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Even though the Arctic is remote, aerosol properties observed there are strongly influenced by anthropogenic emissions from outside the Arctic. This is particularly true for the so-called Arctic haze season (January through April). In summer (June through September), when atmospheric transport patterns change, and precipitation is more frequent, local Arctic sources, i.e., natural sources of aerosols and precursors, play an important role. Over the last few decades, significant reductions in anthropogenic emissions have taken place. At the same time a large body of literature shows evidence that the Arctic is undergoing fundamental environmental changes due to climate forcing, leading to enhanced emissions by natural processes that may impact aerosol properties. In this study, we analyze 9 aerosol chemical species and 4 particle optical properties from 10 Arctic observatories (Alert, Kevo, Pallas, Summit, Thule, Tiksi, Barrow/Utqiaġvik, Villum, and Gruvebadet and Zeppelin Observatory – both at Ny-Ålesund Research Station) to understand changes in anthropogenic and natural aerosol contributions. Variables include equivalent black carbon, particulate sulfate, nitrate, ammonium, methanesulfonic acid, sodium, iron, calcium and potassium, as well as scattering and absorption coefficients, single scattering albedo and scattering Ångström exponent. First, annual cycles are investigated, which despite anthropogenic emission reductions still show the Arctic haze phenomenon. Second, long-term trends are studied using the Mann–Kendall Theil–Sen slope method. We find in total 41 significant trends over full station records, i.e., spanning more than a decade, compared to 26 significant decadal trends. The majority of significantly declining trends is from anthropogenic tracers and occurred during the haze period, driven by emission changes between 1990 and 2000. For the summer period, no uniform picture of trends has emerged. Twenty-six percent of trends, i.e., 19 out of 73, are significant, and of those 5 are positive and 14 are negative. Negative trends include not only anthropogenic tracers such as equivalent black carbon at Kevo, but also natural indicators such as methanesulfonic acid and non-sea-salt calcium at Alert. Positive trends are observed for sulfate at Gruvebadet. No clear evidence of a significant change in the natural aerosol contribution can be observed yet. However, testing the sensitivity of the Mann–Kendall Theil–Sen method, we find that monotonic changes of around 5 % yr−1 in an aerosol property are needed to detect a significant trend within one decade. This highlights that long-term efforts well beyond a decade are needed to capture smaller changes. It is particularly important to understand the ongoing natural changes in the Arctic, where interannual variability can be high, such as with forest fire emissions and their influence on the aerosol population. To investigate the climate-change-induced influence on the aerosol population and the resulting climate feedback, long-term observations of tracers more specific to natural sources are needed, as well as of particle microphysical properties such as size distributions, which can be used to identify changes in particle populations which are not well captured by mass-oriented methods such as bulk chemical composition.

This study presents a multiparameter analysis of aerosol trends over the last 2 decades at regional and global scales. Regional time series have been computed for a set of nine optical, chemical-composition and mass aerosol properties by using the observations from several ground-based networks. From these regional time series the aerosol trends have been derived for the different regions of the world. Most of the properties related to aerosol loading exhibit negative trends, both at the surface and in the total atmospheric column. Significant decreases in aerosol optical depth (AOD) are found in Europe, North America, South America, North Africa and Asia, ranging from −1.2 % yr−1 to −3.1 % yr−1. An error and representativity analysis of the spatially and temporally limited observational data has been performed using model data subsets in order to investigate how much the observed trends represent the actual trends happening in the regions over the full study period from 2000 to 2014. This analysis reveals that significant uncertainty is associated with some of the regional trends due to time and space sampling deficiencies. The set of observed regional trends has then been used for the evaluation of 10 models (6 AeroCom phase III models and 4 CMIP6 models) and the CAMS reanalysis dataset and of their skills in reproducing the aerosol trends. Model performance is found to vary depending on the parameters and the regions of the world. The models tend to capture trends in AOD, the column Ångström exponent, sulfate and particulate matter well (except in North Africa), but they show larger discrepancies for coarse-mode AOD. The rather good agreement of the trends, across different aerosol parameters between models and observations, when co-locating them in time and space, implies that global model trends, including those in poorly monitored regions, are likely correct. The models can help to provide a global picture of the aerosol trends by filling the gaps in regions not covered by observations. The calculation of aerosol trends at a global scale reveals a different picture from that depicted by solely relying on ground-based observations. Using a model with complete diagnostics (NorESM2), we find a global increase in AOD of about 0.2 % yr−1 between 2000 and 2014, primarily caused by an increase in the loads of organic aerosols, sulfate and black carbon.

