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Using an interactive aerosol‐climate model we find that absorbing anthropogenic aerosols, whether coexisting with scattering aerosols or not, can significantly affect the Indian summer monsoon system. We also show that the influence is reflected in a perturbation to the moist static energy in the sub‐cloud layer, initiated as a heating by absorbing aerosols to the planetary boundary layer. The perturbation appears mostly over land, extending from just north of the Arabian Sea to northern India along the southern slope of the Tibetan Plateau. As a result, during the summer monsoon season, modeled convective precipitation experiences a clear northward shift, coincidently in general agreement with observed monsoon precipitation changes in recent decades particularly during the onset season. We demonstrate that the sub‐cloud layer moist static energy is a useful quantity for determining the impact of aerosols on the northward extent and to a certain degree the strength of monsoon convection.

Asian emissions of anthropogenic aerosols and their precursors have increased rapidly since 1980, with half of the increase since the pre-industrial era occurring in this period. Transient experiments with the HadGEM3-GC2 coupled model were designed to isolate the impact of Asian anthropogenic aerosols on global climate in boreal winter. It is found that this increase has resulted in local circulation changes, which in turn have driven decreases in precipitation over China, alongside an intensification of the offshore monsoon flow. No large temperature changes are seen over China. Over India, the opposite response is found, with decreasing temperatures and increasing precipitation. The dominant feature of the local circulation changes is an increase in low-level convergence, ascent, and precipitation over the Maritime Continent, which forms part of a tropical Pacific-wide La Niña-like response. HadGEM3-GC2 also simulates pronounced far-field responses. A decreased meridional temperature gradient in the North Pacific leads to a positive Pacific–North American circulation pattern, with associated temperature anomalies over the North Pacific and North America. Anomalous northeasterly flow over northeast Europe drives advection of cold air into central and western Europe, causing cooling in this region. An anomalous anticyclonic circulation over the North Atlantic causes drying over western Europe. Using a steady-state primitive equation model, LUMA, we demonstrate that these far-field midlatitude responses arise primarily as a result of Rossby waves generated over China, rather than in the equatorial Pacific.

In recent years, sea spray as well as the biological material it contains has received increased attention as a source of ice-nucleating particles (INPs). Such INPs may play a role in remote marine regions, where other sources of INPs are scarce or absent. In the Arctic, these INPs can influence water–ice partitioning in low-level clouds and thereby the cloud lifetime, with consequences for the surface energy budget, sea ice formation and melt, and climate. Marine aerosol is of a diverse nature, so identifying sources of INPs is challenging. One fraction of marine bioaerosol (phytoplankton and their exudates) has been a particular focus of marine INP research. In our study we attempt to address three main questions. Firstly, we compare the ice-nucleating ability of two common phytoplankton species with Arctic seawater microlayer samples using the same instrumentation to see if these phytoplankton species produce ice-nucleating material with sufficient activity to account for the ice nucleation observed in Arctic microlayer samples. We present the first measurements of the ice-nucleating ability of two predominant phytoplankton species: Melosira arctica, a common Arctic diatom species, and Skeletonema marinoi, a ubiquitous diatom species across oceans worldwide. To determine the potential effect of nutrient conditions and characteristics of the algal culture, such as the amount of organic carbon associated with algal cells, on the ice nucleation activity, Skeletonema marinoi was grown under different nutrient regimes. From comparison of the ice nucleation data of the algal cultures to those obtained from a range of sea surface microlayer (SML) samples obtained during three different field expeditions to the Arctic (ACCACIA, NETCARE, and ASCOS), we found that they were not as ice active as the investigated microlayer samples, although these diatoms do produce ice-nucleating material. Secondly, to improve our understanding of local Arctic marine sources as atmospheric INPs we applied two aerosolization techniques to analyse the ice-nucleating ability of aerosolized microlayer and algal samples. The aerosols were generated either by direct nebulization of the undiluted bulk solutions or by the addition of the samples to a sea spray simulation chamber filled with artificial seawater. The latter method generates aerosol particles using a plunging jet to mimic the process of oceanic wave breaking. We observed that the aerosols produced using this approach can be ice active, indicating that the ice-nucleating material in seawater can indeed transfer to the aerosol phase. Thirdly, we attempted to measure ice nucleation activity across the entire temperature range relevant for mixed-phase clouds using a suite of ice nucleation measurement techniques – an expansion cloud chamber, a continuous-flow diffusion chamber, and a cold stage. In order to compare the measurements made using the different instruments, we have normalized the data in relation to the mass of salt present in the nascent sea spray aerosol. At temperatures above 248 K some of the SML samples were very effective at nucleating ice, but there was substantial variability between the different samples. In contrast, there was much less variability between samples below 248 K. We discuss our results in the context of aerosol–cloud interactions in the Arctic with a focus on furthering our understanding of which INP types may be important in the Arctic atmosphere.

