Combustion-induced carbonaceous aerosols, particularly black carbon (BC) and brown carbon (BrC), have been largely considered as the only significant anthropogenic contributors to shortwave ...atmospheric heating. Natural iron oxide (FeO
) has been recognized as an important contributor, but the potential contribution of anthropogenic FeO
is unknown. In this study, we quantify the abundance of FeO
over East Asia through aircraft measurements using a modified single-particle soot photometer. The majority of airborne FeO
particles in the continental outflows are of anthropogenic origin in the form of aggregated magnetite nanoparticles. The shortwave absorbing powers (P
) attributable to FeO
and to BC are calculated on the basis of their size-resolved mass concentrations and the mean P
(FeO
)/P
(BC) ratio in the continental outflows is estimated to be at least 4-7%. We demonstrate that in addition to carbonaceous aerosols the aggregate of magnetite nanoparticles is a significant anthropogenic contributor to shortwave atmospheric heating.
Abstract
The terminal velocity of cloud drops and raindrops used in numerical model calculations can significantly affect weather predictions. Current formulations rely on laboratory experiments made ...in the 1940s and 1960s. Because these experiments were performed only at typical environmental conditions of 20°C and 1013 hPa, parameterizations have been introduced to deduce the terminal velocity aloft without rigorous evaluation. In this study, an incompressible two-phase flow direct numerical simulation model is used to calculate the free-falling motion of axisymmetric drops with diameters between 0.025 and 0.5 mm to study the terminal fall velocity. Simulated terminal fall velocities of free-falling drops at 20°C and 1013 hPa agree within 3.2% with the previous empirical parameterization (Beard formula), and 4.5% with existing laboratory data in the diameter range between 0.3 and 0.5 mm. The velocities converge to the analytic Hadamard–Rybczynski solution within 2% for small Reynolds numbers, demonstrating the robustness of our simulations. Simulations under various atmospheric conditions show that existing empirical parameterizations that account for the air density dependence of the terminal velocity have errors up to 11.8% under the conditions examined in this study. We propose a new empirical formula that describes the air density dependence of the terminal velocity. It is also shown that the falling speed of a small drop is not sensitive to shape oscillation, and the terminal velocity decreases by only less than 1.3% when the axis ratio increases by 12% with reduced surface tension. Internal circulation within falling drops is also presented and compared with previous studies.
Abstract
Black carbon (BC) from anthropogenic and natural sources has a pronounced climatic effect on the polar environment. The interaction of BC with low-level Arctic clouds, important for ...understanding BC deposition from the atmosphere, is studied using the first long-term observational data set of equivalent black carbon (eBC) inside and outside of clouds observed at Zeppelin Observatory, Svalbard. We show that the measured cloud residual eBC concentrations have a clear seasonal cycle with a maximum in early spring, due to the Arctic haze phenomenon, followed by cleaner summer months with very low concentrations. The scavenged fraction of eBC was positively correlated with the cloud water content and showed lower scavenged fractions at low temperatures, which may be due to mixed-phase cloud processes. A trajectory analysis revealed potential sources of eBC and the need to ensure that aerosol-cloud measurements are collocated, given the differences in air mass origin of cloudy and non-cloudy periods.
The lifetime and spatial distributions of accumulation-mode aerosols in a size range of approximately 0.05-1 μm, and thus their global and regional climate impacts, are primarily constrained by their ...removal via cloud and precipitation (wet removal). However, the microphysical process that predominantly controls the removal efficiency remains unidentified because of observational difficulties. Here, we demonstrate that the activation of aerosols to cloud droplets (nucleation scavenging) predominantly controls the wet removal efficiency of accumulation-mode aerosols, using water-insoluble black carbon as an observable particle tracer during the removal process. From simultaneous ground-based observations of black carbon in air (prior to removal) and in rainwater (after removal) in Tokyo, Japan, we found that the wet removal efficiency depends strongly on particle size, and the size dependence can be explained quantitatively by the observed size-dependent cloud-nucleating ability. Furthermore, our observational method provides an estimate of the effective supersaturation of water vapour in precipitating cloud clusters, a key parameter controlling nucleation scavenging. These novel data firmly indicate the importance of quantitative numerical simulations of the nucleation scavenging process to improve the model's ability to predict the atmospheric aerosol burden and the resultant climate forcings, and enable a new validation of such simulations.
Atmospheric iron affects the global carbon cycle by modulating ocean biogeochemistry through the deposition of soluble iron to the ocean. Iron emitted by anthropogenic (fossil fuel) combustion is a ...source of soluble iron that is currently considered less important than other soluble iron sources, such as mineral dust and biomass burning. Here we show that the atmospheric burden of anthropogenic combustion iron is 8 times greater than previous estimates by incorporating recent measurements of anthropogenic magnetite into a global aerosol model. This new estimation increases the total deposition flux of soluble iron to southern oceans (30-90 °S) by 52%, with a larger contribution of anthropogenic combustion iron than dust and biomass burning sources. The direct radiative forcing of anthropogenic magnetite is estimated to be 0.021 W m
globally and 0.22 W m
over East Asia. Our results demonstrate that anthropogenic combustion iron is a larger and more complex climate forcer than previously thought, and therefore plays a key role in the Earth system.
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