Abstract

We apply a Fourier filtering technique for the global removal of coherent contributions, like perturbed free-induction decay, and noise, to experimental pump–probe spectra. A further filtering scheme gains access to spectra otherwise only recordable by scanning the probe’s center frequency with adjustable spectral resolution. These methods cleanse pump–probe data and allow improved visualization and simpler analysis of the contained dynamics. We demonstrate these filters using visible pump/mid-infrared probe spectroscopy of ligand dissociation in carboxyhemoglobin.

© 2009 Optical Society of America

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  1. B. Fluegel, N. Peyghambarian, G. Olbright, M. Lindberg, S. W. Koch, M. Joffre, D. Hulin, A. Migus, and A. Antonetti, Phys. Rev. Lett. 59, 2588 (1987).
    [CrossRef] [PubMed]
  2. C. H. Brito Cruz, J. P. Gordon, P. C. Becker, R. L. Fork, and C. V. Shank, IEEE J. Quantum Electron. 24, 261 (1988).
    [CrossRef]
  3. M. Joffre, D. Hulin, A. Migus, A. Antonetti, C. Benoit à la Guillaume, N. Peyghambarian, M. Lindberg, and S. W. Koch, Opt. Lett. 13, 276 (1988).
    [CrossRef] [PubMed]
  4. P. Hamm, Chem. Phys. 200, 415 (1995).
    [CrossRef]
  5. K. Neumann, M.-K. Verhoefen, I. Weber, C. Glaubitz, and J. Wachtveitl, Biophys. J. 94, 4796 (2008).
    [CrossRef] [PubMed]
  6. C. Schumann, R. Groß, M. M. N. Wolf, R. Diller, N. Michael, and T. Lamparter, Biophys. J. 94, 3189 (2008).
    [CrossRef] [PubMed]
  7. D. Wolpert, M. Schade, and T. Brixner, J. Chem. Phys. 129, 094504 (2008).
    [CrossRef] [PubMed]
  8. M. Lorenc, M. Ziolek, R. Naskrecki, J. Karolczak, J. Kubicki, and A. Maciejewski, Appl. Phys. B 74, 19 (2002).
    [CrossRef]
  9. T. Polack, Opt. Express 14, 5823 (2006).
    [CrossRef] [PubMed]
  10. K. J. Kubarych, M. Joffre, A. Moore, N. Belabas, and D. M. Jonas, Opt. Lett. 30, 1228 (2005).
    [CrossRef] [PubMed]
  11. J. Treuffet, K. J. Kubarych, J.-C. Lambry, E. Pilet, J.-B. Masson, J.-L. Martin, M. H. Vos, M. Joffre, and A. Alexandrou, Proc. Natl. Acad. Sci. USA 104, 15705 (2007).
    [CrossRef] [PubMed]
  12. P. A. Anfinrud, C. Han, and R. M. Hochstrasser, Proc. Natl. Acad. Sci. USA 86, 8387 (1989).
    [CrossRef] [PubMed]
  13. I. J. Finkelstein, A. M. Massari, and M. D. Fayer, Biophys. J. 92, 3652 (2007).
    [CrossRef] [PubMed]
  14. S. Fechner, F. Dimler, T. Brixner, G. Gerber, and D. J. Tannor, Opt. Express 15, 15387 (2007).
    [CrossRef] [PubMed]
  15. M. D. Fayer, Annu. Rev. Phys. Chem. 52, 315 (2001).
    [CrossRef] [PubMed]

2008 (3)

K. Neumann, M.-K. Verhoefen, I. Weber, C. Glaubitz, and J. Wachtveitl, Biophys. J. 94, 4796 (2008).
[CrossRef] [PubMed]

C. Schumann, R. Groß, M. M. N. Wolf, R. Diller, N. Michael, and T. Lamparter, Biophys. J. 94, 3189 (2008).
[CrossRef] [PubMed]

D. Wolpert, M. Schade, and T. Brixner, J. Chem. Phys. 129, 094504 (2008).
[CrossRef] [PubMed]

2007 (3)

J. Treuffet, K. J. Kubarych, J.-C. Lambry, E. Pilet, J.-B. Masson, J.-L. Martin, M. H. Vos, M. Joffre, and A. Alexandrou, Proc. Natl. Acad. Sci. USA 104, 15705 (2007).
[CrossRef] [PubMed]

