Abstract

We present what we believe to be the first implementation of nonequilibrium two-dimensional IR spectroscopy (2DIR) combining electronic excitation within the Fourier transform (FT) approach. Nonequilibrium 2DIR spectra of Mn2(CO)10 and its photoproducts are obtained in two modalities: photoexcitation at 400nm, either before a 2DIR probe or during the waiting time of the FT 2DIR measurement. Extending FT 2DIR to nonequilibrium systems offers insight into complex condensed-phase reaction dynamics.

© 2008 Optical Society of America

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  1. P. Hamm, M. H. Lim, and R. M. Hochstrasser, J. Phys. Chem. B 102, 6123 (1998).
    [CrossRef]
  2. M. H. Cho, Chem. Rev. 108, 1331 (2008).
    [CrossRef] [PubMed]
  3. J. Bredenbeck, J. Helbing, C. Kolano, and P. Hamm, ChemPhysChem 8, 1747 (2007).
    [CrossRef] [PubMed]
  4. P. Hamm, J. Helbing, and J. Bredenbeck, Annu. Rev. Phys. Chem. 59, 291 (2008).
    [CrossRef]
  5. C. Kolano, J. Helbing, M. Kozinski, W. Sander, and P. Hamm, Nature 444, 469 (2006).
    [CrossRef] [PubMed]
  6. C. Kolano, J. Helbing, G. Bucher, W. Sander, and P. Hamm, J. Phys. Chem. B 111, 11297 (2007).
    [CrossRef] [PubMed]
  7. J. Bredenbeck, J. Helbing, and P. Hamm, J. Am. Chem. Soc. 126, 990 (2004).
    [CrossRef] [PubMed]
  8. H. S. Chung, Z. Ganim, K. C. Jones, and A. Tokmakoff, Proc. Natl. Acad. Sci. USA 104, 14237 (2007).
    [CrossRef] [PubMed]
  9. V. Cervetto, J. Helbing, J. Bredenbeck, and P. Hamm, J. Chem. Phys. 121, 5935 (2004).
    [CrossRef] [PubMed]
  10. K. J. Kubarych, M. Joffre, A. Moore, N. Belabas, and D. M. Jonas, Opt. Lett. 30, 1228 (2005).
    [CrossRef] [PubMed]
  11. M. J. Nee, R. McCanne, K. J. Kubarych, and M. Joffre, Opt. Lett. 32, 713 (2007).
    [CrossRef] [PubMed]
  12. M. Khalil, N. Demirdöven, and A. Tokmakoff, J. Phys. Chem. A 107, 5258 (2003).
    [CrossRef]
  13. M. J. Nee, C. R. Baiz, J. M. Anna, R. McCanne, and K. J. Kubarych, J. Chem. Phys. 129, 084503 (2008).
    [CrossRef] [PubMed]
  14. M. J. Tauber, R. A. Mathies, X. Y. Chen, and S. E. Bradforth, Rev. Sci. Instrum. 74, 4958 (2003).
    [CrossRef]
  15. D. A. Steinhurst, A. P. Baronavski, and J. C. Owrutsky, Chem. Phys. Lett. 361, 513 (2002).
    [CrossRef]

2008 (3)

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

P. Hamm, J. Helbing, and J. Bredenbeck, Annu. Rev. Phys. Chem. 59, 291 (2008).
[CrossRef]

M. J. Nee, C. R. Baiz, J. M. Anna, R. McCanne, and K. J. Kubarych, J. Chem. Phys. 129, 084503 (2008).
[CrossRef] [PubMed]

2007 (4)

M. J. Nee, R. McCanne, K. J. Kubarych, and M. Joffre, Opt. Lett. 32, 713 (2007).
[CrossRef] [PubMed]

J. Bredenbeck, J. Helbing, C. Kolano, and P. Hamm, ChemPhysChem 8, 1747 (2007).
[CrossRef] [PubMed]

C. Kolano, J. Helbing, G. Bucher, W. Sander, and P. Hamm, J. Phys. Chem. B 111, 11297 (2007).
[CrossRef] [PubMed]

H. S. Chung, Z. Ganim, K. C. Jones, and A. Tokmakoff, Proc. Natl. Acad. Sci. USA 104, 14237 (2007).
[CrossRef] [PubMed]

2006 (1)

