Molecular structure - two-photon absorption property relations in polymethine dyes

    Authors

    J. Fu; L. A. Padilha; D. J. Hagan; E. W. Van Stryland; O. V. Przhonska; M. V. Bondar; Y. L. Slominsky;A. D. Kachkovski

    Comments

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    Abbreviated Journal Title

    J. Opt. Soc. Am. B-Opt. Phys.

    Keywords

    CROSS-SECTIONS; ORGANIC CHROMOPHORES; SINGLE-BEAM; ENHANCEMENT; Optics

    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. (c) 2006 Optical Society of America.

    Journal Title

    Journal of the Optical Society of America B-Optical Physics

    Volume

    24

    Issue/Number

    1

    Publication Date

    1-1-2007

    Document Type

    Article

    Language

    English

    First Page

    56

    Last Page

    66

    WOS Identifier

    WOS:000243347800010

    ISSN

    0740-3224

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