Abstract

We describe push–pull molecules, using a two-form two-state model, and define a parameter, MIX, that characterizes the mixing between the two limiting-resonance forms. MIX is related to the difference between the weight of each form in either the ground or the first-excited state. We have established analytical relationships between static polarizabilities and MIX. The optimum MIX value that yields maximized quadratic polarizability βmax(0) occurs when the mixing is intermediate between equivalent contributions of the two limiting forms and the strong predominance of either form. By examining experimental results obtained with push–pull polyenes, we show that not only MIX but also βmax(0) is affected by the nature of the donor–acceptor end groups as well as by the size of the polyenic linker. The results also help us to understand the length dependences of the quadratic polarizability measured in solution for series of push–pull polyenes. These dependences result from a combination of MIX and βmax(0) variations with increasing chain length.

© 1998 Optical Society of America

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  1. D. S. Chemla and J. Zyss, Nonlinear Optical Properties of Organic Molecules and Crystals (Academic, New York, 1987), Vols. 1 and 2.
  2. S. R. Marder, J. E. Sohn, and G. D. Stucky, Materials for Nonlinear Optics: Chemical Perspectives, ACS Symp. Ser. 455 (1991).
  3. M. Blanchard-Desce, S. R. Marder, and M. Barzoukas, in Supramolecular Technology, D. N. Reinhoudt, ed., Vol. 10 of Comprehensive Supramolecular Chemistry (Elsevier, Amsterdam, 1996), pp. 833–863.
  4. J.-L. Oudar and D. S. Chemla, J. Chem. Phys. 66, 2664 (1977).
    [CrossRef]
  5. J.-L. Oudar, J. Chem. Phys. 67, 446 (1977).
    [CrossRef]
  6. M. Blanchard-Desce, R. Wortmann, S. Lebus, J.-M. Lehn, and P. Krämer, Chem. Phys. Lett. 243, 526 (1995).
    [CrossRef]
  7. M. Blanchard-Desce, V. Alain, L. Midrier, R. Wortmann, S. Lebus, C. Glania, P. Krämer, A. Fort, J. Muller, and M. Barzoukas, J. Photochem. Photobiol. A 105, 115 (1997).
    [CrossRef]
  8. M. Blanchard-Desce, V. Alain, P. V. Bedworth, S. R. Marder, A. Fort, C. Runser, M. Barzoukas, S. Lebus, and R. Wortmann, Chem. Eur. 3, 1091 (1997).
  9. S. R. Marder, D. N. Beratan, and L.-T. Cheng, Science 252, 103 (1991).
    [CrossRef] [PubMed]
  10. C. B. Gorman and S. R. Marder, Proc. Natl. Acad. Sci. USA 90, 11297 (1993).
    [CrossRef]
  11. S. R. Marder, C. B. Gorman, F. Meyers, J. W. Perry, G. Bourhill, J.-L. Brédas, and B. M. Pierce, Science 265, 632 (1994).
    [CrossRef] [PubMed]
  12. F. Meyers, S. R. Marder, B. M. Pierce, and J.-L. Brédas, J. Am. Chem. Soc. 116, 10703 (1994).
    [CrossRef]
  13. C. B. Gorman and S. R. Marder, Chem. Mater. 7, 215 (1995).
    [CrossRef]
  14. D. Lu, G. Chen, J. W. Perry, and W. A. Goddard III, J. Am. Chem. Soc. 116, 10670 (1994).
    [CrossRef]
  15. D. Lu, G. Chen, and W. A. Goddard III, J. Chem. Phys. 101, 5860 (1994).
    [CrossRef]
  16. C. Castiglioni, M. Del Zoppo, and G. Zerbi, Phys. Rev. B 53, 13319 (1996).
    [CrossRef]
  17. M. Barzoukas, C. Runser, A. Fort, and M. Blanchard-Desce, Chem. Phys. Lett. 257, 531 (1996).
    [CrossRef]
  18. M. Barzoukas, A. Fort, and M. Blanchard-Desce, J. Nonlinear Opt. Phys. Mater. 5, 757 (1996).
    [CrossRef]
  19. M. Barzoukas, J. Muller, A. Fort, S. R. Marder, V. Alain, and M. Blanchard-Desce, in Nonlinear Optical Properties of Organic Materials IX, G. R. Moehlmann, ed., Proc. SPIE 2852, 132 (1996).
    [CrossRef]
  20. M. Barzoukas, A. Fort, and M. Blanchard-Desce, New J. Chem. 21, 309 (1997).
  21. M. Blanchard-Desce, C. Runser, A. Fort, M. Barzoukas, J.-M. Lehn, V. Bloy, and V. Alain, Chem. Phys. 199, 253 (1995).
    [CrossRef]
  22. A. Willets, J. E. Rice, D. M. Burland, and D. P. Shelton, J. Chem. Phys. 97, 7590 (1992).
    [CrossRef]

