Abstract

We report a compact, easy to align, and passively phase-stabilized setup for recording two-dimensional (2D) electronic spectra in three different phase-matching directions in the boxcar geometry. Passive phase stabilization is achieved by a diffractive optical element, the use of refractive optics for introducing pulse delays, and the use of common optics for all pulses. Representative 2D spectra correlating single- and double-quantum coherences in a molecular aggregate are presented.

© 2009 Optical Society of America

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  1. T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, Nature 434, 625 (2005).
    [CrossRef] [PubMed]
  2. T. Zhang, C. N. Borca, X. Li, and S. T. Cundiff, Opt. Express 13, 7432 (2005).
    [CrossRef] [PubMed]
  3. A. Nemeth, F. Milota, J. Sperling, D. Abramavicius, S. Mukamel, and H. F. Kauffmann, Chem. Phys. Lett. 469, 130 (2009).
    [CrossRef]
  4. K. Lazonder, M. S. Pshenichnikov, and D. A. Wiersma, Opt. Lett. 31, 3354 (2006).
    [CrossRef] [PubMed]
  5. A. Nemeth, F. Milota, T. Mančal, V. Lukeš, H. F. Kauffmann, and J. Sperling, Chem. Phys. Lett. 459, 49 (2008).
    [CrossRef]
  6. A. Nemeth, V. Lukeš, J. Sperling, F. Milota, H. F. Kauffmann, and T. Mančal, Phys. Chem. Chem. Phys. 11, 5986 (2009).
    [CrossRef] [PubMed]
  7. M. L. Cowan, J. P. Ogilvie, and R. J. D. Miller, Chem. Phys. Lett. 386, 184 (2004).
    [CrossRef]
  8. T. Brixner, I. V. Stiopkin, and G. R. Fleming, Opt. Lett. 29, 884 (2004).
    [CrossRef] [PubMed]
  9. K. Gundogdu, K. W. Stone, D. B. Turner, and K. A. Nelson, Chem. Phys. 341, 89 (2007).
    [CrossRef]
  10. E. M. Grumstrup, S.-H. Shim, M. A. Montgomery, N. H. Damrauer, and M. T. Zanni, Opt. Express 15, 16681 (2007).
    [CrossRef] [PubMed]
  11. K. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, Science 324, 1169 (2009).
    [CrossRef] [PubMed]
  12. A. D. Bristow, D. Karaiskaj, X. Dai, T. Zhang, C. Carlsson, K. R. Hagen, R. Jimenez, and S. T. Cundiff, arXiv:0905.0947.
  13. V. I. Prokhorenko, A. Halpin, and R. J. D. Miller, Opt. Express 17, 9764 (2009).
    [CrossRef] [PubMed]
  14. P. Baum, M. Breuer, E. Riedle, and G. Steinmeyer, Opt. Lett. 31, 2220 (2006).
    [CrossRef] [PubMed]
  15. P. Baum and E. Riedle, J. Opt. Soc. Am B 22, 1875 (2005).
    [CrossRef]
  16. M. J. Tauber, R. A. Mathies, X. Chen, and S. E. Bradforth, Rev. Sci. Instrum. 74, 4958 (2003).
    [CrossRef]
  17. M. Khalil, N. Demirdöven, and A. Tokmakoff, Phys. Rev. Lett. 90, 047401 (2003).
    [CrossRef] [PubMed]
  18. D. Abramavicius, D. V. Voronine, and S. Mukamel, Proc. Natl. Acad. Sci. USA 105, 8525 (2008).
    [CrossRef] [PubMed]
  19. I. Stiopkin, T. Brixner, M. Yang, and G. R. Fleming, J. Phys. Chem. B 110, 20032 (2006).
    [CrossRef] [PubMed]
  20. D. M. Jonas, Annu. Rev. Phys. Chem. 54, 425 (2003).
    [CrossRef] [PubMed]

2009 (4)

A. Nemeth, F. Milota, J. Sperling, D. Abramavicius, S. Mukamel, and H. F. Kauffmann, Chem. Phys. Lett. 469, 130 (2009).
[CrossRef]

A. Nemeth, V. Lukeš, J. Sperling, F. Milota, H. F. Kauffmann, and T. Mančal, Phys. Chem. Chem. Phys. 11, 5986 (2009).
[CrossRef] [PubMed]

K. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, Science 324, 1169 (2009).
[CrossRef] [PubMed]

V. I. Prokhorenko, A. Halpin, and R. J. D. Miller, Opt. Express 17, 9764 (2009).
[CrossRef] [PubMed]

2008 (2)

A. Nemeth, F. Milota, T. Mančal, V. Lukeš, H. F. Kauffmann, and J. Sperling, Chem. Phys. Lett. 459, 49 (2008).
[CrossRef]

