Abstract

We report a novel Fourier transform method for measuring two-photon excitation spectra. We demonstrate this method using simple dye molecules and discuss its applications in two-photon fluorescence microscopy and optimal control. This method facilitates an intuitive interpretation of recent control experiments in terms of tuning the nonlinear spectrum of the exciting laser source.

© 2005 Optical Society of America

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    [CrossRef] [PubMed]
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2004 (1)

2003 (3)

T. Brixner, N. H. Damrauer, B. Kiefer, and G. Gerber, J. Chem. Phys. 118, 3692 (2003).
[CrossRef]

V. V. Lozovoy, I. Pastirk, K. A. Walowicz, and M. Dantus, J. Chem. Phys. 118, 3187 (2003).
[CrossRef]

D. M. Jonas, Annu. Rev. Phys. Chem. 54, 425 (2003).
[CrossRef]

2002 (3)

F. Bestvater, E. Spiess, G. Stobrawa, M. Hacker, T. Feurer, T. Porwol, U. Berchner-Pfannschmidt, C. Wotzlaw, and H. Acker, J. Microsc. 208, 108 (2002).
[CrossRef] [PubMed]

N. Dudovich, D. Oron, and Y. Silberberg, Nature 418, 512 (2002).
[CrossRef] [PubMed]

K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, J. Phys. Chem. A 106, 9369 (2002).
[CrossRef]

2001 (2)

T. Brixner, N. H. Damrauer, P. Niklaus, and G. Gerber, Nature 414, 57 (2001).
[CrossRef] [PubMed]

D. Zeidler, S. Frey, K. L. Kompa, and M. Motzkus, Phys. Rev. A 64, 023420 (2001).
[CrossRef]

1998 (2)

D. Meshulach and Y. Silberberg, Nature 396, 239 (1998).
[CrossRef]

M. A. Albota, C. Xu, and W. Webb, Appl. Opt. 37, 7352 (1998).
[CrossRef]

1997 (4)

1996 (1)

1995 (1)

1992 (2)

B. Broers, L. D. Noordam, and H. B. van Linden van den Heuvell, Phys. Rev. A 46, 2749 (1992).
[CrossRef] [PubMed]

R. S. Judson and H. Rabitz, Phys. Rev. Lett. 68, 1500 (1992).
[CrossRef] [PubMed]

1989 (1)

K. Naganuma, K. Mogi, and H. Yamada, IEEE J. Quantum Electron. 25, 1225 (1989).
[CrossRef]

1978 (1)

M. M. Salour, Rev. Mod. Phys. 50, 667 (1978).
[CrossRef]

Acker, H.

F. Bestvater, E. Spiess, G. Stobrawa, M. Hacker, T. Feurer, T. Porwol, U. Berchner-Pfannschmidt, C. Wotzlaw, and H. Acker, J. Microsc. 208, 108 (2002).
[CrossRef] [PubMed]

Albota, M. A.

Baltuska, A.

Bartoli, A.

Bellini, M.

Berchner-Pfannschmidt, U.

F. Bestvater, E. Spiess, G. Stobrawa, M. Hacker, T. Feurer, T. Porwol, U. Berchner-Pfannschmidt, C. Wotzlaw, and H. Acker, J. Microsc. 208, 108 (2002).
[CrossRef] [PubMed]

Bestvater, F.

F. Bestvater, E. Spiess, G. Stobrawa, M. Hacker, T. Feurer, T. Porwol, U. Berchner-Pfannschmidt, C. Wotzlaw, and H. Acker, J. Microsc. 208, 108 (2002).
[CrossRef] [PubMed]

Blanchet, V.

V. Blanchet, C. Nicole, M.-A. Bouchene, and B. Girard, Phys. Rev. Lett. 78, 2716 (1997).
[CrossRef]

Bouchene, M.-A.

V. Blanchet, C. Nicole, M.-A. Bouchene, and B. Girard, Phys. Rev. Lett. 78, 2716 (1997).
[CrossRef]

Brixner, T.

