materialscloud:2019.0010/v2
Published February 14, 2020 | Version v2
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Enhanced sampling of transition states

Creators

  • 1. Department of Chemistry and Applied Biosciences, ETH Zurich, c/o USI Campus, Via Giuseppe Buffi 13, CH-6900, Lugano, Switzerland
  • 2. Department of Physics, ETH Zurich, c/o USI Campus, Via Giuseppe Buffi 13, CH-6900, Lugano, Switzerland

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Description

The free energy landscapes of several fundamental processes are characterized by high barriers separating long-lived metastable states. In order to explore these type of landscapes enhanced sampling methods are used. While many such methods are able to obtain sufficient sampling in order to draw the free energy, the transition states are often sparsely sampled. We propose an approach based on the Variationally Enhanced Sampling Method to enhance sampling in the transition region. To this effect, we introduce a dynamic target distribution which uses the derivative of the instantaneous free energy surface to locate the transition regions on the fly and modulate the probability of sampling different regions. Finally, we exemplify the effectiveness of this approach in enriching the number of configurations in the transition state region in the cases of a chemical reaction and of a nucleation process.

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References

Preprint (Preprint where the method and a few of its applications are discussed.)
J. Debnath, M. Invernizzi, M. Parrinello, arXiv preprint, arXiv:1812.09032

Journal reference (Paper in which the method is explained and the results are discussed.)
J. Debnath, M. Invernizzi, M. Parrinello, J. Chem. Theory Comput. 15, 4 (2019), 2454-2459, doi: 10.1021/acs.jctc.8b01283

Journal reference (Paper in which the method is explained and the results are discussed.)
J. Debnath, M. Invernizzi, M. Parrinello, J. Chem. Theory Comput. 15, 4 (2019), 2454-2459