D. Abramavicius, D. V. Voronine, and S. Mukamel, Proc. Natl. Acad. Sci. USA 105, 8525 (2008).
[CrossRef] [PubMed]

2007 (2)

2006 (3)

2005 (3)

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

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

P. Baum and E. Riedle, J. Opt. Soc. Am B 22, 1875 (2005).
[CrossRef]

2004 (2)

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

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

2003 (3)

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

M. J. Tauber, R. A. Mathies, X. Chen, and S. E. Bradforth, Rev. Sci. Instrum. 74, 4958 (2003).
[CrossRef]

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

Abramavicius, D.

A. Nemeth, F. Milota, J. Sperling, D. Abramavicius, S. Mukamel, and H. F. Kauffmann, Chem. Phys. Lett. 469, 130 (2009).
[CrossRef]

D. Abramavicius, D. V. Voronine, and S. Mukamel, Proc. Natl. Acad. Sci. USA 105, 8525 (2008).
[CrossRef] [PubMed]

Baum, P.

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.

Bradforth, S. E.

M. J. Tauber, R. A. Mathies, X. Chen, and S. E. Bradforth, Rev. Sci. Instrum. 74, 4958 (2003).
[CrossRef]

Breuer, M.

Bristow, A. D.

A. D. Bristow, D. Karaiskaj, X. Dai, T. Zhang, C. Carlsson, K. R. Hagen, R. Jimenez, and S. T. Cundiff, arXiv:0905.0947.

Brixner, T.

I. Stiopkin, T. Brixner, M. Yang, and G. R. Fleming, J. Phys. Chem. B 110, 20032 (2006).
[CrossRef] [PubMed]

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]

Carlsson, C.

A. D. Bristow, D. Karaiskaj, X. Dai, T. Zhang, C. Carlsson, K. R. Hagen, R. Jimenez, and S. T. Cundiff, arXiv:0905.0947.

Chen, X.

M. J. Tauber, R. A. Mathies, X. Chen, and S. E. Bradforth, Rev. Sci. Instrum. 74, 4958 (2003).
[CrossRef]

Cho, M.

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.

K. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, Science 324, 1169 (2009).
[CrossRef] [PubMed]

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

A. D. Bristow, D. Karaiskaj, X. Dai, T. Zhang, C. Carlsson, K. R. Hagen, R. Jimenez, and S. T. Cundiff, arXiv:0905.0947.

Dai, X.

A. D. Bristow, D. Karaiskaj, X. Dai, T. Zhang, C. Carlsson, K. R. Hagen, R. Jimenez, and S. T. Cundiff, arXiv:0905.0947.

Damrauer, N. H.

Demirdöven, N.

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

Fleming, G. R.

I. Stiopkin, T. Brixner, M. Yang, and G. R. Fleming, J. Phys. Chem. B 110, 20032 (2006).
[CrossRef] [PubMed]

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]

Grumstrup, E. M.

Gundogdu, K.

K. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, Science 324, 1169 (2009).
[CrossRef] [PubMed]

K. Gundogdu, K. W. Stone, D. B. Turner, and K. A. Nelson, Chem. Phys. 341, 89 (2007).
[CrossRef]

Hagen, K. R.

A. D. Bristow, D. Karaiskaj, X. Dai, T. Zhang, C. Carlsson, K. R. Hagen, R. Jimenez, and S. T. Cundiff, arXiv:0905.0947.

Halpin, A.

Jimenez, R.

A. D. Bristow, D. Karaiskaj, X. Dai, T. Zhang, C. Carlsson, K. R. Hagen, R. Jimenez, and S. T. Cundiff, arXiv:0905.0947.

Jonas, D. M.

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

Karaiskaj, D.

A. D. Bristow, D. Karaiskaj, X. Dai, T. Zhang, C. Carlsson, K. R. Hagen, R. Jimenez, and S. T. Cundiff, arXiv:0905.0947.

Kauffmann, H. F.

A. Nemeth, F. Milota, J. Sperling, D. Abramavicius, S. Mukamel, and H. F. Kauffmann, Chem. Phys. Lett. 469, 130 (2009).
[CrossRef]

A. Nemeth, V. Lukeš, J. Sperling, F. Milota, H. F. Kauffmann, and T. Mančal, Phys. Chem. Chem. Phys. 11, 5986 (2009).
[CrossRef] [PubMed]

A. Nemeth, F. Milota, T. Mančal, V. Lukeš, H. F. Kauffmann, and J. Sperling, Chem. Phys. Lett. 459, 49 (2008).
[CrossRef]

Khalil, M.

