The influence of synoptic weather regimes on UK air quality: Regional model studies of tropospheric column NO2

Synoptic meteorology can have a significant influence on UK air quality. Cyclonic conditions lead to the dispersion of air pollutants away from source regions, while anticyclonic conditions lead to their accumulation over source regions. Meteorology also modifies atmospheric chemistry processes such as photolysis and wet deposition. Previous studies have shown a relationship between observed satellite tropospheric column NO2 and synoptic meteorology in different seasons. Here, we test whether the UK Met Office Air Quality in the Unified Model (AQUM) can reproduce these observations and then use the model to explore the relative importance of various factors. We show that AQUM successfully captures the observed relationships when sampled under the Lamb weather types, an objective classification of midday UK circulation patterns. By using a range of idealized NOx-like tracers with different e-folding lifetimes, we show that under different synoptic regimes the NO2 lifetime in AQUM is approximately 6 h in summer and 12 h in winter. The longer lifetime can explain why synoptic spatial tropospheric column NO2 variations are more significant in winter compared to summer, due to less NO2 photochemical loss. We also show that cyclonic conditions have more seasonality in tropospheric column NO2 than anticyclonic conditions as they result in more extreme spatial departures from the wintertime seasonal average. Within a season (summer or winter) under different synoptic regimes, a large proportion of the spatial pattern in the UK tropospheric column NO2 field can be explained by the idealized model tracers, showing that transport is an important factor in governing the variability of UK air quality on seasonal synoptic timescales

Solar cycle response and long-term trends in the mesospheric metal layers

The meteoric metal layers (Na, Fe, and K)—which form as a result of the ablation of incoming meteors—act as unique tracers for chemical and dynamical processes that occur within the upper mesosphere/lower thermosphere region. In this work, we examine whether these metal layers are sensitive indicators of decadal long-term changes within the upper atmosphere. Output from a whole-atmosphere climate model is used to assess the response of the Na, K, and Fe layers across a 50 year period (1955–2005). At short timescales, the K layer has previously been shown to exhibit a very different seasonal behavior compared to the other metals. Here we show that this unusual behavior is also exhibited at longer timescales (both the ~11 year solar cycle and 50 year periods), where K displays a much more pronounced response to atmospheric temperature changes than either Na or Fe. The contrasting solar cycle behavior of the K and Na layers predicted by the model is confirmed using satellite and lidar observations for the period 2004–2013

Evaluating year-to-year anomalies in tropical wetland methane emissions using satellite CH₄ observations

Natural wetlands are the largest source of methane emissions, contributing 20–40% of global emissions and dominating the inter-annual variability. Large uncertainties remain on their variability and response to climate change. This study uses atmospheric methane observations from the GOSAT satellite to evaluate methane wetland emission estimates. We assess how well simulations reproduce the observed methane inter-annual variability by evaluating the detrended seasonal cycle. The latitudinal means agree well but maximum differences in the tropics of 28.1–34.8 ppb suggest that all simulations fail to capture the extent of the tropical wetland seasonal cycle. We focus further analysis on the major natural wetlands in South America: the seasonally flooded savannah of the Pantanal (Brazil) and Llanos de Moxos (Bolivia) regions; and the riverine wetlands formed by the Paraná River (Argentina). We see large discrepancies between simulation and observation over the Pantanal and Llanos de Moxos region in 2010, 2011 and 2014 and over the Paraná River region in 2010 and 2014. We find highly consistent behaviour between the time and location of these methane anomalies and the change in wetland extent, driven by precipitation related to El Niño Southern Oscillation activity. We conclude that the inability of land surface models to increase wetland extent through overbank inundation is the primary cause of these observed discrepancies and can lead to under-estimation of methane fluxes by as much as 50% (5.3–11.8 Tg yr −1 ) of the observed emissions for the combined Pantanal and Paraná regions. As the hydrology of these regions is heavily linked to ENSO variability, being able to reproduce changes in wetland behaviour is important for successfully predicting their methane emissions

On the Cause of Recent Variations in Lower Stratospheric Ozone

We use height‐resolved and total column satellite observations and 3‐D chemical transport model simulations to study stratospheric ozone variations during 1998–2017 as ozone‐depleting substances decline. In 2017 extrapolar lower stratospheric ozone displayed a strong positive anomaly following much lower values in 2016. This points to large interannual variability rather than an ongoing downward trend, as reported recently by Ball et al. (2018, https://doi.org/10.5194/acp‐18‐1379‐2018). The observed ozone variations are well captured by the chemical transport model throughout the stratosphere and are largely driven by meteorology. Model sensitivity experiments show that the contribution of past trends in short‐lived chlorine species to the ozone changes is small. Similarly, the potential impact of modest trends in natural brominated short‐lived species is small. These results confirm the important role that atmospheric dynamics plays in controlling ozone in the extrapolar lower stratosphere on multiannual time scales and the continued importance of monitoring ozone profiles as the stratosphere changes

