Molecular physics and kinetics of high-temperature planetary atmospheres

Capitelli, M.; Bruno, D.; Colonna, G.; D’Ammando, G.; Esposito, Fabrizio; Laricchiuta, Annarita; Pietanza, Lucia Daniela

doi:10.1007/s12210-011-0132-6

Cited by 6 publications

(3 citation statements)

References 44 publications

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“…The formation of highly vibrationally excited molecules under conditions of high temperature and pressure, typical of plasmas or hypersonic flows, is mainly due to energy exchange during collisions. The most investigated typical exchange is the one occurring between the vibrational degrees of freedom of identical molecules (VV exchange), e.g., N 2 *( v = 1) + N 2 ( v = 0) → N 2 ( v = 0) + N 2 *( v = 1) or CO 2 (0 0 1) + CO 2 (0 0 0) → CO 2 (0 0 0) + CO 2 (0 0 1).…”

Section: Introductionmentioning

confidence: 99%

Modeling of Energy Transfer From Vibrationally Excited CO₂ Molecules: Cross Sections and Probabilities for Kinetic Modeling of Atmospheres, Flows, and Plasmas

et al. 2013

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We present extended applications of an established theoretical and computational machinery suitable for the study of the dynamics of CO2+CO2 collisions, focusing on vibrational energy exchange, considered over a wide range of energies and rotational temperatures. Calculations are based on quasi-classical trajectories on a potential energy function (a critical component of dynamics simulations), tailored to accurately describe the intermolecular interactions, modeled by the recently proposed bond-bond semiempirical formulation that allows the colliding molecules to be stretchable, rather than frozen at their equilibrium geometry. In a previous work, the same potential energy surface has been used to show that modifications in the geometry (and in physical properties such as polarizability and charge distribution) of the colliding partners affect the intermolecular interaction and determine the features of the energy exchange, to a large extent driven by long-range forces. As initial partitioning of the energy among the molecular degrees of freedom, we consider the excitation of the vibrational bending mode, assuming an initial rotational distribution and a rotational temperature. The role of the vibrational angular momentum is also carefully assessed. Results are obtained by portable implementations of this approach in a Grid-computing framework and on high performance platforms. Cross sections are basic ingredients to obtain rate constants of use in advanced state-to-state kinetic models, under equilibrium or nonequilibrium conditions, and this approach is suitable for gas dynamics applications to plasmas and modeling of hypersonic flows.

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Section: Introductionmentioning

confidence: 99%

Modeling of Energy Transfer From Vibrationally Excited CO₂ Molecules: Cross Sections and Probabilities for Kinetic Modeling of Atmospheres, Flows, and Plasmas

et al. 2013

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“…[1,2] The energy transfer occurring in CO 2 1 N 2 collisions, especially those involving vibrational excitation of the colliding partners, affects the energy balance and influences the complicated network of processes that determine the chemistry of the atmospheres. In general, for the study of any gaseous mixture, an accurate quantification of the efficiency of the energy transfer processes is required to build up reliable kinetic models, and a detailed characterization of the exchanges of energy is fundamental for modeling elementary processes involved in combustion chemistry, chemistry of plasmas, gases under flow conditions (e.g., in aircraft and spacecraft design [3][4][5] ). More recent technological applications focus on carbon capture, where a necessary step is the separation of CO 2 from abundant N 2 .…”

Section: Introductionmentioning

confidence: 99%

Energy transfer dynamics and kinetics of elementary processes (promoted) by gas‐phase CO₂‐N₂ collisions: Selectivity control by the anisotropy of the interaction

et al. 2016

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In this work, we exploit a new formulation of the potential energy and of the related computational procedures, which embodies the coupling between the intra and intermolecular components, to characterize possible propensities of the collision dynamics in energy transfer processes of interest for simulation and control of phenomena occurring in a variety of equilibrium and nonequilibrium environments. The investigation reported in the paper focuses on the prototype CO2 -N2 system, whose intramolecular component of the interaction is modeled in terms of a many body expansion while the intermolecular component is modeled in terms of a recently developed bonds-as-interacting-molecular-centers' approach. The main advantage of this formulation of the potential energy surface is that of being (a) truly full dimensional (i.e., all the variations of the coordinates associated with the molecular vibrations and rotations on the geometrical and electronic structure of the monomers, are explicitly taken into account without freezing any bonds or angles), (b) more flexible than other usual formulations of the interaction and (c) well suited for fitting procedures better adhering to accurate ab initio data and sensitive to experimental arrangement dependent information. Specific attention has been given to the fact that a variation of vibrational and rotational energy has a higher (both qualitative and quantitative) impact on the energy transfer when a more accurate formulation of the intermolecular interaction (with respect to that obtained when using rigid monomers) is adopted. This makes the potential energy surface better suited for the kinetic modeling of gaseous mixtures in plasma, combustion and atmospheric chemistry computational applications. © 2016 Wiley Periodicals, Inc.

