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We found the primary finite-size effect on ionic fluid thermodynamic properties. This Coulomb energy correction scales with temperature and particle number, crucial for accurate simulations of charged systems.

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Area of Science:

  • Physical Chemistry
  • Computational Physics
  • Statistical Mechanics

Background:

  • Accurate simulation of ionic fluids requires understanding system-size dependence.
  • Finite-size artifacts, particularly in Coulomb energy, can impact thermodynamic property calculations.
  • Periodic boundary conditions are commonly used but introduce size-dependent effects.

Purpose of the Study:

  • To determine the leading-order finite-size artifact in the Coulomb energy per particle for classical ionic fluids.
  • To develop analytical approximations for size dependence in excess thermodynamic properties within the weak-coupling regime.
  • To compare theoretical predictions with existing and new simulation data for charged fluids.

Main Methods:

  • Adaptation of a quantum Monte Carlo simulation approach for classical ionic systems.
  • Derivation of analytical expressions using linearized Debye-Hückel theory.
  • Comparison with simulations of the one-component plasma and primitive-model electrolyte solutions.

Main Results:

  • The leading-order finite-size artifact in Coulomb energy per particle is identified as -kBT(2N)-1.
  • Analytical approximations for size dependence in excess thermodynamic properties were obtained for the weak-coupling regime.
  • Theoretical results show good agreement with simulation data for both one-component plasmas and electrolyte solutions.

Conclusions:

  • The derived formula provides a key correction for finite-size effects in simulations of charged fluids.
  • The study offers a theoretical framework for estimating and correcting size-dependent artifacts.
  • Results are applicable to simulations of various charged systems, including those with explicit solvents.