Abstract

Wavelength-tunable 100fs pulses generated through the soliton self-frequency shift in a photonic-crystal fiber are employed to visualize femtosecond coherence and population relaxation dynamics in molecular aggregates by means of time-resolved sum-frequency generation. This technique reveals an ultrafast dephasing of coherent molecular excitations with a phase relaxation time of about 120fs and resolves an ultrafast switching of the nonlinear-optical response of molecular aggregates.

© 2006 Optical Society of America

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2006

2005

2004

S. O. Konorov, D. A. Akimov, E. E. Serebryannikov, A. A. Ivanov, M. V. Alfimov, and A. M. Zheltikov, Phys. Rev. E 70, 057601 (2004).
[CrossRef]

2003

2002

Th. Udem, R. Holzwarth, and T. W. Hänsch, Nature 416, 233 (2002).
[CrossRef] [PubMed]

2001

2000

1993

J. Knoester, Phys. Rev. A 47, 2083 (1993).
[CrossRef] [PubMed]

1989

F. C. Spano and S. Mukamel, Phys. Rev. A 40, 5783 (1989).
[CrossRef] [PubMed]

Agrawal, G. P.

G. P. Agrawal, Nonlinear Fiber Optics (Academic, 2001).

Akimov, D. A.

Alfimov, M. V.

S. O. Konorov, D. A. Akimov, E. E. Serebryannikov, A. A. Ivanov, M. V. Alfimov, and A. M. Zheltikov, Phys. Rev. E 70, 057601 (2004).
[CrossRef]

Andresen, E. R.

Baltuska, A.

Biancalana, F.

W. H. Reeves, D. V. Skryabin, F. Biancalana, J. C. Knight, P. St. J. Russell, F. G. Omenetto, A. Efimov, and A. J. Taylor, Nature 424, 511 (2003).
[CrossRef] [PubMed]

Birkedal, V.

Chudoba, C.

Dukel'skii, K. V.

Efimov, A.

W. H. Reeves, D. V. Skryabin, F. Biancalana, J. C. Knight, P. St. J. Russell, F. G. Omenetto, A. Efimov, and A. J. Taylor, Nature 424, 511 (2003).
[CrossRef] [PubMed]

Fuji, T.

Fujimoto, J. G.

Hamaguchi, H.

Hänsch, T. W.

Th. Udem, R. Holzwarth, and T. W. Hänsch, Nature 416, 233 (2002).
[CrossRef] [PubMed]

Hartl, I.

Hilligsøe, K. M.

Holzwarth, R.

Ishii, N.

Ivanov, A. A.

S. O. Konorov, D. A. Akimov, E. E. Serebryannikov, A. A. Ivanov, M. V. Alfimov, and A. M. Zheltikov, Phys. Rev. E 70, 057601 (2004).
[CrossRef]

Kannari, F.

Kano, H.

Keiding, S. R.

Kiefer, W.

Knight, J. C.

W. H. Reeves, D. V. Skryabin, F. Biancalana, J. C. Knight, P. St. J. Russell, F. G. Omenetto, A. Efimov, and A. J. Taylor, Nature 424, 511 (2003).
[CrossRef] [PubMed]

J. C. Knight, Nature 424, 847 (2003).
[CrossRef] [PubMed]

Knoester, J.

J. Knoester, Phys. Rev. A 47, 2083 (1993).
[CrossRef] [PubMed]

Ko, T. H.

Kobayashi, K.

Köhler, S.

Kondrat'ev, Yu. N.

Konorov, S. O.

S. O. Konorov, D. A. Akimov, E. E. Serebryannikov, A. A. Ivanov, M. V. Alfimov, and A. M. Zheltikov, Phys. Rev. E 70, 057601 (2004).
[CrossRef]

Krausz, F.

Larsen, J. J.

Li, X. D.

Maksimenka, R.

Metzger, T.

Miura, T.

Mukamel, S.

F. C. Spano and S. Mukamel, Phys. Rev. A 40, 5783 (1989).
[CrossRef] [PubMed]

Omenetto, F. G.

W. H. Reeves, D. V. Skryabin, F. Biancalana, J. C. Knight, P. St. J. Russell, F. G. Omenetto, A. Efimov, and A. J. Taylor, Nature 424, 511 (2003).
[CrossRef] [PubMed]

Paulsen, H. N.

Ranka, J. K.

Reeves, W. H.

W. H. Reeves, D. V. Skryabin, F. Biancalana, J. C. Knight, P. St. J. Russell, F. G. Omenetto, A. Efimov, and A. J. Taylor, Nature 424, 511 (2003).
[CrossRef] [PubMed]

Rhanta, R. K.

