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We use a regional chemistry transport model (Weather Research and Forecasting model coupled with chemistry, WRF-Chem) in conjunction with surface observations of tropospheric ozone and Ozone Monitoring Instrument (OMI) satellite retrievals of tropospheric column NO2 to evaluate processes controlling the regional distribution of tropospheric ozone over western Siberia for late spring and summer in 2011. This region hosts a range of anthropogenic and natural ozone precursor sources, and it serves as a gateway for near-surface transport of Eurasian pollution to the Arctic. However, there is a severe lack of in situ observations to constrain tropospheric ozone sources and sinks in the region. We show widespread negative bias in WRF-Chem tropospheric column NO2 when compared to OMI satellite observations from May–August, which is reduced when using ECLIPSE (Evaluating the Climate and Air Quality Impacts of Short-Lived Pollutants) v5a emissions (fractional mean bias (FMB) = −0.82 to −0.73) compared with the EDGAR (Emissions Database for Global Atmospheric Research)-HTAP (Hemispheric Transport of Air Pollution) v2.2 emissions data (FMB = −0.80 to −0.70). Despite the large negative bias, the spatial correlations between model and observed NO2 columns suggest that the spatial pattern of NOx sources in the region is well represented. Scaling transport and energy emissions in the ECLIPSE v5a inventory by a factor of 2 reduces column NO2 bias (FMB = −0.66 to −0.35), but with overestimates in some urban regions and little change to a persistent underestimate in background regions. Based on the scaled ECLIPSE v5a emissions, we assess the influence of the two dominant anthropogenic emission sectors (transport and energy) and vegetation fires on surface NOx and ozone over Siberia and the Russian Arctic. Our results suggest regional ozone is more sensitive to anthropogenic emissions, particularly from the transport sector, and the contribution from fire emissions maximises in June and is largely confined to latitudes south of 60∘ N. Ozone dry deposition fluxes from the model simulations show that the dominant ozone dry deposition sink in the region is to forest vegetation, averaging 8.0 Tg of ozone per month, peaking at 10.3 Tg of ozone deposition during June. The impact of fires on ozone dry deposition within the domain is small compared to anthropogenic emissions and is negligible north of 60∘ N. Overall, our results suggest that surface ozone in the region is controlled by an interplay between seasonality in atmospheric transport patterns, vegetation dry deposition, and a dominance of transport and energy sector emissions.

The 2019/2020 Australian wildfires emitted large quantities of atmospheric pollutant gases and aerosols. Using state-of-the-art near-real-time satellite measurements of tropospheric composition, we present an analysis of several emitted trace gases and their long-range transport, and compare to the previous (2018/2019) fire season. Observations of carbon monoxide (CO) show that fire emissions were so intense that the distinct Australian fire plume managed to circumnavigate the Southern Hemisphere (SH) within a few weeks, with eastward propagation over the South Pacific, South America, the South Atlantic, Africa, and the Indian Ocean. Elevated atmospheric methane levels were also detected in January 2020 fire plumes over the Pacific, defined using CO as a plume tracer, even though sampling was restricted spatially by aerosols and clouds. Observations also show significant enhancements of methanol (CH3OH) from the fires, where CH3OH:CO enhancement ratios increased within the aged plume downwind over the South Pacific indicating secondary in-plume CH3OH formation.

Nitrogen oxides (NOx, NO+NO2) are potent air pollutants which directly impact on human health and which aid the formation of other hazardous pollutants such as ozone (O3) and particulate matter. In this study, we use satellite tropospheric column nitrogen dioxide (TCNO2) data to evaluate the spatiotemporal variability and magnitude of the United Kingdom (UK) bottom-up National Atmospheric Emissions Inventory (NAEI) NOx emissions. Although emissions and TCNO2 represent different quantities, for UK city sources we find a spatial correlation of ~0.5 between the NAEI NOx emissions and TCNO2 from the high-spatial-resolution TROPOspheric Monitoring Instrument (TROPOMI), suggesting a good spatial distribution of emission sources in the inventory. Between 2005 and 2015, the NAEI total UK NOx emissions and long-term TCNO2 record from the Ozone Monitoring Instrument (OMI), averaged over England, show decreasing trends of 4.4 % and 2.2 %, respectively. Top-down NOx emissions were derived in this study by applying a simple mass balance approach to TROPOMI observed downwind NO2 plumes from city sources. Overall, these top-down estimates were consistent with the NAEI, but for larger cities such as London and Manchester the inventory is significantly (> 25 %) less than the top-down emissions. This NAEI NOx emission underestimate is supported by comparing simulations from the GEOS-Chem atmospheric chemistry model, driven by the NAEI emissions, with satellite and surface NO2 observations over the UK. This yields substantial model negative biases, providing further evidence to demonstrate that the NAEI may be underestimating NOx emissions in London and Manchester.

