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- ItemVertical profiles of aerosol mass concentration derived by unmanned airborne in situ and remote sensing instruments during dust events(Katlenburg-Lindau : Copernicus, 2018) Mamali, Dimitra; Marinou, Eleni; Sciare, Jean; Pikridas, Michael; Kokkalis, Panagiotis; Kottas, Michael; Binietoglou, Ioannis; Tsekeri, Alexandra; Keleshis, Christos; Engelmann, Ronny; Baars, Holger; Ansmann, Albert; Amiridis, Vassilis; Russchenberg, Herman; Biskos, GeorgeIn situ measurements using unmanned aerial vehicles (UAVs) and remote sensing observations can independently provide dense vertically resolved measurements of atmospheric aerosols, information which is strongly required in climate models. In both cases, inverting the recorded signals to useful information requires assumptions and constraints, and this can make the comparison of the results difficult. Here we compare, for the first time, vertical profiles of the aerosol mass concentration derived from light detection and ranging (lidar) observations and in situ measurements using an optical particle counter on board a UAV during moderate and weak Saharan dust episodes. Agreement between the two measurement methods was within experimental uncertainty for the coarse mode (i.e. particles having radii > 0.5 μm), where the properties of dust particles can be assumed with good accuracy. This result proves that the two techniques can be used interchangeably for determining the vertical profiles of aerosol concentrations, bringing them a step closer towards their systematic exploitation in climate models.
- ItemImportance of size representation and morphology in modelling optical properties of black carbon: comparison between laboratory measurements and model simulations(Katlenburg-Lindau : Copernicus, 2022) Romshoo, Baseerat; Pöhlker, Mira; Wiedensohler, Alfred; Pfeifer, Sascha; Saturno, Jorge; Nowak, Andreas; Ciupek, Krzysztof; Quincey, Paul; Vasilatou, Konstantina; Ess, Michaela N.; Gini, Maria; Eleftheriadis, Konstantinos; Robins, Chris; Gaie-Levrel, François; Müller, ThomasBlack carbon (BC) from incomplete combustion of biomass or fossil fuels is the strongest absorbing aerosol component in the atmosphere. Optical properties of BC are essential in climate models for quantification of their impact on radiative forcing. The global climate models, however, consider BC to be spherical particles, which causes uncertainties in their optical properties. Based on this, an increasing number of model-based studies provide databases and parameterization schemes for the optical properties of BC, using more realistic fractal aggregate morphologies. In this study, the reliability of the different modelling techniques of BC was investigated by comparing them to laboratory measurements. The modelling techniques were examined for bare BC particles in the first step and for BC particles with organic material in the second step. A total of six morphological representations of BC particles were compared, three each for spherical and fractal aggregate morphologies. In general, the aggregate representation performed well for modelling the particle light absorption coefficient σabs, single-scattering albedo SSA, and mass absorption cross-section MACBC for laboratory-generated BC particles with volume mean mobility diameters dp,V larger than 100nm. However, for modelling Ångström absorption exponent AAE, it was difficult to suggest a method due to size dependence, although the spherical assumption was in better agreement in some cases. The BC fractal aggregates are usually modelled using monodispersed particles, since their optical simulations are computationally expensive. In such studies, the modelled optical properties showed a 25% uncertainty in using the monodisperse size method. It is shown that using the polydisperse size distribution in combination with fractal aggregate morphology reduces the uncertainty in measured σabs to 10% for particles with dp,V between 60-160nm. Furthermore, the sensitivities of the BC optical properties to the various model input parameters such as the real and imaginary parts of the refractive index (mre and mim), the fractal dimension (Df), and the primary particle radius (app) of an aggregate were investigated. When the BC particle is small and rather fresh, the change in the Df had relatively little effect on the optical properties. There was, however, a significant relationship between app and the particle light scattering, which increased by a factor of up to 6 with increasing total particle size. The modelled optical properties of BC are well aligned with laboratory-measured values when the following assumptions are used in the fractal aggregate representation: mre between 1.6 and 2, mim between 0.50 and 1, Df from 1.7 to 1.9, and app between 10 and 14nm. Overall, this study provides experimental support for emphasizing the importance of an appropriate size representation (polydisperse size method) and an appropriate morphological representation for optical modelling and parameterization scheme development of BC.