D-region ion–neutral coupled chemistry (Sodankylä Ion Chemistry, SIC) within the Whole Atmosphere Community Climate Model (WACCM 4) – WACCM-SIC and WACCM-rSIC

This study presents a new ion–neutral chemical model coupled into the Whole Atmosphere Community Climate Model (WACCM). The ionospheric D-region (altitudes ∼  50–90 km) chemistry is based on the Sodankylä Ion Chemistry (SIC) model, a one-dimensional model containing 307 ion–neutral and ion recombination, 16 photodissociation and 7 photoionization reactions of neutral species, positive and negative ions, and electrons. The SIC mechanism was reduced using the simulation error minimization connectivity method (SEM-CM) to produce a reaction scheme of 181 ion–molecule reactions of 181 ion–molecule reactions of 27 positive and 18 negative ions. This scheme describes the concentration profiles at altitudes between 20 km and 120 km of a set of major neutral species (HNO3, O3, H2O2, NO, NO2, HO2, OH, N2O5) and ions (O2+, O4+, NO+, NO+(H2O), O2+(H2O), H+(H2O), H+(H2O)2, H+(H2O)3, H+(H2O)4, O3−, NO2−, O−, O2, OH−, O2−(H2O), O2−(H2O)2, O4−, CO3−, CO3−(H2O), CO4−, HCO3−, NO2−, NO3−, NO3−(H2O), NO3−(H2O)2, NO3−(HNO3), NO3−(HNO3)2, Cl−, ClO−), which agree with the full SIC mechanism within a 5 % tolerance. Four 3-D model simulations were then performed, using the impact of the January 2005 solar proton event (SPE) on D-region HOx and NOx chemistry as a test case of four different model versions: the standard WACCM (no negative ions and a very limited set of positive ions); WACCM-SIC (standard WACCM with the full SIC chemistry of positive and negative ions); WACCM-D (standard WACCM with a heuristic reduction of the SIC chemistry, recently used to examine HNO3 formation following an SPE); and WACCM-rSIC (standard WACCM with a reduction of SIC chemistry using the SEM-CM method). The standard WACCM misses the HNO3 enhancement during the SPE, while the full and reduced model versions predict significant NOx, HOx and HNO3 enhancements in the mesosphere during solar proton events. The SEM-CM reduction also identifies the important ion–molecule reactions that affect the partitioning of odd nitrogen (NOx), odd hydrogen (HOx) and O3 in the stratosphere and mesosphere

High resolution satellite observations give new view of UK air quality

New state‐of‐the‐art satellite measurements of tropospheric column NO2 from the TROPOMI instrument on‐board Sentinel‐5 Precursor (S5P), launched in October 2017, allow for an unprecedented high resolution (sub‐10km) assessment of UK air quality (AQ) from space. We present the first results from TROPOMI and compare them with its predecessor, the Ozone Monitoring Instrument (OMI), to quantify previously unresolved UK pollution hotspots (e.g. Bristol, Southampton and Liverpool). The TROPOMI tropospheric column NO2 data represents a powerful new tool to quantify UK AQ, evaluate atmospheric composition models and potentially derive new emission inventories from space

High resolution satellite observations give new view of UK air quality

New state‐of‐the‐art satellite measurements of tropospheric column NO2 from the TROPOMI instrument on‐board Sentinel‐5 Precursor (S5P), launched in October 2017, allow for an unprecedented high resolution (sub‐10km) assessment of UK air quality (AQ) from space. We present the first results from TROPOMI and compare them with its predecessor, the Ozone Monitoring Instrument (OMI), to quantify previously unresolved UK pollution hotspots (e.g. Bristol, Southampton and Liverpool). The TROPOMI tropospheric column NO2 data represents a powerful new tool to quantify UK AQ, evaluate atmospheric composition models and potentially derive new emission inventories from space

Determination of the atmospheric lifetime and global warming potential of sulfur hexafluoride using a three-dimensional model

