ALBERT

Description: It is important to understand how future environmental policies will impact both climate change and air pollution. Although targeting near-term climate forcers (NTCFs), defined here as aerosols, tropospheric ozone, and precursor gases, should improve air quality, NTCF reductions will also impact climate. Prior assessments of the impact of NTCF mitigation on air quality and climate have been limited. This is related to the idealized nature of some prior studies, simplified treatment of aerosols and chemically reactive gases, as well as a lack of a sufficiently large number of models to quantify model diversity and robust responses. Here, we quantify the 2015–2055 climate and air quality effects of non-methane NTCFs using nine state-of-the-art chemistry–climate model simulations conducted for the Aerosol and Chemistry Model Intercomparison Project (AerChemMIP). Simulations are driven by two future scenarios featuring similar increases in greenhouse gases (GHGs) but with “weak” (SSP3-7.0) versus “strong” (SSP3-7.0-lowNTCF) levels of air quality control measures. As SSP3-7.0 lacks climate policy and has the highest levels of NTCFs, our results (e.g., surface warming) represent an upper bound. Unsurprisingly, we find significant improvements in air quality under NTCF mitigation (strong versus weak air quality controls). Surface fine particulate matter (PM2.5) and ozone (O3) decrease by -2.2±0.32 µg m−3 and -4.6±0.88 ppb, respectively (changes quoted here are for the entire 2015–2055 time period; uncertainty represents the 95 % confidence interval), over global land surfaces, with larger reductions in some regions including south and southeast Asia. Non-methane NTCF mitigation, however, leads to additional climate change due to the removal of aerosol which causes a net warming effect, including global mean surface temperature and precipitation increases of 0.25±0.12 K and 0.03±0.012 mm d−1, respectively. Similarly, increases in extreme weather indices, including the hottest and wettest days, also occur. Regionally, the largest warming and wetting occurs over Asia, including central and north Asia (0.66±0.20 K and 0.03±0.02 mm d−1), south Asia (0.47±0.16 K and 0.17±0.09 mm d−1), and east Asia (0.46±0.20 K and 0.15±0.06 mm d−1). Relatively large warming and wetting of the Arctic also occur at 0.59±0.36 K and 0.04±0.02 mm d−1, respectively. Similar surface warming occurs in model simulations with aerosol-only mitigation, implying weak cooling due to ozone reductions. Our findings suggest that future policies that aggressively target non-methane NTCF reductions will improve air quality but will lead to additional surface warming, particularly in Asia and the Arctic. Policies that address other NTCFs including methane, as well as carbon dioxide emissions, must also be adopted to meet climate mitigation goals.

Description: The largest contributors to the uncertainty in assessing the anthropogenic contribution in radiative forcing are the direct and indirect effects of aerosol particles on the Earth's radiative budget. Soot particles are of special interest since their properties can change significantly due to aging processes once they are emitted into the atmosphere. Probably the largest obstacle for the investigation of these processes in the laboratory is the long atmospheric lifetime of 1 week, requiring tailored experiments that cover this time span. This work presents results on the ability of two types of soot, obtained using a miniCAST soot generator, to act as cloud condensation nuclei (CCN) after exposure to atmospherically relevant levels of ozone (O3) and humidity. Aging times of up to 12 h were achieved by successful application of the continuous-flow stirred tank reactor (CSTR) concept while allowing for size selection of particles prior to the aging step. Particles of 100 nm diameter and rich in organic carbon (OC) that were initially CCN inactive showed significant CCN activity at supersaturations (SS) down to 0.3 % after 10 h of exposure to 200 ppb of O3. While this process was not affected by different levels of relative humidity in the range of 5 %–75 %, a high sensitivity towards the ambient/reaction temperature was observed. Soot particles with a lower OC content required an approximately 4-fold longer aging duration to show CCN activity at the same SS. Prior to the slow change in the CCN activity, a rapid increase in the particle diameter was detected which occurred within several minutes. This study highlights the applicability of the CSTR approach for the simulation of atmospheric aging processes, as aging durations beyond 12 h can be achieved in comparably small aerosol chamber volumes (

