A characterization of the structure and optical properties of a series of metallotexaphyrin (MTXP) complexes is conducted using standard and novel measurement techniques, including degenerate four-wave mixing, Z-scan, optical power limiting, simulation of excited-state population dynamics, and semiempirical and ab initio calculations of molecular hyperpolarizability. The design and construction of a new and powerful tunable laser source allow for unparalleled characterization of materials across a broad wavelength range. This research provides for a better fundamental understanding of the origins of nonlinear optical response in MTXP complexes and for the facilitation of a systematic design procedure for these high-χ(3) excited-state absorbing materials. |