Journal: The Journal of Physical Chemistry Letters, 8, 3152-3158 (2017)
Author: Seong Jun Park†§⊥, Sanggeun Song†‡§⊥, In-Chun Jeong†‡§, Hye Ran Koh†‡, Ji-Hyun Kim*†, and Jaeyoung Sung*†‡§
†National Creative Research Initiative Center for Chemical Dynamics in Living Cells, Chung-Ang University, Seoul 06974, Korea
‡Department of Chemistry, Chung-Ang University, Seoul 06974, Korea
§National Institute of Innovative Functional Imaging, Chung-Ang University, Seoul 06974, Korea
DOI: doi.org/10.1021/acs.jpclett.7b01218
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.