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At least 163 records · Page 9

Methods for estimating the optical constants of atmospheric hazes based on complex optical measurements

The methods of multifrequency laser sounding (MLS) are the most effective remote methods for investigating the atmospheric aerosols, since it is possible to obtain complete information on aerosol microstructure and the effective methods for estimating the aerosol optical constants can be developed. The MLS data interpretation consists in the solution of the set of equations containing those of laser sounding and equations for polydispersed optical characteristics. As a rule, the laser sounding equation is written in the approximation of single scattering and the equations for optical characteristics are written assuming that the atmospheric aerosol is formed by spherical and homogeneous particles. To remove the indeterminacy of equations, the method of optical sounding of atmospheric aerosol, consisting in a joint use of a mutifrequency lidar and a spectral photometer in common geometrical scheme of the optical experiment was suggested. The method is used for investigating aerosols in the cases when absorption by particles is small and indicates the minimum necessary for interpretation of a series of measurements.

Zuev, V. E.↗

Changes in Saturn's south-temperate haze distribution during the summer of 1973-1980

Attention is given to the results of a long term monitoring study of Saturn's H2 quadrupole and CH4 band absorptions outside the equatorial zone, over an interval of half a Saturn year that covers most of the perihelion half of Saturn's elliptical orbit (which is approximately bounded by the equinoxes). Marked long term changes are noted in the CH4 absorption, accompanied by weakly opposite changes in the H2 absorption. Seasonal changes are inferred on the basis of temporal variations in absorption. Spatial measurements have also been made in the 6450 A NH3 band since the 1980 equinox.

Trafton, L.↗

Enhancement of Cloud Cover and Suppression of Nocturnal Drizzle in Stratocumulus Polluted by Haze

Recent satellite observations indicate a significant decrease of cloud water in ship tracks, in contrast to an ensemble of in situ ship-track measurements that show no average change in cloud water relative to the surrounding clouds. We find through large-eddy simulations of stratocumulus that the trend in the satellite data is likely an artifact of sampling only overcast clouds. The simulations instead show cloud cover increasing with droplet concentrations. Our simulations also show that increases in cloud water from drizzle suppression (by increasing droplet concentrations) are favored at night or at extremely low droplet concentrations.

Ackerman, Andrew S.↗

Influence of Benzene on the Optical Properties of Titan Haze Laboratory Analogs in the Mid-Visible

The Cassini Ion and Neutral Mass Spectrometer (Waite, Jr., et al., 2007) and the Composite Infrared Spectrometer (Coustenis, A., et al., 2007) have detected benzene in the upper atmosphere and stratosphere of Titan. Photochemical reactions involving benzene in Titan's atmosphere may influence polycyclic aromatic hydrocarbon formation, aerosol formation, and the radiative balance of Titan's atmosphere. We measure the effect of benzene on the optical properties of Titan analog particles in the laboratory. Using cavity ring-down aerosol extinction spectroscopy, we determine the real and imaginary refractive index at 532 nm of particles formed by benzene photolysis and Titan analog particles formed with ppm-levels of benzene. These studies are compared to the previous study by Hasenkopf, et a1. (2010) of Titan analog particles formed by methane photolysis.

Yoon, Y. Heidi↗

Active Upper-atmosphere Chemistry and Dynamics from Polar Circulation Reversal on Titan

Saturn's moon Titan has a nitrogen atmosphere comparable to Earth's, with a surface pressure of 1.4 bar. Numerical models reproduce the tropospheric conditions very well but have trouble explaining the observed middle-atmosphere temperatures, composition and winds. The top of the middle-atmosphere circulation has been thought to lie at an altitude of 450 to 500 kilometres, where there is a layer of haze that appears to be separated from the main haze deck. This 'detached' haze was previously explained as being due to the colocation of peak haze production and the limit of dynamical transport by the circulation's upper branch. Herewe report a build-up of trace gases over the south pole approximately two years after observing the 2009 post-equinox circulation reversal, from which we conclude that middle-atmosphere circulation must extend to an altitude of at least 600 kilometres. The primary drivers of this circulation are summer-hemisphere heating of haze by absorption of solar radiation and winter-hemisphere cooling due to infrared emission by haze and trace gases; our results therefore imply that these effects are important well into the thermosphere (altitudes higher than 500 kilometres). This requires both active upper-atmosphere chemistry, consistent with the detection of high-complexity molecules and ions at altitudes greater than 950 kilometres, and an alternative explanation for the detached haze, such as a transition in haze particle growth from monomers to fractal structures.

