Implementing a sectional scheme for early aerosol growth from new particle formation in the Norwegian Earth System Model v2 : comparison to observations and climate impacts

Aerosol-cloud interactions contribute to a large portion of the spread in estimates of climate forcing, climate sensitivity and future projections. An important part of this uncertainty is how much new particle formation (NPF) contributes to cloud condensation nuclei (CCN) and, furthermore, how this changes with changes in anthropogenic emissions. Incorporating NPF and early growth in Earth system models (ESMs) is, however, challenging due to uncertain parameters (e.g. participating vapours), structural issues (numerical description of growth from similar to 1 to similar to 100 nm) and the large scale of an ESM grid compared to the NPF scale. A common approach in ESMs is to represent the particle size distribution by a certain number of log-normal modes. Sectional schemes, on the other hand, in which the size distribution is represented by bins, are considered closer to first principles because they do not make an a priori assumption about the size distribution. In order to improve the representation of early growth, we have implemented a sectional scheme for the smallest particles (5-39.6 nm diameter) in the Norwegian Earth System Model (NorESM), feeding particles into the original aerosol scheme. This is, to our knowledge, the first time such an approach has been tried. We find that including the sectional scheme for early growth improves the aerosol number concentration in the model when comparing against observations, particularly in the 50-100 nm diameter range. Furthermore, we find that the model with the sectional scheme produces much fewer particles than the original scheme in polluted regions, while it produces more in remote regions and the free troposphere, indicating a potential impact on the estimated aerosol forcing. Finally, we analyse the effect on cloud-aerosol interactions and find that the effect of changes in NPF efficiency on clouds is highly heterogeneous in space. While in remote regions, more efficient NPF leads to higher cloud droplet number concentration (CDNC), in polluted regions the opposite is in fact the case.Peer reviewe

BVOC-aerosol-climate feedbacks investigated using NorESM

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.Peer reviewe

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

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

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

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.Peer reviewe

Process-evaluation of forest aerosol-cloud-climate feedback shows clear evidence from observations and large uncertainty in models

Abstract Natural aerosol feedbacks are expected to become more important in the future, as anthropogenic aerosol emissions decrease due to air quality policy. One such feedback is initiated by the increase in biogenic volatile organic compound (BVOC) emissions with higher temperatures, leading to higher secondary organic aerosol (SOA) production and a cooling of the surface via impacts on cloud radiative properties. Motivated by the considerable spread in feedback strength in Earth System Models (ESMs), we here use two long-term observational datasets from boreal and tropical forests, together with satellite data, for a process-based evaluation of the BVOC-aerosol-cloud feedback in four ESMs. The model evaluation shows that the weakest modelled feedback estimates can likely be excluded, but highlights compensating errors making it difficult to draw conclusions of the strongest estimates. Overall, the method of evaluating along process chains shows promise in pin-pointing sources of uncertainty and constraining modelled aerosol feedbacks

Potential pre-industrial–like new particle formation induced by pure biogenic organic vapors in Finnish peatland

Pure biogenic new particle formation (NPF) induced by highly oxygenated organic molecules (HOMs) could be an important mechanism for pre-industrial aerosol formation. However, it has not been unambiguously confirmed in the ambient due to the scarcity of truly pristine continental locations in the present-day atmosphere or the lack of chemical characterization of NPF precursors. Here, we report ambient observations of pure biogenic HOM-driven NPF over a peatland in southern Finland. Meteorological decoupling processes formed an “air pocket” (i.e., a very shallow surface layer) at night and favored NPF initiated entirely by biogenic HOM from this peatland, whose atmospheric environment closely resembles that of the pre-industrial era. Our study sheds light on pre-industrial aerosol formation, which represents the baseline for estimating the impact of present and future aerosol on climate, as well as on future NPF, the features of which may revert toward pre-industrial–like conditions due to air pollution mitigation.Peer reviewe