Abstract

We determine the molecular first-order hyperpolarizability β of the highly nonlinear organic salt 4-N,N-dimethylamino-4-N-methyl stilbazolium tosylate (DAST, βzzz=(1540±250)×10-40m4/V at λ = 1542 nm) and the cocrystal 4-{2-[1-(2-hydroxyethyl)-4-pyridylidene]-ethylidene}-cyclo-hexa-2,5-dien-1-one)–(methyl 2,4-dihydroxybenzoate) (M2-MDB, βzzz=(1510±250)×10-40m4/V at λ = 1907 nm) in solution. These values are compared with the molecular first-order hyperpolarizabilities in the solid state, calculated with the measured nonlinear optical coefficient of the crystals. For both materials we show that the molecular nonlinearity in the solid state is considerably smaller than in solution. This lowering of the nonlinearity is attributed to the relatively strong Coulomb interactions in DAST and to the very strong hydrogen bonding in M2-MDB.

© 2001 Optical Society of America

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  1. F. Pan, G. Knöpfle, Ch. Bosshard, S. Follonier, R. Spreiter, M. S. Wong, and P. Günter, “Electro-optic properties of the organic salt 4-N, N-dimethylamino-4′-N′-methylstilbazolium tosylate,” Appl. Phys. Lett. 69, 13–15 (1996).
    [CrossRef]
  2. R. Spreiter, Ch. Bosshard, and P. Günter, “High frequency response and acoustic phonon contribution of the linear electro-optic effect in DAST,” Opt. Lett. 22, 564–566 (1997).
    [CrossRef] [PubMed]
  3. M. S. Wong, F. Pan, M. Bösch, R. Spreiter, Ch. Bosshard, and P. Günter, “Novel electro-optic molecular co-crystals with ideal chromophoric orientation and large second-order nonlinearities,” J. Opt. Soc. Am. B 15, 426–431 (1998).
    [CrossRef]
  4. J. L. Oudar and D. S. Chemla, “Hyperpolarizabilities of the nitroanilines and their relations to the excited state dipole moment,” J. Chem. Phys. 66, 2664–2668 (1977).
    [CrossRef]
  5. C. C. Teng and A. F. Garito, “Dispersion of the nonlinear second-order optical susceptibility of organic systems,” Phys. Rev. B 28, 6766–6773 (1983).
    [CrossRef]
  6. J. Zyss and J. L. Oudar, “Relation between microscopic and macroscopic low-order optical nonlinearities of molecular crystals with one- or two-dimensional units,” Phys. Rev. A 26, 2028–2048 (1982).
    [CrossRef]
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    [CrossRef]
  9. B. F. Levine, C. G. Bethea, E. Wasserman, and L. Leenders, “Solvent dependent hyperpolarizability of a merocyanine dye,” J. Chem. Phys. 68, 5042–5045 (1978).
    [CrossRef]
  10. A. Dulic and C. Flytzanis, “A new class of conjugated molecules with large second order polarizability,” Opt. Commun. 25, 402–406 (1978).
    [CrossRef]
  11. Ch. Bosshard, F. Pan, M. S. Wong, S. Manetta, R. Spreiter, C. Cai, P. Günter, and V. Gramlich, “Nonlinear optical organic co-crystals of merocyanine dyes and phenolic derivatives with short hydrogen bonds,” Chem. Phys. 245, 377–394 (1999).
    [CrossRef]
  12. R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurement of nonlinear light scattering,” Phys. Rev. Lett. 14, 681–684 (1965).
    [CrossRef]
  13. K. Clays and A. Persoons, “Hyper-Rayleigh scattering in solution,” Phys. Rev. Lett. 66, 2980–2983 (1991).
    [CrossRef] [PubMed]
  14. S. Kielich, “Optical second-harmonic generation by electrically polarized isotropic media,” IEEE J. Quantum Electron. 5, 562–568 (1969).
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  15. H. A. Kurtz, “Calculation of the nonlinear optical properties of molecules,” J. Comput. Chem. 11, 82 (1989).
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  18. U. Gubler and Ch. Bosshard, “Optical third-harmonic generation of fused silica in gas atmosphere: absolute value of the third-order susceptibility χ(3),” Phys. Rev. B 61, 10702–10710 (2000).
    [CrossRef]
  19. I. Liakatas, M. S. Wong, V. Gramlich, Ch. Bosshard, and P. Günter, “Novel, highly nonlinear optical molecular crystals based on multidonor-substituted 4-nitro-phenylhydrazones,” Adv. Mater. 10, 777–782 (1998).
    [CrossRef]
  20. Ph. Kaatz, E. A. Donley, and D. Shelton, “A comparison of molecular hyperpolarizabilities from gas and liquid phase measurements,” J. Chem. Phys. 108, 849–856 (1998).
    [CrossRef]
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    [CrossRef]
  23. Ch. Bosshard, R. Spreiter, P. Günter, R. R. Tykwinski, M. Schreiber, and F. Diederich, “Structure–property relationships in nonlinear optical tetrathynylethenes,” Adv. Mater. 8, 231–234 (1996).
    [CrossRef]
  24. J. Zyss, “Hyperpolarizabilities of substituted conjugated molecules. I. Perturbated INDO approach to monosubstituted benzene,” J. Chem. Phys. 70, 3333–3340 (1979).
    [CrossRef]
  25. U. Meier, M. Bösch, Ch. Bosshard, F. Pan, and P. Günter, “Parametric interactions in the organic salt 4-N, N-dimethylamino-4′-N′-methyl-stilbazolium tosylate at telecommunication wavelengths,” J. Appl. Phys. 83, 3486–3489 (1998).
    [CrossRef]
  26. Z. Kotler, R. Hierle, D. Josse, J. Zyss, and R. Masse, “Quadratic nonlinear optical properties of a transparent and highly efficient organic-inorganic crystal: 2-amino-5-nitropyridinium dihydrogen phosphate (2A5NPDP),” J. Opt. Soc. Am. B 9, 534–547 (1992).
    [CrossRef]

