scholarly journals Tropospheric ozone changes and ozone sensitivity from present-day to future under shared socio-economic pathways

2021 ◽  
Author(s):  
Zhenze Liu ◽  
Ruth M. Doherty ◽  
Oliver Wild ◽  
Fiona M. O’Connor ◽  
Steven T. Turnock
Keyword(s):  
North America ◽  
Tropospheric Ozone ◽  
Surface Ozone ◽  
Nox Emissions ◽  
Limited Region ◽  
Voc Emissions ◽  
Ozone Concentrations ◽  
Ozone Sensitivity ◽  
The Future ◽  
High Emission

Abstract. Tropospheric ozone is important to future air quality and climate. We investigate ozone changes and ozone sensitivity to changing emissions in the context of climate change from the present day (2004–2014) to the future (2045–2055) under a range of shared socio-economic pathways (SSPs). We apply the United Kingdom Earth System Model, UKESM1, with an extended chemistry scheme including more reactive volatile organic compounds (VOCs) to quantify ozone burdens as well as ozone sensitivities globally and regionally based on nitrogen oxide (NOx) and VOC concentrations. We show that the tropospheric ozone burden increases by 4 % under a development pathway with higher NOx and VOC emissions (SSP3-7.0), but decreases by 7 % under the same pathway if NOx and VOC emissions are reduced (SSP3-7.0-lowNTCF) and by 5 % if atmospheric methane (CH4) concentrations are reduced (SSP3-7.0-lowCH4). Global mean surface ozone concentrations are reduced by 3–5 ppb under SSP3-7.0-lowNTCF and by 2–3 ppb under SSP3-7.0-lowCH4. However, surface ozone changes vary substantially by season in high-emission regions under future pathways, with decreased ozone concentrations in summer and increased ozone concentrations in winter when NOx emissions are reduced. VOC-limited areas are more extensive in winter (7 %) than in summer (3 %) across the globe. North America, Europe and East Asia are the dominant VOC-limited regions in the present day but North America and Europe become more NOx-limited in the future mainly due to reductions in NOx emissions. The impacts of VOC emissions on O3 sensitivity are limited in North America and Europe because reduced anthropogenic VOC emissions are offset by higher biogenic VOC emissions. O3 sensitivity is not greatly influenced by changing CH4 concentrations. South Asia becomes the dominant VOC-limited region under future pathways. We highlight that reductions in NOx emissions are required to transform O3 production from VOC- to NOx-limitation, but that these lead to increased O3 concentrations in high-emission regions, and hence emission controls on VOC and CH4 are also necessary.

scholarly journals Foreign influences on tropospheric ozone over East Asia through global atmospheric transport

2019 ◽  
Vol 19 (19) ◽  
pp. 12495-12514 ◽  
Author(s):  
Han Han ◽  
Jane Liu ◽  
Huiling Yuan ◽  
Tijian Wang ◽  
Bingliang Zhuang ◽  
...  
Keyword(s):  
North America ◽  
East Asia ◽  
Tropospheric Ozone ◽  
Large Scale ◽  
Transport Model ◽  
Surface Ozone ◽  
East Asian ◽  
South Asian High ◽  
Upper Troposphere ◽  
Ozone Concentrations

