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Optical Non linearity in (EDT-DSDTFVO)2.FeBr4, an Intriguing Molecular Material with Metallic Conductivity, Magnetoresistance Effects, and Quadratic Nonlinear Optical Properties

P. G. Lacroix, T. Hayashi, T. Sugimoto, K. Nakatani and V. Rodriguez J. Phys. Chem. C, 2010, 114 (49), 21762-21769

The quadratic (proportional to E-2) nonlinear optical (NLO) properties of (EDT-DSDTFVO)2 center dot FeBr4 have been investigated: an efficiency equal to 3-6 times that of urea in second-harmonic generation at 1.907 mu m has been observed by a powder test, and an effective (d(eff)) nonlinear optical susceptibility (chi((2))) tensor component equal to 110 pm/V at 1.064 mu m has been determined by confocal mu-SHG in the backscattering geometry. The origin of this effect is ascribable to the presence of strongly interacting EDT-DSDTFVO species organized in non-centrosymmetric stacks in solid state. A computational (ZINDO) investigation carried out on a [(EDT-DSDTFVO)(4)](2+) tetrameric entity at the fractional (rho = 0.5) oxidation state leads to a static molecular hyperpolarizability (beta(0)) equal to 854 x 10(-30) cm(5) esu(-1) per tetrameric unit. (EDT-DSDTFVO)(2)center dot FeBr4 is the first multifunctional molecular material exhibiting simultaneously conducting, magnetic, and NLO effects. The possibilities of using such absorbent species as micrometer size materials with efficient NLO properties are thoroughly evaluated.

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Publication

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Paru le 1 décembre 2010

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doi 10.1021/jp109646u