Modeling lightning-NO<sub><i>x</i></sub> chemistry on a sub-grid scale in a global chemical transport model

For the first time, a plume-in-grid approach is implemented in a chemical transport model (CTM) to parameterize the effects of the nonlinear reactions occurring within high concentrated NO<sub><i>x</i></sub> plumes from lightning NO<sub><i>x</i></sub>...

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Main Authors: A. Gressent, B. Sauvage, D. Cariolle, M. Evans, M. Leriche, C. Mari, V. Thouret
Format: Article
Language:English
Published: Copernicus Publications 2016-05-01
Series:Atmospheric Chemistry and Physics
Online Access:https://www.atmos-chem-phys.net/16/5867/2016/acp-16-5867-2016.pdf
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author A. Gressent
B. Sauvage
D. Cariolle
D. Cariolle
M. Evans
M. Leriche
C. Mari
V. Thouret
author_facet A. Gressent
B. Sauvage
D. Cariolle
D. Cariolle
M. Evans
M. Leriche
C. Mari
V. Thouret
author_sort A. Gressent
collection DOAJ
description For the first time, a plume-in-grid approach is implemented in a chemical transport model (CTM) to parameterize the effects of the nonlinear reactions occurring within high concentrated NO<sub><i>x</i></sub> plumes from lightning NO<sub><i>x</i></sub> emissions (LNO<sub><i>x</i></sub>) in the upper troposphere. It is characterized by a set of parameters including the plume lifetime, the effective reaction rate constant related to NO<sub><i>x</i></sub>–O<sub>3</sub> chemical interactions, and the fractions of NO<sub><i>x</i></sub> conversion into HNO<sub>3</sub> within the plume. Parameter estimates were made using the Dynamical Simple Model of Atmospheric Chemical Complexity (DSMACC) box model, simple plume dispersion simulations, and the 3-D Meso-NH (non-hydrostatic mesoscale atmospheric model). In order to assess the impact of the LNO<sub><i>x</i></sub> plume approach on the NO<sub><i>x</i></sub> and O<sub>3</sub> distributions on a large scale, simulations for the year 2006 were performed using the GEOS-Chem global model with a horizontal resolution of 2° × 2.5°. The implementation of the LNO<sub><i>x</i></sub> parameterization implies an NO<sub><i>x</i></sub> and O<sub>3</sub> decrease on a large scale over the region characterized by a strong lightning activity (up to 25 and 8 %, respectively, over central Africa in July) and a relative increase downwind of LNO<sub><i>x</i></sub> emissions (up to 18 and 2 % for NO<sub><i>x</i></sub> and O<sub>3</sub>, respectively, in July). The calculated variability in NO<sub><i>x</i></sub> and O<sub>3</sub> mixing ratios around the mean value according to the known uncertainties in the parameter estimates is at a maximum over continental tropical regions with ΔNO<sub><i>x</i></sub> [−33.1, +29.7] ppt and ΔO<sub>3</sub> [−1.56, +2.16] ppb, in January, and ΔNO<sub><i>x</i></sub> [−14.3, +21] ppt and ΔO<sub>3</sub> [−1.18, +1.93] ppb, in July, mainly depending on the determination of the diffusion properties of the atmosphere and the initial NO mixing ratio injected by lightning. This approach allows us (i) to reproduce a more realistic lightning NO<sub><i>x</i></sub> chemistry leading to better NO<sub><i>x</i></sub> and O<sub>3</sub> distributions on the large scale and (ii) to focus on other improvements to reduce remaining uncertainties from processes related to NO<sub><i>x</i></sub> chemistry in CTM.