- ItemComparison of particle number size distribution trends in ground measurements and climate models(Katlenburg-Lindau : EGU, 2022) Leinonen, Ville; Kokkola, Harri; Yli-Juuti, Taina; Mielonen, Tero; Kühn, Thomas; Nieminen, Tuomo; Heikkinen, Simo; Miinalainen, Tuuli; Bergman, Tommi; Carslaw, Ken; Decesari, Stefano; Fiebig, Markus; Hussein, Tareq; Kivekäs, Niku; Krejci, Radovan; Kulmala, Markku; Leskinen, Ari; Massling, Andreas; Mihalopoulos, Nikos; Mulcahy, Jane P.; Noe, Steffen M.; van Noije, Twan; O'Connor, Fiona M.; O'Dowd, Colin; Olivie, Dirk; Pernov, Jakob B.; Petäjä, Tuukka; Seland, Øyvind; Schulz, Michael; Scott, Catherine E.; Skov, Henrik; Swietlicki, Erik; Tuch, Thomas; Wiedensohler, Alfred; Virtanen, Annele; Mikkonen, SanttuDespite a large number of studies, out of all drivers of radiative forcing, the effect of aerosols has the largest uncertainty in global climate model radiative forcing estimates. There have been studies of aerosol optical properties in climate models, but the effects of particle number size distribution need a more thorough inspection. We investigated the trends and seasonality of particle number concentrations in nucleation, Aitken, and accumulation modes at 21 measurement sites in Europe and the Arctic. For 13 of those sites, with longer measurement time series, we compared the field observations with the results from five climate models, namely EC-Earth3, ECHAM-M7, ECHAM-SALSA, NorESM1.2, and UKESM1. This is the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five earth system models (ESMs). We found that the trends of particle number concentrations were mostly consistent and decreasing in both measurements and models. However, for many sites, climate models showed weaker decreasing trends than the measurements. Seasonal variability in measured number concentrations, quantified by the ratio between maximum and minimum monthly number concentration, was typically stronger at northern measurement sites compared to other locations. Models had large differences in their seasonal representation, and they can be roughly divided into two categories: for EC-Earth and NorESM, the seasonal cycle was relatively similar for all sites, and for other models the pattern of seasonality varied between northern and southern sites. In addition, the variability in concentrations across sites varied between models, some having relatively similar concentrations for all sites, whereas others showed clear differences in concentrations between remote and urban sites. To conclude, although all of the model simulations had identical input data to describe anthropogenic mass emissions, trends in differently sized particles vary among the models due to assumptions in emission sizes and differences in how models treat size-dependent aerosol processes. The inter-model variability was largest in the accumulation mode, i.e. sizes which have implications for aerosol-cloud interactions. Our analysis also indicates that between models there is a large variation in efficiency of long-range transportation of aerosols to remote locations. The differences in model results are most likely due to the more complex effect of different processes instead of one specific feature (e.g. the representation of aerosol or emission size distributions). Hence, a more detailed characterization of microphysical processes and deposition processes affecting the long-range transport is needed to understand the model variability.
- ItemGlobal relevance of marine organic aerosol as ice nucleating particles(Katlenburg-Lindau : EGU, 2018) Huang, Wan Ting Katty; Ickes, Luisa; Tegen, Ina; Rinaldi, Matteo; Ceburnis, Darius; Lohmann, UlrikeIce nucleating particles (INPs) increase the temperature at which supercooled droplets start to freeze. They are therefore of particular interest in mixed-phase cloud temperature regimes, where supercooled liquid droplets can persist for extended periods of time in the absence of INPs. When INPs are introduced to such an environment, the cloud can quickly glaciate following ice multiplication processes and the Wegener–Bergeron–Findeisen (WBF) process. The WBF process can also cause the ice to grow to precipitation size and precipitate out. All of these processes alter the radiative properties. Despite their potential influence on climate, the ice nucleation ability and importance of different aerosol species is still not well understood and is a field of active research. In this study, we use the aerosol–climate model ECHAM6-HAM2 to examine the global relevance of marine organic aerosol (MOA), which has drawn much interest in recent years as a potentially important INPs in remote marine regions. We address the uncertainties in emissions and ice nucleation activity of MOA with a range of reasonable set-ups and find a wide range of resulting MOA burdens. The relative importance of MOA as an INP compared to dust is investigated and found to depend strongly on the type of ice nucleation parameterisation scheme chosen. On the zonal mean, freezing due to MOA leads to relative increases in the cloud ice occurrence and in-cloud number concentration close to the surface in the polar regions during summer. Slight but consistent decreases in the in-cloud ice crystal effective radius can also be observed over the same regions during all seasons. Regardless, MOA was not found to affect the radiative balance significantly on the global scale, due to its relatively weak ice activity and a low sensitivity of cloud ice properties to heterogeneous ice nucleation in our model.
