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Binding reactions at finite systems.
Ronen Zangi1,2
1POLYMAT & Department of Organic Chemistry I, University of the Basque Country UPV/EHU, Avenida de Tolosa 72, 20018, Donostia-San Sebastián, Spain. r.zangi@ikerbasque.org.
Averages of binding reaction properties differ between small and large systems. However, the equilibrium constant remains consistent across system sizes when reactant concentration correlations are considered.
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Area of Science:
- Statistical Mechanics
- Physical Chemistry
- Computational Science
Background:
- Scientists aim to study small physical systems, mirroring experimental single-molecule tracking.
- A key question is whether properties observed in small systems match those in large, macroscopic systems.
Purpose of the Study:
- To investigate if averages of intensive parameters in finite systems differ from those in large systems.
- To explore the implications for binding reactions, equilibrium constants, and reaction rate constants.
Main Methods:
- Utilized statistical-mechanics formulations in fixed-particle-number ensembles.
- Derived relations to predict system composition from equilibrium constants and system size.
- Validated predictions using Monte Carlo and molecular dynamics simulations.
Main Results:
- Properties of binding reactions are not homogeneous functions; averages differ between finite and large systems.
- Discrepancies in averages increase with decreasing temperature, volume, and particle number.
- The equilibrium constant remains consistent across system sizes when reactant concentration correlations are accounted for.
Conclusions:
- Correlations in reactant concentrations are significant in small systems and must be included in the equilibrium constant expression.
- The expression for the equilibrium constant in finite systems depends on elementary processes, not just the chemical equation.
- Derived relations allow prediction of system composition based on equilibrium constants and system size.