Mid-latitude tropospheric ozone columns from the MOZAIC program: climatology and interannual variability

Several thousands of ozone vertical profiles collected in the course of the MOZAIC programme (Measurements of Ozone, Water Vapour, Carbon Monoxide and Nitrogen Oxides by In-Service Airbus Aircraft) from August 1994 to February 2002 are investigated to bring out climatological and interannual variability aspects. The study is centred on the most frequently visited MOZAIC airports, i.e. Frankfurt (Germany), Paris (France), New York (USA) and the cluster of Tokyo, Nagoya and Osaka (Japan). The analysis focuses on the vertical integration of ozone from the ground to the dynamical tropopause and the vertical integration of stratospheric-origin ozone throughout the troposphere. The characteristics of the MOZAIC profiles: frequency of flights, accuracy, precision, and depth of the troposphere observed, are presented. The climatological analysis shows that the Tropospheric Ozone Column (<I>TOC</I>) seasonal cycle ranges from a wintertime minimum at all four stations to a spring-summer maximum in Frankfurt, Paris, and New York. Over Japan, the maximum occurs in spring presumably because of the earlier springtime sun. The incursion of monsoon air masses into the boundary layer and into the mid troposphere then steeply diminishes the summertime value. Boundary layer contributions to the <I>TOC</I> are 10% higher in New York than in Frankfurt and Paris during spring and summer, and are 10% higher in Japan than in New York, Frankfurt and Paris during autumn and early spring. Local and remote anthropogenic emissions, and biomass burning over upstream regions of Asia may be responsible for the larger low- and mid-tropospheric contributions to the tropospheric ozone column over Japan throughout the year except during the summer-monsoon season. A simple Lagrangian analysis has shown that a minimum of 10% of the <I>TOC</I> is of stratospheric-origin throughout the year. Investigation of the short-term trends of the <I>TOC</I> over the period 1995&ndash;2001 shows a linear increase 0.7%/year in Frankfurt, 0.8%/year in Japan, 1.1%/year in New York and 1.6%/year in Paris for the reduced 1995&ndash;1999 period. Dominant ingredients of these positive short-term trends are the continuous increase of wintertime tropospheric ozone columns from 1996 to 1999 and the positive contributions of the mid troposphere whatever the season

Tropospheric ozone over Equatorial Africa: regional aspects from the MOZAIC data

We analyze ozone observations recorded over Equatorial Africa between April 1997 and March 2003 by the MOZAIC programme, providing the first ozone climatology deriving from continental in-situ data over this region. Three-dimensional streamlines strongly suggests connections between the characteristics of the ozone monthly mean vertical profiles, the most persistent circulation patterns in the troposphere over Equatorial Africa (on a monthly basis) such as the Harmattan, the African Easterly Jet, the Trades and the regions of ozone precursors emissions by biomass burning. During the biomass burning season in each hemisphere, the lower troposphere exhibits layers of enhanced ozone (i.e. 70 ppbv over the coast of Gulf of Guinea in December-February and 85 ppbv over Congo in June-August). The characteristics of the ozone monthly mean vertical profiles are clearly connected to the regional flow regime determined by seasonal dynamic forcing. The mean ozone profile over the coast of Gulf of Guinea in the burning season is characterized by systematically high ozone below 650hPa ; these are due to the transport by the Harmattan and the AEJ of the pollutants originating from upwind fires. The confinement of high ozone to the lower troposphere is due to the high stability of the Harmattan and the blocking Saharan anticyclone which prevents efficient vertical mixing. In contrast, ozone enhancements observed over Central Africa during the local dry season (June-August) are not only found in the lower troposphere but throughout the troposphere. Moreover, this study highlights a connection between the regions of the coast of Gulf of Guinea and regions of Congo to the south that appears on a semi annual basis. Vertical profiles in wet-season regions exhibit ozone enhancements in the lower troposphere due to biomass burning products transport from fires situated in the opposite dry-season hemisphere

A linear CO chemistry parameterization in a chemistry-transport model: evaluation and application to data assimilation

