Abstract

A novel transient scattering technique is proposed for femtosecond dephasing time measurements. This technique provides several advantages compared with existing techniques for time-domain dephasing measurements, including resolution below the pulse width, insensitivity to rapid energy relaxation, and clear demarcation between homogeneous and inhomogeneous broadening. We report experimental results for the dye Nile blue in solution; the dephasing time T2 is determined to be less than 20 fsec.

© 1984 Optical Society of America

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  1. T. Yajima, Y. Taira, J. Phys. Soc. Jpn. 47, 1620 (1979).
    [CrossRef]
  2. T. Yajima, Y. Ishida, Y. Taira, Picosecond Phenomena II, R. M. Hochstrasser, W. Kaiser, C. V. Shank, eds. (Springer-Verlag, New York, 1980), p. 190.
    [CrossRef]
  3. J. G. Fujimoto, E. P. Ippen, Opt. Lett. 8, 446 (1983).
    [CrossRef] [PubMed]
  4. H. Eichler, G. Salje, H. Stahl, J. Appl. Phys. 44, 5383 (1973).
    [CrossRef]
  5. D. W. Phillion, D. J. Kuizenga, A. E. Siegman, Appl. Phys. Lett. 27, 85 (1975).
    [CrossRef]
  6. A. L. Smirl, T. F. Boggess, B. S. Wherrett, G. P. Perryman, A. Miller, IEEE J. Quantum Electron. QE-19, 690 (1983).
    [CrossRef]
  7. R. L. Fork, B. I. Greene, C. V. Shank, Appl. Phys. Lett. 38, 671 (1981).
    [CrossRef]
  8. J. M. Wiesenfeld, E. P. Ippen, Chem. Phys. Lett. 67, 213 (1979).
    [CrossRef]
  9. T. Mossberg, A. Flusberg, R. Kachru, S. R. Hartmann, Phys. Rev. Lett. 42, 1665 (1979).
    [CrossRef]
  10. H. J. Eichler, U. Klein, D. Langhans, Appl. Phys. 21, 215 (1980).
    [CrossRef]
  11. J. A. Shirley, R. J. Hall, A. C. Eckbreth, Opt. Lett. 5, 380 (1980).
    [CrossRef] [PubMed]
  12. J. J. Song, J. H. Lee, M. D. Levenson, Phys. Rev. A 17, 1439 (1978).
    [CrossRef]

1983 (2)

J. G. Fujimoto, E. P. Ippen, Opt. Lett. 8, 446 (1983).
[CrossRef] [PubMed]

A. L. Smirl, T. F. Boggess, B. S. Wherrett, G. P. Perryman, A. Miller, IEEE J. Quantum Electron. QE-19, 690 (1983).
[CrossRef]

1981 (1)

R. L. Fork, B. I. Greene, C. V. Shank, Appl. Phys. Lett. 38, 671 (1981).
[CrossRef]

1980 (2)

H. J. Eichler, U. Klein, D. Langhans, Appl. Phys. 21, 215 (1980).
[CrossRef]

J. A. Shirley, R. J. Hall, A. C. Eckbreth, Opt. Lett. 5, 380 (1980).
[CrossRef] [PubMed]

1979 (3)

J. M. Wiesenfeld, E. P. Ippen, Chem. Phys. Lett. 67, 213 (1979).
[CrossRef]

T. Mossberg, A. Flusberg, R. Kachru, S. R. Hartmann, Phys. Rev. Lett. 42, 1665 (1979).
[CrossRef]

T. Yajima, Y. Taira, J. Phys. Soc. Jpn. 47, 1620 (1979).
[CrossRef]

1978 (1)

J. J. Song, J. H. Lee, M. D. Levenson, Phys. Rev. A 17, 1439 (1978).
[CrossRef]

1975 (1)

D. W. Phillion, D. J. Kuizenga, A. E. Siegman, Appl. Phys. Lett. 27, 85 (1975).
[CrossRef]

1973 (1)

H. Eichler, G. Salje, H. Stahl, J. Appl. Phys. 44, 5383 (1973).
[CrossRef]

Boggess, T. F.

A. L. Smirl, T. F. Boggess, B. S. Wherrett, G. P. Perryman, A. Miller, IEEE J. Quantum Electron. QE-19, 690 (1983).
[CrossRef]

Eckbreth, A. C.

Eichler, H.

H. Eichler, G. Salje, H. Stahl, J. Appl. Phys. 44, 5383 (1973).
[CrossRef]

Eichler, H. J.

