Abstract

Shot-to-shot broadband detection is common in ultrafast pump–probe spectroscopy. Taking advantage of the intensity correlation of subsequent laser pulses improves the signal-to-noise ratio. Finite data readout times of CCD chips in the employed spectrometer and the maximum available speed of mechanical pump-beam choppers typically limit this approach to lasers with repetition rates of a few kHz. For high-repetition (≥ 100 kHz) systems, one typically averages over a larger number of laser shots leading to inferior signal-to-noise ratios or longer measurement times. Here we demonstrate broadband shot-to-shot detection in transient absorption spectroscopy with a 100-kHz femtosecond laser system. This is made possible using a home-built high-speed chopper with external laser synchronization and a fast CCD line camera. Shot-to-shot detection can reduce the data acquisition time by two orders of magnitude compared to few-kHz lasers while keeping the same signal-to-noise ratio.

© 2014 Optical Society of America

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    [CrossRef]
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    [CrossRef] [PubMed]
  4. G. Auböck, C. Consani, R. Monni, A. Cannizzo, F. v. Mourik, and M. Chergui, “Femtosecond pump/supercontinuum-probe setup with 20 kHz repetition rate,” Rev. Sci. Instrum. 83, 093105 (2012).
    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef] [PubMed]
  7. U. Megerle, I. Pugliesi, C. Schriever, C. Sailer, and E. Riedle, “Sub-50 fs broadband absorption spectroscopy with tunable excitation: Putting the analysis of ultrafast molecular dynamics on solid ground,” Appl. Phys. B 96, 215–231 (2009).
    [CrossRef]
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef]
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2014 (1)

S. D. McClure, D. B. Turner, P. C. Arpin, T. Mirkovic, and G. D. Scholes, “Coherent oscillations in the PC577 cryptophyte antenna occur in the excited electronic state,” J. Phys. Chem. B 118, 1296–1308 (2014).
[CrossRef] [PubMed]

2012 (2)

G. Auböck, C. Consani, R. Monni, A. Cannizzo, F. v. Mourik, and M. Chergui, “Femtosecond pump/supercontinuum-probe setup with 20 kHz repetition rate,” Rev. Sci. Instrum. 83, 093105 (2012).
[CrossRef] [PubMed]

J. J. Snellenburg, S. P. Laptenok, R. Seger, K. M. Mullen, and I. H. M. van Stokkum, “Glotaran: a Java-based Graphical User Interface for the R-package TIMP,” J. Stat. Softw. 49, 1–22 (2012).

2010 (2)

J. Buback, M. Kullmann, F. Langhojer, P. Nuernberger, R. Schmidt, F. Würthner, and T. Brixner, “Ultrafast bidirectional photoswitching of a spiropyran,” J. Am. Chem. Soc. 132, 16510–16519 (2010).
[CrossRef] [PubMed]

A. Yabushita, Y.-H. Lee, and T. Kobayashi, “Development of a multiplex fast-scan system for ultrafast time-resolved spectroscopy,” Rev. Sci. Instrum. 81, 063110 (2010).
[CrossRef] [PubMed]

2009 (3)

K. F. Lee, A. Bonvalet, P. Nuernberger, and M. Joffre, “Unobtrusive interferometer tracking by path length oscillation for multidimensional spectroscopy,” Opt. Express 17, 12379–12384 (2009).
[CrossRef] [PubMed]

U. Megerle, I. Pugliesi, C. Schriever, C. Sailer, and E. Riedle, “Sub-50 fs broadband absorption spectroscopy with tunable excitation: Putting the analysis of ultrafast molecular dynamics on solid ground,” Appl. Phys. B 96, 215–231 (2009).
[CrossRef]

M. Bradler, P. Baum, and E. Riedle, “Femtosecond continuum generation in bulk laser host materials with sub-μJ pump pulses,” Appl. Phys. B 97, 561–574 (2009).
[CrossRef]

2008 (1)

C. Schriever, S. Lochbrunner, E. Riedle, and D. J. Nesbitt, “Ultrasensitive ultraviolet-visible 20 fs absorption spectroscopy of low vapor pressure molecules in the gas phase,” Rev. Sci. Instrum. 79, 013107 (2008).
[CrossRef]

2007 (2)

D. Polli, L. Lüer, and G. Cerullo, “High-time-resolution pump-probe system with broadband detection for the study of time-domain vibrational dynamics,” Rev. Sci. Instrum. 78, 103108 (2007).
[CrossRef] [PubMed]

K. M. Mullen and I. H. M. van Stokkum, “TIMP: an R package for modeling multi-way spectroscopic measurements,” J. Stat. Softw. 18, 1–46 (2007).

