scholarly journals Influence of altitude on ozone levels and variability in the lower troposphere: a ground-based study for western Europe over the period 2001–2004

2007 ◽  
Vol 7 (16) ◽  
pp. 4311-4326 ◽  
Author(s):  
A. Chevalier ◽  
F. Gheusi ◽  
R. Delmas ◽  
C. Ordóñez ◽  
C. Sarrat ◽  
...  

Abstract. The PAES (French acronym for synoptic scale atmospheric pollution) network focuses on the chemical composition (ozone, CO, NOx/y and aerosols) of the lower troposphere (0–3000 m). Its high-altitude surface stations located in different mountainous areas in France complete the low-altitude rural MERA stations (the French contribution to the european program EMEP, European Monitoring and Evaluation Program). They are representative of pollution at the scale of the French territory because they are away from any major source of pollution. This study deals with ozone observations between 2001 and 2004 at 11 stations from PAES and MERA, in addition to 16 elevated stations located in mountainous areas of Switzerland, Germany, Austria, Italy and Spain. The set of stations covers a range of altitudes between 115 and 3550 m. The comparison between recent ozone mixing ratios to those of the last decade at Pic du Midi (2877 m), as well as trends calculated over 14-year data series at three high-altitude sites in the Alps (Jungfraujoch, Sonnblick and Zugspitze) reveal that ozone is still increasing but at a slower rate than in the 1980s and 1990s. The 2001–2004 mean levels of ozone from surface stations capture the ozone stratification revealed by climatological profiles from the airborne observation system MOZAIC (Measurement of OZone and water vapour by Airbus In-service airCraft) and from ozone soundings above Payerne (Switzerland). In particular all data evidence a clear transition at about 1000–1200 m a.s.l. between a sharp gradient below (of the order of +30 ppb/km) and a gentler gradient (+3 ppb/km) above. The same altitude (1200 m) is also found to be a threshold regarding how well the ozone levels at the surface stations agree with the free-tropospheric reference (MOZAIC or soundings). Below the departure can be as large as 40%, but suddenly drops within 15% above. For stations above 2000 m, the departure is even less than 8%. Ozone variability also reveals a clear transition between boundary-layer and free-tropospheric regimes around 1000 m a.s.l. Below, diurnal photochemistry accounts for about the third of the variability in summer, but less than 20% above – and at all levels in winter – where ozone variability is mostly due to day-to-day changes (linked to weather conditions or synoptic transport). In summary, the altitude range 1000–1200 m clearly turns out in our study to be an upper limit below which specific surface effects dominate the ozone content. Monthly-mean ozone mixing-ratios show at all levels a minimum in winter and the classical summer broad maximum in spring and summer – which is actually the superposition of the tropospheric spring maximum (April–May) and regional pollution episodes linked to persistent anticyclonic conditions that may occur from June to September. To complement this classical result it is shown that summer maxima are associated with considerably more variability than the spring maximum. This ensemble of findings support the relevance of mountain station networks such as PAES for the long-term observation of free-tropospheric ozone over Europe.

2007 ◽  
Vol 7 (1) ◽  
pp. 1327-1356 ◽  
Author(s):  
A. Chevalier ◽  
F. Gheusi ◽  
R. Delmas ◽  
C. Ordó\\ nez ◽  
C. Sarrat ◽  
...  

