OSA's Digital Library

Optics Express

Optics Express

  • Editor: Andrew M. Weiner
  • Vol. 21, Iss. 17 — Aug. 26, 2013
  • pp: 20145–20158

A novel setup for femtosecond pump-repump-probe IR spectroscopy with few cycle CEP stable pulses

Maximilian Bradler, Jasper C. Werhahn, Daniel Hutzler, Simon Fuhrmann, Rupert Heider, Eberhard Riedle, Hristo Iglev, and Reinhard Kienberger  »View Author Affiliations

Optics Express, Vol. 21, Issue 17, pp. 20145-20158 (2013)

View Full Text Article

Enhanced HTML    Acrobat PDF (1557 KB)

Browse Journals / Lookup Meetings

Browse by Journal and Year


Lookup Conference Papers

Close Browse Journals / Lookup Meetings

Article Tools



We present a three-color mid-IR setup for vibrational pump-repump-probe experiments with a temporal resolution well below 100 fs and a freely selectable spectral resolution of 20 to 360 cm−1 for the pump and repump. The usable probe range without optical realignment is 900 cm−1. The experimental design employed is greatly simplified compared to the widely used setups, highly robust and includes a novel means for generation of tunable few-cycle pulses with stable carrier-envelope phase. A Ti:sapphire pump system operating with 1 kHz and a modest 150 fs pulse duration supplies the total pump energy of just 0.6 mJ. The good signal-to-noise ratio of the setup allows the determination of spectrally resolved transient probe changes smaller than 6·10−5 OD at 130 time delays in just 45 minutes. The performance of the spectrometer is demonstrated with transient IR spectra and decay curves of HDO molecules in lithium nitrate trihydrate and ice and a first all MIR pump-repump-probe measurement.

© 2013 OSA

OCIS Codes
(300.6190) Spectroscopy : Spectrometers
(300.6340) Spectroscopy : Spectroscopy, infrared
(300.6500) Spectroscopy : Spectroscopy, time-resolved
(300.6530) Spectroscopy : Spectroscopy, ultrafast
(320.7110) Ultrafast optics : Ultrafast nonlinear optics
(320.7150) Ultrafast optics : Ultrafast spectroscopy

ToC Category:

Original Manuscript: May 23, 2013
Revised Manuscript: July 26, 2013
Manuscript Accepted: July 27, 2013
Published: August 20, 2013

Maximilian Bradler, Jasper C. Werhahn, Daniel Hutzler, Simon Fuhrmann, Rupert Heider, Eberhard Riedle, Hristo Iglev, and Reinhard Kienberger, "A novel setup for femtosecond pump-repump-probe IR spectroscopy with few cycle CEP stable pulses," Opt. Express 21, 20145-20158 (2013)

