| Organic structures have become promising candidates for nonlinear optical materials in recently years due to their excellent optical responses and structural flexibilities. Many potential applications based on two-photon absorption (TPA) process are proposed and demonstrated by using organic compounds in the past few years. These applications mainly rely on large molecular two-photon absorptivity which is an intrinsic property of the material itself. In order to effectively design and utilize organic materials with enhanced two-photon absorption for the applications, it is necessary to analyze structure-property relationship systematically. On the other hand, the development of improved techniques for the characterization of molecular nonlinear absorption behavior is another important task.; The combination of molecular design and reliable characterization method development toward the understanding of structure-TPA property relationship is the original purpose of this thesis. It starts with the synthesis of several series of model organic compounds derivatized from trans-stilbene with various structural effects which are expected to influence molecular two-photon absorptivities. It followed by the development of efficient measurement method to probe molecular two-photon absorption behavior. Combining the measured results from our recently accomplished two-photon absorption spectra acquisition method, some detailed structural parameters of these model compounds are studied and discovered.; Other than the major parts, this thesis also includes our most recent experimental result of three-photon induced up-converted stimulated emission behavior from a chromophore solution and the electroluminescence properties of selected three model compounds. |