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Mechanistic studies of class I diterpene synthases

Recognizing that rice produced numerous labdane-related diterpenoid natural products, and the opportunity presented by the publication of the rice genome sequence, we began by carrying out a functional genomics based investigation of the rice diterpene synthases.  Given the relative paucity of characterized diterpene synthases at that time, this effort more than doubled the number of molecularly identified functionally distinct such enzymes.  Strikingly, we further uncovered a functionally distinct pair of alleles for one of the rice class I diterpene synthases, which led to isola

Mechanistic studies of class II diterpene cyclases

The class II diterpene cyclases catalyze protonation-initiated (bi)cyclization reactions that characterize labdane-related diterpenoid biosynthesis. In collaboration with Prof. David Christianson (Univ. Penn), we have provided the first crystal structures for class II diterpene cyclases.  From these we have generated significant insights into the underlying determinants of enzymatic catalysis, including the generation of enzymes wherein single residue changes have led to novel product outcome.