T. Brixner, N. H. Damrauer, B. Kiefer, and G. Gerber, J. Chem. Phys. 118, 3692 (2003).
[CrossRef]

T. Brixner, N. H. Damrauer, P. Niklaus, and G. Gerber, Nature 414, 57 (2001).
[CrossRef] [PubMed]

Broers, B.

B. Broers, L. D. Noordam, and H. B. van Linden van den Heuvell, Phys. Rev. A 46, 2749 (1992).
[CrossRef] [PubMed]

Chen, J.

Damrauer, N. H.

T. Brixner, N. H. Damrauer, B. Kiefer, and G. Gerber, J. Chem. Phys. 118, 3692 (2003).
[CrossRef]

T. Brixner, N. H. Damrauer, P. Niklaus, and G. Gerber, Nature 414, 57 (2001).
[CrossRef] [PubMed]

Dantus, M.

V. V. Lozovoy, I. Pastirk, K. A. Walowicz, and M. Dantus, J. Chem. Phys. 118, 3187 (2003).
[CrossRef]

K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, J. Phys. Chem. A 106, 9369 (2002).
[CrossRef]

Denk, W.

Dudovich, N.

N. Dudovich, D. Oron, and Y. Silberberg, Nature 418, 512 (2002).
[CrossRef] [PubMed]

Feurer, T.

F. Bestvater, E. Spiess, G. Stobrawa, M. Hacker, T. Feurer, T. Porwol, U. Berchner-Pfannschmidt, C. Wotzlaw, and H. Acker, J. Microsc. 208, 108 (2002).
[CrossRef] [PubMed]

Frey, S.

D. Zeidler, S. Frey, K. L. Kompa, and M. Motzkus, Phys. Rev. A 64, 023420 (2001).
[CrossRef]

Gaeta, A. L.

Gerber, G.

T. Brixner, N. H. Damrauer, B. Kiefer, and G. Gerber, J. Chem. Phys. 118, 3692 (2003).
[CrossRef]

T. Brixner, N. H. Damrauer, P. Niklaus, and G. Gerber, Nature 414, 57 (2001).
[CrossRef] [PubMed]

Girard, B.

V. Blanchet, C. Nicole, M.-A. Bouchene, and B. Girard, Phys. Rev. Lett. 78, 2716 (1997).
[CrossRef]

Guild, J.

Hacker, M.

F. Bestvater, E. Spiess, G. Stobrawa, M. Hacker, T. Feurer, T. Porwol, U. Berchner-Pfannschmidt, C. Wotzlaw, and H. Acker, J. Microsc. 208, 108 (2002).
[CrossRef] [PubMed]

Hansch, T. W.

Jonas, D. M.

D. M. Jonas, Annu. Rev. Phys. Chem. 54, 425 (2003).
[CrossRef]

Judson, R. S.

R. S. Judson and H. Rabitz, Phys. Rev. Lett. 68, 1500 (1992).
[CrossRef] [PubMed]

Kannari, F.

Kawano, H.

Kiefer, B.

T. Brixner, N. H. Damrauer, B. Kiefer, and G. Gerber, J. Chem. Phys. 118, 3692 (2003).
[CrossRef]

Kompa, K. L.

D. Zeidler, S. Frey, K. L. Kompa, and M. Motzkus, Phys. Rev. A 64, 023420 (2001).
[CrossRef]

Lozovoy, V. V.

V. V. Lozovoy, I. Pastirk, K. A. Walowicz, and M. Dantus, J. Chem. Phys. 118, 3187 (2003).
[CrossRef]

K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, J. Phys. Chem. A 106, 9369 (2002).
[CrossRef]

Meshulach, D.

D. Meshulach and Y. Silberberg, Nature 396, 239 (1998).
[CrossRef]

Midorikawa, K.

Miyawaki, A.

Mizuno, H.

Mogi, K.

K. Naganuma, K. Mogi, and H. Yamada, IEEE J. Quantum Electron. 25, 1225 (1989).
[CrossRef]

Motzkus, M.

D. Zeidler, S. Frey, K. L. Kompa, and M. Motzkus, Phys. Rev. A 64, 023420 (2001).
[CrossRef]

Nabekawa, Y.

