Abstract

We introduce an inherently phase-stable setup for coherent two-dimensional femtosecond spectroscopy in noncollinear box geometry using only conventional beam splitters, mirrors, and delay stages. Avoiding diffractive optics, pulse shapers, and active phase-locking loops, our spectroscopy setup is simple, robust, and works for ultrabroad bandwidths in all spectral regimes (infrared, visible, and ultraviolet).

© 2008 Optical Society of America

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  1. S. Mukamel, Annu. Rev. Phys. Chem. 51, 691 (2000).
    [CrossRef] [PubMed]
  2. D. M. Jonas, Annu. Rev. Phys. Chem. 54, 425 (2003).
    [CrossRef] [PubMed]
  3. M. Cho, Chem. Rev. 108, 1331 (2008).
    [CrossRef] [PubMed]
  4. J. D. Hybl, A. W. Albrecht, S. M. G. Faeder, and D. M. Jonas, Chem. Phys. Lett. 297, 307 (1998).
    [CrossRef]
  5. P. Hamm, M. H. Lim, and R. M. Hochstrasser, J. Phys. Chem. B 102, 6123 (1998).
    [CrossRef]
  6. S. Woutersen and P. Hamm, J. Phys. Chem. B 104, 11316 (2000).
    [CrossRef]
  7. O. Golonzka, M. Khalil, N. Demirdöven, and A. Tokmakoff, Phys. Rev. Lett. 86, 2154 (2001).
    [CrossRef] [PubMed]
  8. T. Brixner, I. V. Stiopkin, and G. R. Fleming, Opt. Lett. 29, 884 (2004).
    [CrossRef] [PubMed]
  9. T. Brixner, T. Mančal, I. V. Stiopkin, and G. R. Fleming, J. Chem. Phys. 121, 4221 (2004).
    [CrossRef] [PubMed]
  10. M. L. Cowan, J. P. Ogilvie, and R. J. D. Miller, Chem. Phys. Lett. 386, 184 (2004).
    [CrossRef]
  11. T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, Nature 434, 625 (2005).
    [CrossRef] [PubMed]
  12. X. Li, T. Zhang, C. N. Borca, and S. T. Cundiff, Phys. Rev. Lett. 96, 057406 (2006).
    [CrossRef] [PubMed]
  13. A. A. Maznev, K. A. Nelson, and J. A. Rogers, Opt. Lett. 23, 1319 (1998).
    [CrossRef]
  14. G. D. Goodno, G. Dadusc, and R. J. D. Miller, J. Opt. Soc. Am. B 15, 1791 (1998).
    [CrossRef]
  15. P. Tian, D. Keusters, Y. Suzaki, and W. S. Warren, Science 300, 1553 (2003).
    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
  17. T. Hornung, J. C. Vaughan, T. Feurer, and K. A. Nelson, Opt. Lett. 29, 2052 (2004).
    [CrossRef] [PubMed]
  18. T. Zhang, C. N. Borca, X. Li, and S. T. Cundiff, Opt. Express 13, 7432 (2005).
    [CrossRef] [PubMed]
  19. V. Volkov, R. Schanz, and P. Hamm, Opt. Lett. 30, 2010 (2005).
    [CrossRef] [PubMed]
  20. P. Tekavec, G. A. Lott, and A. H. Marcus, J. Chem. Phys. 127, 214307 (2007).
    [CrossRef] [PubMed]
  21. U. Selig, F. Langhojer, F. Dimler, and T. Brixner, “Vorrichtung und Verfahren zur kohärenten zwei-dimensionalen optischen Spektroskopie,” patent pending 10 2008 025 170.4, German Patent and Trade Mark Office, 80297 Munich, Germany (2008).

2008 (2)

M. Cho, Chem. Rev. 108, 1331 (2008).
[CrossRef] [PubMed]

U. Selig, F. Langhojer, F. Dimler, and T. Brixner, “Vorrichtung und Verfahren zur kohärenten zwei-dimensionalen optischen Spektroskopie,” patent pending 10 2008 025 170.4, German Patent and Trade Mark Office, 80297 Munich, Germany (2008).

