Direct energy transfer from excited organic adsorbates to intrinsic defect sites in silicalite

Leheny, A. R.; Turro, Nicholas J.; Drake, J. M.

The decay of the excited singlet state of an aromatic molecule such as naphthalene adsorbed to the surface of silica is nonexponential. This nonexponential decay is shown to result from a multipolar interaction between the excited adsorbate and the intrinsic defects of silica. We present experimental evidence for direct energy transfer between the donor molecules, naphthalene and 2-methoxynaphthalene, and acceptor defects sites of a crystalline silica zeloite (silicalite). The principal condition for direct energy transfer, spectral overlap between the optical absorption of the defects and the fluorescence emission of the adsorbate is demonstrated for this system, and the nonexponential relaxation of the donor is shown to be described by a Forster-type stretched exponential. Based on the spectral overlap and energy transfer rate determined, the intrinsic defect density of silicalite is calculated to be 3±2×10 cm^-3.


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Journal of Chemical Physics

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July 27, 2010