Abstract

We have measured the third-harmonic response, γ, of a centrosymmetric squaraine dye (ISQ) in chloroform at a range of frequencies for which the third harmonic is above the strong, narrow peak in the dye’s linear absorption spectrum but below the UV absorption band. By fitting the experimental dispersion of γ using a four-level model, we determine the strength, location, and width of the lowest-lying two-photon transition. We find that the 21Ag state appears just above the 11Bu state in energy and that the 11Bu–21Ag transition moment is somewhat smaller than the transition moment between the ground state and the 1 1Bu state but much larger than previously predicted for comparable squaraine dyes.

© 1994 Optical Society of America

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Corrections

James H. Andrews, John D. V. Khaydarov, and Kenneth D. Singer, "Contribution of the 2 1Ag state to the third-order optical nonlinearity in a squaraine dye: errata," Opt. Lett. 19, 1909-1909 (1994)
https://www.osapublishing.org/ol/abstract.cfm?uri=ol-19-22-1909

References

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    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef] [PubMed]

1994 (1)

1993 (3)

Q. L. Zhou, R. F. Shi, O. Zamani-Khamari, A. F. Garito, Nonlinear Opt. 6, 145 (1993).

C. Poga, M. G. Kuzyk, S. Martinez, C. W. Dirk, Proc. Soc. Photo-Opt. Instrum. Eng. 2025, 363 (1993).

S. R. Marder, J. W. Perry, G. Bourhill, C. B. Gorman, B. G. Tiemann, K. Mansour, Science 261, 186 (1993).
[CrossRef] [PubMed]

1992 (1)

C. W. Dirk, L.-T. Cheng, M. G. Kuzyk, Int. J. Quantum Chem. 43, 27 (1992).
[CrossRef]

1991 (2)

B. M. Pierce, Proc. Soc. Photo-Opt. Instrum. Eng. 1560, 148 (1991).

J. R. Heflin, Y. M. Cai, A. F. Garito, J. Opt. Soc. Am. B 8, 2132 (1991).
[CrossRef]

1990 (3)

M. G. Kuzyk, C. W. Dirk, Phys. Rev. A 41, 5098 (1990).
[CrossRef] [PubMed]

C. W. Dirk, M. G. Kuzyk, Chem. Mat. 2, 4 (1990).
[CrossRef]

C. W. Dirk, H. E. Katz, M. L. Schilling, L. A. King, Chem. Mat. 2, 700 (1990).
[CrossRef]

1987 (1)

F. Kajzar, J. Messier, Rev. Sci. Instrum. 58, 2081 (1987).
[CrossRef]

Andrews, J. H.

Bourhill, G.

S. R. Marder, J. W. Perry, G. Bourhill, C. B. Gorman, B. G. Tiemann, K. Mansour, Science 261, 186 (1993).
[CrossRef] [PubMed]

Cai, Y. M.

Cheng, L.-T.

C. W. Dirk, L.-T. Cheng, M. G. Kuzyk, Int. J. Quantum Chem. 43, 27 (1992).
[CrossRef]

Dirk, C. W.

C. Poga, M. G. Kuzyk, S. Martinez, C. W. Dirk, Proc. Soc. Photo-Opt. Instrum. Eng. 2025, 363 (1993).

C. W. Dirk, L.-T. Cheng, M. G. Kuzyk, Int. J. Quantum Chem. 43, 27 (1992).
[CrossRef]

C. W. Dirk, M. G. Kuzyk, Chem. Mat. 2, 4 (1990).
[CrossRef]

M. G. Kuzyk, C. W. Dirk, Phys. Rev. A 41, 5098 (1990).
[CrossRef] [PubMed]

C. W. Dirk, H. E. Katz, M. L. Schilling, L. A. King, Chem. Mat. 2, 700 (1990).
[CrossRef]

Garito, A. F.

