Solvating machine-learning interatomic potentials for solution-phase chemistry
Organizations: Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA
Abstract
Most machine-learning interatomic potentials (MLIPs) are trained on gas-phase data, which limits their use for chemistry in solution. Here, we introduce AnySolv, a transferable implicit solvation potential that provides solvent-dependent energy and force corrections to existing gas-phase potentials without retraining them. It is trained on 1.4 million solvation energies and forces computed with density functional theory (DFT) and SMD in 36 solvents, spanning charged, open-shell, and transition-state structures. Because solvents are represented by continuous physical descriptors, AnySolv supports 179 solvents, including those absent from training. On external benchmarks, AnySolv reproduces DFT-SMD solvation energies to 2-4 meV mean absolute error at more than three orders of magnitude lower cost, and it matches the accuracy of DFT-SMD against experimental solvation free energies. This enables screening of the mechanisms of 120 nucleophilic aromatic substitution reactions in six phases as well as molecular dynamics simulations that reproduce the experimentally observed solvent-dependent conformational preferences of alanine dipeptide. By providing transferable solvation corrections to existing MLIPs, AnySolv enables scalable simulations of solvent-dependent chemical reactivity and molecular dynamics.
Figures & tables
| Descriptor | Definition | ||
|---|---|---|---|
| index of refraction (293 K) | 0.0684 | ||
| Abraham H-bond acidity, | – | 0.182 | |
| Abraham H-bond basicity, | – | 0.235 | |
| surface tension (cal mol -1 Å -2 ) | – | 11.69 | |
| dielectric constant (298 K) | 0.165 | ||
| aromaticity | – | 0.322 |
| MoE | compact | ||||||
|---|---|---|---|---|---|---|---|
| Solutes | |||||||
| all | 36,847 | 0.016 | 0.026 | 0.970 | 0.020 | 0.030 | 0.963 |
| neutral | 27,523 | 0.012 | 0.021 | 0.974 | 0.014 | 0.024 | 0.970 |
| cations | 4,894 | 0.024 | 0.038 | 0.948 | 0.034 | 0.046 | 0.932 |
| anions | 4,430 | 0.028 | 0.038 | 0.971 | 0.042 | 0.052 | 0.953 |
| MoE | compact | DFT-SMD | ||||||
|---|---|---|---|---|---|---|---|---|
| Solutes | ||||||||
| Solv@TUM neutral | 4,510 | 0.92 ( 0.27) | 0.89 ( 0.24) | 0.99 ( 0.48) | 0.92 ( 0.26) | 0.89 ( 0.22) | 0.98 ( 0.45) | 0.93 ( 0.24) |
| FlexiSol neutral | 529 | 2.48 ( 1.29) | 2.46 ( 1.03) | 2.47 ( 0.52) | 2.48 ( 1.29) | 2.45 ( 1.03) | 2.45 ( 0.57) | 2.51 ( 1.34) |
| MNSol neutral | 2,530 | 0.83 ( 0.24) | 0.84 ( 0.35) | 0.95 ( 0.52) | 0.82 ( 0.22) | 0.83 ( 0.33) | 0.93 ( 0.50) | 0.83 ( 0.22) |
| MNSol cations | 132 | 4.77 ( 3.92) | 4.60 ( 3.64) | 4.56 ( 3.64) | 4.78 ( 3.92) | 4.60 ( 3.64) | 4.60 ( 3.69) | 4.79 ( 3.94) |
| MNSol anions | 222 | 5.59 ( 3.25) | 5.08 ( 2.40) | 5.17 ( 2.60) | 5.73 ( 3.57) | 5.19 ( 2.70) | 5.29 ( 2.92) | 5.49 ( 3.13) |
| (kcal/mol) | (kcal/mol) | (Å) | (Å) | |||||||||
|---|---|---|---|---|---|---|---|---|---|---|---|---|
| Phase | DFT-SMD | MoE | compact | DFT-SMD | MoE | compact | DFT-SMD | MoE | compact | DFT-SMD | MoE | compact |
| gas phase | 43.1 | 43.0 | 43.0 | 41.2 | 41.4 | 41.4 | 2.45 | 2.46 | 2.46 | 2.77 | 2.77 | 2.77 |
| -hexane | 32.8 | 32.7 | 33.5 | 18.9 | 18.8 | 18.9 | 2.33 | 2.32 | 2.32 | 3.00 | 3.06 | 3.04 |
| chloroform | 27.0 | 26.8 | 28.2 | 1.1 | 0.3 | 5.5 | 2.27 | 2.26 | 2.24 | 3.25 | 3.43 | 4.60 |
| methanol | 23.8 | 23.5 | 25.0 | 10.9 | 11.4 | 19.6 | 2.23 | 2.22 | 2.22 | 3.62 | 3.51 | 4.49 |
| acetonitrile | 23.4 | 23.7 | 25.1 | 11.3 | 12.0 | 21.1 | 2.23 | 2.23 | 2.23 | 3.61 | 3.49 | 4.50 |
| Gas phase | Solvated | |||||
| Gas-phase model | MSE | MAE | MSE | MAE | ||
| Trained on OMol25 | ||||||
| UMA-S-1.2 | 0.0 | 0.2 | 0.1 | 0.3 | 0.7 | 0.7 |
| MACE-POLAR-1-M | 0.4 | 0.2 | 0.5 | 0.5 | 0.4 | 0.4 |
| OrbMol-v2 | 0.2 | 0.1 | 0.2 | 0.4 | 0.8 | 0.8 |
Appendix figures & tables8 assets
Supplementary material from the paper’s appendix.
