Search

Ozone is a potent air pollutant in the lower troposphere and an important short-lived climate forcer (SLCF) in the upper troposphere. Studies investigating long-term trends in the tropospheric column ozone (TCO 3) have shown large-scale spatio-temporal inconsistencies. Here, we investigate the long-term trends in lower-tropospheric column ozone (LTCO 3 , surface–450 hPa sub-column) by exploiting a synergy of satellite and ozonesonde data sets and an Earth system model (UK's Earth System Model, UKESM) over North America, Europe, and East Asia for the decade 2008–2017. Overall, we typically find small LTCO 3 linear trends with large uncertainty ranges using the Ozone Monitoring Instrument (OMI) and the Infrared Atmospheric Sounding Interferometer (IASI), while model simulations indicate a stable LTCO 3 tendency. The satellite a priori data sets show negligible trends, indicating that any year-to-year changes in the spatio-temporal sampling of these satellite data sets over the period concerned have not artificially influenced their LTCO 3 temporal evolution. The application of the satellite averaging kernels (AKs) to the UKESM simulated ozone profiles, accounting for the satellite vertical sensitivity and allowing for like-for-like comparisons, has a limited impact on the modelled LTCO 3 tendency in most cases. While, in relative terms, this is more substantial (e.g. on the order of 100 %), the absolute magnitudes of the model trends show negligible change. However, as the model has a near-zero tendency, artificial trends were imposed on the model time series (i.e. LTCO 3 values rearranged from smallest to largest) to test the influence of the AKs, but simulated LTCO 3 trends remained small. Therefore, the LTCO 3 tendencies between 2008 and 2017 in northern-hemispheric regions are likely to be small, with large uncertainties, and it is difficult to detect any small underlying linear trends due to interannual variability or other factors which require further investigation (e.g. the radiative transfer scheme (RTS) used and/or the inputs (e.g. meteorological fields) used in the RTS). [ABSTRACT FROM AUTHOR]

Using state-of-the-art satellite ozone profile products, and a chemical transport model, we provide an updated estimate of the tropospheric ozone radiative effect (TO 3 RE) and observational constraint on its variability over the decade 2008–2017. Previous studies have shown the short-term (i.e. a few years) globally weighted average TO 3 RE to be 1.17 ± 0.03 W m -2. However, from our analysis, using decadal (2008–2017) ozone profile datasets from the Infrared Atmospheric Sounding Interferometer, average TO 3 RE ranges between 1.21 and 1.26 W m -2. Over this decade, the modelled and observational TO 3 RE linear trends show a negligible change (e.g. ± 0.1 % yr -1). Two model sensitivity experiments fixing emissions and meteorology to 1 year (i.e. start year – 2008) show that temporal changes in ozone precursor emissions (increasing contribution) and meteorological factors (decreasing contribution) have counteracting tendencies, leading to a negligible globally weighted average TO 3 RE trend. [ABSTRACT FROM AUTHOR]

Ozone is a potent air pollutant in the lower troposphere and an important short-lived climate forcer (SLCF) in the upper troposphere. Studies investigating long-term trends in tropospheric column ozone (TCO3) have shown large-scale spatiotemporal inconsistencies. Here, we investigate the long-term trends in lower tropospheric column ozone (LTCO3, surface-450 hPa sub-column) by exploiting a synergy of satellite and ozonesonde datasets and an Earth System Model (UKESM) over North America, Europe and East Asia for the decade 2008–2017. Overall, we typically find small LTCO3 linear trends with large uncertainty ranges from the Ozone Monitoring Instrument (OMI) and the Infrared Atmospheric Sounding Interferometer (IASI), while model simulations indicate a stable LTCO3 tendency. Trends in the satellite a priori datasets show negligible trends indicating year-to-year sampling is not an issue. The application of the satellite averaging kernels (AKs) to the UKESM ozone profiles, accounting for the satellite vertical sensitivity and allowing for like-for-like comparisons, has a limited impact on the modelled LTCO3 tendency in most cases. While, in relative terms, this is more substantial (e.g. in the order of 100 %), the absolute magnitudes of the model trends show negligible change. However, as the model has a near-zero tendency, artificial trends were imposed on the model time-series (i.e. LTCO3 values rearranged from smallest to largest) to test the influence of the AKs but simulated LTCO3 trends remained small. Therefore, the LTCO3 tendency between 2008 and 2017 in northern hemispheric regions are likely small, with large uncertainties, and it is difficult to detect any small underlying linear trends due to inter-annual variability or other factors which require further investigation. [ABSTRACT FROM AUTHOR]

