Kalman Filter Analysis of Boundary Layer Ozone in Europe with a Chemistry Transport Model

Author(s):  
Remus G. Hanea ◽  
Guus J.M. Velders ◽  
Arnold W. Heemink
2010 ◽  
Vol 10 (16) ◽  
pp. 7763-7773 ◽  
Author(s):  
X. Yang ◽  
J. A. Pyle ◽  
R. A. Cox ◽  
N. Theys ◽  
M. Van Roozendael

Abstract. In the last two decades, significant depletion of boundary layer ozone (ozone depletion events, ODEs) has been observed in both Arctic and Antarctic spring. ODEs are attributed to catalytic destruction by bromine radicals (Br plus BrO), especially during bromine explosion events (BEs), when high concentrations of BrO periodically occur. However, neither the exact source of bromine nor the mechanism for sustaining the observed high BrO concentrations is completely understood. Here, by considering the production of sea salt aerosol from snow lying on sea ice during blowing snow events and the subsequent release of bromine, we successfully simulate the BEs using a global chemistry transport model. We find that heterogeneous reactions play an important role in sustaining a high fraction of the total inorganic bromine as BrO. We also find that emissions of bromine associated with blowing snow contribute significantly to BrO at mid-latitudes. Modeled tropospheric BrO columns generally compare well with the tropospheric BrO columns retrieved from the GOME satellite instrument (Global Ozone Monitoring Experiment). The additional blowing snow bromine source, identified here, reduces modeled high latitude lower tropospheric ozone amounts by up to an average 8% in polar spring.


2005 ◽  
Vol 131 (606) ◽  
pp. 477-502 ◽  
Author(s):  
A. J. Segers ◽  
H. J. Eskes ◽  
R. J. van der A ◽  
R. F. van Oss ◽  
P. F. J. van Velthoven

2017 ◽  
Author(s):  
Heiko Bozem ◽  
Tim M. Butler ◽  
Mark G. Lawrence ◽  
Hartwig Harder ◽  
Monica Martinez ◽  
...  

Abstract. Ozone (O3) is an important atmospheric oxidant, a greenhouse gas, and a hazard to human health and agriculture. Here we describe airborne in-situ measurements and model simulations of O3 and its precursors during tropical and extratropical field campaigns over South America and Europe, respectively. Using the measurements, net ozone formation/destruction tendencies are calculated and compared to 3D chemistry-transport model simulations. In general, observation-based net ozone tendencies are positive in the continental boundary layer and the upper troposphere at altitudes above ~ 6 km in both environments. On the other hand, in the marine boundary layer and the middle troposphere, from the top of the boundary layer to about 6–8 km altitude, net O3 destruction prevails. The ozone tendencies are controlled by ambient concentrations of nitrogen oxides (NOx). In regions with net ozone destruction the available NOx is below the threshold value at which production and destruction of O3 balance. While threshold NO values increase with altitude, in the upper troposphere NOx concentrations are generally higher, probably due to the integral effect of convective precursor transport from the boundary layer and NOx produced by lightning. Two case studies indicate that in fresh convective outflow of electrified thunderstorms net ozone production is enhanced by a factor 5–6 compared to the undisturbed upper tropospheric background. The chemistry-transport model MATCH-MPIC generally reproduces the pattern of observation-based net ozone tendencies, but mostly underestimates the magnitude of the net tendency (for both net ozone production and destruction).


2017 ◽  
Vol 17 (17) ◽  
pp. 10565-10582 ◽  
Author(s):  
Heiko Bozem ◽  
Tim M. Butler ◽  
Mark G. Lawrence ◽  
Hartwig Harder ◽  
Monica Martinez ◽  
...  

