Case study of the diurnal variability of chemically active species with respect to boundary layer dynamics during DOMINO

B.J.H. van Stratum, J. Vilà-Guerau de Arellano, H.G. Ouwersloot, K. van den Dries, T.W. van Laar, M. Martinez, J. Lelieveld, J.M. Diesch, F. Drewnick, H. Fischer, Z. Hosaynali Beygi, H. Harder, E. Regelin, V. Sinha, J.A. Adame, M. Sörgel, R. Sander, H. Bozem, W. Song, J. Williams & 1 others N. Yassaa

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Abstract

We study the interactions between atmospheric boundary layer (ABL) dynamics and atmospheric chemistry using a mixed-layer model coupled to chemical reaction schemes. Guided by both atmospheric and chemical measurements obtained during the DOMINO (Diel Oxidant Mechanisms in relation to Nitrogen Oxides) campaign (2008), numerical experiments are performed to study the role of ABL dynamics and the accuracy of chemical schemes with different complexity: the Model for Ozone and Related chemical Tracers, version 4 (MOZART-4) and a reduced mechanism of this chemical system. Both schemes produce satisfactory results, indicating that the reduced scheme is capable of reproducing the O3-NOx-VOC-HOx diurnal cycle during conditions characterized by a low NOx regime and small O3 tendencies (less than 1 ppb per hour). By focusing on the budget equations of chemical species in the mixedlayer model, we show that for species like O3, NO and NO2, the influence of entrainment and boundary layer growth is of the same order as chemical production/loss. This indicates that an accurate representation of ABL processes is crucial in understanding the diel cycle of chemical species. By comparing the time scales of chemical reactive species with the mixing time scale of turbulence, we propose a classification based on the Damk¨ohler number to further determine the importance of dynamics on chemistry during field campaigns. Our findings advocate an integrated approach, simultaneously solving the ABL dynamics and chemical reactions, in order to obtain a better understanding of chemical pathways and processes and the interpretation of the results obtained during measurement campaigns.
LanguageEnglish
Pages5329-5341
JournalAtmospheric Chemistry and Physics
Volume12
DOIs
Publication statusPublished - 2012

Fingerprint

nitrogen oxides
oxidant
boundary layer
chemical reaction
timescale
chemical
atmospheric chemistry
integrated approach
entrainment
mixed layer
volatile organic compound
turbulence
tracer
ozone

Keywords

  • volatile organic-compounds
  • tropical forest
  • oh reactivity
  • isoprene
  • chemistry
  • campaign
  • air
  • segregation
  • turbulence
  • gabriel

Cite this

van Stratum, B.J.H. ; Vilà-Guerau de Arellano, J. ; Ouwersloot, H.G. ; van den Dries, K. ; van Laar, T.W. ; Martinez, M. ; Lelieveld, J. ; Diesch, J.M. ; Drewnick, F. ; Fischer, H. ; Hosaynali Beygi, Z. ; Harder, H. ; Regelin, E. ; Sinha, V. ; Adame, J.A. ; Sörgel, M. ; Sander, R. ; Bozem, H. ; Song, W. ; Williams, J. ; Yassaa, N. / Case study of the diurnal variability of chemically active species with respect to boundary layer dynamics during DOMINO. In: Atmospheric Chemistry and Physics. 2012 ; Vol. 12. pp. 5329-5341.
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title = "Case study of the diurnal variability of chemically active species with respect to boundary layer dynamics during DOMINO",
abstract = "We study the interactions between atmospheric boundary layer (ABL) dynamics and atmospheric chemistry using a mixed-layer model coupled to chemical reaction schemes. Guided by both atmospheric and chemical measurements obtained during the DOMINO (Diel Oxidant Mechanisms in relation to Nitrogen Oxides) campaign (2008), numerical experiments are performed to study the role of ABL dynamics and the accuracy of chemical schemes with different complexity: the Model for Ozone and Related chemical Tracers, version 4 (MOZART-4) and a reduced mechanism of this chemical system. Both schemes produce satisfactory results, indicating that the reduced scheme is capable of reproducing the O3-NOx-VOC-HOx diurnal cycle during conditions characterized by a low NOx regime and small O3 tendencies (less than 1 ppb per hour). By focusing on the budget equations of chemical species in the mixedlayer model, we show that for species like O3, NO and NO2, the influence of entrainment and boundary layer growth is of the same order as chemical production/loss. This indicates that an accurate representation of ABL processes is crucial in understanding the diel cycle of chemical species. By comparing the time scales of chemical reactive species with the mixing time scale of turbulence, we propose a classification based on the Damk¨ohler number to further determine the importance of dynamics on chemistry during field campaigns. Our findings advocate an integrated approach, simultaneously solving the ABL dynamics and chemical reactions, in order to obtain a better understanding of chemical pathways and processes and the interpretation of the results obtained during measurement campaigns.",
keywords = "volatile organic-compounds, tropical forest, oh reactivity, isoprene, chemistry, campaign, air, segregation, turbulence, gabriel",
author = "{van Stratum}, B.J.H. and {Vil{\`a}-Guerau de Arellano}, J. and H.G. Ouwersloot and {van den Dries}, K. and {van Laar}, T.W. and M. Martinez and J. Lelieveld and J.M. Diesch and F. Drewnick and H. Fischer and {Hosaynali Beygi}, Z. and H. Harder and E. Regelin and V. Sinha and J.A. Adame and M. S{\"o}rgel and R. Sander and H. Bozem and W. Song and J. Williams and N. Yassaa",
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doi = "10.5194/acp-12-5329-2012",
language = "English",
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van Stratum, BJH, Vilà-Guerau de Arellano, J, Ouwersloot, HG, van den Dries, K, van Laar, TW, Martinez, M, Lelieveld, J, Diesch, JM, Drewnick, F, Fischer, H, Hosaynali Beygi, Z, Harder, H, Regelin, E, Sinha, V, Adame, JA, Sörgel, M, Sander, R, Bozem, H, Song, W, Williams, J & Yassaa, N 2012, 'Case study of the diurnal variability of chemically active species with respect to boundary layer dynamics during DOMINO', Atmospheric Chemistry and Physics, vol. 12, pp. 5329-5341. https://doi.org/10.5194/acp-12-5329-2012