I. J. Finkelstein, A. M. Massari, and M. D. Fayer, Biophys. J. 92, 3652 (2007).
[CrossRef] [PubMed]

S. Fechner, F. Dimler, T. Brixner, G. Gerber, and D. J. Tannor, Opt. Express 15, 15387 (2007).
[CrossRef] [PubMed]

2006 (1)

2005 (1)

2002 (1)

M. Lorenc, M. Ziolek, R. Naskrecki, J. Karolczak, J. Kubicki, and A. Maciejewski, Appl. Phys. B 74, 19 (2002).
[CrossRef]

2001 (1)

M. D. Fayer, Annu. Rev. Phys. Chem. 52, 315 (2001).
[CrossRef] [PubMed]

1995 (1)

P. Hamm, Chem. Phys. 200, 415 (1995).
[CrossRef]

1989 (1)

P. A. Anfinrud, C. Han, and R. M. Hochstrasser, Proc. Natl. Acad. Sci. USA 86, 8387 (1989).
[CrossRef] [PubMed]

1988 (2)

C. H. Brito Cruz, J. P. Gordon, P. C. Becker, R. L. Fork, and C. V. Shank, IEEE J. Quantum Electron. 24, 261 (1988).
[CrossRef]

M. Joffre, D. Hulin, A. Migus, A. Antonetti, C. Benoit à la Guillaume, N. Peyghambarian, M. Lindberg, and S. W. Koch, Opt. Lett. 13, 276 (1988).
[CrossRef] [PubMed]

1987 (1)

B. Fluegel, N. Peyghambarian, G. Olbright, M. Lindberg, S. W. Koch, M. Joffre, D. Hulin, A. Migus, and A. Antonetti, Phys. Rev. Lett. 59, 2588 (1987).
[CrossRef] [PubMed]

Alexandrou, A.

J. Treuffet, K. J. Kubarych, J.-C. Lambry, E. Pilet, J.-B. Masson, J.-L. Martin, M. H. Vos, M. Joffre, and A. Alexandrou, Proc. Natl. Acad. Sci. USA 104, 15705 (2007).
[CrossRef] [PubMed]

Anfinrud, P. A.

P. A. Anfinrud, C. Han, and R. M. Hochstrasser, Proc. Natl. Acad. Sci. USA 86, 8387 (1989).
[CrossRef] [PubMed]

Antonetti, A.

M. Joffre, D. Hulin, A. Migus, A. Antonetti, C. Benoit à la Guillaume, N. Peyghambarian, M. Lindberg, and S. W. Koch, Opt. Lett. 13, 276 (1988).
[CrossRef] [PubMed]

B. Fluegel, N. Peyghambarian, G. Olbright, M. Lindberg, S. W. Koch, M. Joffre, D. Hulin, A. Migus, and A. Antonetti, Phys. Rev. Lett. 59, 2588 (1987).
[CrossRef] [PubMed]

Becker, P. C.

C. H. Brito Cruz, J. P. Gordon, P. C. Becker, R. L. Fork, and C. V. Shank, IEEE J. Quantum Electron. 24, 261 (1988).
[CrossRef]

Belabas, N.

Benoit à la Guillaume, C.

Brito Cruz, C. H.

C. H. Brito Cruz, J. P. Gordon, P. C. Becker, R. L. Fork, and C. V. Shank, IEEE J. Quantum Electron. 24, 261 (1988).
[CrossRef]

Brixner, T.

Diller, R.

C. Schumann, R. Groß, M. M. N. Wolf, R. Diller, N. Michael, and T. Lamparter, Biophys. J. 94, 3189 (2008).
[CrossRef] [PubMed]

Dimler, F.

Fayer, M. D.

I. J. Finkelstein, A. M. Massari, and M. D. Fayer, Biophys. J. 92, 3652 (2007).
[CrossRef] [PubMed]

M. D. Fayer, Annu. Rev. Phys. Chem. 52, 315 (2001).
[CrossRef] [PubMed]

Fechner, S.

Finkelstein, I. J.