2000

Ch. Bosshard, U. Gubler, P. Kaatz, W. Mazerant, and U. Meier, “Non-phase-matched optical third-harmonic generation in noncentrosymmetric media: cascaded second-order contributions for the calibration of third-order nonlinearities,” Phys. Rev. B 61, 10688–10701 (2000).
[CrossRef]

U. Gubler and Ch. Bosshard, “Optical third-harmonic generation of fused silica in gas atmosphere: absolute value of the third-order susceptibility χ(3),” Phys. Rev. B 61, 10702–10710 (2000).
[CrossRef]

1999

Ch. Bosshard, F. Pan, M. S. Wong, S. Manetta, R. Spreiter, C. Cai, P. Günter, and V. Gramlich, “Nonlinear optical organic co-crystals of merocyanine dyes and phenolic derivatives with short hydrogen bonds,” Chem. Phys. 245, 377–394 (1999).
[CrossRef]

1998

I. Liakatas, M. S. Wong, V. Gramlich, Ch. Bosshard, and P. Günter, “Novel, highly nonlinear optical molecular crystals based on multidonor-substituted 4-nitro-phenylhydrazones,” Adv. Mater. 10, 777–782 (1998).
[CrossRef]

Ph. Kaatz, E. A. Donley, and D. Shelton, “A comparison of molecular hyperpolarizabilities from gas and liquid phase measurements,” J. Chem. Phys. 108, 849–856 (1998).
[CrossRef]

U. Meier, M. Bösch, Ch. Bosshard, F. Pan, and P. Günter, “Parametric interactions in the organic salt 4-N, N-dimethylamino-4′-N′-methyl-stilbazolium tosylate at telecommunication wavelengths,” J. Appl. Phys. 83, 3486–3489 (1998).
[CrossRef]

M. S. Wong, F. Pan, M. Bösch, R. Spreiter, Ch. Bosshard, and P. Günter, “Novel electro-optic molecular co-crystals with ideal chromophoric orientation and large second-order nonlinearities,” J. Opt. Soc. Am. B 15, 426–431 (1998).
[CrossRef]

1997

1996

F. Pan, G. Knöpfle, Ch. Bosshard, S. Follonier, R. Spreiter, M. S. Wong, and P. Günter, “Electro-optic properties of the organic salt 4-N, N-dimethylamino-4′-N′-methylstilbazolium tosylate,” Appl. Phys. Lett. 69, 13–15 (1996).
[CrossRef]

Ch. Bosshard, R. Spreiter, P. Günter, R. R. Tykwinski, M. Schreiber, and F. Diederich, “Structure–property relationships in nonlinear optical tetrathynylethenes,” Adv. Mater. 8, 231–234 (1996).
[CrossRef]

1994

S. Marker, L.-T. Cheng, B. G. Tiemann, A. C. Friedli, M. Blanchard-Desce, J. W. Perry, and J. Sindhoj, “Large first hyperpolarizability in push-pull polyenes by tuning of the bond length alternation and aromaticity,” Science 263, 511–514 (1994).
[CrossRef]

1992

1991

K. Clays and A. Persoons, “Hyper-Rayleigh scattering in solution,” Phys. Rev. Lett. 66, 2980–2983 (1991).
[CrossRef] [PubMed]

1989

H. A. Kurtz, “Calculation of the nonlinear optical properties of molecules,” J. Comput. Chem. 11, 82 (1989).
[CrossRef]

1983

C. C. Teng and A. F. Garito, “Dispersion of the nonlinear second-order optical susceptibility of organic systems,” Phys. Rev. B 28, 6766–6773 (1983).
[CrossRef]

1982

J. Zyss and J. L. Oudar, “Relation between microscopic and macroscopic low-order optical nonlinearities of molecular crystals with one- or two-dimensional units,” Phys. Rev. A 26, 2028–2048 (1982).
[CrossRef]

1979

J. Zyss, “Hyperpolarizabilities of substituted conjugated molecules. I. Perturbated INDO approach to monosubstituted benzene,” J. Chem. Phys. 70, 3333–3340 (1979).
[CrossRef]

1978

B. F. Levine, C. G. Bethea, E. Wasserman, and L. Leenders, “Solvent dependent hyperpolarizability of a merocyanine dye,” J. Chem. Phys. 68, 5042–5045 (1978).
[CrossRef]

A. Dulic and C. Flytzanis, “A new class of conjugated molecules with large second order polarizability,” Opt. Commun. 25, 402–406 (1978).
[CrossRef]

1977

J. L. Oudar and D. S. Chemla, “Hyperpolarizabilities of the nitroanilines and their relations to the excited state dipole moment,” J. Chem. Phys. 66, 2664–2668 (1977).
[CrossRef]

1969

S. Kielich, “Optical second-harmonic generation by electrically polarized isotropic media,” IEEE J. Quantum Electron. 5, 562–568 (1969).
[CrossRef]

1965

R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurement of nonlinear light scattering,” Phys. Rev. Lett. 14, 681–684 (1965).
[CrossRef]

1951

L. G. S. Brooker, G. H. Keyes, and D. W. Heseltine, “Color and constitution. XI. Anhydronium bases of p-hydroxystyryl dyes as solvent polarity indicators,” J. Am. Chem. Soc. 73, 5330 (1951).
[CrossRef]

Bethea, C. G.

