ALBERT

Description: We simulate nitrogen deposition over the US in 2006–2008 by using the GEOS-Chem global chemical transport model at 1/2°×2/3° horizontal resolution over North America and adjacent oceans. US emissions of NOx and NH3 in the model are 6.7 and 2.9 Tg N a−1 respectively, including a 20% natural contribution for each. Ammonia emissions are a factor of 3 lower in winter than summer, providing a good match to US network observations of NHx (≡NH3 gas + ammonium aerosol) and ammonium wet deposition fluxes. Model comparisons to observed deposition fluxes and surface air concentrations of oxidized nitrogen species (NOy) show overall good agreement but excessive wintertime HNO3 production over the US Midwest and Northeast. This suggests a model overestimate N2O5 hydrolysis in aerosols, and a possible factor is inhibition by aerosol nitrate. Model results indicate a total nitrogen deposition flux of 6.5 Tg N a−1 over the contiguous US, including 4.2 as NOy and 2.3 as NHx. Domestic anthropogenic, foreign anthropogenic, and natural sources contribute respectively 78%, 6%, and 16% of total nitrogen deposition over the contiguous US in the model. The domestic anthropogenic contribution generally exceeds 70% in the east and in populated areas of the west, and is typically 50–70% in remote areas of the west. Total nitrogen deposition in the model exceeds 10 kg N ha−1 a−1 over 35% of the contiguous US.

Description: We simulated elemental carbon (EC) and organic carbon (OC) aerosols in China and compared model results to surface measurements at Chinese rural and background sites, with the goal of deriving "top-down" emission estimates of EC and OC, as well as better quantifying the secondary sources of OC. We included in the model state-of-the-science Chinese "bottom-up" emission inventories for EC (1.92 TgC yr−1) and OC (3.95 TgC yr−1), as well as updated secondary OC formation pathways. The average simulated annual mean EC concentration at rural and background sites was 1.1 μgC m−3, 56% lower than the observed 2.5 μgC m−3. The average simulated annual mean OC concentration at rural and background sites was 3.4 μgC m−3, 76% lower than the observed 14 μgC m−3. Multiple regression to fit surface monthly mean EC observations at rural and background sites yielded the best estimate of Chinese EC source of 3.05 ± 0.78 TgC yr−1. Based on the top-down EC emission estimate and observed seasonal primary OC/EC ratios, we estimated Chinese OC emissions to be 6.67 ± 1.30 TgC yr−1. Using these top-down estimates, the simulated average annual mean EC concentration at rural and background sites was significantly improved to 1.9 μgC m−3. However, the model still significantly underestimated observed OC in all seasons (simulated average annual mean OC at rural and background sites was 5.4 μgC m−3), with little skill in capturing the spatiotemporal variability. Secondary formation accounts for 21% of Chinese annual mean surface OC in the model, with isoprene being the most important precursor. In summer, as high as 62% of the observed surface OC may be due to secondary formation in eastern China. Our analysis points to four shortcomings in the current bottom-up inventories of Chinese carbonaceous aerosols: (1) the anthropogenic source is underestimated on a national scale, particularly for OC; (2) the spatiotemporal distributions of emissions are misrepresented; (3) there is a missing source in western China, likely associated with the use of biofuels or other low-quality fuels for heating; and (4) sources in fall are not well represented, either because the seasonal shifting of emissions and/or secondary formation are poorly captured or because specific fall emission events are missing. In addition, secondary production of OC in China is severely underestimated. More regional measurements with better spatiotemporal coverage are needed to resolve these shortcomings.