I. J. Finkelstein, A. M. Massari, and M. D. Fayer, Biophys. J. 92, 3652 (2007).
[CrossRef] [PubMed]

Fluegel, B.

B. Fluegel, N. Peyghambarian, G. Olbright, M. Lindberg, S. W. Koch, M. Joffre, D. Hulin, A. Migus, and A. Antonetti, Phys. Rev. Lett. 59, 2588 (1987).
[CrossRef] [PubMed]

Fork, R. L.

C. H. Brito Cruz, J. P. Gordon, P. C. Becker, R. L. Fork, and C. V. Shank, IEEE J. Quantum Electron. 24, 261 (1988).
[CrossRef]

Gerber, G.

Glaubitz, C.

K. Neumann, M.-K. Verhoefen, I. Weber, C. Glaubitz, and J. Wachtveitl, Biophys. J. 94, 4796 (2008).
[CrossRef] [PubMed]

Gordon, J. P.

C. H. Brito Cruz, J. P. Gordon, P. C. Becker, R. L. Fork, and C. V. Shank, IEEE J. Quantum Electron. 24, 261 (1988).
[CrossRef]

Groß, R.

C. Schumann, R. Groß, M. M. N. Wolf, R. Diller, N. Michael, and T. Lamparter, Biophys. J. 94, 3189 (2008).
[CrossRef] [PubMed]

Hamm, P.

P. Hamm, Chem. Phys. 200, 415 (1995).
[CrossRef]

Han, C.

P. A. Anfinrud, C. Han, and R. M. Hochstrasser, Proc. Natl. Acad. Sci. USA 86, 8387 (1989).
[CrossRef] [PubMed]

Hochstrasser, R. M.

P. A. Anfinrud, C. Han, and R. M. Hochstrasser, Proc. Natl. Acad. Sci. USA 86, 8387 (1989).
[CrossRef] [PubMed]

Hulin, D.

M. Joffre, D. Hulin, A. Migus, A. Antonetti, C. Benoit à la Guillaume, N. Peyghambarian, M. Lindberg, and S. W. Koch, Opt. Lett. 13, 276 (1988).
[CrossRef] [PubMed]

B. Fluegel, N. Peyghambarian, G. Olbright, M. Lindberg, S. W. Koch, M. Joffre, D. Hulin, A. Migus, and A. Antonetti, Phys. Rev. Lett. 59, 2588 (1987).
[CrossRef] [PubMed]

Joffre, M.

J. Treuffet, K. J. Kubarych, J.-C. Lambry, E. Pilet, J.-B. Masson, J.-L. Martin, M. H. Vos, M. Joffre, and A. Alexandrou, Proc. Natl. Acad. Sci. USA 104, 15705 (2007).
[CrossRef] [PubMed]

K. J. Kubarych, M. Joffre, A. Moore, N. Belabas, and D. M. Jonas, Opt. Lett. 30, 1228 (2005).
[CrossRef] [PubMed]

M. Joffre, D. Hulin, A. Migus, A. Antonetti, C. Benoit à la Guillaume, N. Peyghambarian, M. Lindberg, and S. W. Koch, Opt. Lett. 13, 276 (1988).
[CrossRef] [PubMed]

B. Fluegel, N. Peyghambarian, G. Olbright, M. Lindberg, S. W. Koch, M. Joffre, D. Hulin, A. Migus, and A. Antonetti, Phys. Rev. Lett. 59, 2588 (1987).
[CrossRef] [PubMed]

Jonas, D. M.

Karolczak, J.

M. Lorenc, M. Ziolek, R. Naskrecki, J. Karolczak, J. Kubicki, and A. Maciejewski, Appl. Phys. B 74, 19 (2002).
[CrossRef]

Koch, S. W.

M. Joffre, D. Hulin, A. Migus, A. Antonetti, C. Benoit à la Guillaume, N. Peyghambarian, M. Lindberg, and S. W. Koch, Opt. Lett. 13, 276 (1988).
[CrossRef] [PubMed]

B. Fluegel, N. Peyghambarian, G. Olbright, M. Lindberg, S. W. Koch, M. Joffre, D. Hulin, A. Migus, and A. Antonetti, Phys. Rev. Lett. 59, 2588 (1987).
[CrossRef] [PubMed]

Kubarych, K. J.

