Abstract

We performed a detailed experimental investigation and quantum-chemical analysis of two-photon absorption (2PA) spectra of a series of symmetrical cationic polymethines and neutral squaraines having similar structures. Degenerate 2PA spectra of these molecules are taken by using two-photon fluorescence spectroscopy and the Z-scan technique. All measurements are made with 150fs laser pulses of 1kHz repetition rate in the tuning range of 5202100nm (0.62.4eV). Comparing 2PA spectra of polymethines and squaraines, we find that we can access considerably larger 2PA cross sections (8600×1050cm4s/photon) in the squaraines owing to narrower linear absorption spectra and an increase in the density of unoccupied molecular orbitals introduced by the squaraine acceptor group in the conjugated chain.

© 2006 Optical Society of America

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  1. S. R. Marder, "Organic nonlinear optical materials: where we have been and where we are going," Chem. Commun. (Cambridge) 2006, 131-134.
  2. M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
    [CrossRef] [PubMed]
  3. T. Kogej, D. Beljonne, F. Meyers, J. W. Perry, S. R. Marder, and J. L. Bredas, "Mechanisms for enhancement of two-photon absorption in donor-acceptor conjugated chromophores," Chem. Phys. Lett. 298, 1-3 (1998).
    [CrossRef]
  4. M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
    [CrossRef]
  5. G. S. He, T.-C. Lin, J. Dai, P. N. Prasad, R. Kannan, A. G. Dombroskie, R. A. Vaia, and L.-S. Tan, "Degenerate two-photon-absorption spectral studies of highly two-photon active organic chromophores," J. Chem. Phys. 120, 5275-5284 (2004).
    [CrossRef] [PubMed]
  6. C.-K. Wang, P. Macak, Y. Luo, and H. Agren, "Effects of π centers and symmetry on two-photon absorption cross sections of organic chromophores," J. Chem. Phys. 114, 9813-9820 (2001).
    [CrossRef]
  7. E. Zojer, D. Beljonne, T. Kogej, H. Vogel, S. R. Marder, J. W. Perry, and J. L. Bredas, "Tuning the two-photon absorption response of quadrupolar organic molecules," J. Chem. Phys. 116, 3646-3658 (2002).
    [CrossRef]
  8. E. Zojer, D. Beljonne, P. Pacher, and J. L. Bredas, "Two-photon absorption in quadrupolar π-conjugated molecules: influence of the nature of the conjugated bridge and the donor-acceptor separation," Chem.-Eur. J. 10, 2668-2680 (2004).
    [CrossRef] [PubMed]
  9. R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Excited-state absorption dynamics in polymethine dyes detected by polarization-resolved pump-probe measurements," Chem. Phys. 286, 277-291 (2003).
    [CrossRef]
  10. J. M. Hales, D. J. Hagan, E. W. Van Stryland, K. J. Schafer, A. R. Morales, K. D. Belfield, P. Pacher, O. Kwon, E. Zojer, and J. L. Bredas, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," J. Chem. Phys. 121, 3152-3160 (2004).
    [CrossRef] [PubMed]
  11. M. Hamer, The Cyanine Dyes and Related Compounds (Interscience, 1964).
  12. J. R. Lakowicz, Principles of Fluorescence Spectroscopy (Kluwer Academic/Plenum, 1999).
  13. C. Xu and W. W. Webb, "Measurement of two-photon excitation cross sections of molecular fluorophores with data from 690to1050 nm," J. Opt. Soc. Am. B 13, 481-491 (1996).
    [CrossRef]
  14. M. Fisher and J. Georges, "Fluorescence quantum yield of Rhodamine 6G in ethanol as a function of concentration using thermal lens spectrometry," Chem. Phys. Lett. 260, 115-118 (1996).
    [CrossRef]
  15. M. Sheik-Bahae, A. A. Said, and E. W. Van Stryland, "High-sensitivity, single-beam n2 measurements," Opt. Lett. 14, 955-957 (1989).
    [CrossRef] [PubMed]
  16. M. Sheik-Bahae, A. A. Said, T.-H. Wei, D. R. Hagan, and E. W. Van Stryland, "Sensitive measurement of optical nonlinearities using a single beam," IEEE J. Quantum Electron. 26, 760-769 (1990).
    [CrossRef]
  17. T. H. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, "Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines," Appl. Phys. B 54, 46-51 (1992).
    [CrossRef]
  18. R. A. Negras, J. M. Hales, A. Kobyakov, D. J. Hagan, and E. W. Van Stryland, "Experiment and analysis of two-photon absorption spectroscopy using a white-light continuum probe," IEEE J. Quantum Electron. 38, 1205-1216 (2002).
    [CrossRef]
  19. M. J. S. Dewar, The Molecular Orbital Theory of Organic Chemistry (McGraw-Hill, 1969).
  20. J. S. Craw, J. R. Reimers, G. B. Bacskay, A. T. Wong, and N. S. Hush, "Solitons in finite- and infinite-length negative-defect trans-polyacetylene and the corresponding Brooker (polymethinecyanine) cations," Chem. Phys. 167, 77-99 (1992).
    [CrossRef]
  21. D. Scherer, R. Dorfler, A. Feldner, T. Vogtmann, M. Schwoerer, U. Lawrentz, W. Grahn, and C. Lambert, "Two-photon states in squaraine monomers and oligomers," Chem. Phys. 279, 179-207 (2002).
    [CrossRef]
  22. J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Two-photon anisotropy: analytical description and molecular modeling for symmetrical and asymmetrical organic dyes," Chem. Phys. 321, 257-268 (2006).
    [CrossRef]
  23. J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, unpublished results.
  24. K. Kamada, K. Ohta, Y. Iwase, and K. Kondo, "Two-photon absorption properties of symmetric substituted diacetylene: drastic enhancement of the cross section near the one-photon absorption peak," Chem. Phys. Lett. 372, 386-393 (2003).
    [CrossRef]
  25. J. P. Moreno and M. G. Kuzyk, "Fundamental limits of the dispersion of the two-photon absorption cross section," J. Chem. Phys. 123, 194101-194113 (2005).
    [CrossRef]
  26. B. J. Orr and J. F. Ward, "Perturbation theory of the non-linear optical polarization of an isolated system," Mol. Phys. 20, 513-526 (1971).
    [CrossRef]
  27. M. G. Kuzyk, "Fundamental limits on two-photon absorption cross sections," J. Chem. Phys. 119, 8327-8334 (2003).
    [CrossRef]

