Abstract

We performed a comprehensive experimental investigation of two-photon absorption (2PA) spectra of a series of 12 symmetrical and asymmetrical cationic polymethine dyes, including complete one-and two-photon excitation anisotropy measurements. Quantum-chemical calculations were performed with the goal of understanding the nature of 2PA bands and of uncovering structure-property relations. We found that there are 2PA bands in the spectral region between the first absorption band and that for twice its energy. A weakly allowed 2PA band within the short-wavelength shoulder of the first absorption band was observed owing to the effects of vibrational and charge distribution symmetry breaking. The nature of the strongest 2PA band is connected to the electron transition from the molecular orbital localized at the benzene rings of the terminal groups to the lowest unoccupied molecular orbital (LUMO). Structure-property relations revealed that the 2PA cross section tends to be enhanced by either an increase in the length of the polymethine chromophore or an increase in the donor strengths in the terminal groups.

© 2006 Optical Society of America

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    [CrossRef]

2007 (1)

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]

2004 (4)

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, J. Fu, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Nature of the electronic transitions in thiacarbocyanines with a long polymethine chain," Chem. Phys. 305, 259-270 (2004).
[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]

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]

2003 (2)

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]

2002 (2)

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]

2001 (1)

C.-K. Wang, P. Macak, Yi 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," Chin. Phys. Lasers 260, 115-118 (1996).
[CrossRef]

1992 (1)

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]

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. Sel. Top. Quantum Electron. 26, 760-769 (1990).
[CrossRef]

1989 (1)

Agren, H.

C.-K. Wang, P. Macak, Yi 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, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Experimental and theoretical approaches to understanding two-photon absorption spectra in polymethine and squaraine molecules," J. Opt. Soc. Am. B 24, 67-76 (2007).
[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]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, J. Fu, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Nature of the electronic transitions in thiacarbocyanines with a long polymethine chain," Chem. Phys. 305, 259-270 (2004).
[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]

Bredas, J. L.

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]

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]

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," Chin. Phys. Lasers 260, 115-118 (1996).
[CrossRef]

Fu, J.

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, "Experimental and theoretical approaches to understanding two-photon absorption spectra in polymethine and squaraine molecules," J. Opt. Soc. Am. B 24, 67-76 (2007).
[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]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, J. Fu, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Nature of the electronic transitions in thiacarbocyanines with a long polymethine chain," Chem. Phys. 305, 259-270 (2004).
[CrossRef]

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," Chin. Phys. Lasers 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, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Experimental and theoretical approaches to understanding two-photon absorption spectra in polymethine and squaraine molecules," J. Opt. Soc. Am. B 24, 67-76 (2007).
[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]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, J. Fu, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Nature of the electronic transitions in thiacarbocyanines with a long polymethine chain," Chem. Phys. 305, 259-270 (2004).
[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]

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. Sel. Top. Quantum Electron. 26, 760-769 (1990).
[CrossRef]

Hales, J. M.

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, J. Fu, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Nature of the electronic transitions in thiacarbocyanines with a long polymethine chain," Chem. Phys. 305, 259-270 (2004).
[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]

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, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Experimental and theoretical approaches to understanding two-photon absorption spectra in polymethine and squaraine molecules," J. Opt. Soc. Am. B 24, 67-76 (2007).
[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]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, J. Fu, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Nature of the electronic transitions in thiacarbocyanines with a long polymethine chain," Chem. Phys. 305, 259-270 (2004).
[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]

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]

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]

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, J. Fu, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Nature of the electronic transitions in thiacarbocyanines with a long polymethine chain," Chem. Phys. 305, 259-270 (2004).
[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]

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, Yi

C.-K. Wang, P. Macak, Yi 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, Yi 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)131-134 (2006).

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]

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]

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, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Experimental and theoretical approaches to understanding two-photon absorption spectra in polymethine and squaraine molecules," J. Opt. Soc. Am. B 24, 67-76 (2007).
[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]

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]

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, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Experimental and theoretical approaches to understanding two-photon absorption spectra in polymethine and squaraine molecules," J. Opt. Soc. Am. B 24, 67-76 (2007).
[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]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, J. Fu, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Nature of the electronic transitions in thiacarbocyanines with a long polymethine chain," Chem. Phys. 305, 259-270 (2004).
[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]

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. Sel. Top. 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]

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. Sel. Top. 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, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Experimental and theoretical approaches to understanding two-photon absorption spectra in polymethine and squaraine molecules," J. Opt. Soc. Am. B 24, 67-76 (2007).
[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]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, J. Fu, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Nature of the electronic transitions in thiacarbocyanines with a long polymethine chain," Chem. Phys. 305, 259-270 (2004).
[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]

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, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Experimental and theoretical approaches to understanding two-photon absorption spectra in polymethine and squaraine molecules," J. Opt. Soc. Am. B 24, 67-76 (2007).
[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]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, J. Fu, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Nature of the electronic transitions in thiacarbocyanines with a long polymethine chain," Chem. Phys. 305, 259-270 (2004).
[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]

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. Sel. Top. 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]

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, Yi 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]

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.