- ItemCRI-HOM: A novel chemical mechanism for simulating highly oxygenated organic molecules (HOMs) in global chemistry-aerosol-climate models(Katlenburg-Lindau : EGU, 2020) Weber, James; Archer-Nicholls, Scott; Griffiths, Paul; Berndt, Torsten; Jenkin, Michael; Gordon, Hamish; Knote, Christoph; Archibald, Alexander T.We present here results from a new mechanism, CRI-HOM, which we have developed to simulate the formation of highly oxygenated organic molecules (HOMs) from the gas-phase oxidation of-pinene, one of the most widely emitted biogenic volatile organic compounds (BVOCs) by mass. This concise scheme adds 12 species and 66 reactions to the Common Representative Intermediates (CRI) mechanism v2.2 Reduction 5 and enables the representation of semi-explicit HOM treatment suitable for long-term global chemistry-aerosol-climate modelling, within a comprehensive tropospheric chemical mechanism. The key features of the new mechanism are (i) representation of the autoxidation of peroxy radicals from the hydroxyl radical and ozone initiated reactions of-pinene, (ii) formation of multiple generations of peroxy radicals, (iii) formation of accretion products (dimers), and (iv) isoprene-driven suppression of accretion product formation, as observed in experiments. The mechanism has been constructed through optimisation against a series of flow tube laboratory experiments. The mechanism predicts a HOM yield of 2 %-4.5% under conditions of low to moderate NOx , in line with experimental observations, and reproduces qualitatively the decline in HOM yield and concentration at higher NOx levels. The mechanism gives a HOM yield that also increases with temperature, in line with observations, and our mechanism compares favourably to some of the limited observations of [HOM] observed in the boreal forest in Finland and in the southeast USA. The reproduction of isoprene-driven suppression of HOMs is a key step forward as it enables global climate models to capture the interaction between the major BVOC species, along with the potential climatic feedbacks. This suppression is demonstrated when the mechanism is used to simulate atmospheric profiles over the boreal forest and rainforest; different isoprene concentrations result in different [HOM] distributions, illustrating the importance of BVOC interactions in atmospheric composition and climate. Finally particle nucleation rates calculated from [HOM] in present-day and preindustrial atmospheres suggest that "sulfuric-acid-free"nucleation can compete effectively with other nucleation pathways in the boreal forest, particularly in the pre-industrial period, with important implications for the aerosol budget and radiative forcing. © Author(s) 2020.
- ItemAerosol hygroscopicity parameter derived from the light scattering enhancement factor measurements in the North China Plain(Göttingen : Copernicus, 2014) Chen, J.; Zhao, C.S.; Ma, N.; Yan, P.The relative humidity (RH) dependence of aerosol light scattering is an essential parameter for accurate estimation of the direct radiative forcing induced by aerosol particles. Because of insufficient information on aerosol hygroscopicity in climate models, a more detailed parameterization of hygroscopic growth factors and resulting optical properties with respect to location, time, sources, aerosol chemistry and meteorology are urgently required. In this paper, a retrieval method to calculate the aerosol hygroscopicity parameter, κ, is proposed based on the in situ measured aerosol light scattering enhancement factor, namely f(RH), and particle number size distribution (PNSD) obtained from the HaChi (Haze in China) campaign. Measurements show that f(RH) increases sharply with increasing RH, and that the time variance of f(RH) is much greater at higher RH. A sensitivity analysis reveals that the f(RH) is more sensitive to the aerosol hygroscopicity than PNSD. f(RH) for polluted cases is distinctly higher than that for clean periods at a specific RH. The derived equivalent κ, combined with the PNSD measurements, is applied in the prediction of the cloud condensation nuclei (CCN) number concentration. The predicted CCN number concentration with the derived equivalent κ agrees well with the measured ones, especially at high supersaturations. The proposed calculation algorithm of κ with the f(RH) measurements is demonstrated to be reasonable and can be widely applied.
