Analysis of ozone and nitric acid in spring and summer Arctic pollution using aircraft, ground-based, satellite observations and MOZART-4 model: source attribution and partitioning

In this paper, we analyze tropospheric O_3 together with HNO_3 during the POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols, and Transport) program, combining observations and model results. Aircraft observations from the NASA ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) and NOAA ARCPAC (Aerosol, Radiation and Cloud Processes affecting Arctic Climate) campaigns during spring and summer of 2008 are used together with the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4) to assist in the interpretation of the observations in terms of the source attribution and transport of O_3 and HNO_3 into the Arctic (north of 60° N). The MOZART-4 simulations reproduce the aircraft observations generally well (within 15%), but some discrepancies in the model are identified and discussed. The observed correlation of O_3 with HNO_3 is exploited to evaluate the MOZART-4 model performance for different air mass types (fresh plumes, free troposphere and stratospheric-contaminated air masses). Based on model simulations of O_3 and HNO_3 tagged by source type and region, we find that the anthropogenic pollution from the Northern Hemisphere is the dominant source of O3 and HNO3 in the Arctic at pressures greater than 400 hPa, and that the stratospheric influence is the principal contribution at pressures less 400 hPa. During the summer, intense Russian fire emissions contribute some amount to the tropospheric columns of both gases over the American sector of the Arctic. North American fire emissions (California and Canada) also show an important impact on tropospheric ozone in the Arctic boundary layer. Additional analysis of tropospheric O_3 measurements from ground-based FTIR and from the IASI satellite sounder made at the Eureka (Canada) and Thule (Greenland) polar sites during POLARCAT has been performed using the tagged contributions. It demonstrates the capability of these instruments for observing pollution at northern high latitudes. Differences between contributions from the sources to the tropospheric columns as measured by FTIR and IASI are discussed in terms of vertical sensitivity associated with these instruments. The first analysis of O_3 tropospheric columns observed by the IASI satellite instrument over the Arctic is also provided. Despite its limited vertical sensitivity in the lowermost atmospheric layers, we demonstrate that IASI is capable of detecting low-altitude pollution transported into the Arctic with some limitations

Measurements of hydrogen cyanide (HCN) and acetylene (C2H2) from the Infrared Atmospheric Sounding Interferometer (IASI)

Hydrogen cyanide (HCN) and acetylene (C2H2) are ubiquitous atmospheric trace gases with medium lifetime, which are frequently used as indicators of combustion sources and as tracers for atmospheric transport and chemistry. Because of their weak infrared absorption, overlapped by the CO2 Q branch near 720 cm−1, nadir sounders have up to now failed to measure these gases routinely. Taking into account CO2 line mixing, we provide for the first time extensive measurements of HCN and C2H2 total columns at Reunion Island (21° S, 55° E) and Jungfraujoch (46° N, 8° E) in 2009–2010 using observations from the Infrared Atmospheric Sounding Interferometer (IASI). A first order comparison with local ground-based Fourier transform InfraRed (FTIR) measurements has been carried out allowing tests of seasonal consistency which is reasonably captured, except for HCN at Jungfraujoch. The IASI data shows a greater tendency to high C2H2 values. We also examine a nonspecific biomass burning plume over austral Africa and show that the emission ratios with respect to CO agree with previously reported values

The influence of boreal biomass burning emissions on the distribution of tropospheric ozone over North America and the North Atlantic during 2010

We have analysed the sensitivity of the tropospheric ozone distribution over North America and the North Atlantic to boreal biomass burning emissions during the summer of 2010 using the GEOS-Chem 3-D global tropospheric chemical transport model and observations from in situ and satellite instruments. We show that the model ozone distribution is consistent with observations from the Pico Mountain Observatory in the Azores, ozonesondes across Canada, and the Tropospheric Emission Spectrometer (TES) and Infrared Atmospheric Sounding Instrument (IASI) satellite instruments. Mean biases between the model and observed ozone mixing ratio in the free troposphere were less than 10 ppbv. We used the adjoint of GEOS-Chem to show the model ozone distribution in the free troposphere over Maritime Canada is largely sensitive to NO<sub>x</sub> emissions from biomass burning sources in Central Canada, lightning sources in the central US, and anthropogenic sources in the eastern US and south-eastern Canada. We also used the adjoint of GEOS-Chem to evaluate the Fire Locating And Monitoring of Burning Emissions (FLAMBE) inventory through assimilation of CO observations from the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument. The CO inversion showed that, on average, the FLAMBE emissions needed to be reduced to 89% of their original values, with scaling factors ranging from 12% to 102%, to fit the MOPITT observations in the boreal regions. Applying the CO scaling factors to all species emitted from boreal biomass burning sources led to a decrease of the model tropospheric distributions of CO, PAN, and NO<sub>x</sub> by as much as −20 ppbv, −50 pptv, and −20 pptv respectively. The modification of the biomass burning emission estimates reduced the model ozone distribution by approximately −3 ppbv (−8%) and on average improved the agreement of the model ozone distribution compared to the observations throughout the free troposphere, reducing the mean model bias from 5.5 to 4.0 ppbv for the Pico Mountain Observatory, 3.0 to 0.9 ppbv for ozonesondes, 2.0 to 0.9 ppbv for TES, and 2.8 to 1.4 ppbv for IASI