J. Treuffet, K. J. Kubarych, J.-C. Lambry, E. Pilet, J.-B. Masson, J.-L. Martin, M. H. Vos, M. Joffre, and A. Alexandrou, Proc. Natl. Acad. Sci. USA 104, 15705 (2007).
[CrossRef] [PubMed]

K. J. Kubarych, M. Joffre, A. Moore, N. Belabas, and D. M. Jonas, Opt. Lett. 30, 1228 (2005).
[CrossRef] [PubMed]

Kubicki, J.

M. Lorenc, M. Ziolek, R. Naskrecki, J. Karolczak, J. Kubicki, and A. Maciejewski, Appl. Phys. B 74, 19 (2002).
[CrossRef]

Lambry, J.-C.

J. Treuffet, K. J. Kubarych, J.-C. Lambry, E. Pilet, J.-B. Masson, J.-L. Martin, M. H. Vos, M. Joffre, and A. Alexandrou, Proc. Natl. Acad. Sci. USA 104, 15705 (2007).
[CrossRef] [PubMed]

Lamparter, T.

C. Schumann, R. Groß, M. M. N. Wolf, R. Diller, N. Michael, and T. Lamparter, Biophys. J. 94, 3189 (2008).
[CrossRef] [PubMed]

Lindberg, M.

M. Joffre, D. Hulin, A. Migus, A. Antonetti, C. Benoit à la Guillaume, N. Peyghambarian, M. Lindberg, and S. W. Koch, Opt. Lett. 13, 276 (1988).
[CrossRef] [PubMed]

B. Fluegel, N. Peyghambarian, G. Olbright, M. Lindberg, S. W. Koch, M. Joffre, D. Hulin, A. Migus, and A. Antonetti, Phys. Rev. Lett. 59, 2588 (1987).
[CrossRef] [PubMed]

Lorenc, M.

M. Lorenc, M. Ziolek, R. Naskrecki, J. Karolczak, J. Kubicki, and A. Maciejewski, Appl. Phys. B 74, 19 (2002).
[CrossRef]

Maciejewski, A.

M. Lorenc, M. Ziolek, R. Naskrecki, J. Karolczak, J. Kubicki, and A. Maciejewski, Appl. Phys. B 74, 19 (2002).
[CrossRef]

Martin, J.-L.

J. Treuffet, K. J. Kubarych, J.-C. Lambry, E. Pilet, J.-B. Masson, J.-L. Martin, M. H. Vos, M. Joffre, and A. Alexandrou, Proc. Natl. Acad. Sci. USA 104, 15705 (2007).
[CrossRef] [PubMed]

Massari, A. M.

I. J. Finkelstein, A. M. Massari, and M. D. Fayer, Biophys. J. 92, 3652 (2007).
[CrossRef] [PubMed]

Masson, J.-B.

J. Treuffet, K. J. Kubarych, J.-C. Lambry, E. Pilet, J.-B. Masson, J.-L. Martin, M. H. Vos, M. Joffre, and A. Alexandrou, Proc. Natl. Acad. Sci. USA 104, 15705 (2007).
[CrossRef] [PubMed]

Michael, N.

C. Schumann, R. Groß, M. M. N. Wolf, R. Diller, N. Michael, and T. Lamparter, Biophys. J. 94, 3189 (2008).
[CrossRef] [PubMed]

Migus, A.

M. Joffre, D. Hulin, A. Migus, A. Antonetti, C. Benoit à la Guillaume, N. Peyghambarian, M. Lindberg, and S. W. Koch, Opt. Lett. 13, 276 (1988).
[CrossRef] [PubMed]

B. Fluegel, N. Peyghambarian, G. Olbright, M. Lindberg, S. W. Koch, M. Joffre, D. Hulin, A. Migus, and A. Antonetti, Phys. Rev. Lett. 59, 2588 (1987).
[CrossRef] [PubMed]

Moore, A.

Naskrecki, R.

M. Lorenc, M. Ziolek, R. Naskrecki, J. Karolczak, J. Kubicki, and A. Maciejewski, Appl. Phys. B 74, 19 (2002).
[CrossRef]

Neumann, K.

