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The Alaskan Layered Pollution And Chemical Analysis (ALPACA) field experiment was a collaborative study designed to improve understanding of pollution sources and chemical processes during winter (cold climate and low-photochemical activity), to investigate indoor pollution, and to study dispersion of pollution as affected by frequent temperature inversions. A number of the research goals were motivated by questions raised by residents of Fairbanks, Alaska, where the study was held. This paper describes the measurement strategies and the conditions encountered during the January and February 2022 field experiment, and reports early examples of how the measurements addressed research goals, particularly those of interest to the residents. Outdoor air measurements showed high concentrations of particulate matter and pollutant gases including volatile organic carbon species. During pollution events, low winds and extremely stable atmospheric conditions trapped pollution below 73 m, an extremely shallow vertical scale. Tethered-balloon-based measurements intercepted plumes aloft, which were associated with power plant point sources through transport modeling. Because cold climate residents spend much of their time indoors, the study included an indoor air quality component, where measurements were made inside and outside a house to study infiltration and indoor sources. In the absence of indoor activities such as cooking and/or heating with a pellet stove, indoor particulate matter concentrations were lower than outdoors; however, cooking and pellet stove burns often caused higher indoor particulate matter concentrations than outdoors. The mass-normalized particulate matter oxidative potential, a health-relevant property measured here by the reactivity with dithiothreiol, of indoor particles varied by source, with cooking particles having less oxidative potential per mass than pellet stove particles.

Lagrangian tracer simulations are deployed to investigate processes influencing vertical and horizontal dispersion of anthropogenic pollution in Fairbanks, Alaska, during the ALPACA-2022 field campaign. Simulations of carbon monoxide (CO), sulphur dioxide (SO2) and nitrogen oxides (NOx), including surface and elevated emissions, are highest at the surface under very cold stable conditions. Regional enhancements, simulated up to 200 m, are due to elevated power plant emissions above 50 m, with south-westerly pollutant outflow. Fairbanks regional pollution may be contributing to wintertime Arctic haze. Inclusion of a novel power plant plume rise treatment that considers the presence of surface and elevated temperature inversion layers leads to improved agreement with observed CO and NOx plumes with discrepancies attributed to, for example, displacement of plumes by modelled winds. At the surface, model results show that observed CO variability is largely driven by meteorology and to a lesser extent by emissions, although simulated tracers are sensitive to modelled vertical dispersion. Modelled underestimation of surface NOx during very cold polluted conditions is considerably improved following the inclusion of substantial increases in diesel vehicle NOx emissions at cold temperatures (e.g. a factor of 6 at -30 °C). In contrast, overestimation of surface SO2 is attributed to issues related to the vertical dispersion of elevated space heating emissions during strongly and weakly stable conditions. This study highlights the need for improvements to local wintertime Arctic anthropogenic surface and elevated emissions and improved simulation of Arctic stable boundary layers. [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]

IASI-A, B and C (Infrared Atmospheric Sounding Interferometer) are nadir looking thermal infrared sensors which are monitoring the atmospheric composition since 2008. Atmospheric Carbon monoxide (CO) is retrieved from IASI radiances with two algorithms: the SOftware for a Fast Retrieval of IASI Data (SOFRID) and the Fast Optimal Retrievals on Layers for IASI (FORLI). The airborne in-situ observations from the In-service Aircraft for a Global Observing System (IAGOS) European Research Infrastructure have been used to validate the IASI CO retrievals. The validation study of IASI CO data performed in 2011 whith IAGOS data was limited to two airports (Frankfurt and Windhoek) and 2 years because of the limited sampling at the other IAGOS sites. The extension of the IAGOS infrastructure during the last decade enables a validation with enough temporal sampling at 33 airports worldwide over the whole IASI-A period (2008–2020). The retrievals provide between 1.5 and 3 independent pieces of information about the CO vertical profile and we have selected to validate the surface-600 hPa and 600–200 hPa partial columns in addition to the total column. The ability of the retrievals to capture the CO variabilities is slightly different for the two retrieval algorithms. The correlation coefficients are generally larger for SOFRID, especially for the total and lower tropospheric columns, meaning a better representation of the phase of the variability, while the amplitude of the variations of FORLI are in better agreement with IAGOS in the mid-upper troposphere. On average SOFRID and FORLI retrievals are underestimating the IAGOS total columns of CO (TCC) by 8±16 % and 6±14 % respectively. This global TCC agreement between the algorithms is hiding significant vertical and geographical differences. In the lower troposphere (Surface-600 hPa) the bias is larger for FORLI (-11±27 %) than for SOFRID (-4±24 %). In the mid-upper troposphere the situation is reversed with a bias of -6±15 % for FORLI and of -11±13 % for SOFRID. The largest differences between the retrievals are detected south of Bangkok where SOFRID underestimation is systematically larger for the TCC and mid-upper tropospheric column. North of Philadelphia FORLI biases are significantly larger than SOFRID ones for the TCC and the lower tropospheric columns. Our validation results will provide a better characterisation of IASI-CO data to the users and help improve the retrievals for future versions. [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]

