Basdogan, YaseminGroenenboom, Mitchell C.Henderson, EthanDe, SandipRempe, Susan B.Keith, John A.2020-03-032020-03-032020-03-032020-01-0110.1021/acs.jctc.9b00605https://infoscience.epfl.ch/handle/20.500.14299/166801WOS:000508474800049Molecular-level understanding and characterization of solvation environments are often needed across chemistry, biology, and engineering. Toward practical modeling of local solvation effects of any solute in any solvent, we report a static and all-quantum mechanics-based cluster-continuum approach for calculating single-ion solvation free energies. This approach uses a global optimization procedure to identify low-energy molecular clusters with different numbers of explicit solvent molecules and then employs the smooth overlap for atomic positions learning kernel to quantify the similarity between different low-energy solute environments. From these data, we use sketch maps, a nonlinear dimensionality reduction algorithm, to obtain a two-dimensional visual representation of the similarity between solute environments in differently sized microsolvated clusters. After testing this approach on different ions having charges 2+, 1+, 1-, and 2-, we find that the solvation environment around each ion can be seen to usually become more similar in hand with its calculated single-ion solvation free energy. Without needing either dynamics simulations or an a priori knowledge of local solvation structure of the ions, this approach can be used to calculate solvation free energies within 5% of experimental measurements for most cases, and it should be transferable for the study of other systems where dynamics simulations are not easily carried out.Chemistry, PhysicalPhysics, Atomic, Molecular & ChemicalChemistryPhysicsquasi-chemical theoryhydration free-energydensity-functional theorygibbs free-energymolecular-dynamicsab-initiocontinuum calculationsion solvationgas phasewatertext::journal::journal article::research article