ALBERT

Description: Oxidation products of monoterpenes and isoprene have a major influence on the global secondary organic aerosol (SOA) burden and the production of atmospheric nanoparticles and cloud condensation nuclei (CCN). Here, we investigate the formation of extremely low volatility organic compounds (ELVOC) from O3 and OH radical oxidation of several monoterpenes and isoprene in a series of laboratory experiments. We show that ELVOC from all precursors are formed within the first minute after the initial attack of an oxidant. We demonstrate that under atmospherically relevant concentrations, species with an endocyclic double bond efficiently produce ELVOC from ozonolysis, whereas the yields from OH radical-initiated reactions are smaller. If the double bond is exocyclic or the compound itself is acyclic, ozonolysis produces less ELVOC and the role of the OH radical-initiated ELVOC formation is increased. Isoprene oxidation produces marginal quantities of ELVOC regardless of the oxidant. Implementing our laboratory findings into a global modeling framework shows that biogenic SOA formation in general, and ELVOC in particular, play crucial roles in atmospheric CCN production. Monoterpene oxidation products enhance atmospheric new particle formation and growth in most continental regions, thereby increasing CCN concentrations, especially at high values of cloud supersaturation. Isoprene-derived SOA tends to suppress atmospheric new particle formation, yet it assists the growth of sub-CCN-size primary particles to CCN. Taking into account compound specific monoterpene emissions has a moderate effect on the modeled global CCN budget.

Description: We have developed new parameterizations of electrically neutral homogeneous and ion-induced sulfuric acid-water particle formation for large ranges of environmental conditions, based on an improved model that has been validated against a particle formation rate data set produced by Cosmics Leaving OUtdoor Droplets (CLOUD) experiments at European Organization for Nuclear Research (CERN). The model uses a thermodynamically consistent version of the Classical Nucleation Theory normalized using quantum chemical data. Unlike the earlier parameterizations for H2SO4-H2O nucleation, the model is applicable to extreme dry conditions where the one-component sulfuric acid limit is approached. Parameterizations are presented for the critical cluster sulfuric acid mole fraction, the critical cluster radius, the total number of molecules in the critical cluster, and the particle formation rate. If the critical cluster contains only one sulfuric acid molecule, a simple formula for kinetic particle formation can be used: this threshold has also been parameterized. The parameterization for electrically neutral particle formation is valid for the following ranges: temperatures 165–400 K, sulfuric acid concentrations 104–1013 cm−3, and relative humidities 0.001–100%. The ion-induced particle formation parameterization is valid for temperatures 195–400 K, sulfuric acid concentrations 104–1016 cm−3, and relative humidities 10−5–100%. The new parameterizations are thus applicable for the full range of conditions in the Earth's atmosphere relevant for binary sulfuric acid-water particle formation, including both tropospheric and stratospheric conditions. They are also suitable for describing particle formation in the atmosphere of Venus. ©2017. American Geophysical Union. All Rights Reserved.

Description: 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.

Description: This study assesses the change in anthropogenic aerosol forcing from the mid-1970s to the mid-2000s. Both decades had similar global-mean anthropogenic aerosol optical depths but substantially different global distributions. For both years, we quantify (i) the forcing spread due to model-internal variability and (ii) the forcing spread among models. Our assessment is based on new ensembles of atmosphere-only simulations with five state-of-the-art Earth system models. Four of these models will be used in the sixth Coupled Model Intercomparison Project (CMIP6; Eyring et al., 2016). Here, the complexity of the anthropogenic aerosol has been reduced in the participating models. In all our simulations, we prescribe the same patterns of the anthropogenic aerosol optical properties and associated effects on the cloud droplet number concentration. We calculate the instantaneous radiative forcing (RF) and the effective radiative forcing (ERF). Their difference defines the net contribution from rapid adjustments. Our simulations show a model spread in ERF from −0.4 to −0.9 W m−2. The standard deviation in annual ERF is 0.3 W m−2, based on 180 individual estimates from each participating model. This result implies that identifying the model spread in ERF due to systematic differences requires averaging over a sufficiently large number of years. Moreover, we find almost identical ERFs for the mid-1970s and mid-2000s for individual models, although there are major model differences in natural aerosols and clouds. The model-ensemble mean ERF is −0.54 W m−2 for the pre-industrial era to the mid-1970s and −0.59 W m−2 for the pre-industrial era to the mid-2000s. Our result suggests that comparing ERF changes between two observable periods rather than absolute magnitudes relative to a poorly constrained pre-industrial state might provide a better test for a model's ability to represent transient climate changes.