2006 (1)

2004 (2)

I. H. M. van Stokkum, D. S. Larsen, and R. van Grondelle, “Global and target analysis of time-resolved spectra,” Biochim. Biophys. Acta, Bioenerg. 1657, 82–104 (2004).
[CrossRef]

T. Polack, J. P. Ogilvie, S. Franzen, M. H. Vos, M. Joffre, J.-L. Martin, and A. Alexandrou, “CO vibration as a probe of ligand dissociation and transfer in myoglobin,” Phys. Rev. Lett. 93, 018102 (2004).
[CrossRef] [PubMed]

2003 (1)

D. Wang, H. Jiang, S. Wu, H. Yang, Q. Gong, J. Xiang, and G. Xu, “An investigation of solvent effects on the optical properties of dye IR-140 using the pump supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 5, 515–519 (2003).
[CrossRef]

2002 (1)

D. Wang, H. Jiang, H. Yang, C. Liu, Q. Gong, J. Xiang, and G. Xu, “Investigation on photoexcited dynamics of IR-140 dye in ethanol by femtosecond supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 4, 155–159 (2002).
[CrossRef]

2000 (1)

A. H. Zewail, “Femtochemistry: atomic-scale dynamics of the chemical bond,” J. Phys. Chem. A 104, 5660–5694 (2000).
[CrossRef]

1998 (1)

Y. H. Meyer, M. Pittman, and P. Plaza, “Transient absorption of symmetrical carbocyanines,” J. Photochem. Photobiol. A 114, 1–21 (1998).
[CrossRef]

1997 (1)

P. Tournois, “Acousto-optic programmable dispersive filter for adaptive compensation of group delay time dispersion in laser systems,” Opt. Commun. 140, 245–249 (1997).
[CrossRef]

1995 (1)

1986 (1)

D. Linde, “Characterization of the noise in continuously operating mode-locked lasers,” Appl. Phys. B 39, 201–217 (1986).
[CrossRef]

Alexandrou, A.

T. Polack, J. P. Ogilvie, S. Franzen, M. H. Vos, M. Joffre, J.-L. Martin, and A. Alexandrou, “CO vibration as a probe of ligand dissociation and transfer in myoglobin,” Phys. Rev. Lett. 93, 018102 (2004).
[CrossRef] [PubMed]

Arpin, P. C.

S. D. McClure, D. B. Turner, P. C. Arpin, T. Mirkovic, and G. D. Scholes, “Coherent oscillations in the PC577 cryptophyte antenna occur in the excited electronic state,” J. Phys. Chem. B 118, 1296–1308 (2014).
[CrossRef] [PubMed]

Auböck, G.

G. Auböck, C. Consani, R. Monni, A. Cannizzo, F. v. Mourik, and M. Chergui, “Femtosecond pump/supercontinuum-probe setup with 20 kHz repetition rate,” Rev. Sci. Instrum. 83, 093105 (2012).
[CrossRef] [PubMed]

Baum, P.

M. Bradler, P. Baum, and E. Riedle, “Femtosecond continuum generation in bulk laser host materials with sub-μJ pump pulses,” Appl. Phys. B 97, 561–574 (2009).
[CrossRef]

Bonvalet, A.

Bradler, M.

M. Bradler, P. Baum, and E. Riedle, “Femtosecond continuum generation in bulk laser host materials with sub-μJ pump pulses,” Appl. Phys. B 97, 561–574 (2009).
[CrossRef]

Brixner, T.

J. Buback, M. Kullmann, F. Langhojer, P. Nuernberger, R. Schmidt, F. Würthner, and T. Brixner, “Ultrafast bidirectional photoswitching of a spiropyran,” J. Am. Chem. Soc. 132, 16510–16519 (2010).
[CrossRef] [PubMed]

Buback, J.

J. Buback, M. Kullmann, F. Langhojer, P. Nuernberger, R. Schmidt, F. Würthner, and T. Brixner, “Ultrafast bidirectional photoswitching of a spiropyran,” J. Am. Chem. Soc. 132, 16510–16519 (2010).
[CrossRef] [PubMed]

Cannizzo, A.

G. Auböck, C. Consani, R. Monni, A. Cannizzo, F. v. Mourik, and M. Chergui, “Femtosecond pump/supercontinuum-probe setup with 20 kHz repetition rate,” Rev. Sci. Instrum. 83, 093105 (2012).
[CrossRef] [PubMed]

Cerullo, G.

