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Research Interest -

Research Interest - - Research Interest Sean E Hightower...

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Research Interest Sean E. Hightower __________________________________________________________________________________________ 1 Figure 1: MO’s responsible for the LMCT transitions in [Re(dmpe) 3 ] 2+ Overview The four proposals revolve around the general area of preparative and physical inorganic/ organic chemistry, and its relation with the rapidly emerging field of materials/energy chemistry. The proposals focus on the preparation and complete characterization of the various metal complexes utilizing a variety of spectroscopic techniques to examine their energy/electron transfer pathways. My research group will focus on these motivating issues: (1) The development of highly oxidizing ligand-to-metal charge transfer excited states. (2) Investigation of the chemistry of carborane based metal complexes and their potential use as multielectron and/or multiphoton catalyst . (3) The development of multi photon device based on both trans-disposed ligand- to-metal charge transfer (LMCT) and metal-to-ligand charge transfer (MLCT) excited states. (4) The preparation of dual mode imaging agents based on luminescent technetium (Tc) complexes. Proposal I: New Chromophores for Solar Energy Conversion based on Highly Oxidizing Ligand-to-Metal Charge Transfer Excited States While the design of transition-metal based molecular sensitizers for use in artificial photosynthesis has been primarily confined to metal-to-ligand charge transfer (MLCT) excited states, much less attention has been focused on the development of molecular sensitizers with ligand-to-metal charge transfer (LMCT) excited states. The recent discovery that the LMCT excited state of [Re(dmpe) 3 ] 2+ has the highest highly oxidizing excited state potential for any simple coordination complex of a transition metal may indeed set a new precedent for the future of photocatalysis. Of particular importance is that this potential is available using a photon of visible light (M = Re(Tc); E 1/2 * = + 2.61 (+ 2.52) V calculated vs. SCE). The implications towards artificial photosynthesis for generating solar electricity are multifarious including the ability of such metal complexes to become highly oxidizing excited states (HOES) via absorption of visible light. Proposal II: Carborane Bridging Ligands for Rod-Like Oligometallic Complexes As natural stores of hydrocarbons dwindle, we are faced with the task of developing new technologies for fuel and chemical synthesis. Given the multielectron nature of the redox processes inherent with oligomeric complexes, there exist the promise of either accelerating the rate and/or changing the nature of the product distribution based on the type of ligand bridging the various sites. Carborane dianion spacers, which will convey novel properties such as low overall charge, rod-like behavior, short bridging distances, and possibly large electronic coupling to the resultant species may offer additional advantages in the design of molecular assemblies.
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