C. Kolano, J. Helbing, M. Kozinski, W. Sander, and P. Hamm, Nature 444, 469 (2006).
[CrossRef] [PubMed]

2005 (1)

2004 (2)

V. Cervetto, J. Helbing, J. Bredenbeck, and P. Hamm, J. Chem. Phys. 121, 5935 (2004).
[CrossRef] [PubMed]

J. Bredenbeck, J. Helbing, and P. Hamm, J. Am. Chem. Soc. 126, 990 (2004).
[CrossRef] [PubMed]

2003 (2)

M. Khalil, N. Demirdöven, and A. Tokmakoff, J. Phys. Chem. A 107, 5258 (2003).
[CrossRef]

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

2002 (1)

D. A. Steinhurst, A. P. Baronavski, and J. C. Owrutsky, Chem. Phys. Lett. 361, 513 (2002).
[CrossRef]

1998 (1)

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

Anna, J. M.

M. J. Nee, C. R. Baiz, J. M. Anna, R. McCanne, and K. J. Kubarych, J. Chem. Phys. 129, 084503 (2008).
[CrossRef] [PubMed]

Baiz, C. R.

M. J. Nee, C. R. Baiz, J. M. Anna, R. McCanne, and K. J. Kubarych, J. Chem. Phys. 129, 084503 (2008).
[CrossRef] [PubMed]

Baronavski, A. P.

D. A. Steinhurst, A. P. Baronavski, and J. C. Owrutsky, Chem. Phys. Lett. 361, 513 (2002).
[CrossRef]

Belabas, N.

Bradforth, S. E.

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

Bredenbeck, J.

P. Hamm, J. Helbing, and J. Bredenbeck, Annu. Rev. Phys. Chem. 59, 291 (2008).
[CrossRef]

J. Bredenbeck, J. Helbing, C. Kolano, and P. Hamm, ChemPhysChem 8, 1747 (2007).
[CrossRef] [PubMed]

V. Cervetto, J. Helbing, J. Bredenbeck, and P. Hamm, J. Chem. Phys. 121, 5935 (2004).
[CrossRef] [PubMed]

J. Bredenbeck, J. Helbing, and P. Hamm, J. Am. Chem. Soc. 126, 990 (2004).
[CrossRef] [PubMed]

Bucher, G.

C. Kolano, J. Helbing, G. Bucher, W. Sander, and P. Hamm, J. Phys. Chem. B 111, 11297 (2007).
[CrossRef] [PubMed]

Cervetto, V.

V. Cervetto, J. Helbing, J. Bredenbeck, and P. Hamm, J. Chem. Phys. 121, 5935 (2004).
[CrossRef] [PubMed]

Chen, X. Y.

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

Cho, M. H.

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

Chung, H. S.

H. S. Chung, Z. Ganim, K. C. Jones, and A. Tokmakoff, Proc. Natl. Acad. Sci. USA 104, 14237 (2007).
[CrossRef] [PubMed]

Demirdöven, N.

M. Khalil, N. Demirdöven, and A. Tokmakoff, J. Phys. Chem. A 107, 5258 (2003).
[CrossRef]

Ganim, Z.

H. S. Chung, Z. Ganim, K. C. Jones, and A. Tokmakoff, Proc. Natl. Acad. Sci. USA 104, 14237 (2007).
[CrossRef] [PubMed]

Hamm, P.

P. Hamm, J. Helbing, and J. Bredenbeck, Annu. Rev. Phys. Chem. 59, 291 (2008).
[CrossRef]

C. Kolano, J. Helbing, G. Bucher, W. Sander, and P. Hamm, J. Phys. Chem. B 111, 11297 (2007).
[CrossRef] [PubMed]

J. Bredenbeck, J. Helbing, C. Kolano, and P. Hamm, ChemPhysChem 8, 1747 (2007).
[CrossRef] [PubMed]

C. Kolano, J. Helbing, M. Kozinski, W. Sander, and P. Hamm, Nature 444, 469 (2006).
[CrossRef] [PubMed]

V. Cervetto, J. Helbing, J. Bredenbeck, and P. Hamm, J. Chem. Phys. 121, 5935 (2004).
[CrossRef] [PubMed]

J. Bredenbeck, J. Helbing, and P. Hamm, J. Am. Chem. Soc. 126, 990 (2004).
[CrossRef] [PubMed]

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

Helbing, J.