B. F. Levine, C. G. Bethea, E. Wasserman, and L. Leenders, “Solvent dependent hyperpolarizability of a merocyanine dye,” J. Chem. Phys. 68, 5042–5045 (1978).
[CrossRef]

Blanchard-Desce, M.

S. Marker, L.-T. Cheng, B. G. Tiemann, A. C. Friedli, M. Blanchard-Desce, J. W. Perry, and J. Sindhoj, “Large first hyperpolarizability in push-pull polyenes by tuning of the bond length alternation and aromaticity,” Science 263, 511–514 (1994).
[CrossRef]

Bösch, M.

U. Meier, M. Bösch, Ch. Bosshard, F. Pan, and P. Günter, “Parametric interactions in the organic salt 4-N, N-dimethylamino-4′-N′-methyl-stilbazolium tosylate at telecommunication wavelengths,” J. Appl. Phys. 83, 3486–3489 (1998).
[CrossRef]

M. S. Wong, F. Pan, M. Bösch, R. Spreiter, Ch. Bosshard, and P. Günter, “Novel electro-optic molecular co-crystals with ideal chromophoric orientation and large second-order nonlinearities,” J. Opt. Soc. Am. B 15, 426–431 (1998).
[CrossRef]

Bosshard, Ch.

U. Gubler and Ch. Bosshard, “Optical third-harmonic generation of fused silica in gas atmosphere: absolute value of the third-order susceptibility χ(3),” Phys. Rev. B 61, 10702–10710 (2000).
[CrossRef]

Ch. Bosshard, U. Gubler, P. Kaatz, W. Mazerant, and U. Meier, “Non-phase-matched optical third-harmonic generation in noncentrosymmetric media: cascaded second-order contributions for the calibration of third-order nonlinearities,” Phys. Rev. B 61, 10688–10701 (2000).
[CrossRef]

Ch. Bosshard, F. Pan, M. S. Wong, S. Manetta, R. Spreiter, C. Cai, P. Günter, and V. Gramlich, “Nonlinear optical organic co-crystals of merocyanine dyes and phenolic derivatives with short hydrogen bonds,” Chem. Phys. 245, 377–394 (1999).
[CrossRef]

U. Meier, M. Bösch, Ch. Bosshard, F. Pan, and P. Günter, “Parametric interactions in the organic salt 4-N, N-dimethylamino-4′-N′-methyl-stilbazolium tosylate at telecommunication wavelengths,” J. Appl. Phys. 83, 3486–3489 (1998).
[CrossRef]

I. Liakatas, M. S. Wong, V. Gramlich, Ch. Bosshard, and P. Günter, “Novel, highly nonlinear optical molecular crystals based on multidonor-substituted 4-nitro-phenylhydrazones,” Adv. Mater. 10, 777–782 (1998).
[CrossRef]

M. S. Wong, F. Pan, M. Bösch, R. Spreiter, Ch. Bosshard, and P. Günter, “Novel electro-optic molecular co-crystals with ideal chromophoric orientation and large second-order nonlinearities,” J. Opt. Soc. Am. B 15, 426–431 (1998).
[CrossRef]

R. Spreiter, Ch. Bosshard, and P. Günter, “High frequency response and acoustic phonon contribution of the linear electro-optic effect in DAST,” Opt. Lett. 22, 564–566 (1997).
[CrossRef] [PubMed]

Ch. Bosshard, R. Spreiter, P. Günter, R. R. Tykwinski, M. Schreiber, and F. Diederich, “Structure–property relationships in nonlinear optical tetrathynylethenes,” Adv. Mater. 8, 231–234 (1996).
[CrossRef]

F. Pan, G. Knöpfle, Ch. Bosshard, S. Follonier, R. Spreiter, M. S. Wong, and P. Günter, “Electro-optic properties of the organic salt 4-N, N-dimethylamino-4′-N′-methylstilbazolium tosylate,” Appl. Phys. Lett. 69, 13–15 (1996).
[CrossRef]

Brooker, L. G. S.

L. G. S. Brooker, G. H. Keyes, and D. W. Heseltine, “Color and constitution. XI. Anhydronium bases of p-hydroxystyryl dyes as solvent polarity indicators,” J. Am. Chem. Soc. 73, 5330 (1951).
[CrossRef]

Cai, C.

Ch. Bosshard, F. Pan, M. S. Wong, S. Manetta, R. Spreiter, C. Cai, P. Günter, and V. Gramlich, “Nonlinear optical organic co-crystals of merocyanine dyes and phenolic derivatives with short hydrogen bonds,” Chem. Phys. 245, 377–394 (1999).
[CrossRef]

Chemla, D. S.