Q. L. Zhou, R. F. Shi, O. Zamani-Khamari, A. F. Garito, Nonlinear Opt. 6, 145 (1993).

J. R. Heflin, Y. M. Cai, A. F. Garito, J. Opt. Soc. Am. B 8, 2132 (1991).
[CrossRef]

Gorman, C. B.

S. R. Marder, J. W. Perry, G. Bourhill, C. B. Gorman, B. G. Tiemann, K. Mansour, Science 261, 186 (1993).
[CrossRef] [PubMed]

Heflin, J. R.

Kajzar, F.

F. Kajzar, J. Messier, Rev. Sci. Instrum. 58, 2081 (1987).
[CrossRef]

Katz, H. E.

C. W. Dirk, H. E. Katz, M. L. Schilling, L. A. King, Chem. Mat. 2, 700 (1990).
[CrossRef]

Khaydarov, J. D. V.

King, L. A.

C. W. Dirk, H. E. Katz, M. L. Schilling, L. A. King, Chem. Mat. 2, 700 (1990).
[CrossRef]

Kuzyk, M. G.

C. Poga, M. G. Kuzyk, S. Martinez, C. W. Dirk, Proc. Soc. Photo-Opt. Instrum. Eng. 2025, 363 (1993).

C. W. Dirk, L.-T. Cheng, M. G. Kuzyk, Int. J. Quantum Chem. 43, 27 (1992).
[CrossRef]

C. W. Dirk, M. G. Kuzyk, Chem. Mat. 2, 4 (1990).
[CrossRef]

M. G. Kuzyk, C. W. Dirk, Phys. Rev. A 41, 5098 (1990).
[CrossRef] [PubMed]

Mansour, K.

S. R. Marder, J. W. Perry, G. Bourhill, C. B. Gorman, B. G. Tiemann, K. Mansour, Science 261, 186 (1993).
[CrossRef] [PubMed]

Marder, S. R.

S. R. Marder, J. W. Perry, G. Bourhill, C. B. Gorman, B. G. Tiemann, K. Mansour, Science 261, 186 (1993).
[CrossRef] [PubMed]

Martinez, S.

C. Poga, M. G. Kuzyk, S. Martinez, C. W. Dirk, Proc. Soc. Photo-Opt. Instrum. Eng. 2025, 363 (1993).

Messier, J.

F. Kajzar, J. Messier, Rev. Sci. Instrum. 58, 2081 (1987).
[CrossRef]

Perry, J. W.

S. R. Marder, J. W. Perry, G. Bourhill, C. B. Gorman, B. G. Tiemann, K. Mansour, Science 261, 186 (1993).
[CrossRef] [PubMed]

Pierce, B. M.

B. M. Pierce, Proc. Soc. Photo-Opt. Instrum. Eng. 1560, 148 (1991).

Poga, C.

C. Poga, M. G. Kuzyk, S. Martinez, C. W. Dirk, Proc. Soc. Photo-Opt. Instrum. Eng. 2025, 363 (1993).

Schilling, M. L.

C. W. Dirk, H. E. Katz, M. L. Schilling, L. A. King, Chem. Mat. 2, 700 (1990).
[CrossRef]

Shi, R. F.

Q. L. Zhou, R. F. Shi, O. Zamani-Khamari, A. F. Garito, Nonlinear Opt. 6, 145 (1993).

Singer, K. D.

Tiemann, B. G.

S. R. Marder, J. W. Perry, G. Bourhill, C. B. Gorman, B. G. Tiemann, K. Mansour, Science 261, 186 (1993).
[CrossRef] [PubMed]

Zamani-Khamari, O.

Q. L. Zhou, R. F. Shi, O. Zamani-Khamari, A. F. Garito, Nonlinear Opt. 6, 145 (1993).

Zhou, Q. L.