K. Neumann, M.-K. Verhoefen, I. Weber, C. Glaubitz, and J. Wachtveitl, Biophys. J. 94, 4796 (2008).
[CrossRef] [PubMed]

Olbright, G.

B. Fluegel, N. Peyghambarian, G. Olbright, M. Lindberg, S. W. Koch, M. Joffre, D. Hulin, A. Migus, and A. Antonetti, Phys. Rev. Lett. 59, 2588 (1987).
[CrossRef] [PubMed]

Peyghambarian, N.

M. Joffre, D. Hulin, A. Migus, A. Antonetti, C. Benoit à la Guillaume, N. Peyghambarian, M. Lindberg, and S. W. Koch, Opt. Lett. 13, 276 (1988).
[CrossRef] [PubMed]

B. Fluegel, N. Peyghambarian, G. Olbright, M. Lindberg, S. W. Koch, M. Joffre, D. Hulin, A. Migus, and A. Antonetti, Phys. Rev. Lett. 59, 2588 (1987).
[CrossRef] [PubMed]

Pilet, E.

J. Treuffet, K. J. Kubarych, J.-C. Lambry, E. Pilet, J.-B. Masson, J.-L. Martin, M. H. Vos, M. Joffre, and A. Alexandrou, Proc. Natl. Acad. Sci. USA 104, 15705 (2007).
[CrossRef] [PubMed]

Polack, T.

Schade, M.

D. Wolpert, M. Schade, and T. Brixner, J. Chem. Phys. 129, 094504 (2008).
[CrossRef] [PubMed]

Schumann, C.

C. Schumann, R. Groß, M. M. N. Wolf, R. Diller, N. Michael, and T. Lamparter, Biophys. J. 94, 3189 (2008).
[CrossRef] [PubMed]

Shank, C. V.

C. H. Brito Cruz, J. P. Gordon, P. C. Becker, R. L. Fork, and C. V. Shank, IEEE J. Quantum Electron. 24, 261 (1988).
[CrossRef]

Tannor, D. J.

Treuffet, J.

J. Treuffet, K. J. Kubarych, J.-C. Lambry, E. Pilet, J.-B. Masson, J.-L. Martin, M. H. Vos, M. Joffre, and A. Alexandrou, Proc. Natl. Acad. Sci. USA 104, 15705 (2007).
[CrossRef] [PubMed]

Verhoefen, M.-K.

K. Neumann, M.-K. Verhoefen, I. Weber, C. Glaubitz, and J. Wachtveitl, Biophys. J. 94, 4796 (2008).
[CrossRef] [PubMed]

Vos, M. H.

J. Treuffet, K. J. Kubarych, J.-C. Lambry, E. Pilet, J.-B. Masson, J.-L. Martin, M. H. Vos, M. Joffre, and A. Alexandrou, Proc. Natl. Acad. Sci. USA 104, 15705 (2007).
[CrossRef] [PubMed]

Wachtveitl, J.

K. Neumann, M.-K. Verhoefen, I. Weber, C. Glaubitz, and J. Wachtveitl, Biophys. J. 94, 4796 (2008).
[CrossRef] [PubMed]

Weber, I.

K. Neumann, M.-K. Verhoefen, I. Weber, C. Glaubitz, and J. Wachtveitl, Biophys. J. 94, 4796 (2008).
[CrossRef] [PubMed]

Wolf, M. M. N.

C. Schumann, R. Groß, M. M. N. Wolf, R. Diller, N. Michael, and T. Lamparter, Biophys. J. 94, 3189 (2008).
[CrossRef] [PubMed]

Wolpert, D.

D. Wolpert, M. Schade, and T. Brixner, J. Chem. Phys. 129, 094504 (2008).
[CrossRef] [PubMed]

Ziolek, M.