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: How clouds change in a warmer climate remains one of the largest uncertainties for the equilibrium climate sensitivity (ECS). While a large spread in the cloud feedback arises from low-level clouds, it was recently shown that mixed-phase clouds are also important for ECS. If mixed-phase clouds in the current climate contain too few supercooled cloud droplets, too much ice will change to liquid water in a warmer climate. As shown by Tan et al. (2016), this overestimates the negative cloud-phase feedback and underestimates ECS in the CAM global climate model (GCM). Here we use the newest version of the ECHAM6-HAM2 GCM to investigate the importance of mixed-phase and ice clouds for ECS. Although we also considerably underestimate the fraction of supercooled liquid water globally in the reference version of the ECHAM6-HAM2 GCM, we do not obtain increases in ECS in simulations with more supercooled liquid water in the present-day climate, different from the findings by Tan et al. (2016). We hypothesize that it is not the global supercooled liquid water fraction that matters, but only how well low- and mid-level mixed-phase clouds with cloud-top temperatures in the mixed-phase temperature range between 0 and −35 ∘C that are not shielded by higher-lying ice clouds are simulated. These occur most frequently in midlatitudes, in particular over the Southern Ocean where they determine the amount of absorbed shortwave radiation. In ECHAM6-HAM2 the amount of absorbed shortwave radiation over the Southern Ocean is only significantly overestimated if all clouds below 0 ∘C consist exclusively of ice. Only in this simulation is ECS significantly smaller than in all other simulations and the cloud optical depth feedback is the dominant cloud feedback. In all other simulations, the cloud optical depth feedback is weak and changes in cloud feedbacks associated with cloud amount and cloud-top pressure dominate the overall cloud feedback. However, apart from the simulation with only ice below 0 ∘C, differences in the overall cloud feedback are not translated into differences in ECS in our model. This insensitivity to the cloud feedback in our model is explained with compensating effects in the clear sky.

Description: In situ cloud observations at mountain-top research stations regularly measure ice crystal number concentrations (ICNCs) orders of magnitudes higher than expected from measurements of ice nucleating particle (INP) concentrations. Thus, several studies suggest that mountain-top in situ cloud microphysical measurements are influenced by surface processes, e.g., blowing snow, hoar frost or riming on snow-covered trees, rocks and the snow surface. This limits the relevance of such measurements for the study of microphysical properties and processes in free-floating clouds. This study assesses the impact of surface processes on in situ cloud observations at the Sonnblick Observatory in the Hohen Tauern region, Austria. Vertical profiles of ICNCs above a snow-covered surface were observed up to a height of 10 m. The ICNC decreases at least by a factor of 2 at 10 m if the ICNC at the surface is larger than 100 L−1. This decrease can be up to 1 order of magnitude during in-cloud conditions and reached its maximum of more than 2 orders of magnitudes when the station was not in cloud. For one case study, the ICNC for regular and irregular ice crystals showed a similar relative decrease with height. This suggests that either surface processes produce both irregular and regular ice crystals or other effects modify the ICNCs near the surface. Therefore, two near-surface processes are proposed to enrich ICNCs near the surface. Either sedimenting ice crystals are captured in a turbulent layer above the surface or the ICNC is enhanced in a convergence zone because the cloud is forced over a mountain. These two processes would also have an impact on ICNCs measured at mountain-top stations if the surrounding surface is not snow covered. Conclusively, this study strongly suggests that ICNCs measured at mountain-top stations are not representative of the properties of a cloud further away from the surface.

Description: The complexity of atmospheric aerosol causes large uncertainties in its parameterization in atmospheric models. In a process-based comparison of two aerosol and chemistry schemes within the regional atmospheric modeling framework COSMO-ART (Consortium for Small-Scale Modelling, Aersosol and Reactive Trace gases extension), we identify key sensitivities of aerosol parameterizations. We consider the aerosol module MADE (Modal Aerosol Dynamics model for Europe) in combination with full gas-phase chemistry and the aerosol module M7 in combination with a constant-oxidant-field-based sulfur cycle. For a Saharan dust outbreak reaching Europe, modeled aerosol populations are more sensitive to structural differences between the schemes, in particular the consideration of aqueous-phase sulfate production, the selection of aerosol species and modes, and modal composition, than to parametric choices like modal standard deviation and the parameterization of aerosol dynamics. The same observation applies to aerosol optical depth (AOD) and the concentrations of cloud condensation nuclei (CCN). Differences in the concentrations of ice-nucleating particles (INPs) are masked by uncertainties between two ice-nucleation parameterizations and their coupling to the aerosol scheme. Differences in cloud droplet and ice crystal number concentrations are buffered by cloud microphysics as we show in a susceptibility analysis.

