Effect of configuration-dependent multi-body forces on interconversion kinetics of a chiral tetramer model

Nikolai D. Petsev, Frank H. Stillinger, Pablo G. Debenedetti

Research output: Contribution to journalArticlepeer-review

Abstract

We describe a reformulation of the four-site molecular model for chiral phenomena introduced by Latinwo et al. [“Molecular model for chirality phenomena,” J. Chem. Phys. 145, 154503 (2016)]. The reformulation includes an additional eight-body force that arises from an explicit configuration-dependent term in the potential energy function, resulting in a coarse-grained energy-conserving force field for molecular dynamics simulations of chirality phenomena. In this model, the coarse-grained interaction energy between two tetramers depends on their respective chiralities and is controlled by a parameter λ, where λ < 0 favors local configurations involving tetramers of opposite chirality and λ > 0 gives energetic preference to configurations involving tetramers of the same chirality. We compute the autocorrelation function for a quantitative chirality metric and demonstrate that the multi-body force modifies the interconversion kinetics such that λ ≠ 0 increases the effective barrier for enantiomer inversion. Our simulations reveal that for λ > 0 and temperatures below a sharply defined threshold value, this effect is dramatic, giving rise to spontaneous chiral symmetry breaking and locking molecules into their chiral identity.

Original languageEnglish (US)
Article number084105
JournalJournal of Chemical Physics
Volume155
Issue number8
DOIs
StatePublished - Aug 28 2021

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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