The influence of boreal biomass burning emissions on the distribution of tropospheric ozone over North America and the North Atlantic during 2010

We have analysed the sensitivity of the tropospheric ozone distribution over North America and the North Atlantic to boreal biomass burning emissions during the summer of 2010 using the GEOS-Chem 3-D global tropospheric chemical transport model and observations from in situ and satellite instruments. We show that the model ozone distribution is consistent with observations from the Pico Mountain Observatory in the Azores, ozonesondes across Canada, and the Tropospheric Emission Spectrometer (TES) and Infrared Atmospheric Sounding Instrument (IASI) satellite instruments. Mean biases between the model and observed ozone mixing ratio in the free troposphere were less than 10 ppbv. We used the adjoint of GEOS-Chem to show the model ozone distribution in the free troposphere over Maritime Canada is largely sensitive to NOx emissions from biomass burning sources in Central Canada, lightning sources in the central US, and anthropogenic sources in the eastern US and south-eastern Canada. We also used the adjoint of GEOS-Chem to evaluate the Fire Locating And Monitoring of Burning Emissions (FLAMBE) inventory through assimilation of CO observations from the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument. The CO inversion showed that, on average, the FLAMBE emissions needed to be reduced to 89% of their original values, with scaling factors ranging from 12% to 102%, to fit the MOPITT observations in the boreal regions. Applying the CO scaling factors to all species emitted from boreal biomass burning sources led to a decrease of the model tropospheric distributions of CO, PAN, and NOx by as much as -20 ppbv, -50 pptv, and -20 pptv respectively. The modification of the biomass burning emission estimates reduced the model ozone distribution by approximately -3 ppbv (-8%) and on average improved the agreement of the model ozone distribution compared to the observations throughout the free troposphere, reducing the mean model bias from 5.5 to 4.0 ppbv for the Pico Mountain Observatory, 3.0 to 0.9 ppbv for ozonesondes, 2.0 to 0.9 ppbv for TES, and 2.8 to 1.4 ppbv for IASI

An examination of the long-term CO records from MOPITT and IASI: comparison of retrieval methodology

International audienceCarbon monoxide (CO) is a key atmospheric compound that can be remotely sensed by satellite on the global scale. Fifteen years of continuous observations are now available from the MOPITT/Terra mission (2000 to present). Another fifteen and more years of observations will be provided by the IASI/MetOp instrument series (2007–2023>). In order to study long term variability and trends, a homogeneous record is required, which is not straightforward as the retrieved products are instrument and processing dependent. The present study aims at evaluating the consistency between the CO products derived from the MOPITT and IASI missions, both for total columns and vertical profiles, during a six year overlap period (2008–2013). The analysis is performed by first comparing the available 2013 versions of the retrieval algorithms, and second using a dedicated reprocessing of MOPITT CO profiles and columns based on the IASI a priori constraints. MOPITT v5T total columns are generally slightly higher over land (bias ranging from 0 to 13%) than IASI v20100815 data. When IASI and MOPITT data are retrieved with the same a priori constraints, correlation coefficients are slightly improved. Large discrepancies (total column bias over 15%) observed in the Northern Hemisphere during the winter months are reduced by a factor of 2 to 2.5. The detailed analysis of retrieved vertical profiles compared with collocated aircraft data from the MOZAIC-IAGOS network, illustrates the advantages and disadvantages of a constant vs. a variable a priori. On one hand, MOPITT agrees better with the aircraft profiles for observations with persisting high levels of CO throughout the year due to pollution or seasonal fire activity (because the climatology-based a priori is supposed to be closer to the real atmospheric state). On the other hand, IASI performs better when unexpected events leading to high levels of CO occur, due to the less constrained variance-covariance matrix

Acetylene (C2H2) and hydrogen cyanide (HCN) from IASI satellite observations: Global distributions, validation, and comparison with model

