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The ability of a coupled meteorology–chemistry model, i.e., Weather Research and Forecast and Community Multiscale Air Quality (WRF-CMAQ), to reproduce the historical trend in aerosol optical depth (AOD) and clear-sky shortwave radiation (SWR) over the Northern Hemisphere has been evaluated through a comparison of 21-year simulated results with observation-derived records from 1990 to 2010. Six satellite-retrieved AOD products including AVHRR, TOMS, SeaWiFS, MISR, MODIS-Terra and MODIS-Aqua as well as long-term historical records from 11 AERONET sites were used for the comparison of AOD trends. Clear-sky SWR products derived by CERES at both the top of atmosphere (TOA) and surface as well as surface SWR data derived from seven SURFRAD sites were used for the comparison of trends in SWR. The model successfully captured increasing AOD trends along with the corresponding increased TOA SWR (upwelling) and decreased surface SWR (downwelling) in both eastern China and the northern Pacific. The model also captured declining AOD trends along with the corresponding decreased TOA SWR (upwelling) and increased surface SWR (downwelling) in the eastern US, Europe and the northern Atlantic for the period of 2000–2010. However, the model underestimated the AOD over regions with substantial natural dust aerosol contributions, such as the Sahara Desert, Arabian Desert, central Atlantic and northern Indian Ocean. Estimates of the aerosol direct radiative effect (DRE) at TOA are comparable with those derived by measurements. Compared to global climate models (GCMs), the model exhibits better estimates of surface-aerosol direct radiative efficiency (<i>E</i><sub>τ</sub>). However, surface-DRE tends to be underestimated due to the underestimated AOD in land and dust regions. Further investigation of TOA-<i>E</i><sub>τ</sub> estimations as well as the dust module used for estimates of windblown-dust emissions is needed.
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Trends in the vertical distribution of ozone are reported and compared for a number of new and recently revised data sets. The amount of ozone-depleting compounds in the stratosphere (as measured by equivalent effective stratospheric chlorine – EESC) was maximised in the second half of the 1990s. We examine the periods before and after the peak to see if any change in trend is discernible in the ozone record that might be attributable to a change in the EESC trend, though no attribution is attempted. Prior to 1998, trends in the upper stratosphere (~ 45 km, 4 hPa) are found to be −5 to −10 % per decade at mid-latitudes and closer to −5 % per decade in the tropics. No trends are found in the mid-stratosphere (28 km, 30 hPa). Negative trends are seen in the lower stratosphere at mid-latitudes in both hemispheres and in the deep tropics. However, it is hard to be categorical about the trends in the lower stratosphere for three reasons: (i) there are fewer measurements, (ii) the data quality is poorer, and (iii) the measurements in the 1990s are perturbed by aerosols from the Mt Pinatubo eruption in 1991. These findings are similar to those reported previously even though the measurements for the main satellite and ground-based records have been revised. <br><br> There is no sign of a continued negative trend in the upper stratosphere since 1998: instead there is a hint of an average positive trend of ~ 2 % per decade in mid-latitudes and ~ 3 % per decade in the tropics. The significance of these upward trends is investigated using different assumptions of the independence of the trend estimates found from different data sets. The averaged upward trends are significant if the trends derived from various data sets are assumed to be independent (as in Pawson et al., 2014) but are generally not significant if the trends are not independent. This occurs because many of the underlying measurement records are used in more than one merged data set. At this point it is not possible to say which assumption is best. Including an estimate of the drift of the overall ozone observing system decreases the significance of the trends. The significance will become clearer as (i) more years are added to the observational record, (ii) further improvements are made to the historic ozone record (e.g. through algorithm development), and (iii) the data merging techniques are refined, particularly through a more rigorous treatment of uncertainties.