D. Polli, L. Lüer, and G. Cerullo, “High-time-resolution pump-probe system with broadband detection for the study of time-domain vibrational dynamics,” Rev. Sci. Instrum. 78, 103108 (2007).
[CrossRef] [PubMed]

Chergui, M.

G. Auböck, C. Consani, R. Monni, A. Cannizzo, F. v. Mourik, and M. Chergui, “Femtosecond pump/supercontinuum-probe setup with 20 kHz repetition rate,” Rev. Sci. Instrum. 83, 093105 (2012).
[CrossRef] [PubMed]

Consani, C.

G. Auböck, C. Consani, R. Monni, A. Cannizzo, F. v. Mourik, and M. Chergui, “Femtosecond pump/supercontinuum-probe setup with 20 kHz repetition rate,” Rev. Sci. Instrum. 83, 093105 (2012).
[CrossRef] [PubMed]

Eichberger, R.

Ernstorfer, R.

Feldstein, M. J.

Franzen, S.

T. Polack, J. P. Ogilvie, S. Franzen, M. H. Vos, M. Joffre, J.-L. Martin, and A. Alexandrou, “CO vibration as a probe of ligand dissociation and transfer in myoglobin,” Phys. Rev. Lett. 93, 018102 (2004).
[CrossRef] [PubMed]

Gong, Q.

D. Wang, H. Jiang, S. Wu, H. Yang, Q. Gong, J. Xiang, and G. Xu, “An investigation of solvent effects on the optical properties of dye IR-140 using the pump supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 5, 515–519 (2003).
[CrossRef]

D. Wang, H. Jiang, H. Yang, C. Liu, Q. Gong, J. Xiang, and G. Xu, “Investigation on photoexcited dynamics of IR-140 dye in ethanol by femtosecond supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 4, 155–159 (2002).
[CrossRef]

Gundlach, L.

Jiang, H.

D. Wang, H. Jiang, S. Wu, H. Yang, Q. Gong, J. Xiang, and G. Xu, “An investigation of solvent effects on the optical properties of dye IR-140 using the pump supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 5, 515–519 (2003).
[CrossRef]

D. Wang, H. Jiang, H. Yang, C. Liu, Q. Gong, J. Xiang, and G. Xu, “Investigation on photoexcited dynamics of IR-140 dye in ethanol by femtosecond supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 4, 155–159 (2002).
[CrossRef]

Joffre, M.

K. F. Lee, A. Bonvalet, P. Nuernberger, and M. Joffre, “Unobtrusive interferometer tracking by path length oscillation for multidimensional spectroscopy,” Opt. Express 17, 12379–12384 (2009).
[CrossRef] [PubMed]

T. Polack, J. P. Ogilvie, S. Franzen, M. H. Vos, M. Joffre, J.-L. Martin, and A. Alexandrou, “CO vibration as a probe of ligand dissociation and transfer in myoglobin,” Phys. Rev. Lett. 93, 018102 (2004).
[CrossRef] [PubMed]

Kobayashi, T.

A. Yabushita, Y.-H. Lee, and T. Kobayashi, “Development of a multiplex fast-scan system for ultrafast time-resolved spectroscopy,” Rev. Sci. Instrum. 81, 063110 (2010).
[CrossRef] [PubMed]

Kullmann, M.

J. Buback, M. Kullmann, F. Langhojer, P. Nuernberger, R. Schmidt, F. Würthner, and T. Brixner, “Ultrafast bidirectional photoswitching of a spiropyran,” J. Am. Chem. Soc. 132, 16510–16519 (2010).
[CrossRef] [PubMed]

Langhojer, F.

J. Buback, M. Kullmann, F. Langhojer, P. Nuernberger, R. Schmidt, F. Würthner, and T. Brixner, “Ultrafast bidirectional photoswitching of a spiropyran,” J. Am. Chem. Soc. 132, 16510–16519 (2010).
[CrossRef] [PubMed]

Laptenok, S. P.

J. J. Snellenburg, S. P. Laptenok, R. Seger, K. M. Mullen, and I. H. M. van Stokkum, “Glotaran: a Java-based Graphical User Interface for the R-package TIMP,” J. Stat. Softw. 49, 1–22 (2012).

Larsen, D. S.

I. H. M. van Stokkum, D. S. Larsen, and R. van Grondelle, “Global and target analysis of time-resolved spectra,” Biochim. Biophys. Acta, Bioenerg. 1657, 82–104 (2004).
[CrossRef]

Lee, K. F.

Lee, Y.-H.

A. Yabushita, Y.-H. Lee, and T. Kobayashi, “Development of a multiplex fast-scan system for ultrafast time-resolved spectroscopy,” Rev. Sci. Instrum. 81, 063110 (2010).
[CrossRef] [PubMed]

Linde, D.

