Figure presents the total binding free energy (left) and the average binding free energy contribution from each SA-DMA or SA-AM pair in the clusters (right). As a comparison, we also plotted the data of the SA-AM clusters reported by Besel et al. and the SA-DMA clusters reported by Myllys et al. These are calculated at the DLPNO-CCSD(T 0 )/augcc-pVTZ//ωB97X-D/6-31++G(d,p) level of theory and the data are denoted as the "BM" series in the figures. As also pointed out in previous studies, the total binding free energy ∆G bind decreases almost linearly as the cluster size increases. This is seen to be almost perfectly linear for SA-DMA, whereas there is a slight fluctuation observed for SA-AM. This is most likely due to the complexity of the SA-AM clusters, having a higher degree of freedom compared to the SA-DMA clusters. The SA-DMA systems consistently exhibit lower free energies compared to the SA-AM systems. This is curious as the encapsulation of an aminium ion should destabilize the clusters. However, this finding indicates that the preference for sulfuric acid to bind more strongly to DMA compared to AM is retained even for large clusters. One could speculate that mixed SA-AM-DMA clusters might be even more stable than the SA-DMA clusters by having an ammonium ion encapsulated in the core. DePalma et al. reported that SA-AM and SA-DMA have different preference for hydration. While our study of dry clusters shows that SA-DMA is unequivocally more stable than SA-AM, hydration can be an interesting topic for further study.