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Hydrocarbons are key precursors to two priority air pollutants, ozone and particulate matter. Those with two to seven carbons have historically been straightforward to observe and have been successfully reduced in many developed cities through air quality policy interventions. Longer chain hydrocarbons released from diesel vehicles are not considered explicitly as part of air quality strategies and there are few direct measurements of their gaseous abundance in the atmosphere. This study describes the chemically comprehensive and continuous measurements of organic compounds in a developed megacity (London), which demonstrate that on a seasonal median basis, diesel-related hydrocarbons represent only 20–30 % of the total hydrocarbon mixing ratio but comprise more than 50 % of the atmospheric hydrocarbon mass and are a dominant local source of secondary organic aerosols. This study shows for the first time that 60 % of the winter primary hydrocarbon hydroxyl radical reactivity is from diesel-related hydrocarbons and using the maximum incremental reactivity scale, we predict that they contribute up to 50 % of the ozone production potential in London. Comparing real-world urban composition with regulatory emissions inventories in the UK and US highlights a previously unaccounted for, but very significant, under-reporting of diesel-related hydrocarbons; an underestimation of a factor ~4 for C<sub>9</sub> species rising to a factor of over 70 for C<sub>12</sub> during winter. These observations show that hydrocarbons from diesel vehicles can dominate gas phase reactive carbon in cities with high diesel fleet fractions. Future control of urban particulate matter and ozone in such locations requires a shift in policy focus onto gas phase hydrocarbons released from diesels as this vehicle type continues to displace gasoline world-wide.
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Upwelling branch of the Brewer–Dobson circulation (BDC) controls the tropical lower stratospheric water vapor (WV) through dynamic cooling near the tropopause. Downwelling branch of BDC dominates the extratropical middle-lower stratospheric Hydrogen Chloride (HCl) by dynamic transport. Climatologically, a symmetric weakening BDC indicates increasing tropical lower stratospheric WV and decreasing extratropical middle-lower stratospheric HCl. However, the global ozone chemistry and related trace gas data records for the stratosphere data (GOZCARDS) show that the tropical lowermost stratospheric WV increased by 18 % decade<sup>−1</sup> during 2001–2011 and the boreal mid-latitude lower stratospheric HCl rose 25 % decade<sup>−1</sup> after 2006. We interpret this as resulting from a slowdown of the tropical upwelling and a speedup of the mid-latitude downwelling. This interpretation is supported by composite analysis of Eliasen–Palm Flux (EPF), zonal wind and regression of temperature on the EPF from the ERA-Interim data. Results present that the enhancing polar vortex and weakening planetary wave activity leads to a downwelling branch narrowing equatorward and a local speedup of 24 % at 20 hPa in the mid-latitudes. Moreover, there are regressive temperature increase of 1.5 K near the tropical tropopause and that of 0.5 K in the mid-latitude middle stratosphere, which also indicates the tropical upwelling slowdown and the mid-latitude downwelling speedup during 2001–2011.
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We estimate future area burned in the Alaskan and Canadian forest by the mid-century (2046–2065) based on the simulated meteorology from 13 climate models under the A1B scenario. We develop ecoregion-dependent regressions using observed relationships between annual total area burned and a suite of meteorological variables and fire weather indices, and apply these regressions to the simulated meteorology. We find that for Alaska and western Canada, almost all models predict significant (<i>p</i> < 0.05) increases in area burned at the mid-century, with median values ranging from 150 to 390 %, depending on the ecoregion. Such changes are attributed to the higher surface air temperatures and 500 hPa geopotential heights relative to present day, which together lead to favorable conditions for wildfire spread. Elsewhere the model predictions are not as robust. For the central and southern Canadian ecoregions, the models predict increases in area burned of 45–90 %. Except for the Taiga Plain, where area burned decreases by 50 %, no robust trends are found in northern Canada, due to the competing effects of hotter weather and wetter conditions there. Using the GEOS-Chem chemical transport model, we find that changes in wildfire emissions alone increase mean summertime surface ozone levels by 5 ppbv for Alaska, 3 ppbv for Canada, and 1 ppbv for the western US by the mid-century. In the northwestern US states, local wildfire emissions at the mid-century enhance surface ozone by an average of 1 ppbv, while transport of boreal fire pollution further degrades ozone air quality by an additional 0.5 ppbv. The projected changes in wildfire activity increase daily summertime surface ozone above the 95th percentile by 1 ppbv in the northwestern US, 5 ppbv in the high latitudes of Canada, and 15 ppbv in Alaska, suggesting a greater frequency of pollution episodes in the future atmosphere.
