Abstract

We have developed a new method of determining in time both the real and the imaginary parts of third-order nonlinear-optical coefficients. In this method the phase-conjugated four-wave-mixing signal beam interferes with one of the transmitted pump beams. By comparing the interference pattern with that of a known reference, we are able to determine the real and the imaginary parts of the third-order optical nonlinearity for an unknown sample. The real and the imaginary parts can also be separated when one incoming beam is delayed. We apply this method to a bis-thienyl polyene molecule containing five conjugate double bonds and find that the hyperpolarizability is γ1111 = (−2.5 − 0.17i) × 10−30 esu.

© 1996 Optical Society of America

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References

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  1. Y. R. Shen, The Principles of Nonlinear Optics (Wiley, New York, 1984), Chap. 1, p. 4.
  2. R. W. Hellwarth, Prog. Quantum Electron. 5, 1 (1977).
    [CrossRef]
  3. X. F. Cao, J. P. Jiang, D. P. Bloch, R. W. Hellwarth, L. P. Yu, L. Dalton, J. Appl. Phys. 65, 5012 (1989).
    [CrossRef]
  4. N. Tang, J. P. Partanen, R. W. Hellwarth, R. J. Knize, Phys. Rev. B 48, 8404 (1993).
    [CrossRef]
  5. M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
    [CrossRef]
  6. S. M. Saltiel, B. Van Wonterghem, P. M. Rentzepis, Opt. Lett. 14, 183 (1989).
    [CrossRef] [PubMed]
  7. P. N. Butcher, D. Cotter, The Elements of Nonlinear Optics (Cambridge U. Press, Cambridge, 1990), Chap. 7, p. 232.
  8. C. W. Spangler, M. Q. He, J. Laquindanum, L. Dalton, N. Tang, J. P. Partanen, R. W. Hellwarth, in Electrical, Optical, and Magnetic Properties of Organic Solid State Materials, A. F. Garito, A. K-Y. Jen, L. R. Dalton, C. C. Lee, eds., Vol. 328 of MRS Symposium Proceedings Series (Materials Research Society, Pittsburgh, Pa., 1994), p. 655.
  9. N. Tang, “Experimental and theoretical studies of the nonlinear optical response of certain fullerenes, polymers and glasses,” Ph.D. dissertation (University of Southern California, Los Angeles, August1994).

1993

N. Tang, J. P. Partanen, R. W. Hellwarth, R. J. Knize, Phys. Rev. B 48, 8404 (1993).
[CrossRef]

1990

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

1989

S. M. Saltiel, B. Van Wonterghem, P. M. Rentzepis, Opt. Lett. 14, 183 (1989).
[CrossRef] [PubMed]

X. F. Cao, J. P. Jiang, D. P. Bloch, R. W. Hellwarth, L. P. Yu, L. Dalton, J. Appl. Phys. 65, 5012 (1989).
[CrossRef]

1977

R. W. Hellwarth, Prog. Quantum Electron. 5, 1 (1977).
[CrossRef]

Bloch, D. P.

X. F. Cao, J. P. Jiang, D. P. Bloch, R. W. Hellwarth, L. P. Yu, L. Dalton, J. Appl. Phys. 65, 5012 (1989).
[CrossRef]

Butcher, P. N.

P. N. Butcher, D. Cotter, The Elements of Nonlinear Optics (Cambridge U. Press, Cambridge, 1990), Chap. 7, p. 232.

Cao, X. F.

X. F. Cao, J. P. Jiang, D. P. Bloch, R. W. Hellwarth, L. P. Yu, L. Dalton, J. Appl. Phys. 65, 5012 (1989).
[CrossRef]

Cotter, D.

P. N. Butcher, D. Cotter, The Elements of Nonlinear Optics (Cambridge U. Press, Cambridge, 1990), Chap. 7, p. 232.

Dalton, L.