J. L. Oudar and D. S. Chemla, “Hyperpolarizabilities of the nitroanilines and their relations to the excited state dipole moment,” J. Chem. Phys. 66, 2664–2668 (1977).
[CrossRef]

Cheng, L.-T.

S. Marker, L.-T. Cheng, B. G. Tiemann, A. C. Friedli, M. Blanchard-Desce, J. W. Perry, and J. Sindhoj, “Large first hyperpolarizability in push-pull polyenes by tuning of the bond length alternation and aromaticity,” Science 263, 511–514 (1994).
[CrossRef]

Clays, K.

K. Clays and A. Persoons, “Hyper-Rayleigh scattering in solution,” Phys. Rev. Lett. 66, 2980–2983 (1991).
[CrossRef] [PubMed]

Diederich, F.

Ch. Bosshard, R. Spreiter, P. Günter, R. R. Tykwinski, M. Schreiber, and F. Diederich, “Structure–property relationships in nonlinear optical tetrathynylethenes,” Adv. Mater. 8, 231–234 (1996).
[CrossRef]

Donley, E. A.

Ph. Kaatz, E. A. Donley, and D. Shelton, “A comparison of molecular hyperpolarizabilities from gas and liquid phase measurements,” J. Chem. Phys. 108, 849–856 (1998).
[CrossRef]

Dulic, A.

A. Dulic and C. Flytzanis, “A new class of conjugated molecules with large second order polarizability,” Opt. Commun. 25, 402–406 (1978).
[CrossRef]

Flytzanis, C.

A. Dulic and C. Flytzanis, “A new class of conjugated molecules with large second order polarizability,” Opt. Commun. 25, 402–406 (1978).
[CrossRef]

Follonier, S.

F. Pan, G. Knöpfle, Ch. Bosshard, S. Follonier, R. Spreiter, M. S. Wong, and P. Günter, “Electro-optic properties of the organic salt 4-N, N-dimethylamino-4′-N′-methylstilbazolium tosylate,” Appl. Phys. Lett. 69, 13–15 (1996).
[CrossRef]

Friedli, A. C.

S. Marker, L.-T. Cheng, B. G. Tiemann, A. C. Friedli, M. Blanchard-Desce, J. W. Perry, and J. Sindhoj, “Large first hyperpolarizability in push-pull polyenes by tuning of the bond length alternation and aromaticity,” Science 263, 511–514 (1994).
[CrossRef]

Garito, A. F.

C. C. Teng and A. F. Garito, “Dispersion of the nonlinear second-order optical susceptibility of organic systems,” Phys. Rev. B 28, 6766–6773 (1983).
[CrossRef]

Gramlich, V.

Ch. Bosshard, F. Pan, M. S. Wong, S. Manetta, R. Spreiter, C. Cai, P. Günter, and V. Gramlich, “Nonlinear optical organic co-crystals of merocyanine dyes and phenolic derivatives with short hydrogen bonds,” Chem. Phys. 245, 377–394 (1999).
[CrossRef]

I. Liakatas, M. S. Wong, V. Gramlich, Ch. Bosshard, and P. Günter, “Novel, highly nonlinear optical molecular crystals based on multidonor-substituted 4-nitro-phenylhydrazones,” Adv. Mater. 10, 777–782 (1998).
[CrossRef]

Gubler, U.

Ch. Bosshard, U. Gubler, P. Kaatz, W. Mazerant, and U. Meier, “Non-phase-matched optical third-harmonic generation in noncentrosymmetric media: cascaded second-order contributions for the calibration of third-order nonlinearities,” Phys. Rev. B 61, 10688–10701 (2000).
[CrossRef]

U. Gubler and Ch. Bosshard, “Optical third-harmonic generation of fused silica in gas atmosphere: absolute value of the third-order susceptibility χ(3),” Phys. Rev. B 61, 10702–10710 (2000).
[CrossRef]

Günter, P.

Ch. Bosshard, F. Pan, M. S. Wong, S. Manetta, R. Spreiter, C. Cai, P. Günter, and V. Gramlich, “Nonlinear optical organic co-crystals of merocyanine dyes and phenolic derivatives with short hydrogen bonds,” Chem. Phys. 245, 377–394 (1999).
[CrossRef]

U. Meier, M. Bösch, Ch. Bosshard, F. Pan, and P. Günter, “Parametric interactions in the organic salt 4-N, N-dimethylamino-4′-N′-methyl-stilbazolium tosylate at telecommunication wavelengths,” J. Appl. Phys. 83, 3486–3489 (1998).
[CrossRef]

I. Liakatas, M. S. Wong, V. Gramlich, Ch. Bosshard, and P. Günter, “Novel, highly nonlinear optical molecular crystals based on multidonor-substituted 4-nitro-phenylhydrazones,” Adv. Mater. 10, 777–782 (1998).
[CrossRef]

M. S. Wong, F. Pan, M. Bösch, R. Spreiter, Ch. Bosshard, and P. Günter, “Novel electro-optic molecular co-crystals with ideal chromophoric orientation and large second-order nonlinearities,” J. Opt. Soc. Am. B 15, 426–431 (1998).
[CrossRef]

