Li, JianghuaZhang, JinfangZhang, ChiHumphrey, Mark2015-12-101434-1948http://hdl.handle.net/1885/62965This article provides a concise summary of recent research progress, including synthetic strategies, structural diversity, theoretical studies, and third-order nonlinear optical (NLO) properties, on Mo(W)/S(Se)/Ag heterobimetallic clusters. It offers a preliminary analysis of their metal-cation-directed synthesis, structures, and the subtle interplay of structural-functional relationships. Furthermore, DFT was used to provide an insight into the electronic transitions and spectral characterization of these clusters. Recent trends and perspectives of these clusters as NLO materials are also described. The metal-cation-directed synthesis of multifarious novel zero- and one-dimensional Mo(W)/S(Se)/Ag heterobimetallic clusters is comprehensively summarized. The factors influencing the synthesis and structures of the clusters, and correlations between the molecular structures and NLO properties are discussed.Keywords: Cluster compounds; Density functional calculations; Molybdenum; Nonlinear optics; Selenium; Silver; Structure elucidation; Sulfur; Tungsten201310.1002/ejic.2012007352016-02-24