- ItemHow the extreme 2019-2020 Australian wildfires affected global circulation and adjustments(Katlenburg-Lindau : EGU, 2023) Senf, Fabian; Heinold, Bernd; Kubin, Anne; Müller, Jason; Schrödner, Roland; Tegen, InaWildfires are a significant source of absorbing aerosols in the atmosphere. Extreme fires in particular, such as those during the 2019-2020 Australian wildfire season (Black Summer fires), can have considerable large-scale effects. In this context, the climate impact of extreme wildfires unfolds not only because of the emitted carbon dioxide but also due to smoke aerosol released up to an altitude of 17ĝ€¯km. The overall aerosol effects depend on a variety of factors, such as the amount emitted, the injection height, and the composition of the burned material, and is therefore subject to considerable uncertainty. In the present study, we address the global impact caused by the exceptionally strong and high-reaching smoke emissions from the Australian wildfires using simulations with a global aerosol-climate model. We show that the absorption of solar radiation by the black carbon contained in the emitted smoke led to a shortwave radiative forcing of more than +5ĝ€¯Wm-2 in the southern mid-latitudes of the lower stratosphere. Subsequent adjustment processes in the stratosphere slowed down the diabatically driven meridional circulation, thus redistributing the heating perturbation on a global scale. As a result of these stratospheric adjustments, a positive temperature perturbation developed in both hemispheres, leading to additional longwave radiation emitted back to space. According to the model results, this adjustment occurred in the stratosphere within the first 2 months after the event. At the top of the atmosphere (TOA), the net effective radiative forcing (ERF) averaged over the Southern Hemisphere was initially dominated by the instantaneous positive radiative forcing of about +0.5ĝ€¯Wm-2, for which the positive sign resulted mainly from the presence of clouds above the Southern Ocean. The longwave adjustments led to a compensation of the initially net positive TOA ERF, which is seen in the Southern Hemisphere, the tropics, and the northern mid-latitudes. The simulated changes in the lower stratosphere also affected the upper troposphere through a thermodynamic downward coupling. Subsequently, increased temperatures were also obtained in the upper troposphere, causing a global decrease in relative humidity, cirrus amount, and the ice water path of about 0.2ĝ€¯%. As a result, surface precipitation also decreased by a similar amount, which was accompanied by a weakening of the tropospheric circulation due to the given energetic constraints. In general, it appears that the radiative effects of smoke from single extreme wildfire events can lead to global impacts that affect the interplay of tropospheric and stratospheric budgets in complex ways. This emphasizes that future changes in extreme wildfires need to be included in projections of aerosol radiative forcing.
- ItemGeoengineering climate by stratospheric sulfur injections: Earth system vulnerability to technological failure(Dordrecht [u.a.] : Springer, 2009) Brovkin, V.; Petoukhov, V.; Claussen, M.; Bauer, E.; Archer, D.; Jaeger, C.We use a coupled climate-carbon cycle model of intermediate complexity to investigate scenarios of stratospheric sulfur injections as a measure to compensate for CO2-induced global warming. The baseline scenario includes the burning of 5,000 GtC of fossil fuels. A full compensation of CO2-induced warming requires a load of about 13 MtS in the stratosphere at the peak of atmospheric CO2 concentration. Keeping global warming below 2°C reduces this load to 9 MtS. Compensation of CO 2 forcing by stratospheric aerosols leads to a global reduction in precipitation, warmer winters in the high northern latitudes and cooler summers over northern hemisphere landmasses. The average surface ocean pH decreases by 0.7, reducing the calcifying ability of marine organisms. Because of the millennial persistence of the fossil fuel CO2 in the atmosphere, high levels of stratospheric aerosol loading would have to continue for thousands of years until CO2 was removed from the atmosphere. A termination of stratospheric aerosol loading results in abrupt global warming of up to 5°C within several decades, a vulnerability of the Earth system to technological failure. © 2008 The Author(s).