R. Spreiter, Ch. Bosshard, and P. Günter, “High frequency response and acoustic phonon contribution of the linear electro-optic effect in DAST,” Opt. Lett. 22, 564–566 (1997).
[CrossRef] [PubMed]

Ch. Bosshard, R. Spreiter, P. Günter, R. R. Tykwinski, M. Schreiber, and F. Diederich, “Structure–property relationships in nonlinear optical tetrathynylethenes,” Adv. Mater. 8, 231–234 (1996).
[CrossRef]

F. Pan, G. Knöpfle, Ch. Bosshard, S. Follonier, R. Spreiter, M. S. Wong, and P. Günter, “Electro-optic properties of the organic salt 4-N, N-dimethylamino-4′-N′-methylstilbazolium tosylate,” Appl. Phys. Lett. 69, 13–15 (1996).
[CrossRef]

Heseltine, D. W.

L. G. S. Brooker, G. H. Keyes, and D. W. Heseltine, “Color and constitution. XI. Anhydronium bases of p-hydroxystyryl dyes as solvent polarity indicators,” J. Am. Chem. Soc. 73, 5330 (1951).
[CrossRef]

Hierle, R.

Josse, D.

Kaatz, P.

Ch. Bosshard, U. Gubler, P. Kaatz, W. Mazerant, and U. Meier, “Non-phase-matched optical third-harmonic generation in noncentrosymmetric media: cascaded second-order contributions for the calibration of third-order nonlinearities,” Phys. Rev. B 61, 10688–10701 (2000).
[CrossRef]

Kaatz, Ph.

Ph. Kaatz, E. A. Donley, and D. Shelton, “A comparison of molecular hyperpolarizabilities from gas and liquid phase measurements,” J. Chem. Phys. 108, 849–856 (1998).
[CrossRef]

Keyes, G. H.

L. G. S. Brooker, G. H. Keyes, and D. W. Heseltine, “Color and constitution. XI. Anhydronium bases of p-hydroxystyryl dyes as solvent polarity indicators,” J. Am. Chem. Soc. 73, 5330 (1951).
[CrossRef]

Kielich, S.

S. Kielich, “Optical second-harmonic generation by electrically polarized isotropic media,” IEEE J. Quantum Electron. 5, 562–568 (1969).
[CrossRef]

Knöpfle, G.

F. Pan, G. Knöpfle, Ch. Bosshard, S. Follonier, R. Spreiter, M. S. Wong, and P. Günter, “Electro-optic properties of the organic salt 4-N, N-dimethylamino-4′-N′-methylstilbazolium tosylate,” Appl. Phys. Lett. 69, 13–15 (1996).
[CrossRef]

Kotler, Z.

Kurtz, H. A.

H. A. Kurtz, “Calculation of the nonlinear optical properties of molecules,” J. Comput. Chem. 11, 82 (1989).
[CrossRef]

Leenders, L.

B. F. Levine, C. G. Bethea, E. Wasserman, and L. Leenders, “Solvent dependent hyperpolarizability of a merocyanine dye,” J. Chem. Phys. 68, 5042–5045 (1978).
[CrossRef]

Levine, B. F.

B. F. Levine, C. G. Bethea, E. Wasserman, and L. Leenders, “Solvent dependent hyperpolarizability of a merocyanine dye,” J. Chem. Phys. 68, 5042–5045 (1978).
[CrossRef]

Liakatas, I.

I. Liakatas, M. S. Wong, V. Gramlich, Ch. Bosshard, and P. Günter, “Novel, highly nonlinear optical molecular crystals based on multidonor-substituted 4-nitro-phenylhydrazones,” Adv. Mater. 10, 777–782 (1998).
[CrossRef]

Maker, P. D.

R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurement of nonlinear light scattering,” Phys. Rev. Lett. 14, 681–684 (1965).
[CrossRef]

Manetta, S.

Ch. Bosshard, F. Pan, M. S. Wong, S. Manetta, R. Spreiter, C. Cai, P. Günter, and V. Gramlich, “Nonlinear optical organic co-crystals of merocyanine dyes and phenolic derivatives with short hydrogen bonds,” Chem. Phys. 245, 377–394 (1999).
[CrossRef]

Marker, S.

S. Marker, L.-T. Cheng, B. G. Tiemann, A. C. Friedli, M. Blanchard-Desce, J. W. Perry, and J. Sindhoj, “Large first hyperpolarizability in push-pull polyenes by tuning of the bond length alternation and aromaticity,” Science 263, 511–514 (1994).
[CrossRef]

Masse, R.

Mazerant, W.

Ch. Bosshard, U. Gubler, P. Kaatz, W. Mazerant, and U. Meier, “Non-phase-matched optical third-harmonic generation in noncentrosymmetric media: cascaded second-order contributions for the calibration of third-order nonlinearities,” Phys. Rev. B 61, 10688–10701 (2000).
[CrossRef]

Meier, U.

Ch. Bosshard, U. Gubler, P. Kaatz, W. Mazerant, and U. Meier, “Non-phase-matched optical third-harmonic generation in noncentrosymmetric media: cascaded second-order contributions for the calibration of third-order nonlinearities,” Phys. Rev. B 61, 10688–10701 (2000).
[CrossRef]

U. Meier, M. Bösch, Ch. Bosshard, F. Pan, and P. Günter, “Parametric interactions in the organic salt 4-N, N-dimethylamino-4′-N′-methyl-stilbazolium tosylate at telecommunication wavelengths,” J. Appl. Phys. 83, 3486–3489 (1998).
[CrossRef]

Oudar, J. L.

