2022, Lückerath, Janine, Held, Andreas, Siebert, Holger, Michalkow, Michel, Wehner, Birgit

Aerosol particles are important for radiation effects, cloud formation, and therefore the climate system. A detailed understanding of the spatial distribution of aerosol particles within the atmospheric boundary layer, which depends on sources and sinks, as well as long-range transport and vertical exchange, is important. Especially in marine regions, where the climate effect of clouds is comparably high, long-range transport with subsequent vertical mixing dominates over local aerosol sources. In this study, three different methods were applied to estimate the vertical aerosol particle flux in the marine boundary layer (MBL) and the vertical exchange between the MBL and the free troposphere (FT): eddy covariance (EC), flux–gradient similarity (K theory), and the mixed-layer gradient method (MLG). For the first time, MBL aerosol fluxes derived from these three methods were compared in the framework of the “Azores Stratocumulus Measurements of Radiation, Turbulence and Aerosols” (ACORES) field campaign in the Azores region in the northeastern Atlantic Ocean in July 2017. Meteorological parameters and aerosol and cloud properties were measured in the marine troposphere using the helicopter-borne measurement platform ACTOS (Airborne Cloud Turbulence Observation System). All three methods were applied to estimate the net particle exchange between MBL and FT. In many cases, the entrainment fluxes of the MLG method agreed within the range of uncertainty with the EC and K-theory flux estimates close to the top of the MBL, while the surface flux estimates of the different methods diverged. It was not possible to measure directly above the surface with the helicopter-borne payload, which might be a source of uncertainty in the surface fluxes. The observed particle fluxes at the top of the MBL ranged from 0 to 10×106 m−2 s−1 both in the upward and the downward direction, and the associated uncertainties were on the same order of magnitude. Even though the uncertainties of all three methods are considerable, the results of this study contribute to an improved understanding of the transport of particles between the MBL and FT and their distribution in the MBL.

2017, Leck, C., Bigg, E.K., Covert, D.S., Heintzenberg, J., Maenhaut, W., Nilsson, E.D., Wiedensohler, A.

The broad aim of the Atmospheric program of the International Arctic Ocean Expedition (IAOE-91) was to test the hypothesis that marine biogenically produced dimethyl sulfide (DMS) gas can exert a significant global climatic control. The hypothesis states that DMS is transferred to the atmosphere and is oxidised to form airborne particles. Some of these grow large enough to act as cloud condensation nuclei (CCN) which help determine cloud droplet concentration. The latter has a strong influence on cloud albedo and hence on the radiation balance of the area affected. In summer, the central Arctic is a specially favourable region for studying the natural sulfur cycle in that the open waters surrounding the pack ice are the only significant sources of DMS and there are almost no anthropogenic particle sources. Concentrations of seawater and atmospheric DMS decreased at about the same rate during the period of measurements, (1 August to 6 October, latitudes 75°N to 90°N) spanning about three orders of magnitude. Methane sulfonate and nonsea salt sulfate in the submicrometer particles, which may be derived from atmospheric DMS, also decreased similarly, suggesting that the first part of the hypothesis under test was true. Influences on cloud droplet concentration and radiation balance could not be measured. Size-resolved aerosol chemistry showed a much lower proportion of methane sulfonate to be associated with supermicrometer particles than has been found elsewhere. Its molar ratio to nonsea salt sulfate suggested that the processes controlling the particulate chemistry do not exhibit a net temperature dependence. Elemental analysis of the aerosol also revealed the interesting possibility that debris from Siberian rivers transported on the moving ice represent a fairly widespread source of supermicrometer crustal material within the pack ice. Highly resolved measurements of aerosol number size distributions were made in the diameter range 3 nm to 500 nm. 3 distinct modal sizes were usually present, the “ultrafine”, “Aitken” and “accumulation” modes centred on 14, 45 and 170 nm diameter, respectively. The presence of ultrafine particles, implying recent production, was more frequent than has been found in lower latitude remote marine areas. Evidence suggests that they were mixed to the surface from higher levels. Sudden and often drastic changes in aerosol concentration and size distribution were surprisingly frequent in view of the relatively slowly changing meteorology of the central Arctic during the study period and the absence of strong pollution sources. They were most common in particles likely to have taken part in cloud formation (> 80 nm diameter). 2 factors appear to have been involved in these sudden changes. The 1st was the formation of vertical gradients in aerosol concentration due to interactions between particles and clouds or favoured regions for new particle production during periods of stability. The 2nd was sporadic localised breakdowns of the stability, bringing changed particle concentrations to the measurement level. Probable reasons for these sporadic mixing events were indicated by the structure of the Marine Boundary Layer (MBL) investigated with high resolution rawinsondes. Low level jets were present about 60% of the time, producing conditions conductive to turbulence and shear-induced waves. It is concluded that an even more detailed study of meteorological processes in the MBL in conjunction with more highly time-resolved measurements of gas-aerosol physics and chemistry appears to be essential in any future research aimed at studying the indirect, cloud mediated, effect of aerosol particles.