Materials with nonlinear optical (NLO) properties can be used to control and process light beams and consequently, have enormous importance in a wide range of technologies including photonics, nanotechnology, and medicine. A molecule that can exist in two stable states, interconvertible by application of an external stimulus such as light, heat, pressure, current, etc., is a molecular switch. In organometallic systems, the incorporation of one or more metal atoms into an organic framework can often introduce novel optical, electronic and/or magnetic properties; particularly in the case of organometallic cluster molecules. In principle, the optical, electronic, magnetic, and other properties can be switched independently and therefore such systems are potentially of use in higher-order logic operations because the switching increases the number of distinct addressable NLO “states”. We are using DFT and time-dependent DFT (TD-DFT) methods to explore organometallic systems comprising multiple elements (photochemical, electrochemical, thermochemical, conformational) that permit independent switching of NLO properties. These studies will direct the synthetic efforts of chemists in the design of materials with a large number of distinct, independently addressable NLO “states”, which in principle will allow superior control over NLO properties.
Optimized structure of the trans-RuCl(dppm)2C2Ph(C2H2Ph)3NO2 complex which is calculated to have significant second-order non-linear optical properties.