Abstract. Ozone (O3) is an important atmospheric oxidant, a greenhouse gas, and a hazard to human health and agriculture. Here we describe airborne in situ measurements and model simulations of O3 and its precursors during tropical and extratropical field campaigns over South America and Europe, respectively. Using the measurements, net ozone formation/destruction tendencies are calculated and compared to 3-D chemistry–transport model simulations. In general, observation-based net ozone tendencies are positive in the continental boundary layer and the upper troposphere at altitudes above  ∼  6 km in both environments. On the other hand, in the marine boundary layer and the middle troposphere, from the top of the boundary layer to about 6–8 km altitude, net O3 destruction prevails. The ozone tendencies are controlled by ambient concentrations of nitrogen oxides (NOx). In regions with net ozone destruction the available NOx is below the threshold value at which production and destruction of O3 balance. While threshold NO values increase with altitude, in the upper troposphere NOx concentrations are generally higher due to the integral effect of convective precursor transport from the boundary layer, downward transport from the stratosphere and NOx produced by lightning. Two case studies indicate that in fresh convective outflow of electrified thunderstorms net ozone production is enhanced by a factor 5–6 compared to the undisturbed upper tropospheric background. The chemistry–transport model MATCH-MPIC generally reproduces the pattern of observation-based net ozone tendencies but mostly underestimates the magnitude of the net tendency (for both net ozone production and destruction).


2013 ◽  
Vol 13 (1) ◽  
pp. 689-727 ◽  
Author(s):  
H. Lee ◽  
S. C. Olsen ◽  
D. J. Wuebbles ◽  
D. Youn

Abstract. The continuing increase in demand for commercial aviation transport raises questions about the effects of resulting emissions on the environment. The purpose of this study is to investigate, using a global chemistry transport model, to what extent aviation emissions outside the boundary layer influence air quality in the boundary layer. The effects of current levels of aircraft emissions were studied through comparison of multiple simulations allowing for the separated effects of aviation emissions occurring in the low, middle and upper troposphere. We show that emissions near cruise altitudes rather than emissions during landing and take-off are responsible for most of the total odd-nitrogen (NOy), ozone (O3) and aerosol perturbations near the ground with a noticeable seasonal difference. Overall, the perturbations of these species are smaller than 1 ppb even in winter when the perturbations are greater than in summer. Based on the widely used air quality standards and uncertainty of state-of-the-art models, we conclude that aviation-induced perturbations have a negligible effect on air quality even in areas with heavy air traffic. Aviation emissions lead to a less than 1% aerosol enhancement in the boundary layer due to a slight increase in ammonium nitrate (NH4NO3) during cold seasons and a statistically insignificant aerosol perturbation in summer. In addition, statistical analysis using probability density functions, Hellinger distance, and p-value indicate that aviation emissions outside the boundary layer do not affect the occurrence of extremely high aerosol concentrations in the boundary layer. An additional sensitivity simulation assuming the doubling of surface ammonia emissions demonstrates that the aviation induced aerosol increase near the ground is highly dependent on background ammonia concentrations whose current range of uncertainty is large.


2010 ◽  
Vol 10 (3) ◽  
pp. 8135-8164 ◽  
Author(s):  
◽  
J. A. Pyle ◽  
R. A. Cox ◽  
N. Theys ◽  
M. Van Roozendael

Abstract. In the last two decades, significant depletion of boundary layer ozone (ozone depletion events, ODEs) has been observed in both Arctic and Antarctic spring. ODEs are attributed to catalytic destruction by bromine radicals (Br plus BrO), especially during bromine explosion events (BEs), when high concentrations of BrO periodically occur. However, neither the exact source of bromine nor the mechanism for sustaining the observed high BrO concentrations is completely understood. Here, by considering the production of sea salt aerosol from snow lying on sea ice during blowing snow events and the subsequent release of bromine, we successfully simulate the BEs using a global chemistry transport model. We find that heterogeneous reactions play an important role in sustaining a high fraction of the total inorganic bromine as BrO. Modeled tropospheric BrO columns generally compare well with the tropospheric BrO columns retrieved from the GOME satellite instrument (Global Ozone Monitoring Experiment). The additional blowing snow bromine source, identified here, reduces modeled high latitude lower tropospheric ozone amounts by up to an average 8% in polar spring.


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