2006 (1)

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Two-photon anisotropy: analytical description and molecular modeling for symmetrical and asymmetrical organic dyes," Chem. Phys. 321, 257-268 (2006).
[CrossRef]

2005 (1)

J. P. Moreno and M. G. Kuzyk, "Fundamental limits of the dispersion of the two-photon absorption cross section," J. Chem. Phys. 123, 194101-194113 (2005).
[CrossRef]

2004 (3)

G. S. He, T.-C. Lin, J. Dai, P. N. Prasad, R. Kannan, A. G. Dombroskie, R. A. Vaia, and L.-S. Tan, "Degenerate two-photon-absorption spectral studies of highly two-photon active organic chromophores," J. Chem. Phys. 120, 5275-5284 (2004).
[CrossRef] [PubMed]

E. Zojer, D. Beljonne, P. Pacher, and J. L. Bredas, "Two-photon absorption in quadrupolar π-conjugated molecules: influence of the nature of the conjugated bridge and the donor-acceptor separation," Chem.-Eur. J. 10, 2668-2680 (2004).
[CrossRef] [PubMed]

J. M. Hales, D. J. Hagan, E. W. Van Stryland, K. J. Schafer, A. R. Morales, K. D. Belfield, P. Pacher, O. Kwon, E. Zojer, and J. L. Bredas, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," J. Chem. Phys. 121, 3152-3160 (2004).
[CrossRef] [PubMed]

2003 (3)

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Excited-state absorption dynamics in polymethine dyes detected by polarization-resolved pump-probe measurements," Chem. Phys. 286, 277-291 (2003).
[CrossRef]

K. Kamada, K. Ohta, Y. Iwase, and K. Kondo, "Two-photon absorption properties of symmetric substituted diacetylene: drastic enhancement of the cross section near the one-photon absorption peak," Chem. Phys. Lett. 372, 386-393 (2003).
[CrossRef]

M. G. Kuzyk, "Fundamental limits on two-photon absorption cross sections," J. Chem. Phys. 119, 8327-8334 (2003).
[CrossRef]

2002 (3)

D. Scherer, R. Dorfler, A. Feldner, T. Vogtmann, M. Schwoerer, U. Lawrentz, W. Grahn, and C. Lambert, "Two-photon states in squaraine monomers and oligomers," Chem. Phys. 279, 179-207 (2002).
[CrossRef]

E. Zojer, D. Beljonne, T. Kogej, H. Vogel, S. R. Marder, J. W. Perry, and J. L. Bredas, "Tuning the two-photon absorption response of quadrupolar organic molecules," J. Chem. Phys. 116, 3646-3658 (2002).
[CrossRef]

R. A. Negras, J. M. Hales, A. Kobyakov, D. J. Hagan, and E. W. Van Stryland, "Experiment and analysis of two-photon absorption spectroscopy using a white-light continuum probe," IEEE J. Quantum Electron. 38, 1205-1216 (2002).
[CrossRef]

2001 (1)

C.-K. Wang, P. Macak, Y. Luo, and H. Agren, "Effects of π centers and symmetry on two-photon absorption cross sections of organic chromophores," J. Chem. Phys. 114, 9813-9820 (2001).
[CrossRef]

2000 (1)

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

1998 (2)

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

T. Kogej, D. Beljonne, F. Meyers, J. W. Perry, S. R. Marder, and J. L. Bredas, "Mechanisms for enhancement of two-photon absorption in donor-acceptor conjugated chromophores," Chem. Phys. Lett. 298, 1-3 (1998).
[CrossRef]

1996 (2)

C. Xu and W. W. Webb, "Measurement of two-photon excitation cross sections of molecular fluorophores with data from 690to1050 nm," J. Opt. Soc. Am. B 13, 481-491 (1996).
[CrossRef]

M. Fisher and J. Georges, "Fluorescence quantum yield of Rhodamine 6G in ethanol as a function of concentration using thermal lens spectrometry," Chem. Phys. Lett. 260, 115-118 (1996).
[CrossRef]

1992 (2)

J. S. Craw, J. R. Reimers, G. B. Bacskay, A. T. Wong, and N. S. Hush, "Solitons in finite- and infinite-length negative-defect trans-polyacetylene and the corresponding Brooker (polymethinecyanine) cations," Chem. Phys. 167, 77-99 (1992).
[CrossRef]

T. H. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, "Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines," Appl. Phys. B 54, 46-51 (1992).
[CrossRef]

1990 (1)

M. Sheik-Bahae, A. A. Said, T.-H. Wei, D. R. Hagan, and E. W. Van Stryland, "Sensitive measurement of optical nonlinearities using a single beam," IEEE J. Quantum Electron. 26, 760-769 (1990).
[CrossRef]

1989 (1)

1971 (1)

B. J. Orr and J. F. Ward, "Perturbation theory of the non-linear optical polarization of an isolated system," Mol. Phys. 20, 513-526 (1971).
[CrossRef]

Agren, H.

C.-K. Wang, P. Macak, Y. Luo, and H. Agren, "Effects of π centers and symmetry on two-photon absorption cross sections of organic chromophores," J. Chem. Phys. 114, 9813-9820 (2001).
[CrossRef]

Albota, M.

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Bacskay, G. B.

J. S. Craw, J. R. Reimers, G. B. Bacskay, A. T. Wong, and N. S. Hush, "Solitons in finite- and infinite-length negative-defect trans-polyacetylene and the corresponding Brooker (polymethinecyanine) cations," Chem. Phys. 167, 77-99 (1992).
[CrossRef]

Barlow, S.

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

Belfield, K. D.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Two-photon anisotropy: analytical description and molecular modeling for symmetrical and asymmetrical organic dyes," Chem. Phys. 321, 257-268 (2006).
[CrossRef]

J. M. Hales, D. J. Hagan, E. W. Van Stryland, K. J. Schafer, A. R. Morales, K. D. Belfield, P. Pacher, O. Kwon, E. Zojer, and J. L. Bredas, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," J. Chem. Phys. 121, 3152-3160 (2004).
[CrossRef] [PubMed]

Beljonne, D.

