Abstract

We briefly outline a modelling strategy, combining quantum chemistry and molecular dynamics simulations, for obtaining macroscopic nonlinear optical coeffcients in guest-host systems like chromophores in solutions or in polymer matrices. The parameters required for the calculation of the macroscopic nonlinear optical property, like the chromophore number density, local field factors, and the order parameter of the chromophore molecules, are derived. These parameters, together with the molecular first hyperpolarizabilities, obtained from quantum chemistry calculations, are used to estimate the macroscopic electro-optic coeffcients. The combined approach leads to some new conclusions about the relation of the chromophore property and its solvent interactions in order to optimize the nonlinear optical coeffcient. For instance, from the simulation results a totally different notion is derived about the collective properties of octupolar molecules. We find that such molecules receive a solvent induced dipole moment that makes it possible to pole them by an external electric field, but also that they can aggregate as an effect of this solvent interaction.

© 2005 Chinese Optics Letters

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  1. L. R. Dalton, W. H. Steier, B. H. Robinson, C. Zhang, A. Ren, S. Garner, A. Chen, T. Londergan, L. Irwin, B. Carlson, L. Fifield, G. Phelan, C. Kincaid, J. Amend, and A. Jen, J. Mater. Chem. 9, 1905 (1999).
  2. L. Dalton, A. Harper, A. Ren, F. Wang, G. Todorova, J. Chen, C. Zhang, and M. Lee, Ind. Eng. Chem. Res. 38, 8 (1999).
  3. S. R. Marder, C. B. Gorman, F. Meyers, J. W. Perry, G. Bourhill, J.-L. Bredas, and B. M. Pierce, Science 265, 632 (1994).
  4. A. K.-Y. Jen, Y. Cai, P. V. Bedworth, and S. R. Marder, Adv. Mater. 9, 132 (1997).
  5. D. M. Burland, R. D. Miller, and C. A. Walsh, Chem. Rev. 94, 31 (1994).
  6. W.-K. Kim and L. M. Hayden, J. Chem. Phys. 111, 5212 (1999).
  7. M. Makowska-Janusik, H. Reis, M. G. Papadopoulos, I. G. Economou, and N. Zacharopoulos, J. Phys. Chem. B 108, 588 (2004).
  8. Y. Yamaguchi, Y. Yokomichi, S. Yokoyama, and S. Mashiko, Theo. Chem. 545, 187 (2001).
  9. Y. Tu, Y. Luo, and H. Agren, Can octupolar molecules be poled by an external electric field? (submitted).
  10. Y. Tu, Y. Luo, and H. Agren, Theoretical study of electro-optic activity of dipolar chromophore solutions (submitted).
  11. J. Wang, R. M. Wolf, J. W. Caldwell, P. A. Kollman, and D. A. Case, J. Comput. Chem. 25, 1157 (2004).
  12. J. Wang, R. M. Wolf, J. W. Caldwell, P. A. Kollman, and D. A. Case, J. Comput. Chem. 26, 114 (2005).
  13. C. I. Bayly, P. Cieplak, W. D. Cornell, and P. A. Kollman, J. Phys. Chem. 97, 10269 (1993).
  14. D. R. Lide, CRC Handbook of Chemistry and Physics (73rd edn.) (CRC Press, 1992).
  15. J. Zyss and I. Ledoux, Chem. Rev. 94, 77 (1994).
  16. DALTON, Release 2.0, http://www.kjemi.uio.no/software/dalton/dalton.html (2005).
  17. Y. Wang, L. Frediani, P. Salek, and H. Agren, (to be published).
  18. L. R. Dalton, A. W. Harper, and B. H. Robinson, Proc. Natl. Acad. Sci. 94, 4842 (1997).

2005 (1)

J. Wang, R. M. Wolf, J. W. Caldwell, P. A. Kollman, and D. A. Case, J. Comput. Chem. 26, 114 (2005).

2004 (2)

M. Makowska-Janusik, H. Reis, M. G. Papadopoulos, I. G. Economou, and N. Zacharopoulos, J. Phys. Chem. B 108, 588 (2004).

