Lattice model of spatial correlations in catalysis

Area of Science:

• Chemical kinetics
• Single-molecule biophysics
• Catalysis science

Background:

• Single-turnover measurements offer detailed insights into catalyst behavior.
• Stochastic fluorescence trajectories reveal individual reaction and dissociation events.
• Bulk measurements average dynamics, obscuring single-event details.

Purpose of the Study:

• To model spatial correlations in catalytic activity.
• To investigate the influence of reactant transport among multiple active sites.
• To analyze how structure and dynamics affect catalytic efficiency.

Main Methods:

• Optically detected single-molecule catalysis measurements.
• Analysis of stochastic fluorescence trajectories.
• Development of a model for spatial correlations in catalysis.
• Application of perturbation theory to couple transport and reaction dynamics.

Main Results:

• Calculated mean dwell time of reactants on active sites.
• Determined correlations between reactant dwell times at different locations.
• Demonstrated how transport influences catalytic activity.
• Established a framework for understanding spatially correlated catalytic events.

Conclusions:

• Single-molecule measurements provide unprecedented detail on catalytic processes.
• Transport dynamics significantly impact catalytic activity and reaction correlations.
• The developed model offers a pathway to understand complex catalytic systems.
• Superresolution techniques can spatially resolve catalytic activity correlations.