OSA's Digital Library

Journal of the Optical Society of America B

Journal of the Optical Society of America B

| OPTICAL PHYSICS

  • Editor: Henry M. Van Driel
  • Vol. 24, Iss. 1 — Jan. 1, 2007
  • pp: 67–76

Experimental and theoretical approaches to understanding two-photon absorption spectra in polymethine and squaraine molecules

Jie Fu, Lazaro A. Padilha, David J. Hagan, Eric W. Van Stryland, Olga V. Przhonska, Mikhail V. Bondar, Yuriy L. Slominsky, and Alexei D. Kachkovski  »View Author Affiliations


JOSA B, Vol. 24, Issue 1, pp. 67-76 (2007)
http://dx.doi.org/10.1364/JOSAB.24.000067


View Full Text Article

Enhanced HTML    Acrobat PDF (455 KB)





Browse Journals / Lookup Meetings

Browse by Journal and Year


   


Lookup Conference Papers

Close Browse Journals / Lookup Meetings

Article Tools

Share
Citations

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 150 fs laser pulses of 1 kHz repetition rate in the tuning range of 520 2100 nm ( 0.6 2.4 eV ) . Comparing 2PA spectra of polymethines and squaraines, we find that we can access considerably larger 2PA cross sections ( 8600 × 10 50 cm 4 s /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

OCIS Codes
(190.4180) Nonlinear optics : Multiphoton processes
(190.4710) Nonlinear optics : Optical nonlinearities in organic materials

ToC Category:
Nonlinear Optics

History
Original Manuscript: July 20, 2006
Manuscript Accepted: August 21, 2006

Virtual Issues
Vol. 2, Iss. 2 Virtual Journal for Biomedical Optics

Citation
Jie Fu, Lazaro A. Padilha, David J. Hagan, Eric W. Van Stryland, Olga V. Przhonska, Mikhail V. Bondar, Yuriy L. Slominsky, and Alexei 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)
http://www.opticsinfobase.org/josab/abstract.cfm?URI=josab-24-1-67


Sort:  Author  |  Year  |  Journal  |  Reset  

References

  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]

Cited By

Alert me when this paper is cited

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


« Previous Article  |  Next Article »

OSA is a member of CrossRef.

CrossCheck Deposited