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Ozone (O<sub>3</sub>) plays an important role in chemical reactions and is usually incorporated in chemical data assimilation (DA). In tropical cyclones (TCs), O<sub>3</sub> usually shows a lower concentration inside the eyewall and an elevated concentration around the eye, impacting meteorological as well as chemical variables. To identify the impact of O<sub>3</sub> observations on TC structure, including meteorological and chemical information, we developed a coupled meteorology–chemistry DA system by employing the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) and an ensemble-based DA algorithm – the maximum likelihood ensemble filter (MLEF). For a TC case that occurred over East Asia, Typhoon Nabi (2005), our results indicate that the ensemble forecast is reasonable, accompanied with larger background state uncertainty over the TC, and also over eastern China. Similarly, the assimilation of O<sub>3</sub> observations impacts meteorological and chemical variables near the TC and over eastern China. The strongest impact on air quality in the lower troposphere was over China, likely due to the pollution advection. In the vicinity of the TC, however, the strongest impact on chemical variables adjustment was at higher levels. The impact on meteorological variables was similar in both over China and near the TC. The analysis results are verified using several measures that include the cost function, root mean square (RMS) error with respect to observations, and degrees of freedom for signal (DFS). All measures indicate a positive impact of DA on the analysis – the cost function and RMS error have decreased by 16.9 and 8.87 %, respectively. In particular, the DFS indicates a strong positive impact of observations in the TC area, with a weaker maximum over northeastern China.
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Anthropogenic atmospheric emissions of typical toxic heavy metals have caused worldwide concern due to their adverse effects on human health and the ecosystem. By determining the best available representation of time-varying emission factors with S-shape curves, we establish the multiyear comprehensive atmospheric emission inventories of 12 typical toxic heavy metals (Hg, As, Se, Pb, Cd, Cr, Ni, Sb, Mn, Co, Cu, and Zn) from primary anthropogenic activities in China for the period of 1949–2012 for the first time. Further, we allocate the annual emissions of these heavy metals in 2010 at a high spatial resolution of 0.5° × 0.5° grid with ArcGIS methodology and surrogate indexes, such as regional population and gross domestic product (GDP). Our results show that the historical emissions of Hg, As, Se, Cd, Cr, Ni, Sb, Mn, Co, Cu, and Zn, during the period of 1949–2012, increased by about 22–128 times at an annual average growth rate of 5.1–8.0 %, reaching about 526.9–22 319.6 t in 2012. Nonferrous metal smelting, coal combustion of industrial boilers, brake and tyre wear, and ferrous metal smelting represent the dominant sources of heavy metal emissions. In terms of spatial variation, the majority of emissions are concentrated in relatively developed regions, especially for the northern, eastern, and southern coastal regions. In addition, because of the flourishing nonferrous metal smelting industry, several southwestern and central-southern provinces play a prominent role in some specific toxic heavy metals emissions, like Hg in Guizhou and As in Yunnan. Finally, integrated countermeasures are proposed to minimize the final toxic heavy metals discharge on account of the current and future demand of energy-saving and pollution reduction in China.