1997

M. Blanchard-Desce, V. Alain, L. Midrier, R. Wortmann, S. Lebus, C. Glania, P. Krämer, A. Fort, J. Muller, and M. Barzoukas, J. Photochem. Photobiol. A 105, 115 (1997).
[CrossRef]

M. Barzoukas, A. Fort, and M. Blanchard-Desce, New J. Chem. 21, 309 (1997).

1996

C. Castiglioni, M. Del Zoppo, and G. Zerbi, Phys. Rev. B 53, 13319 (1996).
[CrossRef]

M. Barzoukas, C. Runser, A. Fort, and M. Blanchard-Desce, Chem. Phys. Lett. 257, 531 (1996).
[CrossRef]

M. Barzoukas, A. Fort, and M. Blanchard-Desce, J. Nonlinear Opt. Phys. Mater. 5, 757 (1996).
[CrossRef]

M. Barzoukas, J. Muller, A. Fort, S. R. Marder, V. Alain, and M. Blanchard-Desce, in Nonlinear Optical Properties of Organic Materials IX, G. R. Moehlmann, ed., Proc. SPIE 2852, 132 (1996).
[CrossRef]

1995

M. Blanchard-Desce, C. Runser, A. Fort, M. Barzoukas, J.-M. Lehn, V. Bloy, and V. Alain, Chem. Phys. 199, 253 (1995).
[CrossRef]

C. B. Gorman and S. R. Marder, Chem. Mater. 7, 215 (1995).
[CrossRef]

M. Blanchard-Desce, R. Wortmann, S. Lebus, J.-M. Lehn, and P. Krämer, Chem. Phys. Lett. 243, 526 (1995).
[CrossRef]

1994

S. R. Marder, C. B. Gorman, F. Meyers, J. W. Perry, G. Bourhill, J.-L. Brédas, and B. M. Pierce, Science 265, 632 (1994).
[CrossRef] [PubMed]

F. Meyers, S. R. Marder, B. M. Pierce, and J.-L. Brédas, J. Am. Chem. Soc. 116, 10703 (1994).
[CrossRef]

D. Lu, G. Chen, J. W. Perry, and W. A. Goddard III, J. Am. Chem. Soc. 116, 10670 (1994).
[CrossRef]

D. Lu, G. Chen, and W. A. Goddard III, J. Chem. Phys. 101, 5860 (1994).
[CrossRef]

1993

C. B. Gorman and S. R. Marder, Proc. Natl. Acad. Sci. USA 90, 11297 (1993).
[CrossRef]

1992

A. Willets, J. E. Rice, D. M. Burland, and D. P. Shelton, J. Chem. Phys. 97, 7590 (1992).
[CrossRef]

1991

S. R. Marder, D. N. Beratan, and L.-T. Cheng, Science 252, 103 (1991).
[CrossRef] [PubMed]

1977

J.-L. Oudar and D. S. Chemla, J. Chem. Phys. 66, 2664 (1977).
[CrossRef]

J.-L. Oudar, J. Chem. Phys. 67, 446 (1977).
[CrossRef]

Alain, V.

M. Blanchard-Desce, V. Alain, L. Midrier, R. Wortmann, S. Lebus, C. Glania, P. Krämer, A. Fort, J. Muller, and M. Barzoukas, J. Photochem. Photobiol. A 105, 115 (1997).
[CrossRef]

M. Barzoukas, J. Muller, A. Fort, S. R. Marder, V. Alain, and M. Blanchard-Desce, in Nonlinear Optical Properties of Organic Materials IX, G. R. Moehlmann, ed., Proc. SPIE 2852, 132 (1996).
[CrossRef]

M. Blanchard-Desce, C. Runser, A. Fort, M. Barzoukas, J.-M. Lehn, V. Bloy, and V. Alain, Chem. Phys. 199, 253 (1995).
[CrossRef]

Barzoukas, M.

