Computational studies have been shown to provide theoretical support to the synthetic chemist. Compounds with high electronic asymmetry (by incorporating an electron donor and an electron acceptor on opposite sites of the molecule), highly conjugated -systems and large molecular weights (eg going from mono- to bi- to trimetallic complexes) have been shown to exhibit high NLO responses. However, the synthesis of these complexes can be costly and time consuming. Thus, theoretical / computational studies have greatly evolved over the past half-decade in order to guide the chemist in understanding the molecular electronic structure responsible for high NLO responses. Amsterdam Density Functional (ADF) and Gaussian09 softwares has been utilized in this work in order to provide information on how to design a highly potential material with high NLO responses in order to help facilitate the experimental works undertaking. The same software was also been used to study other related projects, as detailed in the talk.