H. J. Eichler, U. Klein, D. Langhans, Appl. Phys. 21, 215 (1980).
[CrossRef]

Flusberg, A.

T. Mossberg, A. Flusberg, R. Kachru, S. R. Hartmann, Phys. Rev. Lett. 42, 1665 (1979).
[CrossRef]

Fork, R. L.

R. L. Fork, B. I. Greene, C. V. Shank, Appl. Phys. Lett. 38, 671 (1981).
[CrossRef]

Fujimoto, J. G.

Greene, B. I.

R. L. Fork, B. I. Greene, C. V. Shank, Appl. Phys. Lett. 38, 671 (1981).
[CrossRef]

Hall, R. J.

Hartmann, S. R.

T. Mossberg, A. Flusberg, R. Kachru, S. R. Hartmann, Phys. Rev. Lett. 42, 1665 (1979).
[CrossRef]

Ippen, E. P.

J. G. Fujimoto, E. P. Ippen, Opt. Lett. 8, 446 (1983).
[CrossRef] [PubMed]

J. M. Wiesenfeld, E. P. Ippen, Chem. Phys. Lett. 67, 213 (1979).
[CrossRef]

Ishida, Y.

T. Yajima, Y. Ishida, Y. Taira, Picosecond Phenomena II, R. M. Hochstrasser, W. Kaiser, C. V. Shank, eds. (Springer-Verlag, New York, 1980), p. 190.
[CrossRef]

Kachru, R.

T. Mossberg, A. Flusberg, R. Kachru, S. R. Hartmann, Phys. Rev. Lett. 42, 1665 (1979).
[CrossRef]

Klein, U.

H. J. Eichler, U. Klein, D. Langhans, Appl. Phys. 21, 215 (1980).
[CrossRef]

Kuizenga, D. J.

D. W. Phillion, D. J. Kuizenga, A. E. Siegman, Appl. Phys. Lett. 27, 85 (1975).
[CrossRef]

Langhans, D.

H. J. Eichler, U. Klein, D. Langhans, Appl. Phys. 21, 215 (1980).
[CrossRef]

Lee, J. H.

J. J. Song, J. H. Lee, M. D. Levenson, Phys. Rev. A 17, 1439 (1978).
[CrossRef]

Levenson, M. D.

J. J. Song, J. H. Lee, M. D. Levenson, Phys. Rev. A 17, 1439 (1978).
[CrossRef]

Miller, A.

A. L. Smirl, T. F. Boggess, B. S. Wherrett, G. P. Perryman, A. Miller, IEEE J. Quantum Electron. QE-19, 690 (1983).
[CrossRef]

Mossberg, T.

T. Mossberg, A. Flusberg, R. Kachru, S. R. Hartmann, Phys. Rev. Lett. 42, 1665 (1979).
[CrossRef]

Perryman, G. P.

A. L. Smirl, T. F. Boggess, B. S. Wherrett, G. P. Perryman, A. Miller, IEEE J. Quantum Electron. QE-19, 690 (1983).
[CrossRef]

Phillion, D. W.

D. W. Phillion, D. J. Kuizenga, A. E. Siegman, Appl. Phys. Lett. 27, 85 (1975).
[CrossRef]

Salje, G.

H. Eichler, G. Salje, H. Stahl, J. Appl. Phys. 44, 5383 (1973).
[CrossRef]

Shank, C. V.

R. L. Fork, B. I. Greene, C. V. Shank, Appl. Phys. Lett. 38, 671 (1981).
[CrossRef]

Shirley, J. A.

Siegman, A. E.

D. W. Phillion, D. J. Kuizenga, A. E. Siegman, Appl. Phys. Lett. 27, 85 (1975).
[CrossRef]

Smirl, A. L.

A. L. Smirl, T. F. Boggess, B. S. Wherrett, G. P. Perryman, A. Miller, IEEE J. Quantum Electron. QE-19, 690 (1983).
[CrossRef]

Song, J. J.

J. J. Song, J. H. Lee, M. D. Levenson, Phys. Rev. A 17, 1439 (1978).
[CrossRef]

Stahl, H.

H. Eichler, G. Salje, H. Stahl, J. Appl. Phys. 44, 5383 (1973).
[CrossRef]

Taira, Y.

