OSA's Digital Library

Optics Express

Optics Express

  • Editor: C. Martijn de Sterke
  • Vol. 18, Iss. 26 — Dec. 20, 2010
  • pp: 26843–26853

Excited-state enhancement of third-order optical nonlinearities: photodynamics and characterization

Bing Gu, Kai Lou, Jing Chen, Yongnan Li, Hui-Tian Wang, and Wei Ji  »View Author Affiliations

Optics Express, Vol. 18, Issue 26, pp. 26843-26853 (2010)

View Full Text Article

Enhanced HTML    Acrobat PDF (1839 KB)

Browse Journals / Lookup Meetings

Browse by Journal and Year


Lookup Conference Papers

Close Browse Journals / Lookup Meetings

Article Tools



Based on the simplified five-level rate-equation theory, we investigate the hybrid third-order optical nonlinear processes which combine the instantaneous nonlinearity and the one-photon absorption induced excited-state nonlinearity. We obtain the analytical third-order nonlinear absorption and refraction coefficients originating from the singlet and triplet excited-state effects. We explore the photodynamic process and give the corresponding level diagram in the nanosecond, picosecond, and femtosecond regimes. We develop the pulse-duration-dependent Z-scan theory for characterizing the simultaneous instantaneous nonlinearity and cumulative effect of the excited-state nonlinearity. We also demonstrate the validity of the presented theory to analyze the experimental results.

© 2010 Optical Society of America

OCIS Codes
(190.4710) Nonlinear optics : Optical nonlinearities in organic materials
(320.2250) Ultrafast optics : Femtosecond phenomena
(320.4240) Ultrafast optics : Nanosecond phenomena
(320.5390) Ultrafast optics : Picosecond phenomena

ToC Category:
Nonlinear Optics

Original Manuscript: September 24, 2010
Revised Manuscript: November 4, 2010
Manuscript Accepted: November 17, 2010
Published: December 7, 2010

Bing Gu, Kai Lou, Jing Chen, Yongnan Li, Hui-Tian Wang, and Wei Ji, "Excited-state enhancement of third-order optical nonlinearities: photodynamics and characterization," Opt. Express 18, 26843-26853 (2010)