2007 (2)

2006 (1)

X. Li, T. Zhang, C. N. Borca, and S. T. Cundiff, Phys. Rev. Lett. 96, 057406 (2006).
[CrossRef] [PubMed]

2005 (3)

2004 (4)

T. Brixner, I. V. Stiopkin, and G. R. Fleming, Opt. Lett. 29, 884 (2004).
[CrossRef] [PubMed]

T. Hornung, J. C. Vaughan, T. Feurer, and K. A. Nelson, Opt. Lett. 29, 2052 (2004).
[CrossRef] [PubMed]

T. Brixner, T. Mančal, I. V. Stiopkin, and G. R. Fleming, J. Chem. Phys. 121, 4221 (2004).
[CrossRef] [PubMed]

M. L. Cowan, J. P. Ogilvie, and R. J. D. Miller, Chem. Phys. Lett. 386, 184 (2004).
[CrossRef]

2003 (2)

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

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

2001 (1)

O. Golonzka, M. Khalil, N. Demirdöven, and A. Tokmakoff, Phys. Rev. Lett. 86, 2154 (2001).
[CrossRef] [PubMed]

2000 (2)

S. Woutersen and P. Hamm, J. Phys. Chem. B 104, 11316 (2000).
[CrossRef]

S. Mukamel, Annu. Rev. Phys. Chem. 51, 691 (2000).
[CrossRef] [PubMed]

1998 (4)

J. D. Hybl, A. W. Albrecht, S. M. G. Faeder, and D. M. Jonas, Chem. Phys. Lett. 297, 307 (1998).
[CrossRef]

P. Hamm, M. H. Lim, and R. M. Hochstrasser, J. Phys. Chem. B 102, 6123 (1998).
[CrossRef]

G. D. Goodno, G. Dadusc, and R. J. D. Miller, J. Opt. Soc. Am. B 15, 1791 (1998).
[CrossRef]

A. A. Maznev, K. A. Nelson, and J. A. Rogers, Opt. Lett. 23, 1319 (1998).
[CrossRef]

Albrecht, A. W.

J. D. Hybl, A. W. Albrecht, S. M. G. Faeder, and D. M. Jonas, Chem. Phys. Lett. 297, 307 (1998).
[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]

Borca, C. N.

X. Li, T. Zhang, C. N. Borca, and S. T. Cundiff, Phys. Rev. Lett. 96, 057406 (2006).
[CrossRef] [PubMed]

T. Zhang, C. N. Borca, X. Li, and S. T. Cundiff, Opt. Express 13, 7432 (2005).
[CrossRef] [PubMed]

Brixner, T.

U. Selig, F. Langhojer, F. Dimler, and T. Brixner, “Vorrichtung und Verfahren zur kohärenten zwei-dimensionalen optischen Spektroskopie,” patent pending 10 2008 025 170.4, German Patent and Trade Mark Office, 80297 Munich, Germany (2008).

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

T. Brixner, I. V. Stiopkin, and G. R. Fleming, Opt. Lett. 29, 884 (2004).
[CrossRef] [PubMed]

T. Brixner, T. Mančal, I. V. Stiopkin, and G. R. Fleming, J. Chem. Phys. 121, 4221 (2004).
[CrossRef] [PubMed]

Cho, M.

M. Cho, Chem. Rev. 108, 1331 (2008).
[CrossRef] [PubMed]

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

Cowan, M. L.

M. L. Cowan, J. P. Ogilvie, and R. J. D. Miller, Chem. Phys. Lett. 386, 184 (2004).
[CrossRef]

Cundiff, S. T.

X. Li, T. Zhang, C. N. Borca, and S. T. Cundiff, Phys. Rev. Lett. 96, 057406 (2006).
[CrossRef] [PubMed]

T. Zhang, C. N. Borca, X. Li, and S. T. Cundiff, Opt. Express 13, 7432 (2005).
[CrossRef] [PubMed]

Dadusc, G.

Damrauer, N. H.

Demirdöven, N.

O. Golonzka, M. Khalil, N. Demirdöven, and A. Tokmakoff, Phys. Rev. Lett. 86, 2154 (2001).
[CrossRef] [PubMed]

Dimler, F.

U. Selig, F. Langhojer, F. Dimler, and T. Brixner, “Vorrichtung und Verfahren zur kohärenten zwei-dimensionalen optischen Spektroskopie,” patent pending 10 2008 025 170.4, German Patent and Trade Mark Office, 80297 Munich, Germany (2008).

Faeder, S. M. G.

J. D. Hybl, A. W. Albrecht, S. M. G. Faeder, and D. M. Jonas, Chem. Phys. Lett. 297, 307 (1998).
[CrossRef]

Feurer, T.

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]

T. Brixner, I. V. Stiopkin, and G. R. Fleming, Opt. Lett. 29, 884 (2004).
[CrossRef] [PubMed]

T. Brixner, T. Mančal, I. V. Stiopkin, and G. R. Fleming, J. Chem. Phys. 121, 4221 (2004).
[CrossRef] [PubMed]

Golonzka, O.