X. F. Cao, J. P. Jiang, D. P. Bloch, R. W. Hellwarth, L. P. Yu, L. Dalton, J. Appl. Phys. 65, 5012 (1989).
[CrossRef]

C. W. Spangler, M. Q. He, J. Laquindanum, L. Dalton, N. Tang, J. P. Partanen, R. W. Hellwarth, in Electrical, Optical, and Magnetic Properties of Organic Solid State Materials, A. F. Garito, A. K-Y. Jen, L. R. Dalton, C. C. Lee, eds., Vol. 328 of MRS Symposium Proceedings Series (Materials Research Society, Pittsburgh, Pa., 1994), p. 655.

Hagan, D. J.

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

He, M. Q.

C. W. Spangler, M. Q. He, J. Laquindanum, L. Dalton, N. Tang, J. P. Partanen, R. W. Hellwarth, in Electrical, Optical, and Magnetic Properties of Organic Solid State Materials, A. F. Garito, A. K-Y. Jen, L. R. Dalton, C. C. Lee, eds., Vol. 328 of MRS Symposium Proceedings Series (Materials Research Society, Pittsburgh, Pa., 1994), p. 655.

Hellwarth, R. W.

N. Tang, J. P. Partanen, R. W. Hellwarth, R. J. Knize, Phys. Rev. B 48, 8404 (1993).
[CrossRef]

X. F. Cao, J. P. Jiang, D. P. Bloch, R. W. Hellwarth, L. P. Yu, L. Dalton, J. Appl. Phys. 65, 5012 (1989).
[CrossRef]

R. W. Hellwarth, Prog. Quantum Electron. 5, 1 (1977).
[CrossRef]

C. W. Spangler, M. Q. He, J. Laquindanum, L. Dalton, N. Tang, J. P. Partanen, R. W. Hellwarth, in Electrical, Optical, and Magnetic Properties of Organic Solid State Materials, A. F. Garito, A. K-Y. Jen, L. R. Dalton, C. C. Lee, eds., Vol. 328 of MRS Symposium Proceedings Series (Materials Research Society, Pittsburgh, Pa., 1994), p. 655.

Jiang, J. P.

X. F. Cao, J. P. Jiang, D. P. Bloch, R. W. Hellwarth, L. P. Yu, L. Dalton, J. Appl. Phys. 65, 5012 (1989).
[CrossRef]

Knize, R. J.

N. Tang, J. P. Partanen, R. W. Hellwarth, R. J. Knize, Phys. Rev. B 48, 8404 (1993).
[CrossRef]

Laquindanum, J.

C. W. Spangler, M. Q. He, J. Laquindanum, L. Dalton, N. Tang, J. P. Partanen, R. W. Hellwarth, in Electrical, Optical, and Magnetic Properties of Organic Solid State Materials, A. F. Garito, A. K-Y. Jen, L. R. Dalton, C. C. Lee, eds., Vol. 328 of MRS Symposium Proceedings Series (Materials Research Society, Pittsburgh, Pa., 1994), p. 655.

Partanen, J. P.

N. Tang, J. P. Partanen, R. W. Hellwarth, R. J. Knize, Phys. Rev. B 48, 8404 (1993).
[CrossRef]

C. W. Spangler, M. Q. He, J. Laquindanum, L. Dalton, N. Tang, J. P. Partanen, R. W. Hellwarth, in Electrical, Optical, and Magnetic Properties of Organic Solid State Materials, A. F. Garito, A. K-Y. Jen, L. R. Dalton, C. C. Lee, eds., Vol. 328 of MRS Symposium Proceedings Series (Materials Research Society, Pittsburgh, Pa., 1994), p. 655.

Rentzepis, P. M.

Said, A. A.

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Saltiel, S. M.

Sheik-Bahae, M.

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Shen, Y. R.

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, New York, 1984), Chap. 1, p. 4.

Spangler, C. W.

C. W. Spangler, M. Q. He, J. Laquindanum, L. Dalton, N. Tang, J. P. Partanen, R. W. Hellwarth, in Electrical, Optical, and Magnetic Properties of Organic Solid State Materials, A. F. Garito, A. K-Y. Jen, L. R. Dalton, C. C. Lee, eds., Vol. 328 of MRS Symposium Proceedings Series (Materials Research Society, Pittsburgh, Pa., 1994), p. 655.