Abstract. Tropospheric ozone in East Asia is influenced by the transport of ozone from foreign regions around the world. However, the magnitudes and variations in such influences remain unclear. This study was performed to investigate the influences using a global chemical transport model, GEOS-Chem, through the tagged ozone and emission perturbation simulations. The results show that foreign ozone is transported to East Asia (20–60∘ N, 95–150∘ E) mainly through the middle and upper troposphere. In East Asia, the influence of foreign ozone increases rapidly with altitude. In the middle and upper troposphere, the regional mean concentrations of foreign ozone range from 32 to 65 ppbv, being 0.8–4.8 times higher than its native counterpart (11–18 ppbv). Annually, ∼60 % of foreign ozone in the East Asian middle and upper troposphere comes from North America (5–13 ppbv) and Europe (5–7 ppbv), as well as from foreign oceanic regions (9–21 ppbv). Over the East Asian tropospheric columns, foreign ozone appears most in spring when ozone concentrations in the foreign regions are high and the westerlies are strong and least in summer when the South Asian High blocks eastward foreign ozone from reaching East Asia south of 35∘ N. At the East Asian surface, the annual mean of foreign ozone concentrations is ∼22.2 ppbv, which is comparable to its native counterpart of ∼20.4 ppbv. In the meantime, the annual mean of anthropogenic ozone concentrations from foreign regions is ∼4.7 ppbv, half of which comes from North America (1.3 ppbv) and Europe (1.0 ppbv). Seasonally, foreign ozone concentrations at the East Asian surface are highest in winter (27.1 ppbv) and lowest in summer (16.5 ppbv). This strong seasonality is largely modulated by the East Asian monsoon (EAM) via its influence on vertical motion. The large-scale subsidence prevailing during the East Asian winter monsoon (EAWM) favours the downdraft of foreign ozone to the surface, while widespread convection in the East Asian summer monsoon (EASM) blocks such transport. Interannually, the variation in foreign ozone at the East Asian surface is found to be closely related to the intensity of the EAM. Specifically, the stronger the EAWM is in a winter, the more ozone from North America and Europe reaches the East Asian surface because of the stronger subsidence behind the East Asian trough. In summer, ozone from South and South-east Asia is reduced in strong EASM years due to weakened south-westerly monsoon winds. This study suggests substantial foreign influences on ozone at the East Asian surface and in its tropospheric columns. It also underscores the importance of the EAM in the seasonal and interannual variations in foreign influences on surface ozone in East Asia.

scholarly journals Unraveling pathways of elevated ozone induced by the 2020 lockdown in Europe by an observationally constrained regional model using TROPOMI

2021 ◽  
Vol 21 (24) ◽  
pp. 18227-18245
Author(s):  
Amir H. Souri ◽  
Kelly Chance ◽  
Juseon Bak ◽  
Caroline R. Nowlan ◽  
Gonzalo González Abad ◽  
...  
Keyword(s):  
Transport Model ◽  
Atmospheric Transport ◽  
Model Simulation ◽  
Surface Ozone ◽  
Ozone Production ◽  
Anthropogenic Emissions ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Voc Emissions ◽  
Constrained Model

Abstract. Questions about how emissions are changing during the COVID-19 lockdown periods cannot be answered by observations of atmospheric trace gas concentrations alone, in part due to simultaneous changes in atmospheric transport, emissions, dynamics, photochemistry, and chemical feedback. A chemical transport model simulation benefiting from a multi-species inversion framework using well-characterized observations should differentiate those influences enabling to closely examine changes in emissions. Accordingly, we jointly constrain NOx and VOC emissions using well-characterized TROPOspheric Monitoring Instrument (TROPOMI) HCHO and NO2 columns during the months of March, April, and May 2020 (lockdown) and 2019 (baseline). We observe a noticeable decline in the magnitude of NOx emissions in March 2020 (14 %–31 %) in several major cities including Paris, London, Madrid, and Milan, expanding further to Rome, Brussels, Frankfurt, Warsaw, Belgrade, Kyiv, and Moscow (34 %–51 %) in April. However, NOx emissions remain at somewhat similar values or even higher in some portions of the UK, Poland, and Moscow in March 2020 compared to the baseline, possibly due to the timeline of restrictions. Comparisons against surface monitoring stations indicate that the constrained model underrepresents the reduction in surface NO2. This underrepresentation correlates with the TROPOMI frequency impacted by cloudiness. During the month of April, when ample TROPOMI samples are present, the surface NO2 reductions occurring in polluted areas are described fairly well by the model (model: −21 ± 17 %, observation: −29 ± 21 %). The observational constraint on VOC emissions is found to be generally weak except for lower latitudes. Results support an increase in surface ozone during the lockdown. In April, the constrained model features a reasonable agreement with maximum daily 8 h average (MDA8) ozone changes observed at the surface (r=0.43), specifically over central Europe where ozone enhancements prevail (model: +3.73 ± 3.94 %, +1.79 ppbv, observation: +7.35 ± 11.27 %, +3.76 ppbv). The model suggests that physical processes (dry deposition, advection, and diffusion) decrease MDA8 surface ozone in the same month on average by −4.83 ppbv, while ozone production rates dampened by largely negative JNO2[NO2]-kNO+O3[NO][O3] become less negative, leading ozone to increase by +5.89 ppbv. Experiments involving fixed anthropogenic emissions suggest that meteorology contributes to 42 % enhancement in MDA8 surface ozone over the same region with the remaining part (58 %) coming from changes in anthropogenic emissions. Results illustrate the capability of satellite data of major ozone precursors to help atmospheric models capture ozone changes induced by abrupt emission anomalies.

