scholarly journals Model simulations and aircraft measurements of vertical, seasonal and latitudinal O<sub>3</sub> and CO distributions over Europe

2006 ◽  
Vol 6 (2) ◽  
pp. 339-348 ◽  
Author(s):  
H. Fischer ◽  
M. Lawrence ◽  
Ch. Gurk ◽  
P. Hoor ◽  
J. Lelieveld ◽  
...  

Abstract. During a series of 8 measurement campaigns within the SPURT project (2001-2003), vertical profiles of CO and O3 have been obtained at subtropical, middle and high latitudes over western Europe, covering the troposphere and lowermost stratosphere up to ~14 km altitude during all seasons. The seasonal and latitudinal variation of the measured trace gas profiles are compared to simulations with the chemical transport model MATCH. In the troposphere reasonable agreement between observations and model predictions is achieved for CO and O3, in particular at subtropical and mid-latitudes, while the model overestimates (underestimates) CO (O3 in the lowermost stratosphere particularly at high latitudes, indicating too strong simulated bi-directional exchange across the tropopause. By the use of tagged tracers in the model, long-range transport of Asian air masses is identified as the dominant source of CO pollution over Europe in the free troposphere.

2005 ◽  
Vol 5 (5) ◽  
pp. 9065-9096 ◽  
Author(s):  
H. Fischer ◽  
M. Lawrence ◽  
Ch. Gurk ◽  
P. Hoor ◽  
J. Lelieveld ◽  
...  

Abstract. During a series of 8 measurement campaigns within the SPURT project (2001–2003), vertical profiles of CO and O3 have been obtained at subtropical, middle and high latitudes over western Europe, covering the troposphere and lowermost stratosphere up to ~14 km altitude during all seasons. The seasonal and latitudinal variation of the measured trace gas profiles are compared to simulations with the chemical transport model MATCH. In the troposphere reasonable agreement between observations and model predictions is achieved for CO and O3, in particular at subtropical and mid-latitudes, while the model overestimates (underestimates) CO (O3) in the lowermost stratosphere particularly at high latitudes, indicating too strong simulated bi-directional exchange across the tropopause. By the use of tagged tracers in the model, long-range transport of Asian air masses is identified as the dominant source of CO pollution over Europe in the free troposphere.


2003 ◽  
Vol 3 (3) ◽  
pp. 3051-3094
Author(s):  
A. Ladstätter-Weißenmayer ◽  
J. Heland ◽  
R. Kormann ◽  
R. v. Kuhlmann ◽  
M. G. Lawrence ◽  
...  

Abstract. The MINOS (Mediterranean INtensive Oxidant Study) campaign was an international, multi-platform field campaign to measure long-range transport of air-pollution and aerosols from South East Asia and Europe towards the Mediterranean basin during August 2001. High pollution events were observed during this campaign. For the Mediterranean region enhanced tropospheric nitrogen dioxide (NO2) and formaldehyde (HCHO), which are precursors of tropospheric ozone (O3), were detected by the satellite based GOME (Global Ozone Monitoring Experiment) instrument and compared with air-borne in-situ-measurements as well as with the output from the global 3D photochemistry-transport model MATCH-MPIC (Model of Atmospheric Transport and CHemistry - Max-Planck-Institute for Chemistry). The increase of pollution in that region leads to severe air quality degradation with regional and global implications.


2003 ◽  
Vol 3 (5) ◽  
pp. 1887-1902 ◽  
Author(s):  
A. Ladstätter-Weißenmayer ◽  
J. Heland ◽  
R. Kormann ◽  
R. von Kuhlmann ◽  
M. G. Lawrence ◽  
...  

Abstract. The MINOS (Mediterranean INtensive Oxidant Study) campaign was an international, multi-platform field campaign to measure long-range transport of air-pollution and aerosols from South East Asia and Europe towards the Mediterranean basin during August 2001. High pollution events were observed during this campaign. For the Mediterranean region enhanced tropospheric nitrogen dioxide (NO2) and formaldehyde (HCHO), which are precursors of tropospheric ozone (O3), were detected by the satellite based GOME (Global Ozone Monitoring Experiment) instrument and compared with airborne in situ measurements as well as with the output from the global 3D photochemistry-transport model MATCH-MPIC (Model of Atmospheric Transport and CHemistry - Max Planck Institute for Chemistry). The increase of pollution in that region leads to severe air quality degradation with regional and global implications.