Abstract. The PAES (French acronym for synoptic scale atmospheric pollution) network focuses on the chemical composition (ozone, CO, NOx/y and aerosols) of the lower troposphere (0–3000 m). Its high-altitude surface stations located in different mountainous areas in France complete the low-altitude rural MERA stations (the French contribution to the european program EMEP, European Monitoring and Evaluation Program). They are representative of pollution at the scale of the French territory because they are away from any major source of pollution. This study deals with ozone observations between 2001 and 2004 at 11 stations from PAES and MERA, in addition to 16 elevated stations located in mountainous areas of Switzerland, Germany, Austria, Italy and Spain. The set of stations covers a range of altitudes between 115 and 3550 m. The comparison between recent ozone mixing ratios with those of the last decade found in the literature for two high-elevation sites (Pic du Midi, 2877 m and Jungfraujoch, 3580 m) leads to a trend that has slowed down compared to old trends but remains positive. This could be attribuable to the reduction of ozone precursors at European scale, that however do not compensate an ozone increase at the global scale. Averaged levels of ozone increase with elevation in good agreement with data provided by the airborne observation system MOZAIC (Measurement of OZone and water vapour by Airbus In-service airCraft), showing a highly stratified ozone field in the lower troposphere, with a transition at about 1000 m asl between a sharp gradient (30 ppb/km) below but a gentler gradient (3 ppb/km) above. Ozone variability also reveals a clear transition between boundary-layer and free-tropospheric regimes at the same altitude. Below, diurnal photochemistry accounts for about the third of the variability in summer, but less than 20% above – and at all levels in winter – where ozone variability is mostly due to day-to-day changes (linked to weather conditions or synoptic transport). Monthly-mean ozone mixing-ratios show at all levels a minimum in winter and the classical summer broad maximum in spring and summer – which is actually the superposition of the tropospheric spring maximum (April–May) and regional pollution episodes linked to persistent anticyclonic conditions that may occur from June to September. To complement this classical result it is shown that summer maxima are associated with considerably more variability than the spring maximum. This ensemble of findings support the relevance of mountain station networks such as PAES for the long-term observation of free-tropospheric ozone over Europe.


2003 ◽  
Vol 3 (2) ◽  
pp. 459-468 ◽  
Author(s):  
M. Traub ◽  
H. Fischer ◽  
M. de Reus ◽  
R. Kormann ◽  
H. Heland ◽  
...  

Abstract. During the Mediterranean Intensive Oxidant Study (MINOS) in August 2001 a total of 14 measurement flights were performed with the DLR Falcon jet aircraft from Heraklion, Crete. One objective of this campaign was to investigate the role of long-range transport of pollutants into the Mediterranean area. An analysis of 5-day back trajectories indicates that in the lower troposphere (0-4 km) air masses originated from eastern and western Europe, in the mid-troposphere (4-8 km) from the North Atlantic Ocean region and in the upper troposphere (8-14 km) from North Atlantic Ocean/North America (NANA) as well as South Asia. We allocated all back trajectories to clusters based on their ending height and source region. The mixing ratios of ozone, nitrogen oxide, total reactive oxidized nitrogen (NOy), formaldehyde, methanol, acetonitrile, acetone, peroxyacetyl nitrate (PAN), carbon dioxide, carbon monoxide and methane measured along the flight tracks are examined in relation to the different cluster trajectories. In the lower troposphere the mean trace gas mixing ratios of the eastern Europe cluster trajectories were significantly higher than those from western Europe. In the upper troposphere air from the NANA region seems to be influenced by the stratosphere, in addition, air masses were transported from South Asia, being influenced by strong convection in the Indian monsoon.


2013 ◽  
Vol 6 (7) ◽  
pp. 1633-1646 ◽  
Author(s):  
H. M. Worden ◽  
D. P. Edwards ◽  
M. N. Deeter ◽  
D. Fu ◽  
S. S. Kulawik ◽  
...  

Abstract. A current obstacle to the observation system simulation experiments (OSSEs) used to quantify the potential performance of future atmospheric composition remote sensing systems is a computationally efficient method to define the scene-dependent vertical sensitivity of measurements as expressed by the retrieval averaging kernels (AKs). We present a method for the efficient prediction of AKs for multispectral retrievals of carbon monoxide (CO) and ozone (O3) based on actual retrievals from MOPITT (Measurements Of Pollution In The Troposphere) on the Earth Observing System (EOS)-Terra satellite and TES (Tropospheric Emission Spectrometer) and OMI (Ozone Monitoring Instrument) on EOS-Aura, respectively. This employs a multiple regression approach for deriving scene-dependent AKs using predictors based on state parameters such as the thermal contrast between the surface and lower atmospheric layers, trace gas volume mixing ratios (VMRs), solar zenith angle, water vapor amount, etc. We first compute the singular value decomposition (SVD) for individual cloud-free AKs and retain the first three ranked singular vectors in order to fit the most significant orthogonal components of the AK in the subsequent multiple regression on a training set of retrieval cases. The resulting fit coefficients are applied to the predictors from a different test set of test retrievals cased to reconstruct predicted AKs, which can then be evaluated against the true retrieval AKs from the test set. By comparing the VMR profile adjustment resulting from the use of the predicted vs. true AKs, we quantify the CO and O3 VMR profile errors associated with the use of the predicted AKs compared to the true AKs that might be obtained from a computationally expensive full retrieval calculation as part of an OSSE. Similarly, we estimate the errors in CO and O3 VMRs from using a single regional average AK to represent all retrievals, which has been a common approximation in chemical OSSEs performed to date. For both CO and O3 in the lower troposphere, we find a significant reduction in error when using the predicted AKs as compared to a single average AK. This study examined data from the continental United States (CONUS) for 2006, but the approach could be applied to other regions and times.