Description: Understanding how sediment concentrations vary with land use/cover is critical for evaluating the current and future impacts of human activities on river systems. This paper presents suspended sediment concentration (SSC) dynamics and the relationship between SSC and discharge (Q) in the 8973 km2 Du catchment and its sub-catchment (4635 km2). In the Du catchment and its sub-catchment, 4235 and 3980 paired Q-SSC samples, respectively, were collected over 30 years. Under the influence of the "Household Contract Responsibility System" and Grain-for-Green projects in China, three periods were designated, the original period (1980s), cultivation period (1990s), and reforestation period (2000s). The results of a Mann–Kendall test showed that rainfall slightly increased during the study years; however, the annual discharge and sediment load significantly decreased. The annual suspended sediment yield of the Du catchment varied between 4 and 332 kg s−1, and that of the sub-catchment varied between 2 and 135 kg s−1. The SSCs in the catchment and sub-catchment fluctuated between 1 and 22 400 g m−3 and between 1 and 31 800 g m−3, respectively. The mean SSC of the Du catchment was relatively stable during the three periods (±83 g m−3). ANOVA indicated that the SSC did not significantly change under cultivation for low and moderate flows, but was significantly different under high flow during reforestation of the Du catchment. The SSC in the sub-catchment was more variable, and the mean-SSC in the sub-catchment varied from 1058 g m−3 in the 1980s to 1256 g m−3 in the 1990s and 891 g m−3 in the 2000s. Reforestation significantly decreased the SSCs during low and moderate flows, whereas cultivation increased the SSCs during high flow. The sediment rating curves showed a stable relationship between the SSC and Q in the Du catchment during the three periods. However, the SSC-Q of the sub-catchment exhibited scattered relationships during the original and cultivation periods and a more linear relationship during the reforestation period.

Description: Understanding how sediment concentrations vary with land use/cover is critical for evaluating the current and future impacts of human activities on river systems. This paper presents suspended sediment concentration (SSC) dynamics and the relationship between SSC and discharge (Q) in the 8973 km2 Du catchment and its sub-catchment (4635 km2). In the Du catchment and its sub-catchment, 4235 and 3980 paired SSC–Q samples, respectively, were collected over 30 years. Under the influence of the Household Contract Responsibility System and Grain-for-Green projects in China, three periods were designated, the original period (1980s), cultivation period (1990s) and reforestation period (2000s). The results of a Mann–Kendall test showed that rainfall slightly increased during the study years; however, the annual discharge and sediment load significantly decreased. The annual suspended sediment yield of the Du catchment varied between 1.3  ×  108 and 1.0  ×  1010 kg, and that of the sub-catchment varied between 6.3  ×  107 and 4.3  ×  109 kg. The SSCs in the catchment and sub-catchment fluctuated between 1 and 22400 g m−3 and between 1 and 31800 g m−3, respectively. The mean SSC of the Du catchment was relatively stable during the three periods (±83 g m−3). ANOVA (analysis of variance) indicated that the SSC did not significantly change under cultivation for low and moderate flows, but was significantly different under high flow during reforestation of the Du catchment. The SSC in the sub-catchment was more variable, and the mean SSC in the sub-catchment varied from 1058 ± 2217 g m−3 in the 1980s to 1256 ± 2496 g m−3 in the 1990s and 891 ± 1558 g m−3 in the 2000s. Reforestation significantly decreased the SSCs during low and moderate flows, whereas cultivation increased the SSCs during high flow. The sediment rating curves showed a stable relationship between the SSC and Q in the Du catchment during the three periods. However, the SSC–Q of the sub-catchment exhibited scattered relationships during the original and cultivation periods and a more linear relationship during the reforestation period.

Description: We simulate nitrogen deposition over the US in 2006–2008 by using the GEOS-Chem global chemical transport model at 1/2° × 2/3° horizontal resolution over North America and adjacent oceans. US emissions of NOx and NH3 in the model are 6.7 and 2.9 Tg N a−1 respectively, including a 20% natural contribution for each. Ammonia emissions are a factor of 3 lower in winter than summer, providing a good match to US network observations of NHx (≡NH3 gas + ammonium aerosol) and ammonium wet deposition fluxes. Model comparisons to observed deposition fluxes and surface air concentrations of oxidized nitrogen species (NOy) show overall good agreement but excessive wintertime HNO3 production over the US Midwest and Northeast. This suggests a model overestimate N2O5 hydrolysis in aerosols, and a possible factor is inhibition by aerosol nitrate. Model results indicate a total nitrogen deposition flux of 6.5 Tg N a−1 over the contiguous US, including 4.2 as NOy and 2.3 as NHx. Domestic anthropogenic, foreign anthropogenic, and natural sources contribute respectively 78%, 6%, and 16% of total nitrogen deposition over the contiguous US in the model. The domestic anthropogenic contribution generally exceeds 70% in the east and in populated areas of the west, and is typically 50–70% in remote areas of the west. Total nitrogen deposition in the model exceeds 10 kg N ha−1 a−1 over 35% of the contiguous US.