2012 ◽  
Vol 12 (6) ◽  
pp. 15337-15372
Author(s):  
A. Wada ◽  
H. Matsueda ◽  
S. Murayama ◽  
S. Taguchi ◽  
A. Kamada ◽  
...  

Abstract. We used the observed CO/222Rn ratio in Asian outflows at Minamitorishima (MNM), Yonagunijima (YON), and Ryori (RYO) over the Western North Pacific from 2007 to 2011, together with a three-dimensional chemical transport model (STAG), in order to estimate anthropogenic emissions of CO in East Asia. The measurements captured high-frequency synoptic variations of enhanced 222Rn (ERN) events associated with long-range transport of continental air masses. 222Rn and CO showed high correlation during the ERN events observed at MNM and YON in the winter and spring, but not at RYO. The STAG transport model reproduced well the concentration of observed 222Rn when forced with constant and uniform flux density of 1.0 atom cm−2 s−1, but underestimated the associated enhancement of synoptically variable CO caused by the underestimated flux values in the EDGAR ver. 4.1 emission database used in the model for East Asia. Better estimates for the East Asian emission were derived using a radon tracer method based on the difference in the enhancement ratio of CO/222Rn between observation and model. The anthropogenic emission of CO for China, Japan, and Korea was estimated to be 203 Tg CO yr−1, 93% of which originated in China. When compared with other estimated emissions of CO, our estimated result showed consistency with those of the inverse method, whereas the emission database of EDGAR was about 45% smaller than our anthropogenic estimation for China.


2012 ◽  
Vol 12 (24) ◽  
pp. 12119-12132 ◽  
Author(s):  
A. Wada ◽  
H. Matsueda ◽  
S. Murayama ◽  
S. Taguchi ◽  
A. Kamada ◽  
...  

Abstract. We used the observed CO/222Rn ratio in the Asian outflows at Minamitorishima (MNM), Yonagunijima (YON), and Ryori (RYO) in the western North Pacific from 2007 to 2011, together with a three-dimensional chemical transport model (STAG), in order to estimate anthropogenic emissions of CO in East Asia. The measurements captured high-frequency synoptic variations of enhanced 222Rn (ERN) events associated with the long-range transport of continental air masses. 222Rn and CO showed high correlation during the ERN events observed at MNM and YON in the winter and spring, but not at RYO. The STAG transport model reproduced well the concentrations of observed 222Rn when forced with a constant and uniform flux density of 1.0 atom cm−2 s−1, but underestimated the associated enhancement of synoptically variable CO caused by the underestimated flux values in the EDGAR ver. 4.1 emission database used in the model for East Asia. Better estimates for the East Asian emission were derived using a radon tracer method based on the difference in the enhancement ratio of CO/222Rn between the observation and the model. The anthropogenic emissions of CO for China, Japan, and Korea were estimated to be 203 Tg CO yr−1, 91% of which originated in China. When compared with other estimated emissions of CO, our estimated result showed consistency with those of the inverse method, whereas the emission database of EDGAR was about 45% smaller than our anthropogenic estimation for China.


2012 ◽  
Vol 12 (2) ◽  
pp. 5939-6018
Author(s):  
C. A. Stroud ◽  
M. D. Moran ◽  
P. A. Makar ◽  
S. Gong ◽  
W. Gong ◽  
...  

