title: Diabat Interpolation for Polymorph Free-Energy Differences.
abstract: Existing methods to compute free-energy differences between polymorphs use harmonic approximations, advanced non-Boltzmann bias sampling techniques, and/or multistage free-energy perturbations. This work demonstrates how Bennett's diabat interpolation method ( J. Comput. Phys. 1976, 22, 245 ) can be combined with energy gaps from lattice-switch Monte Carlo techniques ( Phys. Rev. E 2000, 61, 906 ) to swiftly estimate polymorph free-energy differences. The new method requires only two unbiased molecular dynamics simulations, one for each polymorph. To illustrate the new method, we compute the free-energy difference between face-centered cubic and body-centered cubic polymorphs for a Gaussian core solid. We discuss the justification for parabolic models of the free-energy diabats and similarities to methods that have been used in studies of electron transfer.
authors.affiliation: Department of Chemical Engineering and ‡Department of Chemistry and Biochemistry, University of California , Santa Barbara, California 93106, United States.
authors.forename: Kartik
authors.identifier: http://orcid.org/0000-0002-0909-8839
authors.initials: K
authors.lastname: Kamat
authors.affiliation: Department of Chemical Engineering and ‡Department of Chemistry and Biochemistry, University of California , Santa Barbara, California 93106, United States.
authors.forename: Baron
authors.initials: B
authors.lastname: Peters