossRef] [PubMed]

O. Golonzka, M. Khalil, N. Demirdoven, and A. Tokmakoff, J. Chem. Phys. 115, 10814 (2001).
[CrossRef]

Ding, F.

Faeder, S. M. G.

S. M. G. Faeder and D. M. Jonas, J. Phys. Chem. A 103, 10489 (1999).
[CrossRef]

Feurer, T.

Galler, A.

Gnanakaran, S.

M. T. Zanni, S. Gnanakaran, J. Stenger, and R. M. Hochstrasser, J. Phys. Chem. B 105, 6520 (2001).
[CrossRef]

Golonzka, O.

O. Golonzka, M. Khalil, N. Demirdoven, and A. Tokmakoff, J. Chem. Phys. 115, 10814 (2001).
[CrossRef]

Grumstrup, E. M.

Hochstrasser, R. M.

R. M. Hochstrasser, ed., special issue, Proc. Natl. Acad. Sci. U.S.A. 104, 14189 (2007).
[CrossRef] [PubMed]

M. T. Zanni, S. Gnanakaran, J. Stenger, and R. M. Hochstrasser, J. Phys. Chem. B 105, 6520 (2001).
[CrossRef]

R. M. Hochstrasser, Chem. Phys. 266, 273 (2001).
[CrossRef]

S. Mukamel and R. M. Hochstrasser, eds., special issue, Chem. Phys. 266, 135 (2001).
[CrossRef]

M. Lim and R. M. Hochstrasser, J. Chem. Phys. 115, 7629 (2001).
[CrossRef]

Hornung, T.

J. C. Vaughan, T. Hornung, K. W. Stone, and K. A. Nelson, J. Phys. Chem. A 111, 4873 (2007).
[CrossRef] [PubMed]

Jonas, D. M.

S. M. G. Faeder and D. M. Jonas, J. Phys. Chem. A 103, 10489 (1999).
[CrossRef]

Keusters, D.

P. F. Tian, D. Keusters, Y. Suzaki, and W. S. Warren, Science 300, 1553 (2003).
[CrossRef] [PubMed]

Khalil, M.

M. Khalil, N. Demirdoven, and A. Tokmakoff, Phys. Rev. Lett. 90, 047401 (2003).
[CrossRef] [PubMed]

O. Golonzka, M. Khalil, N. Demirdoven, and A. Tokmakoff, J. Chem. Phys. 115, 10814 (2001).
[CrossRef]

Lim, M.

M. Lim and R. M. Hochstrasser, J. Chem. Phys. 115, 7629 (2001).
[CrossRef]

Ling, Y. L.

S. H. Shim, D. B. Strasfeld, Y. L. Ling, and M. T. Zanni, Proc. Natl. Acad. Sci. U.S.A. 104, 14197 (2007).
[CrossRef] [PubMed]

Masihzadeh, O.

Montgomery, M. A.

Mukamel, S.

W. Zhuang, D. Abramavicius, and S. Mukamel, Proc. Natl. Acad. Sci. U.S.A. 103, 18934 (2006).
[CrossRef] [PubMed]

S. Mukamel and R. M. Hochstrasser, eds., special issue, Chem. Phys. 266, 135 (2001).
[CrossRef]

S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford U. Press, 1995).

Mukherjee, P.

Nelson, K. A.

J. C. Vaughan, T. Hornung, K. W. Stone, and K. A. Nelson, J. Phys. Chem. A 111, 4873 (2007).
[CrossRef] [PubMed]

Nicodemus, R. A.

Ninck, M.

Schlup, P.

Shim, S. H.

E. M. Grumstrup, S. H. Shim, M. A. Montgomery, N. H. Damrauer, and M. T. Zanni, Opt. Express 15, 16681 (2007).
[CrossRef] [PubMed]

S. H. Shim, D. B. Strasfeld, Y. L. Ling, and M. T. Zanni, Proc. Natl. Acad. Sci. U.S.A. 104, 14197 (2007).
[CrossRef] [PubMed]

Stenger, J.

M. T. Zanni, S. Gnanakaran, J. Stenger, and R. M. Hochstrasser, J. Phys. Chem. B 105, 6520 (2001).
[CrossRef]

Stone, K. W.

J. C. Vaughan, T. Hornung, K. W. Stone, and K. A. Nelson, J. Phys. Chem. A 111, 4873 (2007).
[CrossRef] [PubMed]

Strasfeld, D. B.

S. H. Shim, D. B. Strasfeld, Y. L. Ling, and M. T. Zanni, Proc. Natl. Acad. Sci. U.S.A. 104, 14197 (2007).
[CrossRef] [PubMed]

Suzaki, Y.

P. F. Tian, D. Keusters, Y. Suzaki, and W. S. Warren, Science 300, 1553 (2003).
[CrossRef] [PubMed]

Tian, P. F.

P. F. Tian, D. Keusters, Y. Suzaki, and W. S. Warren, Science 300, 1553 (2003).
[CrossRef] [PubMed]

Tokmakoff, A.