E. Zojer, D. Beljonne, P. Pacher, and J. L. Bredas, "Two-photon absorption in quadrupolar π-conjugated molecules: influence of the nature of the conjugated bridge and the donor-acceptor separation," Chem.-Eur. J. 10, 2668-2680 (2004).
[CrossRef] [PubMed]

E. Zojer, D. Beljonne, T. Kogej, H. Vogel, S. R. Marder, J. W. Perry, and J. L. Bredas, "Tuning the two-photon absorption response of quadrupolar organic molecules," J. Chem. Phys. 116, 3646-3658 (2002).
[CrossRef]

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

T. Kogej, D. Beljonne, F. Meyers, J. W. Perry, S. R. Marder, and J. L. Bredas, "Mechanisms for enhancement of two-photon absorption in donor-acceptor conjugated chromophores," Chem. Phys. Lett. 298, 1-3 (1998).
[CrossRef]

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Bondar, M. V.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Two-photon anisotropy: analytical description and molecular modeling for symmetrical and asymmetrical organic dyes," Chem. Phys. 321, 257-268 (2006).
[CrossRef]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Excited-state absorption dynamics in polymethine dyes detected by polarization-resolved pump-probe measurements," Chem. Phys. 286, 277-291 (2003).
[CrossRef]

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, unpublished results.

Bredas, J. L.

J. M. Hales, D. J. Hagan, E. W. Van Stryland, K. J. Schafer, A. R. Morales, K. D. Belfield, P. Pacher, O. Kwon, E. Zojer, and J. L. Bredas, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," J. Chem. Phys. 121, 3152-3160 (2004).
[CrossRef] [PubMed]

E. Zojer, D. Beljonne, P. Pacher, and J. L. Bredas, "Two-photon absorption in quadrupolar π-conjugated molecules: influence of the nature of the conjugated bridge and the donor-acceptor separation," Chem.-Eur. J. 10, 2668-2680 (2004).
[CrossRef] [PubMed]

E. Zojer, D. Beljonne, T. Kogej, H. Vogel, S. R. Marder, J. W. Perry, and J. L. Bredas, "Tuning the two-photon absorption response of quadrupolar organic molecules," J. Chem. Phys. 116, 3646-3658 (2002).
[CrossRef]

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

T. Kogej, D. Beljonne, F. Meyers, J. W. Perry, S. R. Marder, and J. L. Bredas, "Mechanisms for enhancement of two-photon absorption in donor-acceptor conjugated chromophores," Chem. Phys. Lett. 298, 1-3 (1998).
[CrossRef]

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Coulter, D. R.

T. H. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, "Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines," Appl. Phys. B 54, 46-51 (1992).
[CrossRef]

Craw, J. S.

J. S. Craw, J. R. Reimers, G. B. Bacskay, A. T. Wong, and N. S. Hush, "Solitons in finite- and infinite-length negative-defect trans-polyacetylene and the corresponding Brooker (polymethinecyanine) cations," Chem. Phys. 167, 77-99 (1992).
[CrossRef]

Dai, J.

G. S. He, T.-C. Lin, J. Dai, P. N. Prasad, R. Kannan, A. G. Dombroskie, R. A. Vaia, and L.-S. Tan, "Degenerate two-photon-absorption spectral studies of highly two-photon active organic chromophores," J. Chem. Phys. 120, 5275-5284 (2004).
[CrossRef] [PubMed]

Dewar, M. J. S.

M. J. S. Dewar, The Molecular Orbital Theory of Organic Chemistry (McGraw-Hill, 1969).

Dombroskie, A. G.

G. S. He, T.-C. Lin, J. Dai, P. N. Prasad, R. Kannan, A. G. Dombroskie, R. A. Vaia, and L.-S. Tan, "Degenerate two-photon-absorption spectral studies of highly two-photon active organic chromophores," J. Chem. Phys. 120, 5275-5284 (2004).
[CrossRef] [PubMed]

Dorfler, R.

D. Scherer, R. Dorfler, A. Feldner, T. Vogtmann, M. Schwoerer, U. Lawrentz, W. Grahn, and C. Lambert, "Two-photon states in squaraine monomers and oligomers," Chem. Phys. 279, 179-207 (2002).
[CrossRef]

Ehrlich, J. E.

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Feldner, A.

D. Scherer, R. Dorfler, A. Feldner, T. Vogtmann, M. Schwoerer, U. Lawrentz, W. Grahn, and C. Lambert, "Two-photon states in squaraine monomers and oligomers," Chem. Phys. 279, 179-207 (2002).
[CrossRef]

Fisher, M.

M. Fisher and J. Georges, "Fluorescence quantum yield of Rhodamine 6G in ethanol as a function of concentration using thermal lens spectrometry," Chem. Phys. Lett. 260, 115-118 (1996).
[CrossRef]

Fu, J.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Two-photon anisotropy: analytical description and molecular modeling for symmetrical and asymmetrical organic dyes," Chem. Phys. 321, 257-268 (2006).
[CrossRef]

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, unpublished results.

Fu, J.-Y.

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Georges, J.

M. Fisher and J. Georges, "Fluorescence quantum yield of Rhodamine 6G in ethanol as a function of concentration using thermal lens spectrometry," Chem. Phys. Lett. 260, 115-118 (1996).
[CrossRef]

Grahn, W.