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Positive matrix factorisation (PMF) analysis was applied to PM<sub>10</sub> chemical composition and particle number size distribution (NSD) data measured at an urban background site (North Kensington) in London, UK, for the whole of 2011 and 2012. The PMF analyses for these 2 years revealed six and four factors respectively which described seven sources or aerosol types. These included nucleation, traffic, urban background, secondary, fuel oil, marine and non-exhaust/crustal sources. Urban background, secondary and traffic sources were identified by both the chemical composition and particle NSD analysis, but a nucleation source was identified only from the particle NSD data set. Analysis of the PM<sub>10</sub> chemical composition data set revealed fuel oil, marine, non-exhaust traffic/crustal sources which were not identified from the NSD data. The two methods appear to be complementary, as the analysis of the PM<sub>10</sub> chemical composition data is able to distinguish components contributing largely to particle mass, whereas the number particle size distribution data set – although limited to detecting sources of particles below the diameter upper limit of the SMPS (604 nm) – is more effective for identifying components making an appreciable contribution to particle number. Analysis was also conducted on the combined chemical composition and NSD data set, revealing five factors representing urban background, nucleation, secondary, aged marine and traffic sources. However, the combined analysis appears not to offer any additional power to discriminate sources above that of the aggregate of the two separate PMF analyses. Day-of-the-week and month-of-the-year associations of the factors proved consistent with their assignment to source categories, and bivariate polar plots which examined the wind directional and wind speed association of the different factors also proved highly consistent with their inferred sources. Source attribution according to the air mass back trajectory showed, as expected, higher concentrations from a number of source types in air with continental origins. However, when these were weighted according to their frequency of occurrence, air with maritime origins made a greater contribution to annual mean concentrations.
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Understanding how historical climate and land cover changes have affected tropospheric ozone in East Asia would help constrain the large uncertainties associated with future East Asian air quality projections. We perform a series of simulations using a global chemical transport model driven by assimilated meteorological data and a suite of land cover and land use data to examine the public health effects associated with changes in climate, land cover, land use, and anthropogenic emissions between the 5-year periods 1981–1985 and 2007–2011 in East Asia. We find that between these two periods land cover change alone could lead to a decrease in summertime surface ozone by up to 4 ppbv in East Asia and ~ 2000 fewer ozone-related premature deaths per year, driven mostly by enhanced dry deposition resulting from climate- and CO<sub>2</sub>-induced increase in vegetation density, which more than offsets the effect of reduced isoprene emission arising from cropland expansion. Climate change alone could lead to an increase in summertime ozone by 2–10 ppbv in most regions of East Asia and ~ 6000 more premature deaths annually, mostly attributable to warming. The combined impacts (−2 to +12 ppbv) show that while the effect of climate change is more pronounced, land cover change could offset part of the climate effect and lead to a previously unknown public health benefit. While the changes in anthropogenic emissions remain the largest contributor to deteriorating ozone air quality in East Asia over the past 30 years, we show that climate change and land cover changes could lead to a substantial modification of ozone levels, and thus should come into consideration when formulating future air quality management strategies. We also show that the sensitivity of surface ozone to land cover change is more dependent on dry deposition than on isoprene emission in most of East Asia, leading to ozone responses that are quite distinct from that in North America, where most ozone-vegetation sensitivity studies to date have been conducted.
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In 1997 the International Maritime Organisation (IMO) adopted MARPOL Annex VI to prevent air pollution by shipping emissions. It regulates, among other issues, the sulfur content in shipping fuels, which is transformed into the air pollutant sulfur dioxide (SO<sub>2</sub>) during combustion. Within designated Sulfur Emission Control Areas (SECA), the sulfur content was limited to 1 %, and on 1 January 2015, this limit was further reduced to 0.1 %. Here we present the set-up and measurement results of a permanent ship emission monitoring site near Hamburg harbour in the North Sea SECA. Trace gas measurements are conducted with in situ instruments and a data set from September 2014 to January 2015 is presented. By combining measurements of carbon dioxide (CO<sub>2</sub>) and SO<sub>2</sub> with ship position data, it is possible to deduce the sulfur fuel content of individual ships passing the measurement station, thus facilitating the monitoring of compliance of ships with the IMO regulations. While compliance is almost 100 % for the 2014 data, it decreases only very little in 2015 to 95.4 % despite the much stricter limit. We analysed more than 1400 ship plumes in total and for months with favourable conditions, up to 40 % of all ships entering and leaving Hamburg harbour could be checked for their sulfur fuel content.