scholarly journals Estimation of Lower-Stratosphere-to-Troposphere Ozone Profile Using Long Short-Term Memory (LSTM)

2021 ◽  
Vol 13 (7) ◽  
pp. 1374
Author(s):  
Xinxin Zhang ◽  
Ying Zhang ◽  
Xiaoyan Lu ◽  
Lu Bai ◽  
Liangfu Chen ◽  
...  
Keyword(s):  
Air Pollution ◽  
Northern Hemisphere ◽  
Tropospheric Ozone ◽  
Lower Stratosphere ◽  
Short Term Memory ◽  
Surface Ozone ◽  
Short Term ◽  
Term Memory ◽  
Ozone Concentrations ◽  
Long Short Term Memory

Climate change and air pollution are emerging topics due to their possible enormous implications for health and social perspectives. In recent years, tropospheric ozone has been recognized as an important greenhouse gas and pollutant that is detrimental to human health, agriculture, and natural ecosystems, and has shown a trend of increasing interest. Machine-learning-based approaches have been widely applied to the estimation of tropospheric ozone concentrations, but few studies have included tropospheric ozone profiles. This study aimed to predict the Northern Hemisphere distribution of Lower-Stratosphere-to-Troposphere (LST) ozone at a pressure of 100 hPa to the near surface by employing a deep learning Long Short-Term Memory (LSTM) model. We referred to a history of all the observed parameters (meteorological data of European Centre for Medium-Range Weather Forecasts (ECMWF) Reanalysis v5 (ERA5), satellite data, and the ozone profiles of the World Ozone and Ultraviolet Data Center (WOUDC)) between 2014 and 2018 for training the predictive models. Model–measurement comparisons for the monitoring sites of WOUDC for the period 2019–2020 show that the mean correlation coefficients (R2) in the Northern Hemisphere at high latitude (NH), Northern Hemisphere at middle latitude (NM), and Northern Hemisphere at low latitude (NL) are 0.928, 0.885, and 0.590, respectively, indicating reasonable performance for the LSTM forecasting model. To improve the performance of the model, we applied the LSTM migration models to the Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) flights in the Northern Hemisphere from 2018 to 2019 and three urban agglomerations (the Sichuan Basin (SCB), North China Plain (NCP), and Yangtze River Delta region (YRD)) between 2018 and 2019. The results show that our models performed well on the CARIBIC data set, with a high R2 equal to 0.754. The daily and monthly surface ozone concentrations for 2018–2019 in the three urban agglomerations were estimated from meteorological and ancillary variables. Our results suggest that the LSTM models can accurately estimate the monthly surface ozone concentrations in the three clusters, with relatively high coefficients of 0.815–0.889, root mean square errors (RMSEs) of 7.769–8.729 ppb, and mean absolute errors (MAEs) of 6.111–6.930 ppb. The daily scale performance was not as high as the monthly scale performance, with the accuracy of R2 = 0.636~0.737, RMSE = 14.543–16.916 ppb, MAE = 11.130–12.687 ppb. In general, the trained module based on LSTM is robust and can capture the variation of the atmospheric ozone distribution. Moreover, it also contributes to our understanding of the mechanism of air pollution, especially increasing our comprehension of pollutant areas.