We present global distributions of C$_{2}$H$_{2}$ and hydrogen cyanide (HCN) total columns derived from the Infrared Atmospheric Sounding Interferometer (IASI) for the years 2008–2010. These distributions are obtained with a fast method allowing to retrieve C$_{2}$H$_{2}$ abundance globally with a 5% precision and HCN abundance in the tropical (subtropical) belt with a 10% (25 %) precision. IASI data are compared for validation purposes with ground-based Fourier transform infrared (FTIR) spectrometer measurements at four selected stations.We show that there is an overall agreement between the ground-based and space measurements with correlation coefficients for daily mean measurements ranging from 0.28 to 0.81, depending on the site. Global C$_{2}$H$_{2}$ and subtropical HCN abundances retrieved from IASI spectra show the expected seasonality linked to variations in the anthropogenic emissions and seasonal biomass burning activity, as well as exceptional events, and are in good agreement with previous spaceborne studies. Total columns simulated by the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4) are compared to the ground-based FTIR measurements at the four selected stations. The model is able to capture the seasonality in the two species in most of the cases, with correlation coefficients for daily mean measurements ranging from 0.50 to 0.86, depending on the site. IASI measurements are also compared to the distributions from MOZART-4. Seasonal cycles observed from satellite data are reasonably well reproduced by the model with correlation coefficients ranging from -0.31 to 0.93 for C$_{2}$H$_{2}$ daily means, and from 0.09 to 0.86 for HCN daily means, depending on the considered region. However, the anthropogenic (biomass burning) emissions used in the model seem to be overestimated (underestimated), and a negative global mean bias of 1% (16 %) of the model relative to the satellite observations was found for C$_{2}$H$_{2}$ (HCN)

Validation of the IASI FORLI/EUMETSAT ozone products using satellite (GOME-2), ground-based (Brewer–Dobson, SAOZ, FTIR) and ozonesonde measurements

This paper assesses the quality of IASI (Infrared Atmospheric Sounding Interferometer)/Metop-A (IASI-A) and IASI/Metop-B (IASI-B) ozone (O3) products (total and partial O3 columns) retrieved with the Fast Optimal Retrievals on Layers for IASI Ozone (FORLI-O3; v20151001) software for 9 years (2008–July 2017) through an extensive intercomparison and validation exercise using independent observations (satellite, ground-based and ozonesonde). Compared with the previous version of FORLI-O3 (v20140922), several improvements have been introduced in FORLI-O3 v20151001, including absorbance look-up tables recalculated to cover a larger spectral range, with additional numerical corrections. This leads to a change of  ∼ 4&thinsp;% in the total ozone column (TOC) product, which is mainly associated with a decrease in the retrieved O3 concentration in the middle stratosphere (above 30&thinsp;hPa/25&thinsp;km). IASI-A and IASI-B TOCs are consistent, with a global mean difference of less than 0.3&thinsp;% for both daytime and nighttime measurements; IASI-A is slightly higher than IASI-B. A global difference of less than 2.4&thinsp;% is found for the tropospheric (TROPO) O3 column product (IASI-A is lower than IASI-B), which is partly due to a temporary issue related to the IASI-A viewing angle in 2015. Our validation shows that IASI-A and IASI-B TOCs are consistent with GOME-2 (Global Ozone Monitoring Experiment-2), Dobson, Brewer, SAOZ (Système d'Analyse par Observation Zénithale) and FTIR (Fourier transform infrared) TOCs, with global mean differences in the range of 0.1&thinsp;%–2&thinsp;% depending on the instruments compared. The worst agreement with UV–vis retrieved TOC (satellite and ground) is found at the southern high latitudes. The IASI-A and ground-based TOC comparison for the period from 2008 to July 2017 shows the long-term stability of IASI-A, with insignificant or small negative drifts of 1&thinsp;%–3&thinsp;%&thinsp;decade−1. The comparison results of IASI-A and IASI-B against smoothed FTIR and ozonesonde partial O3 columns vary with altitude and latitude, with the maximum standard deviation being seen for the 300–150&thinsp;hPa column (20&thinsp;%–40&thinsp;%) due to strong ozone variability and large total retrievals errors. Compared with ozonesonde data, the IASI-A and IASI-B O3 TROPO column (defined as the column between the surface and 300&thinsp;hPa) is positively biased in the high latitudes (4&thinsp;%–5&thinsp;%) and negatively biased in the midlatitudes and tropics (11&thinsp;%–13&thinsp;% and 16&thinsp;%–19&thinsp;%, respectively). The IASI-A-to-ozonesonde TROPO comparison for the period from 2008 to 2016 shows a significant negative drift in the Northern Hemisphere of −8.6±3.4&thinsp;%&thinsp;decade−1, which is also found in the IASI-A-to-FTIR TROPO comparison. When considering the period from 2011 to 2016, the drift value for the TROPO column decreases and becomes statistically insignificant. The observed negative drifts of the IASI-A TROPO O3 product (8&thinsp;%–16&thinsp;%&thinsp;decade−1) over the 2008–2017 period might be taken into consideration when deriving trends from this product and this time period.</p

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