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  4. Simulating Solvation and Acidity in Complex Mixtures with First-Principles Accuracy: The Case of CH3SO3H and H2O2 in Phenol
 
research article

Simulating Solvation and Acidity in Complex Mixtures with First-Principles Accuracy: The Case of CH3SO3H and H2O2 in Phenol

Rossi, Kevin  
•
Juraskova, Veronika  
•
Wischert, Raphael
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August 11, 2020
Journal of Chemical Theory and Computation

We present a generally applicable computational framework for the efficient and accurate characterization of molecular structural patterns and acid properties in an explicit solvent using H2O2 and CH3SO3H in phenol as an example. To address the challenges posed by the complexity of the problem, we resort to a set of data-driven methods and enhanced sampling algorithms. The synergistic application of these techniques makes the first-principle estimation of the chemical properties feasible without renouncing to the use of explicit solvation, involving extensive statistical sampling. Ensembles of neural network (NN) potentials are trained on a set of configurations carefully selected out of preliminary simulations performed at a low-cost density functional tight-binding (DFTB) level. The energy and forces of these configurations are then recomputed at the hybrid density functional theory (DFT) level and used to train the neural networks. The stability of the NN model is enhanced by using DFTB energetics as a baseline, but the efficiency of the direct NN (i.e., baseline-free) is exploited via a multiple-time-step integrator. The neural network potentials are combined with enhanced sampling techniques, such as replica exchange and metadynamics, and used to characterize the relevant protonated species and dominant noncovalent interactions in the mixture, also considering nuclear quantum effects.

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Type
research article
DOI
10.1021/acs.jctc.0c00362
Web of Science ID

WOS:000562139200031

Author(s)
Rossi, Kevin  
Juraskova, Veronika  
Wischert, Raphael
Garel, Laurent
Corminboeuf, Clemence  
Ceriotti, Michele  
Date Issued

2020-08-11

Publisher

AMER CHEMICAL SOC

Published in
Journal of Chemical Theory and Computation
Volume

16

Issue

8

Start page

5139

End page

5149

Subjects

Chemistry, Physical

•

Physics, Atomic, Molecular & Chemical

•

Chemistry

•

Physics

•

potential-energy surfaces

•

molecular-dynamics simulations

•

chemistry

•

constants

•

mechanism

•

driven

•

tool

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LCMD  
COSMO  
Available on Infoscience
September 10, 2020
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/171532
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