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spelling doaj.art-1ead1c0dfd0d4c6a9a73962ce71fe1ae2022-12-22T02:25:46ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242016-05-01165867588910.5194/acp-16-5867-2016Modeling lightning-NO<sub><i>x</i></sub> chemistry on a sub-grid scale in a global chemical transport modelA. Gressent0B. Sauvage1D. Cariolle2D. Cariolle3M. Evans4M. Leriche5C. Mari6V. Thouret7LA, CNRS, Université de Toulouse, Toulouse, FranceLA, CNRS, Université de Toulouse, Toulouse, FranceMétéo France, Toulouse, FranceCentre Européen de Recherche et de Formation Avancée en Calcul Scientifique, CERFACS, Toulouse, FranceThe Wolfson Atmospheric Chemistry Laboratories, University of York, York, UKLA, CNRS, Université de Toulouse, Toulouse, FranceLA, CNRS, Université de Toulouse, Toulouse, FranceLA, CNRS, Université de Toulouse, Toulouse, FranceFor the first time, a plume-in-grid approach is implemented in a chemical transport model (CTM) to parameterize the effects of the nonlinear reactions occurring within high concentrated NO<sub><i>x</i></sub> plumes from lightning NO<sub><i>x</i></sub> emissions (LNO<sub><i>x</i></sub>) in the upper troposphere. It is characterized by a set of parameters including the plume lifetime, the effective reaction rate constant related to NO<sub><i>x</i></sub>–O<sub>3</sub> chemical interactions, and the fractions of NO<sub><i>x</i></sub> conversion into HNO<sub>3</sub> within the plume. Parameter estimates were made using the Dynamical Simple Model of Atmospheric Chemical Complexity (DSMACC) box model, simple plume dispersion simulations, and the 3-D Meso-NH (non-hydrostatic mesoscale atmospheric model). In order to assess the impact of the LNO<sub><i>x</i></sub> plume approach on the NO<sub><i>x</i></sub> and O<sub>3</sub> distributions on a large scale, simulations for the year 2006 were performed using the GEOS-Chem global model with a horizontal resolution of 2° × 2.5°. The implementation of the LNO<sub><i>x</i></sub> parameterization implies an NO<sub><i>x</i></sub> and O<sub>3</sub> decrease on a large scale over the region characterized by a strong lightning activity (up to 25 and 8 %, respectively, over central Africa in July) and a relative increase downwind of LNO<sub><i>x</i></sub> emissions (up to 18 and 2 % for NO<sub><i>x</i></sub> and O<sub>3</sub>, respectively, in July). The calculated variability in NO<sub><i>x</i></sub> and O<sub>3</sub> mixing ratios around the mean value according to the known uncertainties in the parameter estimates is at a maximum over continental tropical regions with ΔNO<sub><i>x</i></sub> [−33.1, +29.7] ppt and ΔO<sub>3</sub> [−1.56, +2.16] ppb, in January, and ΔNO<sub><i>x</i></sub> [−14.3, +21] ppt and ΔO<sub>3</sub> [−1.18, +1.93] ppb, in July, mainly depending on the determination of the diffusion properties of the atmosphere and the initial NO mixing ratio injected by lightning. This approach allows us (i) to reproduce a more realistic lightning NO<sub><i>x</i></sub> chemistry leading to better NO<sub><i>x</i></sub> and O<sub>3</sub> distributions on the large scale and (ii) to focus on other improvements to reduce remaining uncertainties from processes related to NO<sub><i>x</i></sub> chemistry in CTM.https://www.atmos-chem-phys.net/16/5867/2016/acp-16-5867-2016.pdf
spellingShingle A. Gressent
B. Sauvage
D. Cariolle
D. Cariolle
M. Evans
M. Leriche
C. Mari
V. Thouret
Modeling lightning-NO<sub><i>x</i></sub> chemistry on a sub-grid scale in a global chemical transport model
Atmospheric Chemistry and Physics
title Modeling lightning-NO<sub><i>x</i></sub> chemistry on a sub-grid scale in a global chemical transport model
title_full Modeling lightning-NO<sub><i>x</i></sub> chemistry on a sub-grid scale in a global chemical transport model
title_fullStr Modeling lightning-NO<sub><i>x</i></sub> chemistry on a sub-grid scale in a global chemical transport model
title_full_unstemmed Modeling lightning-NO<sub><i>x</i></sub> chemistry on a sub-grid scale in a global chemical transport model
title_short Modeling lightning-NO<sub><i>x</i></sub> chemistry on a sub-grid scale in a global chemical transport model
title_sort modeling lightning no sub i x i sub chemistry on a sub grid scale in a global chemical transport model
url https://www.atmos-chem-phys.net/16/5867/2016/acp-16-5867-2016.pdf
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