Titan Atmosphere↗

Limitations in Representation of Physical Processes Prevents Successful Simulation of PM2.5 During KORUS-AQ

High levels of fine particulate matter (PM2.5) pollution in East Asia often exceed local air quality standards. Observations from the Korea United States-Air Quality (KORUS-AQ) field campaign in May and June 2016 showed that development of extreme pollution (haze) occurred through a combination of long-range transport and favorable meteorological conditions that enhanced local production of PM2.5. Atmospheric models often have difficulty simulating PM2.5 chemical composition during haze, which is of concern for the development of successful control measures. We use observations from KORUS-AQ to examine the ability of the GEOS-Chem chemical transport model to simulate PM2.5 composition throughout the campaign and identify the mechanisms driving the pollution event. At the surface, the model underestimates sulfate by -64% but overestimates nitrate by +36%. The largest underestimate in sulfate occurs during the pollution event, where models typically struggle to generate elevated sulfate concentrations due to missing heterogeneous chemistry in aerosol liquid water in the polluted boundary layer. Hourly surface observations show that the model nitrate bias is driven by an overestimation of the nighttime peak. In the model, nitrate formation is limited by the supply of nitric acid, which is biased by +100% against aircraft observations. We hypothesize that this is due to a large missing sink, which we implement here as a factor of five increase in dry deposition. We show that the resulting increased deposition velocity is consistent with observations of total nitrate as a function of photochemical age. The model does not account for factors such as the urban heat island effect or the heterogeneity of the built-up urban landscape resulting in insufficient model turbulence and surface area over the study area that likely results in insufficient dry deposition. Other species such as NH3 could be similarly affected but were not measured during the campaign. Nighttime production of nitrate is driven by NO2 hydrolysis in the model, while observations show that unexpectedly elevated nighttime ozone (not present in the model) should result in N2O5 hydrolysis as the primary pathway. The model is unable to represent nighttime ozone due to an overly rapid collapse of the afternoon mixed layer and excessive titration by NO. We attribute this to missing nighttime heating driving deeper nocturnal mixing that would be expected to occur in a city like Seoul. This urban heating is not considered in air quality models run at large enough scales to treat both local chemistry and long-range transport. Key model failures in simulating nitrate, mainly overestimated daytime nitric acid, incorrect representation of nighttime chemistry, and an overly shallow and insufficiently turbulent nighttime mixed layer, exacerbate the model’s inability to simulate the buildup of PM2.5 during haze pollution. To address the underestimate in sulfate most evident during the haze event, heterogeneous aerosol uptake of SO2 is added to the model which previously only considered aqueous production of sulfate from SO2 in cloud water. Implementing a simple parameterization of this chemistry improves the model abundance of sulfate but degrades the SO2 simulation implying that emissions are underestimated. We find that improving model simulations of sulfate has direct relevance to determining local vs. transboundary contributions to PM2.5. During the haze pollution event, the inclusion of heterogeneous aerosol uptake of SO2 decreases the fraction of PM2.5 attributable to long-range transport from 66% to 54%. Locally-produced sulfate increased from 1% to 25% of locally-produced PM2.5, implying that local emissions controls would have a larger effect than previously thought. However, this additional uptake of SO2 is coupled to the model nitrate prediction which affects the aerosol liquid water abundance and chemistry driving sulfate-nitrate-ammonium partitioning. An additional simulation of the haze pollution with heterogeneous uptake of SO2 to aerosol and simple improvements to the model nitrate simulation results in 30% less sulfate due to 40% less nitrate and aerosol water, and results in an underestimate of sulfate during the haze event. Future studies need to better consider the impact of model physical processes such as dry deposition and nighttime boundary layer mixing on the simulation of nitrate and the effect of improved nitrate simulations on the overall simulation of secondary inorganic aerosol (sulfate+nitrate+ammonium) in East Asia. Foreign emissions are rapidly changing, increasing the need to understand the impact of local emissions on PM2.5 in South Korea to ensure continued air quality improvements.

Katherine R. Travis↗