D. Scherer, R. Dorfler, A. Feldner, T. Vogtmann, M. Schwoerer, U. Lawrentz, W. Grahn, and C. Lambert, "Two-photon states in squaraine monomers and oligomers," Chem. Phys. 279, 179-207 (2002).
[CrossRef]

Hagan, D. J.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Two-photon anisotropy: analytical description and molecular modeling for symmetrical and asymmetrical organic dyes," Chem. Phys. 321, 257-268 (2006).
[CrossRef]

J. M. Hales, D. J. Hagan, E. W. Van Stryland, K. J. Schafer, A. R. Morales, K. D. Belfield, P. Pacher, O. Kwon, E. Zojer, and J. L. Bredas, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," J. Chem. Phys. 121, 3152-3160 (2004).
[CrossRef] [PubMed]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Excited-state absorption dynamics in polymethine dyes detected by polarization-resolved pump-probe measurements," Chem. Phys. 286, 277-291 (2003).
[CrossRef]

R. A. Negras, J. M. Hales, A. Kobyakov, D. J. Hagan, and E. W. Van Stryland, "Experiment and analysis of two-photon absorption spectroscopy using a white-light continuum probe," IEEE J. Quantum Electron. 38, 1205-1216 (2002).
[CrossRef]

T. H. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, "Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines," Appl. Phys. B 54, 46-51 (1992).
[CrossRef]

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, unpublished results.

Hagan, D. R.

M. Sheik-Bahae, A. A. Said, T.-H. Wei, D. R. Hagan, and E. W. Van Stryland, "Sensitive measurement of optical nonlinearities using a single beam," IEEE J. Quantum Electron. 26, 760-769 (1990).
[CrossRef]

Hales, J. M.

J. M. Hales, D. J. Hagan, E. W. Van Stryland, K. J. Schafer, A. R. Morales, K. D. Belfield, P. Pacher, O. Kwon, E. Zojer, and J. L. Bredas, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," J. Chem. Phys. 121, 3152-3160 (2004).
[CrossRef] [PubMed]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Excited-state absorption dynamics in polymethine dyes detected by polarization-resolved pump-probe measurements," Chem. Phys. 286, 277-291 (2003).
[CrossRef]

R. A. Negras, J. M. Hales, A. Kobyakov, D. J. Hagan, and E. W. Van Stryland, "Experiment and analysis of two-photon absorption spectroscopy using a white-light continuum probe," IEEE J. Quantum Electron. 38, 1205-1216 (2002).
[CrossRef]

Hamer, M.

M. Hamer, The Cyanine Dyes and Related Compounds (Interscience, 1964).

He, G. S.

G. S. He, T.-C. Lin, J. Dai, P. N. Prasad, R. Kannan, A. G. Dombroskie, R. A. Vaia, and L.-S. Tan, "Degenerate two-photon-absorption spectral studies of highly two-photon active organic chromophores," J. Chem. Phys. 120, 5275-5284 (2004).
[CrossRef] [PubMed]

Heikal, A. A.

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Hess, S.

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Hu, Z.

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

Hush, N. S.

J. S. Craw, J. R. Reimers, G. B. Bacskay, A. T. Wong, and N. S. Hush, "Solitons in finite- and infinite-length negative-defect trans-polyacetylene and the corresponding Brooker (polymethinecyanine) cations," Chem. Phys. 167, 77-99 (1992).
[CrossRef]

Iwase, Y.

K. Kamada, K. Ohta, Y. Iwase, and K. Kondo, "Two-photon absorption properties of symmetric substituted diacetylene: drastic enhancement of the cross section near the one-photon absorption peak," Chem. Phys. Lett. 372, 386-393 (2003).
[CrossRef]

Kachkovski, A. D.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Two-photon anisotropy: analytical description and molecular modeling for symmetrical and asymmetrical organic dyes," Chem. Phys. 321, 257-268 (2006).
[CrossRef]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Excited-state absorption dynamics in polymethine dyes detected by polarization-resolved pump-probe measurements," Chem. Phys. 286, 277-291 (2003).
[CrossRef]

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, unpublished results.

Kamada, K.

K. Kamada, K. Ohta, Y. Iwase, and K. Kondo, "Two-photon absorption properties of symmetric substituted diacetylene: drastic enhancement of the cross section near the one-photon absorption peak," Chem. Phys. Lett. 372, 386-393 (2003).
[CrossRef]

Kannan, R.

G. S. He, T.-C. Lin, J. Dai, P. N. Prasad, R. Kannan, A. G. Dombroskie, R. A. Vaia, and L.-S. Tan, "Degenerate two-photon-absorption spectral studies of highly two-photon active organic chromophores," J. Chem. Phys. 120, 5275-5284 (2004).
[CrossRef] [PubMed]

Kobyakov, A.

R. A. Negras, J. M. Hales, A. Kobyakov, D. J. Hagan, and E. W. Van Stryland, "Experiment and analysis of two-photon absorption spectroscopy using a white-light continuum probe," IEEE J. Quantum Electron. 38, 1205-1216 (2002).
[CrossRef]

Kogej, T.

E. Zojer, D. Beljonne, T. Kogej, H. Vogel, S. R. Marder, J. W. Perry, and J. L. Bredas, "Tuning the two-photon absorption response of quadrupolar organic molecules," J. Chem. Phys. 116, 3646-3658 (2002).
[CrossRef]

T. Kogej, D. Beljonne, F. Meyers, J. W. Perry, S. R. Marder, and J. L. Bredas, "Mechanisms for enhancement of two-photon absorption in donor-acceptor conjugated chromophores," Chem. Phys. Lett. 298, 1-3 (1998).
[CrossRef]

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Kondo, K.

K. Kamada, K. Ohta, Y. Iwase, and K. Kondo, "Two-photon absorption properties of symmetric substituted diacetylene: drastic enhancement of the cross section near the one-photon absorption peak," Chem. Phys. Lett. 372, 386-393 (2003).
[CrossRef]

Kuzyk, M. G.

J. P. Moreno and M. G. Kuzyk, "Fundamental limits of the dispersion of the two-photon absorption cross section," J. Chem. Phys. 123, 194101-194113 (2005).
[CrossRef]

M. G. Kuzyk, "Fundamental limits on two-photon absorption cross sections," J. Chem. Phys. 119, 8327-8334 (2003).
[CrossRef]

Kwon, O.

J. M. Hales, D. J. Hagan, E. W. Van Stryland, K. J. Schafer, A. R. Morales, K. D. Belfield, P. Pacher, O. Kwon, E. Zojer, and J. L. Bredas, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," J. Chem. Phys. 121, 3152-3160 (2004).
[CrossRef] [PubMed]

Lakowicz, J. R.

J. R. Lakowicz, Principles of Fluorescence Spectroscopy (Kluwer Academic/Plenum, 1999).

Lambert, C.

