# Ring polymer molecular dynamics and active learning of moment tensor potential for gas-phase barrierless reactions: Application to S + H2.

@article{Novikov2019RingPM,
title={Ring polymer molecular dynamics and active learning of moment tensor potential for gas-phase barrierless reactions: Application to S + H2.},
author={Ivan S. Novikov and Alexander V. Shapeev and Yury V. Suleimanov},
journal={The Journal of chemical physics},
year={2019},
volume={151 22},
pages={
224105
}
}
• Published 13 September 2019
• Chemistry
• The Journal of chemical physics
Ring polymer molecular dynamics (RPMD) has proven to be an accurate approach for calculating thermal rate coefficients of various chemical reactions. For wider application of this methodology, efficient ways to generate the underlying full-dimensional potential energy surfaces (PESs) and the corresponding energy gradients are required. Recently, we have proposed a fully automated procedure based on combining the original RPMDrate code with active learning for PES on-the-fly using moment tensor…
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## References

SHOWING 1-10 OF 61 REFERENCES
Ring polymer molecular dynamics fast computation of rate coefficients on accurate potential energy surfaces in local configuration space: Application to the abstraction of hydrogen from methane.
• Chemistry
The Journal of chemical physics
• 2016
A segmented strategy for fitting suitable potential energy surface (PES) on which ring-polymer molecular dynamics (RPMD) simulations are performed, on which qualitative agreement between present RPMD rates and those from previous simulations as well as experimental results are found.
Bimolecular reaction rates from ring polymer molecular dynamics: application to H + CH4 → H2 + CH3.
• Chemistry
The Journal of chemical physics
• 2011
The results indicate that the previous assessment of the accuracy of the RPMD approximation for atom-diatom reactions remains valid for more complex polyatomic reactions, and suggest that the sensitivity of the QTST and QI rate coefficients to the choice of the transition state dividing surface becomes more of an issue as the dimensionality of the reaction increases.
Communication: Rate coefficients of the H + CH4 → H2 + CH3 reaction from ring polymer molecular dynamics on a highly accurate potential energy surface.
• Chemistry, Physics
The Journal of chemical physics
• 2015
The present RPMD rates are in excellent agreement with quantum rates computed on the same potential energy surface, as well as with the experimental measurements, demonstrating further that the RPMD is capable of producing accurate rates for polyatomic chemical reactions even at rather low temperatures.
Ring-polymer molecular dynamics: rate coefficient calculations for energetically symmetric (near thermoneutral) insertion reactions (X + H2) → HX + H(X = C(1D), S(1D)).
• Chemistry, Physics
The Journal of chemical physics
• 2014
For both chemical reactions, RPMD displays remarkable accuracy and agreement with the previous quantum dynamic results that make it encouraging for the future application of the RPMD to other barrier-less, complex-forming reactions involving polyatomic reactants with any exothermicity.
Chemical reaction rates from ring polymer molecular dynamics.
• Physics
The Journal of chemical physics
• 2005
The ring-polymer molecular dynamics method can be adapted to calculate approximate Kubo-transformed flux-side correlation functions, and hence rate coefficients for condensed phase reactions, and it gives the exact quantum-mechanical rate constant for the transmission through a parabolic barrier.
Ring-Polymer Molecular Dynamics Rate Coefficient Calculations for Insertion Reactions: X + H2 → HX + H (X = N, O).
• Physics, Materials Science
The journal of physical chemistry letters
• 2014
It is shown that the unique ability of the RPMD approach among the existing theoretical methods to capture the quantum effects, e.g., tunneling and zero-point energy, as well as recrossing dynamics quantum mechanically with ring-polymer trajectories leads to excellent agreement with rigorous quantum dynamics calculations.
A refined ring polymer molecular dynamics theory of chemical reaction rates.
• Physics, Chemistry
The Journal of chemical physics
• 2005
The long-time limit of the new flux-side correlation function, and hence the fully converged RPMD reaction rate, is rigorously independent of the choice of the transition state dividing surface, which is especially significant because the optimum dividing surface can often be very difficult to determine for reactions in complex chemical systems.
Thermal Rate Coefficients for the Astrochemical Process C + CH+ → C2+ + H by Ring Polymer Molecular Dynamics.
• Physics
The journal of physical chemistry. A
• 2016
There is a significant discrepancy between the RPMD rate coefficients and the previous theoretical results that can lead to overestimation of the rate coefficients for the title reaction by several orders of magnitude at very low temperatures.
Ring-Polymer Molecular Dynamics for the Prediction of Low-Temperature Rates: An Investigation of the C((1)D) + H2 Reaction.
• Chemistry
The journal of physical chemistry letters
• 2015
The ring-polymer molecular dynamics method is proposed as an accurate and efficient alternative for determining the kinetics and dynamics of a wide range of low-temperature reactions by analyzing the behavior of the barrierless C((1)D) + H2 reaction over the two lowest singlet potential energy surfaces.
Bimolecular reaction rates from ring polymer molecular dynamics.
• Physics, Chemistry
The Journal of chemical physics
• 2009
We describe an efficient procedure for calculating the rates of bimolecular chemical reactions in the gas phase within the ring polymer molecular dynamics approximation. A key feature of the