OSA's Digital Library

Journal of the Optical Society of America B

Journal of the Optical Society of America B


  • Vol. 18, Iss. 11 — Nov. 1, 2001
  • pp: 1620–1626

Microscopic nonlinearities of two-component organic crystals

Christian Bosshard, Rolf Spreiter, and Peter Günter  »View Author Affiliations

JOSA B, Vol. 18, Issue 11, pp. 1620-1626 (2001)

View Full Text Article

Enhanced HTML    Acrobat PDF (251 KB)

Browse Journals / Lookup Meetings

Browse by Journal and Year


Lookup Conference Papers

Close Browse Journals / Lookup Meetings

Article Tools



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

OCIS Codes
(160.4330) Materials : Nonlinear optical materials
(160.4890) Materials : Organic materials
(190.4400) Nonlinear optics : Nonlinear optics, materials
(190.4710) Nonlinear optics : Optical nonlinearities in organic materials

Christian Bosshard, Rolf Spreiter, and Peter Günter, "Microscopic nonlinearities of two-component organic crystals," J. Opt. Soc. Am. B 18, 1620-1626 (2001)

Sort:  Author  |  Year  |  Journal  |  Reset  


  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]
  7. C. J. Boettcher, Theory of Electric Polarization (Elsevier, Amsterdam, 1952).
  8. 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]
  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). [CrossRef]
  15. H. A. Kurtz, “Calculation of the nonlinear optical properties of molecules,” J. Comput. Chem. 11, 82 (1989). [CrossRef]
  16. Ch. Bosshard, M. Bösch, I. Liakatas, M. Jäger, and P. Günter, “Second-order nonlinear optical organic materials: recent developments,” in Nonlinear Optical Effects and Materials, P. Günter, eds., Vol. 72 of Springer Series in Optical Sciences (Springer Verlag, New York, 2000), pp. 163–299. [CrossRef]
  17. 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]
  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]
  21. Ch. Bosshard, “Third-order nonlinear optics in polar materials,” in Nonlinear Optical Effects and Materials, P. Günter, ed., Vol. 72 of Springer Series in Optical Sciences (Springer Verlag, New York, 2000), pp. 7–161.
  22. 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]
  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]

Cited By

Alert me when this paper is cited

OSA is able to provide readers links to articles that cite this paper by participating in CrossRef's Cited-By Linking service. CrossRef includes content from more than 3000 publishers and societies. In addition to listing OSA journal articles that cite this paper, citing articles from other participating publishers will also be listed.

« Previous Article  |  Next Article »

OSA is a member of CrossRef.

CrossCheck Deposited