Campus Units

Mechanical Engineering, Electrical and Computer Engineering, Plant Sciences Institute

Document Type


Publication Version

Submitted Manuscript

Publication Date


Journal or Book Title

Journal of Chemical Information and Modeling




As new generations of thin-film semiconductors are moving towards solution-based processing, the development of printing formulations will require information pertaining to the free energies of mixing of complex mixtures. From the standpoint of in silico materials design, this move necessitates the development of methods that can accurately and quickly evaluate these formulations in order to maximize processing speed and reproducibility. Here, we make use of molecular dynamics (MD) simulations in combination with the two-phase thermodynamic (2PT) model to explore the free energy of mixing surfaces for a series of halogenated solvents and high boiling point solvent additives used in the development of thin-film organic semiconductors. While the combined methods generally show good agreement with available experimental data, the computational cost to traverse the free-energy landscape is considerable. Hence, we demonstrate how a Bayesian optimization scheme, coupled with the MD and 2PT approaches, can drastically reduce the number of simulations required, in turn shrinking dramatically both the computational cost and time.


This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Journal of Chemical Information and Modeling, copyright © American Chemical Society after peer review. To access the final edited and published work see 10.1021/acs.jcim.9b01113. Posted with permission.

Copyright Owner

American Chemical Society



File Format


Published Version