P. Hamm, J. Helbing, and J. Bredenbeck, Annu. Rev. Phys. Chem. 59, 291 (2008).
[CrossRef]

C. Kolano, J. Helbing, G. Bucher, W. Sander, and P. Hamm, J. Phys. Chem. B 111, 11297 (2007).
[CrossRef] [PubMed]

J. Bredenbeck, J. Helbing, C. Kolano, and P. Hamm, ChemPhysChem 8, 1747 (2007).
[CrossRef] [PubMed]

C. Kolano, J. Helbing, M. Kozinski, W. Sander, and P. Hamm, Nature 444, 469 (2006).
[CrossRef] [PubMed]

V. Cervetto, J. Helbing, J. Bredenbeck, and P. Hamm, J. Chem. Phys. 121, 5935 (2004).
[CrossRef] [PubMed]

J. Bredenbeck, J. Helbing, and P. Hamm, J. Am. Chem. Soc. 126, 990 (2004).
[CrossRef] [PubMed]

Hochstrasser, R. M.

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

Joffre, M.

Jonas, D. M.

Jones, K. C.

H. S. Chung, Z. Ganim, K. C. Jones, and A. Tokmakoff, Proc. Natl. Acad. Sci. USA 104, 14237 (2007).
[CrossRef] [PubMed]

Khalil, M.

M. Khalil, N. Demirdöven, and A. Tokmakoff, J. Phys. Chem. A 107, 5258 (2003).
[CrossRef]

Kolano, C.

J. Bredenbeck, J. Helbing, C. Kolano, and P. Hamm, ChemPhysChem 8, 1747 (2007).
[CrossRef] [PubMed]

C. Kolano, J. Helbing, G. Bucher, W. Sander, and P. Hamm, J. Phys. Chem. B 111, 11297 (2007).
[CrossRef] [PubMed]

C. Kolano, J. Helbing, M. Kozinski, W. Sander, and P. Hamm, Nature 444, 469 (2006).
[CrossRef] [PubMed]

Kozinski, M.

C. Kolano, J. Helbing, M. Kozinski, W. Sander, and P. Hamm, Nature 444, 469 (2006).
[CrossRef] [PubMed]

Kubarych, K. J.

Lim, M. H.

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

Mathies, R. A.

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

McCanne, R.

M. J. Nee, C. R. Baiz, J. M. Anna, R. McCanne, and K. J. Kubarych, J. Chem. Phys. 129, 084503 (2008).
[CrossRef] [PubMed]

M. J. Nee, R. McCanne, K. J. Kubarych, and M. Joffre, Opt. Lett. 32, 713 (2007).
[CrossRef] [PubMed]

Moore, A.

Nee, M. J.

M. J. Nee, C. R. Baiz, J. M. Anna, R. McCanne, and K. J. Kubarych, J. Chem. Phys. 129, 084503 (2008).
[CrossRef] [PubMed]

M. J. Nee, R. McCanne, K. J. Kubarych, and M. Joffre, Opt. Lett. 32, 713 (2007).
[CrossRef] [PubMed]

Owrutsky, J. C.

D. A. Steinhurst, A. P. Baronavski, and J. C. Owrutsky, Chem. Phys. Lett. 361, 513 (2002).
[CrossRef]

Sander, W.

C. Kolano, J. Helbing, G. Bucher, W. Sander, and P. Hamm, J. Phys. Chem. B 111, 11297 (2007).
[CrossRef] [PubMed]

C. Kolano, J. Helbing, M. Kozinski, W. Sander, and P. Hamm, Nature 444, 469 (2006).
[CrossRef] [PubMed]

Steinhurst, D. A.