Description: A regional air quality simulation framework including the Weather Research and Forecasting modelling system (WRF), the Community Multi-scale Air Quality modeling system (CMAQ), and precursor emissions to simulate tropospheric ozone over South and East Asia is introduced. Concentrations of tropospheric ozone and related species simulated by the framework are validated by comparing with observation data of surface monitorings, ozone zondes, and satellites obtained in 2010. The simulation demonstrates acceptable performance on tropospheric ozone over South and East Asia at regional scale. Future energy consumption, carbon dioxide (CO2), nitrogen oxides (NOx), and volatile organic compound (VOC) emissions in 2030 under three future scenarios are estimated. One of the scenarios assumes a business-as-usual (BAU) pathway, and other two scenarios consider implementation of additional energy and environmental strategies to reduce energy consumption, CO2, NOx, and VOC emissions in China and India. Future surface ozone under these three scenarios is predicted by the simulation. The simulation indicates future surface ozone significantly increases around India for a whole year and around north eastern China in summer. NOx is a main driver on significant seasonal increase of surface ozone, whereas VOC as well as increasing background ozone and methane is also an important factor on annual average of surface ozone in East Asia. Warmer weather around India is also preferable for significant increase of surface ozone. Additional energy and environmental strategies assumed in future scenarios are expected to be effective to reduce future surface ozone over South and East Asia.

Description: The aerosol–radiation–cloud feedbacks on meteorology and air quality over eastern China under severe winter haze conditions during January~2013 are simulated using the fully coupled on-line Weather Research and Forecasting/Chemistry (WRF-Chem) model. Three simulation scenarios including different aerosol configurations are undertaken to distinguish the impact of aerosol radiative (direct and semi-direct) and indirect effects on meteorological variables and air quality. Simulated spatial and temporal variations of PM2.5 are generally consistent with surface observations, with a mean bias of −18.9 μg m−3 (−15.0%) averaged over 71 big cities in China. Comparisons between different scenarios reveal that aerosol radiative effects (direct effect and semi-direct effects) result in reductions of downward shortwave flux at the surface, 2 m temperature, 10 m wind speed and planetary boundary layer (PBL) height by up to 84.0 W m−2, 3.2 °C, 0.8 m s−1, and 268 m, respectively. The simulated impact of the aerosol indirect effects is comparatively smaller. Through reducing the PBL height and wind speeds, the aerosol effects lead to increases in surface concentrations of primary pollutants (CO and SO2) and PM2.5. The aerosol feedbacks on secondary pollutants such as surface ozone and PM2.5 mass concentrations show some spatial variations. Surface O3 mixing ratio is reduced by up to 6.9 ppb due to reduced incoming solar radiation and lower temperature. Comparisons of model results with observations show that inclusion of aerosol feedbacks in the model significantly improves model's performances in simulating meteorological variables and improves simulations of PM2.5 temporal distributions over the North China Plain, the Yangtze River Delta, the Pearl River Delta, and Central China. Although the aerosol–radiation–cloud feedbacks on aerosol mass concentrations are subject to uncertainties, this work demonstrates the significance of aerosol–radiation–cloud feedbacks for real-time air quality forecasting under haze conditions.

