ALBERT

Description: The recent update on the US National Ambient Air Quality Standards (NAAQS) of the ground-level ozone (O3) can benefit from a better understanding of its source contributions in different US regions during recent years. In the Hemispheric Transport of Air Pollution experiment phase 1 (HTAP1), various global models were used to determine the O3 source–receptor (SR) relationships among three continents in the Northern Hemisphere in 2001. In support of the HTAP phase 2 (HTAP2) experiment that studies more recent years and involves higher-resolution global models and regional models' participation, we conduct a number of regional-scale Sulfur Transport and dEposition Model (STEM) air quality base and sensitivity simulations over North America during May–June 2010. STEM's top and lateral chemical boundary conditions were downscaled from three global chemical transport models' (i.e., GEOS-Chem, RAQMS, and ECMWF C-IFS) base and sensitivity simulations in which the East Asian (EAS) anthropogenic emissions were reduced by 20 %. The mean differences between STEM surface O3 sensitivities to the emission changes and its corresponding boundary condition model's are smaller than those among its boundary condition models, in terms of the regional/period-mean (

Description: This study is based on model results from TF HTAP (Task Force on Hemispheric Transport of Air Pollution) phase II, in which a set of source receptor model experiments have been defined, reducing global (and regional) anthropogenic emissions by 20 % in different source regions throughout the globe, with the main focus on the year 2010. All the participating models use the same set of anthropogenic emissions. Comparisons of model results to measurements are shown for selected European surface sites and for ozone sondes, but the main focus here is on the contributions to European ozone levels from different world regions, and how and why these contributions differ depending on the model. We investigate the origins by use of a novel stepwise approach, combining simple tracer calculations and calculations of CO and O3. To highlight the differences, we analyse the vertical transects of the midlatitude effects from the 20 % emission reductions.The spread in the model results increases from the simple CO tracer to CO and then to ozone as the complexity of the physical and chemical processes involved increase. As a result of non-linear ozone chemistry, the contributions from non-European relative to European sources are larger for ozone compared to the CO and the CO tracer. For annually averaged ozone the contributions from the rest of the world is larger than the effects from European emissions alone, with the largest contributions from North America and eastern Asia. There are also considerable contributions from other nearby regions to the east and from international shipping. The calculated contributions to European annual average ozone from other major source regions relative to all contributions from all major sources (RAIR – Relative Annual Intercontinental Response) have increased from 43 % in HTAP1 to 82 % in HTAP2. This increase is mainly caused by a better definition of Europe, with increased emissions outside of Europe relative to those in Europe, and by including a nearby non-European source for external-to-Europe regions. European contributions to ozone metrics reflecting human health and ecosystem damage, which mostly accumulated in the summer months, are larger than for annual ozone. Whereas ozone from European sources peaks in the summer months, the largest contributions from non-European sources are mostly calculated for the spring months, when ozone production over the polluted continents starts to increase, while at the same time the lifetime of ozone in the free troposphere is relatively long. At the surface, contributions from non-European sources are of similar magnitude for all European subregions considered, defined as TF HTAP receptor regions (north-western, south-western, eastern and south-eastern Europe).

