Atmospheric correlation time measurements using coherent CO2 lidar

A pulsed TEA-CO2 lidar with coherent detection was used to measure the correlation time of backscatter from an ensemble of atmospheric aerosol particles which are illuminated by the pulsed radiation. The correlation time of the backscatter return signal is important in studies of atmospheric turbulence and its effects on optical propagation and backscatter. If the temporal coherence of the pulse is large enough, then the temporal coherence of the return signal is dominated by the turbulence and shear for a variety of interesting atmospheric conditions. Various techniques for correlation time measurement are discussed and evaluated

Comparison of long term tropospheric ozone trends measured by lidar and ECC ozonesondes from 1991 to 2010 in Southern France

International audienceECC (Electrochemical Concentration Cell) ozonesondes and UV DIAL (DIfferential Absorption Lidar) measurements have been carried out simultaneously at OHP (Observatoire de Haute Provence, 44°N, 6.7°E, 690 m) since 1991. A unique long-term trend assessment by two different instruments operated routinely at the same location is possible. Air mass trajectories have been calculated for all the ozone observations available at OHP. The bias between the seasonal mean calculated with lidar and ECC ozone vertical profiles for 4 time- periods of 5 years is 0.6 ppbv in the free troposphere (4-8 km). Larger differences (> 10 ppbv) are explained by the need for clear sky conditions during lidar observations. The measurements of both instruments have been combined to decrease the impact of short-term atmospheric variability on the trend estimate

Analysis of a 7 year tropospheric ozone vertical distribution at the Observatoire de Haute Provence

A seven year (1984-90) climatology of tropospheric vertical ozone soundings, performed by electrochemical sondes at the OHP (44 deg N, 6 deg E, 700 m ASL) in Southern France, is presented. Its seasonal variation shows a broad spring/summer maximum in the troposphere. The contribution of photochemical ozone production and transport from the stratosphere to this seasonal variation are studied by a correlative analysis of ozone concentrations and meteorological variables, with emphasis on potential vorticity. This analysis shows the impact of dynamical and photochemical processes on the spatial and temporal ozone variability. In particular, a positive correlation (r = 04.0, significance greater than 99.9 percent) of ozone with potential vorticity is observed in the middle troposphere, reflecting the impact of stratosphere-troposphere exchange on the vertical ozone distribution

A Lagrangian analysis of the impact of transport and transformation on the ozone stratification observed in the free troposphere during the ESCOMPTE campaign

The ozone variability observed by tropospheric ozone lidars during the ESCOMPTE campaign is analyzed by means of a hybrid-Lagrangian modeling study. Transport processes responsible for the formation of ozone-rich layers are identified using a semi-Lagrangian analysis of mesoscale simulations to identify the planetary boundary layer (PBL) footprint in the free troposphere. High ozone concentrations are related to polluted air masses exported from the Iberian PBL. The chemical composition of air masses coming from the PBL and transported in the free troposphere is evaluated using a Lagrangian chemistry model. The initial concentrations are provided by a model of chemistry and transport. Different scenarios are tested for the initial conditions and for the impact of mixing with background air in order to perform a quantitative comparison with the lidar observations. For this meteorological situation, the characteristic mixing time is of the order of 2 to 6 days depending on the initial conditions. Ozone is produced in the free troposphere within most air masses exported from the Iberian PBL at an average rate of 0.2 ppbv h^−1, with a maximum ozone production of 0.4 ppbv h^−1. Transport processes from the PBL are responsible for an increase of 13.3 ppbv of ozone concentrations in the free troposphere compared to background levels; about 45% of this increase is attributed to in situ production during the transport rather than direct export of ozone

Tropospheric Ozone Assessment Report: present-day distribution and trends of tropospheric ozone relevant to climate and global atmospheric chemistry model evaluation

