Following the analysis of the OH region in the IR spectrum (Figure ), it is evident that the C/d strategy outperforms the Q/s approach, indicating that the populations derived from the classical MD trajectory better reflect the experimental behavior. But which factors account for the superiority of C/d populations over those from Q/s? To address this question, we need to consider the two thermodynamic contributions to population distributions: the enthalpic and entropic terms associated with the formation of aggregate.