Parametric sensitivity and uncertainty analysis of dimethylsulfide oxidation in the clear-sky remote marine boundary layer
Local and global sensitivity and uncertainty methods are applied to a box model of the dimethylsulfide (DMS) oxidation cycle in the remote marine boundary layer in order to determine the key physical and chemical parameters and sources of uncertainty. The model considers 58uncertain parameters, and...
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ftdoajarticles:oai:doaj.org/article:fd90777c92a34e938af535b4bfe1ffd4 2023-05-15T18:25:56+02:00 Parametric sensitivity and uncertainty analysis of dimethylsulfide oxidation in the clear-sky remote marine boundary layer D. D. Lucas R. G. Prinn 2005-01-01T00:00:00Z https://doaj.org/article/fd90777c92a34e938af535b4bfe1ffd4 EN eng Copernicus Publications http://www.atmos-chem-phys.net/5/1505/2005/acp-5-1505-2005.pdf https://doaj.org/toc/1680-7316 https://doaj.org/toc/1680-7324 1680-7316 1680-7324 https://doaj.org/article/fd90777c92a34e938af535b4bfe1ffd4 Atmospheric Chemistry and Physics, Vol 5, Iss 6, Pp 1505-1525 (2005) Physics QC1-999 Chemistry QD1-999 article 2005 ftdoajarticles 2022-12-31T14:19:23Z Local and global sensitivity and uncertainty methods are applied to a box model of the dimethylsulfide (DMS) oxidation cycle in the remote marine boundary layer in order to determine the key physical and chemical parameters and sources of uncertainty. The model considers 58uncertain parameters, and simulates the diurnal gas-phase cycles of DMS, SO 2 , methanesulfonic acid (MSA), and H 2 SO 4 for clear-sky summertime conditions observed over the Southern Ocean. The results of this study depend on many underlying assumptions, including the DMS mechanism, simulation conditions, and probability distribution functions of the uncertain parameters. A local direct integration method is used to calculate first-order local sensitivity coefficients for infinitesimal perturbations about the parameter means. Key parameters identified by this analysis are related to DMS emissions, vertical mixing, heterogeneous removal, and the DMS+OH abstraction and addition reactions. MSA and H 2 SO 4 are also sensitive to numerous rate constants, which limits the ability of using parameterized mechanisms to predict their concentrations. Of the chemistry, H 2 SO 4 is highly sensitive to the rate constants for a set of nighttime reactions that lead to its production through a non-SO 2 path initiated by the oxidation of DMS by NO 3 . For the global analysis, the probabilistic collocation method is used to propagate the uncertain parameters through the model. The concentrations of DMS and SO 2 are uncertain (1-σ) by factors of 3.5 and 2.5, respectively, while MSA and H 2 SO 4 have uncertainty factors that range between 4.1 and 8.6. The main sources of uncertainty in the four species are from DMS emissions and heterogeneous scavenging, but the uncertain rate constants collectively account for up to 59% of the total uncertainty in MSA and 43% in H 2 SO 4 . Of the uncertain DMS chemistry, reactions that form and destroy CH 3 S(O)OO and CH 3 SO 3 are identified as important targets for reducing the uncertainties. Article in Journal/Newspaper Southern Ocean Directory of Open Access Journals: DOAJ Articles Southern Ocean |
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Open Polar |
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Directory of Open Access Journals: DOAJ Articles |
op_collection_id |
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language |
English |
topic |
Physics QC1-999 Chemistry QD1-999 |
spellingShingle |
Physics QC1-999 Chemistry QD1-999 D. D. Lucas R. G. Prinn Parametric sensitivity and uncertainty analysis of dimethylsulfide oxidation in the clear-sky remote marine boundary layer |
topic_facet |
Physics QC1-999 Chemistry QD1-999 |
description |
Local and global sensitivity and uncertainty methods are applied to a box model of the dimethylsulfide (DMS) oxidation cycle in the remote marine boundary layer in order to determine the key physical and chemical parameters and sources of uncertainty. The model considers 58uncertain parameters, and simulates the diurnal gas-phase cycles of DMS, SO 2 , methanesulfonic acid (MSA), and H 2 SO 4 for clear-sky summertime conditions observed over the Southern Ocean. The results of this study depend on many underlying assumptions, including the DMS mechanism, simulation conditions, and probability distribution functions of the uncertain parameters. A local direct integration method is used to calculate first-order local sensitivity coefficients for infinitesimal perturbations about the parameter means. Key parameters identified by this analysis are related to DMS emissions, vertical mixing, heterogeneous removal, and the DMS+OH abstraction and addition reactions. MSA and H 2 SO 4 are also sensitive to numerous rate constants, which limits the ability of using parameterized mechanisms to predict their concentrations. Of the chemistry, H 2 SO 4 is highly sensitive to the rate constants for a set of nighttime reactions that lead to its production through a non-SO 2 path initiated by the oxidation of DMS by NO 3 . For the global analysis, the probabilistic collocation method is used to propagate the uncertain parameters through the model. The concentrations of DMS and SO 2 are uncertain (1-σ) by factors of 3.5 and 2.5, respectively, while MSA and H 2 SO 4 have uncertainty factors that range between 4.1 and 8.6. The main sources of uncertainty in the four species are from DMS emissions and heterogeneous scavenging, but the uncertain rate constants collectively account for up to 59% of the total uncertainty in MSA and 43% in H 2 SO 4 . Of the uncertain DMS chemistry, reactions that form and destroy CH 3 S(O)OO and CH 3 SO 3 are identified as important targets for reducing the uncertainties. |
format |
Article in Journal/Newspaper |
author |
D. D. Lucas R. G. Prinn |
author_facet |
D. D. Lucas R. G. Prinn |
author_sort |
D. D. Lucas |
title |
Parametric sensitivity and uncertainty analysis of dimethylsulfide oxidation in the clear-sky remote marine boundary layer |
title_short |
Parametric sensitivity and uncertainty analysis of dimethylsulfide oxidation in the clear-sky remote marine boundary layer |
title_full |
Parametric sensitivity and uncertainty analysis of dimethylsulfide oxidation in the clear-sky remote marine boundary layer |
title_fullStr |
Parametric sensitivity and uncertainty analysis of dimethylsulfide oxidation in the clear-sky remote marine boundary layer |
title_full_unstemmed |
Parametric sensitivity and uncertainty analysis of dimethylsulfide oxidation in the clear-sky remote marine boundary layer |
title_sort |
parametric sensitivity and uncertainty analysis of dimethylsulfide oxidation in the clear-sky remote marine boundary layer |
publisher |
Copernicus Publications |
publishDate |
2005 |
url |
https://doaj.org/article/fd90777c92a34e938af535b4bfe1ffd4 |
geographic |
Southern Ocean |
geographic_facet |
Southern Ocean |
genre |
Southern Ocean |
genre_facet |
Southern Ocean |
op_source |
Atmospheric Chemistry and Physics, Vol 5, Iss 6, Pp 1505-1525 (2005) |
op_relation |
http://www.atmos-chem-phys.net/5/1505/2005/acp-5-1505-2005.pdf https://doaj.org/toc/1680-7316 https://doaj.org/toc/1680-7324 1680-7316 1680-7324 https://doaj.org/article/fd90777c92a34e938af535b4bfe1ffd4 |
_version_ |
1766207670182739968 |