J. Wang, R. M. Wolf, J. W. Caldwell, P. A. Kollman, and D. A. Case, J. Comput. Chem. 25, 1157 (2004).

2001 (1)

Y. Yamaguchi, Y. Yokomichi, S. Yokoyama, and S. Mashiko, Theo. Chem. 545, 187 (2001).

1999 (3)

W.-K. Kim and L. M. Hayden, J. Chem. Phys. 111, 5212 (1999).

L. R. Dalton, W. H. Steier, B. H. Robinson, C. Zhang, A. Ren, S. Garner, A. Chen, T. Londergan, L. Irwin, B. Carlson, L. Fifield, G. Phelan, C. Kincaid, J. Amend, and A. Jen, J. Mater. Chem. 9, 1905 (1999).

L. Dalton, A. Harper, A. Ren, F. Wang, G. Todorova, J. Chen, C. Zhang, and M. Lee, Ind. Eng. Chem. Res. 38, 8 (1999).

1997 (2)

A. K.-Y. Jen, Y. Cai, P. V. Bedworth, and S. R. Marder, Adv. Mater. 9, 132 (1997).

L. R. Dalton, A. W. Harper, and B. H. Robinson, Proc. Natl. Acad. Sci. 94, 4842 (1997).

1994 (3)

J. Zyss and I. Ledoux, Chem. Rev. 94, 77 (1994).

D. M. Burland, R. D. Miller, and C. A. Walsh, Chem. Rev. 94, 31 (1994).

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

1993 (1)

C. I. Bayly, P. Cieplak, W. D. Cornell, and P. A. Kollman, J. Phys. Chem. 97, 10269 (1993).

Adv. Mater. (1)

A. K.-Y. Jen, Y. Cai, P. V. Bedworth, and S. R. Marder, Adv. Mater. 9, 132 (1997).

Chem. Rev. (2)

D. M. Burland, R. D. Miller, and C. A. Walsh, Chem. Rev. 94, 31 (1994).

J. Zyss and I. Ledoux, Chem. Rev. 94, 77 (1994).

Ind. Eng. Chem. Res. (1)

L. Dalton, A. Harper, A. Ren, F. Wang, G. Todorova, J. Chen, C. Zhang, and M. Lee, Ind. Eng. Chem. Res. 38, 8 (1999).

J. Chem. Phys. (1)

W.-K. Kim and L. M. Hayden, J. Chem. Phys. 111, 5212 (1999).

J. Comput. Chem. (2)

J. Wang, R. M. Wolf, J. W. Caldwell, P. A. Kollman, and D. A. Case, J. Comput. Chem. 25, 1157 (2004).

J. Wang, R. M. Wolf, J. W. Caldwell, P. A. Kollman, and D. A. Case, J. Comput. Chem. 26, 114 (2005).

J. Mater. Chem. (1)

L. R. Dalton, W. H. Steier, B. H. Robinson, C. Zhang, A. Ren, S. Garner, A. Chen, T. Londergan, L. Irwin, B. Carlson, L. Fifield, G. Phelan, C. Kincaid, J. Amend, and A. Jen, J. Mater. Chem. 9, 1905 (1999).

J. Phys. Chem. (1)

C. I. Bayly, P. Cieplak, W. D. Cornell, and P. A. Kollman, J. Phys. Chem. 97, 10269 (1993).

J. Phys. Chem. B (1)

M. Makowska-Janusik, H. Reis, M. G. Papadopoulos, I. G. Economou, and N. Zacharopoulos, J. Phys. Chem. B 108, 588 (2004).

Proc. Natl. Acad. Sci. (1)

L. R. Dalton, A. W. Harper, and B. H. Robinson, Proc. Natl. Acad. Sci. 94, 4842 (1997).

Science (1)

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

Theo. Chem. (1)

Y. Yamaguchi, Y. Yokomichi, S. Yokoyama, and S. Mashiko, Theo. Chem. 545, 187 (2001).

Other (5)

Y. Tu, Y. Luo, and H. Agren, Can octupolar molecules be poled by an external electric field? (submitted).

Y. Tu, Y. Luo, and H. Agren, Theoretical study of electro-optic activity of dipolar chromophore solutions (submitted).

D. R. Lide, CRC Handbook of Chemistry and Physics (73rd edn.) (CRC Press, 1992).

DALTON, Release 2.0, http://www.kjemi.uio.no/software/dalton/dalton.html (2005).

Y. Wang, L. Frediani, P. Salek, and H. Agren, (to be published).

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