scholarly journals Low modeled ozone production suggests underestimation of precursor emissions (especially NO<sub><i>x</i></sub>) in Europe

2018 ◽  
Vol 18 (3) ◽  
pp. 2175-2198 ◽  
Author(s):  
Emmanouil Oikonomakis ◽  
Sebnem Aksoyoglu ◽  
Giancarlo Ciarelli ◽  
Urs Baltensperger ◽  
André Stephan Henry Prévôt
Keyword(s):  
Air Quality ◽  
Surface Ozone ◽  
Model Performance ◽  
Ozone Production ◽  
Nox Emissions ◽  
Air Quality Model ◽  
Quality Model ◽  
Voc Emissions ◽  
Mixing Ratios ◽  
The Impact

Abstract. High surface ozone concentrations, which usually occur when photochemical ozone production takes place, pose a great risk to human health and vegetation. Air quality models are often used by policy makers as tools for the development of ozone mitigation strategies. However, the modeled ozone production is often not or not enough evaluated in many ozone modeling studies. The focus of this work is to evaluate the modeled ozone production in Europe indirectly, with the use of the ozone–temperature correlation for the summer of 2010 and to analyze its sensitivity to precursor emissions and meteorology by using the regional air quality model, the Comprehensive Air Quality Model with Extensions (CAMx). The results show that the model significantly underestimates the observed high afternoon surface ozone mixing ratios (≥ 60 ppb) by 10–20 ppb and overestimates the lower ones (< 40 ppb) by 5–15 ppb, resulting in a misleading good agreement with the observations for average ozone. The model also underestimates the ozone–temperature regression slope by about a factor of 2 for most of the measurement stations. To investigate the impact of emissions, four scenarios were tested: (i) increased volatile organic compound (VOC) emissions by a factor of 1.5 and 2 for the anthropogenic and biogenic VOC emissions, respectively, (ii) increased nitrogen oxide (NOx) emissions by a factor of 2, (iii) a combination of the first two scenarios and (iv) increased traffic-only NOx emissions by a factor of 4. For southern, eastern, and central (except the Benelux area) Europe, doubling NOx emissions seems to be the most efficient scenario to reduce the underestimation of the observed high ozone mixing ratios without significant degradation of the model performance for the lower ozone mixing ratios. The model performance for ozone–temperature correlation is also better when NOx emissions are doubled. In the Benelux area, however, the third scenario (where both NOx and VOC emissions are increased) leads to a better model performance. Although increasing only the traffic NOx emissions by a factor of 4 gave very similar results to the doubling of all NOx emissions, the first scenario is more consistent with the uncertainties reported by other studies than the latter, suggesting that high uncertainties in NOx emissions might originate mainly from the road-transport sector rather than from other sectors. The impact of meteorology was examined with three sensitivity tests: (i) increased surface temperature by 4 ∘C, (ii) reduced wind speed by 50 % and (iii) doubled wind speed. The first two scenarios led to a consistent increase in all surface ozone mixing ratios, thus improving the model performance for the high ozone values but significantly degrading it for the low ozone values, while the third scenario had exactly the opposite effects. Overall, the modeled ozone is predicted to be more sensitive to its precursor emissions (especially traffic NOx) and therefore their uncertainties, which seem to be responsible for the model underestimation of the observed high ozone mixing ratios and ozone production.

scholarly journals Effects of temperature-dependent NO<sub>x</sub> emissions on continental ozone production