L. P. DeFlores, R. A. Nicodemus, and A. Tokmakoff, Opt. Lett. 32, 2966 (2007).
[CrossRef] [PubMed]

M. Khalil, N. Demirdoven, and A. Tokmakoff, Phys. Rev. Lett. 90, 047401 (2003).
[CrossRef] [PubMed]

O. Golonzka, M. Khalil, N. Demirdoven, and A. Tokmakoff, J. Chem. Phys. 115, 10814 (2001).
[CrossRef]

Vaughan, J. C.

J. C. Vaughan, T. Hornung, K. W. Stone, and K. A. Nelson, J. Phys. Chem. A 111, 4873 (2007).
[CrossRef] [PubMed]

Warren, W. S.

P. F. Tian, D. Keusters, Y. Suzaki, and W. S. Warren, Science 300, 1553 (2003).
[CrossRef] [PubMed]

Zanni, M. T.

S. H. Shim, D. B. Strasfeld, Y. L. Ling, and M. T. Zanni, Proc. Natl. Acad. Sci. U.S.A. 104, 14197 (2007).
[CrossRef] [PubMed]

E. M. Grumstrup, S. H. Shim, M. A. Montgomery, N. H. Damrauer, and M. T. Zanni, Opt. Express 15, 16681 (2007).
[CrossRef] [PubMed]

F. Ding, P. Mukherjee, and M. T. Zanni, Opt. Lett. 31, 2918 (2006).
[CrossRef] [PubMed]

M. T. Zanni, S. Gnanakaran, J. Stenger, and R. M. Hochstrasser, J. Phys. Chem. B 105, 6520 (2001).
[CrossRef]

Zhuang, W.

W. Zhuang, D. Abramavicius, and S. Mukamel, Proc. Natl. Acad. Sci. U.S.A. 103, 18934 (2006).
[CrossRef] [PubMed]

Chem. Phys.

S. Mukamel and R. M. Hochstrasser, eds., special issue, Chem. Phys. 266, 135 (2001).
[CrossRef]

R. M. Hochstrasser, Chem. Phys. 266, 273 (2001).
[CrossRef]

J. Chem. Phys.

M. Lim and R. M. Hochstrasser, J. Chem. Phys. 115, 7629 (2001).
[CrossRef]

O. Golonzka, M. Khalil, N. Demirdoven, and A. Tokmakoff, J. Chem. Phys. 115, 10814 (2001).
[CrossRef]

J. Phys. Chem. A

J. C. Vaughan, T. Hornung, K. W. Stone, and K. A. Nelson, J. Phys. Chem. A 111, 4873 (2007).
[CrossRef] [PubMed]

S. M. G. Faeder and D. M. Jonas, J. Phys. Chem. A 103, 10489 (1999).
[CrossRef]

J. Phys. Chem. B

M. T. Zanni, S. Gnanakaran, J. Stenger, and R. M. Hochstrasser, J. Phys. Chem. B 105, 6520 (2001).
[CrossRef]

Opt. Express

Opt. Lett.

Phys. Rev. Lett.

M. Khalil, N. Demirdoven, and A. Tokmakoff, Phys. Rev. Lett. 90, 047401 (2003).
[CrossRef] [PubMed]

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

S. H. Shim, D. B. Strasfeld, Y. L. Ling, and M. T. Zanni, Proc. Natl. Acad. Sci. U.S.A. 104, 14197 (2007).
[CrossRef] [PubMed]

R. M. Hochstrasser, ed., special issue, Proc. Natl. Acad. Sci. U.S.A. 104, 14189 (2007).
[CrossRef] [PubMed]

W. Zhuang, D. Abramavicius, and S. Mukamel, Proc. Natl. Acad. Sci. U.S.A. 103, 18934 (2006).
[CrossRef] [PubMed]

Science

P. F. Tian, D. Keusters, Y. Suzaki, and W. S. Warren, Science 300, 1553 (2003).
[CrossRef] [PubMed]

Other

S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford U. Press, 1995).

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Figures (2)

Fig. 1
Fig. 1

Schematic of beam geometries used to collect 2D spectra with (a) boxcar and (b) pump–probe phase-matching conditions. In the boxcar configuration the three excitation pulses have unique wave vectors k n so that the signal is emitted in the unique direction k s = k 1 k 2 + k 3 and heterodyned by a separate pulse called a local oscillator k LO . In pump–probe geometry, the first and second pluses are collinear (e.g., k 1 = k 2 ) so that k s = k 3 , and k 3 also serves as the local oscillator. The polarizer (P) that is placed prior to the detector is also shown in (b).

Fig. 2
Fig. 2

Comparison of time- and frequency-domain data for the antisymmetric stretch of acetic acid measured with (a)–(c) 0 1 ° , 0 2 ° , 90 3 ° , 90 S ° and (d)–(f) 0 1 ° , 90 2 ° , 0 3 ° , 90 S ° ; (a) and (d) two-dimensional IR spectra in the frequency range near the asymmetric stretch; (b) and (e) time-domain data at ω probe = 1703 (solid) and 1716 (dashed) cm 1 ; inset, expanded view from 240 to 370 fs to better illustrate the signal oscillations; (c) and (f) corresponding frequency-domain data. Contour lines are shown at 2% intervals.

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