Tang, N.

N. Tang, J. P. Partanen, R. W. Hellwarth, R. J. Knize, Phys. Rev. B 48, 8404 (1993).
[CrossRef]

C. W. Spangler, M. Q. He, J. Laquindanum, L. Dalton, N. Tang, J. P. Partanen, R. W. Hellwarth, in Electrical, Optical, and Magnetic Properties of Organic Solid State Materials, A. F. Garito, A. K-Y. Jen, L. R. Dalton, C. C. Lee, eds., Vol. 328 of MRS Symposium Proceedings Series (Materials Research Society, Pittsburgh, Pa., 1994), p. 655.

N. Tang, “Experimental and theoretical studies of the nonlinear optical response of certain fullerenes, polymers and glasses,” Ph.D. dissertation (University of Southern California, Los Angeles, August1994).

Van Stryland, E. W.

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Van Wonterghem, B.

Wei, T. H.

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Yu, L. P.

X. F. Cao, J. P. Jiang, D. P. Bloch, R. W. Hellwarth, L. P. Yu, L. Dalton, J. Appl. Phys. 65, 5012 (1989).
[CrossRef]

IEEE J. Quantum Electron.

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

J. Appl. Phys.

X. F. Cao, J. P. Jiang, D. P. Bloch, R. W. Hellwarth, L. P. Yu, L. Dalton, J. Appl. Phys. 65, 5012 (1989).
[CrossRef]

Opt. Lett.

Phys. Rev. B

N. Tang, J. P. Partanen, R. W. Hellwarth, R. J. Knize, Phys. Rev. B 48, 8404 (1993).
[CrossRef]

Prog. Quantum Electron.

R. W. Hellwarth, Prog. Quantum Electron. 5, 1 (1977).
[CrossRef]

Other

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, New York, 1984), Chap. 1, p. 4.

P. N. Butcher, D. Cotter, The Elements of Nonlinear Optics (Cambridge U. Press, Cambridge, 1990), Chap. 7, p. 232.

C. W. Spangler, M. Q. He, J. Laquindanum, L. Dalton, N. Tang, J. P. Partanen, R. W. Hellwarth, in Electrical, Optical, and Magnetic Properties of Organic Solid State Materials, A. F. Garito, A. K-Y. Jen, L. R. Dalton, C. C. Lee, eds., Vol. 328 of MRS Symposium Proceedings Series (Materials Research Society, Pittsburgh, Pa., 1994), p. 655.

N. Tang, “Experimental and theoretical studies of the nonlinear optical response of certain fullerenes, polymers and glasses,” Ph.D. dissertation (University of Southern California, Los Angeles, August1994).

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Figures (4)

Fig. 1
Fig. 1

FWM interferometer arrangement. The pinhole has a diameter of 2200 μm. M’s, mirrors.

Fig. 2
Fig. 2

Typical DFWM interference pattern UI of our sample 5-BTP. Also shown are two sets of interference patterns from our reference CS2 with the same cell, taken just before and right after the 5-BTP sample run. The vertical solid lines are guides.

Fig. 3
Fig. 3

Temporal response of the DFWM signal from 5-BTP.

Fig. 4
Fig. 4

Energy distributions at the photodiode array in the case of reference CS2: (a) DFWM signal beam, (b) backward-transmitted beam, and (c) their interference pattern. The solid curves in (a) and (b) represent the best fit to Gaussian profiles, and the solid curve in (c) follows Eq. (3).

Equations (4)

Equations on this page are rendered with MathJax. Learn more.

φ T = φ B + 2 π n L λ + 2 π l T λ ,
φ S = ( φ F + φ B φ P ) + 2 π n L λ + 2 π l S λ + φ ( 3 ) .
U I = U S + U T + 2 A exp [ ( x / r ) 2 ] cos ( Δ k x + Δ φ ) ,
Δ φ = [ 2 π ( l S l T ) λ + ( φ F φ P ) ] + φ ( 3 ) .

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