Abstract

A recently developed theory concerning the physical limits on optical hyperpolarizabilities is shown to be useful in the theoretical prediction of contributions of multiphoton fluorescence to experimentally determined hyperpolarizability values. Recent experimental results are compared with the theoretical limit. Without correction for the fluorescence contribution, results for the first hyperpolarizability in the forbidden region can be obtained. Proper correction of the systematic error shifts these values to the theoretical limit. Hence, experimental values above the theoretical upper limit should be suspect, but an appropriate fluorescence suppression technique is available. Reversing the argument, the observation that artificially overestimated values for the first hyperpolarizability are reduced from the forbidden region to exactly this upper limit is found to corroborate the limiting theory.

© 2001 Optical Society of America

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References

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  1. M. G. Kuzyk, Opt. Lett. 25, 1183 (2000).
    [CrossRef]
  2. M. G. Kuzyk, Phys. Rev. Lett. 85, 1218 (2000).
    [CrossRef] [PubMed]
  3. K. Clays and A. Persoons, Phys. Rev. Lett. 66, 2980 (1991).
    [CrossRef] [PubMed]
  4. K. Clays and A. Persoons, Rev. Sci. Instrum. 63, 3285 (1992).
    [CrossRef]
  5. K. Clays, A. Persoons, and L. De Maeyer, in Modern Nonlinear Optics, M. Evans and S. Kielich, eds., Vol. 85 of Advances in Chemical Physics (Wiley, New York, 1994), Part 3, p. 455.
  6. M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, and L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
    [CrossRef]
  7. G. Olbrechts, R. Strobbe, K. Clays, and A. Persoons, Rev. Sci. Instrum. 69, 2233 (1998).
    [CrossRef]
  8. G. Olbrechts, K. Wostyn, K. Clays, and A. Persoons, Opt. Lett. 24, 403 (1999).
    [CrossRef]
  9. G. Olbrechts, K. Clays, and A. Persoons, J. Opt. Soc. Am. B 17, 1867 (2000).
    [CrossRef]
  10. K. Clays, G. Olbrechts, T. Munters, A. Persoons, O.-K. Kim, and L.-S. Choi, Chem. Phys. Lett. 293, 337 (1998).
    [CrossRef]
  11. G. Olbrechts, K. Wostyn, K. Clays, A. Persoons, S. H. Kang, and K. Kim, Chem. Phys. Lett. 308, 173 (1999).
    [CrossRef]
  12. K. Clays, K. Wostyn, G. Olbrechts, A. Persoons, A. Watanabe, K. Nogi, X.-M. Duan, S. Okada, H. Oikawa, H. Nakanishi, D. Beljonne, H. Vogel, and J.-L. Brédas, J. Opt. Soc. Am. B 17, 256 (2000).
    [CrossRef]

2000 (4)

1999 (2)

G. Olbrechts, K. Wostyn, K. Clays, A. Persoons, S. H. Kang, and K. Kim, Chem. Phys. Lett. 308, 173 (1999).
[CrossRef]

G. Olbrechts, K. Wostyn, K. Clays, and A. Persoons, Opt. Lett. 24, 403 (1999).
[CrossRef]

1998 (2)

G. Olbrechts, R. Strobbe, K. Clays, and A. Persoons, Rev. Sci. Instrum. 69, 2233 (1998).
[CrossRef]

K. Clays, G. Olbrechts, T. Munters, A. Persoons, O.-K. Kim, and L.-S. Choi, Chem. Phys. Lett. 293, 337 (1998).
[CrossRef]

1995 (1)

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, and L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

1992 (1)

K. Clays and A. Persoons, Rev. Sci. Instrum. 63, 3285 (1992).
[CrossRef]

1991 (1)

K. Clays and A. Persoons, Phys. Rev. Lett. 66, 2980 (1991).
[CrossRef] [PubMed]

Beljonne, D.

Brédas, J.-L.

Choi, L.-S.

K. Clays, G. Olbrechts, T. Munters, A. Persoons, O.-K. Kim, and L.-S. Choi, Chem. Phys. Lett. 293, 337 (1998).
[CrossRef]

Clays, K.

