Analogous to cloud formation, the formation and life cycle of fogs is largely influenced by aerosol particles. The objective of this work is to analyze how changes in aerosol properties affect the ...fog life cycle, with special emphasis on how droplet concentrations change with cloud condensation nuclei (CCN) concentrations and on the effect that absorbing black carbon (BC) particles have on fog dissipation. For our simulation case study, we chose a typical fall time radiation fog at mid-latitudes (45° north) in fairly highly polluted conditions. Our results show that CCN concentrations have a strong influence on the fog lifetime. This is because the immediate effect of CCN on cloud droplet number concentrations (CDNC) is enhanced through two positive feedback loops: (1) Higher CDNC leads to more radiative cooling at the fog top, which leads to even stronger activation and (2) if CDNC is higher, the average droplet size is smaller, which slows down droplet removal through sedimentation. The effect that radiation fogs have on solar surface irradiation is large – the daily mean can change by 50% if CCN concentrations are doubled or halved (considering a reference CCN mixing ratio of 800 #/mg). With the same changes in CCN, the total fog lifetime increases 160 min or decreases 65 min, respectively. Although BC has a noticeable effect on fog height and dissipation time, its relative effect compared to CCN is small, even if BC concentrations are high. The fog formation is very sensitive to initial meteorological conditions which may be altered considerably if fog was present the previous day. This effect was neglected here, and future simulations, which span several days, may thus be a valuable extension of this study.
•Effect of aerosols on radiation fog has been studied using large eddy model.•Due to feedbacks, cloud condensation nuclei concentration affects droplet concentration more in fogs than in clouds.•Increase in aerosol concentration can increase fog lifetime by hours.•Absorbing aerosols shorten fog lifetime through semidirect effect.
Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This ...makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (137Cs) and xenon-133 (133Xe) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. 137Cs size distribution measurements taken close to the power plant suggested that accumulation-mode (AM) sulfate aerosols were the main carriers of cesium. Hence, 137Cs can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas 133Xe behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of 137Cs that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and 133Xe emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled 137Cs and 133Xe concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime τe, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95 % confidence interval 13.1–15.7 days). The equivalent modelled τe lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.4 ± 2.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (133Xe) concentrations in the Arctic as well but to a smaller extent than for the aerosol (137Cs) tracer. This indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.
Both explosive volcanic eruptions, which emit sulfur dioxide into the stratosphere, and stratospheric geoengineering via sulfur injections can potentially cool the climate by increasing the amount of ...scattering particles in the atmosphere. Here we employ a global aerosol-climate model and an Earth system model to study the radiative and climate changes occurring after an erupting volcano during solar radiation management (SRM). According to our simulations the radiative impacts of the eruption and SRM are not additive and the radiative effects and climate changes occurring after the eruption depend strongly on whether SRM is continued or suspended after the eruption. In the former case, the peak burden of the additional stratospheric sulfate as well as changes in global mean precipitation are fairly similar regardless of whether the eruption takes place in a SRM or non-SRM world. However, the maximum increase in the global mean radiative forcing caused by the eruption is approximately 21 % lower compared to a case when the eruption occurs in an unperturbed atmosphere. In addition, the recovery of the stratospheric sulfur burden and radiative forcing is significantly faster after the eruption, because the eruption during the SRM leads to a smaller number and larger sulfate particles compared to the eruption in a non-SRM world. On the other hand, if SRM is suspended immediately after the eruption, the peak increase in global forcing caused by the eruption is about 32 % lower compared to a corresponding eruption into a clean background atmosphere. In this simulation, only about one-third of the global ensemble-mean cooling occurs after the eruption, compared to that occurring after an eruption under unperturbed atmospheric conditions. Furthermore, the global cooling signal is seen only for the 12 months after the eruption in the former scenario compared to over 40 months in the latter. In terms of global precipitation rate, we obtain a 36 % smaller decrease in the first year after the eruption and again a clearly faster recovery in the concurrent eruption and SRM scenario, which is suspended after the eruption. We also found that an explosive eruption could lead to significantly different regional climate responses depending on whether it takes place during geoengineering or into an unperturbed background atmosphere. Our results imply that observations from previous large eruptions, such as Mount Pinatubo in 1991, are not directly applicable when estimating the potential consequences of a volcanic eruption during stratospheric geoengineering.
