Two-Photon Absorption Spectrum of a Single Crystal Cyanine-like Dye

    Authors

    H. H. Hu; D. A. Fishman; A. O. Gerasov; O. V. Przhonska; S. Webster; L. A. Padilha; D. Peceli; M. Shandura; Y. P. Kovtun; A. D. Kachkovski; I. H. Nayyar; A. E. Masunov; P. Tongwa; T. V. Timofeeva; D. J. Hagan;E. W. Van Stryland

    Comments

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    Abbreviated Journal Title

    J. Phys. Chem. Lett.

    Keywords

    Molecular Structure; Quantum Chemistry; General Theory; POLYMETHINE DYES; NONLINEARITIES; FLUORESCENCE; DERIVATIVES; MOLECULES; EMISSION; STORAGE; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, ; Multidisciplinary; Physics, Atomic, Molecular & Chemical

    Abstract

    The two-photon absorption (2PA) spectrum of an organic single crystal is reported. The crystal is grown by self-nucleation of a subsaturated hot solution of acetonitrile, and is composed of an asymmetrical donor-a-acceptor cyanine-like dye molecule. To our knowledge, this is the first report of the 2PA spectrum of single crystals made from a cyanine-like dye. The linear and nonlinear properties of the single crystalline material are investigated and compared with the molecular properties of a toluene solution of its monomeric form. The maximum polarization-dependent 2PA coefficient of the single crystal is 52 +/- 9 cm/GW, which is more than twice as large as that for the inorganic semiconductor CdTe with a similar absorption edge. The optical properties, linear and nonlinear, are strongly dependent upon incident polarization due to anisotropic molecular packing. X-ray diffraction analysis shows a-stacking dimers formation in the crystal, similar to H-aggregates. Quantum chemical calculations demonstrate that this dimerization leads to the splitting of the energy bands and the appearance of new red-shifted 2PA bands when compared to the solution of monomers. This trend is opposite to the blue shift in the linear absorption spectra upon H-aggregation.

    Journal Title

    Journal of Physical Chemistry Letters

    Volume

    3

    Issue/Number

    9

    Publication Date

    1-1-2012

    Document Type

    Article

    Language

    English

    First Page

    1222

    Last Page

    1228

    WOS Identifier

    WOS:000303426200026

    ISSN

    1948-7185

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