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Published July 14, 2020 | Supplemental Material
Journal Article Open

Embedded Mean-Field Theory for Solution-Phase Transition-Metal Polyolefin Catalysis

Abstract

Decreasing the wall-clock time of quantum mechanics/molecular mechanics (QM/MM) calculations without sacrificing accuracy is a crucial prerequisite for widespread simulation of solution-phase dynamical processes. In this work, we demonstrate the use of embedded mean-field theory (EMFT) as the QM engine in QM/MM molecular dynamics (MD) simulations to examine polyolefin catalysts in solution. We show that employing EMFT in this mode preserves the accuracy of hybrid-functional DFT in the QM region, while providing up to 20-fold reductions in the cost per SCF cycle, thereby increasing the accessible simulation time-scales. We find that EMFT reproduces DFT-computed binding energies and optimized bond lengths to within chemical accuracy, as well as consistently ranking conformer stability. Furthermore, solution-phase EMFT/MM simulations provide insight into the interaction strength of strongly coordinating and bulky counterions.

Additional Information

© 2020 American Chemical Society. Received: February 18, 2020; Published: May 22, 2020. This work was carried out with financial support within the University Partnership Initiative from the Dow Chemical Company. This material is based upon work supported by the National Science Foundation Graduate Research Fellowship under Grant No. DGE-1144469. Author Contributions: L.C. and J.L. are cofirst authors. The authors declare the following competing financial interest(s): S.M. is an employee of the Dow Chemical Company. T.F.M. and F.R.M. are co-founders of the company Entos, Inc.

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