Using state-of-the-art satellite ozone profile products, and chemical transport model, we provide an updated estimate of the tropospheric ozone radiative effect (TO3RE) and observational constraint on its variability over the decade 2008–2017. Previous studies have shown the short-term (i.e. a few years) globally weighted average TO3RE to be 1.17±0.03 W/m2, while our analysis suggests that the long-term (2008–2017) average TO3RE to be 1.21–1.28 W/m2. Over this decade, the modelled/observational TO3RE linear trends show negligible change (i.e. ±0.1 %/year), so the tropospheric ozone radiative contribution to climate has remained stable with time. Two model sensitivity experiments fixing emissions and meteorology to one year (i.e. start year – 2008) show that ozone precursor emissions (meteorological factors) have had limited (substantial) impacts on the long-term tendency of globally weighted average TO3RE. Here, the meteorological variability in the tropical/sub-tropical upper troposphere is dampening any tendency in TO3RE from other factors (e.g. emissions, atmospheric chemistry). [ABSTRACT FROM AUTHOR]

The MetOp/Infrared Atmospheric Sounding Interferometer (IASI) instruments have provided data for operational meteorology and document atmospheric composition since 2007. IASI ozone (O3) data have been used extensively to characterize the seasonal and interannual variabilities and the evolution of tropospheric O3 at the global scale. SOftware for a Fast Retrieval of IASI Data (SOFRID) is a fast retrieval algorithm that provides IASI O3 profiles for the whole IASI period. Until now, SOFRID O3 retrievals (v1.5 and v1.6) were performed with a single a priori profile, which resulted in important biases and probably a too-low variability. For the first time, we have implemented a comprehensive dynamical a priori profile for spaceborne O3 retrievals which takes the pixel location, time and tropopause height into account for SOFRID-O3 v3.5 retrievals. In the present study, we validate SOFRID-O3 v1.6 and v3.5 with electrochemical concentration cell (ECC) ozonesonde profiles from the global World Ozone and Ultraviolet Radiation Data Centre (WOUDC) database for the 2008–2017 period. Our validation is based on a thorough statistical analysis using Taylor diagrams. Furthermore, we compare our retrievals with ozonesonde profiles both smoothed by the IASI averaging kernels and raw. This methodology is essential to evaluate the inherent usefulness of the retrievals to assess O3 variability and trends. The use of a dynamical a priori profile largely improves the retrievals concerning two main aspects: (i) it corrects high biases for low-tropospheric O3 regions such as the Southern Hemisphere, and (ii) it increases the retrieved O3 variability, leading to a better agreement with ozonesonde data. Concerning upper troposphere–lower stratosphere (UTLS) and stratospheric O3 , the improvements are less important and the biases are very similar for both versions. The SOFRID tropospheric ozone columns (TOCs) display no significant drifts (<2.5 %) for the Northern Hemisphere and significant negative ones (9.5 % for v1.6 and 4.3 % for v3.5) for the Southern Hemisphere. We have compared our validation results to those of the Fast Optimal Retrievals on Layers for IASI (FORLI) retrieval software from the literature for smoothed ozonesonde data only. This comparison highlights three main differences: (i) FORLI retrievals contain more theoretical information about tropospheric O3 than SOFRID; (ii) root mean square differences (RMSDs) are smaller and correlation coefficients are higher for SOFRID than for FORLI; (iii) in the Northern Hemisphere, the 2010 jump detected in FORLI TOCs is not present in SOFRID. [ABSTRACT FROM AUTHOR]

The Metop/IASI instruments provide data for operational meteorology and document atmospheric composition since 2007. IASI Ozone (O3) data have been used extensively to characterize the seasonal and interrannual variabilities and the evolution of tropospheric O3 at the global scale. The SOFRID (SOftware for a Fast Retrieval of IASI Data) is a fast retrieval algorithm that provides IASI O3 profiles for the whole IASI period. Up to now SOFRID O3 retrievals (v1.5 and 1.6) were performed with a single a priori profile which resulted in important biases and probably a too low variability. For the first time we have implemented a dynamical a priori profile for spaceborne O3 retrievals which takes the pixel location, time and tropopause height into account for SOFRID-O3 v3.5 retrievals. In the present study we validate SOFRID-O3 v1.6 and v3.5 with ECC ozonesonde profiles from the global WOUDC database for the 2008–2017 period. Our validation is based on a thorough statistical analysis using Taylor diagrams. Furthermore we compare our retrievals with ozonesonde profiles both smoothed by the IASI averaging kernels and raw. This methodology is essential to evaluate the inherent usefulness of the retrievals to assess O3 variability and trends. The use of a dynamical a priori largely improves the retrievals concerning two main aspects: (i) it corrects high biases for low-tropospheric O3 regions such as the southern hemisphere (ii) it increases the retrieved O3 variability leading to a better agreement with ozonesonde data. Concerning UTLS and stratospheric O3 the improvements are less important and the biases are very similar for both versions. The SOFRID Tropospheric Ozone Columns (TOC) display no significant drifts (< 2.5 %) for the northern hemisphere and significant negative ones (9.5 % for v1.6 and 4.3 % for v3.5) for the southern hemisphere. We have compared our validation results to those of the FORLI retrieval software from the literature for smoothed ozonesonde data only. This comparison highlights three main differences: (i) FORLI retrievals contain more theoretical information about tropospheric O3 than SOFRID (ii) RMSDs are smaller and correlation coefficients are higher for SOFRID than for FORLI (iii) in the northern hemisphere, no significant temporal drift is detected in SOFRID contrarily to FORLI (∼ 8 %). [ABSTRACT FROM AUTHOR]

