Impact of mineral dust on cloud formation in a Saharan outflow region

We present a numerical modelling study investigating the impact of mineral dust on cloud formation over the Eastern Mediterranean for two case studies: (i) 25 September 2008 and (ii) 28/29 January 2003. In both cases dust plumes crossed the Mediterranean and interacted with clouds forming along frontal systems. For our investigation we used the fully online coupled model WRF-chem. <br><br> The results show that increased aerosol concentrations due to the presence of mineral dust can enhance the formation of ice crystals. This leads to slight shifts of the spatial and temporal precipitation patterns compared to scenarios where dust was not considered to act as ice nuclei. However, the total amount of precipitation did not change significantly. The only exception occurred when dust entered into an area of orographic ascent, causing glaciation of the clouds, leading to a local enhancement of rainfall. The impact of dust particles acting as giant cloud condensation nuclei on precipitation formation was found to be small. Based on our simulations the contribution of dust to the CCN population is potentially significant only for warm phase clouds. Nevertheless, the dust-induced differences in the microphysical structure of the clouds can contribute to a significant radiative forcing, which is important from a climate perspective

Modelling chemistry over the Dead Sea: Bromine and ozone chemistry

Measurements of O3 and BrO concentrations over the Dead Sea indicate that Ozone Depletion Events (ODEs), widely known to happen in polar regions, are also likely to occur over the Dead Sea due to the very high bromine content of the Dead Sea water. However, we show that BrO and O3 levels as they are detected cannot solely be explained by high Br - levels in the Dead Sea water and the release of gas phase halogen species out of sea borne aerosol particles and their conversion to reactive halogen species. It is likely that other sources for reactive halogen compounds are needed to explain the observed concentrations for BrO and O 3. To explain the chemical mechanism taking place over the Dead Sea leading to BrO levels of several pmol/mol we used the single column model MISTRA which calculates microphysics, meteorology, gas and aerosol phase chemistry. We performed pseudo Lagrangian studies by letting the model column first move over the desert which surrounds the Dead Sea region and then let it move over the Dead Sea itself. To include an additional source for gas phase halogen compounds, gas exchange between the Dead Sea water and the atmosphere is treated explicitly. Model calculations indicate that this process has to be included to explain the measurements

Do organic surface films on sea salt aerosols influence atmospheric chemistry? - A model study

Organic material from the ocean's surface can be incorporated into sea salt aerosol particles often producing a surface film on the aerosol. Such an organic coating can reduce the mass transfer between the gas phase and the aerosol phase influencing sea salt chemistry in the marine atmosphere. To investigate these effects and their importance for the marine boundary layer (MBL) we used the one-dimensional numerical model MISTRA. We considered the uncertainties regarding the magnitude of uptake reduction, the concentrations of organic compounds in sea salt aerosols and the oxidation rate of the organics to analyse the possible influence of organic surfactants on gas and liquid phase chemistry with a special focus on halogen chemistry. By assuming destruction rates for the organic coating based on laboratory measurements we get a rapid destruction of the organic monolayer within the first meters of the MBL. Larger organic initial concentrations lead to a longer lifetime of the coating but lead also to an unrealistically strong decrease of O₃ concentrations as the organic film is destroyed by reaction with O₃. The lifetime of the film is increased by assuming smaller reactive uptake coefficients for O₃ or by assuming that a part of the organic surfactants react with OH. With regard to tropospheric chemistry we found that gas phase concentrations for chlorine and bromine species decreased due to the decreased mass transfer between gas phase and aerosol phase. Aqueous phase chlorine concentrations also decreased but aqueous phase bromine concentrations increased. Differences for gas phase concentrations are in general smaller than for liquid phase concentrations. The effect on gas phase NO₂ or NO is very small (reduction less than 5%) whereas liquid phase NO₂ concentrations increased in some cases by nearly 100%. We list suggestions for further laboratory studies which are needed for improved model studies

Dynamics and chemistry of the upper troposphere and lower stratosphere (UTLS)Massive Ozone production from South American wild fires observed during SOUTHTRAC

During the SOUTHTRAC mission, which took place in September and November 2019, the German research aircraft HALO performed several cross sections from the equator to the southern tip of south America. The flight legs were flown along the coast of Brazil at typical altitudes of 13-14 km. During the northbound flight on October, 7th 2019 massive enhancements of pollutants were observed at these altitudes. Notably, in-situ observations show continuously elevated CO values exceeding 200 ppbv over a flight distance of more than 1000 km. These massive enhancements were accompanied by largely elevated NO and NOy as well as CO2 and could be attributed to the large fires in South America during this time. These fires occurred in conjunction with convection over Argentina and Brazil, which led to efficient vertical transport. Lagrangian and chemical model analysis confirmed the potential impact of convection and biomass burning to the observed enhancements of ozone and pollutants.Comparing the tracer observations to previous flights in exactly the same region three weeks earlier, we could estimate the ozone production due to the biomass burning. Based on first results we estimate ozone production in the polluted air masses up to 30-40 ppbv in the UT which is almost 40% of the observed ozone mixing ratio. Given the large extent of the polluted area over 15 degrees of latitude this may have an impact on the local energy budget of the tropopause region