O. Golonzka, M. Khalil, N. Demirdöven, and A. Tokmakoff, Phys. Rev. Lett. 86, 2154 (2001).
[CrossRef] [PubMed]

Goodno, G. D.

Grumstrup, E. M.

Hamm, P.

V. Volkov, R. Schanz, and P. Hamm, Opt. Lett. 30, 2010 (2005).
[CrossRef] [PubMed]

S. Woutersen and P. Hamm, J. Phys. Chem. B 104, 11316 (2000).
[CrossRef]

P. Hamm, M. H. Lim, and R. M. Hochstrasser, J. Phys. Chem. B 102, 6123 (1998).
[CrossRef]

Hochstrasser, R. M.

P. Hamm, M. H. Lim, and R. M. Hochstrasser, J. Phys. Chem. B 102, 6123 (1998).
[CrossRef]

Hornung, T.

Hybl, J. D.

J. D. Hybl, A. W. Albrecht, S. M. G. Faeder, and D. M. Jonas, Chem. Phys. Lett. 297, 307 (1998).
[CrossRef]

Jonas, D. M.

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

J. D. Hybl, A. W. Albrecht, S. M. G. Faeder, and D. M. Jonas, Chem. Phys. Lett. 297, 307 (1998).
[CrossRef]

Keusters, D.

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

Khalil, M.

O. Golonzka, M. Khalil, N. Demirdöven, and A. Tokmakoff, Phys. Rev. Lett. 86, 2154 (2001).
[CrossRef] [PubMed]

Langhojer, F.

U. Selig, F. Langhojer, F. Dimler, and T. Brixner, “Vorrichtung und Verfahren zur kohärenten zwei-dimensionalen optischen Spektroskopie,” patent pending 10 2008 025 170.4, German Patent and Trade Mark Office, 80297 Munich, Germany (2008).

Li, X.

X. Li, T. Zhang, C. N. Borca, and S. T. Cundiff, Phys. Rev. Lett. 96, 057406 (2006).
[CrossRef] [PubMed]

T. Zhang, C. N. Borca, X. Li, and S. T. Cundiff, Opt. Express 13, 7432 (2005).
[CrossRef] [PubMed]

Lim, M. H.

P. Hamm, M. H. Lim, and R. M. Hochstrasser, J. Phys. Chem. B 102, 6123 (1998).
[CrossRef]

Lott, G. A.

P. Tekavec, G. A. Lott, and A. H. Marcus, J. Chem. Phys. 127, 214307 (2007).
[CrossRef] [PubMed]

Mancal, T.

T. Brixner, T. Mančal, I. V. Stiopkin, and G. R. Fleming, J. Chem. Phys. 121, 4221 (2004).
[CrossRef] [PubMed]

Marcus, A. H.

P. Tekavec, G. A. Lott, and A. H. Marcus, J. Chem. Phys. 127, 214307 (2007).
[CrossRef] [PubMed]

Maznev, A. A.

Miller, R. J. D.

M. L. Cowan, J. P. Ogilvie, and R. J. D. Miller, Chem. Phys. Lett. 386, 184 (2004).
[CrossRef]

G. D. Goodno, G. Dadusc, and R. J. D. Miller, J. Opt. Soc. Am. B 15, 1791 (1998).
[CrossRef]

Montgomery, M. A.

Mukamel, S.

S. Mukamel, Annu. Rev. Phys. Chem. 51, 691 (2000).
[CrossRef] [PubMed]

Nelson, K. A.

Ogilvie, J. P.

M. L. Cowan, J. P. Ogilvie, and R. J. D. Miller, Chem. Phys. Lett. 386, 184 (2004).
[CrossRef]

Rogers, J. A.

Schanz, R.

Selig, U.

U. Selig, F. Langhojer, F. Dimler, and T. Brixner, “Vorrichtung und Verfahren zur kohärenten zwei-dimensionalen optischen Spektroskopie,” patent pending 10 2008 025 170.4, German Patent and Trade Mark Office, 80297 Munich, Germany (2008).

Shim, S.-H.

Stenger, J.

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

Stiopkin, I. V.

T. Brixner, I. V. Stiopkin, and G. R. Fleming, Opt. Lett. 29, 884 (2004).
[CrossRef] [PubMed]

T. Brixner, T. Mančal, I. V. Stiopkin, and G. R. Fleming, J. Chem. Phys. 121, 4221 (2004).
[CrossRef] [PubMed]

Suzaki, Y.