Hydrogen cyanide (HCN) is one of the most abundant cyanides present in the global atmosphere, and is a tracer of biomass burning, especially for peatland fires. The HCN lifetime is 2–5 months in the troposphere but several years in the stratosphere. Understanding the physical and chemical mechanisms of HCN variability is important due to its non-negligible role in the nitrogen cycle. The main source of tropospheric HCN is biomass burning with minor contributions from industry and transport. The main loss mechanism of atmospheric HCN is the reaction with the hydroxyl radical (OH). Ocean uptake is also important, while in the stratosphere oxidation by reaction with O(1D) needs to be considered.HCN variability can be investigated using chemical model simulations, such as three-dimensional (3-D) chemical transport models (CTMs). Here we use an adapted version of the TOMCAT 3-D CTM at a 1.2°x1.2° spatial resolution from the surface to ~60 km for 12 idealised HCN tracers which quantify the main loss mechanisms of HCN, including ocean uptake, atmospheric oxidation reactions and their combinations. The TOMCAT output of the HCN distribution in the period 2004-2020 has been compared with HCN profiles measured by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) over an altitude grid from 6 to 42 km. HCN model data have also been compared with ground-based measurements of HCN columns from NDACC FTIR stations and with in-situ volume mixing ratios (VMRs) from NOAA ground-based measurement sites.The model outputs for the HCN tracer with full treatment of the loss processes generally agree well with ACE-FTS measurements, as long as we use recent laboratory values for the atmospheric loss reactions. Diagnosis of the individual loss terms shows that decay of the HCN profile in the upper stratosphere is due mainly to the O(1D) sink. In order to test the magnitude of the tropospheric OH sink and the magnitude of the ocean sink, we also show the comparisons of the model tracers with surface-based observations. The implications of our results for understanding HCN and its variability are then discussed.

The dramatic and sudden reduction in anthropogenic activity due to lockdown measures in the UK in response to the COVID-19 outbreak has resulted in a concerted effort to estimate local and regional changes in air quality, though changes in underlying emissions remain uncertain. Here we combine satellite observations of tropospheric NO2 from TROPOspheric Monitoring Instrument and the Goddard Earth Observing System (GEOS)-Chem 3D chemical transport model to estimate that NO x emissions declined nationwide by ∼20% during the lockdown (23 March to 31 May 2020). Regionally, these range from 22% to 23% in the western portion of the country to 29% in the southeast and Manchester, and >40% in London. We apply a uniform 20% lockdown period emission reduction to GEOS-Chem anthropogenic emissions over the UK to determine that decline in lockdown emissions led to a national decline in PM2.5 of 1.1 μg m−3, ranging from 0.6 μg m−3 in Scotland to 2 μg m−3 in the southwest. The decline in emissions in cities (>40%) is greater than the national average and causes an increase in ozone of ∼2 ppbv in London and Manchester. The change in ozone and PM2.5 concentrations due to emission reductions alone is about half the total change from 2019 to 2020. This emphasizes the need to account for emissions and other factors, in particular meteorology, in future air pollution abatement strategies and regulatory action.

Volcanic eruptions pose a serious threat to the aviation industry causing widespread disruption. To identify any potential impacts, nine Volcanic Ash Advisory Centres (VAACs) provide global monitoring of all eruptions, informing stakeholders how each volcanic eruption might interfere with aviation. Numerical dispersion models represent a vital infrastructure when assessing and forecasting the atmospheric conditions from a volcanic plume.In this study we investigate the 2019 Raikoke eruption, which emitted approximately 1.5 Tg of sulfur dioxide (SO2) representing the largest volcanic emission of SO2 into the stratosphere since the Nabro eruption in 2011. Using the UK Met Office’s Numerical Atmospheric-dispersion Modelling Environment (NAME), we simulate the evolution of the volcanic gas and aerosol particle plumes (SO2 and sulfate, SO4) across the Northern Hemisphere between 21st June and 17th July. We evaluate the skills and limitations of NAME in terms of modelling volcanic SO2 plumes, by comparing our simulations to high-resolution measurements from the Tropospheric Monitoring Instrument (TROPOMI) on-board the European Space Agency (ESA)’s Sentinel 5 – Precursor (S5P) satellite.Our comparisons show that NAME accurately simulates the observed location and shape of the SO2 plume in the first few weeks after the eruption. NAME also reproduces the magnitude of the observed SO2 vertical column densities, when emitting 1.5 Tg of SO2, during the first 48 hours after the eruption. On longer timescales, we find that the model-simulated SO2 plume in NAME is more diffuse than in the TROPOMI measurements, resulting in an underestimation of the peak SO2 vertical column densities in the model. This suggests that the diffusion parameters used in NAME are too large in the upper troposphere and lower stratosphere.Finally, NAME underestimates the total mass of SO2 when compared to estimates from TROPOMI, however emitting 2 Tg of SO2 in the model improves the comparison, resulting in very good agreement with the satellite measurements.

