研究领域

Chemical Education/Organic Chemistry

In our lab we study various aspects of mechanistic organic and biochemistry, using the tools of photochemistry. We both study chemical reactions and use photophysical techniques to study processes that are difficult to investigate in other ways. One main area of research involves studies of bond fragmentation reactions that are initiated by either giving (reduction) or taking away (oxidation) a single electron. Such processes generate radicals and Lewis acids and Lewis bases, which may also be Bronsted acids and bases, all potentially useful catalytic species. We are currently studying extremely fast fragmentation reactions with the goal of developing reactions that occur with no barrier at all! We are also using these reactions as test cases for fundamental reaction rate theories and contemporary computational methods. Another area relates to the oxidative processes in DNA responsible for mutation, disease and aging. Novel photochemical reactions developed in our lab can be used to irreversibly oxidize the purine bases in DNA. We are currently studying the chemistry and physical properties of these species in order to understand the primary events involved in oxidative damage.

近期论文

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Godbout, J. T.; Zuilhof, H.; Heim, G.; Gould, I. R.; Goodman, J. G.; Dinnocenzo, J. P.; Myers Kelley, A. "Resonance Raman Studies of Phenylcyclopropane Radical Cations", J. Raman Spectrosc. 2000, 31, 233. Gould, I. R.; Lenhard, J. R.; Muenter, A. A.; Godleski, S. A.; Farid, S. "Two-Electron Sensitization: A New Concept for Silver Halide Photography", J. Am. Chem. Soc. 2000, 122, 11934. Fyson, J. R.; Twist, P. J.; Gould, I. R. "Electron Transfer Processes in Silver Halide Photography" In Electron Transfer in Chemistry; Balzani, V., Ed.; Wiley-VCH: New York, 2001, Vol. 5, p. 285. Gould, I. R.; Lenhard, J. R.; Muenter, A., A.; Godleski, S. A.; Farid, S. "Two-Electron Sensitization: A New Concept for Silver Halide Photography", Pure Appl. Chem. 2001, 73, 455. Gould, I. R.; Shukla, D.; Giesen, D.; Farid, S. "Energetics of Electron-Transfer Reactions of Photoinitiated Polymerization: Dye-Sensitized Fragmentation of N-alkoxypyridinium Salts", Helv. Chim. Acta 2001, 84, 2796. Lorance, E. D.; Kramer, W. H.; Gould, I. R. "Kinetics of Reductive N-O Bond Fragmentation: The Role of a Conical Intersection" J. Am. Chem. Soc. 2002, 124, 15225. Gould, I. R.; Boiani, J. A.; Gailard, E. B.; Goodman, J. L.; Farid, S "Intersystem Crossing in Charge-Transfer Excited States". J. Phys. Chem. A 2003, 107, 3515. Gould, I. R.; Godleski, S. A.; Zielinski, P. A. Farid, S. "Aminosilanes as Two-Electron Donors. A Technological Application of Radical Cation Chemistry" Can. J. Chem. 2003, 81, 777. Wang, Y.; Luttrull, D. K.; Dinnocenzo, J. P.; Goodman, J. L.; Farid, S, Gould, I. R. "Associative Return Electron Transfer. A Bond-Coupled Electron Transfer in the Photoreactions of Cyclopropylamines", Photochem. Photobiol. Sci. 2003, 11, 1169. Morkin, T. L.; Turro, N. J.; Kleinman, M. H.; Brindle, C. S.; Griffiths, K.; Kramer, W. H.; Gould, I. R. "A Novel Solid-State Photooxidant", J. Am. Chem. Soc. 2003, 125, 14917. Lorance, E. D.; Kramer, W. H.; Gould, I. R. "Barrierless Electron Transfer Bond Fragmentation Reactions " J. Am. Chem. Soc. 2004, 126, 14071. Gould, I. R.; Farid, S. "A Qualitative Curve-Crossing Model Describes the Kinetics of Oxidative Decarboxylation", J. Phys. Chem A. 2004, 108, 10949. Lorance, E. D., Hendrickson, K., Gould, I. R. " Density Functional Theory Accurately Predicts the Barriers for a Radical Reaction in Solution" J. Org. Chem., 2005, 70, 2014. Lorance, E. D.; Gould, I. R. "A Curve-Crossing Model Accurately Describes a Radical Reaction", J. Phys. Chem. A. 2005, 109, 2912. Dombrowski, G.; Dinnocenzo, J. P.; Zielinski, P.; Farid, S.; Wosinska, Z.; Gould, I. R. "Efficient Unimolecular Deprotonation of Aniline Radical Cations", J. Org. Chem. 2005, 70, 3791. Aksyonov, S. A.; Bittner, M.; Bloom, L. B.; Reha-Krantz, L. J.; Gould, I. R.; Hayes, M. A.; Kiernan, U. A.; Niederkofler, E. E.; Pizziconi, V.; Rivera, R. S.; Williams, D. J. B.; Williams, P. "Multiplexed DNA Sequencing-By-Synthesis", Anal. Biochem. 2006, 348, 127. Gould, I. R., Wosinska, Z. M.; Farid, S. "Kinetic Determinations of Accurate Relative Oxidation Potentials of Amines With Reactive Radical Cations", Photochem. Photobiol. 2006, 82, 104. Fu, X. Moss, R. A., Piotrowiak, P., Myahkostupov, M., Gould, I. R. "The Fragmentation of 2,2,2-Triphenylethoxychlorocarbene; Evidence for Ultrafast Fragmentation-Rearrangement in Excited Diaziriness", Org. Letts. 2006, 8, 4807. Gould, I. R., Farid, S. "Radiationless Decay in Exciplexes With Variable Charge-Transfer", J. Phys. Chem. B in press. Wang, Y.; Haze, O., Dinnocenzo, J. P., Farid, S., Farid, R. Gould, I. R. "Bonded Exciplexes. A New Concept in Photochemical Reactions", J. Am. Chem. Soc. submitted.