Molecularly Informed Field Theories from Bottom-up Coarse-Graining

Area of Science:

• Polymer Science
• Computational Chemistry
• Materials Science

Background:

• Atomistic simulations struggle with polymer mesostructures due to scale disparities.
• Field-based simulations require predefined coarse-grained interaction parameters (e.g., χ-parameters).

Purpose of the Study:

• To develop a bottom-up coarse-graining methodology for accurate polymer phase behavior prediction.
• To bridge the gap between atomistic detail and coarse-grained field theories.

Main Methods:

• Leveraging all-atom molecular dynamics to inform coarser field-theoretic models.
• Employing relative-entropy coarse-graining to parameterize particle models.
• Analytically transforming particle models into statistical field theories.

Main Results:

• Successfully reproduced experimental aqueous poly(ethylene oxide) (PEO) cloud-point curves.
• Demonstrated predictive capability without fitting parameters to experimental data.

Conclusions:

• The synergistic multiscale approach overcomes limitations of traditional simulation methods.
• Enables de novo exploration of phase behavior in diverse polymer formulations.