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-for41 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]

The characteristics and seasonal variability in the tropical tropospheric distributions of ozone (O3) and carbon monoxide (CO) were analysed based on in situ measurements provided by the In-service Aircraft for a Global Observing System (IAGOS) programme since 1994 and 2002, respectively, combined with observations from the Infrared Atmospheric Sounding (IASI) instrument on board the MetOp-A satellite since 2008. The SOFT-IO (SOft attribution using FlexparT and carbon monoxide emission inventories for In-situ Observation database) model, which couples back trajectories with CO emission inventories, was used to explore the origins and sources of the tropical CO observed by IAGOS. The highest O3 and CO mixing ratios occur over western Africa in the lower troposphere (LT: surface to 750 hPa) during the fire season (75 ppb of O3 at 2.5 km and 850 ppb of CO at 0.3 km over Lagos in January), mainly due to anthropogenic (AN) emissions and a major contribution from fires. The secondary maxima are observed in Asia in the mid-troposphere (MT: 750–300 hPa) and upper troposphere (UT: 300–200 hPa) in April for O3 and in the LT in January for CO , with larger contributions from AN emissions. The lowest O3 and CO mixing ratios occur over Caracas. In the tropical LT, the majority of the location clusters are affected by local and regional AN emissions. The highest AN impact is found over Asia, Arabia and eastern Africa, and South America (>75 % of CO). Biomass burning (BB) emissions also originate from local or regional sources but with stronger seasonal dependence. The highest BB impact is found over southern tropical Africa (57 %–90 %), except in April, mostly due to local fires, but also from Northern Hemisphere Africa in January (45 %–73 %) and Southern Hemisphere South America in October (29 % over Windhoek). In the MT and UT, AN emissions are more important and dominate in the eastern part of the tropics (from the Middle East to Asia). BB contributions are more important than in the LT, especially from the African fires in January and July and from South East and equatorial Asia in April and October. The overall highest amount of CO is exported from Africa, with the main transport pathway from the dry-season African regions towards the wet-season ones. In contrast, the impact of the Asian emissions in the LT and MT is limited on a local or regional scale. The transport of polluted Asian air masses is important in the UT during the Asian summer monsoon and post-monsoon seasons, when convection is active. [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 characteristics and seasonal variability of the tropical tropospheric distributions of ozone (O3) and carbon monoxide (CO) were analysed based on in situ measurements provided by the In-service Aircraft for a Global Observing System (IAGOS) program since 1994 and 2002 respectively, combined with observations from the Infrared Atmospheric Sounding (IASI) instrument on board the Met-op A satellite since 2008. The SOFT-IO model, which couples back trajectories with CO emissions inventories, was used to explore the origins and sources of the tropical CO observed by IAGOS. The highest tropical O3 and CO maxima occur over Northern Hemisphere (NH) Africa in the low troposphere (LT) (80 ppb and 850 ppb respectively at 2.5 km over Lagos) during the dry season (January). Despite the active local fires, local anthropogenic (AN) emissions (60 %) are dominant for the CO, and consequently the O3 maxima. The importance of the local AN emissions are highlighted over Central Africa, as they cause a persistent polluted surface layer during the transition seasons (40 % in October and 86 % in April). The second highest O3 and CO maxima are observed over Asia. Local or regional Asian AN emissions cause the CO maximum in the LT (0.5 km) in January, and the O3 maximum in the free troposphere (at 6 km) in the post-monsoon season (April). South China is the only Asian site where O3 peaks in the LT (75 ppb at 2.5 km), due to local fires (30 %) in addition to the local (52 %) and regional (15 %) AN emissions. The highest amount of transported CO in the tropics originates from Africa. The main transport pathway is from the dry-season African regions towards the wet-season ones. Contributions from the NH Africa are found over Arabia and Eastern Africa (up to 70 %), and India (40 % in the mid (MT) and 60% in the upper (UT) troposphere) during the dry season. Transport towards NH South America is found all year long, with significant contributions in the MT and UT (30--40 % over Caracas on annual basis). In contrast, the impact of the Asian emissions in the LT and MT is limited on a local or regional scale. Export of polluted Asian air masses is important in the UT during the Asian summer monsoon and post-monsoon seasons, when convection is active. The AN Asian contributions are mostly found over Arabia and Eastern Africa (up to 80 %) during the Asian summer monsoon. During the post-monsoon, CO impacted by the Indonesian fires (resp. SouthEast Asian AN emissions) are transported towards Eastern Africa (64% and 16%) due to the Tropical Easterly Jet. The lowest O3 and CO levels are observed over South America, due to less strong local emissions in comparison to Asia and Africa. The only important CO and O3 enhancement is observed in the MT during the local fires (October), when O3 and precursors impacted by the local AN and fire emissions are trapped in an anticyclone and transported towards South Africa (5--10 ppb from SH and NH South America respectively). [ABSTRACT FROM AUTHOR]