Sort:  Author  |  Year  |  Journal  |  Reset  


  1. H. Graener, G. Seifert, and A. Laubereau, “New spectroscopy of water using tunable picosecond pulses in the infrared,” Phys. Rev. Lett.66(16), 2092–2095 (1991). [CrossRef] [PubMed]
  2. S. Woutersen, U. Emmerichs, and H. J. Bakker, “Femtosecond mid-IR pump-probe spectroscopy of liquid water: evidence for a two-component structure,” Science278(5338), 658–660 (1997). [CrossRef]
  3. M. T. Zanni and R. M. Hochstrasser, “Two-dimensional infrared spectroscopy: a promising new method for the time resolution of structures,” Curr. Opin. Struct. Biol.11(5), 516–522 (2001). [CrossRef] [PubMed]
  4. M. Khalil, N. Demirdöven, and A. Tokmakoff, “Coherent 2D IR spectroscopy: molecular structure and dynamics in solution,” J. Phys. Chem. A107(27), 5258–5279 (2003). [CrossRef]
  5. E. T. J. Nibbering and T. Elsaesser, “Ultrafast vibrational dynamics of hydrogen bonds in the condensed phase,” Chem. Rev.104(4), 1887–1914 (2004). [CrossRef] [PubMed]
  6. D. Kraemer, M. L. Cowan, A. Paarmann, N. Huse, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller, “Temperature dependence of the two-dimensional infrared spectrum of liquid H2O,” Proc. Natl. Acad. Sci. U.S.A.105(2), 437–442 (2008). [CrossRef] [PubMed]
  7. H. J. Bakker and J. L. Skinner, “Vibrational spectroscopy as a probe of structure and dynamics in liquid water,” Chem. Rev.110(3), 1498–1517 (2010). [CrossRef] [PubMed]
  8. J. C. Werhahn, S. Pandelov, S. S. Xantheas, and H. Iglev, “Dynamics of weak, bifurcated, and strong hydrogen bonds in lithium nitrate trihydrate,” J. Phys. Chem. Lett.2(13), 1633–1638 (2011). [CrossRef]
  9. P. Hamm, S. Wiemann, M. Zurek, and W. Zinth, “Highly sensitive multichannel spectrometer for subpicosecond spectroscopy in the midinfrared,” Opt. Lett.19(20), 1642–1644 (1994). [CrossRef] [PubMed]
  10. J. L. Bingaman, C. L. Kohnhorst, G. A. Van Meter, B. A. McElroy, E. A. Rakowski, B. W. Caplins, T. A. Gutowski, C. J. Stromberg, C. E. Webster, and E. J. Heilweil, “Time-resolved vibrational spectroscopy of [FeFe]-hydrogenase model compounds,” J. Phys. Chem. A116(27), 7261–7271 (2012). [CrossRef] [PubMed]
  11. P. M. Donaldson, H. Strzalka, and P. Hamm, “High sensitivity transient infrared spectroscopy: a UV/visible transient grating spectrometer with a heterodyne detected infrared probe,” Opt. Express20(12), 12761–12770 (2012). [CrossRef] [PubMed]
  12. R. A. Kaindl, M. Wurm, K. Reimann, P. Hamm, A. W. Weiner, and M. Woerner, “Generation, shaping, and characterization of intense femtosecond pulses tunable from 3 to 20 µm,” J. Opt. Soc. Am. B17(12), 2086–2094 (2000). [CrossRef]
  13. N. Demirdöven, M. Khalil, O. Golonzka, and A. Tokmakoff, “Dispersion compensation with optical materials for compression of intense sub-100-fs mid-infrared pulses,” Opt. Lett.27(6), 433–435 (2002). [CrossRef] [PubMed]
  14. J. B. Asbury, T. Steinel, and M. D. Fayer, “Vibrational echo correlation spectroscopy probes of hydrogen bond dynamics in water and methanol,” J. Lumin.107(1-4), 271–286 (2004). [CrossRef] [PubMed]
  15. H. S. Chung, M. Khalil, A. W. Smith, and A. Tokmakoff, “Transient two-dimensional IR spectrometer for probing nanosecond temperature-jump kinetics,” Rev. Sci. Instrum.78(6), 063101 (2007). [CrossRef] [PubMed]
  16. S. Park, K. Kwak, and M. D. Fayer, “Ultrafast 2D-IR vibrational echo spectroscopy: a probe of molecular dynamics,” Laser Phys. Lett.4(10), 704–718 (2007). [CrossRef]
  17. S. H. Shim and M. T. Zanni, “How to turn your pump-probe instrument into a multidimensional spectrometer: 2D IR and Vis spectroscopies via pulse shaping,” Phys. Chem. Chem. Phys.11(5), 748–761 (2009). [CrossRef] [PubMed]
  18. K. C. Jones, Z. Ganim, C. S. Peng, and A. Tokmakoff, “Transient two-dimensional spectroscopy with linear absorption corrections applied to temperature-jump two-dimensional infrared,” J. Opt. Soc. Am. B29(1), 118–129 (2012). [CrossRef]
  19. D. R. Skoff, J. E. Laaser, S. S. Mukherjee, C. T. Middleton, and M. T. Zanni, “Simplified and economical 2D IR spectrometer design using a dual acousto-optic modulator,” Chem. Phys.in press., doi:. [CrossRef]
  20. D. Eisenberg and W. Kauzmann, The Structure and Properties of Water (Oxford University, 1969).
  21. F. Franks, Water: A Comprehensive Treatise (Plenum Press, 1972).
  22. Y. Tanimura and S. Mukamel, “2-dimensional femtosecond vibrational spectroscopy of liquids,” J. Chem. Phys.99(12), 9496–9511 (1993). [CrossRef]
  23. M. Bradler, C. Homann, and E. Riedle, “Mid-IR femtosecond pulse generation on the microjoule level up to 5 μm at high repetition rates,” Opt. Lett.36(21), 4212–4214 (2011). [CrossRef] [PubMed]