The decline in Amazonian deforestation rates and biomass burning activity (2001–2012) has been shown to reduce air pollutant emissions (e.g., aerosols) and improve regional air quality. However, in the Cerrado region (savannah grasslands in northeastern Brazil), satellite observations reveal increases in fire activity and tropospheric column nitrogen dioxide (an ozone precursor) during the burning season (August‐October, 2005–2016), which have partially offset these air quality benefits. Simulations from a 3‐D global chemistry transport model (CTM) capture this increase in NO2 with a surface increase of ~1 ppbv per decade. As there are limited long‐term observational tropospheric ozone records, we utilize the well‐evaluated CTM to investigate changes in ozone. Here, the CTM suggests that Cerrado region surface ozone is increasing by ~10 ppbv per decade. If left unmitigated, these positive fire‐sourced ozone trends will substantially increase the regional health risks and impacts from expected future enhancements in South American biomass burning activity under climate change.

We use the ozone dataset from the Copernicus Climate Change Service (C3S) during 1979–2017 to investigate the long-term variations of the total column ozone (TCO) and the relative total ozone low (TOL) over the Tibetan Plateau (TP) during different seasons. Based on various regression models, the wintertime TCO over the TP decreases overall during 1979–2017 with ongoing decreases since 1997. We perform multivariate regression analysis to quantify the influence of dynamical and chemical processes responsible for the long-term TCO variability over the TP. We use both piecewise linear trend (PWLT) and equivalent effective stratospheric chlorine loading (EESC)-based regression models that include explanatory variables such as the 11-year solar cycle, quasi-biennial oscillation (QBO) at 30 hPa and 10 hPa and the geopotential height (GH) at 150 hPa. The 150 hPa GH is found to be a major dynamical contributor to the total ozone variability (8 %) over the TP in wintertime. We also find strong correlation between TCO in DJF and the following JJA, indicating that negative/positive anomalies in the wintertime build up persist into summer. We also use the TOMCAT/SLIMCAT 3-D chemical transport model to investigate the contributions of different factors to the ozone variations over the TP. Using identical regression model on simulated TCO time series, we obtain consistent results with C3S-based data. We perform two sensitivity experiments with repeating dynamics of 2004 and 2008 to further study the role that the GH at 150 hPa plays in the ozone variations over the TP. The GH differences between the two years show an obvious, negative centre near 150 hPa over the TP in DJF. Composite analysis show that GH fluctuations associated with Inter Tropical Convergence Zone, ENSO events or Walker circulation play a key role in controlling TCO variability in the lower stratosphere.

The June 2018 Saddleworth Moor fires were some of the largest UK wildfires on record and lasted for approximately three weeks. They emitted large quantities of smoke, trace gases and aerosols which were transported downwind over the highly populated regions of Manchester and Liverpool. Surface observations of PM2.5 indicate that concentrations were 4–5.5 times higher than the recent seasonal average. State-of-the-art satellite measurements of total column carbon monoxide (TCCO) from the TROPOMI instrument on the Sentinel 5—Precursor (S5P) platform, coupled with measurements from a flight of the UK BAe-146–301 research aircraft, are used to quantify the substantial enhancement in emitted trace gases. The aircraft measured plume enhancements with near-fire CO and PM2.5 concentrations >1500 ppbv and >125 μg m−3 (compared to ∼100 ppbv and ∼5 μg m−3 background concentrations). Downwind fire-plume ozone (O3) values were larger than the near-fire location, indicating O3 production with distance from source. The near-fire O3:CO ratio was (ΔO3/ΔCO) 0.001 ppbv/ppbv, increasing downwind to 0.060–0.105 ppbv/ppbv, suggestive of O3 production enhancement downwind of the fires. Emission rates of CO and CO2 ranged between 1.07 (0.07–4.69) kg s−1 and 13.7 (1.73–50.1) kg s−1, respectively, similar to values expected from a medium sized power station.

Previous studies have used surface observations of pollutants (e.g., nitrogen dioxide [NO₂] and aerosols) to evaluate improvements in United Kingdom (UK) air quality over recent decades. However, surface monitoring networks provide limited spatial coverage and are not always representative of air quality over a wider region. Satellite observations, such as tropospheric column NO₂ (TCNO₂), aerosol optical depth (AOD) and sub‐column (0–6 km) ozone (SCO₃), provide widespread monitoring of air quality on a national scale. In this study, we use such observations to analyse trends in UK air quality, between 2005 and 2015, finding significant decreases in TCNO₂ and AOD over UK pollution hotspots. The largest changes in short‐lived NO₂ are located over populated (i.e., source) regions, associated with large emissions of nitrogen oxides (NOₓ). AOD changes are more spread out, and less strongly associated with source regions, due to a longer aerosol lifetime, secondary aerosol formation and non‐urban aerosol sources. SCO₃ shows no significant trends over England/Wales, but significant positive trends over Scotland, which is consistent with previous studies of changes in background tropospheric ozone in other remote regions of north‐western Europe.