2017 ◽  
Author(s):  
Paul S. Romer ◽  
Kaitlin C. Duffey ◽  
Paul J. Wooldridge ◽  
Eric Edgerton ◽  
Karsten Baumann ◽  
...  
Keyword(s):  
Surface Ozone ◽  
Ozone Production ◽  
Climate Feedback ◽  
Nox Emissions ◽  
Southeast United States ◽  
Average Temperature ◽  
Ozone Concentrations ◽  
Effects Of Temperature ◽  
Positive Climate

Abstract. Surface ozone concentrations are observed to increase with rising temperatures, but the mechanisms responsible for this effect in rural and remote continental regions remain uncertain. Better understanding of the effects of temperature on ozone is crucial to understanding global air quality and how it may be affected by climate change. We combine measurements from a focused ground campaign in summer 2013 with a long-term record from a forested site in the rural southeast United States to examine how daily average temperature affects ozone production. We find that changes to local chemistry are key drivers of increased ozone concentrations on hotter days, with integrated daily ozone production increasing by 2.3 ppb C−1. Nearly half of this increase is attributable to temperature-driven increases in emissions of nitrogen oxides (NOx), most likely by soil microbes. The increase of soil NOx emissions with temperature suggests that ozone will continue to increase with temperature in the future, even as direct anthropogenic NOx emissions decrease dramatically. The links between temperature, soil NOx, and ozone form a positive climate feedback.

scholarly journals Impacts of stratospheric sulfate geoengineering on tropospheric ozone

2017 ◽  
Vol 17 (19) ◽  
pp. 11913-11928 ◽  
Author(s):  
Lili Xia ◽  
Peer J. Nowack ◽  
Simone Tilmes ◽  
Alan Robock
Keyword(s):  
Tropospheric Ozone ◽  
Stratospheric Ozone ◽  
Surface Ozone ◽  
Tropospheric Chemistry ◽  
Dominant Factor ◽  
Solar Radiation Management ◽  
Sulfate Aerosols ◽  
Surface Cooling ◽  
Solar Insolation ◽  
Ozone Concentrations

Abstract. A range of solar radiation management (SRM) techniques has been proposed to counter anthropogenic climate change. Here, we examine the potential effects of stratospheric sulfate aerosols and solar insolation reduction on tropospheric ozone and ozone at Earth's surface. Ozone is a key air pollutant, which can produce respiratory diseases and crop damage. Using a version of the Community Earth System Model from the National Center for Atmospheric Research that includes comprehensive tropospheric and stratospheric chemistry, we model both stratospheric sulfur injection and solar irradiance reduction schemes, with the aim of achieving equal levels of surface cooling relative to the Representative Concentration Pathway 6.0 scenario. This allows us to compare the impacts of sulfate aerosols and solar dimming on atmospheric ozone concentrations. Despite nearly identical global mean surface temperatures for the two SRM approaches, solar insolation reduction increases global average surface ozone concentrations, while sulfate injection decreases it. A fundamental difference between the two geoengineering schemes is the importance of heterogeneous reactions in the photochemical ozone balance with larger stratospheric sulfate abundance, resulting in increased ozone depletion in mid- and high latitudes. This reduces the net transport of stratospheric ozone into the troposphere and thus is a key driver of the overall decrease in surface ozone. At the same time, the change in stratospheric ozone alters the tropospheric photochemical environment due to enhanced ultraviolet radiation. A shared factor among both SRM scenarios is decreased chemical ozone loss due to reduced tropospheric humidity. Under insolation reduction, this is the dominant factor giving rise to the global surface ozone increase. Regionally, both surface ozone increases and decreases are found for both scenarios; that is, SRM would affect regions of the world differently in terms of air pollution. In conclusion, surface ozone and tropospheric chemistry would likely be affected by SRM, but the overall effect is strongly dependent on the SRM scheme. Due to the health and economic impacts of surface ozone, all these impacts should be taken into account in evaluations of possible consequences of SRM.

scholarly journals Update and evaluation of the ozone dry deposition in the Oslo CTM3 v1.0