G. Olbrechts, K. Clays, and A. Persoons, J. Opt. Soc. Am. B 17, 1867 (2000).
[CrossRef]

K. Clays, K. Wostyn, G. Olbrechts, A. Persoons, A. Watanabe, K. Nogi, X.-M. Duan, S. Okada, H. Oikawa, H. Nakanishi, D. Beljonne, H. Vogel, and J.-L. Brédas, J. Opt. Soc. Am. B 17, 256 (2000).
[CrossRef]

G. Olbrechts, K. Wostyn, K. Clays, A. Persoons, S. H. Kang, and K. Kim, Chem. Phys. Lett. 308, 173 (1999).
[CrossRef]

G. Olbrechts, K. Wostyn, K. Clays, and A. Persoons, Opt. Lett. 24, 403 (1999).
[CrossRef]

G. Olbrechts, R. Strobbe, K. Clays, and A. Persoons, Rev. Sci. Instrum. 69, 2233 (1998).
[CrossRef]

K. Clays, G. Olbrechts, T. Munters, A. Persoons, O.-K. Kim, and L.-S. Choi, Chem. Phys. Lett. 293, 337 (1998).
[CrossRef]

K. Clays and A. Persoons, Rev. Sci. Instrum. 63, 3285 (1992).
[CrossRef]

K. Clays and A. Persoons, Phys. Rev. Lett. 66, 2980 (1991).
[CrossRef] [PubMed]

K. Clays, A. Persoons, and L. De Maeyer, in Modern Nonlinear Optics, M. Evans and S. Kielich, eds., Vol. 85 of Advances in Chemical Physics (Wiley, New York, 1994), Part 3, p. 455.

de Jonge, R.

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, and L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

De Maeyer, L.

K. Clays, A. Persoons, and L. De Maeyer, in Modern Nonlinear Optics, M. Evans and S. Kielich, eds., Vol. 85 of Advances in Chemical Physics (Wiley, New York, 1994), Part 3, p. 455.

Duan, X.-M.

Flipse, M. C.

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, and L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Jenneskens, L. W.

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, and L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Kang, S. H.

G. Olbrechts, K. Wostyn, K. Clays, A. Persoons, S. H. Kang, and K. Kim, Chem. Phys. Lett. 308, 173 (1999).
[CrossRef]

Kim, K.

G. Olbrechts, K. Wostyn, K. Clays, A. Persoons, S. H. Kang, and K. Kim, Chem. Phys. Lett. 308, 173 (1999).
[CrossRef]

Kim, O.-K.

K. Clays, G. Olbrechts, T. Munters, A. Persoons, O.-K. Kim, and L.-S. Choi, Chem. Phys. Lett. 293, 337 (1998).
[CrossRef]

Kuzyk, M. G.

M. G. Kuzyk, Opt. Lett. 25, 1183 (2000).
[CrossRef]

M. G. Kuzyk, Phys. Rev. Lett. 85, 1218 (2000).
[CrossRef] [PubMed]

Marsman, A. W.

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, and L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Munters, T.

K. Clays, G. Olbrechts, T. Munters, A. Persoons, O.-K. Kim, and L.-S. Choi, Chem. Phys. Lett. 293, 337 (1998).
[CrossRef]

Nakanishi, H.

Nogi, K.

Oikawa, H.

Okada, S.

Olbrechts, G.

K. Clays, K. Wostyn, G. Olbrechts, A. Persoons, A. Watanabe, K. Nogi, X.-M. Duan, S. Okada, H. Oikawa, H. Nakanishi, D. Beljonne, H. Vogel, and J.-L. Brédas, J. Opt. Soc. Am. B 17, 256 (2000).
[CrossRef]

G. Olbrechts, K. Clays, and A. Persoons, J. Opt. Soc. Am. B 17, 1867 (2000).
[CrossRef]

G. Olbrechts, K. Wostyn, K. Clays, A. Persoons, S. H. Kang, and K. Kim, Chem. Phys. Lett. 308, 173 (1999).
[CrossRef]

G. Olbrechts, K. Wostyn, K. Clays, and A. Persoons, Opt. Lett. 24, 403 (1999).
[CrossRef]

K. Clays, G. Olbrechts, T. Munters, A. Persoons, O.-K. Kim, and L.-S. Choi, Chem. Phys. Lett. 293, 337 (1998).
[CrossRef]

G. Olbrechts, R. Strobbe, K. Clays, and A. Persoons, Rev. Sci. Instrum. 69, 2233 (1998).
[CrossRef]

Persoons, A.