Description: Both higher temperatures and increased CO2 concentrations are (separately) expected to increase the emissions of biogenic volatile organic compounds (BVOCs). This has been proposed to initiate negative climate feedback mechanisms through increased formation of secondary organic aerosol (SOA). More SOA can make the clouds more reflective, which can provide a cooling. Furthermore, the increase in SOA formation has also been proposed to lead to increased aerosol scattering, resulting in an increase in diffuse radiation. This could boost gross primary production (GPP) and further increase BVOC emissions. In this study, we have used the Norwegian Earth System Model (NorESM) to investigate both these feedback mechanisms. Three sets of experiments were set up to quantify the feedback with respect to (1) doubling the CO2, (2) increasing temperatures corresponding to a doubling of CO2 and (3) the combined effect of both doubling CO2 and a warmer climate. For each of these experiments, we ran two simulations, with identical setups, except for the BVOC emissions. One simulation was run with interactive BVOC emissions, allowing the BVOC emissions to respond to changes in CO2 and/or climate. In the other simulation, the BVOC emissions were fixed at present-day conditions, essentially turning the feedback off. The comparison of these two simulations enables us to investigate each step along the feedback as well as estimate their overall relevance for the future climate. We find that the BVOC feedback can have a significant impact on the climate. The annual global BVOC emissions are up to 63 % higher when the feedback is turned on compared to when the feedback is turned off, with the largest response when both CO2 and climate are changed. The higher BVOC levels lead to the formation of more SOA mass (max 53 %) and result in more particles through increased new particle formation as well as larger particles through increased condensation. The corresponding changes in the cloud properties lead to a −0.43 W m−2 stronger net cloud forcing. This effect becomes about 50 % stronger when the model is run with reduced anthropogenic aerosol emissions, indicating that the feedback will become even more important as we decrease aerosol and precursor emissions. We do not find a boost in GPP due to increased aerosol scattering on a global scale. Instead, the fate of the GPP seems to be controlled by the BVOC effects on the clouds. However, the higher aerosol scattering associated with the higher BVOC emissions is found to also contribute with a potentially important enhanced negative direct forcing (−0.06 W m−2). The global total aerosol forcing associated with the feedback is −0.49 W m−2, indicating that it has the potential to offset about 13 % of the forcing associated with a doubling of CO2.

Description: Climate models are important tools that are used for generating climate change projections, in which aerosol–climate interactions are one of the main sources of uncertainties. In order to quantify aerosol–radiation and aerosol–cloud interactions, detailed input of anthropogenic aerosol number emissions is necessary. However, the anthropogenic aerosol number emissions are usually converted from the corresponding mass emissions in pre-compiled emission inventories through a very simplistic method depending uniquely on chemical composition, particle size and density, which are defined for a few, very wide main source sectors. In this work, the anthropogenic particle number emissions converted from the AeroCom mass in the ECHAM-HAM climate model were replaced with the recently formulated number emissions from the Greenhouse Gas and Air Pollution Interactions and Synergies (GAINS) model. In the GAINS model the emission number size distributions vary, for example, with respect to the fuel and technology. Special attention was paid to accumulation mode particles (particle diameter dp 〉 100 nm) because of (i) their capability of acting as cloud condensation nuclei (CCN), thus forming cloud droplets and affecting Earth's radiation budget, and (ii) their dominant role in forming the coagulation sink and thus limiting the concentration of sub-100 nm particles. In addition, the estimates of anthropogenic CCN formation, and thus the forcing from aerosol–climate interactions, are expected to be affected. Analysis of global particle number concentrations and size distributions reveals that GAINS implementation increases CCN concentration compared with AeroCom, with regional enhancement factors reaching values as high as 10. A comparison between modeled and observed concentrations shows that the increase in number concentration for accumulation mode particles agrees well with measurements, but it leads to a consistent underestimation of both nucleation mode and Aitken mode (dp 