2019 ◽  
Author(s):  
Stefanie Falk ◽  
Amund Søvde Haslerud
Keyword(s):  
Dry Deposition ◽  
Surface Ozone ◽  
High Sensitivity ◽  
Ambient Air ◽  
Limiting Factors ◽  
Model Studies ◽  
Ozone Concentrations ◽  
The Future ◽  
Ozone Depleting Substances ◽  
The Impact

Abstract. High concentrations of ozone in ambient air are hazardous not only to humans but to the ecosystem in general. The impact of ozone damage on vegetation and agricultural plants in combination with advancing climate change may affect food security in the future. While the future scenarios in themselves are uncertain, there are limiting factors constraining the accuracy of surface ozone modeling also at present: The distribution and amount of ozone precursors and ozone depleting substances, the stratosphere-troposphere exchange as well as scavenging processes. Removal of any substance through gravitational settling or by uptake by plants and soil is referred to as dry deposition. The process of dry deposition is important for predicting surface ozone concentrations and understanding the observed amount and increase of tropospheric background ozone. The conceptual dry deposition velocities are calculated following a resistance-analogous approach wherein aerodynamic, quasi laminar, and canopy resistances are key components, but these are hard to measure explicitly. In this paper, we present an update of the dry deposition scheme implemented in the Oslo CTM3. We change from a purely empirical dry deposition parameterization to a more process-based one which is taking the state of the atmosphere and vegetation into account. Examining the sensitivity of the scheme to various parameters, our focus lies mainly on the stomatal conductance-based description of the canopy resistance. We evaluate the resulting modeled ozone dry deposition with respect to observations and multi-model studies and also estimate the impact on the modeled ozone concentrations at the surface. We show that the global annual total ozone dry deposition decreases with respect to the previous model version (−47 %), leading to an increase in surface ozone of up to 100 %. While high sensitivity to changes in dry deposition to vegetation is found in the tropics, the largest impact on global scales is associated to changes in dry deposition to the ocean and deserts.

scholarly journals Fifty years of balloon-borne ozone profile measurements at Uccle, Belgium: a short history, the scientific relevance, and the achievements in understanding the vertical ozone distribution

2021 ◽  
Vol 21 (16) ◽  
pp. 12385-12411
Author(s):  
Roeland Van Malderen ◽  
Dirk De Muer ◽  
Hugo De Backer ◽  
Deniz Poyraz ◽  
Willem W. Verstraeten ◽  
...  
Keyword(s):  
Time Series ◽  
Tropospheric Ozone ◽  
Stratospheric Ozone ◽  
Surface Ozone ◽  
Temporal Stability ◽  
Multiple Linear Regression Model ◽  
Perfect Agreement ◽  
Ozone Concentrations ◽  
Satellite Platform ◽  
Ozone Profile