Description: The relative contributions of various source regions to the long-term (1980–2005) increasing trend in surface ozone (O3) over Japan were estimated by a series of tracer-tagging simulations using a global chemical transport model. The model simulated the observed increasing trend in surface O3, including its seasonal variation and geographical features, in Japan well and demonstrated the relative roles of different source regions in forming this trend. Most of the increasing trend in surface O3 over Japan ( ∼  97 %) that was simulated was explained as the sum of trends in contributions of different regions to photochemical O3 production. The increasing trend in O3 produced in China accounted for 36 % of the total increasing trend and those in the other northeast Asian regions (the Korean Peninsula, coastal regions in East Asia, and Japan) each accounted for about 12–15 %. Furthermore, the contributions of O3 created in the entire free troposphere and in western, southern, and southeastern Asian regions also increased, and their increasing trends accounted for 16 and 7 % of the total trend, respectively. The impact of interannual variations in climate, in methane concentration, and in emission of O3 precursors from different source regions on the relative contributions of O3 created in each region estimated above was also investigated. The variation of climate and the increase in methane concentration together caused the increase of photochemical O3 production in several regions, and represented about 19 % of the total increasing trend in surface O3 over Japan. The increase in emission of O3 precursors in China caused an increase of photochemical O3 production not only in China itself but also in the other northeast Asian regions and accounted for about 46 % of the total increase in surface O3 over Japan. Similarly, the relative impact of O3 precursor emission changes in the Korean Peninsula and Japan were estimated as about 16 and 4 % of the total increasing trend, respectively. The O3 precursor emission change in regions other than northeast Asia caused increases in surface O3 over Japan mainly through increasing photochemical O3 production in western, southern, and southeast Asia and the free troposphere and accounted for about 16 % of the total.

Description: The co-occurrence of heat waves and pollution events and the resulting high mortality rates emphasize the importance of the co-occurrence of pollution and temperature extremes. Through the use of extreme value theory and other statistical methods, tropospheric surface ozone and temperature extremes and their joint occurrence are analyzed over the United States during the summer months (JJA) using measurements and simulations of the present and future climate and chemistry. Five simulations from the Chemistry-Climate Model Initiative (CCMI) reference experiment using specified dynamics (REFC1SD) were analyzed: the CESM1 CAM4-chem, CHASER, CMAM, MOCAGE and MRI-ESM1r1 simulations. In addition, a 25-year present-day simulation branched off the CCMI REFC2 simulation in the year 2000 and a 25-year future simulation branched off the CCMI REFC2 simulation in 2100 were analyzed using CESM1 CAM4-chem. The last two simulations differed in their concentration of carbon dioxide (representative of the years 2000 and 2100) but were otherwise identical. In general, regions with relatively high ozone extremes over the US do not occur in regions of relatively high temperature extremes. A new metric, the spectral density, is developed to measure the joint extremal dependence of ozone and temperature by evaluating the spectral dependence of their extremes. While in many areas of the country ozone and temperature are highly correlated overall, the correlation is significantly reduced when examined on the higher end of the distributions. Measures of spectral density are less than about 0.35 everywhere, suggesting that at most only about a third of the time do extreme temperatures coincide with extreme ozone. Two regions of the US have the strongest measured extreme dependence of ozone and temperature: the northeast and the southeast. The simulated future increase in temperature and ozone is primarily due to a shift in their distributions, not to an increase in their extremes. The locations where the right-hand side of the temperature distribution does increase (by up to 30 %) are consistent with locations where soil–moisture feedback may be expected. Future changes in the right-hand side of the ozone distribution range regionally between +20 % and −10 %. The location of future increases in the high-end tail of the ozone distribution are weakly related to those of temperature with a correlation of 0.3. However, the regions where the temperature extremes increase are not located where the extremes in ozone are large, suggesting a muted ozone response.