Southern Africa is a significant source region of atmospheric pollution, yet long-term data on pollutant concentrations and properties from this region are rather limited. A recently established ...atmospheric measurement station in South Africa, Welgegund, is strategically situated to capture regional background concentrations, as well as emissions from the major source regions in the interior of South Africa. We measured non-refractive submicron aerosols (NR-PM1 ) and black carbon over a one year period in Welgegund, and investigated the seasonal and diurnal patterns of aerosol concentration levels, chemical composition, acidity and oxidation level. Based on air mass back trajectories, four distinct source regions were determined for NR-PM1 . Supporting data utilised in our analysis included particle number size distributions, aerosol absorption, trace gas concentrations, meteorological variables and the flux of carbon dioxide. The dominant submicron aerosol constituent during the dry season was organic aerosol, reflecting high contribution from savannah fires and other combustion sources. Organic aerosol concentrations were lower during the wet season, presumably due to wet deposition as well as reduced emissions from combustion sources. Sulfate concentrations were usually high and exceeded organic aerosol concentrations when air-masses were transported over regions containing major point sources. Sulfate and nitrate concentrations peaked when air masses passed over the industrial Highveld (iHV) area. In contrast, concentrations were much lower when air masses passed over the cleaner background (BG) areas. Air masses associated with the anti-cyclonic recirculation (ACBIC) source region contained largely aged OA. Positive Matrix Factorization (PMF) analysis of aerosol mass spectra was used to characterise the organic aerosol (OA) properties. The factors identified were oxidized organic aerosols (OOA) and biomass burning organic aerosols (BBOA) in the dry season and low-volatile (LV-OOA) and semi-volatile (SV-OOA) organic aerosols in the wet season. The results highlight the importance of primary BBOA in the dry season, which represented 33% of the total OA. Aerosol acidity and its potential impact on the evolution of OOA are also discussed.
Large-scale atmospheric models, which typically describe secondary organic aerosol (SOA) formation based on chamber experiments, tend to systematically underestimate observed organic aerosol burdens. ...Since SOA constitutes a significant fraction of atmospheric aerosol, this discrepancy translates into an underestimation of SOA contribution to radiative forcing of atmospheric aerosol. Here we show that the underestimation of SOA yields can be partly explained by wall losses of SOA forming compounds during chamber experiments. We present a chamber experiment where alpha -pinene and ozone are injected into a Teflon chamber. When these two compounds react, we observe rapid formation and growth of new particles. Theoretical analysis of this formation and growth event indicates rapid formation of oxidized volatile organic compounds (OVOC) of very low volatility in the chamber. If these oxidized organic compounds form in the gas phase, their wall losses will have significant implications on their partitioning between the gas and particle phase. Although these OVOCs of very low volatility contribute to the growth of new particles, their mass will almost completely be depleted to the chamber walls during the experiment, while the depletion of OVOCs of higher volatilities is less efficient. According to our model simulations, the volatilities of OVOC contributing to the new particle formation event can be of the order of 10-5 mu g m-3.
Atmospheric aerosols often contain surface active organics. Surface activity can affect cloud droplet formation through both surface partitioning and surface tension reduction in activating droplets. ...However, a comprehensive thermodynamic account for these effects in Köhler modeling is computationally demanding and requires knowledge of both droplet composition and component molecular properties, which is generally unavailable. Here, a simple representation of activation properties for surface active organics is introduced and compared against detailed model predictions and laboratory measurements of CCN activity for mixed surfactant-salt particles from the literature. This simple organic representation is seen to work well for aerosol organic-inorganic composition ranges typically found in the atmosphere, and agreement with both experiments and detailed model predictions increases with surfactant strength. The simple representation does not require resolution of the organic aerosol composition and relies solely on properties of the organic fraction that can be measured directly with available techniques. It can thus potentially be applied to complex and ambient surface active aerosols. It is not computationally demanding, and therefore has high potential for implementation to atmospheric models accounting for cloud microphysics.
Large cloud condensation nuclei (CCN) (e.g., aged dust particles and seasalt) cannot attain their equilibrium size during the typical timescale of cloud droplet activation. Cloud activation ...parameterizations applied to aerosol with a large fraction of large CCN often do not account for this limitation adequately and can give biased predictions of cloud droplet number concentration (CDNC). Here we present a simple approach to address this problem that can easily be incorporated into cloud activation parameterizations. This method is demonstrated with activation parameterizations based on the "population splitting" concept of Nenes and Seinfeld (2003); it is shown that accounting for large CCN effects eliminates a positive bias in CDNC where the aerosol dry geometric diameter is greater than 0.5 μm. The method proposed here can also be extended to include the water vapor depletion from pre-existing droplets and ice crystals in global and regional atmospheric models.