D. Scherer, R. Dorfler, A. Feldner, T. Vogtmann, M. Schwoerer, U. Lawrentz, W. Grahn, and C. Lambert, "Two-photon states in squaraine monomers and oligomers," Chem. Phys. 279, 179-207 (2002).
[CrossRef]

Lawrentz, U.

D. Scherer, R. Dorfler, A. Feldner, T. Vogtmann, M. Schwoerer, U. Lawrentz, W. Grahn, and C. Lambert, "Two-photon states in squaraine monomers and oligomers," Chem. Phys. 279, 179-207 (2002).
[CrossRef]

Lepkowicz, R. S.

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Excited-state absorption dynamics in polymethine dyes detected by polarization-resolved pump-probe measurements," Chem. Phys. 286, 277-291 (2003).
[CrossRef]

Levin, M. D.

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Lin, T.-C.

G. S. He, T.-C. Lin, J. Dai, P. N. Prasad, R. Kannan, A. G. Dombroskie, R. A. Vaia, and L.-S. Tan, "Degenerate two-photon-absorption spectral studies of highly two-photon active organic chromophores," J. Chem. Phys. 120, 5275-5284 (2004).
[CrossRef] [PubMed]

Luo, Y.

C.-K. Wang, P. Macak, Y. Luo, and H. Agren, "Effects of π centers and symmetry on two-photon absorption cross sections of organic chromophores," J. Chem. Phys. 114, 9813-9820 (2001).
[CrossRef]

Macak, P.

C.-K. Wang, P. Macak, Y. Luo, and H. Agren, "Effects of π centers and symmetry on two-photon absorption cross sections of organic chromophores," J. Chem. Phys. 114, 9813-9820 (2001).
[CrossRef]

Marder, S. R.

E. Zojer, D. Beljonne, T. Kogej, H. Vogel, S. R. Marder, J. W. Perry, and J. L. Bredas, "Tuning the two-photon absorption response of quadrupolar organic molecules," J. Chem. Phys. 116, 3646-3658 (2002).
[CrossRef]

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

T. Kogej, D. Beljonne, F. Meyers, J. W. Perry, S. R. Marder, and J. L. Bredas, "Mechanisms for enhancement of two-photon absorption in donor-acceptor conjugated chromophores," Chem. Phys. Lett. 298, 1-3 (1998).
[CrossRef]

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

S. R. Marder, "Organic nonlinear optical materials: where we have been and where we are going," Chem. Commun. (Cambridge) 2006, 131-134.

McCord-Maughon, D.

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Meyers, F.

T. Kogej, D. Beljonne, F. Meyers, J. W. Perry, S. R. Marder, and J. L. Bredas, "Mechanisms for enhancement of two-photon absorption in donor-acceptor conjugated chromophores," Chem. Phys. Lett. 298, 1-3 (1998).
[CrossRef]

Morales, A. R.

J. M. Hales, D. J. Hagan, E. W. Van Stryland, K. J. Schafer, A. R. Morales, K. D. Belfield, P. Pacher, O. Kwon, E. Zojer, and J. L. Bredas, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," J. Chem. Phys. 121, 3152-3160 (2004).
[CrossRef] [PubMed]

Moreno, J. P.

J. P. Moreno and M. G. Kuzyk, "Fundamental limits of the dispersion of the two-photon absorption cross section," J. Chem. Phys. 123, 194101-194113 (2005).
[CrossRef]

Negras, R. A.

R. A. Negras, J. M. Hales, A. Kobyakov, D. J. Hagan, and E. W. Van Stryland, "Experiment and analysis of two-photon absorption spectroscopy using a white-light continuum probe," IEEE J. Quantum Electron. 38, 1205-1216 (2002).
[CrossRef]

Ohta, K.

K. Kamada, K. Ohta, Y. Iwase, and K. Kondo, "Two-photon absorption properties of symmetric substituted diacetylene: drastic enhancement of the cross section near the one-photon absorption peak," Chem. Phys. Lett. 372, 386-393 (2003).
[CrossRef]

Orr, B. J.

B. J. Orr and J. F. Ward, "Perturbation theory of the non-linear optical polarization of an isolated system," Mol. Phys. 20, 513-526 (1971).
[CrossRef]

Pacher, P.

J. M. Hales, D. J. Hagan, E. W. Van Stryland, K. J. Schafer, A. R. Morales, K. D. Belfield, P. Pacher, O. Kwon, E. Zojer, and J. L. Bredas, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," J. Chem. Phys. 121, 3152-3160 (2004).
[CrossRef] [PubMed]

E. Zojer, D. Beljonne, P. Pacher, and J. L. Bredas, "Two-photon absorption in quadrupolar π-conjugated molecules: influence of the nature of the conjugated bridge and the donor-acceptor separation," Chem.-Eur. J. 10, 2668-2680 (2004).
[CrossRef] [PubMed]

Padilha, L. A.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Two-photon anisotropy: analytical description and molecular modeling for symmetrical and asymmetrical organic dyes," Chem. Phys. 321, 257-268 (2006).
[CrossRef]

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, unpublished results.

Parker, T. C.

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

Perry, J. W.

E. Zojer, D. Beljonne, T. Kogej, H. Vogel, S. R. Marder, J. W. Perry, and J. L. Bredas, "Tuning the two-photon absorption response of quadrupolar organic molecules," J. Chem. Phys. 116, 3646-3658 (2002).
[CrossRef]

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

T. Kogej, D. Beljonne, F. Meyers, J. W. Perry, S. R. Marder, and J. L. Bredas, "Mechanisms for enhancement of two-photon absorption in donor-acceptor conjugated chromophores," Chem. Phys. Lett. 298, 1-3 (1998).
[CrossRef]

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

T. H. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, "Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines," Appl. Phys. B 54, 46-51 (1992).
[CrossRef]

Prasad, P. N.

