Global chemical transport models (CTMs) are used extensively to study air pollution and transport at a global scale. These models are limited by coarse horizontal resolutions that do not allow for a detailed representation of small-scale nonlinear processes over the pollutant source regions. Here we couple the global GEOS-Chem CTM and its three high-resolution nested models to simulate the tropospheric carbon monoxide (CO) over the Pacific Ocean during five High-performance Instrumented Airborne Platform for Environmental Research (HIAPER) Pole-to-Pole Observations (HIPPO) campaigns between 2009 and 2011. We develop a two-way coupler, the PeKing University CouPLer (PKUCPL), allowing for the exchange and interaction of chemical constituents between the global model (at 2.5˚ long. x 2˚ lat.) and the three nested models (at 0.667˚ long. x 0.5˚ lat.) covering Asia, North America, and Europe. The coupler obtains nested model results to modify the global model simulation within the respective nested domains, and simultaneously acquires global model results to provide lateral boundary conditions (LBCs) for the nested models.

Compared to the global model alone, the two-way coupled simulation results in enhanced CO concentrations in the nested domains. Sensitivity tests suggest the enhancement to be a result of improved representation of the spatial distributions of CO, nitrogen oxides, and non-methane volatile organic compounds, the meteorological dependence of natural emissions, and other resolution-dependent processes. The relatively long lifetime of CO allows for the enhancement to be accumulated and carried across the globe. We found that the two-way coupled simulation increased the global tropospheric mean CO concentrations in 2009 by 10.4 %, with a greater enhancement at 13.3 % in the Northern Hemisphere. Coincidently, the global tropospheric mean hydroxyl radical (OH) was reduced by 4.2 %, resulting in a 4.2 % enhancement in the methyl chloroform lifetime (MCF; via reaction with tropospheric OH). The resulting CO and OH contents and MCF lifetime are closer to observation-based estimates.

Both the global and the two-way coupled models capture the general spatiotemporal patterns of HIPPO CO over the Pacific. The two-way coupled simulation is much closer to HIPPO CO, with a mean bias of 1.1 ppb (1.4 %) below 9 km compared to the bias at 7.2 ppb (9.2 %) for the global model alone. The improvement is most apparent over the North Pacific. Our test simulations show that the global model alone could resemble the two-way coupled simulation (especially below 4 km) by increasing its global CO emissions by 15 % for HIPPO-1 and HIPPO-3, by 25 % for HIPPO-2 and HIPPO-4, and by 35 % for HIPPO-5. This has important implications for using the global model alone to constrain CO emissions. Thus, the two-way coupled simulation is a significantly improved model tool for studying the global impacts of air pollutants from major anthropogenic source regions.

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Satellite retrievals of vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) normally do not explicitly account for aerosol optical effects and surface reflectance anisotropy that vary with space and time. Here, we conduct an improved retrieval of NO2 VCDs over China, called the POMINO algorithm, based on measurements from the Ozone Monitoring Instrument (OMI), and we test the importance of a number of aerosol and surface reflectance treatments in this algorithm. POMINO uses a parallelized LIDORT-driven AMFv6 package to derive tropospheric air mass factors via pixel-specific radiative transfer calculations with no look-up tables, taking slant column densities from DOMINO v2. Prerequisite cloud optical properties are derived from a dedicated cloud retrieval process that is fully consistent with the main NO2 retrieval. Aerosol optical properties are taken from GEOS-Chem simulations constrained by MODIS AOD values. MODIS bi-directional reflectance distribution function (BRDF) data are used for surface reflectance over land. For the present analysis, POMINO level-2 data for 2012 are aggregated into monthly means on a 0.25 long. x 0.25 lat. grid.

POMINO-retrieved annual mean NO2 VCDs vary from 15–25 x 10^15 cm^-2 over the polluted North China Plain (NCP) to below 10^15 cm^-2 over much of west China. The subsequently-constrained Chinese annual anthropogenic emissions are 9.05 TgN yr^-1, an increase from 2006 (Lin, 2012) by about 19%. Replacing the MODIS BRDF data with the OMLER v1 monthly climatological albedo data affect NO2 VCDs by up to 40% for certain locations and seasons. The effect on constrained NOx emissions is small. Excluding aerosol information from the retrieval process (this is the traditional “implicit” treatment) enhances annual mean NO2 VCDs by 15–40% over much of east China. Seasonally, NO2 VCDs are reduced by 10–20% over parts of the NCP in spring and over north China in winter, despite the general enhancements in summer and fall. The effect on subsequently-constrained annual emissions is (-5)–(+30)% with large seasonal and spatial dependence. The implicit aerosol treatment also tends to exclude days with high pollution, a potentially important sampling bias. Therefore an explicit treatment of aerosols is important for space-based NO2 retrievals and emission constraints.