Abstract. Observations from the 2007 Border Air Quality and Meteorology Study (BAQS-Met 2007) in southern Ontario (ON), Canada, were used to evaluate Environment Canada's regional chemical transport model predictions of primary organic aerosol (POA). Environment Canada's operational numerical weather prediction model and the 2006 Canadian and 2005 US national emissions inventories were used as input to the chemical transport model (named AURAMS). Particle-component-based factor analysis was applied to aerosol mass spectrometer measurements made at one urban site (Windsor, ON) and two rural sites (Harrow and Bear Creek, ON) to derive hydrocarbon-like organic aerosol (HOA) factors. Co-located carbon monoxide (CO), PM2.5 black carbon (BC), and PM1 SO4 measurements were also used for evaluation and interpretation, permitting a detailed diagnostic model evaluation. At the urban site, good agreement was observed for the comparison of daytime campaign PM1 POA and HOA mean values: 1.1 μg m−3 vs. 1.2 μg m−3, respectively. However, a POA overprediction was evident on calm nights due to an overly-stable model surface layer. Biases in model POA predictions trended from positive to negative with increasing HOA values. This trend has several possible explanations, including (1) underweighting of urban locations in particulate matter (PM) spatial surrogate fields, (2) overly-coarse model grid spacing for resolving urban-scale sources, and (3) lack of a model particle POA evaporation process during dilution of vehicular POA tail-pipe emissions to urban scales. Furthermore, a trend in POA bias was observed at the urban site as a function of the BC/HOA ratio, suggesting a possible association of POA underprediction for diesel combustion sources. For several time periods, POA overprediction was also observed for sulphate-rich plumes, suggesting that our model POA fractions for the PM2.5 chemical speciation profiles may be too high for these point sources. At the rural Harrow site, significant underpredictions in PM1 POA concentration were found compared to observed HOA concentration and were associated, based on back-trajectory analysis, with (1) transport from the Detroit/Windsor urban complex, (2) longer-range transport from the US Midwest, and (3) biomass burning. Daytime CO concentrations were significantly overpredicted at Windsor but were unbiased at Harrow. Collectively, these biases provide support for a hypothesis that combines a current underweighting of PM spatial surrogate fields for urban locations with insufficient model vertical mixing for sources close to the urban measurement sites. The magnitude of the area POA emissions sources in the US and Canadian inventories (e.g., food cooking, road and soil dust, waste disposal burning) suggests that more effort should be placed at reducing uncertainties in these sectors, especially spatial and temporal surrogates.


Author(s):  
Jason Welsh ◽  
Jack Fishman

We use a regional scale photochemical transport model to investigate the surface concentrations and column integrated amounts of ozone (O3) and nitrogen dioxide (NO2) during a pollution event that occurred in the St. Louis metropolitan region in 2012. These trace gases will be two of the primary constituents that will be measured by TEMPO, an instrument on a geostationary platform, which will result in a dataset that has hourly temporal resolution during the daytime and ~4 km spatial resolution. Although air quality managers are most concerned with surface concentrations, satellite measurements provide a quantity that reflects a column amount, which may or may not be directly relatable to what is measured at the surface. The model results provide good agreement with observed surface O3 concentrations, which is the only trace gas dataset that can be used for verification. The model shows that a plume of O3 extends downwind from St. Louis and contains an integrated amount of ozone of ~ 16 DU (1 DU = 2.69 x 1016 mol. cm-2), a quantity that is two to three times lower than what was observed by satellite measurements during two massive pollution episodes in the 1980s. Based on the smaller isolatable emissions coming from St. Louis, this quantity is not unreasonable, but may also reflect the reduction of photochemical ozone production due to the implementation of emission controls that have gone into effect in the past few decades.


2019 ◽  
Vol 6 (8) ◽  
pp. 456-461 ◽  
Author(s):  
Jianlin Hu ◽  
Bart Ostro ◽  
Hongliang Zhang ◽  
Qi Ying ◽  
Michael J. Kleeman

2016 ◽  
Vol 16 (7) ◽  
pp. 4641-4659 ◽  
Author(s):  
Hongyu Liu ◽  
David B. Considine ◽  
Larry W. Horowitz ◽  
James H. Crawford ◽  
Jose M. Rodriguez ◽  
...  