M. Lorenc, M. Ziolek, R. Naskrecki, J. Karolczak, J. Kubicki, and A. Maciejewski, Appl. Phys. B 74, 19 (2002).
[CrossRef]

Annu. Rev. Phys. Chem. (1)

M. D. Fayer, Annu. Rev. Phys. Chem. 52, 315 (2001).
[CrossRef] [PubMed]

Appl. Phys. B (1)

M. Lorenc, M. Ziolek, R. Naskrecki, J. Karolczak, J. Kubicki, and A. Maciejewski, Appl. Phys. B 74, 19 (2002).
[CrossRef]

Biophys. J. (3)

K. Neumann, M.-K. Verhoefen, I. Weber, C. Glaubitz, and J. Wachtveitl, Biophys. J. 94, 4796 (2008).
[CrossRef] [PubMed]

C. Schumann, R. Groß, M. M. N. Wolf, R. Diller, N. Michael, and T. Lamparter, Biophys. J. 94, 3189 (2008).
[CrossRef] [PubMed]

I. J. Finkelstein, A. M. Massari, and M. D. Fayer, Biophys. J. 92, 3652 (2007).
[CrossRef] [PubMed]

Chem. Phys. (1)

P. Hamm, Chem. Phys. 200, 415 (1995).
[CrossRef]

IEEE J. Quantum Electron. (1)

C. H. Brito Cruz, J. P. Gordon, P. C. Becker, R. L. Fork, and C. V. Shank, IEEE J. Quantum Electron. 24, 261 (1988).
[CrossRef]

J. Chem. Phys. (1)

D. Wolpert, M. Schade, and T. Brixner, J. Chem. Phys. 129, 094504 (2008).
[CrossRef] [PubMed]

Opt. Express (2)

Opt. Lett. (2)

Phys. Rev. Lett. (1)

B. Fluegel, N. Peyghambarian, G. Olbright, M. Lindberg, S. W. Koch, M. Joffre, D. Hulin, A. Migus, and A. Antonetti, Phys. Rev. Lett. 59, 2588 (1987).
[CrossRef] [PubMed]

Proc. Natl. Acad. Sci. USA (2)

J. Treuffet, K. J. Kubarych, J.-C. Lambry, E. Pilet, J.-B. Masson, J.-L. Martin, M. H. Vos, M. Joffre, and A. Alexandrou, Proc. Natl. Acad. Sci. USA 104, 15705 (2007).
[CrossRef] [PubMed]

P. A. Anfinrud, C. Han, and R. M. Hochstrasser, Proc. Natl. Acad. Sci. USA 86, 8387 (1989).
[CrossRef] [PubMed]

Supplementary Material (1)

» Media 1: AVI (3424 KB)     

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Figures (2)

Fig. 1
Fig. 1

Left, application of the Fourier filtering technique to experimental data (top row) and simulated data (bottom row). (a) 400 nm pump 5.1 μ m probe spectrally resolved Δ T m ( τ , ν ) data of HbCO; (b) filtered data Δ T f ( τ , ν ) using filter (2) as described in the text; (c) filtered data using Eq. (3) as filter to emulate Δ T s ( τ , ν ) that would be obtained in the scanning approach with a 600 fs probe pulse. The evolution of Δ T s ( τ , ν ) for probe durations from 300 fs to 2 ps is available as a movie (Media 1). (d)–(f) Simulations corresponding to (a)–(c). Right, transient absorption signals at (g) 59.6 THz , (h) 59.0 THz ( A 0 band), and (i) 58.5 THz ( A 1 band) before (dots) and after (line) the filtering procedure; (g) and (h) are vertically offset by 2.4 and 1.2 mOD for clarity. In (h), the standard deviation before ( σ ) and after ( σ f ) filtering is given for the indicated interval 0.5 ps < τ < 6 ps ; (i) includes a fit (dashed line) to a single exponential convolved with the IRF. The arrows mark a small coherent spike that is also reduced after filtering.

Fig. 2
Fig. 2

Simulation with two lines at 58.5 and 58.0 THz bleached at τ = 0 and 4 ps , respectively, (a) before and (b) after filtering. Transient absorption at 58.5 THz is shown in (c) before (solid) and after (dashed) filtering.

Equations (3)

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

Δ T m ˆ ( ν τ , t ) = d τ d ν Δ T m ( τ , ν ) e i ( 2 π τ ν τ 2 π ν t ) .
f ̂ ( ν τ , t ) = exp [ | 2 π ν τ t | 2 + i ( 2 π ν τ t ) 2 ] ,
E ̂ ( ν τ , t ) = exp [ ( 2 π ν τ ) 2 Δ t 2 16 ln 2 t 2 ln 2 Δ t 2 + i ( 2 π ν τ t ) 2 ] .

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