This paper presents an evaluation of a new linear parameterization valid for the troposphere and the stratosphere, based on a first order approximation of the carbon monoxide (CO) continuity equation. This linear scheme (hereinafter noted LINCO) has been implemented in the 3-D Chemical Transport Model (CTM) MOCAGE (MOdèle de Chimie Atmospherique Grande Echelle). First, a one and a half years of LINCO simulation has been compared to output obtained from a detailed chemical scheme output. The mean differences between both schemes are about ±25 ppbv (part per billion by volume) or 15% in the troposphere and ±10 ppbv or 100% in the stratosphere. Second, LINCO has been compared to diverse observations from satellite instruments covering the troposphere (Measurements Of Pollution In The Troposphere: MOPITT) and the stratosphere (Microwave Limb Sounder: MLS) and also from aircraft (Measurements of ozone and water vapour by Airbus in-service aircraft: MOZAIC programme) mostly flying in the upper troposphere and lower stratosphere (UTLS). In the troposphere, the LINCO seasonal variations as well as the vertical and horizontal distributions are quite close to MOPITT CO observations. However, a bias of ~&amp;minus;40 ppbv is observed at 700 Pa between LINCO and MOPITT. In the stratosphere, MLS and LINCO present similar large-scale patterns, except over the poles where the CO concentration is underestimated by the model. In the UTLS, LINCO presents small biases less than 2% compared to independent MOZAIC profiles. Third, we assimilated MOPITT CO using a variational 3D-FGAT (First Guess at Appropriate Time) method in conjunction with MOCAGE for a long run of one and a half years. The data assimilation greatly improves the vertical CO distribution in the troposphere from 700 to 350 hPa compared to independent MOZAIC profiles. At 146 hPa, the assimilated CO distribution is also improved compared to MLS observations by reducing the bias up to a factor of 2 in the tropics. This study confirms that the linear scheme is able to simulate reasonably well the CO distribution in the troposphere and in the lower stratosphere. Therefore, the low computing cost of the linear scheme opens new perspectives to make free runs and CO data assimilation runs at high resolution and over periods of several years

A numerical study of tropical cross-tropopause transport by convective overshoots during the TROCCINOX golden day

International audienceObservations obtained during the Tropical Convection, Cirrus and Nitrogen Oxides (TROCCINOX) golden day have revealed the presence of ice particles up to 410 K (18.2 km) 2 km above the local tropopause. The case is investigated using a three-dimensional quadruply nested non-hydrostatic simulation and Meteosat Second Generation (MSG) observations. The simulation fairly well reproduces the measurements along the flight track. A reasonable agreement with MSG observations is also achieved: the 10.8-µm brightness temperature (BT) minimum of 187 K is reproduced (a value 6 K colder than the environmental cold-point temperature) as well as the positive BT difference between the 6.2- and 10.8-µm bands, an overshoot signature. The simulation produces several overshooting plumes up to 410 K yielding an upward transport of water vapour of a few tons per second across the tropical tropopause. The estimated mass flux agree with those derived from over tracer budgets indicating that convection transport mass across the tropopause

The detection of post-monsoon tropospheric ozone variability over south Asia using IASI data

The ozone (O&lt;sub&gt;3&lt;/sub&gt;) variability over south Asia during the 2008 post-monsoon season has been assessed using measurements from the MetOP-A/IASI instrument and O&lt;sub&gt;3&lt;/sub&gt; profiles retrieved with the SOftware for a Fast Retrieval of IASI Data (SOFRID). The information content study and error analyses carried out in this paper show that IASI Level 1 data can be used to retrieve tropospheric O&lt;sub&gt;3&lt;/sub&gt; columns (TOC, surface-225 hPa) and UTLS columns (225–70 hPa) with errors smaller than 20%. Validation with global radiosonde O&lt;sub&gt;3&lt;/sub&gt; profiles obtained during a period of 6 months show the excellent agreement between IASI and radiosonde for the UTLS with correlation coefficient &lt;i&gt;R&lt;/i&gt; &gt; 0.91 and good agreement in the troposphere with correlation coefficient &lt;i&gt;R&lt;/i&gt; &gt; 0.74. For both the UTLS and the troposphere Relative Standard Deviations (RSD) are lower than 23%. Comparison with in-situ measurements from the MOZAIC program around Hyderabad demonstrates that IASI is able to capture the TOC inter and intra-seasonal variability in central India. Nevertheless, the agreement is mitigated by the fact that the smoothing of the true O&lt;sub&gt;3&lt;/sub&gt; profiles by the retrieval results in a reduction of the TOC variability detected by IASI relative to the variability observed by in situ instruments. The post-monsoon temporal variability of the vertical profile of O&lt;sub&gt;3&lt;/sub&gt; around Hyderabad has been investigated with MOZAIC observations. These observations from airborne instruments show that tropospheric O&lt;sub&gt;3&lt;/sub&gt; is steadily elevated during most of the studied period with the exception of two sharp drops following the crossing of tropical storms over India. Lagrangian simulations with the FLEXPART model indicate that elevated O&lt;sub&gt;3&lt;/sub&gt; concentrations in the middle troposphere near Hyderabad are associated with the transport of UTLS air-masses that have followed the Subtropical Westerly Jet (SWJ) and subsided over northern India together with boundary layer polluted air-masses transported from the Indo-gangetic plain by the north-easterly trades. Low O&lt;sub&gt;3&lt;/sub&gt; concentrations result from the uplift and westward transport of pristine air-masses from the marine boundary layer of the Bay of Bengal by tropical storms. In order to extend the analysis of tropospheric O&lt;sub&gt;3&lt;/sub&gt; variability to the whole of south Asia, we have used IASI-SOFRID O&lt;sub&gt;3&lt;/sub&gt; data. We show that IASI O&lt;sub&gt;3&lt;/sub&gt; data around Hyderabad were able to capture the fast variability revealed by MOZAIC. Furthermore, their spatio-temporal coverage demonstrates that the behaviour of tropospheric O&lt;sub&gt;3&lt;/sub&gt; observed near Hyderabad extended over most of central and south India and part of the Bay of Bengal. This result highlights the ability of the IASI sensor to capture fast changes in chemical composition related to dramatic tropical weather conditions