  24. M. Bradler, P. Baum, and E. Riedle, “Femtosecond continuum generation in bulk laser host materials with sub-µJ pump pulses,” Appl. Phys. B97(3), 561–574 (2009). [CrossRef]
  25. J. Piel, M. Beutter, and E. Riedle, “20-50-fs pulses tunable across the near infrared from a blue-pumped noncollinear parametric amplifier,” Opt. Lett.25(3), 180–182 (2000). [CrossRef] [PubMed]
  26. I. Hartl and W. Zinth, “A novel spectrometer system for the investigation of vibrational energy relaxation with sub-picosecond time resolution,” Opt. Commun.160(1–3), 184–190 (1999). [CrossRef]
  27. V. Petrov, F. Rotermund, and F. Noack, “Generation of high-power femtosecond light pulses at 1 kHz in the mid-infrared spectral range between 3 and 12 µm by second-order nonlinear processes in optical crystals,” J. Opt. A, Pure Appl. Opt.3(3), R1–R19 (2001). [CrossRef]
  28. D. Brida, C. Manzoni, G. Cirmi, M. Marangoni, S. De Silvestri, and G. Cerullo, “Generation of broadband mid-infrared pulses from an optical parametric amplifier,” Opt. Express15(23), 15035–15040 (2007). [CrossRef] [PubMed]
  29. W. E. White, F. G. Patterson, R. L. Combs, D. F. Price, and R. L. Shepherd, “Compensation of higher-order frequency-dependent phase terms in chirped-pulse amplification systems,” Opt. Lett.18(16), 1343–1345 (1993). [CrossRef] [PubMed]
  30. R. Trebino, K. W. De Long, D. N. Fittinghoff, J. N. Sweetser, M. A. Krumbügel, B. A. Richman, and D. J. Kane, “Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved gating,” Rev. Sci. Instrum.68(9), 3277–3295 (1997). [CrossRef]
  31. A. Baltuska, M. Überacker, E. Goulielmakis, R. Kienberger, V. S. Yakovlev, T. Udem, T. W. Hänsch, and F. Krausz, “Phase-controlled amplification of few-cycle laser pulses,” IEEE J Sel. Top. Quantum Electron.9(4), 972–989 (2003).
  32. G. Cerullo, A. Baltuska, O. D. Mücke, and C. Vozzi, “Few-optical-cycle light pulses with passive carrier-envelope phase stabilization,” Laser Photonics Rev.5(3), 323–351 (2011). [CrossRef]
  33. S. Pandelov, B. M. Pilles, J. C. Werhahn, and H. Iglev, “Time-resolved dynamics of the OH stretching vibration in aqueous NaCl hydrate,” J. Phys. Chem. A113(38), 10184–10188 (2009). [CrossRef] [PubMed]
  34. H. Graener, G. Seifert, and A. Laubereau, “Vibrational and reorientational dynamics of water molecules in liquid matrices,” Chem. Phys.175(1), 193–204 (1993). [CrossRef]
  35. H. J. Bakker, J. J. Gilijamse, and A. J. Lock, “Energy transfer in single hydrogen-bonded water molecules,” ChemPhysChem6(6), 1146–1156 (2005). [CrossRef] [PubMed]
  36. S. Woutersen, U. Emmerichs, H. K. Nienhuys, and H. J. Bakker, “Anomalous temperature dependence of vibrational lifetimes in water and ice,” Phys. Rev. Lett.81(5), 1106–1109 (1998). [CrossRef]
  37. H. Iglev, M. Schmeisser, K. Simeonidis, A. Thaller, and A. Laubereau, “Ultrafast superheating and melting of bulk ice,” Nature439(7073), 183–186 (2006). [CrossRef] [PubMed]
  38. 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(1), 013107 (2008). [CrossRef] [PubMed]
  39. U. Megerle, I. Pugliesi, C. Schriever, C. F. 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. B96(2-3), 215–231 (2009). [CrossRef]
  40. M. S. Lynch, K. M. Slenkamp, M. Cheng, and M. Khalil, “Coherent fifth-order visible-infrared spectroscopies: ultrafast nonequilibrium vibrational dynamics in solution,” J. Phys. Chem. A116(26), 7023–7032 (2012). [CrossRef] [PubMed]
  41. M. L. Groot, L. J. G. W. van Wilderen, and M. Di Donato, “Time-resolved methods in biophysics. 5. Femtosecond time-resolved and dispersed infrared spectroscopy on proteins,” Photochem. Photobiol. Sci.6(5), 501–507 (2007). [CrossRef] [PubMed]
  42. P. Hamm, R. A. Kaindl, and J. Stenger, “Noise suppression in femtosecond mid-infrared light sources,” Opt. Lett.25(24), 1798–1800 (2000). [CrossRef] [PubMed]
  43. Y. Deng, A. Schwarz, H. Fattahi, M. Ueffing, X. Gu, M. Ossiander, T. Metzger, V. Pervak, H. Ishizuki, T. Taira, T. Kobayashi, G. Marcus, F. Krausz, R. Kienberger, and N. Karpowicz, “Carrier-envelope-phase-stable, 1.2 mJ, 1.5 cycle laser pulses at 2.1 μm,” Opt. Lett.37(23), 4973–4975 (2012). [CrossRef] [PubMed]

Cited By

Alert me when this paper is cited

OSA is able to provide readers links to articles that cite this paper by participating in CrossRef's Cited-By Linking service. CrossRef includes content from more than 3000 publishers and societies. In addition to listing OSA journal articles that cite this paper, citing articles from other participating publishers will also be listed.

« Previous Article  |  Next Article »

OSA is a member of CrossRef.

CrossCheck Deposited