T. Yajima, Y. Taira, J. Phys. Soc. Jpn. 47, 1620 (1979).
[CrossRef]

T. Yajima, Y. Ishida, Y. Taira, Picosecond Phenomena II, R. M. Hochstrasser, W. Kaiser, C. V. Shank, eds. (Springer-Verlag, New York, 1980), p. 190.
[CrossRef]

Wherrett, B. S.

A. L. Smirl, T. F. Boggess, B. S. Wherrett, G. P. Perryman, A. Miller, IEEE J. Quantum Electron. QE-19, 690 (1983).
[CrossRef]

Wiesenfeld, J. M.

J. M. Wiesenfeld, E. P. Ippen, Chem. Phys. Lett. 67, 213 (1979).
[CrossRef]

Yajima, T.

T. Yajima, Y. Taira, J. Phys. Soc. Jpn. 47, 1620 (1979).
[CrossRef]

T. Yajima, Y. Ishida, Y. Taira, Picosecond Phenomena II, R. M. Hochstrasser, W. Kaiser, C. V. Shank, eds. (Springer-Verlag, New York, 1980), p. 190.
[CrossRef]

Appl. Phys. (1)

H. J. Eichler, U. Klein, D. Langhans, Appl. Phys. 21, 215 (1980).
[CrossRef]

Appl. Phys. Lett. (2)

D. W. Phillion, D. J. Kuizenga, A. E. Siegman, Appl. Phys. Lett. 27, 85 (1975).
[CrossRef]

R. L. Fork, B. I. Greene, C. V. Shank, Appl. Phys. Lett. 38, 671 (1981).
[CrossRef]

Chem. Phys. Lett. (1)

J. M. Wiesenfeld, E. P. Ippen, Chem. Phys. Lett. 67, 213 (1979).
[CrossRef]

IEEE J. Quantum Electron. (1)

A. L. Smirl, T. F. Boggess, B. S. Wherrett, G. P. Perryman, A. Miller, IEEE J. Quantum Electron. QE-19, 690 (1983).
[CrossRef]

J. Appl. Phys. (1)

H. Eichler, G. Salje, H. Stahl, J. Appl. Phys. 44, 5383 (1973).
[CrossRef]

J. Phys. Soc. Jpn. (1)

T. Yajima, Y. Taira, J. Phys. Soc. Jpn. 47, 1620 (1979).
[CrossRef]

Opt. Lett. (2)

Phys. Rev. A (1)

J. J. Song, J. H. Lee, M. D. Levenson, Phys. Rev. A 17, 1439 (1978).
[CrossRef]

Phys. Rev. Lett. (1)

T. Mossberg, A. Flusberg, R. Kachru, S. R. Hartmann, Phys. Rev. Lett. 42, 1665 (1979).
[CrossRef]

Other (1)

T. Yajima, Y. Ishida, Y. Taira, Picosecond Phenomena II, R. M. Hochstrasser, W. Kaiser, C. V. Shank, eds. (Springer-Verlag, New York, 1980), p. 190.
[CrossRef]

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Figures (4)

Fig. 1
Fig. 1

Experimental geometry for dephasing measurements by the three-pulse-scattering technique.

Fig. 2
Fig. 2

Two-pulse-scattering data for Nile blue dye in methanol, for both parallel (— — —) and perpendicular (—) polarizations.

Fig. 3
Fig. 3

Three-pulse-scattering data for Nile blue dye in ethylene glycol, for both parallel (—) and perpendicular (·····) polarizations. Also shown are two reference curves, calculated by expression (4) assuming a homogeneously broadened transition. Curve A (— — —) uses the measured absorption spectrum, whereas Curve B (—··—) assumes a Lorentzian line peaked at 625 nm with T2 = 50 fsec. Both curves A and B utilize the actual laser spectrum.

Fig. 4
Fig. 4

Same as in Fig. 3 but expanded in scale and extended to longer time delays. Reference curve B is not shown.

Equations (4)

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U k 3 ± ( k 1 k 2 ) exp ( 2 | τ | / T 2 ) , U k 3 ± ( k 1 k 2 ) exp ( 4 | τ | / T 2 ) u ( τ ) ,
U k 3 ± ( k 1 k 2 ) | d t E ( t ) E * ( t + τ ) | 2 ,
U k 3 ± ( k 1 k 2 ) | d τ h T ( τ + τ ) r * ( τ ) + d τ h T * ( τ τ ) r ( τ ) | 2 .
G ( Ω ) α ( ω L + Ω ) ϕ ( ω L + Ω ) ,

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