Appendix
| MoE | compact | |
| initialization | UMA-S-1.2 checkpoint, solvent block grafted | random |
| parameters, total | 291,303,796 | 6,368,052 |
| expert SO(2) weights | 289,406,976 | – |
| router and composition embedding | 70,464 | – |
| parameters after merging for one system | 6,348,340 | 6,368,052 |
| experts per SO(2) linear layer | 64 | 1 |
| ALPB Pretraining | Training with SMD Labels | |
|---|---|---|
| initialization | MoE: UMA-S-1.2 backbone; compact: random | pretrained weights |
| labels | GFN2-xTB/ALPB, 21 solvents (5.46 M) + DFT-SMD water (173 k) | DFT-SMD, 36 solvents (1.35 M) |
| unique training labels | 5,633,695 | 1,355,281 |
| labels sampled per epoch | 3,356,976 | 1,383,400 |
| stage | model | epochs | peak learning rate | steps | GPUs |
|---|---|---|---|---|---|
| ALPB Pretrain | MoE | 4 | 839,244 | H200 | |
| ALPB Pretrain | compact | 8 | 1,678,488 | H200 | |
| DFT-SMD | MoE | 4 | 345,852 | H100 | |
| DFT-SMD | compact | 4 | 345,852 | A100 |
| Solvent | Labels | Solvent | Labels |
| OMol25 labels | |||
| acetone | 34,089 | 1,4-dioxane | 34,241 |
| acetonitrile | 34,249 | ethanol | 34,042 |
| aniline | 33,804 | ethyl acetate | 33,784 |
| benzaldehyde | 34,289 | -hexadecane | 34,303 |
| benzene | 34,341 | -hexane | 34,317 |
| UMA-S-1.2 | MACE-POLAR-1-M | ||||
|---|---|---|---|---|---|
| Solutes | |||||
| Solv@TUM neutral | 4,510 | 0.89 ( 0.24) | 0.99 ( 0.48) | 0.90 ( 0.24) | 1.00 ( 0.49) |
| FlexiSol neutral | 529 | 2.46 ( 1.03) | 2.47 ( 0.52) | 2.46 ( 1.02) | 2.48 ( 0.53) |
| MNSol neutral | 2,530 | 0.84 ( 0.35) | 0.95 ( 0.52) | 0.84 ( 0.35) | 0.96 ( 0.52) |
| MNSol cations | 132 | 4.60 ( 3.64) | 4.56 ( 3.64) | 4.59 ( 3.64) | 4.57 ( 3.67) |
| MNSol anions | 222 | 5.08 ( 2.40) | 5.17 ( 2.60) | 5.06 ( 2.38) | 5.22 ( 2.60) |
| MoE | compact | |
| SAMPL6: RMSE of against experiment | ||
| Boltzmann ensemble | 0.51 | 0.51 |
| lowest-free-energy conformer | 0.53 | 0.54 |
| Zwitterions: error against DFT-SMD (kcal/mol) | ||
| extended, MAE / max | 0.31 / 1.14 | 0.25 / 1.27 |
| cyclic, MAE / max | 0.18 / 1.39 | 0.21 / 1.54 |
Machine Learning Interatomic Potentials
Machine learning interatomic potentials predict atomic energies and forces for fast simulations of molecules and materials.
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