M. Barzoukas, A. Fort, and M. Blanchard-Desce, New J. Chem. 21, 309 (1997).

M. Blanchard-Desce, V. Alain, L. Midrier, R. Wortmann, S. Lebus, C. Glania, P. Krämer, A. Fort, J. Muller, and M. Barzoukas, J. Photochem. Photobiol. A 105, 115 (1997).
[CrossRef]

M. Barzoukas, C. Runser, A. Fort, and M. Blanchard-Desce, Chem. Phys. Lett. 257, 531 (1996).
[CrossRef]

M. Barzoukas, A. Fort, and M. Blanchard-Desce, J. Nonlinear Opt. Phys. Mater. 5, 757 (1996).
[CrossRef]

M. Barzoukas, J. Muller, A. Fort, S. R. Marder, V. Alain, and M. Blanchard-Desce, in Nonlinear Optical Properties of Organic Materials IX, G. R. Moehlmann, ed., Proc. SPIE 2852, 132 (1996).
[CrossRef]

M. Blanchard-Desce, C. Runser, A. Fort, M. Barzoukas, J.-M. Lehn, V. Bloy, and V. Alain, Chem. Phys. 199, 253 (1995).
[CrossRef]

Beratan, D. N.

S. R. Marder, D. N. Beratan, and L.-T. Cheng, Science 252, 103 (1991).
[CrossRef] [PubMed]

Blanchard-Desce, M.

M. Blanchard-Desce, V. Alain, L. Midrier, R. Wortmann, S. Lebus, C. Glania, P. Krämer, A. Fort, J. Muller, and M. Barzoukas, J. Photochem. Photobiol. A 105, 115 (1997).
[CrossRef]

M. Barzoukas, A. Fort, and M. Blanchard-Desce, New J. Chem. 21, 309 (1997).

M. Barzoukas, C. Runser, A. Fort, and M. Blanchard-Desce, Chem. Phys. Lett. 257, 531 (1996).
[CrossRef]

M. Barzoukas, A. Fort, and M. Blanchard-Desce, J. Nonlinear Opt. Phys. Mater. 5, 757 (1996).
[CrossRef]

M. Barzoukas, J. Muller, A. Fort, S. R. Marder, V. Alain, and M. Blanchard-Desce, in Nonlinear Optical Properties of Organic Materials IX, G. R. Moehlmann, ed., Proc. SPIE 2852, 132 (1996).
[CrossRef]

M. Blanchard-Desce, R. Wortmann, S. Lebus, J.-M. Lehn, and P. Krämer, Chem. Phys. Lett. 243, 526 (1995).
[CrossRef]

M. Blanchard-Desce, C. Runser, A. Fort, M. Barzoukas, J.-M. Lehn, V. Bloy, and V. Alain, Chem. Phys. 199, 253 (1995).
[CrossRef]

Bloy, V.

M. Blanchard-Desce, C. Runser, A. Fort, M. Barzoukas, J.-M. Lehn, V. Bloy, and V. Alain, Chem. Phys. 199, 253 (1995).
[CrossRef]

Bourhill, G.

S. R. Marder, C. B. Gorman, F. Meyers, J. W. Perry, G. Bourhill, J.-L. Brédas, and B. M. Pierce, Science 265, 632 (1994).
[CrossRef] [PubMed]

Brédas, J.-L.

S. R. Marder, C. B. Gorman, F. Meyers, J. W. Perry, G. Bourhill, J.-L. Brédas, and B. M. Pierce, Science 265, 632 (1994).
[CrossRef] [PubMed]

F. Meyers, S. R. Marder, B. M. Pierce, and J.-L. Brédas, J. Am. Chem. Soc. 116, 10703 (1994).
[CrossRef]

Burland, D. M.

A. Willets, J. E. Rice, D. M. Burland, and D. P. Shelton, J. Chem. Phys. 97, 7590 (1992).
[CrossRef]

Castiglioni, C.