The European Research Infrastructure IAGOS (In-service Aircraft for a Global Observing System) equips commercial aircraft with a system for measuring atmospheric composition. A range of essential climate variables and air quality parameters are measured throughout the flight, from take-off to landing, giving high resolution information in the vertical in the vicinity of international airports, and in the upper-troposphere/lower-stratosphere during the cruise phase of the flight. Six airlines are currently involved in the programme, achieving a quasi-global coverage under normal circumstances. During the COVID-19 crisis, many airlines were forced to ground their fleets due to a fall in passenger numbers and imposed travel restrictions. Deutsche Lufthansa, a partner in IAGOS since 1994 was able to operate a IAGOS-equipped aircraft during the COVID-19 lockdown, providing regular measurements of ozone and carbon monoxide at Frankfurt airport. The data form a snapshot of an unprecedented time in the 27 year time-series. In May 2020, we see a 39% increase in ozone near the surface with respect to the 26 year climatology, a magnitude similar to that of the 2003 heatwave. The anomaly in May is driven by an increase in ozone at nighttime which might be linked to the reduction of NO during the COVID-19 lockdowns. The anomaly diminishes with altitude becoming a slightly negative anomaly in the free troposphere. The ozone precursor carbon monoxide shows an 11% reduction in MAM near the surface. There is only a small reduction of CO in the free troposphere due to the impact of long-range transport on the CO from emissions in regions outside Europe. This is confirmed by IASI-SOFRID CO retrievals which display a clear drop of CO at 800 hPa over Europe in March but otherwise show little change to the abundance of CO in the free troposphere. [ABSTRACT FROM AUTHOR]

