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Kinetics Study on the Pyrolysis and Oxidation of Energetic Materials by Multireference Second-Order Perturbation Theory and Multireference Coupled-Cluster Theory

EMSL Project ID


Ignition is undoubtedly one of the most critical events governing the satisfactory performance of many combustion devices including rocket engines that launch national security payloads by the three military services. Consequently, the associated propellant ignition chemistry and inherent thermo-physical processes need to be fundamentally understood for the development of reliable ignition devices. Furthermore, handling of these new propellant fuels is also expected to have a much smaller logistical footprint due to the fact that they are being designed to be environmentally benign. However, practical realization of these fuels in propulsion systems will only come after attaining a satisfactory understanding of how to optimize their combustion characteristics in relevant operating environments. Since ignition of the energetic fuel generates highly reactive intermediates which are often difficult to probe experimentally, an application of ab initio chemical kinetics theory is therefore essential for understanding the complex ignition chemistry. We will model these processes with the state-of-the-art methodologies implemented in NWChem package including single- and multi-reference Coupled Cluster codes.

Project Details

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Principal Investigator

Karol Kowalski
Pacific Northwest National Laboratory

Team Members

William Shelton
Louisiana State University

Jeffrey Hammond
Intel Corporation

Jiri Pittner
Academy of Sciences of the Czech Republic

Theresa Windus
Iowa State University

Related Publications

Anisimov V, GH Bauer, K Chadalavada, RM Olson, JW Glenski, WT Kramer, E Apra, and K Kowalski. 2014. "Optimization of the Coupled Cluster Implementation in NWChem on Petascale Parallel Architectures." Journal of Chemical Theory and Computation. doi:10.1021/ct500404c
Apra E, K Kowalski, JR Hammond, and M Klemm. 2014. "NWChem: Quantum Chemistry Simulations at Scale." Chapter 17 in High Performance Parallelism Pearls - Multicore and Many-core Programming Approaches, pp. 287-306. Morgan Kaufmann, Burlington, MA.
Berardo E, H Hu, HJJ van Dam, SA Shevlin, SM Woodley, K Kowalski, and MA Zwijnenburg. 2014. "Describing excited state relaxation and localization in TiO2 nanoparticles using TD-DFT." Journal of Chemical Theory and Computation. doi:10.1021/ct500787x
Bhaskaran-Nair K, K Kowalski, J Moreno, M Jarrell, and WA Shelton. 2014. "Equation of motion coupled cluster methods for electron attachment and ionization potential in fullerenes C60 and C70." Journal of Chemical Physics 141(6):074304-1 to 074304-6. doi:10.1063/1.4891934
Miliordos E, E Apra, and SS Xantheas. 2013. "Optimal geometries and harmonic vibrational frequencies of the global minima of water clusters (H2O)n, n=2-6, and several hexamer local minima at the CCSD(T) level of theory." Journal of Chemical Physics 139(11):114302-13. doi:10.1063/1.4820448