The Tropospheric Ozone Assessment Report (TOAR) is an activity of the International Global Atmospheric Chemistry Project. This paper is a component of the report, focusing on the present-day distribution and trends of tropospheric ozone relevant to climate and global atmospheric chemistry model evaluation. Utilizing the TOAR surface ozone database, several figures present the global distribution and trends of daytime average ozone at 2702 non-urban monitoring sites, highlighting the regions and seasons of the world with the greatest ozone levels. Similarly, ozonesonde and commercial aircraft observations reveal ozone’s distribution throughout the depth of the free troposphere. Long-term surface observations are limited in their global spatial coverage, but data from remote locations indicate that ozone in the 21st century is greater than during the 1970s and 1980s. While some remote sites and many sites in the heavily polluted regions of East Asia show ozone increases since 2000, many others show decreases and there is no clear global pattern for surface ozone changes since 2000. Two new satellite products provide detailed views of ozone in the lower troposphere across East Asia and Europe, revealing the full spatial extent of the spring and summer ozone enhancements across eastern China that cannot be assessed from limited surface observations. Sufficient data are now available (ozonesondes, satellite, aircraft) across the tropics from South America eastwards to the western Pacific Ocean, to indicate a likely tropospheric column ozone increase since the 1990s. The 2014–2016 mean tropospheric ozone burden (TOB) between 60°N–60°S from five satellite products is 300 Tg ± 4%. While this agreement is excellent, the products differ in their quantification of TOB trends and further work is required to reconcile the differences. Satellites can now estimate ozone’s global long-wave radiative effect, but evaluation is difficult due to limited in situ observations where the radiative effect is greatest.Peer ReviewedPostprint (published version

Ozone transport during a cut-off low event studied in the frame of the TOASTE program

A study of ozone transfer to the troposphere has been performed during two phases of the evolution of a cut-off low using both ozone vertical profiles and objective analysis of the ECMWF to compute potential vorticity distributions and air mass trajectories. Ozone profiles were measured by a ground based lidar system at the Observatoire de Haute Provence (OHP, 43 deg 55 N, 5 deg 42 E). A stratospheric ozone transport into the troposphere has been observed during a tropopause fold which occurred at the beginning of the cut-off low formation and during the erosion phase of the cut-off low. From the estimate of the maximum ozone content transferred to the troposphere, both mechanisms have the same order of magnitude of influence on the ozone flux to the troposphere. On a time scale of a few days, the correlation is very good between the potential vorticity and the ozone time evolution in the vicinity of the upper level frontal system

On the relationship between Arctic ice clouds and polluted air masses over the North Slope of Alaska in April 2008

Recently, two Types of Ice Clouds (TICs) properties have been characterized using ISDAC airborne measurements (Alaska, April 2008). TIC-2B were characterized by fewer (110 μm) ice crystals, a larger ice supersaturation (>15%) and a fewer ice nuclei (IN) concentration (<2 order of magnitude) when compared to TIC-1/2A. It has been hypothesized that emissions of SO2 may reduce the ice nucleating properties of IN through acidification, resulting to a smaller concentration of larger ice crystals and leading to precipitation (e.g. cloud regime TIC-2B) because of the reduced competition for the same available moisture. Here, the origin of air masses forming the ISDAC TIC-1/2A (1 April 2008) and TIC-2B (15 April 2008) is investigated using trajectory tools and satellite data. Results show that the synoptic conditions favor air masses transport from the three potentials SO2 emission areas to Alaska: eastern China and Siberia where anthropogenic and biomass burning emission respectively are produced and the volcanic region from the Kamchatka/Aleutians. Weather conditions allow the accumulation of pollutants from eastern China/Siberia over Alaska, most probably with the contribution of acid volcanic aerosol during the TIC-2B period. OMI observations reveal that SO2 concentrations in air masses forming the TIC-2B were larger than in air masses forming the TIC-1/2A. Airborne measurements show high acidity near the TIC-2B flight where humidity was low. These results strongly support the hypothesis that acidic coating on IN are at the origin of the formation of TIC-2B