The Arctic is warming 2 to 3 times faster than the global average, partly due to changes in short-lived climate forcers (SLCFs) including aerosols. In order to study the effects of atmospheric aerosols in this warming, recent past (1990–2014) and future (2015–2050) simulations have been carried out using the GISS-E2.1 Earth system model to study the aerosol burdens and their radiative and climate impacts over the Arctic (>60°N), using anthropogenic emissions from the Eclipse V6b and the Coupled Model Intercomparison Project Phase 6 (CMIP6) databases, while global annual mean greenhouse gas concentrations were prescribed and kept fixed in all simulations. Results showed that the simulations have underestimated observed surface aerosol levels, in particular black carbon (BC) and sulfate (SO2−4), by more than 50 %, with the smallest biases calculated for the atmosphere-only simulations, where winds are nudged to reanalysis data. CMIP6 simulations performed slightly better in reproducing the observed surface aerosol concentrations and climate parameters, compared to the Eclipse simulations. In addition, simulations where atmosphere and ocean are fully coupled had slightly smaller biases in aerosol levels compared to atmosphere-only simulations without nudging. Arctic BC, organic aerosol (OA), and SO2−4 burdens decrease significantly in all simulations by 10 %–60 % following the reductions of 7 %–78 % in emission projections, with the Eclipse ensemble showing larger reductions in Arctic aerosol burdens compared to the CMIP6 ensemble. For the 2030–2050 period, the Eclipse ensemble simulated a radiative forcing due to aerosol–radiation interactions (RFARI) of −0.39 ± 0.01 W/sq. m, which is −0.08 W/sq. m larger than the 1990–2010 mean forcing (−0.32 W/sq. m), of which −0.24 ± 0.01 W/sq. m was attributed to the anthropogenic aerosols. The CMIP6 ensemble simulated a RFARI of −0.35 to −0.40 W/sq. m for the same period, which is −0.01 to −0.06 W/sq. m larger than the 1990–2010 mean forcing of −0.35 W/sq. m. The scenarios with little to no mitigation (worst-case scenarios) led to very small changes in the RFARI, while scenarios with medium to large emission mitigations led to increases in the negative RFARI, mainly due to the decrease in the positive BC forcing and the decrease in the negative SO2−4 forcing. The anthropogenic aerosols accounted for −0.24 to −0.26 W/sq. m of the net RFARI in 2030–2050 period, in Eclipse and CMIP6 ensembles, respectively. Finally, all simulations showed an increase in the Arctic surface air temperatures throughout the simulation period. By 2050, surface air temperatures are projected to increase by 2.4 to 2.6 °C in the Eclipse ensemble and 1.9 to 2.6 °C in the CMIP6 ensemble, compared to the 1990–2010 mean. Overall, results show that even the scenarios with largest emission reductions leads to similar impact on the future Arctic surface air temperatures and sea-ice extent compared to scenarios with smaller emission reductions, implying reductions of greenhouse emissions are still necessary to mitigate climate change.

Dimethylsulfide (DMS), outgassed from ocean waters, plays an important role in the climate system, as it oxidizes to methane sulfonic acid (MSA) and sulfur dioxide (SO2), which can lead to the formation of sulfate aerosol. Newly formed sulfate aerosol resulting from DMS oxidation may grow by condensation of gases, in-cloud oxidation, and coagulation to sizes where they may act as cloud condensation nuclei (CCN) and influence cloud properties. Under future global warming conditions, sea ice in the Arctic region is expected to decline significantly, which may lead to increased emissions of DMS from the open ocean and changes in cloud regimes. In this study we evaluate impacts of DMS on Arctic sulfate aerosol budget, changes in cloud droplet number concentration (CDNC), and cloud radiative forcing in the Arctic region under current and future sea ice conditions using an atmospheric global climate model. Given that future DMS concentrations are highly uncertain, several simulations with different surface seawater DMS concentrations and spatial distributions in the Arctic were performed in order to determine the sensitivity of sulfate aerosol budgets, CDNC, and cloud radiative forcing to Arctic surface seawater DMS concentrations. For any given amount and distribution of Arctic surface seawater DMS, similar amounts of sulfate are produced by oxidation of DMS in 2000 and 2050 despite large increases in DMS emission in the latter period due to sea ice retreat in the simulations. This relatively low sensitivity of sulfate burden is related to enhanced sulfate wet removal by precipitation in 2050. However simulated aerosol nucleation rates are higher in 2050, which results in an overall increase in CDNC and substantially more negative cloud radiative forcing. Thus potential future reductions in sea ice extent may cause cloud albedos to increase, resulting in a negative climate feedback on radiative forcing in the Arctic associated with ocean DMS emissions.

