Optimizing the sensitivity of the instantaneous entropy of mixing

Abstract

We present a systematic optimization of a recently presented formulation for the calculation of the configurational entropy of mixing of a molecular liquid. The approach is based on the transformation of the particle coordinates to a partial density distribution with a certain broadening parameter. In this work, we investigate the influence of the broadening parameter on the numerical values of the computed entropy of mixing. The optimization of this parameter with respect to the sensitivity of the computed entropy yields a range of values in which the broadening can be chosen safely for most molecular situations. We illustrate how a problem-specific optimization of the broadening parameter can further improve the sensitivity.