Naganuma, K.

K. Naganuma, K. Mogi, and H. Yamada, IEEE J. Quantum Electron. 25, 1225 (1989).
[CrossRef]

Nicole, C.

V. Blanchet, C. Nicole, M.-A. Bouchene, and B. Girard, Phys. Rev. Lett. 78, 2716 (1997).
[CrossRef]

Niklaus, P.

T. Brixner, N. H. Damrauer, P. Niklaus, and G. Gerber, Nature 414, 57 (2001).
[CrossRef] [PubMed]

Noordam, L. D.

B. Broers, L. D. Noordam, and H. B. van Linden van den Heuvell, Phys. Rev. A 46, 2749 (1992).
[CrossRef] [PubMed]

Oron, D.

N. Dudovich, D. Oron, and Y. Silberberg, Nature 418, 512 (2002).
[CrossRef] [PubMed]

Pastirk, I.

V. V. Lozovoy, I. Pastirk, K. A. Walowicz, and M. Dantus, J. Chem. Phys. 118, 3187 (2003).
[CrossRef]

K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, J. Phys. Chem. A 106, 9369 (2002).
[CrossRef]

Porwol, T.

F. Bestvater, E. Spiess, G. Stobrawa, M. Hacker, T. Feurer, T. Porwol, U. Berchner-Pfannschmidt, C. Wotzlaw, and H. Acker, J. Microsc. 208, 108 (2002).
[CrossRef] [PubMed]

Pshenichnikov, M. S.

Rabitz, H.

R. S. Judson and H. Rabitz, Phys. Rev. Lett. 68, 1500 (1992).
[CrossRef] [PubMed]

Ranka, J. K.

Salour, M. M.

M. M. Salour, Rev. Mod. Phys. 50, 667 (1978).
[CrossRef]

Silberberg, Y.

N. Dudovich, D. Oron, and Y. Silberberg, Nature 418, 512 (2002).
[CrossRef] [PubMed]

D. Meshulach and Y. Silberberg, Nature 396, 239 (1998).
[CrossRef]

Spiess, E.

F. Bestvater, E. Spiess, G. Stobrawa, M. Hacker, T. Feurer, T. Porwol, U. Berchner-Pfannschmidt, C. Wotzlaw, and H. Acker, J. Microsc. 208, 108 (2002).
[CrossRef] [PubMed]

Stobrawa, G.

F. Bestvater, E. Spiess, G. Stobrawa, M. Hacker, T. Feurer, T. Porwol, U. Berchner-Pfannschmidt, C. Wotzlaw, and H. Acker, J. Microsc. 208, 108 (2002).
[CrossRef] [PubMed]

Tanabe, T.

Tournois, P.

P. Tournois, Opt. Commun. 140, 245 (1997).
[CrossRef]

van Linden van den Heuvell, H. B.

B. Broers, L. D. Noordam, and H. B. van Linden van den Heuvell, Phys. Rev. A 46, 2749 (1992).
[CrossRef] [PubMed]

Walowicz, K. A.

V. V. Lozovoy, I. Pastirk, K. A. Walowicz, and M. Dantus, J. Chem. Phys. 118, 3187 (2003).
[CrossRef]

K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, J. Phys. Chem. A 106, 9369 (2002).
[CrossRef]

Webb, W.

Wiersma, D. A.

Wotzlaw, C.

F. Bestvater, E. Spiess, G. Stobrawa, M. Hacker, T. Feurer, T. Porwol, U. Berchner-Pfannschmidt, C. Wotzlaw, and H. Acker, J. Microsc. 208, 108 (2002).
[CrossRef] [PubMed]

Xu, C.

Yamada, H.

K. Naganuma, K. Mogi, and H. Yamada, IEEE J. Quantum Electron. 25, 1225 (1989).
[CrossRef]

Zeidler, D.