We have used the Whole Atmosphere Community Climate Model (WACCM), with an updated treatment of loss processes, to determine the atmospheric lifetime of sulfur hexafluoride (SF6). The model includes the following SF6 removal processes: photolysis, electron attachment and reaction with mesospheric metal atoms. The Sodankylä Ion Chemistry (SIC) model is incorporated into the standard version of WACCM to produce a new version with a detailed D region ion chemistry with cluster ions and negative ions. This is used to determine a latitude- and altitude-dependent scaling factor for the electron density in the standard WACCM in order to carry out multi-year SF6 simulations. The model gives a mean SF6 lifetime over an 11-year solar cycle (τ) of 1278 years (with a range from 1120 to 1475 years), which is much shorter than the currently widely used value of 3200 years, due to the larger contribution (97.4 %) of the modelled electron density to the total atmospheric loss. The loss of SF6 by reaction with mesospheric metal atoms (Na and K) is far too slow to affect the lifetime. We investigate how this shorter atmospheric lifetime impacts the use of SF6 to derive stratospheric age of air. The age of air derived from this shorter lifetime SF6 tracer is longer by 9 % in polar latitudes at 20 km compared to a passive SF6 tracer. We also present laboratory measurements of the infrared spectrum of SF6 and find good agreement with previous studies. We calculate the resulting radiative forcings and efficiencies to be, on average, very similar to those reported previously. Our values for the 20-, 100- and 500-year global warming potentials are 18 000, 23 800 and 31 300, respectively

Quantifying The Causes of Differences in Tropospheric OH within Global Models

The hydroxyl radical (OH) is the primary daytime oxidant in the troposphere and provides the main loss mechanism for many pollutants and greenhouse gases, including methane (CH4). Global mean tropospheric OH differs by as much as 80% among various global models, for reasons that are not well understood. We use neural networks (NNs), trained using archived output from eight chemical transport models (CTMs) that participated in the POLARCAT Model Intercomparison Project (POLMIP), to quantify the factors responsible for differences in tropospheric OH and resulting CH4 lifetime (τCH4) between these models. Annual average τCH4, for loss by OH only, ranges from 8.0–11.6 years for the eight POLMIP CTMs. The factors driving these differences were quantified by inputting 3-D chemical fields from one CTM into the trained NN of another CTM. Across all CTMs, the largest mean differences in τCH4 (ΔτCH4) result from variations in chemical mechanisms (ΔτCH4 = 0.46 years), the photolysis frequency (J) of O3→O(1D) (0.31 years), local O3 (0.30 years), and CO (0.23 years). The ΔτCH4 due to CTM differences in NOx (NO + NO2) is relatively low (0.17 years), though large regional variation in OH between the CTMs is attributed to NOx. Differences in isoprene and J(NO2) have negligible overall effect on globally averaged tropospheric OH, though the extent of OH variations due to each factor depends on the model being examined. This study demonstrates that NNs can serve as a useful tool for quantifying why tropospheric OH varies between global models, provided essential chemical fields are archived

Quantifying the transboundary contribution of nitrogen oxides to UK air quality

Nitrogen dioxide (NO2) pollution is an important contributor to poor air quality (AQ) and a significant cause of premature deaths in the UK. Although transboundary (i.e., international) transport of pollution to the UK is believed to have an impact on UK pollutant concentrations, large uncertainties remain in these estimates. Therefore, the extent to which emission reductions in neighbouring countries would benefit UK AQ relative to local emission reductions also remains unknown. We have used a back‐trajectory model in conjunction with synoptic scale classifications of UK circulation patterns (Lamb Weather Types [LWT]), to quantify the accumulation of nitrogen oxide (NO x = NO2 + NO) emissions in air masses en‐route to the UK. This novel method presents a computationally inexpensive and useful method of quantifying the accumulation of pollutants under different circulation patterns. We find the highest accumulated NO x totals occur under south‐easterly and southerly flows (>15 μg⋅m−2), with a substantial contribution from outwith the UK (>25%). In contrast, the total accumulated NO x under northerly and westerly flows is lower (∼10 μg⋅m−2), and dominated by UK emissions (>95%). This indicates that European emissions can contribute substantially to UK local‐scale pollution in urban areas under south‐easterly and southerly flows. The sensitivity of integrated NO x emission totals under different air masses is investigated by modelling future European emission contributions based on emission reduction targets. Under targets set by the European Union, there would be a decrease in accumulated NO x emissions in London under most wind directions except for north‐westerly, westerly and northerly flow. The largest benefits to UK AQ from transboundary contributions occur with emission reductions in the Benelux region, due to its close proximity and high NO x emission rates, emphasising the importance of international cooperation in improving local AQ