Machine Learning Approach to Vertical Energy Gap in Redox Processes

Ronit Sarangi, Suman Maity, Atanu Acharya

Research output: Contribution to journalArticlepeer-review

Abstract

A straightforward approach to calculating the free energy change (ΔG) and reorganization energy of a redox process is linear response approximation (LRA). However, accurate prediction of redox properties is still challenging due to difficulties in conformational sampling and vertical energy-gap sampling. Expensive hybrid quantum mechanical/molecular mechanical (QM/MM) calculations are typically employed in sampling energy gaps using conformations from simulations. To alleviate the computational cost associated with the expensive QM method in the QM/MM calculation, we propose machine learning (ML) methods to predict the vertical energy gaps (VEGs). We tested several ML models to predict the VEGs and observed that simple models like linear regression show excellent performance (mean absolute error ∼0.1 eV) in predicting VEGs in all test systems, even when using features extracted from cheaper semiempirical methods. Our best ML model (extra trees regressor) shows a mean absolute error of around 0.1 eV while using features from the cheapest QM method. We anticipate our approach can be generalized to larger macromolecular systems with more complex redox centers.

Original languageEnglish (US)
Pages (from-to)6747-6755
Number of pages9
JournalJournal of Chemical Theory and Computation
Volume20
Issue number15
DOIs
StatePublished - Aug 13 2024

ASJC Scopus subject areas

  • Computer Science Applications
  • Physical and Theoretical Chemistry

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