The global aerosol extinction from the CALIOP space lidar was used to compute aerosol optical depth (AOD) over a 9-year period (2007–2015) and partitioned between the boundary layer (BL) and the free troposphere (FT) using BL heights obtained from the ERA-Interim archive. The results show that the vertical distribution of AOD does not follow the diurnal cycle of the BL but remains similar between day and night highlighting the presence of a residual layer during night. The BL and FT contribute 69 and 31 %, respectively, to the global tropospheric AOD during daytime in line with observations obtained in Aire sur l'Adour (France) using the Light Optical Aerosol Counter (LOAC) instrument. The FT AOD contribution is larger in the tropics than at mid-latitudes which indicates that convective transport largely controls the vertical profile of aerosols. Over oceans, the FT AOD contribution is mainly governed by long-range transport of aerosols from emission sources located within neighboring continents. According to the CALIOP aerosol classification, dust and smoke particles are the main aerosol types transported into the FT. Overall, the study shows that the fraction of AOD in the FT – and thus potentially located above low-level clouds – is substantial and deserves more attention when evaluating the radiative effect of aerosols in climate models. More generally, the results have implications for processes determining the overall budgets, sources, sinks and transport of aerosol particles and their description in atmospheric models.

We perform a model intercomparison of summertime high Arctic (> 80∘ N) clouds observed during the 2008 Arctic Summer Cloud Ocean Study (ASCOS) campaign, when observed cloud condensation nuclei (CCN) concentrations fell below 1 cm−3. Previous analyses have suggested that at these low CCN concentrations the liquid water content (LWC) and radiative properties of the clouds are determined primarily by the CCN concentrations, conditions that have previously been referred to as the tenuous cloud regime. The intercomparison includes results from three large eddy simulation models (UCLALES-SALSA, COSMO-LES, and MIMICA) and three numerical weather prediction models (COSMO-NWP, WRF, and UM-CASIM). We test the sensitivities of the model results to different treatments of cloud droplet activation, including prescribed cloud droplet number concentrations (CDNCs) and diagnostic CCN activation based on either fixed aerosol concentrations or prognostic aerosol with in-cloud processing. There remains considerable diversity even in experiments with prescribed CDNCs and prescribed ice crystal number concentrations (ICNC). The sensitivity of mixed-phase Arctic cloud properties to changes in CDNC depends on the representation of the cloud droplet size distribution within each model, which impacts autoconversion rates. Our results therefore suggest that properly estimating aerosol–cloud interactions requires an appropriate treatment of the cloud droplet size distribution within models, as well as in situ observations of hydrometeor size distributions to constrain them. The results strongly support the hypothesis that the liquid water content of these clouds is CCN limited. For the observed meteorological conditions, the cloud generally did not collapse when the CCN concentration was held constant at the relatively high CCN concentrations measured during the cloudy period, but the cloud thins or collapses as the CCN concentration is reduced. The CCN concentration at which collapse occurs varies substantially between models. Only one model predicts complete dissipation of the cloud due to glaciation, and this occurs only for the largest prescribed ICNC tested in this study. Global and regional models with either prescribed CDNCs or prescribed aerosol concentrations would not reproduce these dissipation events. Additionally, future increases in Arctic aerosol concentrations would be expected to decrease the frequency of occurrence of such cloud dissipation events, with implications for the radiative balance at the surface. Our results also show that cooling of the sea-ice surface following cloud dissipation increases atmospheric stability near the surface, further suppressing cloud formation. Therefore, this suggests that linkages between aerosol and clouds, as well as linkages between clouds, surface temperatures, and atmospheric stability need to be considered for weather and climate predictions in this region.

Pulses of warm and moist air from lower latitudes provide energy to the Arctic and form its main energy source outside of the summer months. These pulses can cause substantial surface warming and trigger ice melt. Air-mass transport in the opposite direction, away from the Arctic, leads to cold-air outbreaks. The outbreaks are often associated with cold extremes over continents, and extreme surface heat fluxes and occasional polar lows over oceans. Air masses advected across the strong Arctic-to-mid-latitude temperature gradient are rapidly transformed into colder and dryer or warmer and moister air masses by clouds, radiative and turbulent processes, particularly in the boundary layer. Phase changes from liquid to ice within boundary-layer clouds are critical in these air-mass transformations. The presence of liquid water determines the radiative effects of these clouds, whereas the presence of ice is crucial for subsequent cloud decay or dissipation, processes that are poorly represented in weather and climate models. We argue that a better understanding of how air masses are transformed on their way into and out of the Arctic is essential for improved prediction of weather and climate in the Arctic and mid-latitudes. Observational and modelling exercises should take an air-mass-following Lagrangian approach to attain these goals.