J. Zyss and J. L. Oudar, “Relation between microscopic and macroscopic low-order optical nonlinearities of molecular crystals with one- or two-dimensional units,” Phys. Rev. A 26, 2028–2048 (1982).
[CrossRef]

J. L. Oudar and D. S. Chemla, “Hyperpolarizabilities of the nitroanilines and their relations to the excited state dipole moment,” J. Chem. Phys. 66, 2664–2668 (1977).
[CrossRef]

Pan, F.

Ch. Bosshard, F. Pan, M. S. Wong, S. Manetta, R. Spreiter, C. Cai, P. Günter, and V. Gramlich, “Nonlinear optical organic co-crystals of merocyanine dyes and phenolic derivatives with short hydrogen bonds,” Chem. Phys. 245, 377–394 (1999).
[CrossRef]

U. Meier, M. Bösch, Ch. Bosshard, F. Pan, and P. Günter, “Parametric interactions in the organic salt 4-N, N-dimethylamino-4′-N′-methyl-stilbazolium tosylate at telecommunication wavelengths,” J. Appl. Phys. 83, 3486–3489 (1998).
[CrossRef]

M. S. Wong, F. Pan, M. Bösch, R. Spreiter, Ch. Bosshard, and P. Günter, “Novel electro-optic molecular co-crystals with ideal chromophoric orientation and large second-order nonlinearities,” J. Opt. Soc. Am. B 15, 426–431 (1998).
[CrossRef]

F. Pan, G. Knöpfle, Ch. Bosshard, S. Follonier, R. Spreiter, M. S. Wong, and P. Günter, “Electro-optic properties of the organic salt 4-N, N-dimethylamino-4′-N′-methylstilbazolium tosylate,” Appl. Phys. Lett. 69, 13–15 (1996).
[CrossRef]

Perry, J. W.

S. Marker, L.-T. Cheng, B. G. Tiemann, A. C. Friedli, M. Blanchard-Desce, J. W. Perry, and J. Sindhoj, “Large first hyperpolarizability in push-pull polyenes by tuning of the bond length alternation and aromaticity,” Science 263, 511–514 (1994).
[CrossRef]

Persoons, A.

K. Clays and A. Persoons, “Hyper-Rayleigh scattering in solution,” Phys. Rev. Lett. 66, 2980–2983 (1991).
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R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurement of nonlinear light scattering,” Phys. Rev. Lett. 14, 681–684 (1965).
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Ch. Bosshard, R. Spreiter, P. Günter, R. R. Tykwinski, M. Schreiber, and F. Diederich, “Structure–property relationships in nonlinear optical tetrathynylethenes,” Adv. Mater. 8, 231–234 (1996).
[CrossRef]

Shelton, D.

Ph. Kaatz, E. A. Donley, and D. Shelton, “A comparison of molecular hyperpolarizabilities from gas and liquid phase measurements,” J. Chem. Phys. 108, 849–856 (1998).
[CrossRef]

Sindhoj, J.

S. Marker, L.-T. Cheng, B. G. Tiemann, A. C. Friedli, M. Blanchard-Desce, J. W. Perry, and J. Sindhoj, “Large first hyperpolarizability in push-pull polyenes by tuning of the bond length alternation and aromaticity,” Science 263, 511–514 (1994).
[CrossRef]

Spreiter, R.

Ch. Bosshard, F. Pan, M. S. Wong, S. Manetta, R. Spreiter, C. Cai, P. Günter, and V. Gramlich, “Nonlinear optical organic co-crystals of merocyanine dyes and phenolic derivatives with short hydrogen bonds,” Chem. Phys. 245, 377–394 (1999).
[CrossRef]

M. S. Wong, F. Pan, M. Bösch, R. Spreiter, Ch. Bosshard, and P. Günter, “Novel electro-optic molecular co-crystals with ideal chromophoric orientation and large second-order nonlinearities,” J. Opt. Soc. Am. B 15, 426–431 (1998).
[CrossRef]

R. Spreiter, Ch. Bosshard, and P. Günter, “High frequency response and acoustic phonon contribution of the linear electro-optic effect in DAST,” Opt. Lett. 22, 564–566 (1997).
[CrossRef] [PubMed]

Ch. Bosshard, R. Spreiter, P. Günter, R. R. Tykwinski, M. Schreiber, and F. Diederich, “Structure–property relationships in nonlinear optical tetrathynylethenes,” Adv. Mater. 8, 231–234 (1996).
[CrossRef]

F. Pan, G. Knöpfle, Ch. Bosshard, S. Follonier, R. Spreiter, M. S. Wong, and P. Günter, “Electro-optic properties of the organic salt 4-N, N-dimethylamino-4′-N′-methylstilbazolium tosylate,” Appl. Phys. Lett. 69, 13–15 (1996).
[CrossRef]

Teng, C. C.

C. C. Teng and A. F. Garito, “Dispersion of the nonlinear second-order optical susceptibility of organic systems,” Phys. Rev. B 28, 6766–6773 (1983).
[CrossRef]

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R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurement of nonlinear light scattering,” Phys. Rev. Lett. 14, 681–684 (1965).
[CrossRef]

Tiemann, B. G.

