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J Phys Chem Lett. 2017 Jul 6;8(13):3152-3158. doi: 10.1021/acs.jpclett.7b01218. Epub 2017 Jun 26.

Nonclassical Kinetics of Clonal yet Heterogeneous Enzymes.

Park SJ1,2, Song S1,3,2, Jeong IC1,3,2, Koh HR1,3, Kim JH1, Sung J1,3,2.

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National Creative Research Initiative Center for Chemical Dynamics in Living Cells, Chung-Ang University , Seoul 06974, Korea.
National Institute of Innovative Functional Imaging, Chung-Ang University , Seoul 06974, Korea.
Department of Chemistry, Chung-Ang University , Seoul 06974, Korea.


Enzyme-to-enzyme variation in the catalytic rate is ubiquitous among single enzymes created from the same genetic information, which persists over the lifetimes of living cells. Despite advances in single-enzyme technologies, the lack of an enzyme reaction model accounting for the heterogeneous activity of single enzymes has hindered a quantitative understanding of the nonclassical stochastic outcome of single enzyme systems. Here we present a new statistical kinetics and exactly solvable models for clonal yet heterogeneous enzymes with possibly nonergodic state dynamics and state-dependent reactivity, which enable a quantitative understanding of modern single-enzyme experimental results for the mean and fluctuation in the number of product molecules created by single enzymes. We also propose a new experimental measure of the heterogeneity and nonergodicity for a system of enzymes.

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