Search

Atmospheric aerosols affect weather and global general circulation by modifying cloud and precipitation processes, but the magnitude of cloud adjustment by aerosols remains poorly quantified and represents the largest uncertainty in estimated forcing of climate change. Here we assess the effects of anthropogenic aerosols on the Pacific storm track, using a multiscale global aerosol-climate model (GCM). Simulations of two aerosol scenarios corresponding to the present day and preindustrial conditions reveal long-range transport of anthropogenic aerosols across the north Pacific and large resulting changes in the aerosol optical depth, cloud droplet number concentration, and cloud and ice water paths. Shortwave and longwave cloud radiative forcing at the top of atmosphere are changed by -2.5 and +1.3 W m-2, respectively, by emission changes from preindustrial to present day, and an increased cloud top height indicates invigorated midlatitude cyclones. The overall increased precipitation and poleward heat transport reflect intensification of the Pacific storm track by anthropogenic aerosols. Hence, this work provides, for the first time to the authors' knowledge, a global perspective of the effects of Asian pollution outflows from GCMs. Furthermore, our results suggest that the multiscale modeling framework is essential in producing the aerosol invigoration effect of deep convective clouds on a global scale. [ABSTRACT FROM AUTHOR]

Photochemical oxidation of aromatic hydrocarbons leads to tropospheric ozone and secondary organic aerosol (SOA) formation, with profound implications for air quality, human health, and climate. Toluene is the most abundant aromatic compound under urban environments, but its detailed chemical oxidation mechanism remains uncertain. From combined laboratory experiments and quantum chemical calculations, we show a toluene oxidation mechanism that is different from the one adopted in current atmospheric models. Our experimental work indicates a larger-than-expected branching ratio for cresols, but a negligible formation of ring-opening products (e.g., methylglyoxal). Quantum chemical calculations also demonstrate that cresols are much more stable than their corresponding peroxy radicals, and, for the most favorable OH ( ortho ) addition, the pathway of H extraction by O 2 to form the cresol proceeds with a smaller barrier than O 2 addition to form the peroxy radical. Our results reveal that phenolic (rather than peroxy radical) formation represents the dominant pathway for toluene oxidation, highlighting the necessity to reassess its role in ozone and SOA formation in the atmosphere., Competing Interests: The authors declare no conflict of interest.

Sulfate aerosols exert profound impacts on human and ecosystem health, weather, and climate, but their formation mechanism remains uncertain. Atmospheric models consistently underpredict sulfate levels under diverse environmental conditions. From atmospheric measurements in two Chinese megacities and complementary laboratory experiments, we show that the aqueous oxidation of SO 2 by NO 2 is key to efficient sulfate formation but is only feasible under two atmospheric conditions: on fine aerosols with high relative humidity and NH 3 neutralization or under cloud conditions. Under polluted environments, this SO 2 oxidation process leads to large sulfate production rates and promotes formation of nitrate and organic matter on aqueous particles, exacerbating severe haze development. Effective haze mitigation is achievable by intervening in the sulfate formation process with enforced NH 3 and NO 2 control measures. In addition to explaining the polluted episodes currently occurring in China and during the 1952 London Fog, this sulfate production mechanism is widespread, and our results suggest a way to tackle this growing problem in China and much of the developing world., Competing Interests: The authors declare no conflict of interest.

Atmospheric aerosols affect weather and global general circulation by modifying cloud and precipitation processes, but the magnitude of cloud adjustment by aerosols remains poorly quantified and represents the largest uncertainty in estimated forcing of climate change. Here we assess the effects of anthropogenic aerosols on the Pacific storm track, using a multiscale global aerosol-climate model (GCM). Simulations of two aerosol scenarios corresponding to the present day and preindustrial conditions reveal long-range transport of anthropogenic aerosols across the north Pacific and large resulting changes in the aerosol optical depth, cloud droplet number concentration, and cloud and ice water paths. Shortwave and longwave cloud radiative forcing at the top of atmosphere are changed by -2.5 and +1.3 W m(-2), respectively, by emission changes from preindustrial to present day, and an increased cloud top height indicates invigorated midlatitude cyclones. The overall increased precipitation and poleward heat transport reflect intensification of the Pacific storm track by anthropogenic aerosols. Hence, this work provides, for the first time to the authors' knowledge, a global perspective of the effects of Asian pollution outflows from GCMs. Furthermore, our results suggest that the multiscale modeling framework is essential in producing the aerosol invigoration effect of deep convective clouds on a global scale.