D. Linde, “Characterization of the noise in continuously operating mode-locked lasers,” Appl. Phys. B 39, 201–217 (1986).
[CrossRef]

Liu, C.

D. Wang, H. Jiang, H. Yang, C. Liu, Q. Gong, J. Xiang, and G. Xu, “Investigation on photoexcited dynamics of IR-140 dye in ethanol by femtosecond supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 4, 155–159 (2002).
[CrossRef]

Lochbrunner, S.

C. Schriever, S. Lochbrunner, E. Riedle, and D. J. Nesbitt, “Ultrasensitive ultraviolet-visible 20 fs absorption spectroscopy of low vapor pressure molecules in the gas phase,” Rev. Sci. Instrum. 79, 013107 (2008).
[CrossRef]

Lüer, L.

D. Polli, L. Lüer, and G. Cerullo, “High-time-resolution pump-probe system with broadband detection for the study of time-domain vibrational dynamics,” Rev. Sci. Instrum. 78, 103108 (2007).
[CrossRef] [PubMed]

Martin, J.-L.

T. Polack, J. P. Ogilvie, S. Franzen, M. H. Vos, M. Joffre, J.-L. Martin, and A. Alexandrou, “CO vibration as a probe of ligand dissociation and transfer in myoglobin,” Phys. Rev. Lett. 93, 018102 (2004).
[CrossRef] [PubMed]

McClure, S. D.

S. D. McClure, D. B. Turner, P. C. Arpin, T. Mirkovic, and G. D. Scholes, “Coherent oscillations in the PC577 cryptophyte antenna occur in the excited electronic state,” J. Phys. Chem. B 118, 1296–1308 (2014).
[CrossRef] [PubMed]

Megerle, U.

U. Megerle, I. Pugliesi, C. Schriever, C. Sailer, and E. Riedle, “Sub-50 fs broadband absorption spectroscopy with tunable excitation: Putting the analysis of ultrafast molecular dynamics on solid ground,” Appl. Phys. B 96, 215–231 (2009).
[CrossRef]

Meyer, Y. H.

Y. H. Meyer, M. Pittman, and P. Plaza, “Transient absorption of symmetrical carbocyanines,” J. Photochem. Photobiol. A 114, 1–21 (1998).
[CrossRef]

Mirkovic, T.

S. D. McClure, D. B. Turner, P. C. Arpin, T. Mirkovic, and G. D. Scholes, “Coherent oscillations in the PC577 cryptophyte antenna occur in the excited electronic state,” J. Phys. Chem. B 118, 1296–1308 (2014).
[CrossRef] [PubMed]

Monni, R.

G. Auböck, C. Consani, R. Monni, A. Cannizzo, F. v. Mourik, and M. Chergui, “Femtosecond pump/supercontinuum-probe setup with 20 kHz repetition rate,” Rev. Sci. Instrum. 83, 093105 (2012).
[CrossRef] [PubMed]

Mourik, F. v.

G. Auböck, C. Consani, R. Monni, A. Cannizzo, F. v. Mourik, and M. Chergui, “Femtosecond pump/supercontinuum-probe setup with 20 kHz repetition rate,” Rev. Sci. Instrum. 83, 093105 (2012).
[CrossRef] [PubMed]

Mullen, K. M.

J. J. Snellenburg, S. P. Laptenok, R. Seger, K. M. Mullen, and I. H. M. van Stokkum, “Glotaran: a Java-based Graphical User Interface for the R-package TIMP,” J. Stat. Softw. 49, 1–22 (2012).

K. M. Mullen and I. H. M. van Stokkum, “TIMP: an R package for modeling multi-way spectroscopic measurements,” J. Stat. Softw. 18, 1–46 (2007).

Nesbitt, D. J.

C. Schriever, S. Lochbrunner, E. Riedle, and D. J. Nesbitt, “Ultrasensitive ultraviolet-visible 20 fs absorption spectroscopy of low vapor pressure molecules in the gas phase,” Rev. Sci. Instrum. 79, 013107 (2008).
[CrossRef]

Nuernberger, P.

J. Buback, M. Kullmann, F. Langhojer, P. Nuernberger, R. Schmidt, F. Würthner, and T. Brixner, “Ultrafast bidirectional photoswitching of a spiropyran,” J. Am. Chem. Soc. 132, 16510–16519 (2010).
[CrossRef] [PubMed]

K. F. Lee, A. Bonvalet, P. Nuernberger, and M. Joffre, “Unobtrusive interferometer tracking by path length oscillation for multidimensional spectroscopy,” Opt. Express 17, 12379–12384 (2009).
[CrossRef] [PubMed]

Ogilvie, J. P.