2009 ◽  
Vol 9 (12) ◽  
pp. 4157-4175 ◽  
Author(s):  
O. A. Tarasova ◽  
I. A. Senik ◽  
M. G. Sosonkin ◽  
J. Cui ◽  
J. Staehelin ◽  
...  

Abstract. Long-term ozone measurements of two background mountain sites, namely the Kislovodsk High Mountain Station in Caucasus, Russia (KHMS, 43.70° N, 42.70° E, 2070 m a.s.l.) and the Jungfraujoch in Switzerland (JFJ, 46.55° N, 7.98° E, 3580 m a.s.l.) are compared. Despite of more than 1.5 km altitude difference ozone mixing ratios are comparable at JFJ an KHMS in the beginning of measurements (1990–1993) while the annually averaged levels at JFJ are around 15 ppb higher than the ones at KHMS for the most recent years (1997–2006). The seasonal cycle of the surface ozone mixing ratios is characterized by a double spring-summer maximum at both sites with a spring one being more pronounced for the air masses with the longest contact with the upper free troposphere and stratosphere. Ozone mixing ratio increased at JFJ but decreased at KHMS for the period 1990–2006. Trends are more pronounced for the 1990s (+0.73±0.20 ppb/year at JFJ and −0.91±0.17 ppb/year at KHMS for the period 1991–2001) in comparison with the later years (+0.04±0.21 ppb/year at JFJ and −0.37±0.14 ppb/year at KHMS for the period 1997–2006). Trends show a distinct seasonality, which is different for the different periods. To investigate possible reasons for this remarkable trends difference 3-D trajectories using LAGRANTO trajectory model are used. Effects of horizontal and vertical transport on ozone trends are considered. No substantial systematic changes in the transport patterns were detected which could lead to strong changes in the trend magnitude between 1991–2001 and 1997–2006. The geographical position of the sites relative to the main topographic features and emission sources as well as distance from the coast are interpreted to be among the main reasons for the opposite surface ozone trends. During the 90s the JFJ trend reflects increase of the ozone in the upper free troposphere/lower stratosphere, while KHMS is not sensitive to this change or even showing the opposite tendency. The analysis provided evidence for a stronger influence of processes in the lower troposphere, in particular the dramatic emission decrease in the earlier 1990s in former USSR and emissions regulations in Western Europe on the surface ozone trend at KHMS.


2003 ◽  
Vol 3 (1) ◽  
pp. 107-134 ◽  
Author(s):  
M. Traub ◽  
H. Fischer ◽  
M. de Reus ◽  
R. Kormann ◽  
J. Heland ◽  
...  

Abstract. During the Mediterranean Intensive Oxidant Study (MINOS) in August 2001 a total of 14 measurement flights were performed with the DLR Falcon aircraft from Heraklion, Crete. One objective of this campaign was to investigate the role of long-range transport of pollutants into the Mediterranean area. An analysis of 5-day back trajectories indicates that in the lower troposphere (0–4 km) air masses originated from eastern and western Europe, in the mid-troposphere (4–8 km) from the Atlantic Ocean region and in the upper troposphere (8–14 km) from North Artlantic Ocean/North America  (NAONA) as well as South Asia. We allocated all back trajectories to clusters based on their ending height and source region. The mixing ratios of ozone, nitrogen oxide, total reactive oxidized nitrogen (NOy), formaldehyde, methanol, acetonitrile, acetone, peroxyacetyl nitrate (PAN), carbon dioxide, carbon monoxide and methane measured along the flight tracks are examined in relation to the different cluster trajectories. In the lower troposphere the mean gas mixing ratios of the eastern Europe cluster trajectories were significantly higher than that from western Europe. Considering 2-day instead of 5-day trajectories the relative differences between the concentrations of these two clusters increased. In the upper troposphere relatively high concentrations of  O3 and NOy, combined with low CO of the NAONA trajectories indicate mixing with stratospheric air masses.