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

Tekavec, P.

P. Tekavec, G. A. Lott, and A. H. Marcus, J. Chem. Phys. 127, 214307 (2007).
[CrossRef] [PubMed]

Tian, P.

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

Tokmakoff, A.

O. Golonzka, M. Khalil, N. Demirdöven, and A. Tokmakoff, Phys. Rev. Lett. 86, 2154 (2001).
[CrossRef] [PubMed]

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]

Vaughan, J. C.

Volkov, V.

Warren, W. S.

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

Woutersen, S.

S. Woutersen and P. Hamm, J. Phys. Chem. B 104, 11316 (2000).
[CrossRef]

Zanni, M. T.

Zhang, T.

X. Li, T. Zhang, C. N. Borca, and S. T. Cundiff, Phys. Rev. Lett. 96, 057406 (2006).
[CrossRef] [PubMed]

T. Zhang, C. N. Borca, X. Li, and S. T. Cundiff, Opt. Express 13, 7432 (2005).
[CrossRef] [PubMed]

Annu. Rev. Phys. Chem. (2)

S. Mukamel, Annu. Rev. Phys. Chem. 51, 691 (2000).
[CrossRef] [PubMed]

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

Chem. Phys. Lett. (2)

J. D. Hybl, A. W. Albrecht, S. M. G. Faeder, and D. M. Jonas, Chem. Phys. Lett. 297, 307 (1998).
[CrossRef]

M. L. Cowan, J. P. Ogilvie, and R. J. D. Miller, Chem. Phys. Lett. 386, 184 (2004).
[CrossRef]

Chem. Rev. (1)

M. Cho, Chem. Rev. 108, 1331 (2008).
[CrossRef] [PubMed]

J. Chem. Phys. (2)

P. Tekavec, G. A. Lott, and A. H. Marcus, J. Chem. Phys. 127, 214307 (2007).
[CrossRef] [PubMed]

T. Brixner, T. Mančal, I. V. Stiopkin, and G. R. Fleming, J. Chem. Phys. 121, 4221 (2004).
[CrossRef] [PubMed]

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

J. Phys. Chem. B (2)

P. Hamm, M. H. Lim, and R. M. Hochstrasser, J. Phys. Chem. B 102, 6123 (1998).
[CrossRef]

S. Woutersen and P. Hamm, J. Phys. Chem. B 104, 11316 (2000).
[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]

Opt. Express (2)

Opt. Lett. (4)

Phys. Rev. Lett. (2)

X. Li, T. Zhang, C. N. Borca, and S. T. Cundiff, Phys. Rev. Lett. 96, 057406 (2006).
[CrossRef] [PubMed]

O. Golonzka, M. Khalil, N. Demirdöven, and A. Tokmakoff, Phys. Rev. Lett. 86, 2154 (2001).
[CrossRef] [PubMed]

Science (1)

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

Other (1)

U. Selig, F. Langhojer, F. Dimler, and T. Brixner, “Vorrichtung und Verfahren zur kohärenten zwei-dimensionalen optischen Spektroskopie,” patent pending 10 2008 025 170.4, German Patent and Trade Mark Office, 80297 Munich, Germany (2008).

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Figures (3)

Fig. 1
Fig. 1

Experimental setup. The inset shows a side view at the first beam splitter; BS1/M1 creates two vertically displaced parallel beams. The lower one (solid line) travels below DS1 before reaching BS2 where it is split into beams 1 and 2; the upper beam (dashed line) is delayed along DS1 before reaching BS2 where it is split into 3 and 4. See text for further explanation.

Fig. 2
Fig. 2

Phase stability and reproducibility. (a) The phase deviation of the third-order signal from Nile Blue in acetonitrile versus the local oscillator is shown for T = τ = 0 fs with respect to the phase at the beginning of the measurement. (b) The heterodyne component of the spectral interference pattern (after scattering correction) is shown for a τ scan recorded at T = 0 . (c) Interference spectra are shown for T = τ = 0 fs from three separate τ scans; the second (middle) and the third one (bottom) were recorded 38 and 117 min after the first one (top).

Fig. 3
Fig. 3

2D spectrum of Nile Blue in acetonitrile showing (a) absolute magnitude and (b) phase for T = 0 fs . Contour lines are drawn in steps of 10% for the absolute magnitude and in steps of π 6 for the phase.

Equations (1)

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ω 0 ( Δ t 1 + Δ t 2 + Δ t 3 Δ t 4 ) = 0 ,

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