Between December 2005 and 2013, the In-service Aircraft for a Global Observing System (IAGOS) program produced almost daily in situ measurements of CO and O3 between Europe and southern Africa. IAGOS data combined with measurements from the IASI instrument onboard the Metop-A satellite (2008-2013) are used to characterize meridional distributions and seasonality of CO and O3 in the African upper troposphere (UT). The FLEXPART particle dispersion model and the SOFT-IO model which combines the FLEXPART model with CO emission inventories are used to explore the sources and origins of the observed transects of CO and O3. We focus our analysis on two main seasons: December to March (DJFM) and June to October (JJASO). These seasons have been defined according to the position of Intertropical Convergence Zone (ITCZ), determined using in situ measurements from IAGOS. During both seasons, the UT CO meridional transects are characterized by maximum mixing ratios located 10° from the position of the ITCZ above the dry regions inside the hemisphere of the strongest Hadley cell (132 to 165 ppb at 0-5° N in DJFM and 128 to 149 ppb at 3-7° S in JJASO), and decreasing values south- and north-ward. The O3 meridional transects are characterized by mixing ratio minima of ~ 42-54 ppb at the ITCZ (10-16° S in DJFM and 5-8° N in JJASO) framed by local maxima (~ 53-71 ppb) coincident with the wind shear zones North and South of the ITCZ. O3 gradients are strongest in the hemisphere of the strongest Hadley cell. IASI UT O3 distributions in DJFM have revealed that the maxima are a part of a crescent-shaped O3 plume above the Atlantic Ocean around the Gulf of Guinea. CO emitted at the surface is transported towards the ITCZ by the trade winds and then convectively uplifted. Once in the upper troposphere, CO enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maximum CO mixing ratios are found. Anthropogenic and fires both contribute, by the same order of magnitude, to the CO budget of the African upper troposphere. Local fires have the highest contribution, drive the location of the observed UT CO maxima, and are related to the following transport pathway: CO emitted at the surface is transported towards the ITCZ by the trade winds and further convectively uplifted. Then UT CO enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maxima are located. Anthropogenic CO contribution is mostly from Africa during the entire year, with a low seasonal variability, and is related to similar transport circulation than fire air masses. There is also a large contribution from Asia in JJASO related to the fast convective uplift of polluted air masses in the Asian monsoon region which are further westward transported by the tropical easterly jet (TEJ) and the Asian monsoon anticyclone (AMA). O3 minima correspond to air masses that were recently uplifted from the surface where mixing ratios are low at the ITCZ. The O3 maxima correspond to old high altitude air masses uplifted from either local or long distance area of high O3 precursor emissions (Africa and South America during all the year, South Asia mainly in JJASO), and must be created during transport by photochemistry. This analysis of meridional transects contribute to a better understanding of distributions of CO and O3 in the intertropical African upper troposphere and the processes which drive these distributions. Therefore, it provides a solid basis for comparison and improvement of models and satellite products in order to get the good O3 for the good reasons. [ABSTRACT FROM AUTHOR]

The StratoClim airborne campaign took place in Nepal from 27 July to 10 August 2017 to document the physical and chemical properties of the South Asian Upper Troposphere Lower Stratosphere (UTLS) during the Asian Summer Monsoon (ASM). In the present paper, simulations with the Meso-NH cloud-chemistry model at a horizontal resolution of 15 km are performed over the Asian region to characterize the impact of monsoon deep convection on the composition of Asian Monsoon Anticyclone (AMA) and on the formation of the Asian Tropopause Aerosol Layer (ATAL) during the StratoClim campaign. StratoClim took place during a break phase of the monsoon with an intense convective activity over south China and Sichuan. Comparisons between Brightness Temperature (BT) at 10.8 microns observed by satellite sensors and simulated by Meso-NH highlight the ability of the model to correctly reproduce the life cycle of deep convective clouds. Comparison between CO and O3 concentrations from Meso-NH and airborne observations (StratoClim and IAGOS) demonstrates that the model captures most of the observed variabilities. Nevertheless, for both gases, the model tends to overestimate the concentrations and misses some thin CO plumes related to local convective events probably because of a too coarse resolution, but the convective uplift of pollution is very well captured by the model. We have therefore focused on the impact of Sichuan convection on the AMA composition. A dedicated sensitivity simulation showed that the 7 August convective event brought large amounts of CO deep into the AMA and even across the 380 K isentropic level located at 17.8 km. This Sichuan contribution enhanced the CO concentration by ~15 % to reach more than 180 ppbv over a large area around 15 km height. Noteworthy, Meso-NH captures the impact of the diluted Sichuan plume on the CO concentration during a StratoClim flight south of Kathmandu highlighting its ability to reproduce the transport pathway of Sichuan pollution. According to the model, primary organic aerosol and black carbon particles originating from Sichuan are transported following the same pathway as CO. The large particles are heavily scavenged within the precipitating part of the convective clouds but remain the most important contributor to the particle mass in the AMA. Over the whole AMA region, the 7 August convective event resulted in a 0.5% increase of CO over the 10-20 km range that lasted about 2 days. The impact of pollution uplift from three regions (India, China and Sichuan) averaged over the first 10 days of August has also been evaluated with sensitivity simulations. Even during this monsoon break phase, the results confirm the predominant role of India relative to China with respective contributions of 11 and 7 % to CO in the 10[sup -1]5 km layer. Moreover, during this period a large part (35 %) of the Chinese contribution comes from the Sichuan basin alone. [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]