2008 ◽  
Vol 8 (1) ◽  
pp. 3313-3356 ◽  
Author(s):  
A. Chevalier ◽  
F. Gheusi ◽  
J.-L. Attié ◽  
R. Delmas ◽  
R. Zbinden ◽  
...  

Abstract. Continuous CO measurements performed at 3 high-altitude stations in France are analyzed for the first time. Data are provided by the new PAES (Pollution Atmospherique à l'Echelle Synoptique) network since 2002 for the Puy de Dôme and 2004 for the Pic du Midi and the Donon. CO measurements of 5 another European stations have been analysed to put the PAES stations in an European perspective. The January 2002–April 2005 CO mean levels of surface stations capture the stratification revealed by climatological CO profiles from the airborne observation system MOZAIC (Measurement of OZone and water vapour by Airbus In-service Aircraft). The deviation between the free tropospheric reference MOZAIC and surface data above 2000 m is less than 10% and this deviation can be explained in term of spatial variability, as evidenced by MOPITT CO retrievals at 700 hPa. This suggests that, averaged at a seasonal time scale (4 months), surface data at stations above 2000 m are representative of background CO concentration. This paper focuses then on trends since the 1980s–1990s. The comparison between old (1982–1983) and recent CO mixing ratio (2005) at the Pic du Midi leads to a 10% decrease, consistent with the continuous data series at Zugspitze (ZSP) from 1991 to 2004. This decrease was found to be mainly due to a negative trend of January–April mean levels. The decrease in CO sources over France and Europe appears to be responsible for that trend. The stable values of June–September mean levels suggest that the summertime oxidizing capacity of the atmosphere related to OH radicals is important enough to counterbalance any CO inputs into the troposphere. Our study shows a recent change in CO evolution since 2000 over Western Europe, with a slowed down decrease in CO concentration. Studying specifically the interactions between CO, CH4 and OH turns out to be needed, however, to find definitive explanations to those observations.


2007 ◽  
Vol 7 (14) ◽  
pp. 3783-3790 ◽  
Author(s):  
P. D. Kalabokas ◽  
A. Volz-Thomas ◽  
J. Brioude ◽  
V. Thouret ◽  
J.-P. Cammas ◽  
...  

Abstract. Vertical ozone profiles measured in the period 1996–2002 in the framework of the MOZAIC project (Measurement of Ozone and Water Vapor by Airbus in Service Aircraft) for flights connecting Central Europe to the Eastern Mediterranean basin (Heraklion, Rhodes, Antalya) were analysed in order to evaluate the high rural ozone levels recorded in the Mediterranean area during summertime. The 77 flights during summer (JJAS) showed substantially (10–12 ppb, 20–40%) enhanced ozone mixing ratios in the lower troposphere over the Eastern Mediterranean frequently exceeding the 60 ppb, 8-h EU air quality standard, whereas ozone between 700 hPa and 400 hPa was only slightly (3–5 ppb, 5–10%) higher than over Central Europe. Analysis of composite weather maps for the high and low ozone cases, as well as back-trajectories and vertical profiles of carbon monoxide, suggest that the main factor leading to high tropospheric ozone values in the area is anticyclonic influence, in combination with a persistent northerly flow in the lower troposphere during summertime over the Aegean. On the other hand the lowest ozone levels are associated with low-pressure systems, especially the extension of the Middle East low over the Eastern Mediterranean area.


2007 ◽  
Vol 7 (1) ◽  
pp. 2249-2274 ◽  
Author(s):  
P. D. Kalabokas ◽  
A. Volz-Thomas ◽  
J. Brioude ◽  
V. Thouret ◽  
J.-P. Cammas ◽  
...  