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Small-scale nonlinear chemical and physical processes over pollution source regions affect the tropospheric ozone (O3), but these processes are not captured by current global chemical transport models (CTMs) and chemistry– climate models that are limited by coarse horizontal resolutions (100–500 km, typically 200 km). These models tend to contain large (and mostly positive) tropospheric O3 biases in the Northern Hemisphere. Here we use the recently built two-way coupling system of the GEOS-Chem CTM to simulate the regional and global tropospheric O3 in 2009. The system couples the global model (at 2.5^N long.^B2^N lat.) and its three nested models (at 0.667^N long.^B0.5^N lat.) covering Asia, North America and Europe, respectively. Specifically, the nested models take lateral boundary conditions (LBCs) from the global model, better capture small-scale processes and feed back to modify the global model simulation within the nested domains, with a subsequent effect on their LBCs.

Compared to the global model alone, the two-way coupled system better simulates the tropospheric O3 both within and outside the nested domains, as found by evaluation against a suite of ground (1420 sites from the World Data Centre for Greenhouse Gases (WDCGG), the United States National Oceanic and Atmospheric Administration (NOAA) Earth System Research Laboratory Global Monitoring Division (GMD), the Chemical Coordination Centre of European Monitoring and Evaluation Programme (EMEP), and the United States Environmental Protection Agency Air Quality System (AQS)), aircraft (the High-performance Instrumented Airborne Platform for Environmental Research (HIAPER) Pole-to-Pole Observations (HIPPO) and Measurement of Ozone and Water Vapor by Airbus In- Service Aircraft (MOZAIC)) and satellite measurements (two Ozone Monitoring Instrument (OMI) products). The two-way coupled simulation enhances the correlation in day-to-day variation of afternoon mean surface O3 with the ground measurements from 0.53 to 0.68, and it reduces the mean model bias from 10.8 to 6.7 ppb. Regionally, the coupled system reduces the bias by 4.6 ppb over Europe, 3.9 ppb over North America and 3.1 ppb over other regions. The two-way coupling brings O3 vertical profiles much closer to the HIPPO (for remote areas) and MOZAIC (for polluted regions) data, reducing the tropospheric (0–9 km) mean bias by 3–10 ppb at most MOZAIC sites and by 5.3 ppb for HIPPO profiles. The twoway coupled simulation also reduces the global tropospheric column ozone by 3.0DU (9.5 %, annual mean), bringing them closer to the OMI data in all seasons. Additionally, the two-way coupled simulation also reduces the global tropospheric mean hydroxyl radical by 5% with improved estimates of methyl chloroform and methane lifetimes. Simulation improvements are more significant in the Northern Hemisphere, and are mainly driven by improved representation of spatial inhomogeneity in chemistry/emissions.

Within the nested domains, the two-way coupled simulation reduces surface ozone biases relative to typical GEOSChem one-way nested simulations, due to much improved LBCs. The bias reduction is 1–7 times the bias reduction from the global to the one-way nested simulation. Improving model representations of small-scale processes is important for understanding the global and regional tropospheric chemistry.

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International trade separates regions consuming goods and services from regions where goods and related aerosol pollution are produced. Yet the role of trade in aerosol climate forcing attributed to di^[erent regions has never been quantified. Here, we contrast the direct radiative forcing of aerosols related to regions’ consumption of goods and services against the forcing due to emissions produced in each region. Aerosols assessed include black carbon, primary organic aerosol, and secondary inorganic aerosols, including sulfate, nitrate and ammonium. We find that global aerosol radiative forcing due to emissions produced in East Asia is much stronger than the forcing related to goods and services ultimately consumed in that region because of its large net export of emissions-intensive goods. The opposite is true for net importers such as Western Europe and North America: global radiative forcing related to consumption is much greater than the forcing due to emissions produced in these regions. Overall, trade is associated with a shift of radiative forcing from net importing to net exporting regions. Compared to greenhouse gases such as carbon dioxide, the short atmospheric lifetimes of aerosols cause large localized di^[erences between consumption- and production-related radiative forcing. International e^[orts to reduce emissions in the exporting countries will help alleviate trade-related climate and health impacts of aerosols while lowering global emissions.