Abstract. Starting in 1969 and comprising three launches a week, the Uccle (Brussels, Belgium) ozonesonde dataset is one of longest and densest in the world. Moreover, as the only major change was the switch from Brewer-Mast (BM) to electrochemical concentration cell (ECC) ozonesonde types in 1997 (when the emissions of ozone-depleting substances peaked), the Uccle time series is very homogenous. In this paper, we briefly describe the efforts that were undertaken during the first 3 decades of the 50 years of ozonesonde observations to guarantee the homogeneity between ascent and descent profiles, under changing environmental conditions (e.g. SO2), and between the different ozonesonde types. This paper focuses on the 50-year-long Uccle ozonesonde dataset and aims to demonstrate its past, present, and future relevance to ozone research in two application areas: (i) the assessment of the temporal evolution of ozone from the surface to the (middle) stratosphere, and (ii) as the backbone for validation and stability analysis of both stratospheric and tropospheric satellite ozone retrievals. Using the Long-term Ozone Trends and Uncertainties in the Stratosphere (LOTUS) multiple linear regression model (SPARC/IO3C/GAW, 2019), we found that the stratospheric ozone concentrations at Uccle have declined at a significant rate of around 2 % per decade since 1969, which is also rather consistent over the different stratospheric levels. This overall decrease can mainly be assigned to the 1969–1996 period with a rather consistent rate of decrease of around −4 % per decade. Since 2000, a recovery of between +1 % per decade and +3 % per decade of the stratospheric ozone levels above Uccle has been observed, although it is not significant and is not seen for the upper stratospheric levels measured by ozonesondes. Throughout the entire free troposphere, a very consistent increase in the ozone concentrations of 2 % per decade to 3 % per decade has been measured since both 1969 and 1995, with the trend since 1995 being in almost perfect agreement with the trends derived from the In-service Aircraft for a Global Observing System (IAGOS) ascent/descent profiles at Frankfurt. As the number of tropopause folding events in the Uccle time series has increased significantly over time, increased stratosphere-to-troposphere transport of recovering stratospheric ozone might partly explain these increasing tropospheric ozone concentrations, despite the levelling-off of (tropospheric) ozone precursor emissions and notwithstanding the continued increase in mean surface ozone concentrations. Furthermore, we illustrate the crucial role of ozonesonde measurements for the validation of satellite ozone profile retrievals. With the operational validation of the Global Ozone Monitoring Experiment-2 (GOME-2), we show how the Uccle dataset can be used to evaluate the performance of a degradation correction for the MetOp-A/GOME-2 UV (ultraviolet) sensors. In another example, we illustrate that the Microwave Limb Sounder (MLS) overpass ozone profiles in the stratosphere agree within ±5 % with the Uccle ozone profiles between 10 and 70 hPa. Another instrument on the same Aura satellite platform, the Tropospheric Emission Spectrometer (TES), is generally positively biased with respect to the Uccle ozonesondes in the troposphere by up to ∼ 10 ppbv, corresponding to relative differences of up to ∼ 15 %. Using the Uccle ozonesonde time series as a reference, we also demonstrate that the temporal stability of those last two satellite retrievals is excellent.

scholarly journals Unraveling Pathways of Elevated Ozone Induced by the 2020 Lockdown in Europe by an Observationally Constrained Regional Model: Non-Linear Joint Inversion of NO<sub>x</sub> and VOC Emissions using TROPOMI

2021 ◽  
Author(s):  
Amir H. Souri ◽  
Kelly Chance ◽  
Juseon Bak ◽  
Caroline R. Nowlan ◽  
Gonzalo González Abad ◽  
...  
Keyword(s):  
Central Europe ◽  
Joint Inversion ◽  
Surface Ozone ◽  
Ozone Production ◽  
Anthropogenic Emissions ◽  
Nox Emissions ◽  
Physical Processes ◽  
Model Estimate ◽  
Large Variability ◽  
Voc Emissions