Abstract. We use the Global Modeling Initiative (GMI) modeling framework to assess the utility of cosmogenic beryllium-7 (7Be), a natural aerosol tracer, for evaluating cross-tropopause transport in global models. The GMI chemical transport model (CTM) was used to simulate atmospheric 7Be distributions using four different meteorological data sets (GEOS1-STRAT DAS, GISS II′ GCM, fvGCM, and GEOS4-DAS), featuring significantly different stratosphere–troposphere exchange (STE) characteristics. The simulations were compared with the upper troposphere and/or lower stratosphere (UT/LS) 7Be climatology constructed from  ∼  25 years of aircraft and balloon data, as well as climatological records of surface concentrations and deposition fluxes. Comparison of the fraction of surface air of stratospheric origin estimated from the 7Be simulations with observationally derived estimates indicates excessive cross-tropopause transport at mid-latitudes in simulations using GEOS1-STRAT and at high latitudes using GISS II′ meteorological data. These simulations also overestimate 7Be deposition fluxes at mid-latitudes (GEOS1-STRAT) and at high latitudes (GISS II′), respectively. We show that excessive cross-tropopause transport of 7Be corresponds to overestimated stratospheric contribution to tropospheric ozone. Our perspectives on STE in these meteorological fields based on 7Be simulations are consistent with previous modeling studies of tropospheric ozone using the same meteorological fields. We conclude that the observational constraints for 7Be and observed 7Be total deposition fluxes can be used routinely as a first-order assessment of cross-tropopause transport in global models.


2012 ◽  
Vol 12 (18) ◽  
pp. 8297-8321 ◽  
Author(s):  
C. A. Stroud ◽  
M. D. Moran ◽  
P. A. Makar ◽  
S. Gong ◽  
W. Gong ◽  
...  

Abstract. Observations from the 2007 Border Air Quality and Meteorology Study (BAQS-Met 2007) in Southern Ontario, Canada, were used to evaluate predictions of primary organic aerosol (POA) and two other carbonaceous species, black carbon (BC) and carbon monoxide (CO), made for this summertime period by Environment Canada's AURAMS regional chemical transport model. Particle component-based factor analysis was applied to aerosol mass spectrometer measurements made at one urban site (Windsor, ON) and two rural sites (Harrow and Bear Creek, ON) to derive hydrocarbon-like organic aerosol (HOA) factors. A novel diagnostic model evaluation was performed by investigating model POA bias as a function of HOA mass concentration and indicator ratios (e.g. BC/HOA). Eight case studies were selected based on factor analysis and back trajectories to help classify model bias for certain POA source types. By considering model POA bias in relation to co-located BC and CO biases, a plausible story is developed that explains the model biases for all three species. At the rural sites, daytime mean PM1 POA mass concentrations were under-predicted compared to observed HOA concentrations. POA under-predictions were accentuated when the transport arriving at the rural sites was from the Detroit/Windsor urban complex and for short-term periods of biomass burning influence. Interestingly, the daytime CO concentrations were only slightly under-predicted at both rural sites, whereas CO was over-predicted at the urban Windsor site with a normalized mean bias of 134%, while good agreement was observed at Windsor for the comparison of daytime PM1 POA and HOA mean values, 1.1 μg m−3 and 1.2 μg m−3, respectively. Biases in model POA predictions also trended from positive to negative with increasing HOA values. Periods of POA over-prediction were most evident at the urban site on calm nights due to an overly-stable model surface layer. This model behaviour can be explained by a combination of model under-estimation of vertical mixing at the urban location, under-representation of PM emissions for on-road traffic exhaust along major urban roads and highways, and a more structured allocation of area POA sources such as food cooking and dust emissions to urban locations. A downward trend in POA bias was also observed at the urban site as a function of the BC/HOA indicator ratio, suggesting a possible association of POA under-prediction with under-representation of diesel combustion sources. An investigation of the emission inventories for the province of Ontario and the nearby US state of Indiana also suggested that the top POA area emission sources (food cooking, organic-bound to dust, waste disposal burning) dominated over mobile and point sources, again consistent with a mobile under-estimation. We conclude that more effort should be placed at reducing uncertainties in the treatment of several large POA emission sources, in particular food cooking, fugitive dust, waste disposal burning, and on-road traffic sources, and especially their spatial surrogates and temporal profiles. This includes using higher spatial resolution model grids to better resolve the urban road network and urban food cooking locations. We also recommend that additional sources of urban-scale vertical mixing in the model, such as a stronger urban heat island effect and vehicle-induced turbulence, would help model predictions at urban locations, especially at night time.


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