The influence of biogenic emissions from Africa on tropical tropospheric ozone during 2006: a global modeling study

We have performed simulations using a 3-D global chemistry-transport model to investigate the influence that biogenic emissions from the African continent exert on the composition of the troposphere in the tropical region. For this purpose we have applied two recently developed biogenic emission inventories provided for use in large-scale global models (Granier et al., 2005; LathiSre et al., 2006) whose seasonality and temporal distribution for biogenic emissions of isoprene, other volatile organic compounds and NO is markedly different. The use of the 12 year average values for biogenic emissions provided by LathiSre et al. (2006) results in an increase in the amount of nitrogen sequestrated into longer lived reservoir compounds which contributes to the reduction in the tropospheric ozone burden in the tropics. The associated re-partitioning of nitrogen between PAN, HNO3 and organic nitrates also results in a similar to 5% increase in the loss of nitrogen by wet deposition. At a global scale there is a reduction in the oxidizing capacity of the model atmosphere which increases the atmospheric lifetimes of CH4 and CO by similar to 1.5% and similar to 4%, respectively. Comparisons against a range of different measurements indicate that applying the 12 year average of LathiSre et al. (2006) improves the performance of TM4_AMMA for 2006 in the tropics. By the use of sensitivity studies we show that the release of NO from soils in Africa accounts for between similar to 2-45% of tropospheric ozone in the African troposphere, similar to 10% in the upper troposphere and between similar to 5-20% of the tropical tropospheric ozone column over the tropical Atlantic Ocean. The subsequent reduction in OH over the source regions allows enhanced transport of CO out of the region. For biogenic volatile organic C1 to C3 species released from Africa, the effects on tropical tropospheric ozone are rather limited, although this source contributes to the global burden of VOC by between similar to 2-4% and has a large influence on the organic composition of the troposphere over the tropical Atlantic Ocean

the Creative Commons Attribution 3.0 License. Atmospheric Chemistry and Physics

The influence of biogenic emissions from Africa on tropical tropospheric ozone during 2006: a global modeling stud

Air pollution during the 2003 European heat wave as seen by MOZAIC airliners

This study presents an analysis of both MOZAIC profiles above Frankfurt and Lagrangian dispersion model simulations for the 2003 European heat wave. The comparison of MOZAIC measurements in summer 2003 with the 11-year MOZAIC climatology reflects strong temperature anomalies (exceeding 4&amp;deg;C) throughout the lower troposphere. Higher positive anomalies of temperature and negative anomalies of both wind speed and relative humidity are found for the period defined here as the heat wave (2&amp;ndash;14 August 2003), compared to the periods before (16&amp;ndash;31 July 2003) and after (16&amp;ndash;31 August 2003) the heat wave. In addition, Lagrangian model simulations in backward mode indicate the suppressed long-range transport in the mid- to lower troposphere and the enhanced southern origin of air masses for all tropospheric levels during the heat wave. Ozone and carbon monoxide also present strong anomalies (both ~+40 ppbv) during the heat wave, with a maximum vertical extension reaching 6 km altitude around 11 August 2003. Pollution in the planetary boundary layer (PBL) is enhanced during the day, with ozone mixing ratios two times higher than climatological values. This is due to a combination of factors, such as high temperature and radiation, stagnation of air masses and weak dry deposition, which favour the accumulation of ozone precursors and the build-up of ozone. A negligible role of a stratospheric-origin ozone tracer has been found for the lower troposphere in this study. From 29 July to 15 August 2003 forest fires burnt around 0.3&amp;times;10&lt;sup&gt;6&lt;/sup&gt; ha in Portugal and added to atmospheric pollution in Europe. Layers with enhanced CO and NO&lt;sub&gt;y&lt;/sub&gt; mixing ratios, advected from Portugal, were crossed by the MOZAIC aircraft in the free troposphere over Frankfurt. A series of forward and backward Lagrangian model simulations have been performed to investigate the origin of anomalies during the whole heat wave. European anthropogenic emissions present the strongest contribution to the measured CO levels in the lower troposphere (near 30%). This source is followed by Portuguese forest fires which affect the lower troposphere after 6 August 2003 and even the PBL around 10 August 2003. The averaged biomass burning contribution reaches 35% during the affected period. Anthropogenic CO of North American origin only marginally influences CO levels over Europe during that period

Tropospheric ozone climatology over Beijing : analysis of aircraft data from the MOZAIC program

Author name used in this publication: Wang, T.2007-2008 > Academic research: refereed > Publication in refereed journalVersion of RecordPublishe