T. Polack, J. P. Ogilvie, S. Franzen, M. H. Vos, M. Joffre, J.-L. Martin, and A. Alexandrou, “CO vibration as a probe of ligand dissociation and transfer in myoglobin,” Phys. Rev. Lett. 93, 018102 (2004).
[CrossRef] [PubMed]

Piel, J.

Pittman, M.

Y. H. Meyer, M. Pittman, and P. Plaza, “Transient absorption of symmetrical carbocyanines,” J. Photochem. Photobiol. A 114, 1–21 (1998).
[CrossRef]

Plaza, P.

Y. H. Meyer, M. Pittman, and P. Plaza, “Transient absorption of symmetrical carbocyanines,” J. Photochem. Photobiol. A 114, 1–21 (1998).
[CrossRef]

Polack, T.

T. Polack, J. P. Ogilvie, S. Franzen, M. H. Vos, M. Joffre, J.-L. Martin, and A. Alexandrou, “CO vibration as a probe of ligand dissociation and transfer in myoglobin,” Phys. Rev. Lett. 93, 018102 (2004).
[CrossRef] [PubMed]

T. Polack, “Spectroscopie infrarouge impulsionnelle appliquee au transfert de ligands dans les hémoprotéines,” Ph.D. thesis, École Polytechnique, Paris (2003).

Polli, D.

D. Polli, L. Lüer, and G. Cerullo, “High-time-resolution pump-probe system with broadband detection for the study of time-domain vibrational dynamics,” Rev. Sci. Instrum. 78, 103108 (2007).
[CrossRef] [PubMed]

Pugliesi, I.

U. Megerle, I. Pugliesi, C. Schriever, C. Sailer, and E. Riedle, “Sub-50 fs broadband absorption spectroscopy with tunable excitation: Putting the analysis of ultrafast molecular dynamics on solid ground,” Appl. Phys. B 96, 215–231 (2009).
[CrossRef]

Riedle, E.

U. Megerle, I. Pugliesi, C. Schriever, C. Sailer, and E. Riedle, “Sub-50 fs broadband absorption spectroscopy with tunable excitation: Putting the analysis of ultrafast molecular dynamics on solid ground,” Appl. Phys. B 96, 215–231 (2009).
[CrossRef]

M. Bradler, P. Baum, and E. Riedle, “Femtosecond continuum generation in bulk laser host materials with sub-μJ pump pulses,” Appl. Phys. B 97, 561–574 (2009).
[CrossRef]

C. Schriever, S. Lochbrunner, E. Riedle, and D. J. Nesbitt, “Ultrasensitive ultraviolet-visible 20 fs absorption spectroscopy of low vapor pressure molecules in the gas phase,” Rev. Sci. Instrum. 79, 013107 (2008).
[CrossRef]

J. Piel, E. Riedle, L. Gundlach, R. Ernstorfer, and R. Eichberger, “Sub-20 fs visible pulses with 750 nJ energy from a 100 kHz noncollinear optical parametric amplifier,” Opt. Lett. 31, 1289–1291 (2006).
[CrossRef] [PubMed]

Sailer, C.

U. Megerle, I. Pugliesi, C. Schriever, C. Sailer, and E. Riedle, “Sub-50 fs broadband absorption spectroscopy with tunable excitation: Putting the analysis of ultrafast molecular dynamics on solid ground,” Appl. Phys. B 96, 215–231 (2009).
[CrossRef]

Scherer, N. F.

Schmidt, R.

J. Buback, M. Kullmann, F. Langhojer, P. Nuernberger, R. Schmidt, F. Würthner, and T. Brixner, “Ultrafast bidirectional photoswitching of a spiropyran,” J. Am. Chem. Soc. 132, 16510–16519 (2010).
[CrossRef] [PubMed]

Scholes, G. D.

S. D. McClure, D. B. Turner, P. C. Arpin, T. Mirkovic, and G. D. Scholes, “Coherent oscillations in the PC577 cryptophyte antenna occur in the excited electronic state,” J. Phys. Chem. B 118, 1296–1308 (2014).
[CrossRef] [PubMed]

Schriever, C.

U. Megerle, I. Pugliesi, C. Schriever, C. Sailer, and E. Riedle, “Sub-50 fs broadband absorption spectroscopy with tunable excitation: Putting the analysis of ultrafast molecular dynamics on solid ground,” Appl. Phys. B 96, 215–231 (2009).
[CrossRef]

C. Schriever, S. Lochbrunner, E. Riedle, and D. J. Nesbitt, “Ultrasensitive ultraviolet-visible 20 fs absorption spectroscopy of low vapor pressure molecules in the gas phase,” Rev. Sci. Instrum. 79, 013107 (2008).
[CrossRef]

Seger, R.