S. Marker, L.-T. Cheng, B. G. Tiemann, A. C. Friedli, M. Blanchard-Desce, J. W. Perry, and J. Sindhoj, “Large first hyperpolarizability in push-pull polyenes by tuning of the bond length alternation and aromaticity,” Science 263, 511–514 (1994).
[CrossRef]

Tykwinski, R. R.

Ch. Bosshard, R. Spreiter, P. Günter, R. R. Tykwinski, M. Schreiber, and F. Diederich, “Structure–property relationships in nonlinear optical tetrathynylethenes,” Adv. Mater. 8, 231–234 (1996).
[CrossRef]

Wasserman, E.

B. F. Levine, C. G. Bethea, E. Wasserman, and L. Leenders, “Solvent dependent hyperpolarizability of a merocyanine dye,” J. Chem. Phys. 68, 5042–5045 (1978).
[CrossRef]

Wong, M. S.

Ch. Bosshard, F. Pan, M. S. Wong, S. Manetta, R. Spreiter, C. Cai, P. Günter, and V. Gramlich, “Nonlinear optical organic co-crystals of merocyanine dyes and phenolic derivatives with short hydrogen bonds,” Chem. Phys. 245, 377–394 (1999).
[CrossRef]

I. Liakatas, M. S. Wong, V. Gramlich, Ch. Bosshard, and P. Günter, “Novel, highly nonlinear optical molecular crystals based on multidonor-substituted 4-nitro-phenylhydrazones,” Adv. Mater. 10, 777–782 (1998).
[CrossRef]

M. S. Wong, F. Pan, M. Bösch, R. Spreiter, Ch. Bosshard, and P. Günter, “Novel electro-optic molecular co-crystals with ideal chromophoric orientation and large second-order nonlinearities,” J. Opt. Soc. Am. B 15, 426–431 (1998).
[CrossRef]

F. Pan, G. Knöpfle, Ch. Bosshard, S. Follonier, R. Spreiter, M. S. Wong, and P. Günter, “Electro-optic properties of the organic salt 4-N, N-dimethylamino-4′-N′-methylstilbazolium tosylate,” Appl. Phys. Lett. 69, 13–15 (1996).
[CrossRef]

Zyss, J.

Z. Kotler, R. Hierle, D. Josse, J. Zyss, and R. Masse, “Quadratic nonlinear optical properties of a transparent and highly efficient organic-inorganic crystal: 2-amino-5-nitropyridinium dihydrogen phosphate (2A5NPDP),” J. Opt. Soc. Am. B 9, 534–547 (1992).
[CrossRef]

J. Zyss and J. L. Oudar, “Relation between microscopic and macroscopic low-order optical nonlinearities of molecular crystals with one- or two-dimensional units,” Phys. Rev. A 26, 2028–2048 (1982).
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J. Zyss, “Hyperpolarizabilities of substituted conjugated molecules. I. Perturbated INDO approach to monosubstituted benzene,” J. Chem. Phys. 70, 3333–3340 (1979).
[CrossRef]

Adv. Mater.

I. Liakatas, M. S. Wong, V. Gramlich, Ch. Bosshard, and P. Günter, “Novel, highly nonlinear optical molecular crystals based on multidonor-substituted 4-nitro-phenylhydrazones,” Adv. Mater. 10, 777–782 (1998).
[CrossRef]

Ch. Bosshard, R. Spreiter, P. Günter, R. R. Tykwinski, M. Schreiber, and F. Diederich, “Structure–property relationships in nonlinear optical tetrathynylethenes,” Adv. Mater. 8, 231–234 (1996).
[CrossRef]

Appl. Phys. Lett.

F. Pan, G. Knöpfle, Ch. Bosshard, S. Follonier, R. Spreiter, M. S. Wong, and P. Günter, “Electro-optic properties of the organic salt 4-N, N-dimethylamino-4′-N′-methylstilbazolium tosylate,” Appl. Phys. Lett. 69, 13–15 (1996).
[CrossRef]

Chem. Phys.

Ch. Bosshard, F. Pan, M. S. Wong, S. Manetta, R. Spreiter, C. Cai, P. Günter, and V. Gramlich, “Nonlinear optical organic co-crystals of merocyanine dyes and phenolic derivatives with short hydrogen bonds,” Chem. Phys. 245, 377–394 (1999).
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U. Meier, M. Bösch, Ch. Bosshard, F. Pan, and P. Günter, “Parametric interactions in the organic salt 4-N, N-dimethylamino-4′-N′-methyl-stilbazolium tosylate at telecommunication wavelengths,” J. Appl. Phys. 83, 3486–3489 (1998).
[CrossRef]

J. Chem. Phys.

B. F. Levine, C. G. Bethea, E. Wasserman, and L. Leenders, “Solvent dependent hyperpolarizability of a merocyanine dye,” J. Chem. Phys. 68, 5042–5045 (1978).
[CrossRef]

J. L. Oudar and D. S. Chemla, “Hyperpolarizabilities of the nitroanilines and their relations to the excited state dipole moment,” J. Chem. Phys. 66, 2664–2668 (1977).
[CrossRef]

J. Zyss, “Hyperpolarizabilities of substituted conjugated molecules. I. Perturbated INDO approach to monosubstituted benzene,” J. Chem. Phys. 70, 3333–3340 (1979).
[CrossRef]

Ph. Kaatz, E. A. Donley, and D. Shelton, “A comparison of molecular hyperpolarizabilities from gas and liquid phase measurements,” J. Chem. Phys. 108, 849–856 (1998).
[CrossRef]

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Opt. Lett.