D. Zeidler, S. Frey, K. L. Kompa, and M. Motzkus, Phys. Rev. A 64, 023420 (2001).
[CrossRef]

Annu. Rev. Phys. Chem. (1)

D. M. Jonas, Annu. Rev. Phys. Chem. 54, 425 (2003).
[CrossRef]

Appl. Opt. (1)

IEEE J. Quantum Electron. (1)

K. Naganuma, K. Mogi, and H. Yamada, IEEE J. Quantum Electron. 25, 1225 (1989).
[CrossRef]

J. Chem. Phys. (2)

T. Brixner, N. H. Damrauer, B. Kiefer, and G. Gerber, J. Chem. Phys. 118, 3692 (2003).
[CrossRef]

V. V. Lozovoy, I. Pastirk, K. A. Walowicz, and M. Dantus, J. Chem. Phys. 118, 3187 (2003).
[CrossRef]

J. Microsc. (1)

F. Bestvater, E. Spiess, G. Stobrawa, M. Hacker, T. Feurer, T. Porwol, U. Berchner-Pfannschmidt, C. Wotzlaw, and H. Acker, J. Microsc. 208, 108 (2002).
[CrossRef] [PubMed]

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

J. Phys. Chem. A (1)

K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, J. Phys. Chem. A 106, 9369 (2002).
[CrossRef]

Nature (3)

N. Dudovich, D. Oron, and Y. Silberberg, Nature 418, 512 (2002).
[CrossRef] [PubMed]

D. Meshulach and Y. Silberberg, Nature 396, 239 (1998).
[CrossRef]

T. Brixner, N. H. Damrauer, P. Niklaus, and G. Gerber, Nature 414, 57 (2001).
[CrossRef] [PubMed]

Opt. Commun. (1)

P. Tournois, Opt. Commun. 140, 245 (1997).
[CrossRef]

Opt. Express (1)

Opt. Lett. (3)

Phys. Rev. A (2)

D. Zeidler, S. Frey, K. L. Kompa, and M. Motzkus, Phys. Rev. A 64, 023420 (2001).
[CrossRef]

B. Broers, L. D. Noordam, and H. B. van Linden van den Heuvell, Phys. Rev. A 46, 2749 (1992).
[CrossRef] [PubMed]

Phys. Rev. Lett. (2)

R. S. Judson and H. Rabitz, Phys. Rev. Lett. 68, 1500 (1992).
[CrossRef] [PubMed]

V. Blanchet, C. Nicole, M.-A. Bouchene, and B. Girard, Phys. Rev. Lett. 78, 2716 (1997).
[CrossRef]

Rev. Mod. Phys. (1)

M. M. Salour, Rev. Mod. Phys. 50, 667 (1978).
[CrossRef]

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Figures (3)

Fig. 1
Fig. 1

Experimental setup for Fourier transform measurements of TPE spectra (Dazzler present for the control and pulse-shaping measurements only). DBSs, dichroic beam splitters; PBS, polarizing beam splitter; BS, beam splitter; DC, dispersion compensation (to balance dispersion after the BS); L 1 , f = 15 cm lens; L 2 ’s, f = 5 cm lenses; PMT, photomultiplier tube; Ti:Sapph, Ti:sapphire.

Fig. 2
Fig. 2

(a) 2 ω 0 components of the Fourier transforms of the second-order IACs recorded with the two-photon diode (solid curve) and the fluorescence of Coumarin 460 (crosses) and Rhodamine 590 (open circles). (b) Recovered TPEs—Coumarin 460 (crosses), Rhodamine 590 (open circles)—and their one-photon absorption spectra—Coumarin 460 (solid curve), Rhodamine 590 (dashed curve).

Fig. 3
Fig. 3

Comparison of the SH spectrum of the transform-limited pulse (solid curve) and the measured (open circles) and calculated (dashed curve) SH spectra for the optimal pulse found in Coumarin 460 by the GA search. Inset, spectral amplitude (solid curve) and first derivative of the spectral phase (dashed curve) of the optimal pulse.

Equations (1)

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E ( 2 ) ( ω ) 2 E ( ω ) E ( ω ω ) exp { i [ φ ( ω ) + φ ( ω ω ) ] } d ω 2 ,

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