J. J. Snellenburg, S. P. Laptenok, R. Seger, K. M. Mullen, and I. H. M. van Stokkum, “Glotaran: a Java-based Graphical User Interface for the R-package TIMP,” J. Stat. Softw. 49, 1–22 (2012).

Snellenburg, J. J.

J. J. Snellenburg, S. P. Laptenok, R. Seger, K. M. Mullen, and I. H. M. van Stokkum, “Glotaran: a Java-based Graphical User Interface for the R-package TIMP,” J. Stat. Softw. 49, 1–22 (2012).

Tournois, P.

P. Tournois, “Acousto-optic programmable dispersive filter for adaptive compensation of group delay time dispersion in laser systems,” Opt. Commun. 140, 245–249 (1997).
[CrossRef]

Turner, D. B.

S. D. McClure, D. B. Turner, P. C. Arpin, T. Mirkovic, and G. D. Scholes, “Coherent oscillations in the PC577 cryptophyte antenna occur in the excited electronic state,” J. Phys. Chem. B 118, 1296–1308 (2014).
[CrossRef] [PubMed]

van Grondelle, R.

I. H. M. van Stokkum, D. S. Larsen, and R. van Grondelle, “Global and target analysis of time-resolved spectra,” Biochim. Biophys. Acta, Bioenerg. 1657, 82–104 (2004).
[CrossRef]

van Stokkum, I. H. M.

J. J. Snellenburg, S. P. Laptenok, R. Seger, K. M. Mullen, and I. H. M. van Stokkum, “Glotaran: a Java-based Graphical User Interface for the R-package TIMP,” J. Stat. Softw. 49, 1–22 (2012).

K. M. Mullen and I. H. M. van Stokkum, “TIMP: an R package for modeling multi-way spectroscopic measurements,” J. Stat. Softw. 18, 1–46 (2007).

I. H. M. van Stokkum, D. S. Larsen, and R. van Grondelle, “Global and target analysis of time-resolved spectra,” Biochim. Biophys. Acta, Bioenerg. 1657, 82–104 (2004).
[CrossRef]

Vöhringer, P.

Vos, M. H.

T. Polack, J. P. Ogilvie, S. Franzen, M. H. Vos, M. Joffre, J.-L. Martin, and A. Alexandrou, “CO vibration as a probe of ligand dissociation and transfer in myoglobin,” Phys. Rev. Lett. 93, 018102 (2004).
[CrossRef] [PubMed]

Wang, D.

D. Wang, H. Jiang, S. Wu, H. Yang, Q. Gong, J. Xiang, and G. Xu, “An investigation of solvent effects on the optical properties of dye IR-140 using the pump supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 5, 515–519 (2003).
[CrossRef]

D. Wang, H. Jiang, H. Yang, C. Liu, Q. Gong, J. Xiang, and G. Xu, “Investigation on photoexcited dynamics of IR-140 dye in ethanol by femtosecond supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 4, 155–159 (2002).
[CrossRef]

Wu, S.

D. Wang, H. Jiang, S. Wu, H. Yang, Q. Gong, J. Xiang, and G. Xu, “An investigation of solvent effects on the optical properties of dye IR-140 using the pump supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 5, 515–519 (2003).
[CrossRef]

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J. Buback, M. Kullmann, F. Langhojer, P. Nuernberger, R. Schmidt, F. Würthner, and T. Brixner, “Ultrafast bidirectional photoswitching of a spiropyran,” J. Am. Chem. Soc. 132, 16510–16519 (2010).
[CrossRef] [PubMed]

Xiang, J.

D. Wang, H. Jiang, S. Wu, H. Yang, Q. Gong, J. Xiang, and G. Xu, “An investigation of solvent effects on the optical properties of dye IR-140 using the pump supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 5, 515–519 (2003).
[CrossRef]

D. Wang, H. Jiang, H. Yang, C. Liu, Q. Gong, J. Xiang, and G. Xu, “Investigation on photoexcited dynamics of IR-140 dye in ethanol by femtosecond supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 4, 155–159 (2002).
[CrossRef]

Xu, G.

D. Wang, H. Jiang, S. Wu, H. Yang, Q. Gong, J. Xiang, and G. Xu, “An investigation of solvent effects on the optical properties of dye IR-140 using the pump supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 5, 515–519 (2003).
[CrossRef]

D. Wang, H. Jiang, H. Yang, C. Liu, Q. Gong, J. Xiang, and G. Xu, “Investigation on photoexcited dynamics of IR-140 dye in ethanol by femtosecond supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 4, 155–159 (2002).
[CrossRef]

Yabushita, A.