Phys. Rev. A

J. Zyss and J. L. Oudar, “Relation between microscopic and macroscopic low-order optical nonlinearities of molecular crystals with one- or two-dimensional units,” Phys. Rev. A 26, 2028–2048 (1982).
[CrossRef]

Phys. Rev. B

C. C. Teng and A. F. Garito, “Dispersion of the nonlinear second-order optical susceptibility of organic systems,” Phys. Rev. B 28, 6766–6773 (1983).
[CrossRef]

Ch. Bosshard, U. Gubler, P. Kaatz, W. Mazerant, and U. Meier, “Non-phase-matched optical third-harmonic generation in noncentrosymmetric media: cascaded second-order contributions for the calibration of third-order nonlinearities,” Phys. Rev. B 61, 10688–10701 (2000).
[CrossRef]

U. Gubler and Ch. Bosshard, “Optical third-harmonic generation of fused silica in gas atmosphere: absolute value of the third-order susceptibility χ(3),” Phys. Rev. B 61, 10702–10710 (2000).
[CrossRef]

Phys. Rev. Lett.

R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurement of nonlinear light scattering,” Phys. Rev. Lett. 14, 681–684 (1965).
[CrossRef]

K. Clays and A. Persoons, “Hyper-Rayleigh scattering in solution,” Phys. Rev. Lett. 66, 2980–2983 (1991).
[CrossRef] [PubMed]

Science

S. Marker, L.-T. Cheng, B. G. Tiemann, A. C. Friedli, M. Blanchard-Desce, J. W. Perry, and J. Sindhoj, “Large first hyperpolarizability in push-pull polyenes by tuning of the bond length alternation and aromaticity,” Science 263, 511–514 (1994).
[CrossRef]

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[CrossRef]

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Figures (6)

Fig. 1
Fig. 1

(a) Molecular units of the ionic DAST crystal. The negatively charged tosylate and the positively charged, nonlinear optical chromophore stilbazolium. (b) The molecules are shown as they are embedded in the crystal lattice.

Fig. 2
Fig. 2

(a) Resonance structures of the merocyanine dyes M1 and M2. (A) is the quinoid form and (B) is the zwitterionic form. (b) Molecular units of M2-MDB. The MDB guest molecule (right) and the nonlinear optical modified merocyanine chromophore (left) form a molecular aggregate by building a very short hydrogen bond. (c) The molecules as they are arranged in the crystal lattice.

Fig. 3
Fig. 3

Measured dependence of the third-order susceptibility ΓL of M2, M2-MDB, and M1 on the chromophore weight fraction in methanol.

Fig. 4
Fig. 4

Experimental setup for the HRS experiment. The scattered second-harmonic power is measured as a function of the fundamental power.

Fig. 5
Fig. 5

Typical measurement of a solution of 0.8 wt. % DAST in the solvent DMSO heated to 50 °C. Shown are the calculated contributions from second-harmonic generation and three-photon-induced luminescence.

Fig. 6
Fig. 6

Second-harmonic signal of DAST in DMSO versus concentration. The second-harmonic intensity is relative to that of DR1 in a 1.0 wt % solution in dioxane.

Tables (4)

Tables Icon

Table 1 Measured First-Order Hyperpolarizabilities of the Merocyanine Dyes at λ = 1907 nm and DAST at λ = 1542 nma

Tables Icon

Table 2 Calculated First-Order Hyperpolarizabilities βMOPAC and Absolute Values of the Experimental First-Order Hyperpolarizabilities Extrapolated to Infinite Wavelengths and Multiplied by 6/5 to Convert to the Calculated Values [see Eq. (8)]

Tables Icon

Table 3 Measured Nonlinear Optical Coefficients d111 (at λ = 1542 nm) and Wavelength of Maximum Absorption of DAST and M2-MDB (Phases I and II) in the Solid State Derived from the Dispersion of the Refractive Indicesa

Tables Icon

Table 4 Comparison of the First-Order Hyperpolarizabilities of DAST and M2-MDB in Solution and in the Solid Statea

Equations (8)

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

pi(t)=μi+0[αijE˜j(t)+βijkE˜j(t)E˜k(t)+γijklE˜j(t)E˜k(t)E˜l(t)+],
βzzz(-2ω, ω, ω)=ωeg4(ωeg2-ω2)(ωeg2-4ω2)β0
dijk(-2ω, ω ω)=12χijk(-2ω, ω ω)=12Nn(g)fi2ωfjωfkωsn(g)lmn3cos θils cos θjms×cos θknsβlmn(-2ω, ω, ω).
βzzz=βzzzref(fωref)2(f2ωref)(fω)2(f2ω)I2ωNrefI2ωrefN,
I2ω(Iω)=a2Iω2+a3Iω3.
βzzz21/2DAST=(1.34±0.2)×βzzz21/2DRI.
βzzz=(1540±250)×10-40 m4/V.
βMOPAC=65β0Exp.

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