Description: In this study we introduce a hybrid ensemble consisting of air quality models operating at both the global and regional scale. The work is motivated by the fact that these different types of models treat specific portions of the atmospheric spectrum with different levels of detail, and it is hypothesized that their combination can generate an ensemble that performs better than mono-scale ensembles. A detailed analysis of the hybrid ensemble is carried out in the attempt to investigate this hypothesis and determine the real benefit it produces compared to ensembles constructed from only global-scale or only regional-scale models. The study utilizes 13 regional and 7 global models participating in the Hemispheric Transport of Air Pollutants phase 2 (HTAP2)–Air Quality Model Evaluation International Initiative phase 3 (AQMEII3) activity and focuses on surface ozone concentrations over Europe for the year 2010. Observations from 405 monitoring rural stations are used for the evaluation of the ensemble performance. The analysis first compares the modelled and measured power spectra of all models and then assesses the properties of the mono-scale ensembles, particularly their level of redundancy, in order to inform the process of constructing the hybrid ensemble. This study has been conducted in the attempt to identify that the improvements obtained by the hybrid ensemble relative to the mono-scale ensembles can be attributed to its hybrid nature. The improvements are visible in a slight increase of the diversity (4 % for the hourly time series, 10 % for the daily maximum time series) and a smaller improvement of the accuracy compared to diversity. Root mean square error (RMSE) improved by 13–16 % compared to G and by 2–3 % compared to R. Probability of detection (POD) and false-alarm rate (FAR) show a remarkable improvement, with a steep increase in the largest POD values and smallest values of FAR across the concentration ranges. The results show that the optimal set is constructed from an equal number of global and regional models at only 15 % of the stations. This implies that for the majority of the cases the regional-scale set of models governs the ensemble. However given the high degree of redundancy that characterizes the regional-scale models, no further improvement could be expected in the ensemble performance by adding yet more regional models to it. Therefore the improvement obtained with the hybrid set can confidently be attributed to the different nature of the global models. The study strongly reaffirms the importance of an in-depth inspection of any ensemble of opportunity in order to extract the maximum amount of information and to have full control over the data used in the construction of the ensemble.

Description: An assessment of global particulate nitrate and ammonium aerosol based on simulations from nine models participating in the Aerosol Comparisons between Observations and Models (AeroCom) phase III study is presented. A budget analysis was conducted to understand the typical magnitude, distribution, and diversity of the aerosols and their precursors among the models. To gain confidence regarding model performance, the model results were evaluated with various observations globally, including ground station measurements over North America, Europe, and east Asia for tracer concentrations and dry and wet depositions, as well as with aircraft measurements in the Northern Hemisphere mid-to-high latitudes for tracer vertical distributions. Given the unique chemical and physical features of the nitrate occurrence, we further investigated the similarity and differentiation among the models by examining (1) the pH-dependent NH3 wet deposition; (2) the nitrate formation via heterogeneous chemistry on the surface of dust and sea salt particles or thermodynamic equilibrium calculation including dust and sea salt ions; and (3) the nitrate coarse-mode fraction (i.e., coarse/total). It is found that HNO3, which is simulated explicitly based on full O3-HOx-NOx-aerosol chemistry by all models, differs by up to a factor of 9 among the models in its global tropospheric burden. This partially contributes to a large difference in NO3−, whose atmospheric burden differs by up to a factor of 13. The atmospheric burdens of NH3 and NH4+ differ by 17 and 4, respectively. Analyses at the process level show that the large diversity in atmospheric burdens of NO3−, NH3, and NH4+ is also related to deposition processes. Wet deposition seems to be the dominant process in determining the diversity in NH3 and NH4+ lifetimes. It is critical to correctly account for contributions of heterogeneous chemical production of nitrate on dust and sea salt, because this process overwhelmingly controls atmospheric nitrate production (typically 〉 80 %) and determines the coarse- and fine-mode distribution of nitrate aerosol.