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

Lazonder, K.

Li, X.

K. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, Science 324, 1169 (2009).
[CrossRef] [PubMed]

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

Lukeš, V.

A. Nemeth, V. Lukeš, J. Sperling, F. Milota, H. F. Kauffmann, and T. Mančal, Phys. Chem. Chem. Phys. 11, 5986 (2009).
[CrossRef] [PubMed]

A. Nemeth, F. Milota, T. Mančal, V. Lukeš, H. F. Kauffmann, and J. Sperling, Chem. Phys. Lett. 459, 49 (2008).
[CrossRef]

Mancal, T.

A. Nemeth, V. Lukeš, J. Sperling, F. Milota, H. F. Kauffmann, and T. Mančal, Phys. Chem. Chem. Phys. 11, 5986 (2009).
[CrossRef] [PubMed]

A. Nemeth, F. Milota, T. Mančal, V. Lukeš, H. F. Kauffmann, and J. Sperling, Chem. Phys. Lett. 459, 49 (2008).
[CrossRef]

Mathies, R. A.

M. J. Tauber, R. A. Mathies, X. Chen, and S. E. Bradforth, Rev. Sci. Instrum. 74, 4958 (2003).
[CrossRef]

Miller, R. J. D.

V. I. Prokhorenko, A. Halpin, and R. J. D. Miller, Opt. Express 17, 9764 (2009).
[CrossRef] [PubMed]

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

Milota, F.

A. Nemeth, V. Lukeš, J. Sperling, F. Milota, H. F. Kauffmann, and T. Mančal, Phys. Chem. Chem. Phys. 11, 5986 (2009).
[CrossRef] [PubMed]

A. Nemeth, F. Milota, J. Sperling, D. Abramavicius, S. Mukamel, and H. F. Kauffmann, Chem. Phys. Lett. 469, 130 (2009).
[CrossRef]

A. Nemeth, F. Milota, T. Mančal, V. Lukeš, H. F. Kauffmann, and J. Sperling, Chem. Phys. Lett. 459, 49 (2008).
[CrossRef]

Montgomery, M. A.

Mukamel, S.

A. Nemeth, F. Milota, J. Sperling, D. Abramavicius, S. Mukamel, and H. F. Kauffmann, Chem. Phys. Lett. 469, 130 (2009).
[CrossRef]

D. Abramavicius, D. V. Voronine, and S. Mukamel, Proc. Natl. Acad. Sci. USA 105, 8525 (2008).
[CrossRef] [PubMed]

Nelson, K. A.

K. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, Science 324, 1169 (2009).
[CrossRef] [PubMed]

K. Gundogdu, K. W. Stone, D. B. Turner, and K. A. Nelson, Chem. Phys. 341, 89 (2007).
[CrossRef]

Nemeth, A.

A. Nemeth, F. Milota, J. Sperling, D. Abramavicius, S. Mukamel, and H. F. Kauffmann, Chem. Phys. Lett. 469, 130 (2009).
[CrossRef]

A. Nemeth, V. Lukeš, J. Sperling, F. Milota, H. F. Kauffmann, and T. Mančal, Phys. Chem. Chem. Phys. 11, 5986 (2009).
[CrossRef] [PubMed]

A. Nemeth, F. Milota, T. Mančal, V. Lukeš, H. F. Kauffmann, and J. Sperling, Chem. Phys. Lett. 459, 49 (2008).
[CrossRef]

Ogilvie, J. P.

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

Prokhorenko, V. I.

Pshenichnikov, M. S.

Riedle, E.

Shim, S. -H.

Sperling, J.

A. Nemeth, F. Milota, J. Sperling, D. Abramavicius, S. Mukamel, and H. F. Kauffmann, Chem. Phys. Lett. 469, 130 (2009).
[CrossRef]

A. Nemeth, V. Lukeš, J. Sperling, F. Milota, H. F. Kauffmann, and T. Mančal, Phys. Chem. Chem. Phys. 11, 5986 (2009).
[CrossRef] [PubMed]

A. Nemeth, F. Milota, T. Mančal, V. Lukeš, H. F. Kauffmann, and J. Sperling, Chem. Phys. Lett. 459, 49 (2008).
[CrossRef]

Steinmeyer, G.

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.

I. Stiopkin, T. Brixner, M. Yang, and G. R. Fleming, J. Phys. Chem. B 110, 20032 (2006).
[CrossRef] [PubMed]

Stiopkin, I. V.

Stone, K.

K. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, Science 324, 1169 (2009).
[CrossRef] [PubMed]

Stone, K. W.

K. Gundogdu, K. W. Stone, D. B. Turner, and K. A. Nelson, Chem. Phys. 341, 89 (2007).
[CrossRef]

Tauber, M. J.

