Efficient Third Harmonic Generation in a Metal-Organic Framework

As a recently emerged class of inorganic organic hybrid crystals, metal organic frameworks (MOFs) have been investigated for their capabilities for doubling light frequency. We report, for the first time, our observation of an efficient coherent up-conversion via third harmonic generation (THG) in a MOF. It is achieved by utilizing a MOF with a constituent ligand that possesses significant third-order nonlinear optical (NLO) responses. Our THG measurements at fundamental wavelengths ranging from 1200 to 1600 nm show that the MOF constructed with the An2Py ligand exhibits an effective chi((3)) value that is 3 orders of magnitude greater than alpha-quartz. Our findings demonstrate a new avenue to realize efficient third-order NLO responses by utilizing MOFs consisting of strong third-order NLO ligands.