Spectral profiles of two-photon absorption: Coherent versus two-step two-photon absorption

We’re sorry, something doesn't seem to be working properly.

Please try refreshing the page. If that doesn't work, please contact support so we can address the problem.

Abstract

We present a theory of two-photon absorption in solutions which addresses the formation of spectral shapes taking account of the vibrational degrees of freedom. The theory is used to rationalize observed differences between spectral shapes of one- and two-photon absorption. We elaborate on two underlying causes, one trivial and one non-trivial, behind these differences. The first refers simply to the fact that the set of excited electronic states constituting the spectra will have different relative cross sections for one-and two- photon absorption. The second reason is that the two-step and coherent two-photon absorption processes are competing, making the one-and two-photon spectral bands different even considering a single final state. The theory is applied to the N-101 molecule [di-phenyl-amino-nitro-stilbene] which was recently studied experimentally in the paper [ T.-C. Lin, G.S. He, P.N. Prasad, and L.-S. Tan, J. Mater. Chem., 14, 982, 2004.]

This is a preview of subscription content, access via your institution.

References

  1. [1]

    T.-C. Lin, G.S. He, P.N. Prasad, and L.-S. Tan, J. Mater. Chem., 14, 982 (2004).

    CAS  Article  Google Scholar 

  2. [2]

    G.S. He, T.-C. Lin, J. Dai, and P.N. Prasad J. Phys. Chem., 120, 5275 (2004).

    CAS  Article  Google Scholar 

  3. [3]

    F. Gel’mukhanov, A. Baev, P. Macak, Y. Luo, and H. Âgren, J. Opt. Soc. Am., B 19, 937 (2002).

    Article  Google Scholar 

  4. [4]

    A. Baev, F. Gel’mukhanov, P. Macak, Y. Luo, and H. Agren J. Chem. Phys., 117, 6214 (2002).

    CAS  Article  Google Scholar 

  5. [5]

    A. Baev, F. Gel’mukhanov, O. Rubio-Pons, P. Cronstrand, and H. Agren, J. Opt. Soc. Am., B 21, 384 (2004).

    Article  Google Scholar 

  6. [6]

    A. Baev, O. Rubio-Pons, F. Gel’mukhanov, and H. Agren, J. Phys. Chem., A 108, 7406 (2004).

    Article  Google Scholar 

  7. [7]

    A. Baev, V. Kimberg, S. Polyutov, F. Gel’mukhanov, and H. Âgren, J. Opt. Soc. Am. B. 00, 000 (2004).

    Google Scholar 

  8. [8]

    N. Allard and J. Kielkopf, Rev. Mod. Phys., 54, 1103 (1982).

    CAS  Article  Google Scholar 

  9. [9]

    N.J. Turro, Modern Molecular Photochemistry (Benjamin, New York, 1978).

    Google Scholar 

  10. [10]

    K. Kamada (to be published).

  11. [11]

    T. Helgaker and H. J. A. Jensen and P. Jprgensen and J. Olsen and K. Ruud and H. Agren and A.A. Auer and K.L. Bak and V. Bakken and O. Christiansen and S. Coriani and P. Dahle and E. K. Dalskov and T. Enevoldsen and B. Fernandez and C. Huttig and K. Hald and A. Halkier and H. Heiberg and H. Hettema and D. Jonsson and S. Kirpekar and R. Kobayashi and H. Koch and K. V. Mikkelsen and P. Norman and M. J. Packer and T. B. Pedersen and T. A. Ruden and A. Sanchez and T. Sane and S. P. A. Sauer and B. Schimmelpfenning and K. O. Sylvester-Hvid and P. R. Taylor and O. Vahtras, DALTON a molecular electronic structure program — Release 1.2. (2001).

    Google Scholar 

Download references

Acknowledgments

This work was supported by the Swedish Research Council (VR).

Author information

Affiliations

Authors

Corresponding author

Correspondence to S. Polyutov.

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Polyutov, S., Minkov, I., Gel'mukhanov, F. et al. Spectral profiles of two-photon absorption: Coherent versus two-step two-photon absorption. MRS Online Proceedings Library 846, 12 (2004). https://doi.org/10.1557/PROC-846-DD1.2

Download citation