An Extended Energy-Biased Aggregation-Volume-Bias Monte Carlo (EB-AVBMC) Method for Nucleation Simulation of a...

Area of Science:

• Computational Chemistry
• Materials Science
• Chemical Physics

Background:

• The aggregation-volume-bias Monte Carlo (AVBMC) algorithm is established for empirical water models.
• Application of AVBMC to reactive water models for nucleation and vapor-liquid properties is limited.
• Reactive force fields are crucial for accurate molecular simulations.

Purpose of the Study:

• To extend the energy-bias aggregation-volume-bias Monte Carlo (EB-AVBMC) method for reactive water models.
• To calculate nucleation free energies and liquid-vapor properties using a reactive force field.
• To validate the modified method for simulating reactive liquid-vapor systems.

Main Methods:

• Developed an extended EB-AVBMC method incorporating intramolecular energy in acceptance rules.
• Implemented constraints to prevent deletion of dissociated water molecules, ensuring bond topology integrity.
• Utilized a three-body reactive force field based on the Vashishta potential functional form.

Main Results:

• Successfully calculated water nucleation free energies at 298.15 K for varying cluster sizes.
• Obtained results consistent with those from rigid water models, validating the method.
• Demonstrated the method's capability in simulating gas density and surface tension.

Conclusions:

• The modified EB-AVBMC method accurately simulates nucleation free energies and liquid-vapor properties for reactive water models.
• The approach is generalizable to other reactive water force fields.
• This provides a valuable computational tool for studying reactive liquid-vapor phenomena.