C. Castiglioni, M. Del Zoppo, and G. Zerbi, Phys. Rev. B 53, 13319 (1996).
[CrossRef]

Chemla, D. S.

J.-L. Oudar and D. S. Chemla, J. Chem. Phys. 66, 2664 (1977).
[CrossRef]

Chen, G.

D. Lu, G. Chen, and W. A. Goddard III, J. Chem. Phys. 101, 5860 (1994).
[CrossRef]

D. Lu, G. Chen, J. W. Perry, and W. A. Goddard III, J. Am. Chem. Soc. 116, 10670 (1994).
[CrossRef]

Cheng, L.-T.

S. R. Marder, D. N. Beratan, and L.-T. Cheng, Science 252, 103 (1991).
[CrossRef] [PubMed]

Del Zoppo, M.

C. Castiglioni, M. Del Zoppo, and G. Zerbi, Phys. Rev. B 53, 13319 (1996).
[CrossRef]

Fort, A.

M. Blanchard-Desce, V. Alain, L. Midrier, R. Wortmann, S. Lebus, C. Glania, P. Krämer, A. Fort, J. Muller, and M. Barzoukas, J. Photochem. Photobiol. A 105, 115 (1997).
[CrossRef]

M. Barzoukas, A. Fort, and M. Blanchard-Desce, New J. Chem. 21, 309 (1997).

M. Barzoukas, C. Runser, A. Fort, and M. Blanchard-Desce, Chem. Phys. Lett. 257, 531 (1996).
[CrossRef]

M. Barzoukas, A. Fort, and M. Blanchard-Desce, J. Nonlinear Opt. Phys. Mater. 5, 757 (1996).
[CrossRef]

M. Barzoukas, J. Muller, A. Fort, S. R. Marder, V. Alain, and M. Blanchard-Desce, in Nonlinear Optical Properties of Organic Materials IX, G. R. Moehlmann, ed., Proc. SPIE 2852, 132 (1996).
[CrossRef]

M. Blanchard-Desce, C. Runser, A. Fort, M. Barzoukas, J.-M. Lehn, V. Bloy, and V. Alain, Chem. Phys. 199, 253 (1995).
[CrossRef]

Glania, C.

M. Blanchard-Desce, V. Alain, L. Midrier, R. Wortmann, S. Lebus, C. Glania, P. Krämer, A. Fort, J. Muller, and M. Barzoukas, J. Photochem. Photobiol. A 105, 115 (1997).
[CrossRef]

Goddard III, W. A.

D. Lu, G. Chen, J. W. Perry, and W. A. Goddard III, J. Am. Chem. Soc. 116, 10670 (1994).
[CrossRef]

D. Lu, G. Chen, and W. A. Goddard III, J. Chem. Phys. 101, 5860 (1994).
[CrossRef]

Gorman, C. B.

C. B. Gorman and S. R. Marder, Chem. Mater. 7, 215 (1995).
[CrossRef]

S. R. Marder, C. B. Gorman, F. Meyers, J. W. Perry, G. Bourhill, J.-L. Brédas, and B. M. Pierce, Science 265, 632 (1994).
[CrossRef] [PubMed]

C. B. Gorman and S. R. Marder, Proc. Natl. Acad. Sci. USA 90, 11297 (1993).
[CrossRef]

Krämer, P.

M. Blanchard-Desce, V. Alain, L. Midrier, R. Wortmann, S. Lebus, C. Glania, P. Krämer, A. Fort, J. Muller, and M. Barzoukas, J. Photochem. Photobiol. A 105, 115 (1997).
[CrossRef]

M. Blanchard-Desce, R. Wortmann, S. Lebus, J.-M. Lehn, and P. Krämer, Chem. Phys. Lett. 243, 526 (1995).
[CrossRef]

Lebus, S.

M. Blanchard-Desce, V. Alain, L. Midrier, R. Wortmann, S. Lebus, C. Glania, P. Krämer, A. Fort, J. Muller, and M. Barzoukas, J. Photochem. Photobiol. A 105, 115 (1997).
[CrossRef]

M. Blanchard-Desce, R. Wortmann, S. Lebus, J.-M. Lehn, and P. Krämer, Chem. Phys. Lett. 243, 526 (1995).
[CrossRef]

Lehn, J.-M.