he vertical profile of aerosol is important for its radiative effects, but weakly constrained by observations on the global scale, and highly variable among different models. To investigate the controlling factors in one particular model, we investigate the effects of individual processes in HadGEM3–UKCA and compare the resulting diversity of aerosol vertical profiles with the inter-model diversity from the AeroCom Phase II control experiment. In this way we show that (in this model at least) the vertical profile is controlled by a relatively small number of processes, although these vary among aerosol components and particle sizes. We also show that sufficiently coarse variations in these processes can produce a similar diversity to that among different models in terms of the global-mean profile and, to a lesser extent, the zonal-mean vertical position. However, there are features of certain models' profiles that cannot be reproduced, suggesting the influence of further structural differences between models. In HadGEM3–UKCA, convective transport is found to be very important in controlling the vertical profile of all aerosol components by mass. In-cloud scavenging is very important for all except mineral dust. Growth by condensation is important for sulfate and carbonaceous aerosol (along with aqueous oxidation for the former and ageing by soluble material for the latter). The vertical extent of biomass-burning emissions into the free troposphere is also important for the profile of carbonaceous aerosol. Boundary-layer mixing plays a dominant role for sea salt and mineral dust, which are emitted only from the surface. Dry deposition and below-cloud scavenging are important for the profile of mineral dust only. In this model, the microphysical processes of nucleation, condensation and coagulation dominate the vertical profile of the smallest particles by number (e.g. total CN  >  3 nm), while the profiles of larger particles (e.g. CN  >  100 nm) are controlled by the same processes as the component mass profiles, plus the size distribution of primary emissions. We also show that the processes that affect the AOD-normalised radiative forcing in the model are predominantly those that affect the vertical mass distribution, in particular convective transport, in-cloud scavenging, aqueous oxidation, ageing and the vertical extent of biomass-burning emissions.

A tighter integration of modeling frameworks for climate and air quality is urgently needed to assess the impacts of clean air policies on future Arctic and global climate. We combined a new model emulator and comprehensive emissions scenarios for air pollutants and greenhouse gases to assess climate and human health co-benefits of emissions reductions. Fossil fuel use is projected to rapidly decline in an increasingly sustainable world, resulting in far-reaching air quality benefits. Despite human health benefits, reductions in sulfur emissions in a more sustainable world could enhance Arctic warming by 0.8 °C in 2050 relative to the 1995–2014, thereby offsetting climate benefits of greenhouse gas reductions. Targeted and technically feasible emissions reduction opportunities exist for achieving simultaneous climate and human health co-benefits. It would be particularly beneficial to unlock a newly identified mitigation potential for carbon particulate matter, yielding Arctic climate benefits equivalent to those from carbon dioxide reductions by 2050.

The Canadian Earth System Model version 5 (CanESM5) is a global model developed to simulate historical climate change and variability, to make centennial-scale projections of future climate, and to produce initialized seasonal and decadal predictions. This paper describes the model components and their coupling, as well as various aspects of model development, including tuning, optimization, and a reproducibility strategy. We also document the stability of the model using a long control simulation, quantify the model's ability to reproduce large-scale features of the historical climate, and evaluate the response of the model to external forcing. CanESM5 is comprised of three-dimensional atmosphere (T63 spectral resolution equivalent roughly to 2.8∘) and ocean (nominally 1∘) general circulation models, a sea-ice model, a land surface scheme, and explicit land and ocean carbon cycle models. The model features relatively coarse resolution and high throughput, which facilitates the production of large ensembles. CanESM5 has a notably higher equilibrium climate sensitivity (5.6 K) than its predecessor, CanESM2 (3.7 K), which we briefly discuss, along with simulated changes over the historical period. CanESM5 simulations contribute to the Coupled Model Intercomparison Project phase 6 (CMIP6) and will be employed for climate science and service applications in Canada.