G. Olbrechts, K. Clays, and A. Persoons, J. Opt. Soc. Am. B 17, 1867 (2000).
[CrossRef]

K. Clays, K. Wostyn, G. Olbrechts, A. Persoons, A. Watanabe, K. Nogi, X.-M. Duan, S. Okada, H. Oikawa, H. Nakanishi, D. Beljonne, H. Vogel, and J.-L. Brédas, J. Opt. Soc. Am. B 17, 256 (2000).
[CrossRef]

G. Olbrechts, K. Wostyn, K. Clays, A. Persoons, S. H. Kang, and K. Kim, Chem. Phys. Lett. 308, 173 (1999).
[CrossRef]

G. Olbrechts, K. Wostyn, K. Clays, and A. Persoons, Opt. Lett. 24, 403 (1999).
[CrossRef]

G. Olbrechts, R. Strobbe, K. Clays, and A. Persoons, Rev. Sci. Instrum. 69, 2233 (1998).
[CrossRef]

K. Clays, G. Olbrechts, T. Munters, A. Persoons, O.-K. Kim, and L.-S. Choi, Chem. Phys. Lett. 293, 337 (1998).
[CrossRef]

K. Clays and A. Persoons, Rev. Sci. Instrum. 63, 3285 (1992).
[CrossRef]

K. Clays and A. Persoons, Phys. Rev. Lett. 66, 2980 (1991).
[CrossRef] [PubMed]

K. Clays, A. Persoons, and L. De Maeyer, in Modern Nonlinear Optics, M. Evans and S. Kielich, eds., Vol. 85 of Advances in Chemical Physics (Wiley, New York, 1994), Part 3, p. 455.

Strobbe, R.

G. Olbrechts, R. Strobbe, K. Clays, and A. Persoons, Rev. Sci. Instrum. 69, 2233 (1998).
[CrossRef]

van Walree, C. A.

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, and L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Vogel, H.

Watanabe, A.

Wostyn, K.

Woudenberg, R. H.

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, and L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Chem. Phys. Lett. (3)

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, and L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

K. Clays, G. Olbrechts, T. Munters, A. Persoons, O.-K. Kim, and L.-S. Choi, Chem. Phys. Lett. 293, 337 (1998).
[CrossRef]

G. Olbrechts, K. Wostyn, K. Clays, A. Persoons, S. H. Kang, and K. Kim, Chem. Phys. Lett. 308, 173 (1999).
[CrossRef]

J. Opt. Soc. Am. B (2)

Opt. Lett. (2)

Phys. Rev. Lett. (2)

M. G. Kuzyk, Phys. Rev. Lett. 85, 1218 (2000).
[CrossRef] [PubMed]

K. Clays and A. Persoons, Phys. Rev. Lett. 66, 2980 (1991).
[CrossRef] [PubMed]

Rev. Sci. Instrum. (2)

K. Clays and A. Persoons, Rev. Sci. Instrum. 63, 3285 (1992).
[CrossRef]

G. Olbrechts, R. Strobbe, K. Clays, and A. Persoons, Rev. Sci. Instrum. 69, 2233 (1998).
[CrossRef]

Other (1)

K. Clays, A. Persoons, and L. De Maeyer, in Modern Nonlinear Optics, M. Evans and S. Kielich, eds., Vol. 85 of Advances in Chemical Physics (Wiley, New York, 1994), Part 3, p. 455.

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Figures (1)

Fig. 1
Fig. 1

ENR values for the static hyperpolarizability, β0/N3/2, as a function of a wavelength of maximal absorption, λmax, for the electronic transition between the ground and the first-excited states: solid curve, theoretical upper limit according to the theory of Kuzyk2; dashed curve, trend in SOS calculated hyperpolarizability values for the series; downward-pointing triangles, experimental hyperpolarizability values without fluorescence corrections; upward-pointing triangles, experimental hyperpolarizability values after correction; filled triangles, chromophores in solution; open triangles, n=1 chromophore embedded in amylose helix. Note how uncorrected experimental values above the upper limit are reduced to the theoretical limit by the fluorescence-correction method (indicated by the downward-pointing arrows).

Tables (1)

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Table 1 Overview of Relevant Parameters and Experimental Results for the Series (n=  1–5) of Hemicyanine Molecules

Equations (1)

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β2 L*SR34n2+233em3N3/2E107/2.

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