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Adaptive Accelerated ReaxFF Reactive Dynamics with Validation from Simulating Hydrogen Combustion

Cheng, Tao and Jaramillo-Botero, Andres and Goddard, William A., III and Sun, Huai (2014) Adaptive Accelerated ReaxFF Reactive Dynamics with Validation from Simulating Hydrogen Combustion. Journal of the American Chemical Society, 136 (26). pp. 9434-9442. ISSN 0002-7863. https://resolver.caltech.edu/CaltechAUTHORS:20140808-092947724

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Abstract

We develop here the methodology for dramatically accelerating the ReaxFF reactive force field based reactive molecular dynamics (RMD) simulations through use of the bond boost concept (BB), which we validate here for describing hydrogen combustion. The bond order, undercoordination, and overcoordination concepts of ReaxFF ensure that the BB correctly adapts to the instantaneous configurations in the reactive system to automatically identify the reactions appropriate to receive the bond boost. We refer to this as adaptive Accelerated ReaxFF Reactive Dynamics or aARRDyn. To validate the aARRDyn methodology, we determined the detailed sequence of reactions for hydrogen combustion with and without the BB. We validate that the kinetics and reaction mechanisms (that is the detailed sequences of reactive intermediates and their subsequent transformation to others) for H_2 oxidation obtained from aARRDyn agrees well with the brute force reactive molecular dynamics (BF-RMD) at 2498 K. Using aARRDyn, we then extend our simulations to the whole range of combustion temperatures from ignition (798 K) to flame temperature (2998K), and demonstrate that, over this full temperature range, the reaction rates predicted by aARRDyn agree well with the BF-RMD values, extrapolated to lower temperatures. For the aARRDyn simulation at 798 K we find that the time period for half the H_2 to form H_2O product is 538 s, whereas the computational cost was just 1289 ps, a speed increase of 0.42 trillion (10^(12)) over BF-RMD. In carrying out these RMD simulations we found that the ReaxFF-COH2008 version of the ReaxFF force field was not accurate for such intermediates as H_3O. Consequently we reoptimized the fit to a quantum mechanics (QM) level, leading to the ReaxFF–OH2014 force field that was used in the simulations.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/ja5037258DOIArticle
http://pubs.acs.org/doi/abs/10.1021/ja5037258PublisherArticle
http://pubs.acs.org/doi/suppl/10.1021/ja5037258PublisherSupporting Information
http://pubs.acs.org/doi/abs/10.1021/ja507045zErrataAddition / Correction
ORCID:
AuthorORCID
Cheng, Tao0000-0003-4830-177X
Jaramillo-Botero, Andres0000-0003-2844-0756
Goddard, William A., III0000-0003-0097-5716
Additional Information:© 2014 American Chemical Society. Received: April 14, 2014; Published: June 2, 2014. We thank Hai Xiao, Dr. Qi An and Wei-Guang Liu for insightful discussions. This work was funded by the Office of Naval Research (ONR N0014-12-1-0538), the US Department of Transportation, Federal Highway Administration (FHWA), (Award Number BAA No. DTFH61-09-R-00017), the Defense Advanced Research Projects Agency (DARPA N660011214037 and DARPA HR0011-14-2-0003), NSF CHE-1214158, and the National Science Foundation of China (Nos. 21073119 and 21173146), and the National Science Council of Taiwan, R.O.C (NSC 103-3113-P-008-001).
Funders:
Funding AgencyGrant Number
Office of Naval Research (ONR)N0014-12-1-0538
Federal Highway Administration (FHWA)BAA No. DTFH61-09-R-00017
Defense Advanced Research Projects Agency (DARPA)N660011214037
Defense Advanced Research Projects Agency (DARPA)HR0011-14-2-0003
NSFCHE-1214158
National Science Foundation of China21073119
National Science Foundation of China21173146
National Science Council (Taipei)NSC 103-3113-P-008-001
Issue or Number:26
Record Number:CaltechAUTHORS:20140808-092947724
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20140808-092947724
Official Citation:Adaptive Accelerated ReaxFF Reactive Dynamics with Validation from Simulating Hydrogen Combustion Tao Cheng, Andrés Jaramillo-Botero, William A Goddard, III, and Huai Sun Journal of the American Chemical Society 2014 136 (26), 9434-9442
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:48226
Collection:CaltechAUTHORS
Deposited By: Jason Perez
Deposited On:08 Aug 2014 22:42
Last Modified:03 Oct 2019 07:01

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