Effects of regional-scale and convective transports on tropospheric ozone chemistry revealed by aircraft observations during the wet season of the AMMA campaign

The African Monsoon Multidisciplinary Analyses (AMMA) fourth airborne campaign was conducted in July–August 2006 to study the chemical composition of the middle and upper troposphere in West Africa with the major objective to better understand the processing of chemical emissions by the West African Monsoon (WAM) and its associated regional-scale and vertical transports. In particular, the french airborne experiment was organized around two goals. The first was to characterize the impact of Mesoscale Convective Systems (MCSs) on the ozone budget in the upper troposphere and the evolution of the chemical composition of these convective plumes as they move westward toward the Atlantic Ocean. The second objective was to discriminate the impact of remote sources of pollution over West Africa, including transport from the middle east, Europe, Asia and from southern hemispheric fires. Observations of O&lt;sub&gt;3&lt;/sub&gt;, CO, NO&lt;sub&gt;x&lt;/sub&gt;, H&lt;sub&gt;2&lt;/sub&gt;O and hydroperoxide above West Africa along repeated meridional transects were coupled with transport analysis based on the FLEXPART lagrangian model. The cross analysis of trace gas concentrations and transport pathways revealed 5 types of air masses: convective uplift of industrial and urban emissions, convective uplift of biogenic emissions, slow advection from Cotonou polluted plumes near the coast, meridional transport of upper tropospheric air from the subtropical barrier region, and meridional transport of Southern Hemisphere (SH) biomass burning emissions. O&lt;sub&gt;3&lt;/sub&gt;/CO correlation plots and the correlation plots of H&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt; with a OH proxy revealed not only a control of the trace gas variability by transport processes but also significant photochemical reactivity in the mid- and upper troposphere. The study of four MCSs outflow showed contrasted chemical composition and air mass origins depending on the MCSs lifetime and latitudinal position. Favorables conditions for ozone production were found for MCSs with increased MCS lifetime (&amp;gt;1.5 days), which allowed for more H&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt; formation, and with trajectories crossing the 10&amp;deg; N latitude, which increased CO transport to the upper troposphere. The upper tropospheric concentrations sampled in the MCS outflow regions showed mixed origins including local vertical convective transport, and uplifting of air from the low troposphere over the middle-east related to the summer Asian low pressure system or from the southern hemispheric fires

Anthropogenic and forest fire pollution aerosol transported to the Arctic: observations from the POLARCAT-France spring campaign

During the POLARCAT-France airborne measurement campaign in spring 2008, several pollution plumes transported from mid-latitude regions were encountered. The study presented here focuses on air masses from two different geographic origins (Europe and Asia) and from 2 different source types (anthropogenic pollution and forest fires). One case study analyses an European air mass, which was sampled during three consecutive day. Modelling of the aerosol particle ageing by coagulation suggests that coagulation cannot solely explain the evolution of the size distributions, which is particularly true for the accumulation mode. Analyses of the aerosol refractory size distributions indicate that the Aitken mode was mostly composed of volatile compounds, while accumulation mode particles desorbed to a refractory mode yielding a modal mean diameter evolving from 48 to 59 nm for the three consecutive days of sampling the same air mass. The single refractory mode suggests an internally mixed aerosol population which is supported from electron microscopy and subsequent EDX analyses of the accumulation mode particles. Another case study focuses on European air masses polluted by fire emissions and Asian air masses with contributions from both biomass burning and anthropogenic emissions. On the one hand, the aerosol size distributions of the European biomass burning plumes are almost mono-modal with most of the particles found in the aged accumulation mode which desorbed uniformly. On the other hand, Asian air masses were more complex because of the mixing of different source contributions related to more variable and multimodal ambient and refractory aerosol size distributions. Electron microscopy illustrated soot-like inclusions in several samples. Within samples attributed to forest fire sources, the chemical signature is highly associated with the presence of potassium, which is characteristic for biomass burning plumes. The particle images suggest an internal mixing of sampled aerosol particles