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

Chen, Leanne D. and Lawniczak, James J. and Ding, Feizhi and Bygrave, Peter J. and Riahi, Saleh and Manby, Frederick R. and Mukhopadhyay, Sukrit and Miller, Thomas F., III (2020) Embedded Mean-Field Theory for Solution-Phase Transition-Metal Polyolefin Catalysis. Journal of Chemical Theory and Computation, 16 (7). pp. 4226-4237. ISSN 1549-9618. https://resolver.caltech.edu/CaltechAUTHORS:20200526-141455955

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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.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acs.jctc.0c00169DOIArticle
ORCID:
AuthorORCID
Chen, Leanne D.0000-0001-9700-972X
Manby, Frederick R.0000-0001-7611-714X
Miller, Thomas F., III0000-0002-1882-5380
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.
Funders:
Funding AgencyGrant Number
Dow Chemical CompanyUNSPECIFIED
NSF Graduate Research FellowshipDGE-1144469
Issue or Number:7
Record Number:CaltechAUTHORS:20200526-141455955
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200526-141455955
Official Citation:Embedded Mean-Field Theory for Solution-Phase Transition-Metal Polyolefin Catalysis. Leanne D. Chen, James J. Lawniczak, Feizhi Ding, Peter J. Bygrave, Saleh Riahi, Frederick R. Manby, Sukrit Mukhopadhyay, and Thomas F. Miller. Journal of Chemical Theory and Computation 2020 16 (7), 4226-4237; DOI: 10.1021/acs.jctc.0c00169
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:103467
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:26 May 2020 21:21
Last Modified:15 Jul 2020 14:58

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