The prior information used for Level 2 (L2) retrievals in the thermal infrared can influence the quality of the retrievals themselves and, therefore, their further assimilation in atmospheric composition models. In this study we evaluate the differences between assimilating L2 ozone profiles and Level 1 (L1) radiances from the Infrared Atmospheric Sounding Interferometer (IASI). We minimized potential differences between the two approaches by employing the same radiative transfer code (Radiative Transfer for TOVS, RTTOV) and a very similar setup for both the L2 retrievals (1D-Var) and the L1 assimilation (3D-Var). We computed hourly 3D-Var analyses assimilating L1 and L2 data in the chemical transport model MOCAGE and compared the resulting O3 fields among each other and against ozonesondes. We also evaluated the joint assimilation of limb measurements from the Microwave Limb Sounder (MLS) in combination with IASI to assess the impact of stratospheric O3 on tropospheric analyses. Results indicate that significant differences can arise between L2 and L1 assimilation, especially in regions where the L2 prior information is strongly biased (at low latitudes in this study). In these regions the L1 assimilation provides a better variability of the free-troposphere ozone column. L1 and L2 assimilation instead give very similar results at high latitudes, especially when MLS measurements are used to constrain the stratospheric O3 column. A critical analysis of the potential benefits and drawbacks of L1 assimilation is given in the conclusions. We also list remaining issues that are common to both the L1 and L2 approaches and that deserve further research. [ABSTRACT FROM AUTHOR]

We have used ozone data from the Infrared Atmospheric Sounding Interferometer to follow an event of ozoneenriched air-masses in the upper troposphere from eastern Africa to northern India. The ozone transport (hereafter called 'ozone river' or O3R) occurred during the Asian post-monsoon season in 2008 and was associated with Rossby wave propagation. The persistence of the O3R in a narrow channel was confirmed by MOZAIC airborne data over the northwestern Indian coast. The regions of origin of the O3R were identified by a transport analysis based on the Lagrangian model FLEXPART. The Lagrangian simulations combined with potential vorticity fields indicate that stratospheric intrusions are not likely to be the most important contributor to the observed O3 enhancements. A high-resolution Eulerian model, Meso-NH, with tagged tracers was used to discriminate between African biomass burning, lightnings and Indian anthropogenic pollution as potential sources of precursors for the O3R. Lightning NOx emissions, associated with convective clouds over Africa, were found to be the principal contributor to the ozone enhancement over the Indian Ocean taking advantage of a northeastward jet. This case study illustrates African lightning emissions as an important source for enhanced O3 in the upper troposphere over the Indian Ocean region during the post-monsoon season. [ABSTRACT FROM AUTHOR]

We have used ozone data from the Infrared Atmospheric Sounding Interferometer to follow an event of ozone-enriched air-masses in the upper troposphere from eastern Africa to northern India. The ozone transport (hereafter called 'ozone river' or O3R) occurred during the Asian post-monsoon season in 2008 and was associated with Rossby wave propagation. The persistence of the O3R in a narrow channel was confirmed by MOZAIC airborne data over the northwestern Indian coast. The regions of origin of the O3R were identified by a transport analysis based on the Lagrangian model FLEXPART. The Lagrangian simulations combined with potential vorticity fields indicate that stratospheric intrusions are not likely to be the most important contributor to the observed O3 enhancements. A high-resolution Eulerian model, Meso-NH, with tagged tracers was used to discriminate between African biomass burning, lightnings and Indian anthropogenic pollution as potential sources of precursors for the O3R. Lightning NOx emissions, associated with convective clouds over Africa, were found to be the principal contributor to the ozone enhancement over the Indian Ocean taking advantage of a northeastward jet. This case study illustrates African lightning emissions as an important source for enhanced O3 in the upper troposphere over the Indian Ocean region during the post-monsoon season. [ABSTRACT FROM AUTHOR]