Description: Ice 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.

Description: Heterogeneous ice formation by immersion freezing in mixed-phase clouds can be parameterized in general circulation models (GCMs) by classical nucleation theory (CNT). CNT parameterization schemes describe immersion freezing as a stochastic process, including the properties of insoluble aerosol particles in the droplets. There are different ways to parameterize the properties of aerosol particles (i.e., contact angle schemes), which are compiled and tested in this paper. The goal of this study is to find a parameterization scheme for GCMs to describe immersion freezing with the ability to shift and adjust the slope of the freezing curve compared to homogeneous freezing to match experimental data. We showed in a previous publication that the resulting freezing curves from CNT are very sensitive to unconstrained kinetic and thermodynamic parameters in the case of homogeneous freezing. Here we investigate how sensitive the outcome of a parameter estimation for contact angle schemes from experimental data is to unconstrained kinetic and thermodynamic parameters. We demonstrate that the parameters describing the contact angle schemes can mask the uncertainty in thermodynamic and kinetic parameters. Different CNT formulations are fitted to an extensive immersion freezing dataset consisting of size-selected measurements as a function of temperature and time for different mineral dust types, namely kaolinite, illite, montmorillonite, microcline (K-feldspar), and Arizona test dust. We investigated how accurate different CNT formulations (with estimated fit parameters for different contact angle schemes) reproduce the measured freezing data, especially the time and particle size dependence of the freezing process. The results are compared to a simplified deterministic freezing scheme. In this context, we evaluated which CNT-based parameterization scheme able to represent particle properties is the best choice to describe immersion freezing in a GCM.

Description: In situ observations of cloud properties in complex alpine terrain where research aircraft cannot sample are commonly conducted at mountain-top research stations and limited to single-point measurements. The HoloGondel platform overcomes this limitation by using a cable car to obtain vertical profiles of the microphysical and meteorological cloud parameters. The main component of the HoloGondel platform is the HOLographic Imager for Microscopic Objects (HOLIMO 3G), which uses digital in-line holography to image cloud particles. Based on two-dimensional images the microphysical cloud parameters for the size range from small cloud particles to large precipitation particles are obtained for the liquid and ice phase. The low traveling velocity of a cable car on the order of 10 m s−1 allows measurements with high spatial resolution; however, at the same time it leads to an unstable air speed towards the HoloGondel platform. Holographic cloud imagers, which have a sample volume that is independent of the air speed, are therefore well suited for measurements on a cable car. Example measurements of the vertical profiles observed in a liquid cloud and a mixed-phase cloud at the Eggishorn in the Swiss Alps in the winters 2015 and 2016 are presented. The HoloGondel platform reliably observes cloud droplets larger than 6.5 µm, partitions between cloud droplets and ice crystals for a size larger than 25 µm and obtains a statistically significantly size distribution for every 5 m in vertical ascent.

Description: Mineral dust particles from deserts are amongst the most common ice nucleating particles in the atmosphere. The mineralogy of desert dust differs depending on the source region and can further fractionate during the dust emission processes. Mineralogy to a large extent explains the ice nucleation behavior of desert aerosol, but not entirely. Apart from pure mineral dust, desert aerosol particles often exhibit a coating or are mixed with small amounts of biological material. Aging on the ground or during atmospheric transport can deactivate nucleation sites, thus strong ice nucleating minerals may not exhibit their full potential. In the partner paper of this work, it was shown that mineralogy determines most but not all of the ice nucleation behavior in the immersion mode found for desert dust. In this study, the influence of semi-volatile organic compounds and the presence of crystal water on the ice nucleation behavior of desert aerosol is investigated. This work focuses on the deposition and condensation ice nucleation modes at temperatures between 238 and 242 K of 18 dust samples sourced from nine deserts worldwide. Chemical imaging of the particles' surface is used to determine the cause of the observed differences in ice nucleation. It is found that, while the ice nucleation ability of the majority of the dust samples is dominated by their quartz and feldspar content, in one carbonaceous sample it is mostly caused by organic matter, potentially cellulose and/or proteins. In contrast, the ice nucleation ability of an airborne Saharan sample is found to be diminished, likely by semi-volatile species covering ice nucleation active sites of the minerals. This study shows that in addition to mineralogy, other factors such as organics and crystal water content can alter the ice nucleation behavior of desert aerosol during atmospheric transport in various ways.