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Western China has experienced rapid industrialization and urbanization since the implementation of the National Western Development Strategies (the “Go West” movement) in 1999. This transition has affected the spatial and temporal characteristics of nitrogen dioxide (NO2) pollution. In this study, we analyze the trends and variability of tropospheric NO2 vertical column densities (VCDs) from 2005 to 2013 over Western China, based on a wavelet analysis on monthly mean NO2 data derived from the Ozone Monitoring Instrument (OMI) measurements. We focus on the anthropogenic NO2 by subtracting region-specific “background” values dominated by natural sources. After removing the background influences, we find significant anthropogenic NO2 growth over Western China between 2005 and 2013 (8.6^F0.9%yr1 on average, relative to 2005), with the largest increments (15%yr1 or more) over parts of several city clusters. The NO2 pollution in most provinciallevel regions rose rapidly from 2005 to 2011 but stabilized or declined afterwards. The NO2 trends were driven mainly by changes in anthropogenic emissions, as confirmed by a nested GEOS-Chem model simulation and a comparison with Chinese official emission statistics. The rate of NO2 growth during 2005–2013 reaches 11.3^F1.0%yr1 over Northwestern China, exceeding the rates over Southwestern China (5.9^F0.6%yr1) and the three well-known polluted regions in the east (5.3^F0.8%yr1 over Beijing-Tianjin- Hebei, 4.0^F0.6%yr1 over the Yangtze River Delta, and 3.3^F0.3%yr1 over the Pearl River Delta). Subsequent socioeconomic analyses suggest that the rapid NO2 growth over Northwestern China is likely related to the fast developing resource- and pollution-intensive industries along with the “GoWest” movement as well as relatively weak emission controls. Further efforts should be made to alleviate NOx pollution to achieve sustainable development in Western China.

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Long-term visibility measurements offer useful information for aerosol and climate change studies. Recently, a new technique to converting visibility measurements to aerosol optical depth (AOD) has been developed on a station-to-station basis (Lin et al., 2014). However, factors such as human observation differences and local meteorological conditions often impair the spatial consistency of the visibility converted AOD dataset. Here we further adopt AOD spatial information from a chemical transport model GEOS-Chem, and merge visibility inferred and modeled early-afternoon AOD over East China on a 0.667^C long. ^D 0.5^C lat. grid for 2005e2012. Comparisons with MODIS/Aqua retrieved AOD and subsequent spectral decomposition analyses show that the merged dataset successfully corrects the low bias in the model while preserving its spatial pattern, resulting in very good agreement with MODIS in both magnitude and spatio-temporal variability. The low bias is reduced from 0.10 in GEOS-Chem AOD to 0.04 in the merged data averaged over East China, and the correlation in the seasonal and interannual variability between MODIS and merged AOD is well above 0.75 for most regions. Comparisons between the merged and AERONET data also show an overall small bias and high correlation. The merged dataset reveals four major pollution hot spots in China, including the North China Plain, the Yangtze River Delta, the Pearl River Delta and the Sichuan Basin, consistent with previous works. AOD peaks in springsummer over the North China Plain and Yangtze River Delta and in spring over the Pearl River Delta, with no distinct seasonal cycle over the Sichuan Basin. The merged AOD has the largest difference from MODIS over the Sichuan Basin. We also discuss possible benefits of visibility based AOD data that correct the sampling bias in MODIS retrievals related to cloud-free sampling and misclassified heavy haze conditions.

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Millions of people die every year from diseases caused by exposure to outdoor air pollution. Some studies have estimated premature mortality related to local sources of air pollution, but local air quality can also be affected by atmospheric transport of pollution from distant sources. International trade is contributing to the globalization of emission and pollution as a result of the production of goods (and their associated emissions) in one region for consumption in another region. The effects of international trade on air pollutant emissions, air quality and health have been investigated regionally, but a combined, global assessment of the health impacts related to international trade and the transport of atmospheric air pollution is lacking. Here we combine four global models to estimate premature mortality caused by fine particulate matter (PM2.5) pollution as a result of atmospheric transport and the production and consumption of goods and services in different world regions. We find that, of the 3.45 million premature deaths related to PM2.5 pollution in 2007 worldwide, about 12 per cent (411,100 deaths) were related to air pollutants emitted in a region of the world other than that in which the death occurred, and about 22 per cent (762,400 deaths) were associated with goods and services produced in one region for consumption in another. For example, PM2.5 pollution produced in China in 2007 is linked to more than 64,800 premature deaths in regions other than China, including more than 3,100 premature deaths in western Europe and the USA; on the other hand, consumption in western Europe and the USA is linked to more than 108,600 premature deaths in China. Our results reveal that the transboundary health impacts of PM2.5 pollution associated with international trade are greater than those associated with long-distance atmospheric pollutant transport.

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Nitrogen oxides affect health and climate. Their emissions, in the form of nitric oxide, from inland waters such as lakes are generally considered negligible and are absent in air quality and climate models. Here we find unexpected high emissions of nitric oxide from remote lakes on the Tibetan Plateau, based on satellite observations of tropospheric nitrogen dioxide vertical column densities and subsequent emission inversion at a fine resolution of 5 km. The total emissions from 135 lakes larger than 50 km2 reach 1.9 metric tons N h−1, comparable to anthropogenic emissions in individual megacities worldwide or the Tibet Autonomous Region. On average, the emissions per unit area reach 63.4 μg N m−2 h−1, exceeding those from crop fields. Such strong natural emissions from inland waters have not been reported, to the best of our knowledge. The emissions are derived from microbial processes in association with substantial warming and melting of glacier and permafrost on the plateau, constituting a previously unknown feedback between climate, lake ecology and nitrogen emissions.

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