Abstract

In order to obtain a new type of organic-inorganic hybrid material for nonlinear optics, two pyridinium-CdI2 crystals, i.e., bis(4-cyano-1-methyl-pyridinium) tetraiodocadmate (CNP/CdI4) and bis(4-dimethylamino-1-methylpyridinium) tetraio-docadmeate (DAP/CdI4) were prepared. From X-ray crystal structure analyses, the inorganic parts of both of the crystals are found to be the tetrahedral [CdI4]2- structure. Although the CNP/CdI4 crystals have a centrosymmetric layered structure, the DAP/CdI4 crystals do not have layered structures resulting in non-centrosymmetric space group Cc and second-order nonlinear optical activity. Thus, the second-harmonic generation (SHG) coefficients (d) of the DAP/CdI4 crystal were estimated using the oriented gas model. In spite of the shorter cutoff wavelength of DAP/CdI4 compared with that of the well-known 2-methyl-4-nitroaniline (MNA) crystal, the maximum d value was expected to reach one-third of that of the MNA in the diagonal component.

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