G. S. He, T.-C. Lin, J. Dai, P. N. Prasad, R. Kannan, A. G. Dombroskie, R. A. Vaia, and L.-S. Tan, "Degenerate two-photon-absorption spectral studies of highly two-photon active organic chromophores," J. Chem. Phys. 120, 5275-5284 (2004).
[CrossRef] [PubMed]

Przhonska, O. V.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Two-photon anisotropy: analytical description and molecular modeling for symmetrical and asymmetrical organic dyes," Chem. Phys. 321, 257-268 (2006).
[CrossRef]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Excited-state absorption dynamics in polymethine dyes detected by polarization-resolved pump-probe measurements," Chem. Phys. 286, 277-291 (2003).
[CrossRef]

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, unpublished results.

Reimers, J. R.

J. S. Craw, J. R. Reimers, G. B. Bacskay, A. T. Wong, and N. S. Hush, "Solitons in finite- and infinite-length negative-defect trans-polyacetylene and the corresponding Brooker (polymethinecyanine) cations," Chem. Phys. 167, 77-99 (1992).
[CrossRef]

Rockel, H.

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Rocker, H.

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

Rumi, M.

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Said, A. A.

M. Sheik-Bahae, A. A. Said, T.-H. Wei, D. R. Hagan, and E. W. Van Stryland, "Sensitive measurement of optical nonlinearities using a single beam," IEEE J. Quantum Electron. 26, 760-769 (1990).
[CrossRef]

M. Sheik-Bahae, A. A. Said, and E. W. Van Stryland, "High-sensitivity, single-beam n2 measurements," Opt. Lett. 14, 955-957 (1989).
[CrossRef] [PubMed]

Schafer, K. J.

J. M. Hales, D. J. Hagan, E. W. Van Stryland, K. J. Schafer, A. R. Morales, K. D. Belfield, P. Pacher, O. Kwon, E. Zojer, and J. L. Bredas, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," J. Chem. Phys. 121, 3152-3160 (2004).
[CrossRef] [PubMed]

Scherer, D.

D. Scherer, R. Dorfler, A. Feldner, T. Vogtmann, M. Schwoerer, U. Lawrentz, W. Grahn, and C. Lambert, "Two-photon states in squaraine monomers and oligomers," Chem. Phys. 279, 179-207 (2002).
[CrossRef]

Schwoerer, M.

D. Scherer, R. Dorfler, A. Feldner, T. Vogtmann, M. Schwoerer, U. Lawrentz, W. Grahn, and C. Lambert, "Two-photon states in squaraine monomers and oligomers," Chem. Phys. 279, 179-207 (2002).
[CrossRef]

Sence, M. J.

T. H. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, "Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines," Appl. Phys. B 54, 46-51 (1992).
[CrossRef]

Sheik-Bahae, M.

M. Sheik-Bahae, A. A. Said, T.-H. Wei, D. R. Hagan, and E. W. Van Stryland, "Sensitive measurement of optical nonlinearities using a single beam," IEEE J. Quantum Electron. 26, 760-769 (1990).
[CrossRef]

M. Sheik-Bahae, A. A. Said, and E. W. Van Stryland, "High-sensitivity, single-beam n2 measurements," Opt. Lett. 14, 955-957 (1989).
[CrossRef] [PubMed]

Slominsky, Yu. L.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Two-photon anisotropy: analytical description and molecular modeling for symmetrical and asymmetrical organic dyes," Chem. Phys. 321, 257-268 (2006).
[CrossRef]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Excited-state absorption dynamics in polymethine dyes detected by polarization-resolved pump-probe measurements," Chem. Phys. 286, 277-291 (2003).
[CrossRef]

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, unpublished results.

Subramaniam, G.

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Tan, L.-S.

G. S. He, T.-C. Lin, J. Dai, P. N. Prasad, R. Kannan, A. G. Dombroskie, R. A. Vaia, and L.-S. Tan, "Degenerate two-photon-absorption spectral studies of highly two-photon active organic chromophores," J. Chem. Phys. 120, 5275-5284 (2004).
[CrossRef] [PubMed]

Thayumanavan, S.

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

Vaia, R. A.

G. S. He, T.-C. Lin, J. Dai, P. N. Prasad, R. Kannan, A. G. Dombroskie, R. A. Vaia, and L.-S. Tan, "Degenerate two-photon-absorption spectral studies of highly two-photon active organic chromophores," J. Chem. Phys. 120, 5275-5284 (2004).
[CrossRef] [PubMed]

Van Stryland, E. W.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Two-photon anisotropy: analytical description and molecular modeling for symmetrical and asymmetrical organic dyes," Chem. Phys. 321, 257-268 (2006).
[CrossRef]

J. M. Hales, D. J. Hagan, E. W. Van Stryland, K. J. Schafer, A. R. Morales, K. D. Belfield, P. Pacher, O. Kwon, E. Zojer, and J. L. Bredas, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," J. Chem. Phys. 121, 3152-3160 (2004).
[CrossRef] [PubMed]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Excited-state absorption dynamics in polymethine dyes detected by polarization-resolved pump-probe measurements," Chem. Phys. 286, 277-291 (2003).
[CrossRef]

R. A. Negras, J. M. Hales, A. Kobyakov, D. J. Hagan, and E. W. Van Stryland, "Experiment and analysis of two-photon absorption spectroscopy using a white-light continuum probe," IEEE J. Quantum Electron. 38, 1205-1216 (2002).
[CrossRef]

T. H. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, "Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines," Appl. Phys. B 54, 46-51 (1992).
[CrossRef]

M. Sheik-Bahae, A. A. Said, T.-H. Wei, D. R. Hagan, and E. W. Van Stryland, "Sensitive measurement of optical nonlinearities using a single beam," IEEE J. Quantum Electron. 26, 760-769 (1990).
[CrossRef]

M. Sheik-Bahae, A. A. Said, and E. W. Van Stryland, "High-sensitivity, single-beam n2 measurements," Opt. Lett. 14, 955-957 (1989).
[CrossRef] [PubMed]

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, unpublished results.

Vogel, H.

E. Zojer, D. Beljonne, T. Kogej, H. Vogel, S. R. Marder, J. W. Perry, and J. L. Bredas, "Tuning the two-photon absorption response of quadrupolar organic molecules," J. Chem. Phys. 116, 3646-3658 (2002).
[CrossRef]

Vogtmann, T.