M. Blanchard-Desce, R. Wortmann, S. Lebus, J.-M. Lehn, and P. Krämer, Chem. Phys. Lett. 243, 526 (1995).
[CrossRef]

M. Blanchard-Desce, C. Runser, A. Fort, M. Barzoukas, J.-M. Lehn, V. Bloy, and V. Alain, Chem. Phys. 199, 253 (1995).
[CrossRef]

Lu, D.

D. Lu, G. Chen, J. W. Perry, and W. A. Goddard III, J. Am. Chem. Soc. 116, 10670 (1994).
[CrossRef]

D. Lu, G. Chen, and W. A. Goddard III, J. Chem. Phys. 101, 5860 (1994).
[CrossRef]

Marder, S. R.

M. Barzoukas, J. Muller, A. Fort, S. R. Marder, V. Alain, and M. Blanchard-Desce, in Nonlinear Optical Properties of Organic Materials IX, G. R. Moehlmann, ed., Proc. SPIE 2852, 132 (1996).
[CrossRef]

C. B. Gorman and S. R. Marder, Chem. Mater. 7, 215 (1995).
[CrossRef]

S. R. Marder, C. B. Gorman, F. Meyers, J. W. Perry, G. Bourhill, J.-L. Brédas, and B. M. Pierce, Science 265, 632 (1994).
[CrossRef] [PubMed]

F. Meyers, S. R. Marder, B. M. Pierce, and J.-L. Brédas, J. Am. Chem. Soc. 116, 10703 (1994).
[CrossRef]

C. B. Gorman and S. R. Marder, Proc. Natl. Acad. Sci. USA 90, 11297 (1993).
[CrossRef]

S. R. Marder, D. N. Beratan, and L.-T. Cheng, Science 252, 103 (1991).
[CrossRef] [PubMed]

Meyers, F.

S. R. Marder, C. B. Gorman, F. Meyers, J. W. Perry, G. Bourhill, J.-L. Brédas, and B. M. Pierce, Science 265, 632 (1994).
[CrossRef] [PubMed]

F. Meyers, S. R. Marder, B. M. Pierce, and J.-L. Brédas, J. Am. Chem. Soc. 116, 10703 (1994).
[CrossRef]

Midrier, L.

M. Blanchard-Desce, V. Alain, L. Midrier, R. Wortmann, S. Lebus, C. Glania, P. Krämer, A. Fort, J. Muller, and M. Barzoukas, J. Photochem. Photobiol. A 105, 115 (1997).
[CrossRef]

Muller, J.

M. Blanchard-Desce, V. Alain, L. Midrier, R. Wortmann, S. Lebus, C. Glania, P. Krämer, A. Fort, J. Muller, and M. Barzoukas, J. Photochem. Photobiol. A 105, 115 (1997).
[CrossRef]

M. Barzoukas, J. Muller, A. Fort, S. R. Marder, V. Alain, and M. Blanchard-Desce, in Nonlinear Optical Properties of Organic Materials IX, G. R. Moehlmann, ed., Proc. SPIE 2852, 132 (1996).
[CrossRef]

Oudar, J.-L.

J.-L. Oudar, J. Chem. Phys. 67, 446 (1977).
[CrossRef]

J.-L. Oudar and D. S. Chemla, J. Chem. Phys. 66, 2664 (1977).
[CrossRef]

Perry, J. W.

S. R. Marder, C. B. Gorman, F. Meyers, J. W. Perry, G. Bourhill, J.-L. Brédas, and B. M. Pierce, Science 265, 632 (1994).
[CrossRef] [PubMed]

D. Lu, G. Chen, J. W. Perry, and W. A. Goddard III, J. Am. Chem. Soc. 116, 10670 (1994).
[CrossRef]

Pierce, B. M.

F. Meyers, S. R. Marder, B. M. Pierce, and J.-L. Brédas, J. Am. Chem. Soc. 116, 10703 (1994).
[CrossRef]

S. R. Marder, C. B. Gorman, F. Meyers, J. W. Perry, G. Bourhill, J.-L. Brédas, and B. M. Pierce, Science 265, 632 (1994).
[CrossRef] [PubMed]

Rice, J. E.