Description: The Nordic Centre of Excellence CRAICC (Cryosphere–Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011–2016, is the largest joint Nordic research and innovation initiative to date, aiming to strengthen research and innovation regarding climate change issues in the Nordic region. CRAICC gathered more than 100 scientists from all Nordic countries in a virtual centre with the objectives of identifying and quantifying the major processes controlling Arctic warming and related feedback mechanisms, outlining strategies to mitigate Arctic warming, and developing Nordic Earth system modelling with a focus on short-lived climate forcers (SLCFs), including natural and anthropogenic aerosols. The outcome of CRAICC is reflected in more than 150 peer-reviewed scientific publications, most of which are in the CRAICC special issue of the journal Atmospheric Chemistry and Physics. This paper presents an overview of the main scientific topics investigated in the centre and provides the reader with a state-of-the-art comprehensive summary of what has been achieved in CRAICC with links to the particular publications for further detail. Faced with a vast amount of scientific discovery, we do not claim to completely summarize the results from CRAICC within this paper, but rather concentrate here on the main results which are related to feedback loops in climate change–cryosphere interactions that affect Arctic amplification.

Description: Snow consists of non-spherical grains of various shapes and sizes. Still, in radiative transfer calculations, snow grains are often treated as spherical. This also applies to the computation of snow albedo in the Snow, Ice, and Aerosol Radiation (SNICAR) model and in the Los Alamos sea ice model, version 4 (CICE4), both of which are employed in the Community Earth System Model and in the Norwegian Earth System Model (NorESM). In this study, we evaluate the effect of snow grain shape on climate simulated by NorESM in a slab ocean configuration of the model. An experiment with spherical snow grains (SPH) is compared with another (NONSPH) in which the snow shortwave single-scattering properties are based on a combination of three non-spherical snow grain shapes, optimized using measurements of angular scattering by blowing snow. The key difference between these treatments is that the asymmetry parameter is smaller in the non-spherical case (0.77–0.78 in the visible region) than in the spherical case (ca. 0.89). Therefore, for a given snow grain size, the use of non-spherical snow grains leads to a higher snow broadband albedo, typically by 0.02–0.03. Considering the spherical case as the baseline, this results in an instantaneous negative change in net shortwave radiation with a global-mean top-of-the-model value of ca. −0.22 Wm−2. Although this global-mean radiative effect is rather modest, the impacts on the climate simulated by NorESM are substantial. The global annual-mean 2-m air temperature in NONSPH is 1.17 K lower than in SPH, with substantially larger differences at high latitudes. The climatic response is amplified by strong snow and sea ice feedbacks. It is further demonstrated that the effect of snow grain shape could be largely offset by adjusting the snow grain size. When assuming non-spherical snow grains with the parameterized grain size increased by ca. 70 %, the climatic differences to the SPH experiment become very small. Finally, the impact of assumed snow grain shape on the radiative effects of absorbing aerosols in snow is discussed.

Description: Snow consists of non-spherical grains of various shapes and sizes. Still, in radiative transfer calculations, snow grains are often treated as spherical. This also applies to the computation of snow albedo in the Snow, Ice, and Aerosol Radiation (SNICAR) model and in the Los Alamos sea ice model, version 4 (CICE4), both of which are employed in the Community Earth System Model and in the Norwegian Earth System Model (NorESM). In this study, we evaluate the effect of snow grain shape on climate simulated by NorESM in a slab ocean configuration of the model. An experiment with spherical snow grains (SPH) is compared with another (NONSPH) in which the snow shortwave single-scattering properties are based on a combination of three non-spherical snow grain shapes optimized using measurements of angular scattering by blowing snow. The key difference between these treatments is that the asymmetry parameter is smaller in the non-spherical case (0.77–0.78 in the visible region) than in the spherical case ( ≈  0.89). Therefore, for the same effective snow grain size (or equivalently, the same specific projected area), the snow broadband albedo is higher when assuming non-spherical rather than spherical snow grains, typically by 0.02–0.03. Considering the spherical case as the baseline, this results in an instantaneous negative change in net shortwave radiation with a global-mean top-of-the-model value of ca. −0.22 W m−2. Although this global-mean radiative effect is rather modest, the impacts on the climate simulated by NorESM are substantial. The global annual-mean 2 m air temperature in NONSPH is 1.17 K lower than in SPH, with substantially larger differences at high latitudes. The climatic response is amplified by strong snow and sea ice feedbacks. It is further demonstrated that the effect of snow grain shape could be largely offset by adjusting the snow grain size. When assuming non-spherical snow grains with the parameterized grain size increased by ca. 70 %, the climatic differences to the SPH experiment become very small. Finally, the impact of assumed snow grain shape on the radiative effects of absorbing aerosols in snow is discussed.