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- 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.
- 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.
- ItemNOy production, ozone loss and changes in net radiative heating due to energetic particle precipitation in 2002–2010(Katlenburg-Lindau : EGU, 2018-1-29) Sinnhuber, Miriam; Berger, Uwe; Funke, Bernd; Nieder, Holger; Reddmann, Thomas; Stiller, Gabriele; Versick, Stefan; von Clarmann, Thomas; Wissing, Jan MaikWe analyze the impact of energetic particle precipitation on the stratospheric nitrogen budget, ozone abundances and net radiative heating using results from three global chemistry-climate models considering solar protons and geomagnetic forcing due to auroral or radiation belt electrons. Two of the models cover the atmosphere up to the lower thermosphere, the source region of auroral NO production. Geomagnetic forcing in these models is included by prescribed ionization rates. One model reaches up to about 80 km, and geomagnetic forcing is included by applying an upper boundary condition of auroral NO mixing ratios parameterized as a function of geomagnetic activity. Despite the differences in the implementation of the particle effect, the resulting modeled NOy in the upper mesosphere agrees well between all three models, demonstrating that geomagnetic forcing is represented in a consistent way either by prescribing ionization rates or by prescribing NOy at the model top. Compared with observations of stratospheric and mesospheric NOy from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument for the years 2002–2010, the model simulations reproduce the spatial pattern and temporal evolution well. However, after strong sudden stratospheric warmings, particle-induced NOy is underestimated by both high-top models, and after the solar proton event in October 2003, NOy is overestimated by all three models. Model results indicate that the large solar proton event in October 2003 contributed about 1–2 Gmol (109 mol) NOy per hemisphere to the stratospheric NOy budget, while downwelling of auroral NOx from the upper mesosphere and lower thermosphere contributes up to 4 Gmol NOy. Accumulation over time leads to a constant particle-induced background of about 0.5–1 Gmol per hemisphere during solar minimum, and up to 2 Gmol per hemisphere during solar maximum. Related negative anomalies of ozone are predicted by the models in nearly every polar winter, ranging from 10–50 % during solar maximum to 2–10 % during solar minimum. Ozone loss continues throughout polar summer after strong solar proton events in the Southern Hemisphere and after large sudden stratospheric warmings in the Northern Hemisphere. During mid-winter, the ozone loss causes a reduction of the infrared radiative cooling, i.e., a positive change of the net radiative heating (effective warming), in agreement with analyses of geomagnetic forcing in stratospheric temperatures which show a warming in the late winter upper stratosphere. In late winter and spring, the sign of the net radiative heating change turns to negative (effective cooling). This spring-time cooling lasts well into summer and continues until the following autumn after large solar proton events in the Southern Hemisphere, and after sudden stratospheric warmings in the Northern Hemisphere.
- ItemAn assessment of aerosol optical properties from remote-sensing observations and regional chemistry-climate coupled models over Europe(Katlenburg-Lindau : EGU, 2018) Palacios-Peña, Laura; Baró, Rocío; Baklanov, Alexander; Balzarini, Alessandra; Brunner, Dominik; Forkel, Renate; Hirtl, Marcus; Honzak, Luka; López-Romero, José María; Montávez, Juan Pedro; Pérez, Juan Luis; Pirovano, Guido; San José, Roberto; Schröder, Wolfram; Werhahn, Johannes; Wolke, Ralf; Žabkar, Rahela; Jiménez-Guerrero, PedroAtmospheric aerosols modify the radiative budget of the Earth due to their optical, microphysical and chemical properties, and are considered one of the most uncertain climate forcing agents. In order to characterise the uncertainties associated with satellite and modelling approaches to represent aerosol optical properties, mainly aerosol optical depth (AOD) and Ångström exponent (AE), their representation by different remote-sensing sensors and regional online coupled chemistry-climate models over Europe are evaluated. This work also characterises whether the inclusion of aerosol-radiation (ARI) or/and aerosol-cloud interactions (ACI) help improve the skills of modelling outputs. Two case studies were selected within the EuMetChem COST Action ES1004 framework when important aerosol episodes in 2010 all over Europe took place: a Russian wildfire episode and a Saharan desert dust outbreak that covered most of the Mediterranean Sea. The model data came from different regional air-quality-climate simulations performed by working group 2 of EuMetChem, which differed according to whether ARI or ACI was included or not. The remote-sensing data came from three different sensors: MODIS, OMI and SeaWIFS. The evaluation used classical statistical metrics to first compare satellite data versus the ground-based instrument network (AERONET) and then to evaluate model versus the observational data (both satellite and ground-based data). Regarding the uncertainty in the satellite representation of AOD, MODIS presented the best agreement with the AERONET observations compared to other satellite AOD observations. The differences found between remote-sensing sensors highlighted the uncertainty in the observations, which have to be taken into account when evaluating models. When modelling results were considered, a common trend for underestimating high AOD levels was observed. For the AE, models tended to underestimate its variability, except when considering a sectional approach in the aerosol representation. The modelling results showed better skills when ARI+ACI interactions were included; hence this improvement in the representation of AOD (above 30 % in the model error) and AE (between 20 and 75 %) is important to provide a better description of aerosol-radiation-cloud interactions in regional climate models.
- ItemThe value of remote marine aerosol measurements for constraining radiative forcing uncertainty(Katlenburg-Lindau : EGU, 2020) Regayre, Leighton A.; Schmale, Julia; Johnson, Jill S.; Tatzelt, Christian; Baccarini, Andrea; Henning, Silvia; Yoshioka, Masaru; Stratmann, Frank; Gysel-Beer, Martin; Grosvenor, Daniel P.; Carslaw, Ken S.Aerosol measurements over the Southern Ocean are used to constrain aerosol-cloud interaction radiative forcing (RFaci) uncertainty in a global climate model. Forcing uncertainty is quantified using 1 million climate model variants that sample the uncertainty in nearly 30 model parameters. Measurements of cloud condensation nuclei and other aerosol properties from an Antarctic circumnavigation expedition strongly constrain natural aerosol emissions: default sea spray emissions need to be increased by around a factor of 3 to be consistent with measurements. Forcing uncertainty is reduced by around 7% using this set of several hundred measurements, which is comparable to the 8% reduction achieved using a diverse and extensive set of over 9000 predominantly Northern Hemisphere measurements. When Southern Ocean and Northern Hemisphere measurements are combined, uncertainty in RFaci is reduced by 21 %, and the strongest 20% of forcing values are ruled out as implausible. In this combined constraint, observationally plausible RFaci is around 0.17Wm-2 weaker (less negative) with 95% credible values ranging from-2:51 to-1:17Wm-2 (standard deviation of-2:18 to-1:46Wm-2). The Southern Ocean and Northern Hemisphere measurement datasets are complementary because they constrain different processes. These results highlight the value of remote marine aerosol measurements. © 2020 Laser Institute of America. All rights reserved.