Abstract. Vertical ozone profiles measured in the period 1996–2002 in the framework of the MOZAIC project (Measurement of Ozone and Water Vapor by Airbus in Service Aircraft) for flights connecting Central Europe to the Eastern Mediterranean basin (Heraklion, Rhodes; Antalya) were analysed in order to evaluate the high rural ozone levels recorded in the Mediterranean area during summertime. The 77 flights during summer (JJAS) showed significantly (10–12 ppb, 20–40%) enhanced ozone mixing ratios in the lower troposphere over the Eastern Mediterranean frequently exceeding the 60 ppb, 8-h EU air quality standard, whereas ozone between 700 hPa and 400 hPa was only slightly (3–5 ppb, 5–10%) higher than over central Europe. Analysis of composite weather maps for the high and low ozone cases, as well as back-trajectories and vertical profiles of carbon monoxide, suggest that the main factor leading to high tropospheric ozone values in the area is anticyclonic influence, in combination with a persistent northerly flow in the lower troposphere during summertime over the Aegean. On the other hand the lowest ozone levels are associated with low-pressure systems, especially the extension of the Middle East low over the Eastern Mediterranean area.


2013 ◽  
Vol 13 (20) ◽  
pp. 10339-10352 ◽  
Author(s):  
P. D. Kalabokas ◽  
J.-P. Cammas ◽  
V. Thouret ◽  
A. Volz-Thomas ◽  
D. Boulanger ◽  
...  

Abstract. In order to evaluate the observed high rural ozone levels in the eastern Mediterranean area during summertime, vertical profiles of ozone measured in the period 1994–2008 in the framework of the MOZAIC project (Measurement of Ozone and Water Vapor by Airbus in Service Aircraft) over the eastern Mediterranean basin (Cairo, Tel Aviv, Heraklion, Rhodes, Antalya) were analyzed, focusing in the lower troposphere (1.5–5 km). At first, vertical profiles collected during extreme days with very high or very low tropospheric ozone mixing ratios have been examined together with the corresponding back-trajectories. Also, the average profiles of ozone, relative humidity, carbon monoxide, temperature gradient and wind speed corresponding to the 7% highest and the 7% lowest ozone mixing ratios for the 1500–5000 m height layer for Cairo and Tel Aviv have been examined and the corresponding composite maps of geopotential heights at 850 hPa have been plotted. Based on the above analysis, it turns out that the lower-tropospheric ozone variability over the eastern Mediterranean area is controlled mainly by the synoptic meteorological conditions, combined with local topographical and meteorological features. In particular, the highest ozone concentrations in the lower troposphere and subsequently in the boundary layer are associated with large-scale subsidence of ozone-rich air masses from the upper troposphere under anticyclonic conditions while the lowest ozone concentrations are associated with low pressure conditions inducing uplifting of boundary-layer air, poor in ozone and rich in relative humidity, to the lower troposphere.


2013 ◽  
Vol 13 (1) ◽  
pp. 2457-2491 ◽  
Author(s):  
P. D. Kalabokas ◽  
J.-P. Cammas ◽  
V. Thouret ◽  
A. Volz-Thomas ◽  
D. Boulanger ◽  
...  

Abstract. In order to evaluate the observed high rural ozone levels in the Eastern Mediterranean area during summertime, vertical profiles of ozone measured in the period 1994–2008 in the framework of the MOZAIC project (Measurement of Ozone and Water Vapor by Airbus in Service Aircraft) over the Eastern Mediterranean basin (Cairo, Tel-Aviv, Heraklion, Rhodes, Antalya) were analysed, focusing in the lower troposphere (1.5–5 km). At first, vertical profiles collected during extreme days with very high or very low tropospheric ozone mixing ratios have been examined together with the corresponding back-trajectories. Also, the average profiles of ozone, relative humidity, carbon monoxide, temperature gradient and wind speed corresponding to the 7% highest and the 7% lowest ozone mixing ratios for the 1500–5000 m height layer for Cairo and Tel-Aviv have been examined and the corresponding composite maps of geopotential heights at 850 hPa have been plotted. Based on the above analysis, it turns out that the lower-tropospheric ozone variability over the Eastern Mediterranean area is controlled mainly by the synoptic meteorological conditions, combined with local topographical and meteorological features. In particular, the highest ozone concentrations in the lower troposphere and subsequently in the boundary layer are associated with large scale subsidence of ozone rich air masses from the upper troposphere under anticyclonic conditions while the lowest ozone concentrations are associated with low pressure conditions inducing uplifting of boundary layer air, poor in ozone and rich in relative humidity, to the lower troposphere.


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