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Communication: Organometallic chromophores encapsulated in zeolite-like cavities are demonstrated to be a promising system for third-order nonlinear optical effects. Nonasil, by isolating the chromophores, allows the application of strong electric fields. The Figure shows an optical micrograph of a crystal of the title compound flanked by two copper electrodes. When an electric field was applied, a strong second harmonic generation signal was observed.