The importance of light-absorbing organic aerosols, often called brown carbon (BrC), has become evident in recent years. However, there have been relatively few measurement-based estimates for the ...direct radiative effect of BrC so far. In earlier studies, the AErosol RObotic NETwork (AERONET)-measured aerosol absorption optical depth (AAOD) and absorption Angstrom exponent (AAE) were exploited. However, these two pieces of information are clearly not sufficient to separate properly carbonaceous aerosols from dust, while imaginary indices of refraction would contain more and better justified information for this purpose. This is first time that the direct radiative effect (DRE) of BrC is estimated by exploiting the AERONET-retrieved imaginary indices. We estimated it for four sites in the Indo-Gangetic Plain (IGP), Karachi, Lahore, Kanpur and Gandhi College. We found a distinct seasonality, which was generally similar among all the sites, but with slightly different strengths. The monthly warming effect up to 0.5 W m−2 takes place during the spring season. On the other hand, BrC results in an overall cooling effect in the winter season, which can reach levels close to −1 W m−2. We then estimated similarly also the DRE of black carbon and total aerosol, in order to assess the relative significance of the BrC radiative effect in the radiative effects of other components. Even though BrC impact seems minor in this context, we demonstrated that it is not insignificant. Moreover, we demonstrated that it is crucial to perform spectrally resolved radiative transfer calculations to obtain good estimates for the DRE of BrC.
Low-level clouds have a strong climate-cooling effect in oceanic regions due to the much lower albedo of the underlying sea surface. Marine clouds typically have low droplet concentrations, making ...their radiative properties susceptible to changes in cloud condensation nucleus (CCN) concentrations. Here, we use the global aerosol model GLOMAP to investigate the processes that determine variations in marine CCN concentrations, and focus especially on the effects of previously identified wind speed trends in recent decades. Although earlier studies have found a link between linear wind speed trends and CCN concentration, we find that the effects of wind speed trends identified using a dynamic linear model in the Northern Equatorial Pacific (0.56 m s−1 per decade in the period 1990–2004) and the North Atlantic (−0.21 m s−1 per decade) are largely dampened by other processes controlling the CCN concentration, namely nucleation scavenging and transport of continental pollution. A CCN signal from wind speed change is seen only in the most pristine of the studied regions, i.e. over the Southern Ocean, where we simulate 3.4 cm−3 and 0.17 m s−1 increases over the 15-year period in the statistical mean levels of CCN and wind speed, respectively. Our results suggest that future changes in wind-speed-driven aerosol emissions from the oceans can probably have a climate feedback via clouds only in the most pristine regions. On the other hand, a feedback mechanism via changing precipitation patterns and intensities could take place over most oceanic regions, as we have shown that nucleation scavenging has by far the largest absolute effect on CCN concentrations.
The global aerosol-climate model ECHAM5-HAM was modified to improve the representation of new particle formation in the boundary layer. Activation-type nucleation mechanism was introduced to produce ...observed nucleation rates in the lower troposphere. A simple and computationally efficient model for biogenic secondary organic aerosol (BSOA) formation was implemented. Here we study the sensitivity of the aerosol and cloud droplet number concentrations (CDNC) to these additions. Activation-type nucleation significantly increases aerosol number concentrations in the boundary layer. Increased particle number concentrations have a significant effect also on cloud droplet number concentrations and therefore on cloud properties. We performed calculations with activation nucleation coefficient values of 2×10−7s−1, 2×10−6s−1 and 2×10−5s−1 to evaluate the sensitivity to this parameter. For BSOA we have used yields of 0.025, 0.07 and 0.15 to estimate the amount of monoterpene oxidation products available for condensation. The hybrid BSOA formation scheme induces large regional changes to size distribution of organic carbon, and therefore affects particle optical properties and cloud droplet number concentrations locally. Although activation-type nucleation improves modeled aerosol number concentrations in the boundary layer, the use of a global activation coefficient generally leads to overestimation of aerosol number. Overestimation can also arise from underestimation of primary emissions.
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