Description: This study uses multi-model ensemble results of 11 models from the second phase of Task Force Hemispheric Transport of Air Pollution (HTAP II) to calculate the global sulfur (S) and nitrogen (N) deposition in 2010. Modeled wet deposition is evaluated with observation networks in North America, Europe and East Asia. The modeled results agree well with observations, with 76–83 % of stations being predicted within ±50 % of observations. The models underestimate SO42-, NO3- and NH4+ wet depositions in some European and East Asian stations but overestimate NO3- wet deposition in the eastern United States. Intercomparison with previous projects (PhotoComp, ACCMIP and HTAP I) shows that HTPA II has considerably improved the estimation of deposition at European and East Asian stations. Modeled dry deposition is generally higher than the “inferential” data calculated by observed concentration and modeled velocity in North America, but the inferential data have high uncertainty, too. The global S deposition is 84 Tg(S) in 2010, with 49 % in continental regions and 51 % in the ocean (19 % of which coastal). The global N deposition consists of 59 Tg(N) oxidized nitrogen (NOy) deposition and 64 Tg(N) reduced nitrogen (NHx) deposition in 2010. About 65 % of N is deposited in continental regions, and 35 % in the ocean (15 % of which coastal). The estimated outflow of pollution from land to ocean is about 4 Tg(S) for S deposition and 18 Tg(N) for N deposition. Comparing our results to the results in 2001 from HTAP I, we find that the global distributions of S and N deposition have changed considerably during the last 10 years. The global S deposition decreases 2 Tg(S) (3 %) from 2001 to 2010, with significant decreases in Europe (5 Tg(S) and 55 %), North America (3 Tg(S) and 29 %) and Russia (2 Tg(S) and 26 %), and increases in South Asia (2 Tg(S) and 42 %) and the Middle East (1 Tg(S) and 44 %). The global N deposition increases by 7 Tg(N) (6 %), mainly contributed by South Asia (5 Tg(N) and 39 %), East Asia (4 Tg(N) and 21 %) and Southeast Asia (2 Tg(N) and 21 %). The NHx deposition increases with no control policy on NH3 emission in North America. On the other hand, NOy deposition has started to dominate in East Asia (especially China) due to boosted NOx emission.

Description: Global surface emissions of nitrogen oxides (NOx) over a 10-year period (2005–2014) are estimated from an assimilation of multiple satellite data sets: tropospheric NO2 columns from Ozone Monitoring Instrument (OMI), Global Ozone Monitoring Experiment-2 (GOME-2), and Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY), O3 profiles from Tropospheric Emission Spectrometer (TES), CO profiles from Measurement of Pollution in the Troposphere (MOPITT), and O3 and HNO3 profiles from Microwave Limb Sounder (MLS) using an ensemble Kalman filter technique. Chemical concentrations of various species and emission sources of several precursors are simultaneously optimized. This is expected to improve the emission inversion because the emission estimates are influenced by biases in the modelled tropospheric chemistry, which can be partly corrected by also optimizing the concentrations. We present detailed distributions of the estimated emission distributions for all major regions, the diurnal and seasonal variability, and the evolution of these emissions over the 10-year period. The estimated regional total emissions show a strong positive trend over India (+29 % decade−1), China (+26 % decade−1), and the Middle East (+20 % decade−1), and a negative trend over the USA (−38 % decade−1), southern Africa (−8.2 % decade−1), and western Europe (−8.8 % decade−1). The negative trends in the USA and western Europe are larger during 2005–2010 relative to 2011–2014, whereas the trend in China becomes negative after 2011. The data assimilation also suggests a large uncertainty in anthropogenic and fire-related emission factors and an important underestimation of soil NOx sources in the emission inventories. Despite the large trends observed for individual regions, the global total emission is almost constant between 2005 (47.9 Tg N yr−1) and 2014 (47.5 Tg N yr−1).