Upper-tropospheric ice cloud measurements from the Superconducting Submillimeter Limb Emission Sounder (SMILES) on the International Space Station (ISS) are used to study the diurnal cycle of upper-tropospheric ice cloud in the tropics and midlatitudes (40°S–40°N) and to quantitatively evaluate ice cloud diurnal variability simulated by 10 climate models. Over land, the SMILES-observed diurnal cycle has a maximum around 1800 local solar time (LST), while the model-simulated diurnal cycles have phases differing from the observed cycle by −4 to 12 h. Over ocean, the observations show much smaller diurnal cycle amplitudes than over land with a peak at 1200 LST, while the modeled diurnal cycle phases are widely distributed throughout the 24-h period. Most models show smaller diurnal cycle amplitudes over ocean than over land, which is in agreement with the observations. However, there is a large spread of modeled diurnal cycle amplitudes ranging from 20% to more than 300% of the observed over both land and ocean. Empirical orthogonal function (EOF) analysis on the observed and model-simulated variations of ice clouds finds that the first EOF modes over land from both observation and model simulations explain more than 70% of the ice cloud diurnal variations and they have similar spatial and temporal patterns. Over ocean, the first EOF from observation explains 26.4% of the variance, while the first EOF from most models explains more than 70%. The modeled spatial and temporal patterns of the leading EOFs over ocean show large differences from observations, indicating that the physical mechanisms governing the diurnal cycle of oceanic ice clouds are more complicated and not well simulated by the current climate models.

Three aspects of longwave (LW) radiation processes are investigated using numerical experiments with the Canadian Atmospheric Global Climate Model version 4.3 (CanAM4.3). These are the overlapping LW and shortwave (SW) radiation, scattering by clouds, and specification of ocean emissivity. For the overlapping of solar and infrared spectra, using a single band scheme was compared against a method directly inputting solar energy. Offline calculations show that for high clouds using the single band can cause an overestimate of the downward LW flux, whereas a method that accounts for input solar energy in the LW yields results that are more accurate. Longwave scattering by clouds traps more infrared energy in the atmosphere and reduces the outgoing radiation to space. Simulations with CanAM4.3 show that cloud LW scattering can enhance the LW cooling rate above the tropopause and reduce it inside the troposphere, resulting in warmer temperatures, especially in the tropics and low latitudes. This implies a larger temperature gradient toward the polar region, which causes a strengthening of the Hadley circulation and shifting of the intertropical convergence zone (ITCZ). The increase in lower tropospheric temperature also affects the lower troposphere water vapor and precipitation. Sensitivity to the specification of ocean emissivity is examined by comparing a broadband scheme dependent on the surface wind and solar zenith angle against one that resolves the wavelength dependence. Experiments with CanAM4.3 show that the two oceanic emissivity schemes can produce over 1 W m−2 seasonal mean difference of the upward flux at the surface.

The radiative forcing of black carbon (BC) is subject to many complex, interconnected sources of uncertainty. Here we isolate the role of the refractive index, which determines the extent to which BC absorbs and scatters radiation. We compare four refractive index schemes: three that are commonly used in Earth system models and a fourth more recent estimate with higher absorption. With other parameterizations held constant, changing BC's spectrally varying refractive index from the least- to most-absorbing estimate commonly used in Earth system models (m550 nm=1.75–0.44i to m550 nm=1.95–0.79i) increases simulated absorbing aerosol optical depth (AAOD) by 42 % and the effective radiative forcing from BC–radiation interactions (BC ERFari) by 47 %. The more recent estimate, m532 nm=1.48–0.84i, increases AAOD and BC ERFari by 59 % and 100 % respectively relative to the low-absorption case. The AAOD increases are comparable to those from recent updates to aerosol emission inventories and, in BC source regions, up to two-thirds as large as the difference in AAOD retrieved from MISR (Multi-angle Imaging SpectroRadiometer) and POLDER-GRASP (Polarization and Directionality of the Earth's Reflectances instrument with the Generalized Retrieval of Atmosphere and Surface Properties algorithm) satellites. The BC ERFari increases are comparable to previous assessments of overall uncertainties in BC ERFari, even though this source of uncertainty is typically overlooked. Although model sensitivity to the choice of BC refractive index is known to be modulated by other parameterization choices, our results highlight the importance of considering refractive index diversity in model intercomparison projects.