A. Willets, J. E. Rice, D. M. Burland, and D. P. Shelton, J. Chem. Phys. 97, 7590 (1992).
[CrossRef]

Runser, C.

M. Barzoukas, C. Runser, A. Fort, and M. Blanchard-Desce, Chem. Phys. Lett. 257, 531 (1996).
[CrossRef]

M. Blanchard-Desce, C. Runser, A. Fort, M. Barzoukas, J.-M. Lehn, V. Bloy, and V. Alain, Chem. Phys. 199, 253 (1995).
[CrossRef]

Shelton, D. P.

A. Willets, J. E. Rice, D. M. Burland, and D. P. Shelton, J. Chem. Phys. 97, 7590 (1992).
[CrossRef]

Willets, A.

A. Willets, J. E. Rice, D. M. Burland, and D. P. Shelton, J. Chem. Phys. 97, 7590 (1992).
[CrossRef]

Wortmann, R.

M. Blanchard-Desce, V. Alain, L. Midrier, R. Wortmann, S. Lebus, C. Glania, P. Krämer, A. Fort, J. Muller, and M. Barzoukas, J. Photochem. Photobiol. A 105, 115 (1997).
[CrossRef]

M. Blanchard-Desce, R. Wortmann, S. Lebus, J.-M. Lehn, and P. Krämer, Chem. Phys. Lett. 243, 526 (1995).
[CrossRef]

Zerbi, G.

C. Castiglioni, M. Del Zoppo, and G. Zerbi, Phys. Rev. B 53, 13319 (1996).
[CrossRef]

Chem. Mater.

C. B. Gorman and S. R. Marder, Chem. Mater. 7, 215 (1995).
[CrossRef]

Chem. Phys.

M. Blanchard-Desce, C. Runser, A. Fort, M. Barzoukas, J.-M. Lehn, V. Bloy, and V. Alain, Chem. Phys. 199, 253 (1995).
[CrossRef]

Chem. Phys. Lett.

M. Barzoukas, C. Runser, A. Fort, and M. Blanchard-Desce, Chem. Phys. Lett. 257, 531 (1996).
[CrossRef]

M. Blanchard-Desce, R. Wortmann, S. Lebus, J.-M. Lehn, and P. Krämer, Chem. Phys. Lett. 243, 526 (1995).
[CrossRef]

J. Am. Chem. Soc.

F. Meyers, S. R. Marder, B. M. Pierce, and J.-L. Brédas, J. Am. Chem. Soc. 116, 10703 (1994).
[CrossRef]

D. Lu, G. Chen, J. W. Perry, and W. A. Goddard III, J. Am. Chem. Soc. 116, 10670 (1994).
[CrossRef]

J. Chem. Phys.

D. Lu, G. Chen, and W. A. Goddard III, J. Chem. Phys. 101, 5860 (1994).
[CrossRef]

J.-L. Oudar and D. S. Chemla, J. Chem. Phys. 66, 2664 (1977).
[CrossRef]

J.-L. Oudar, J. Chem. Phys. 67, 446 (1977).
[CrossRef]

A. Willets, J. E. Rice, D. M. Burland, and D. P. Shelton, J. Chem. Phys. 97, 7590 (1992).
[CrossRef]

J. Nonlinear Opt. Phys. Mater.

M. Barzoukas, A. Fort, and M. Blanchard-Desce, J. Nonlinear Opt. Phys. Mater. 5, 757 (1996).
[CrossRef]

J. Photochem. Photobiol. A

M. Blanchard-Desce, V. Alain, L. Midrier, R. Wortmann, S. Lebus, C. Glania, P. Krämer, A. Fort, J. Muller, and M. Barzoukas, J. Photochem. Photobiol. A 105, 115 (1997).
[CrossRef]

New J. Chem.

