Open AccessDirect free energy evaluation of classical and quantum many-body systems via field-theoretic simulation
Author(s) -
Glenn H. Fredrickson,
Kris T. Delaney
Publication year - 2022
Publication title -
proceedings of the national academy of sciences of the united states of america
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.011
H-Index - 771
eISSN - 1091-6490
pISSN - 0027-8424
DOI - 10.1073/pnas.2201804119
Subject(s) - degrees of freedom (physics and chemistry) , statistical physics , quantum , operator (biology) , field (mathematics) , gibbs free energy , energy (signal processing) , molecular dynamics , computer science , physics , classical mechanics , quantum mechanics , mathematics , chemistry , biochemistry , repressor , transcription factor , pure mathematics , gene
Significance The accurate evaluation of free energies within molecular simulations is important to many scientific fields, including fluid and solid phase equilibria, biomolecular condensates, and quantum phase transitions, among others. Unfortunately, free energy estimation is tedious and computationally expensive for molecular models whose degrees of freedom are expressed in particle coordinates. We show that alternative representations of a model as a classical or quantum field theory provide access to a chemical potential operator that can be averaged to yield a direct and low-cost estimate of the Gibbs free energy. The averaging is performed using a “field-theoretic” computer simulation that employs fluctuating fields rather than particles.