Sort:  Author  |  Year  |  Journal  |  Reset  


  1. R. L. Sutherland with contributions by D. G. McLean and S. Kikpatrick, Handbook of Nonlinear Optics, 2nd ed. (Dekker, New York, 2003). [CrossRef]
  2. D. N. Christodoulides, I. C. Khoo, G. J. Salamo, G. I. Stegeman, and E. W. Van Stryland, "Nonlinear refraction and absorption: mechanisms and magnitudes," Adv. Opt. Photon. 2, 60 (2010). [CrossRef]
  3. R. Lepkowicz, A. Kobyakov, D. J. Hagan, and E. W. Van Stryland, "Picosecond optical limiting in reverse saturable absorbers: a theoretical and experimental study," J. Opt. Soc. Am. B 19, 94 (2002). [CrossRef]
  4. E. Kuznetsova, R. Kolesov, and O. Kocharovskaya, "Suppression of excited-state absorption: A path to ultraviolet tunable solid-state lasers," Phys. Rev. A 70, 043801 (2004). [CrossRef]
  5. C. P. Singh, K. S. Bindra, and S. M. Oak, "Analysis of effect of excitation pulse characteristics on numerical simulation of reverse saturable absorption," Opt. Commun. 269, 223 (2007). [CrossRef]
  6. S. Scuppa, L. Orian, D. Dini, S. Santi, and M. Meneghetti, "Nonlinear absorption properties and excited state dynamics of Ferrocene," J. Phys. Chem. A 113, 9286 (2009). [CrossRef] [PubMed]
  7. S. V. Rao, N. K. M. N. Srinivas, and D. N. Rao, "Nonlinear absorption and excited state dynamics in Rhodamine B studied using Z-scan and degenerate four wave mixing techniques," Chem. Phys. Lett. 361, 439 (2002). [CrossRef]
  8. N. K. M. N. Srinivas, S. V. Rao, and D. N. Rao, "Saturable and reverse saturable absorption of Rhodamine B in methanol and water," J. Opt. Soc. Am. B 20, 2470 (2003). [CrossRef]
  9. A. Shukla, H. Ghosh, and S. Mazumdar, "Theory of excited-state absorption in phenylene-based π-conjugated polymers," Phys. Rev. B 67, 245203 (2003). [CrossRef]
  10. C. C. Byeon, M. M. Mckerns, W. Sun, T. M. Nordlund, C. M. Lawson, and G. M. Gray, "Excited state lifetime and intersystem crossing rate of asymmetric pentaazadentate porphyrin-like metal complexes," Appl. Phys. Lett. 84, 5174 (2004). [CrossRef]
  11. J. Yang, J. Gu, Y. Song, S. Guang, Y. Wang, W. Zhang, and J. Lang, "Excited state absorption dynamics in metal cluster polymer [WS4Cu3I(4-bpy)3]n solution," J. Phys. Chem. B 111, 7987 (2007). [CrossRef] [PubMed]
  12. P. Poornesh, G. Umesh, P. K. Hegde, M. G. Manjunatha, K. B. Manjunatha, and A. V. Adhikari, "Studies on third order nonlinear optical properties and reverse saturable absorption in polythiophene/poly (methylmethacrylate) composites," Appl. Phys. B 97, 117 (2009). [CrossRef]
  13. S. C. Hayes, and C. Silva, "Analysis of the excited-state absorption spectral bandshape of oligofluorenes," J. Chem. Phys. 132, 214510 (2010). [CrossRef] [PubMed]
  14. C. L. Lee, X. Yang, and N. C. Greenham, "Determination of the triplet excited-state absorption cross section in a polyfluorene by energy transfer from a phosphorescent metal complex," Phys. Rev. B 76, 245201 (2007). [CrossRef]
  15. T. M. Pritchett, W. F. Sun, F. Guo, B. Zhang, M. J. Ferry, J. E. Rogers-Haley, W. ShenskyIII, and A. G. Mott, "Excited-state absorption in a terpyridyl platinum(II) pentynyl complex," Opt. Lett. 33, 1053 (2008). [CrossRef] [PubMed]
  16. T. M. Pritchett, W. F. Sun, B. Zhang, M. J. Ferry, Y. Li, J. E. Haley, D. M. Mackie, W. ShenskyIII, and A. G. Mott, "Excited-state absorption of a bipyridyl platinum(II) complex with alkynyl-benzothiazolylfluorene units," Opt. Lett. 35, 1305 (2010). [CrossRef] [PubMed]
  17. G. Shi, C. He, Y. Li, R. Zou, X. Zhang, Y. Wang, K. Yang, Y. Song, and C. H. Wang, "Excited-state nonlinearity measurements of ZnPcBr4/DMSO," J. Opt. Soc. Am. B 26, 754 (2009). [CrossRef]
  18. A. Marcelli, P. Foggi, L. Moroni, C. Gellini, and P. R. Salvi, "Excited-state absorption and ultrafast relaxiation dynamics of porphyrin, diprotonated porphyrin, and tetraoxaporphyrin dication," J. Phys. Chem. A 112, 1864 (2008).
  19. L. Jiang, T. Jiu, Y. Li, Y. Li, J. Yang, J. Li, C. Li, H. Liu, and Y. Song, "Excited-state absorption and sign tuning of nonlinear refraction in porphyrin derivatives," J. Phys. Chem. B 112, 756 (2008). [CrossRef]
  20. T. Cassano, R. Tommasi, A. P. Meacham, and M. D. Ward, "Investigation of the excited-state absorption of a Ru dioxolene complex by the Z-scan technique," J. Chem. Phys. 122, 154507 (2005). [CrossRef] [PubMed]
  21. D. Weaire, B. S. Wherrett, D. A. B. Miller, and S. D. Smith, "Effect of low-power nonlinear refraction on laser beam propagation in InSb," Opt. Lett. 4, 331 (1979). [CrossRef] [PubMed]
  22. M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, and E. W. Van Stryland, "Sensitive measurement of optical nonlinearities using a single beam," IEEE J. Quantum Electron. 26, 760 (1990). [CrossRef]
  23. B. Gu, W. Ji, and X. Q. Huang, "Analytical expression for femtosecond-pulsed z scans on instantaneous nonlinearity," Appl. Opt. 47, 1187 (2008). [CrossRef] [PubMed]
  24. B. Gu, Y. Sun, and W. Ji, "Two-photon-induced excited-state nonlinearities," Opt. Express 16, 17745 (2008). [CrossRef] [PubMed]
  25. H. L. Fan, X. Q. Wang, Q. Ren, X. Zhao, G. H. Zhang, J. W. Chen, D. Xu, G. Yu, and Z. H. Sun, "Investigation of the nonlinear absorption and optical limiting properties of two [Q]2[Cu(C3S5)2] compounds," Opt. Laser Technol. 42, 732 (2010). [CrossRef]
  26. C. He, G. Shi, W. Duan, Y. Wu, Z. Chen, W. Song, R. Zou, and Y. Song, "Third-order nonlinear optical properties of self-assembled thin films containing tetracarboxylic copper phthalocyanine," J. Porphyrins Phthalocyanines 13, 1243 (2009). [CrossRef]
  27. S. L. Guo, J. Yan, L. Xu, B. Gu, X. Z. Fan, H. T. Wang, and N. B. Ming, "Second Z-scan in materials with nonlinear refraction and nonlinear absorption," J. Opt. A, Pure Appl. Opt. 4, 504 (2002). [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