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Comparison of particle number size distribution trends in ground measurements and climate models

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, Santtu

Despite 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.

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Large difference in aerosol radiative effects from BVOC-SOA treatment in three Earth system models

2020, Sporre, Moa K., Blichner, Sara M., Schrödner, Roland, Karset, Inger H.H., Berntsen, Terje K., van Noije, Twan, Bergman, Tommi, O’Donnell, Declan, Makkonen, Risto

Biogenic volatile organic compounds (BVOCs) emitted from vegetation are oxidised in the atmosphere and can form aerosol particles either by contributing to new particle formation or by condensing onto existing aerosol particles. As the understanding of the importance of BVOCs for aerosol formation has increased over the years, these processes have made their way into Earth system models (ESMs). In this study, sensitivity experiments are run with three different ESMs (the Norwegian Earth System Model (NorESM), EC-Earth and ECHAM) to investigate how the direct and indirect aerosol radiative effects are affected by changes in the formation of secondary organic aerosol (SOA) from BVOCs. In the first two sensitivity model experiments, the yields of SOA precursors from oxidation of BVOCs are changed by ±50 %. For the third sensitivity test, the formed oxidation products do not participate in the formation of new particles but are only allowed to condense onto existing aerosols. In the last two sensitivity experiments, the emissions of BVOC compounds (isoprene and monoterpenes) are turned off, one at a time. The goal of the study is to investigate whether it is of importance to treat SOA formation processes correctly in the models rather than to evaluate the correctness of the current treatment in the models.

The results show that the impact on the direct radiative effect (DRE) is linked to the changes in the SOA production in the models, where more SOA leads to a stronger DRE and vice versa. However, the magnitude by which the DRE changes (maximally 0.15 W m-2 globally averaged) in response to the SOA changes varies between the models, with EC-Earth displaying the largest changes. The results for the cloud radiative effects (CREs) are more complicated than for the DRE. The changes in CRE differ more among the ESMs, and for some sensitivity experiments they even have different signs. The most sensitive models are NorESM and EC-Earth, which have CRE changes of up to 0.82 W m-2. The varying responses in the different models are connected to where in the aerosol size distributions the changes in mass and number due to SOA formation occur, in combination with the aerosol number concentration levels in the models. We also find that interactive gas-phase chemistry as well as the new particle formation parameterisation has important implications for the DRE and CRE in some of the sensitivity experiments. The results from this study indicate that BVOC-SOA treatment in ESMs can have a substantial impact on the modelled climate but that the sensitivity varies greatly between the models. Since BVOC emissions have changed historically and will continue to change in the future, the spread in model results found in this study implies uncertainty into ESM estimates of aerosol forcing from land-use change and BVOC feedback strengths. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.