A. Yabushita, Y.-H. Lee, and T. Kobayashi, “Development of a multiplex fast-scan system for ultrafast time-resolved spectroscopy,” Rev. Sci. Instrum. 81, 063110 (2010).
[CrossRef] [PubMed]

Yang, H.

D. Wang, H. Jiang, S. Wu, H. Yang, Q. Gong, J. Xiang, and G. Xu, “An investigation of solvent effects on the optical properties of dye IR-140 using the pump supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 5, 515–519 (2003).
[CrossRef]

D. Wang, H. Jiang, H. Yang, C. Liu, Q. Gong, J. Xiang, and G. Xu, “Investigation on photoexcited dynamics of IR-140 dye in ethanol by femtosecond supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 4, 155–159 (2002).
[CrossRef]

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Appl. Phys. B (3)

U. Megerle, I. Pugliesi, C. Schriever, C. Sailer, and E. Riedle, “Sub-50 fs broadband absorption spectroscopy with tunable excitation: Putting the analysis of ultrafast molecular dynamics on solid ground,” Appl. Phys. B 96, 215–231 (2009).
[CrossRef]

M. Bradler, P. Baum, and E. Riedle, “Femtosecond continuum generation in bulk laser host materials with sub-μJ pump pulses,” Appl. Phys. B 97, 561–574 (2009).
[CrossRef]

D. Linde, “Characterization of the noise in continuously operating mode-locked lasers,” Appl. Phys. B 39, 201–217 (1986).
[CrossRef]

Biochim. Biophys. Acta, Bioenerg. (1)

I. H. M. van Stokkum, D. S. Larsen, and R. van Grondelle, “Global and target analysis of time-resolved spectra,” Biochim. Biophys. Acta, Bioenerg. 1657, 82–104 (2004).
[CrossRef]

J. Am. Chem. Soc. (1)

J. Buback, M. Kullmann, F. Langhojer, P. Nuernberger, R. Schmidt, F. Würthner, and T. Brixner, “Ultrafast bidirectional photoswitching of a spiropyran,” J. Am. Chem. Soc. 132, 16510–16519 (2010).
[CrossRef] [PubMed]

J. Opt. A: Pure Appl. Opt. (2)

D. Wang, H. Jiang, H. Yang, C. Liu, Q. Gong, J. Xiang, and G. Xu, “Investigation on photoexcited dynamics of IR-140 dye in ethanol by femtosecond supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 4, 155–159 (2002).
[CrossRef]

D. Wang, H. Jiang, S. Wu, H. Yang, Q. Gong, J. Xiang, and G. Xu, “An investigation of solvent effects on the optical properties of dye IR-140 using the pump supercontinuum-probing technique,” J. Opt. A: Pure Appl. Opt. 5, 515–519 (2003).
[CrossRef]

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

J. Photochem. Photobiol. A (1)

Y. H. Meyer, M. Pittman, and P. Plaza, “Transient absorption of symmetrical carbocyanines,” J. Photochem. Photobiol. A 114, 1–21 (1998).
[CrossRef]

J. Phys. Chem. A (1)

A. H. Zewail, “Femtochemistry: atomic-scale dynamics of the chemical bond,” J. Phys. Chem. A 104, 5660–5694 (2000).
[CrossRef]

J. Phys. Chem. B (1)

S. D. McClure, D. B. Turner, P. C. Arpin, T. Mirkovic, and G. D. Scholes, “Coherent oscillations in the PC577 cryptophyte antenna occur in the excited electronic state,” J. Phys. Chem. B 118, 1296–1308 (2014).
[CrossRef] [PubMed]

J. Stat. Softw. (2)

J. J. Snellenburg, S. P. Laptenok, R. Seger, K. M. Mullen, and I. H. M. van Stokkum, “Glotaran: a Java-based Graphical User Interface for the R-package TIMP,” J. Stat. Softw. 49, 1–22 (2012).

K. M. Mullen and I. H. M. van Stokkum, “TIMP: an R package for modeling multi-way spectroscopic measurements,” J. Stat. Softw. 18, 1–46 (2007).