Case study of the diurnal variability of chemically active species with respect to boundary layer dynamics during DOMINO. / van Stratum, B.J.H.; Vilà-Guerau de Arellano, J.; Ouwersloot, H.G.; van den Dries, K.; van Laar, T.W.; Martinez, M.; Lelieveld, J.; Diesch, J.M.; Drewnick, F.; Fischer, H.; Hosaynali Beygi, Z.; Harder, H.; Regelin, E.; Sinha, V.; Adame, J.A.; Sörgel, M.; Sander, R.; Bozem, H.; Song, W.; Williams, J.; Yassaa, N.

In: Atmospheric Chemistry and Physics, Vol. 12, 2012, p. 5329-5341.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Case study of the diurnal variability of chemically active species with respect to boundary layer dynamics during DOMINO

AU - van Stratum, B.J.H.

AU - Vilà-Guerau de Arellano, J.

AU - Ouwersloot, H.G.

AU - van den Dries, K.

AU - van Laar, T.W.

AU - Martinez, M.

AU - Lelieveld, J.

AU - Diesch, J.M.

AU - Drewnick, F.

AU - Fischer, H.

AU - Hosaynali Beygi, Z.

AU - Harder, H.

AU - Regelin, E.

AU - Sinha, V.

AU - Adame, J.A.

AU - Sörgel, M.

AU - Sander, R.

AU - Bozem, H.

AU - Song, W.

AU - Williams, J.

AU - Yassaa, N.

PY - 2012

Y1 - 2012

N2 - We study the interactions between atmospheric boundary layer (ABL) dynamics and atmospheric chemistry using a mixed-layer model coupled to chemical reaction schemes. Guided by both atmospheric and chemical measurements obtained during the DOMINO (Diel Oxidant Mechanisms in relation to Nitrogen Oxides) campaign (2008), numerical experiments are performed to study the role of ABL dynamics and the accuracy of chemical schemes with different complexity: the Model for Ozone and Related chemical Tracers, version 4 (MOZART-4) and a reduced mechanism of this chemical system. Both schemes produce satisfactory results, indicating that the reduced scheme is capable of reproducing the O3-NOx-VOC-HOx diurnal cycle during conditions characterized by a low NOx regime and small O3 tendencies (less than 1 ppb per hour). By focusing on the budget equations of chemical species in the mixedlayer model, we show that for species like O3, NO and NO2, the influence of entrainment and boundary layer growth is of the same order as chemical production/loss. This indicates that an accurate representation of ABL processes is crucial in understanding the diel cycle of chemical species. By comparing the time scales of chemical reactive species with the mixing time scale of turbulence, we propose a classification based on the Damk¨ohler number to further determine the importance of dynamics on chemistry during field campaigns. Our findings advocate an integrated approach, simultaneously solving the ABL dynamics and chemical reactions, in order to obtain a better understanding of chemical pathways and processes and the interpretation of the results obtained during measurement campaigns.

AB - We study the interactions between atmospheric boundary layer (ABL) dynamics and atmospheric chemistry using a mixed-layer model coupled to chemical reaction schemes. Guided by both atmospheric and chemical measurements obtained during the DOMINO (Diel Oxidant Mechanisms in relation to Nitrogen Oxides) campaign (2008), numerical experiments are performed to study the role of ABL dynamics and the accuracy of chemical schemes with different complexity: the Model for Ozone and Related chemical Tracers, version 4 (MOZART-4) and a reduced mechanism of this chemical system. Both schemes produce satisfactory results, indicating that the reduced scheme is capable of reproducing the O3-NOx-VOC-HOx diurnal cycle during conditions characterized by a low NOx regime and small O3 tendencies (less than 1 ppb per hour). By focusing on the budget equations of chemical species in the mixedlayer model, we show that for species like O3, NO and NO2, the influence of entrainment and boundary layer growth is of the same order as chemical production/loss. This indicates that an accurate representation of ABL processes is crucial in understanding the diel cycle of chemical species. By comparing the time scales of chemical reactive species with the mixing time scale of turbulence, we propose a classification based on the Damk¨ohler number to further determine the importance of dynamics on chemistry during field campaigns. Our findings advocate an integrated approach, simultaneously solving the ABL dynamics and chemical reactions, in order to obtain a better understanding of chemical pathways and processes and the interpretation of the results obtained during measurement campaigns.

KW - volatile organic-compounds

KW - tropical forest

KW - oh reactivity

KW - isoprene

KW - chemistry

KW - campaign

KW - air

KW - segregation

KW - turbulence

KW - gabriel

U2 - 10.5194/acp-12-5329-2012

DO - 10.5194/acp-12-5329-2012

M3 - Article

VL - 12

SP - 5329

EP - 5341

JO - Atmospheric Chemistry and Physics

T2 - Atmospheric Chemistry and Physics

JF - Atmospheric Chemistry and Physics

SN - 1680-7316

ER -