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Optics Express

Optics Express

  • Editor: Andrew M. Weiner
  • Vol. 21, Iss. 13 — Jul. 1, 2013
  • pp: 15904–15911

Precise phasing of 2D-electronic spectra in a fully non-collinear phase-matching geometry

Franz Milota, Craig N. Lincoln, and Jürgen Hauer  »View Author Affiliations

Optics Express, Vol. 21, Issue 13, pp. 15904-15911 (2013)

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We report an experimental design for two-dimensional electronic spectroscopy (2D-ES) that avoids the need to measure notoriously weak pump-probe spectra. Retaining a fully non-collinear folded boxcar geometry, the described layout replaces pump-probe with heterodyned transient grating (het-TG). The absorptive component of the het-TG signal is measured directly, following a straightforward optimization routine. The use of het-TG achieves an improvement in signal to noise ratio by almost two orders of magnitude. As a result, 2D-ES-signals down to 0.5% can be clearly resolved.

© 2013 OSA

OCIS Codes
(300.6290) Spectroscopy : Spectroscopy, four-wave mixing
(300.6300) Spectroscopy : Spectroscopy, Fourier transforms
(300.6530) Spectroscopy : Spectroscopy, ultrafast

ToC Category:

Original Manuscript: May 7, 2013
Revised Manuscript: June 5, 2013
Manuscript Accepted: June 7, 2013
Published: June 25, 2013

Franz Milota, Craig N. Lincoln, and Jürgen Hauer, "Precise phasing of 2D-electronic spectra in a fully non-collinear phase-matching geometry," Opt. Express 21, 15904-15911 (2013)