M. J. Tauber, R. A. Mathies, X. Chen, and S. E. Bradforth, Rev. Sci. Instrum. 74, 4958 (2003).
[CrossRef]

Tokmakoff, A.

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

Turner, D. B.

K. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, Science 324, 1169 (2009).
[CrossRef] [PubMed]

K. Gundogdu, K. W. Stone, D. B. Turner, and K. A. Nelson, Chem. Phys. 341, 89 (2007).
[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]

Voronine, D. V.

D. Abramavicius, D. V. Voronine, and S. Mukamel, Proc. Natl. Acad. Sci. USA 105, 8525 (2008).
[CrossRef] [PubMed]

Wiersma, D. A.

Yang, M.

I. Stiopkin, T. Brixner, M. Yang, and G. R. Fleming, J. Phys. Chem. B 110, 20032 (2006).
[CrossRef] [PubMed]

Zanni, M. T.

Zhang, T.

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

A. D. Bristow, D. Karaiskaj, X. Dai, T. Zhang, C. Carlsson, K. R. Hagen, R. Jimenez, and S. T. Cundiff, arXiv:0905.0947.

Annu. Rev. Phys. Chem. (1)

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

Chem. Phys. (1)

K. Gundogdu, K. W. Stone, D. B. Turner, and K. A. Nelson, Chem. Phys. 341, 89 (2007).
[CrossRef]

Chem. Phys. Lett. (3)

A. Nemeth, F. Milota, J. Sperling, D. Abramavicius, S. Mukamel, and H. F. Kauffmann, Chem. Phys. Lett. 469, 130 (2009).
[CrossRef]

A. Nemeth, F. Milota, T. Mančal, V. Lukeš, H. F. Kauffmann, and J. Sperling, Chem. Phys. Lett. 459, 49 (2008).
[CrossRef]

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

J. Opt. Soc. Am B (1)

P. Baum and E. Riedle, J. Opt. Soc. Am B 22, 1875 (2005).
[CrossRef]

J. Phys. Chem. B (1)

I. Stiopkin, T. Brixner, M. Yang, and G. R. Fleming, J. Phys. Chem. B 110, 20032 (2006).
[CrossRef] [PubMed]

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 (3)

Opt. Lett. (3)

Phys. Chem. Chem. Phys. (1)

A. Nemeth, V. Lukeš, J. Sperling, F. Milota, H. F. Kauffmann, and T. Mančal, Phys. Chem. Chem. Phys. 11, 5986 (2009).
[CrossRef] [PubMed]

Phys. Rev. Lett. (1)

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

Proc. Natl. Acad. Sci. USA (1)

D. Abramavicius, D. V. Voronine, and S. Mukamel, Proc. Natl. Acad. Sci. USA 105, 8525 (2008).
[CrossRef] [PubMed]

Rev. Sci. Instrum. (1)

M. J. Tauber, R. A. Mathies, X. Chen, and S. E. Bradforth, Rev. Sci. Instrum. 74, 4958 (2003).
[CrossRef]

Science (1)

K. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, Science 324, 1169 (2009).
[CrossRef] [PubMed]

Other (1)

A. D. Bristow, D. Karaiskaj, X. Dai, T. Zhang, C. Carlsson, K. R. Hagen, R. Jimenez, and S. T. Cundiff, arXiv:0905.0947.

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Figures (3)

Fig. 1
Fig. 1

(a) Schematic of the passively phase-stabilized setup. The incoming beam is focused on the DOE, and the four outgoing beams (being arranged on the four corners of a square on edge) are parallelized by a spherical mirror (SM1). Three pairs of wedges (WP1–WP3) introduce variable delays in all excitation pulses. SM2 focuses the four beams onto the sample (S). (b) Left panel, short-time (20 min, which is the duration of a scan) phase stability with a value of λ / 90 . Right panel, long-time phase stability of the setup, which corresponds to λ / 40 . (c) Schematic representation of the 1Q and 2Q 2D-ES technique.

Fig. 2
Fig. 2

(a) Amplitude and temporal phase (black curve) of an excitation pulse. The black, dark gray, and light gray curves show the temporal phase at optical path delays of 0, + 500 , and −500 fs, respectively. (b) Linear absorption and pump-probe spectrum ( t = 0   fs ) of BIC. A level scheme indicating the electronic structure is shown in the inset.

Fig. 3
Fig. 3

(a) 1Q and (b) 2Q 2D electronic spectra in amplitude (top) and real part (bottom) representation. Red and blue colors in the real part spectra indicate positive and negative features, respectively. Contour lines are drawn on a linear scale, starting at 10% signal intensity.

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