Q. L. Zhou, R. F. Shi, O. Zamani-Khamari, A. F. Garito, Nonlinear Opt. 6, 145 (1993).

Chem. Mat. (2)

C. W. Dirk, M. G. Kuzyk, Chem. Mat. 2, 4 (1990).
[CrossRef]

C. W. Dirk, H. E. Katz, M. L. Schilling, L. A. King, Chem. Mat. 2, 700 (1990).
[CrossRef]

Int. J. Quantum Chem. (1)

C. W. Dirk, L.-T. Cheng, M. G. Kuzyk, Int. J. Quantum Chem. 43, 27 (1992).
[CrossRef]

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

Nonlinear Opt. (1)

Q. L. Zhou, R. F. Shi, O. Zamani-Khamari, A. F. Garito, Nonlinear Opt. 6, 145 (1993).

Opt. Lett. (1)

Phys. Rev. A (1)

M. G. Kuzyk, C. W. Dirk, Phys. Rev. A 41, 5098 (1990).
[CrossRef] [PubMed]

Proc. Soc. Photo-Opt. Instrum. Eng. (2)

B. M. Pierce, Proc. Soc. Photo-Opt. Instrum. Eng. 1560, 148 (1991).

C. Poga, M. G. Kuzyk, S. Martinez, C. W. Dirk, Proc. Soc. Photo-Opt. Instrum. Eng. 2025, 363 (1993).

Rev. Sci. Instrum. (1)

F. Kajzar, J. Messier, Rev. Sci. Instrum. 58, 2081 (1987).
[CrossRef]

Science (1)

S. R. Marder, J. W. Perry, G. Bourhill, C. B. Gorman, B. G. Tiemann, K. Mansour, Science 261, 186 (1993).
[CrossRef] [PubMed]

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Figures (2)

Fig. 1
Fig. 1

Chemical structure and optical absorption spectrum of ISQ in chloroform.

Fig. 2
Fig. 2

Ratio of the third-harmonic amplitudes of 0.215 ± 0.01% ISQ by weight in chloroform to the amplitudes of pure chloroform. The solid curve is a four-level fit with the parameters listed in Table 1. Inset: level diagrams for the two types of terms of Eq. (4).

Tables (1)

Tables Icon

Table 1 Four-Level Fitting Parameters for Third-Harmonic Dispersion of ISQ in Chloroform

Equations (6)

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γ = 1 4 ћ 3 ( l , m , n ' D lmn μ gl μ lm μ mn μ ng l , n ' D ln μ gl μ lg μ gn μ ng ) ,
D lmn = [ ( Ω ng ω ) ( Ω mg 2 ω ) ( Ω lg 3 ω ) ] 1 + [ ( Ω ng * + ω ) ( Ω mg 2 ω ) ( Ω lg ω ) ] 1 + [ ( Ω ng * + ω ) ( Ω mg * + 2 ω ) ( Ω lg ω ) ] 1 + [ ( Ω ng * + ω ) ( Ω mg * + 2 ω ) ( Ω lg * + 3 ω ) ] 1 ,
D ln = [ ( Ω lg ω ) ( Ω lg 3 ω ) ( Ω ng ω ) ] 1 + [ ( Ω lg * + ω ) ( Ω lg ω ) ( Ω ng ω ) ] 1 + [ ( Ω lg ω ) ( Ω lg * + ω ) ( Ω ng * + ω ) ] 1 + [ ( Ω lg * + ω ) ( Ω lg * + 3 ω ) ( Ω ng * + ω ) ] 1 .
γ = μ 01 2 4 ћ 3 ( μ 01 2 D 11 n μ 1 n 2 D 1 n 1 ) ,
A ¯ thg L A ¯ thg R = | ( T GL / Δ n G 2 ) χ G ( 3 ) ( T L / Δ n L 2 ) χ L ( 3 ) [ t L ( 2 ) ] 3 | 2 { ( T GR / Δ n G 2 ) χ G ( 3 ) ( T R / Δ n R 2 ) χ R ( 3 ) [ t R ( 2 ) ] 3 } 2 ,
χ L ( 3 ) χ R ( 3 ) + ( f ω ) 3 f 3 ω N ( γ + i γ ) ISQ ,

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