Quasiclassical trajectory analysis of the N2 + N2 reaction using a new ab initio potential energy surface

Jason D. Bender, Ioannis Nompelis, Paolo Valentini, Thomas E Schwartzentruber, Graham V Candler, Sriram Doraiswamy, Yuliya Paukku, Ke R. Yang, Zoltan Varga, Donald G Truhlar

Research output: Chapter in Book/Report/Conference proceedingConference contribution

11 Citations (Scopus)

Abstract

The N2 + N2 → N2 +N +N dissociation reaction plays an important role in hypersonic flows in the atmosphere. We are studying this reaction using the quasiclassical trajectory method (QCT). We computed trajectories over a range of translational and rovibrational temperatures. The simulations use a new, recently published potential energy surface for the N4 system. The surface was constructed from ab initio electronic structure calculations using complete-active-space second-order perturbation theory (CASPT2) and was fit by analytic functions using permutationally-invariant polynomials. For the QCT calculations, the initial rotational and vibrational states of the N2 reactants are obtained by sampling from a two-temperature ensemble of all quantized bound and quasibound states. All initial parameters are sampled randomly from appropriate distributions, and trajectories are propagated to compute thermal and ensemble-averaged cross sections and reaction rates. After reviewing the methodology, we discuss preliminary results from our calculations, including considerations of statistical convergence and uncertainty. Our reaction rates show reasonable agreement with past research, and they show strong dependence of the reaction rate on the rovibrational temperature. We plan to use ongoing QCT analyses to better inform macroscopic models for computational fluid dynamics simulations of hypersonic reacting flows.

Original languageEnglish (US)
Title of host publicationAIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference
PublisherAmerican Institute of Aeronautics and Astronautics Inc.
ISBN (Print)9781624102813
StatePublished - Jan 1 2014
EventAIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference 2014 - Atlanta, GA, United States
Duration: Jun 16 2014Jun 20 2014

Publication series

NameAIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference

Other

OtherAIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference 2014
CountryUnited States
CityAtlanta, GA
Period6/16/146/20/14

Fingerprint

Potential energy surfaces
Trajectories
Reaction rates
Hypersonic flow
Temperature
Electronic structure
Computational fluid dynamics
Polynomials
Sampling
Computer simulation

Cite this

Bender, J. D., Nompelis, I., Valentini, P., Schwartzentruber, T. E., Candler, G. V., Doraiswamy, S., ... Truhlar, D. G. (2014). Quasiclassical trajectory analysis of the N2 + N2 reaction using a new ab initio potential energy surface. In AIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference (AIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference). American Institute of Aeronautics and Astronautics Inc..

Quasiclassical trajectory analysis of the N2 + N2 reaction using a new ab initio potential energy surface. / Bender, Jason D.; Nompelis, Ioannis; Valentini, Paolo; Schwartzentruber, Thomas E; Candler, Graham V; Doraiswamy, Sriram; Paukku, Yuliya; Yang, Ke R.; Varga, Zoltan; Truhlar, Donald G.

AIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference. American Institute of Aeronautics and Astronautics Inc., 2014. (AIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference).

Research output: Chapter in Book/Report/Conference proceedingConference contribution

Bender, JD, Nompelis, I, Valentini, P, Schwartzentruber, TE, Candler, GV, Doraiswamy, S, Paukku, Y, Yang, KR, Varga, Z & Truhlar, DG 2014, Quasiclassical trajectory analysis of the N2 + N2 reaction using a new ab initio potential energy surface. in AIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference. AIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference, American Institute of Aeronautics and Astronautics Inc., AIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference 2014, Atlanta, GA, United States, 6/16/14.
Bender JD, Nompelis I, Valentini P, Schwartzentruber TE, Candler GV, Doraiswamy S et al. Quasiclassical trajectory analysis of the N2 + N2 reaction using a new ab initio potential energy surface. In AIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference. American Institute of Aeronautics and Astronautics Inc. 2014. (AIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference).
Bender, Jason D. ; Nompelis, Ioannis ; Valentini, Paolo ; Schwartzentruber, Thomas E ; Candler, Graham V ; Doraiswamy, Sriram ; Paukku, Yuliya ; Yang, Ke R. ; Varga, Zoltan ; Truhlar, Donald G. / Quasiclassical trajectory analysis of the N2 + N2 reaction using a new ab initio potential energy surface. AIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference. American Institute of Aeronautics and Astronautics Inc., 2014. (AIAA AVIATION 2014 -11th AIAA/ASME Joint Thermophysics and Heat Transfer Conference).
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