- ItemThe global aerosol-climate model ECHAM6.3-HAM2.3-Part 2: Cloud evaluation, aerosol radiative forcing, and climate sensitivity(Katlenburg-Lindau : Copernicus, 2019) Neubauer, David; Ferrachat, Sylvaine; Siegenthaler-Le Drian, Colombe; Stier, Philip; Partridge, Daniel G.; Tegen, Ina; Bey, Isabelle; Stanelle, Tanja; Kokkola, Harri; Lohmann, UlrikeThe global aerosol–climate model ECHAM6.3–HAM2.3 (E63H23) as well as the previous model versions ECHAM5.5–HAM2.0 (E55H20) and ECHAM6.1–HAM2.2 (E61H22) are evaluated using global observational datasets for clouds and precipitation. In E63H23, the amount of low clouds, the liquid and ice water path, and cloud radiative effects are more realistic than in previous model versions. E63H23 has a more physically based aerosol activation scheme, improvements in the cloud cover scheme, changes in the detrainment of convective clouds, changes in the sticking efficiency for the accretion of ice crystals by snow, consistent ice crystal shapes throughout the model, and changes in mixed-phase freezing; an inconsistency in ice crystal number concentration (ICNC) in cirrus clouds was also removed. Common biases in ECHAM and in E63H23 (and in previous ECHAM–HAM versions) are a cloud amount in stratocumulus regions that is too low and deep convective clouds over the Atlantic and Pacific oceans that form too close to the continents (while tropical land precipitation is underestimated). There are indications that ICNCs are overestimated in E63H23. Since clouds are important for effective radiative forcing due to aerosol–radiation and aerosol–cloud interactions (ERFari+aci) and equilibrium climate sensitivity (ECS), differences in ERFari+aci and ECS between the model versions were also analyzed. ERFari+aci is weaker in E63H23 (−1.0 W m−2) than in E61H22 (−1.2 W m−2) (or E55H20; −1.1 W m−2). This is caused by the weaker shortwave ERFari+aci (a new aerosol activation scheme and sea salt emission parameterization in E63H23, more realistic simulation of cloud water) overcompensating for the weaker longwave ERFari+aci (removal of an inconsistency in ICNC in cirrus clouds in E61H22). The decrease in ECS in E63H23 (2.5 K) compared to E61H22 (2.8 K) is due to changes in the entrainment rate for shallow convection (affecting the cloud amount feedback) and a stronger cloud phase feedback. Experiments with minimum cloud droplet number concentrations (CDNCmin) of 40 cm−3 or 10 cm−3 show that a higher value of CDNCmin reduces ERFari+aci as well as ECS in E63H23.
- ItemCoupling aerosols to (cirrus) clouds in the global EMAC-MADE3 aerosol–climate model(Katlenburg-Lindau : Copernicus, 2020) Righi, Mattia; Hendricks, Johannes; Lohmann, Ulrike; Beer, Christof Gerhard; Hahn, Valerian; Heinold, Bernd; Heller, Romy; Krämer, Martina; Ponater, Michael; Rolf, Christian; Tegen, Ina; Voigt, ChristianeA new cloud microphysical scheme including a detailed parameterization for aerosol-driven ice formation in cirrus clouds is implemented in the global ECHAM/MESSy Atmospheric Chemistry (EMAC) chemistry–climate model and coupled to the third generation of the Modal Aerosol Dynamics model for Europe adapted for global applications (MADE3) aerosol submodel. The new scheme is able to consistently simulate three regimes of stratiform clouds – liquid, mixed-, and ice-phase (cirrus) clouds – considering the activation of aerosol particles to form cloud droplets and the nucleation of ice crystals. In the cirrus regime, it allows for the competition between homogeneous and heterogeneous freezing for the available supersaturated water vapor, taking into account different types of ice-nucleating particles, whose specific ice-nucleating properties can be flexibly varied in the model setup. The new model configuration is tuned to find the optimal set of parameters that minimizes the model deviations with respect to observations. A detailed evaluation is also performed comparing the model results for standard cloud and radiation variables with a comprehensive set of observations from satellite retrievals and in situ measurements. The performance of EMAC-MADE3 in this new coupled configuration is in line with similar global coupled models and with other global aerosol models featuring ice cloud parameterizations. Some remaining discrepancies, namely a high positive bias in liquid water path in the Northern Hemisphere and overestimated (underestimated) cloud droplet number concentrations over the tropical oceans (in the extratropical regions), which are both a common problem in these kinds of models, need to be taken into account in future applications of the model. To further demonstrate the readiness of the new model system for application studies, an estimate of the anthropogenic aerosol effective radiative forcing (ERF) is provided, showing that EMAC-MADE3 simulates a relatively strong aerosol-induced cooling but within the range reported in the Intergovernmental Panel on Climate Change (IPCC) assessments.