Abstract. Questions about how emissions are changing during the COVID-19 lockdown periods cannot be answered by observations of atmospheric trace gas concentrations alone, in part due to simultaneous changes in atmospheric transport, emissions, dynamics, photochemistry, and chemical feedback. A chemical transport model simulation benefiting from a multi-species inversion framework using well-characterized observations should differentiate those influences enabling to closely examine changes in emissions. This approach has another advantage in that we can, to a certain extent, disentangle the chemical and physical processes involved in the formation of ozone. Accordingly, we jointly constrain NOx and VOC emissions using well-characterized TROPOMI HCHO and NO2 columns during the months of March, April, and May 2020 (lockdown) and 2019 (baseline). We observe a noticeable decline in the magnitude of NOx emissions in March 2020 (14–31 %) in several major cities including Paris, London, Madrid, and Milan expanding further to Rome, Brussels, Frankfurt, Warsaw, Belgrade, Kyiv, and Moscow (34–51 %) in April. The large variability of changes in NOx emissions is indicative of different dates and the degree of restrictions enacted to prevent the spread of the virus. For instance, NOx emissions remain at somewhat similar values or even higher in northern Germany and Moscow in March 2020 compared to the baseline. Comparisons against surface monitoring stations indicate that the model estimate of the NO2 reduction is underestimated, a picture that correlates with the TROPOMI frequency impacted by cloudiness. During the month of April, when ample TROPOMI samples are present, the surface NO2 reductions occurring in polluted areas are described fairly well by the model (model: −21 ± 17 %, observation: −29 ± 21 %). Changes in VOC emissions are dominated by eastern European biomass burning activities and biogenic isoprene emissions. In March, however, TROPOMI HCHO sets an upper limit for HCHO changes such that the chemical feedback of NOx on HCHO constrained by TROPOMI NO2 reveals a non-negligible decline in anthropogenic VOC emissions in Paris (−9 %), Milan (−29 %), London (−5 %), and Rome (−5 %). Results support an increase in surface ozone during the lockdown. In April, the constrained model features a reasonable agreement with maximum daily 8 h average (MDA8) ozone changes observed at the surface (r = 0.43), specifically over central Europe where ozone enhancements prevail (model: +3.73 ± 3.94 %, +1.79 ppbv, observation: +7.35 ± 11.27 %, +3.76 ppbv). Results of integrated process rates of MDA8 surface ozone over central Europe in the same month suggest that physical processes (dry deposition, advection and diffusion) decrease ozone on average by −4.83 ppbv, while ozone production rates dampened by largely negative JNO2[NO2]-kNO+O3[NO][O3] become less negative, leading ozone to increase by +5.89 ppbv. Experiments involving fixed anthropogenic emissions suggest that meteorology (mainly as air temperature and photolysis) contributes to 42 % enhancement in MDA8 surface ozone over the same region with the remaining part (58 %) coming from changes in anthropogenic emissions. Results illustrate the capability of satellite data of major ozone precursors to help atmospheric models capture the essential character of ozone changes induced by abrupt emission anomalies.

scholarly journals Improving NO<sub>2</sub> and ozone simulations through global NO<sub><i>x</i></sub> emission inversions

2020 ◽  
Author(s):  
Zhen Qu ◽  
Daven K. Henze ◽  
Owen R. Cooper ◽  
Jessica L. Neu
Keyword(s):  
Tropospheric Ozone ◽  
Surface Ozone ◽  
Nox Emissions ◽  
Regional Models ◽  
Top Down ◽  
Double Peak ◽  
The Us ◽  
Ozone Trends ◽  
Remote Sites ◽  
Temporal Focus

Abstract. Tropospheric ozone simulations have large uncertainties, but their biases, seasonality and trends can be improved with more accurate estimates of precursor gas emissions. We perform global top-down estimates of monthly NOx emissions using two OMI NO2 retrievals (NASAv3 and DOMINOv2) from 2005 to 2016 through a hybrid 4D-Var/mass balance inversion. The 12-year averages of regional NOx budgets from the NASA posterior emissions are 37 % to 53 % smaller than the DOMINO posterior. Compared to surface NO2 measurements, GEOS-Chem adjoint NO2 simulations using the DOMINO posterior NOx emissions have smaller biases in China (by 15 %) and the US (by 22 %), but NO2 trends have more consistent decreases (by 26 %) with the measurements (by 32 %) in the US from 2006 to 2016 when using the NASA posterior. The two posterior NOx emissions datasets have different strengths with respect to simulation of ozone concentrations. Simulations using NASA-based emissions provide better agreement for polluted conditions. Ozone from these shows the highest correlation (R2 = 0.88) with annual MDA8 ozone trends and alleviates the double peak in the prior simulation of global ozone seasonality. The DOMINO-based emissions, on the other hand, are better for simulating ozone at remote sites, making them well-suited to generation of boundary conditions for regional models, and in capturing the interannual variability of daytime-average (R2 = 0.72–0.81) and 24-hour average (R2 = 0.88–0.96) surface ozone. We recommend using NOx emission datasets that have the best performance in the corresponding spatial domain and temporal focus to improve ozone simulations.

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