Unveiling the Role of Solvent in Solution Phase Chemical Reactions Using Deep Potentials-based Enhanced Sampling Simulations

16 July 2024, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

We have used the deep learning-based active learning strategy to develop ab initio accurate machine-learned (ML) potential for a solution phase reactive system. This approach enables us to study the effect of solvents on chemical reactions. As a paradigmatic example, we have investigated the Menshutkin reaction, a classic bimolecular nucleophilic substitution SN2 reaction in aqueous medium. Enhanced sampling simulations using the ML potential enabled efficient sampling of multiple transitions between the reactant and the product states, allowing us to calculate the converged free energy surface. Our analysis revealed that water stabilizes the product state, facilitating the reaction and making it more spontaneous. Our approach expands the scope of studying chemical reactions in explicit solvents at finite temperatures, closely mimicking experiments.

Keywords

Modelling Chemical Reactions
Explicit Solvent Simulations
MD simulations
ML potential
Enhanced Sampling

Supplementary materials

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Title
Unveiling the Role of Solvent in Solution Phase Chemical Reactions using Deep Potentials-based Enhanced Sampling Simulations
Description
The SI contains Computational details - AIMD and AIES simulations, DeepMD setup - Data generation, Training, and Validation, pair-correlation functions, solvent CV details
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