Abstract. Our work explores the impact of two important dimensions of landsystem changes, land use and land cover change (LULCC) as well as directagricultural reactive nitrogen (Nr) emissions from soils, on ozone(O3) and fine particulate matter (PM2.5) in terms of air quality overcontemporary (1992 to 2014) timescales. We account for LULCC andagricultural Nr emissions changes with consistent remote sensingproducts and new global emission inventories respectively estimating theirimpacts on global surface O3 and PM2.5 concentrations as well as Nrdeposition using the GEOS-Chem global chemical transport model. Over thistime period, our model results show that agricultural Nr emissionchanges cause a reduction of annual mean PM2.5 levels over Europe andnorthern Asia (up to −2.1 µg m−3) while increasing PM2.5 levels in India, China and the eastern US (up to +3.5 µg m−3). Land cover changes induce small reductions in PM2.5 (up to −0.7 µg m−3) over Amazonia, China and India due to reduced biogenic volatile organic compound (BVOC) emissions and enhanced deposition of aerosol precursor gases (e.g., NO2, SO2). Agricultural Nr emissionchanges only lead to minor changes (up to ±0.6 ppbv) in annual meansurface O3 levels, mainly over China, India and Myanmar. Meanwhile, ourmodel result suggests a stronger impact of LULCC on surface O3 over the time period across South America; the combination of changes in drydeposition and isoprene emissions results in −0.8 to +1.2 ppbv surfaceozone changes. The enhancement of dry deposition reduces the surface ozone level (up to −1 ppbv) over southern China, the eastern US and central Africa. The enhancement of soil NO emission due to crop expansion also contributes to surface ozone changes (up to +0.6 ppbv) over sub-Saharan Africa. Incertain regions, the combined effects of LULCC and agricultural Nr emission changes on O3 and PM2.5 air quality can be comparable (>20 %) to anthropogenic emission changes over the same time period. Finally, we calculate that the increase in global agricultural Nr emissions leads to a net increase in global land area (+3.67×106km2) that potentially faces exceedance of the critical Nr load (>5 kg N ha−1 yr−1). Our result demonstrates the impacts of contemporary LULCC and agricultural Nr emission changes on PM2.5 and O3 in terms of air quality, as well as the importanceof land system changes for air quality over multidecadal timescales.
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Regional impacts of black carbon morphologies on shortwave aerosol–radiation interactions: a comparative study between the US and China
Abstract. Black carbon (BC) is one of the dominant absorbing aerosol species in the atmosphere. It normally has complex fractal-like structures due to the aggregation process during combustion. A wide range of aerosol–radiation interactions (ARIs) of BC have been reported throughout experimental and modeling studies. One reason for the large discrepancies among multiple studies is the application of the oversimplified spherical morphology for BC in ARI estimates. In current climate models, the Mie theory is commonly used to calculate the optical properties of spherical BC aerosols. Here, we employ a regional chemical transport model coupled with a radiative transfer code that utilizes the non-spherical BC optical simulations to re-evaluate the effects of particles' morphologies on BC shortwave ARI, and the wavelength range of 0.3–4.0 µm was considered. Anthropogenic activities and wildfires are two major sources of BC emissions. Therefore, we choose the typical polluted area in eastern China, which is dominated by anthropogenic emissions, and the fire region in the northwest US, which is dominated by fire emissions in this study. A 1-month simulation in eastern China and a 7 d simulation in the fire region in the northwest US were performed. The fractal BC model generally presents a larger clear-sky ARI compared to the spherical BC model. Assuming BC particles are externally mixed with other aerosols, the relative differences in the time-averaged clear-sky ARI between the fractal model with a fractal dimension (Df) of 1.8 and the spherical model are 12.1 %–20.6 % and 10.5 %–14.9 % for typical polluted urban cities in China and fire sites in the northwest US, respectively. Furthermore, the regional-mean clear-sky ARI is also significantly affected by the BC morphology, and relative differences of 17.1 % and 38.7 % between the fractal model with a Df of 1.8 and the spherical model were observed in eastern China and the northwest US, respectively. However, the existence of clouds would weaken the BC morphological effects. The time-averaged all-sky ARI relative differences between the fractal model with a Df of 1.8 and the spherical model are 4.9 %–6.4 % and 9.0 %–11.3 % in typical urban polluted cities and typical fire sites, respectively. Besides, for the regional-mean all-sky ARI, the relative differences between the fractal model and the spherical model are less than 7.3 % and 16.8 % in the polluted urban area in China and the fire region in the US, respectively. The results imply that current climate modeling may significantly underestimate the BC ARI uncertainties as the morphological effects on BC ARI are ignored in most climate models.
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- Award ID(s):
- 1926817
- PAR ID:
- 10355398
- Date Published:
- Journal Name:
- Atmospheric Chemistry and Physics
- Volume:
- 22
- Issue:
- 11
- ISSN:
- 1680-7324
- Page Range / eLocation ID:
- 7647 to 7666
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.5194/acp-22-7647-2022
