Abstract
Almost three decades ago, the field of nonlinear optics evolved with the discovery of lasers. In the beginning, nonlinear optical (NLO) phenomena were investigated in inorganic materials, leading to the development of traditional NLO materials such as lithium niobate, potassium titanyl phosphate, quartz and gallium arsenide. In the 1970s, the importance of organic materials was realized because of the promise of large NLO responses, high laser damage thresholds, fast optical responses, architectural flexibility and ease of fabrication. Following work with organic materials, the scrutiny of organometallics also began recently. In organometallics, the metal‐ligand bonding is expected to display large molecular hyperpolarizability because of the transfer of electron density between the metal atom and the conjugated ligand system. In organometallics, the diversity of central metals, oxidation states and ligands fosters in optimization of the charge‐transfer interactions. Keeping this in view, second‐ and third‐order NLO properties of organometallics have been reviewed here, highlighting new materials that are emerging. Organometallics may have a wide range of applications in opto‐electronics including integrated optics, optical switching, telecommunications, bistability and modulation.