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  1. D. M. Jonas, “Two-dimensional femtosecond spectroscopy,” Annu. Rev. Phys. Chem.54(1), 425–463 (2003). [CrossRef] [PubMed]
  2. T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, “Two-dimensional spectroscopy of electronic couplings in photosynthesis,” Nature434(7033), 625–628 (2005). [CrossRef] [PubMed]
  3. K. W. Stone, K. Gundogdu, D. B. Turner, X. Q. Li, S. T. Cundiff, and K. A. Nelson, “Two-quantum 2D FT electronic spectroscopy of biexcitons in GaAs quantum wells,” Science324(5931), 1169–1173 (2009). [CrossRef] [PubMed]
  4. J. Sperling, A. Nemeth, J. Hauer, D. Abramavicius, S. Mukamel, H. F. Kauffmann, and F. Milota, “Excitons and disorder in molecular nanotubes: A 2D electronic spectroscopy study and first comparison to a microscopic model,” J. Phys. Chem. A114(32), 8179–8189 (2010). [CrossRef] [PubMed]
  5. T. Mančal, N. Christensson, V. Lukes, F. Milota, O. Bixner, H. F. Kauffmann, and J. Hauer, “System-dependent sgnatures of electronic and vibrational coherences in electronic two-dimensional spectra,” J. Phys. Chem. Lett.3(11), 1497–1502 (2012). [CrossRef]
  6. M. L. Cowan, J. P. Ogilvie, and R. J. D. Miller, “Two-dimensional spectroscopy using diffractive optics based phased-locked photon echoes,” Chem. Phys. Lett.386(1-3), 184–189 (2004). [CrossRef]
  7. A. A. Maznev, T. F. Crimmins, and K. A. Nelson, “How to make femtosecond pulses overlap,” Opt. Lett.23(17), 1378–1380 (1998). [CrossRef] [PubMed]
  8. T. H. Zhang, C. N. Borca, X. Q. Li, and S. T. Cundiff, “Optical two-dimensional Fourier transform spectroscopy with active interferometric stabilization,” Opt. Express13(19), 7432–7441 (2005). [CrossRef] [PubMed]
  9. U. Selig, F. Langhojer, F. Dimler, T. Löhrig, C. Schwarz, B. Gieseking, and T. Brixner, “Inherently phase-stable coherent two-dimensional spectroscopy using only conventional optics,” Opt. Lett.33(23), 2851–2853 (2008). [CrossRef] [PubMed]
  10. P. F. Tian, D. Keusters, Y. Suzaki, and W. S. Warren, “Femtosecond phase-coherent two-dimensional spectroscopy,” Science300(5625), 1553–1555 (2003). [CrossRef] [PubMed]
  11. 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]
  12. J. A. Myers, K. L. M. Lewis, P. F. Tekavec, and J. P. Ogilvie, “Two-color two-dimensional Fourier transform electronic spectroscopy with a pulse-shaper,” Opt. Express16(22), 17420–17428 (2008). [CrossRef] [PubMed]
  13. D. B. Turner, K. W. Stone, K. Gundogdu, and K. A. Nelson, “The coherent optical laser beam recombination technique (COLBERT) spectrometer: Coherent multidimensional spectroscopy made easier,” (Invited) Rev. Sci. Instrum.82(8), 081301 (2011). [CrossRef] [PubMed]
  14. D. Karaiskaj, A. D. Bristow, L. J. Yang, X. C. Dai, R. P. Mirin, S. Mukamel, and S. T. Cundiff, “Two-quantum many-body coherences in two-dimensional Fourier-transform spectra of exciton resonances in semiconductor quantum wells,” Phys. Rev. Lett.104(11), 117401 (2010). [CrossRef] [PubMed]
  15. N. Christensson, F. Milota, A. Nemeth, I. Pugliesi, E. Riedle, J. Sperling, T. Pullerits, H. Kauffmann, and J. Hauer, “Electronic Double-quantum coherences and their impact on ultrafast spectroscopy: The example of beta-carotene,” J. Phys. Chem. Lett.1(23), 3366–3370 (2010). [CrossRef]
  16. D. Abramavicius, A. Nemeth, F. Milota, J. Sperling, S. Mukamel, and H. F. Kauffmann, “Weak exciton scattering in molecular nanotubes revealed by double-quantum two-dimensional electronic spectroscopy,” Phys. Rev. Lett.108(6), 067401 (2012). [CrossRef] [PubMed]
  17. M. Khalil, N. Demirdöven, and A. Tokmakoff, “Obtaining absorptive line shapes in two-dimensional infrared vibrational correlation spectra,” Phys. Rev. Lett.90(4), 047401 (2003). [CrossRef] [PubMed]
  18. W. T. Pollard and R. A. Mathies, “Analysis of femtosecond dynamic absorption spectra of nonstationary states,” Annu. Rev. Phys. Chem.43(1), 497–523 (1992). [CrossRef] [PubMed]
  19. 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(9), 1289–1291 (2006). [CrossRef] [PubMed]
  20. A. Nemeth, J. Sperling, J. Hauer, H. F. Kauffmann, and F. Milota, “Compact phase-stable design for single- and double-quantum two-dimensional electronic spectroscopy,” Opt. Lett.34(21), 3301–3303 (2009). [CrossRef] [PubMed]
  21. T. Brixner, T. Mancal, I. V. Stiopkin, and G. R. Fleming, “Phase-stabilized two-dimensional electronic spectroscopy,” J. Chem. Phys.121(9), 4221–4236 (2004). [CrossRef] [PubMed]
  22. 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]
  23. J. P. Ogilvie, M. Plazanet, G. Dadusc, and R. J. D. Miller, “Dynamics of ligand escape in myoglobin: Q- band transient absorption and four-wave mixing studies,” J. Phys. Chem. B106(40), 10460–10467 (2002). [CrossRef]
  24. F. Milota, V. I. Prokhorenko, T. Mancal, H. von Berlepsch, O. Bixner, H. F. Kauffmann, and J. Hauer, “Vibronic and vibrational coherences in two-dimensional electronic spectra of supramolecular J-aggregates,” J. Phys. Chem. A130318064008000 (2013), doi:. [CrossRef] [PubMed]
  25. B. Cho, M. K. Yetzbacher, K. A. Kitney, E. R. Smith, and D. M. Jonas, “Propagation and beam geometry effects on two-dimensional Fourier transform spectra of multilevel systems,” J. Phys. Chem. A113(47), 13287–13299 (2009). [CrossRef] [PubMed]

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