Description: Here we present results from an evaluation of model simulations from the International Hemispheric Transport of Air Pollution Phase II (HTAPII) and Chemistry Climate Model Initiative (CCMI) model inter-comparison projects against a comprehensive series of ground-based, aircraft and satellite observations of ozone mixing ratios made at various locations across India. The study focuses on the recent past (observations from 2008 to 2013, models from 2009–2010) as this is most pertinent to understanding the health impacts of ozone. To our understanding this is the most comprehensive evaluation of these models' simulations of ozone across the Indian subcontinent to date. This study highlights some significant successes and challenges that the models face in representing the oxidative chemistry of the region. The multi-model range in area-weighted surface ozone over the Indian subcontinent is 37.26–56.11 ppb, whilst the population-weighted range is 41.38–57.5 ppb. When compared against surface observations from the Modelling Atmospheric Pollution and Networking (MAPAN) network of eight semi-urban monitoring sites spread across India, we find that the models tend to simulate higher ozone than that which is observed. However, observations of NOx and CO tend to be much higher than modelled mixing ratios, suggesting that the underlying emissions used in the models do not characterise these regions accurately and/or that the resolution of the models is not adequate to simulate the photo-chemical environment of these surface observations. Empirical orthogonal function (EOF) analysis is used in order to identify the extent to which the models agree with regards to the spatio-temporal distribution of the tropospheric ozone column, derived using OMI-MLS observations. We show that whilst the models agree with the spatial pattern of the first EOF of observed tropospheric ozone column, most of the models simulate a peak in the first EOF seasonal cycle represented by principle component 1, which is later than the observed peak. This suggests a widespread systematic bias in the timing of emissions or some other unknown seasonal process. In addition to evaluating modelled ozone mixing ratios, we explore modelled emissions of NOx, CO, volatile organic compounds (VOCs) and the ozone response to the emissions. We find a high degree of variation in emissions from non-anthropogenic sources (e.g. lightning NOx and biomass burning CO) between models. Total emissions of NOx and CO over India vary more between different models in the same model intercomparison project (MIP) than the same model used in different MIPs, making it impossible to diagnose whether differences in modelled ozone are due to emissions or model processes. We therefore recommend targeted experiments to pinpoint the exact causes of discrepancies between modelled and observed ozone and ozone precursors for this region. To this end, a higher density of long-term monitoring sites measuring not only ozone but also ozone precursors including speciated VOCs, located in more rural regions of the Indian subcontinent, would enable improvements in assessing the biases in models run at the resolution found in HTAPII and CCMI.

Description: Constraints from ozone (O3) observations over oceans are needed in addition to those from terrestrial regions to fully understand global tropospheric chemistry and its impact on the climate. Here, we provide a large data set of ozone and carbon monoxide (CO) levels observed (for 11 666 and 10 681 h, respectively) over oceans. The data set is derived from observations made during 24 research cruise legs of R/V Mirai during 2012 to 2017, in the Southern, Indian, Pacific, and Arctic oceans, covering the region from 67∘ S to 75∘ N. The data are suitable for critical evaluation of the over-ocean distribution of ozone derived from global atmospheric chemistry models. We first give an overview of the statistics in the data set and highlight key features in terms of geographical distribution and air mass type. We then use the data set to evaluate ozone mixing ratio fields from the tropospheric chemistry reanalysis version 2 (TCR-2), produced by assimilating a suite of satellite observations of multiple species into a global atmospheric chemistry model, namely CHASER. For long-range transport of polluted air masses from continents to the oceans, during which the effects of forest fires and fossil fuel combustion were recognized, TCR-2 gave an excellent performance in reproducing the observed temporal variations and photochemical buildup of O3 when assessed from ΔO3∕ΔCO ratios. For clean marine conditions with low and stable CO mixing ratios, two focused analyses were performed. The first was in the Arctic (〉 70∘ N) in September every year from 2013 to 2016; TCR-2 underpredicted O3 levels by 6.7 ppbv (21 %) on average. The observed vertical profiles from O3 soundings from R/V Mirai during September 2014 had less steep vertical gradients at low altitudes (〉 850 hPa) than those obtained by TCR-2. This suggests the possibility of a more efficient descent of the O3-rich air from above than assumed in the models. For TCR-2 (CHASER), dry deposition on the Arctic ocean surface might also have been overestimated. In the second analysis, over the western Pacific equatorial region (125–165∘ E, 10∘ S to 25∘ N), the observed O3 level more frequently decreased to less than 10 ppbv in comparison to that obtained with TCR-2 and also those obtained in most of the Atmospheric Chemistry Climate Model Intercomparison Project (ACCMIP) model runs for the decade from 2000. These results imply loss processes that are unaccounted for in the models. We found that the model's positive bias positively correlated with the daytime residence times of air masses over a particular grid, namely 165–180∘ E and 15–30∘ N; an additional loss rate of 0.25 ppbv h−1 in the grid best explained the gap. Halogen chemistry, which is commonly omitted from currently used models, might be active in this region and could have contributed to additional losses. Our open data set covering wide ocean regions is complementary to the Tropospheric Ozone Assessment Report data set, which basically comprises ground-based observations and enables a fully global study of the behavior of O3.