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Research in our laboratory currently centers around structurally pre-organized chemical architectures, in which the generation, transport, and decay of energy- or charge-carrying species are coupled to molecular recognition events. Presented with appropriate receptor units, these chemical platforms effectively transduce molecular recognition events to readable optoelectronic signal outputs. Synthetic organic and inorganic chemistry thus plays a pivotal role in our research program by providing well-defined d-π or π-π platforms having unusual structural as well as electronic properties. Detailed understanding of such hybrid systems is aided by crystallographic, spectroscopic, electrochemical, and theoretical methods. Fundamental scientific insights obtained from studies of these photo- or electroactive small molecules guide us in the exploration of their linearly conjugated systems (LCSs) of practical importance.
Electron Trafficking between Metal Clusters and Non-innocent Ligand LCSs. In naturally occurring systems, electronically coupled multiple metal centers work in concert to define favorable energy windows and minimize structural reorganizations accompanying electron transfer. Drawing inspiration from biology, we are investigating redox-active metal clusters placed within the charge conduits afforded by "non-innocent" ligand LCSs.
Loosely Held Polyaromatic Scaffolds for Conjugated Polymers (CPs). Site-isolation is a well-known trick in living systems, by which protein matrix gates access to buried binding sites. Emulating such naturally occurring architectural and functional properties, we are investigating 3-D macrocyclic hosts presenting precisely positioned functional group arrays. Grafted onto LCSs, these semi-rigid multidentate "ligands" serve as receptor units for chemical sensing.
Conjugation Beyond π-π: Heteroatom-Containing CPs. Transition metal-catalyzed coupling reactions allow entry into an elusive class of [n,π]-conjugated organic fragments having unusual optoelectronic properties. The oxidation potential of this underutilized functional motif is significantly lower than that of conventional LCSs, and its operational redox window is readily modified using modularly accessible electronic controller groups.
Riddle, J. A.; Jiang, X.; Huffman, J.; Lee, D. Signal-Amplifying Resonance Energy Transfer: A Dynamic Multichromophore Array for Allosteric Switching. Angew. Chem. Int. Ed. 2007, 46, in press.
Lim, Y.-K.; Jiang, X.; Bollinger, J. C.; Lee, D., Molecular engineering of two-dimensional π-conjugation: Expected and unexpected photophysical consequences of simple particle-in-a-box approach. J. Mater. Chem. 2007, 17, 1969-1980.
Lim, Y.-K.; Wallace, S.; Bollinger, J. C.; Chen, X.; Lee, D., Triferrocenes Built on a C<sub>3</sub>-Symmetric Ligand Platform: Entry to Redox-Active Pseudo-Triphenylenes via Chelation-Driven Stereoselection of Triple Schiff Bases. Inorg. Chem. 2007, 46, 1694-1703.
Jiang, X.; Bollinger, J. C.; Lee, D.; Two-Dimensional Electronic Conjucation: Cooperative Folding and Fluorescence Switching. J. Am. Chem. Soc. 2006, 128, 11732-11733.
Riddle, J. A.; Lathrop, S. P.; Bollinger, J. C.; Lee, D., Schiff Base Route to Stackable Pseudo-Triphenylenes: Stereoelectronic Control of Assembly and Luminescence. J. Am. Chem. Soc. 2006, 128, 10986-10987.
Jiang, X.; Bollinger, J. C.; Lee, D., How Bulky Is a Bulky Ligand: Energetic Consequences of Steric Constraint in Ligand-Directed Cluster Assembly and Disassembly. J. Am. Chem. Soc. 2005, 127, 15678-15679.
Riddle, J. A.; Bollinger, J. C.; Lee, D., Escape from a Nonporous Solid: Mechanically Coupled Biconcave Molecules. Angew. Chem. Int. Ed. 2005, 44, 6689-6693.
Jiang, X.; Bollinger, J. C.; Baik, M.-H.; Lee, D. Copper clusters built on bulky amidinate ligands: spin delocalization via superexchange rather than direct metal-metal bonding. Chem. Commun. 2005, 1043-1045.
Lee, D.; Swager, T. M., Defining Space around Conjugated Polymers: New Vistas in Self-Amplifying Sensory Materials. Synlett 2004, 149-154.
Lee, D.; Lippard, S. J. Chapt 8.13 Nonheme Di-iron Enzymes in COMPREHENSIVE COORDINATION CHEMISTRY-II: From Biology to Nanotechnology; Elsevier Science: Oxford, U.K., 2003; Vol 8, pp 309-342.
Lee, D.; Swager, T. M., Defining Space around Conducting Polymers: Reversible Protonic Doping of a Canopied Polypyrrole. J. Am. Chem. Soc. 2003, 125, 6870-6871.
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