Opt. Commun. (1)

P. Tournois, “Acousto-optic programmable dispersive filter for adaptive compensation of group delay time dispersion in laser systems,” Opt. Commun. 140, 245–249 (1997).
[CrossRef]

Opt. Express (1)

Opt. Lett. (1)

Phys. Rev. Lett. (1)

T. Polack, J. P. Ogilvie, S. Franzen, M. H. Vos, M. Joffre, J.-L. Martin, and A. Alexandrou, “CO vibration as a probe of ligand dissociation and transfer in myoglobin,” Phys. Rev. Lett. 93, 018102 (2004).
[CrossRef] [PubMed]

Rev. Sci. Instrum. (4)

G. Auböck, C. Consani, R. Monni, A. Cannizzo, F. v. Mourik, and M. Chergui, “Femtosecond pump/supercontinuum-probe setup with 20 kHz repetition rate,” Rev. Sci. Instrum. 83, 093105 (2012).
[CrossRef] [PubMed]

C. Schriever, S. Lochbrunner, E. Riedle, and D. J. Nesbitt, “Ultrasensitive ultraviolet-visible 20 fs absorption spectroscopy of low vapor pressure molecules in the gas phase,” Rev. Sci. Instrum. 79, 013107 (2008).
[CrossRef]

D. Polli, L. Lüer, and G. Cerullo, “High-time-resolution pump-probe system with broadband detection for the study of time-domain vibrational dynamics,” Rev. Sci. Instrum. 78, 103108 (2007).
[CrossRef] [PubMed]

A. Yabushita, Y.-H. Lee, and T. Kobayashi, “Development of a multiplex fast-scan system for ultrafast time-resolved spectroscopy,” Rev. Sci. Instrum. 81, 063110 (2010).
[CrossRef] [PubMed]

Other (1)

T. Polack, “Spectroscopie infrarouge impulsionnelle appliquee au transfert de ligands dans les hémoprotéines,” Ph.D. thesis, École Polytechnique, Paris (2003).

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Figures (6)

Fig. 1
Fig. 1

Typical scheme for measuring and calculating changes in absorbance Δa. For k probe pulses averaged on the detector the chopper either blocks or transmits k corresponding pump pulses (state of the pump chopper shown in gray). At a given delay time τ the change in absorbance is averaged over n values of Δa, resulting in an overall number of i recorded pulses. Afterwards a set of N transient maps each one consisting of t delay times τ can be averaged. For k = 1 the calculation of Δa is shot-to-shot (inset on lower right).

Fig. 2
Fig. 2

Experimental setup for 100-kHz shot-to-shot transient absorption spectroscopy. A light barrier attached to the chopper produces a 100-kHz master trigger which is synchronized to the trigger signal output of the oscillator. The amplifier is triggered by the synchronized trigger to ensure that only pulses matching the chopper wheel rotation are amplified. A detailed explanation is given in the text. A connectivity diagram of the synchronization box can be found in the Appendix.

Fig. 3
Fig. 3

Transient absorption data of IR 140 in ethanol measured shot-to-shot at 100-kHz repetition rate. a) The transient map was recorded with excitation at 800 nm and a sapphire whitelight probe continuum. Data was averaged for k = 1, n = 500, t = 200, and N = 10. Note that the delay time axis changes from linear to logarithmic scaling for τ > 1 ps. b) The ESA can be seen in the difference spectra for various delay times. The spike in all difference spectra around 590 nm originates from a dip in the whitelight probe spectrum. c) The dynamics of the ESA are shown by transients for three different wavelengths. The dashed lines indicate the results of a global lifetime analysis.

Fig. 4
Fig. 4

Noise and correlation analysis at 537.4 nm. a) The Fourier transform f of i = 7×105 intensities I0,m on one pixel for subsequent probe pulses reveals dominant low-frequency contributions up to roughly 1 kHz. b) The high correlation between probe pulses calculated for i = 215 decreases for greater temporal spacing.

Fig. 5
Fig. 5

Comparative noise-level analysis for k = 100 and k = 1 (shot-to-shot). a) For a single calculation of Δa (n = 1) for each delay time τ the noise level is equivalent for (k = 100, i = 200) and (k = 1, i = 2). b) For the same number of acquired pulses (i = 1000) the noise level is about a factor of 3 smaller for k = 1 than for k = 100.

Fig. 6
Fig. 6

Connectivity diagram of the synchronization electronics.

Tables (1)

Tables Icon

Table 1 Noise contributions and error for the calculated change in absorbance Δa.

Equations (5)

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

a = lg I 0 I ,
Δ a = a p a u = lg I 0 I p lg I 0 I u .
Δ a = lg I u I p .
f = | { I 0 , 1 , I 0 , 2 , , I 0 , i } | .
ρ j = 1 σ 2 i m = 1 i j [ ( I 0 , m μ ) ( I 0 , m + j μ ) ] ,

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