D. Scherer, R. Dorfler, A. Feldner, T. Vogtmann, M. Schwoerer, U. Lawrentz, W. Grahn, and C. Lambert, "Two-photon states in squaraine monomers and oligomers," Chem. Phys. 279, 179-207 (2002).
[CrossRef]

Wang, C.-K.

C.-K. Wang, P. Macak, Y. Luo, and H. Agren, "Effects of π centers and symmetry on two-photon absorption cross sections of organic chromophores," J. Chem. Phys. 114, 9813-9820 (2001).
[CrossRef]

Ward, J. F.

B. J. Orr and J. F. Ward, "Perturbation theory of the non-linear optical polarization of an isolated system," Mol. Phys. 20, 513-526 (1971).
[CrossRef]

Webb, W. W.

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

C. Xu and W. W. Webb, "Measurement of two-photon excitation cross sections of molecular fluorophores with data from 690to1050 nm," J. Opt. Soc. Am. B 13, 481-491 (1996).
[CrossRef]

Wei, T. H.

T. H. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, "Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines," Appl. Phys. B 54, 46-51 (1992).
[CrossRef]

Wei, T.-H.

M. Sheik-Bahae, A. A. Said, T.-H. Wei, D. R. Hagan, and E. W. Van Stryland, "Sensitive measurement of optical nonlinearities using a single beam," IEEE J. Quantum Electron. 26, 760-769 (1990).
[CrossRef]

Wong, A. T.

J. S. Craw, J. R. Reimers, G. B. Bacskay, A. T. Wong, and N. S. Hush, "Solitons in finite- and infinite-length negative-defect trans-polyacetylene and the corresponding Brooker (polymethinecyanine) cations," Chem. Phys. 167, 77-99 (1992).
[CrossRef]

Wu, X.-L.

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Xu, C.

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

C. Xu and W. W. Webb, "Measurement of two-photon excitation cross sections of molecular fluorophores with data from 690to1050 nm," J. Opt. Soc. Am. B 13, 481-491 (1996).
[CrossRef]

Zojer, E.

J. M. Hales, D. J. Hagan, E. W. Van Stryland, K. J. Schafer, A. R. Morales, K. D. Belfield, P. Pacher, O. Kwon, E. Zojer, and J. L. Bredas, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," J. Chem. Phys. 121, 3152-3160 (2004).
[CrossRef] [PubMed]

E. Zojer, D. Beljonne, P. Pacher, and J. L. Bredas, "Two-photon absorption in quadrupolar π-conjugated molecules: influence of the nature of the conjugated bridge and the donor-acceptor separation," Chem.-Eur. J. 10, 2668-2680 (2004).
[CrossRef] [PubMed]

E. Zojer, D. Beljonne, T. Kogej, H. Vogel, S. R. Marder, J. W. Perry, and J. L. Bredas, "Tuning the two-photon absorption response of quadrupolar organic molecules," J. Chem. Phys. 116, 3646-3658 (2002).
[CrossRef]

Appl. Phys. B (1)

T. H. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, "Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines," Appl. Phys. B 54, 46-51 (1992).
[CrossRef]

Chem. Commun. (Cambridge) (1)

S. R. Marder, "Organic nonlinear optical materials: where we have been and where we are going," Chem. Commun. (Cambridge) 2006, 131-134.

Chem. Phys. (4)

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Excited-state absorption dynamics in polymethine dyes detected by polarization-resolved pump-probe measurements," Chem. Phys. 286, 277-291 (2003).
[CrossRef]

J. S. Craw, J. R. Reimers, G. B. Bacskay, A. T. Wong, and N. S. Hush, "Solitons in finite- and infinite-length negative-defect trans-polyacetylene and the corresponding Brooker (polymethinecyanine) cations," Chem. Phys. 167, 77-99 (1992).
[CrossRef]

D. Scherer, R. Dorfler, A. Feldner, T. Vogtmann, M. Schwoerer, U. Lawrentz, W. Grahn, and C. Lambert, "Two-photon states in squaraine monomers and oligomers," Chem. Phys. 279, 179-207 (2002).
[CrossRef]

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Two-photon anisotropy: analytical description and molecular modeling for symmetrical and asymmetrical organic dyes," Chem. Phys. 321, 257-268 (2006).
[CrossRef]

Chem. Phys. Lett. (3)

K. Kamada, K. Ohta, Y. Iwase, and K. Kondo, "Two-photon absorption properties of symmetric substituted diacetylene: drastic enhancement of the cross section near the one-photon absorption peak," Chem. Phys. Lett. 372, 386-393 (2003).
[CrossRef]

T. Kogej, D. Beljonne, F. Meyers, J. W. Perry, S. R. Marder, and J. L. Bredas, "Mechanisms for enhancement of two-photon absorption in donor-acceptor conjugated chromophores," Chem. Phys. Lett. 298, 1-3 (1998).
[CrossRef]

M. Fisher and J. Georges, "Fluorescence quantum yield of Rhodamine 6G in ethanol as a function of concentration using thermal lens spectrometry," Chem. Phys. Lett. 260, 115-118 (1996).
[CrossRef]

Chem.-Eur. J. (1)

E. Zojer, D. Beljonne, P. Pacher, and J. L. Bredas, "Two-photon absorption in quadrupolar π-conjugated molecules: influence of the nature of the conjugated bridge and the donor-acceptor separation," Chem.-Eur. J. 10, 2668-2680 (2004).
[CrossRef] [PubMed]

IEEE J. Quantum Electron. (2)

R. A. Negras, J. M. Hales, A. Kobyakov, D. J. Hagan, and E. W. Van Stryland, "Experiment and analysis of two-photon absorption spectroscopy using a white-light continuum probe," IEEE J. Quantum Electron. 38, 1205-1216 (2002).
[CrossRef]

M. Sheik-Bahae, A. A. Said, T.-H. Wei, D. R. Hagan, and E. W. Van Stryland, "Sensitive measurement of optical nonlinearities using a single beam," IEEE J. Quantum Electron. 26, 760-769 (1990).
[CrossRef]