D. A. Steinhurst, A. P. Baronavski, and J. C. Owrutsky, Chem. Phys. Lett. 361, 513 (2002).
[CrossRef]

Tauber, M. J.

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

Tokmakoff, A.

H. S. Chung, Z. Ganim, K. C. Jones, and A. Tokmakoff, Proc. Natl. Acad. Sci. USA 104, 14237 (2007).
[CrossRef] [PubMed]

M. Khalil, N. Demirdöven, and A. Tokmakoff, J. Phys. Chem. A 107, 5258 (2003).
[CrossRef]

Annu. Rev. Phys. Chem. (1)

P. Hamm, J. Helbing, and J. Bredenbeck, Annu. Rev. Phys. Chem. 59, 291 (2008).
[CrossRef]

Chem. Phys. Lett. (1)

D. A. Steinhurst, A. P. Baronavski, and J. C. Owrutsky, Chem. Phys. Lett. 361, 513 (2002).
[CrossRef]

Chem. Rev. (1)

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

ChemPhysChem (1)

J. Bredenbeck, J. Helbing, C. Kolano, and P. Hamm, ChemPhysChem 8, 1747 (2007).
[CrossRef] [PubMed]

J. Am. Chem. Soc. (1)

J. Bredenbeck, J. Helbing, and P. Hamm, J. Am. Chem. Soc. 126, 990 (2004).
[CrossRef] [PubMed]

J. Chem. Phys. (2)

V. Cervetto, J. Helbing, J. Bredenbeck, and P. Hamm, J. Chem. Phys. 121, 5935 (2004).
[CrossRef] [PubMed]

M. J. Nee, C. R. Baiz, J. M. Anna, R. McCanne, and K. J. Kubarych, J. Chem. Phys. 129, 084503 (2008).
[CrossRef] [PubMed]

J. Phys. Chem. A (1)

M. Khalil, N. Demirdöven, and A. Tokmakoff, J. Phys. Chem. A 107, 5258 (2003).
[CrossRef]

J. Phys. Chem. B (2)

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

C. Kolano, J. Helbing, G. Bucher, W. Sander, and P. Hamm, J. Phys. Chem. B 111, 11297 (2007).
[CrossRef] [PubMed]

Nature (1)

C. Kolano, J. Helbing, M. Kozinski, W. Sander, and P. Hamm, Nature 444, 469 (2006).
[CrossRef] [PubMed]

Opt. Lett. (2)

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

H. S. Chung, Z. Ganim, K. C. Jones, and A. Tokmakoff, Proc. Natl. Acad. Sci. USA 104, 14237 (2007).
[CrossRef] [PubMed]

Rev. Sci. Instrum. (1)

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

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Figures (4)

Fig. 1
Fig. 1

Fourier-transform (a) 2DIR, (b) t-2DIR, and (c) TE-2DIR pulse sequences. Red pulses represent k 1 and k 2 , yellow represents k 3 , the radiated signal is shown in orange, and UV pulses are shown in blue.

Fig. 2
Fig. 2

Nonequilibrium 2DIR spectrometer. The IR and UV beams are color coded according to the pulse sequences in Fig. 1. The dotted beam represents the tracer used for alignment and one-dimensional transient absorption measurements.

Fig. 3
Fig. 3

Schematic representation of the 2D data analysis process with a 25% chopper duty time. The two sets of data (with and without UV pump) are collected simultaneously. After deinterlacing the two sets are interpolated to uniform time points and Fourier transformed separately; the final difference spectrum is computed in the frequency domain.

Fig. 4
Fig. 4

(a) Triggered-exchange 2DIR spectrum at τ TE = 1 ps , t 2 = 25 ps . (b) Transient 2DIR spectrum of Mn 2 ( CO ) 10 at τ = 25 ps , t 2 = 1 ps . Negative features [unboxed (blue online)] arise from the depletion of ground-state reactant molecules, while positive features [boxed (red online)] are due to nonequilibrium photoproducts. Contours smaller than 2% and larger than 30% of the maximum amplitude are omitted for clarity. The spectra are not corrected for the amplitude envelope of the mid-IR pulses.

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