M. Barzoukas, A. Fort, and M. Blanchard-Desce, New J. Chem. 21, 309 (1997).

Phys. Rev. B

C. Castiglioni, M. Del Zoppo, and G. Zerbi, Phys. Rev. B 53, 13319 (1996).
[CrossRef]

Proc. Natl. Acad. Sci. USA

C. B. Gorman and S. R. Marder, Proc. Natl. Acad. Sci. USA 90, 11297 (1993).
[CrossRef]

Proc. SPIE

M. Barzoukas, J. Muller, A. Fort, S. R. Marder, V. Alain, and M. Blanchard-Desce, in Nonlinear Optical Properties of Organic Materials IX, G. R. Moehlmann, ed., Proc. SPIE 2852, 132 (1996).
[CrossRef]

Science

S. R. Marder, D. N. Beratan, and L.-T. Cheng, Science 252, 103 (1991).
[CrossRef] [PubMed]

S. R. Marder, C. B. Gorman, F. Meyers, J. W. Perry, G. Bourhill, J.-L. Brédas, and B. M. Pierce, Science 265, 632 (1994).
[CrossRef] [PubMed]

Other

M. Blanchard-Desce, V. Alain, P. V. Bedworth, S. R. Marder, A. Fort, C. Runser, M. Barzoukas, S. Lebus, and R. Wortmann, Chem. Eur. 3, 1091 (1997).

D. S. Chemla and J. Zyss, Nonlinear Optical Properties of Organic Molecules and Crystals (Academic, New York, 1987), Vols. 1 and 2.

S. R. Marder, J. E. Sohn, and G. D. Stucky, Materials for Nonlinear Optics: Chemical Perspectives, ACS Symp. Ser. 455 (1991).

M. Blanchard-Desce, S. R. Marder, and M. Barzoukas, in Supramolecular Technology, D. N. Reinhoudt, ed., Vol. 10 of Comprehensive Supramolecular Chemistry (Elsevier, Amsterdam, 1996), pp. 833–863.

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Figures (5)

Fig. 1
Fig. 1

Neutral (left) and zwitterionic (right) forms of a push–pull polyene.

Fig. 2
Fig. 2

Structural formulas of the series investigated in this study.

Fig. 3
Fig. 3

Variations of α(0), β(0), and γ(0) versus MIX.

Fig. 4
Fig. 4

Variation of quadratic polarizabilities β(0) with MIX for compounds 1a[1], 1b[1], 1c[1], 2[1], and 3[1]. The filled circles correspond to the EOAM quadratic polarizabilities measured in dioxane.

Fig. 5
Fig. 5

Variation of quadratic polarizability β(0) and MIX for series 2[n]. The plot is limited to the negative range of values of MIX. The filled circles correspond to the EOAM quadratic polarizabilities measured in dioxane.

Tables (4)

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Table 1 Static Quadratic Polarizabilities of Push–Pull Polyenes with Various Donor–Acceptor Pairs Obtained from EFISH Measurements [βEFISH(0)] or Calculated from EOAM Data [βEOAM(0)] a

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Table 2 Static Quadratic Polarizabilities of Two Series of Push–Pull Polyenes of Increasing Length Obtained from EFISH Measurements [βEFISH(0)] or Calculated from EOAM Data in Dioxane [βEOAM(0)] a

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Table 3 Characteristics of Push–Pull Compounds with Various Donor–Acceptor Pairs in Two-Form Two-State Model

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Table 4 Characteristics of Push–Pull Polyenes of Increasing Length in the Two-Form Two-State Model

Equations (17)

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μg(E)=μg+α(0)E+12! β(0)E2+13! γ(0)E3+,
β(0)=6μeg2ΔμEeg2,
|Ψg=cos θ2 |ΨN+sin θ2 |ΨZ,
|Ψe=-sin θ2 |ΨN+cos θ2 |ΨZ,
MIX=-cos2 θ2-sin2 θ2=-cos θ,
MIX=-V(V2+4t2)1/2,
μg=μN+μZ+μCSMIX2,
α(0)=μgMIX MIXEE=0,β(0)=α(0)MIX MIXEE=0,
γ(0)=β(0)MIX MIXEE=0.
MIX=-V-μCSE[(V-μCSE)2+4t2]1/2,
α(0)=(1-MIX2)3/2 μCS24t,
β(0)=-MIX(1-MIX2)2 3μCS38t2,
γ(0)=(5MIX2-1)(1-MIX2)5/2 3μCS416t3.
βmax(0)=6μCS325(5)1/2t2.
βEFISH(0)=3μeg2Δμ2Eeg2.
tan θ=2μegΔμ,
μCS=Δμcos θ.

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