Hostname: page-component-77c89778f8-swr86 Total loading time: 0 Render date: 2024-07-20T06:15:28.414Z Has data issue: false hasContentIssue false
  • English
  • Français

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

Published online by Cambridge University Press:  01 February 2011

S. Polyutov ,
I. Minkov ,
F. Gel'mukhanov ,
K. Kamada ,
A. Baev  and
H. Ågren
S. Polyutov
Affiliation:
Theoretical Chemistry, Roslagstullsbacken 15, Royal Institute of Technology, S-106 91 Stockholm, Sweden
I. Minkov
Affiliation:
Theoretical Chemistry, Roslagstullsbacken 15, Royal Institute of Technology, S-106 91 Stockholm, Sweden
F. Gel'mukhanov
Affiliation:
Theoretical Chemistry, Roslagstullsbacken 15, Royal Institute of Technology, S-106 91 Stockholm, Sweden
K. Kamada
Affiliation:
Photonics Research Institute, National Institute of Advanced Industrial Science and Technology, AIST Kansai Center, Osaka, Japan
A. Baev
Affiliation:
Institute for Lasers, Photonics and Biophotonics, The State University of New York at Buffalo, Buffalo, New York 14260–3000
H. Ågren
Affiliation:
Theoretical Chemistry, Roslagstullsbacken 15, Royal Institute of Technology, S-106 91 Stockholm, Sweden
Get access

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.]

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 846: Symposium DD – Organic and Nanocomposite Optical Materials , 2004 , DD1.2
Copyright
Copyright © Materials Research Society 2005

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

[1] Lin, T.-C., He, G.S., Prasad, P.N., and Tan, L.-S., J. Mater. Chem., 14, 982 (2004).Google Scholar
[2] He, G.S., Lin, T.-C., Dai, J., and Prasad, P.N. J. Phys. Chem., 120, 5275 (2004).Google Scholar
[3] Gel'mukhanov, F., Baev, A., Macak, P., Luo, Y., and Ågren, H., J. Opt. Soc. Am., B 19, 937 (2002).Google Scholar
[4] Baev, A., Gel'mukhanov, F., Macak, P., Luo, Y., and Ågren, H. J. Chem. Phys., 117, 6214 (2002).Google Scholar
[5] Baev, A., Gel'mukhanov, F., Rubio-Pons, O., Cronstrand, P., and Ågren, H., J. Opt. Soc. Am., B 21, 384 (2004).Google Scholar
[6] Baev, A., Rubio-Pons, O., Gel'mukhanov, F., and Ågren, H., J. Phys. Chem., A 108, 7406 (2004).Google Scholar
[7] Baev, A., Kimberg, V., Polyutov, S., Gel'mukhanov, F., and Ågren, H., J. Opt. Soc. Am. B. 00, 000 (2004).Google Scholar
[8] Allard, N. and Kielkopf, J., Rev. Mod. Phys., 54, 1103 (1982).Google Scholar
[9] Turro, N.J., Modern Molecular Photochemistry (Benjamin, New York, 1978).Google Scholar
[10] Kamada, K. (to be published).Google Scholar
[11] Helgaker, T. and Jensen, H. J. A. and Jørgensen, P. and Olsen, J. and Ruud, K. and Ågren, H. and Auer, A.A. and Bak, K.L. and Bakken, V. and Christiansen, O. and Coriani, S. and Dahle, P. and Dalskov, E. K. and Enevoldsen, T. and Fernandez, B. and Hättig, C. and Hald, K. and Halkier, A. and Heiberg, H. and Hettema, H. and Jonsson, D. and Kirpekar, S. and Kobayashi, R. and Koch, H. and Mikkelsen, K. V. and Norman, P. and Packer, M. J. and Pedersen, T. B. and Ruden, T. A. and Sanchez, A. and Saue, T. and Sauer, S. P. A. and Schimmelpfenning, B. and Sylvester-Hvid, K. O. and Taylor, P. R. and Vahtras, O., DALTON a molecular electronic structure program — Release 1.2. (2001).Google Scholar