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“…[3][4][5] The simulation of the early universe is another possible area, since all the elementary processes involving primordial molecules have to be taken into account (see, e.g., Ref. 6).…”

Section: Introductionmentioning

confidence: 99%

Energy transfer upon collision of selectively excited CO2 molecules: State-to-state cross sections and probabilities for modeling of atmospheres and gaseous flows

Lombardi

Faginas-Lago

Pacifici

et al. 2015

The Journal of Chemical Physics

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Carbon dioxide molecules can store and release tens of kcal/mol upon collisions, and such an energy transfer strongly influences the energy disposal and the chemical processes in gases under the extreme conditions typical of plasmas and hypersonic flows. Moreover, the energy transfer involving CO2 characterizes the global dynamics of the Earth-atmosphere system and the energy balance of other planetary atmospheres. Contemporary developments in kinetic modeling of gaseous mixtures are connected to progress in the description of the energy transfer, and, in particular, the attempts to include non-equilibrium effects require to consider state-specific energy exchanges. A systematic study of the state-to-state vibrational energy transfer in CO2 + CO2 collisions is the focus of the present work, aided by a theoretical and computational tool based on quasiclassical trajectory simulations and an accurate full-dimension model of the intermolecular interactions. In this model, the accuracy of the description of the intermolecular forces (that determine the probability of energy transfer in molecular collisions) is enhanced by explicit account of the specific effects of the distortion of the CO2 structure due to vibrations. Results show that these effects are important for the energy transfer probabilities. Moreover, the role of rotational and vibrational degrees of freedom is found to be dominant in the energy exchange, while the average contribution of translations, under the temperature and energy conditions considered, is negligible. Remarkable is the fact that the intramolecular energy transfer only involves stretching and bending, unless one of the colliding molecules has an initial symmetric stretching quantum number greater than a threshold value estimated to be equal to 7.

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Molecular physics and kinetics of high-temperature planetary atmospheres

Cited by 6 publications

References 44 publications

Modeling of Energy Transfer From Vibrationally Excited CO₂ Molecules: Cross Sections and Probabilities for Kinetic Modeling of Atmospheres, Flows, and Plasmas

Modeling of Energy Transfer From Vibrationally Excited CO₂ Molecules: Cross Sections and Probabilities for Kinetic Modeling of Atmospheres, Flows, and Plasmas

Energy transfer dynamics and kinetics of elementary processes (promoted) by gas‐phase CO₂‐N₂ collisions: Selectivity control by the anisotropy of the interaction

Energy transfer upon collision of selectively excited CO2 molecules: State-to-state cross sections and probabilities for modeling of atmospheres and gaseous flows

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Molecular physics and kinetics of high-temperature planetary atmospheres

Cited by 6 publications

References 44 publications

Modeling of Energy Transfer From Vibrationally Excited CO2 Molecules: Cross Sections and Probabilities for Kinetic Modeling of Atmospheres, Flows, and Plasmas

Modeling of Energy Transfer From Vibrationally Excited CO2 Molecules: Cross Sections and Probabilities for Kinetic Modeling of Atmospheres, Flows, and Plasmas

Energy transfer dynamics and kinetics of elementary processes (promoted) by gas‐phase CO2‐N2 collisions: Selectivity control by the anisotropy of the interaction

Energy transfer upon collision of selectively excited CO2 molecules: State-to-state cross sections and probabilities for modeling of atmospheres and gaseous flows

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Modeling of Energy Transfer From Vibrationally Excited CO₂ Molecules: Cross Sections and Probabilities for Kinetic Modeling of Atmospheres, Flows, and Plasmas

Modeling of Energy Transfer From Vibrationally Excited CO₂ Molecules: Cross Sections and Probabilities for Kinetic Modeling of Atmospheres, Flows, and Plasmas

Energy transfer dynamics and kinetics of elementary processes (promoted) by gas‐phase CO₂‐N₂ collisions: Selectivity control by the anisotropy of the interaction