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. Sel. Top. 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]

Chem. Phys. (5)

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, 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. 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]

R. S. Lepkowicz, O. V. Przhonska, J. M. Hales, J. Fu, D. J. Hagan, E. W. Van Stryland, M. V. Bondar, Yu. L. Slominsky, and A. D. Kachkovski, "Nature of the electronic transitions in thiacarbocyanines with a long polymethine chain," Chem. Phys. 305, 259-270 (2004).
[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]

Chem. Phys. Lett. (2)

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]

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]

Chin. Phys. Lasers (1)

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

IEEE J. Sel. Top. Quantum Electron. (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. Sel. Top. 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. (4)

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, Yi 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]

J. Opt. Soc. Am. B (2)

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)

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

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).

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Figures (8)

Fig. 1
Fig. 1

Molecular structures of PDs.

Fig. 2
Fig. 2

Linear (1, 2, 3) and 2PA ( 1 , 2 , 3 ) spectra for polymethine dyes with thiazolium terminal groups in ethanol: PD 25 ( 1 , 1 , open squares); PD 2646 ( 2 , 2 , solid circles); PD 2501 ( 3 , 3 , open triangles). Dashed lines are theoretical fittings based on Eq. (2). For comparison with linear absorption, 2PA spectra are presented as a function of half the excitation wavelength λ exc 2 .

Fig. 3
Fig. 3

Linear (1, 2, 3, 4) and 2PA ( 1 , 2 , 3 , 4 ) spectra for polymethine dyes with indolium terminal groups in ethanol: PD AF ( 1 , 1 , open squares); PD 2350 ( 2 , 2 , solid circles); PD 3428 ( 3 , 3 , open triangles); PD 824 ( 4 , 4 , open circle). Dashed lines are theoretical fittings based on Eq. (2). For comparison with linear absorption, 2PA spectra are presented as a function of half the excitation wavelength λ exc 2 .

Fig. 4
Fig. 4

Linear (thicker curves 1, 2, 3) and 2PA ( 1 , 2 , 3 ) spectra for polymethine dyes with the same conjugated length ( n = 2 ) in ethanol: PD 2646 ( 1 , 1 , open squares); PD 2350 ( 2 , 2 , solid circles); PD 2630 ( 3 , 3 , open triangles). Dashed lines are theoretical fittings based on Eq. (2). For comparison with linear absorption, 2PA spectra are presented as a function of half the excitation wavelength λ exc 2 .

Fig. 5
Fig. 5

(a) Linear (1, 2) and 2PA ( 1 , 2 ) spectra for PD 25 ( 2 , 2 , solid circles) and Styryl 1 ( 1 , 1 open squares) in ethanol. (b) Linear (1, 2) and 2PA ( 1 , 2 ) spectra for PD 2350 ( 2 , 2 , solid circles) and PD 2665 ( 1 , 1 , open squares) in ethanol. Dashed lines are theoretical fittings based on Eq. (2). For comparison with linear absorption, 2PA spectra are presented as a function of half the excitation wavelength λ exc 2 .

Fig. 6
Fig. 6

Graph of two-photon excitation fluorescence anisotropy as a function of the angle between μ 01 and Δ μ at different values of β : β = 5 ° ( 1 ) , β = 10 ° ( 2 ) , β = 15 ° ( 3 ) .

Fig. 7
Fig. 7

Graph of PD 25 in ethanol: 1, linear absorption; 2, fluorescence; 3, 2PA spectra; dashed line, theoretical fitting based on Eq. (2); 4, 5, one- and two-photon excitation anisotropy spectra, respectively, in glycerol. For comparison with linear absorption, 2PA spectra are presented as a function of half the excitation wavelength λ exc 2 .

Fig. 8
Fig. 8

(a) PD 2350 in ethanol: 1, linear absorption; 2, fluorescence; 3, 2PA spectra; dashed line, theoretical fitting based on Eq. (2); 4, 5, one- and two-photon excitation anisotropy spectra, respectively, in glycerol, (b) PD 2630 in ethanol: 1, linear absorption; 2, fluorescence; 3, 2PA spectra; dashed line, theoretical fitting; 4, 5, one- and two-photon excitation anisotropy spectra, respectively, in glycerol. For comparison with linear absorption, 2PA spectra are presented as a function of half the excitation wavelength λ exc 2 .

Tables (6)

Tables Icon

Table 1 Measured and Calculated Parameters for PDs 25, 2646, and 2501 with Different Conjugation Lengths a

Tables Icon

Table 2 Measured and Calculated Parameters as Defined in Table 1 for PDs AF, 2350, 3428, and 824 with Different Conjugation Lengths

Tables Icon

Table 3 Measured and Calculated Parameters as Defined in Table 1 for PDs 2646, 2350, and 2630 with Different Terminal Groups a and Same Conjugation Chain Length ( n = 2 )

Tables Icon

Table 4 Measured and Calculated Parameters as Defined in Table 1 for Symmetric Molecules PDs 25 and 2350 and for Asymmetric Molecules Styry1̱1 and PD 2665

Tables Icon

Table 5 Measured and Calculated Parameters as Defined in Table 1 for Bridged Molecules PDs 200 and 2093 and for Unbridged Molecules PDs 2646 and 3428

Tables Icon

Table 6 Calculated Parameters for the Unsubstituted Polymethine Chain and One Typical Polymethine Dye PD 2350

Equations (3)

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

r 2 P A = 18 cos ( γ β ) cos β cos γ 7 cos 2 γ + 1 7 ( 2 cos 2 γ + 1 ) .
μ 01 = { [ 1500 ( c ) 2 ln 10 ] [ ε 01 ( ν ) d ν ] π N A E 01 } 1 2 ,
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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