A new approach for designing molecules with large hyperpolarizabilities: substituted C36 fullerenes as a test case

A new approach for designing molecules with large hyperpolarizabilities is proposed. As a test case, polarizabilities and hyperpolarizabilities were calculated for a series of amino-ethylene substituted C36 fullerenes. These molecules are symmetrical, and have a non-standard geometrical arrangement, the acceptor group being surrounded by the donating groups. The geometry for each fullerene was optimized at the 6-31G**++/B3LYP level. The α and β tensors were calculated in the vacuum optimized geometries at the 6-31G**++/CPHF level. The results show that these molecules may present high values for non-linear optical properties.