Description: We simulate elemental carbon (EC) and organic carbon (OC) aerosols in China and compare model results to surface measurements at Chinese rural and background sites, with the goal of deriving "top-down" emission estimates of EC and OC, as well as better quantifying the secondary sources of OC. We include in the model state-of-the-science Chinese "bottom-up" emission inventories for EC (1.92 Tg C yr−1) and OC (3.95 Tg C yr−1), as well as updated secondary OC formation pathways. The average simulated annual mean EC concentration at rural and background site is 1.1 μg C m−3, 56% lower than the observed 2.5 μg C m−3. The average simulated annual mean OC concentration at rural and background sites is 3.4 μg C m−3, 76% lower than the observed 14 μg C m−3. Multiple regression to fit surface monthly mean EC observations at rural and background sites yields best estimate of Chinese EC source of 3.05 ± 0.78 Tg C yr−1. Based on the top-down EC emission estimate and observed seasonal primary OC/EC ratios, we estimate Chinese OC total emissions to be 6.67 ± 1.30 Tg C yr−1. Using these top-down estimates, the simulated average annual mean EC concentration at rural and background sites significantly improved to 1.9 μg C m−3. However, the model still significantly underestimates observed OC in all seasons (simulated average annual mean OC at rural and background sites is 5.4 μg C m−3), with little skill in capturing the spatiotemporal variability. Secondary formation accounts for 21% of Chinese annual mean surface OC in the model, with isoprene being the most important precursor. In summer, as high as 62% of the observed surface OC may be due to secondary formation in eastern China. Our analysis points to three shortcomings in the current bottom-up inventories of Chinese carbonaceous aerosols: (1) the anthropogenic source is severely underestimated, particularly for OC; (2) there is a missing source in western China, likely associated with the use of biofuels or other low-quality fuels for heating; and (3) sources in fall are not well represented, either because the seasonal shifting of emissions and/or secondary formation are poorly captured or because specific fall emission events are missing. More regional measurements with better spatiotemporal coverage are needed to resolve these shortcomings.

Description: A regional air quality simulation framework including the Weather Research and Forecasting modeling system (WRF), the Community Multi-scale Air Quality modeling system (CMAQ), and precursor emissions to simulate tropospheric ozone over South and East Asia is introduced. Concentrations of tropospheric ozone and related species simulated by the framework are validated by comparing with observation data of surface monitoring, ozonesondes, and satellites obtained in 2010. The simulation demonstrates acceptable performance on tropospheric ozone over South and East Asia at regional scale. Future energy consumption, carbon dioxide (CO2), nitrogen oxides (NOx), and volatile organic compound (VOC) emissions in 2030 under three future scenarios are estimated. One of the scenarios assumes a business-as-usual (BAU) pathway, and other two scenarios consider implementation of additional energy and environmental strategies to reduce energy consumption, CO2, NOx, and VOC emissions in China and India. Future surface ozone under these three scenarios is predicted by the simulation. The simulation indicates future surface ozone significantly increases around India for a whole year and around northeastern China in summer. NOx is a main driver on significant seasonal increase of surface ozone, whereas VOC as well as increasing background ozone and methane is also an important factor on annual average of surface ozone in East Asia. Warmer weather around India is also preferable for significant increase of surface ozone. Additional energy and environmental strategies assumed in future scenarios are expected to be effective to reduce future surface ozone over South and East Asia.

Description: Chemical transport models (CTMs) driven with high-resolution meteorological fields can better resolve small-scale processes, such as frontal lifting or deep convection, and thus improve the simulation and emission estimates of tropospheric trace gases. In this work, we explore the use of the GEOS-Chem four-dimensional variational (4D-Var) data assimilation system with the nested high-resolution version of the model (0.5° × 0.67°) to quantify North American CO emissions during the period of June 2004–May 2005. With optimized lateral boundary conditions, regional inversion analyses can reduce the sensitivity of the CO source estimates to errors in long-range transport and in the distributions of the hydroxyl radical (OH), the main sink for CO. To further limit the potential impact of discrepancies in chemical aging of air in the free troposphere, associated with errors in OH, we use surface-level multispectral MOPITT (Measurement of Pollution in The Troposphere) CO retrievals, which have greater sensitivity to CO near the surface and reduced sensitivity in the free troposphere, compared to previous versions of the retrievals. We estimate that the annual total anthropogenic CO emission from the contiguous US 48 states was 97 Tg CO, a 14 % increase from the 85 Tg CO in the a priori. This increase is mainly due to enhanced emissions around the Great Lakes region and along the west coast, relative to the a priori. Sensitivity analyses using different OH fields and lateral boundary conditions suggest a possible error, associated with local North American OH distribution, in these emission estimates of 20 % during summer 2004, when the CO lifetime is short. This 20 % OH-related error is 50 % smaller than the OH-related error previously estimated for North American CO emissions using a global inversion analysis. We believe that reducing this OH-related error further will require integrating additional observations to provide a strong constraint on the CO distribution across the domain. Despite these limitations, our results show the potential advantages of combining high-resolution regional inversion analyses with global analyses to better quantify regional CO source estimates.