with the CGF of the total solute-solvent potential energy distribution (with λ = 1). In this context, the (solute-solvent) solvation energy, E U,V = ⟨V U,V ⟩ 1 , corresponds to the first cumulant, i.e. the mean of the distribution, while the solute-solvent entropy, S U,V = -k B ln⟨e +βδ1V U,V ⟩ 1 , corresponds to the remainder of the cumulant expansion, and thus encodes properties of the solute-solvent potential distribution which quantify the effects that correlations between the solute and solvent have on the solvation entropy. When looking at relative differences between -T S U,V values (for instance when taking the difference, ∆ bulk ), a positive difference corresponds to a broadening of the E U,V distribution, which is a fingerprint of structuring of the solvent around the solute due to the fact that a broader E U,V distribution means that the solute-solvent interactions are more sensitive to the solute-solvent structure, thus leading to stronger correlations and hence a decrease in the solute-solvent entropy (and vice versa for negative differences). Throughout the analysis we will refer to this effect in these terms.