The coupled climate model EC-Earth2 is used to investigate the impact of direct radiative effects of aerosols on stationary waves in the northern hemisphere wintertime circulation. The direct effect of aerosols is simulated by introducing prescribed mixing ratios of different aerosol compounds representing pre-industrial and present-day conditions, no indirect effects are included. In the EC-Earth2 results, the surface temperature response is uncorrelated with the highly asymmetric aerosol radiative forcing pattern. Instead, the anomalous extratropical temperature field bears a strong resemblance to the aerosol-induced changes in the stationary-wave pattern. It is demonstrated that the main features of the wave pattern of EC-Earth2 can be replicated by a linear, baroclinic model forced with latent heat changes corresponding to the anomalous convective precipitation generated by EC-Earth2. The tropical latent heat release is an effective means of generating stationary wave trains that propagate into the extratropics. Hence, the results of the present study indicate that aerosol-induced convective precipitation anomalies govern the extratropical wave-field changes, and that the far-field temperature response dominates over local effects of aerosol radiative forcing.

There is a large range of future aerosol emissions scenarios explored in the Shared Socioeconomic Pathways (SSPs), with plausible pathways spanning a range of possibilities from large global reductions in emissions by 2050 to moderate global increases over the same period. Diversity in emissions across the pathways is particularly large over Asia. Rapid reductions in anthropogenic aerosol and precursor emissions between the present day and the 2050s lead to enhanced increases in global and Asian summer monsoon precipitation relative to scenarios with weak air quality policies. However, the effects of aerosol reductions do not persist to the end of the 21st century for precipitation, when instead the response to greenhouse gases dominates differences across the SSPs. The relative magnitude and spatial distribution of aerosol changes are particularly important for South Asian summer monsoon precipitation changes. Precipitation increases here are initially suppressed in SSPs 2-4.5, 3-7.0, and 5-8.5 relative to SSP1-1.9 when the impact of remote emission decreases is counteracted by continued increases in South Asian emissions.

In situ measurements of Arctic clouds frequently show that ice crystal number concentrations (ICNCs) are much higher than the number of available ice-nucleating particles (INPs), suggesting that secondary ice production (SIP) may be active. Here we use a Lagrangian parcel model (LPM) and a large-eddy simulation (LES) to investigate the impact of three SIP mechanisms (rime splintering, break-up from ice–ice collisions and drop shattering) on a summer Arctic stratocumulus case observed during the Aerosol-Cloud Coupling And Climate Interactions in the Arctic (ACCACIA) campaign. Primary ice alone cannot explain the observed ICNCs, and drop shattering is ineffective in the examined conditions. Only the combination of both rime splintering (RS) and collisional break-up (BR) can explain the observed ICNCs, since both of these mechanisms are weak when activated alone. In contrast to RS, BR is currently not represented in large-scale models; however our results indicate that this may also be a critical ice-multiplication mechanism. In general, low sensitivity of the ICNCs to the assumed INP, to the cloud condensation nuclei (CCN) conditions and also to the choice of BR parameterization is found. Finally, we show that a simplified treatment of SIP, using a LPM constrained by a LES and/or observations, provides a realistic yet computationally efficient way to study SIP effects on clouds. This method can eventually serve as a way to parameterize SIP processes in large-scale models.

The potential importance of Aitken mode particles (diameters ∼ 25–80 nm) for stratiform mixed-phase clouds in the summertime high Arctic (>80∘ N) has been investigated using two large-eddy simulation models. We find that, in both models, Aitken mode particles significantly affect the simulated microphysical and radiative properties of the cloud and can help sustain the cloud when accumulation mode concentrations are low (< 10–20 cm−3), even when the particles have low hygroscopicity (hygroscopicity parameter – κ=0.1). However, the influence of the Aitken mode decreases if the overall liquid water content of the cloud is low, either due to a higher ice fraction or due to low radiative cooling rates. An analysis of the simulated supersaturation (ss) statistics shows that the ss frequently reaches 0.5 % and sometimes even exceeds 1 %, which confirms that Aitken mode particles can be activated. The modelling results are in qualitative agreement with observations of the Hoppel minimum obtained from four different expeditions in the high Arctic. Our findings highlight the importance of better understanding Aitken mode particle formation, chemical properties and emissions, particularly in clean environments such as the high Arctic.