Data-Inspired and Physics-Driven Model Reduction for Dissociation: Application to the O$_{\textrm{2}}$+O System. Venturi, S., Sharma, M. P., Lopez, B., & Panesi, M. Journal of Physical Chemistry A, 124(41):8359–8372, October, 2020. Publisher: American Chemical Society![Data-Inspired and Physics-Driven Model Reduction for Dissociation: Application to the O$_{\textrm{2}}$+O System [link]](https://bibbase.org/img/filetypes/link.svg "link")
Paper doi abstract bibtex 1 download This work presents an in-depth discussion on the nonequilibrium dissociation of O2 molecules colliding with O atoms, combining quasi-classical trajectory calculations, master equation, and dimensionality reduction. A rovibrationally resolved database for all of the elementary collisional processes is constructed by including all nine adiabatic electronic states of O3 in the QCT calculations. A detailed analysis of the ab initio data set reveals that for a rovibrational level, the probability of dissociating is mostly dictated by its deficit in internal energy compared to the centrifugal barrier. Because of the assumption of rotational equilibrium, the conventional vibrational-specific calculations fail to characterize such a dependence. Based on this observation, a new physics-based grouping strategy for application to coarse-grained models is proposed. By relying on a hybrid technique made of rovibrationally resolved excitation coupled to coarse-grained dissociation, the new approach is compared to the vibrational-specific model and the direct solution of the rovibrational state-to-state master equation. Simulations are performed in a zero-dimensional isothermal and isochoric chemical reactor for a wide range of temperatures (1500-20,000 K). The study shows that the main contribution to the model inadequacy of vibrational-specific approaches originates from the incapability of characterizing dissociation, rather than the energy transfers. Even when constructed with only twenty groups, the new reduced-order model outperforms the vibrational-specific one in predicting all of the QoIs related to dissociation kinetics. At the highest temperature, the accuracy in the mole fraction is improved by 2000%.
@article{venturi2020a,
title = {Data-{Inspired} and {Physics}-{Driven} {Model} {Reduction} for {Dissociation}: {Application} to the {O}$_{\textrm{2}}$+{O} {System}},
volume = {124},
url = {https://pubs.acs.org/doi/full/10.1021/acs.jpca.0c04516},
doi = {10.1021/ACS.JPCA.0C04516/ASSET/IMAGES/MEDIUM/JP0C04516_M040.GIF},
abstract = {This work presents an in-depth discussion on the nonequilibrium dissociation of O2 molecules colliding with O atoms, combining quasi-classical trajectory calculations, master equation, and dimensionality reduction. A rovibrationally resolved database for all of the elementary collisional processes is constructed by including all nine adiabatic electronic states of O3 in the QCT calculations. A detailed analysis of the ab initio data set reveals that for a rovibrational level, the probability of dissociating is mostly dictated by its deficit in internal energy compared to the centrifugal barrier. Because of the assumption of rotational equilibrium, the conventional vibrational-specific calculations fail to characterize such a dependence. Based on this observation, a new physics-based grouping strategy for application to coarse-grained models is proposed. By relying on a hybrid technique made of rovibrationally resolved excitation coupled to coarse-grained dissociation, the new approach is compared to the vibrational-specific model and the direct solution of the rovibrational state-to-state master equation. Simulations are performed in a zero-dimensional isothermal and isochoric chemical reactor for a wide range of temperatures (1500-20,000 K). The study shows that the main contribution to the model inadequacy of vibrational-specific approaches originates from the incapability of characterizing dissociation, rather than the energy transfers. Even when constructed with only twenty groups, the new reduced-order model outperforms the vibrational-specific one in predicting all of the QoIs related to dissociation kinetics. At the highest temperature, the accuracy in the mole fraction is improved by 2000\%.},
number = {41},
journal = {Journal of Physical Chemistry A},
author = {Venturi, S. and Sharma, M. P. and Lopez, B. and Panesi, M.},
month = oct,
year = {2020},
note = {Publisher: American Chemical Society},
pages = {8359--8372},
}
Downloads: 1
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A detailed analysis of the ab initio data set reveals that for a rovibrational level, the probability of dissociating is mostly dictated by its deficit in internal energy compared to the centrifugal barrier. Because of the assumption of rotational equilibrium, the conventional vibrational-specific calculations fail to characterize such a dependence. Based on this observation, a new physics-based grouping strategy for application to coarse-grained models is proposed. By relying on a hybrid technique made of rovibrationally resolved excitation coupled to coarse-grained dissociation, the new approach is compared to the vibrational-specific model and the direct solution of the rovibrational state-to-state master equation. Simulations are performed in a zero-dimensional isothermal and isochoric chemical reactor for a wide range of temperatures (1500-20,000 K). 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