J. Am. Chem. Soc. (1)

M. Rumi, J. E. Ehrlich, A. A. Heikal, J. W. Perry, S. Barlow, Z. Hu, D. McCord-Maughon, T. C. Parker, H. Rocker, S. Thayumanavan, S. R. Marder, D. Beljonne, and J. L. Bredas, "Structure-property relationships for two-photon absorbing chromophores: bis-donor diphenylpolyene and bis(styryl)benzene derivatives," J. Am. Chem. Soc. 122, 9500-9510 (2000).
[CrossRef]

J. Chem. Phys. (6)

G. S. He, T.-C. Lin, J. Dai, P. N. Prasad, R. Kannan, A. G. Dombroskie, R. A. Vaia, and L.-S. Tan, "Degenerate two-photon-absorption spectral studies of highly two-photon active organic chromophores," J. Chem. Phys. 120, 5275-5284 (2004).
[CrossRef] [PubMed]

C.-K. Wang, P. Macak, Y. Luo, and H. Agren, "Effects of π centers and symmetry on two-photon absorption cross sections of organic chromophores," J. Chem. Phys. 114, 9813-9820 (2001).
[CrossRef]

E. Zojer, D. Beljonne, T. Kogej, H. Vogel, S. R. Marder, J. W. Perry, and J. L. Bredas, "Tuning the two-photon absorption response of quadrupolar organic molecules," J. Chem. Phys. 116, 3646-3658 (2002).
[CrossRef]

J. M. Hales, D. J. Hagan, E. W. Van Stryland, K. J. Schafer, A. R. Morales, K. D. Belfield, P. Pacher, O. Kwon, E. Zojer, and J. L. Bredas, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," J. Chem. Phys. 121, 3152-3160 (2004).
[CrossRef] [PubMed]

M. G. Kuzyk, "Fundamental limits on two-photon absorption cross sections," J. Chem. Phys. 119, 8327-8334 (2003).
[CrossRef]

J. P. Moreno and M. G. Kuzyk, "Fundamental limits of the dispersion of the two-photon absorption cross section," J. Chem. Phys. 123, 194101-194113 (2005).
[CrossRef]

J. Opt. Soc. Am. B (1)

Mol. Phys. (1)

B. J. Orr and J. F. Ward, "Perturbation theory of the non-linear optical polarization of an isolated system," Mol. Phys. 20, 513-526 (1971).
[CrossRef]

Opt. Lett. (1)

Science (1)

M. Albota, D. Beljonne, J. L. Bredas, J. E. Ehrlich, J.-Y. Fu, A. A. Heikal, S. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Rockel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, "Design of organic molecules with large two-photon absorption cross sections," Science 281, 1653-1656 (1998).
[CrossRef] [PubMed]

Other (4)

M. J. S. Dewar, The Molecular Orbital Theory of Organic Chemistry (McGraw-Hill, 1969).

M. Hamer, The Cyanine Dyes and Related Compounds (Interscience, 1964).

J. R. Lakowicz, Principles of Fluorescence Spectroscopy (Kluwer Academic/Plenum, 1999).

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, unpublished results.

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Figures (10)

Fig. 1
Fig. 1

Molecular structure: (1) linear absorption spectrum, (2) one-photon excitation anisotropy, (3) 2PA spectrum for PD 2350 in ethanol, (4) theoretical curve based on a one-intermediate-state and two-final-states model. Uncertainties in 2PA measurements: ± 20 % .

Fig. 2
Fig. 2

Molecular structure: (1) linear absorption spectrum in ethanol, (2) one-photon excitation anisotropy in glycerol, (3) 2PA spectrum in ethanol for SD 2577, (4) theoretical curve based on a one-intermediate-state and three-final-states model. Uncertainties in 2PA measurements: ± 20 % .

Fig. 3
Fig. 3

Molecular structure: (1) linear absorption spectrum in ethanol, (2) one-photon excitation anisotropy in glycerol, (3) 2PA spectrum in ethanol for PD 2630, (4) theoretical curve based on a one-intermediate-state and two-final-states model. Uncertainties in 2PA measurements: ± 20 % .

Fig. 4
Fig. 4

Molecular structure: (1) linear absorption spectrum in dichloromethane (2) one-photon excitation anisotropy in glycerol, (3) 2PA spectrum in dichloromethane for SD 2243, (4) theoretical curve based on a one-intermediate-state and three-final-states model. Uncertainties in 2PA measurements: ± 20 % .

Fig. 5
Fig. 5

Scheme of the electronic levels for the unsubstituted chain PD 2350 and SD 2577.

Fig. 6
Fig. 6

Scheme of the electronic transitions for the unsubstituted chain PD 2350 and SD 2577. Dashed lines, one-photon allowed transitions; solid lines, allowed two-photon transitions; bold solid lines, experimentally observed two-photon transitions.

Fig. 7
Fig. 7

Electron density distribution in the MOs of the (a) unsubstituted chain and the (b) terminal groups.

Fig. 8
Fig. 8

Electron density distribution in the molecular orbitals for PD 2350.

Fig. 9
Fig. 9

Electron density distribution in the molecular orbitals for SD 2257.

Fig. 10
Fig. 10

2PA comparison of PDs and SDs by normalized 2PA cross section Ref. [27]. (a) PD2350 [(1), 1PA spectrum, ( 1 ) normalized 2PA spectrum], SD2577 [(2) 1PA spectrum, ( 2 ) normalized 2PA spectrum] (b) PD2630 [(1) 1PA spectrum, ( 1 ) normalized 2PA spectrum], SD2243 [(2) 1PA spectrum, ( 2 ) normalized 2PA spectrum].

Tables (2)

Tables Icon

Table 1 Calculated Parameters for the Unsubstituted Polymethine Chain PD 2350 and SD 2577

Tables Icon

Table 2 Molecular Parameters for PD 2350, SD 2577, PD 2630, and SD 2243

Equations (1)

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

δ 2 P A ( v p ) = 64 π 3 5 c 2 h E p 2 ( E 01 E p ) 2 + Γ 01 2 [ μ 01 2 μ 1 f 1 2 Γ 0 f 1 ( E 0 f 1 2 E p ) 2 + Γ 0 f 1 2 + μ 01 2 μ 1 f 2 2 Γ 0 f 2 ( E 0 f 2 2 E p ) 2 + Γ 0 f 2 2 ] ,

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