Russell, P. St. J.

W. H. Reeves, D. V. Skryabin, F. Biancalana, J. C. Knight, P. St. J. Russell, F. G. Omenetto, A. Efimov, and A. J. Taylor, Nature 424, 511 (2003).
[CrossRef] [PubMed]

P. St. J. Russell, Science 299, 358 (2003).
[CrossRef] [PubMed]

Schmitt, M.

Serebryannikov, E. E.

Shevandin, V. S.

Sidorov-Biryukov, D. A.

Skryabin, D. V.

W. H. Reeves, D. V. Skryabin, F. Biancalana, J. C. Knight, P. St. J. Russell, F. G. Omenetto, A. Efimov, and A. J. Taylor, Nature 424, 511 (2003).
[CrossRef] [PubMed]

Spano, F. C.

F. C. Spano and S. Mukamel, Phys. Rev. A 40, 5783 (1989).
[CrossRef] [PubMed]

Stentz, A. J.

Takasago, K.

Taylor, A. J.

W. H. Reeves, D. V. Skryabin, F. Biancalana, J. C. Knight, P. St. J. Russell, F. G. Omenetto, A. Efimov, and A. J. Taylor, Nature 424, 511 (2003).
[CrossRef] [PubMed]

Teisset, C. Y.

Thøgersen, J.

Torizuka, K.

Udem, Th.

Th. Udem, R. Holzwarth, and T. W. Hänsch, Nature 416, 233 (2002).
[CrossRef] [PubMed]

Windeler, R. S.

Zhang, Z.

Zheltikov, A. M.

J. Opt. Soc. Am. B

Nature

J. C. Knight, Nature 424, 847 (2003).
[CrossRef] [PubMed]

W. H. Reeves, D. V. Skryabin, F. Biancalana, J. C. Knight, P. St. J. Russell, F. G. Omenetto, A. Efimov, and A. J. Taylor, Nature 424, 511 (2003).
[CrossRef] [PubMed]

Th. Udem, R. Holzwarth, and T. W. Hänsch, Nature 416, 233 (2002).
[CrossRef] [PubMed]

Opt. Express

Opt. Lett.

Phys. Rev. A

F. C. Spano and S. Mukamel, Phys. Rev. A 40, 5783 (1989).
[CrossRef] [PubMed]

J. Knoester, Phys. Rev. A 47, 2083 (1993).
[CrossRef] [PubMed]

Phys. Rev. E

S. O. Konorov, D. A. Akimov, E. E. Serebryannikov, A. A. Ivanov, M. V. Alfimov, and A. M. Zheltikov, Phys. Rev. E 70, 057601 (2004).
[CrossRef]

Science

P. St. J. Russell, Science 299, 358 (2003).
[CrossRef] [PubMed]

Other

G. P. Agrawal, Nonlinear Fiber Optics (Academic, 2001).

T.Kobayashi, ed., J-aggregates (World Scientific, 1996).

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Figures (2)

Fig. 1
Fig. 1

Curve 1, spectrum of the amplified fundamental-wavelength output of the Cr:forsterite laser; 2, spectrum of the frequency-shifted soliton output of the first-type PCF; 3, absorption spectrum of a thin-film sample of molecular aggregates. Inset, SEM image of the PCF.

Fig. 2
Fig. 2

Time-resolved SFG measurements with solitonic output of the PCF. Filled circles, power of the sum-frequency signal generated in a silica plate by amplified Cr:forsterite laser pulses, frequency-shifted pulses from the photonic-crystal fiber, and time-delayed unamplified pulses of the Cr:forsterite laser measured as a function of the delay time between the pulses (cross-correlation trace). Rectangles, power P sf of the sum-frequency signal from a molecular aggregate film measured as a function of the delay time τ between the probe pulse and the pulses providing a TPA-resonant coherent excitation of aggregates. Crosses, fit of the experimental data with the use of expressions for P sf and Q with the dephasing time T 2 = 120 fs and pulse widths θ 1 = θ 2 = 100 fs . Open circles, inverted dependence of the sum-frequency signal from a molecular aggregate film on the delay time between the excitation second-harmonic pulse and the light pulses involved in SFG. Inset 1, chemical structure of thiacarbocyanine dye. Inset 2, diagram of SFG ω sf = 2 ω 1 + ω 2 with a TPA resonance at ω 1 + ω 2 and a time-delayed probe pulse.

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