Bubble nucleation in simple and molecular liquids via the largest spherical cavity method

Area of Science:

• Thermodynamics
• Computational Chemistry
• Physical Chemistry

Background:

• Bubble nucleation is crucial for phase transitions in liquids.
• Accurate calculation of free energy barriers is essential for understanding nucleation.
• Previous methods for monitoring nucleation events can be complex and require arbitrary criteria.

Purpose of the Study:

• To propose a novel methodology for computing bubble nucleation free energy barriers.
• To introduce a simplified order parameter for tracking nucleation events.
• To provide a computationally efficient route for nucleation studies.

Main Methods:

• Utilizing molecular dynamics simulations to generate system trajectories.
• Defining a local order parameter based on the volume of the largest spherical cavity (LSC).
• Employing the mean first passage time technique in conjunction with the LSC parameter.

Main Results:

• The LSC method effectively monitors bubble nucleation events.
• Free energy curves and barriers were computed using the LSC and mean first passage time.
• Calculated free energy barriers show good agreement with previous studies for simple liquids and water.

Conclusions:

• The LSC method provides a versatile and computationally efficient approach for nucleation studies.
• This methodology simplifies the analysis of nucleation events compared to prior techniques.
• The LSC approach is applicable to both simple and molecular liquids.