Black carbon ageing in the Canadian Centre for Climate modelling and analysis atmospheric general circulation model

International audienceBlack carbon (BC) particles in the atmosphere have important impacts on climate. The amount of BC in the atmosphere must be carefully quantified to allow evaluation of the climate effects of this type of aerosol. In this study, we present the treatment of BC aerosol in the developmental version of the 4th generation Canadian Centre for Climate modelling and analysis (CCCma) atmospheric general circulation model (AGCM). The focus of this work is on the conversion of insoluble BC to soluble/mixed BC by physical and chemical ageing. Physical processes include the condensation of sulphuric and nitric acid onto the BC aerosol, and coagulation with more soluble aerosols such as sulphates and nitrates. Chemical processes that may age the BC aerosol include the oxidation of organic coatings by ozone. Four separate parameterizations of the ageing process are compared to a control simulation that assumes no ageing occurs. These simulations use 1) an exponential decay with a fixed 24h half-life, 2) a condensation and coagulation scheme, 3) an oxidative scheme, and 4) a linear combination of the latter two ageing treatments. Global BC burdens are 2.15, 0.15, 0.11, 0.21, and 0.11TgC for the control run, and four ageing schemes, respectively. The BC lifetimes are 98.1, 6.6, 5.0, 9.5, and 4.9 days, respectively. The sensitivity of modelled BC burdens, and concentrations to the factor of two uncertainty in the emissions inventory is shown to be greater than the sensitivity to the parameterization used to represent the BC ageing, except for the oxidation based parameterization. A computationally efficient parameterization that represents the processes of condensation, coagulation, and oxidation is shown to simulate BC ageing well in the CCCma AGCM. As opposed to the globally fixed ageing time scale, this treatment of BC ageing is responsive to varying atmospheric composition

Simulation of mineral dust aerosol with Piecewise Log-normal Approximation (PLA) in CanAM4-PAM

A new size-resolved dust scheme based on the numerical method of piecewise log-normal approximation (PLA) was developed and implemented in the fourth generation of the Canadian Atmospheric Global Climate Model with the PLA Aerosol Model (CanAM4-PAM). The total simulated annual global dust emission is 2500 Tg yr<sup>−1</sup>, and the dust mass load is 19.3 Tg for year 2000. Both are consistent with estimates from other models. Results from simulations are compared with multiple surface measurements near and away from dust source regions, validating the generation, transport and deposition of dust in the model. Most discrepancies between model results and surface measurements are due to unresolved aerosol processes. Biases in long-range transport are also contributing. Radiative properties of dust aerosol are derived from approximated parameters in two size modes using Mie theory. The simulated aerosol optical depth (AOD) is compared with satellite and surface remote sensing measurements and shows general agreement in terms of the dust distribution around sources. The model yields a dust AOD of 0.042 and dust aerosol direct radiative forcing (ADRF) of −1.24 W m<sup>−2</sup> respectively, which show good consistency with model estimates from other studies

Parameterization of sea-salt optical properties and physics of the associated radiative forcing

The optical properties of sea-salt aerosol have been parameterized at shortwave and longwave wavelengths. The optical properties were parameterized in a simple functional form in terms of the ambient relative humidity based on Mie optical property calculations. The proposed parameterization is tested relative to Mie calculations and is found to be accurate to within a few percent. In the parameterization, the effects of the size distribution on the optical properties are accounted for in terms of effective radius of the sea-salt size distribution. This parameterization differs from previous works by being formulated directly with the wet sea-salt size distribution and, to our knowledge, this is the first published sea-salt parameterization to provide a parameterization for both shortwave and longwave wavelengths. <br><br> We have used this parameterization in a set of idealized 1-D radiative transfer calculations to investigate the sensitivity of various attributes of sea-salt forcing, including the dependency on sea-salt column loading, effective variance, solar angle, and surface albedo. From these sensitivity tests, it is found that sea-salt forcings for both shortwave and longwave spectra are linearly related to the sea-salt loading for realistic values of loadings. The radiative forcing results illustrate that the shortwave forcing is an order of magnitude greater than the longwave forcing results and opposite in sign, for various loadings. Forcing sensitivity studies show that the influence of effective variance for sea-salt is minor; therefore, only one value of effective variance is used in the parameterization. The dependence of sea-salt forcing with solar zenith angle illustrates an interesting result that sea-salt can generate a positive top-of-the-atmosphere result (i.e. warming) when the solar zenith angle is relatively small (i.e. <30°). Finally, it is found that the surface albedo significantly affects the shortwave radiative forcing, with the forcing diminishing to zero as the surface albedo tends to unity

Sensitivity of Arctic sulfate aerosol and clouds to changes in future surface seawater dimethylsulfide concentrations

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.</p

Convective response to large-scale forcing in the tropical western Pacific simulated by spCAM5 and CanAM4.3

Changes in the large-scale environment during convective precipitation events in the tropical western Pacific simulated by version 4.3 of the Canadian Atmospheric Model (CanAM4.3) are compared against those simulated by version 5.0 of the super-parameterized Community Atmosphere Model (spCAM5). This is done by compositing sub-hourly output of convective rainfall, convective available potential energy (CAPE), CAPE generation due to large-scale forcing in the free troposphere (dCAPELSFT) and near-surface vertical velocity (ω) over the time period May–July 1997. Compared to spCAM5, CanAM4.3 tends to produce more frequent light convective precipitation (&lt;0.2&thinsp;mm&thinsp;h−1) and underestimates the frequency of extreme convective precipitation (&gt;2&thinsp;mm&thinsp;h−1). In spCAM5, 5&thinsp;% of convective precipitation events lasted less than 1.5&thinsp;h and 75&thinsp;% lasted between 1.5 and 3.0&thinsp;h, while in CanAM4.3 80&thinsp;% of the events lasted less than 1.5&thinsp;h. Convective precipitation in spCAM5 is found to be a function of dCAPELSFT and the large-scale near-surface ω with variations in ω slightly leading variations in convective precipitation. Convective precipitation in CanAM4.3 does not have the same dependency and instead is found to be a function of CAPE.</p

Arctic air pollution: Challenges and opportunities for the next decade

The Arctic is a sentinel of global change. This region is influenced by multiple physical and socio-economic drivers and feedbacks, impacting both the natural and human environment. Air pollution is one such driver that impacts Arctic climate change, ecosystems and health but significant uncertainties still surround quantification of these effects. Arctic air pollution includes harmful trace gases (e.g. tropospheric ozone) and particles (e.g. black carbon, sulphate) and toxic substances (e.g. polycyclic aromatic hydrocarbons) that can be transported to the Arctic from emission sources located far outside the region, or emitted within the Arctic from activities including shipping, power production, and other industrial activities. This paper qualitatively summarizes the complex science issues motivating the creation of a new international initiative, PACES (air Pollution in the Arctic: Climate, Environment and Societies). Approaches for coordinated, international and interdisciplinary research on this topic are described with the goal to improve predictive capability via new understanding about sources, processes, feedbacks and impacts of Arctic air pollution. Overarching research actions are outlined, in which we describe our recommendations for 1) the development of trans-disciplinary approaches combining social and economic research with investigation of the chemical and physical aspects of Arctic air pollution; 2) increasing the quality and quantity of observations in the Arctic using long-term monitoring and intensive field studies, both at the surface and throughout the troposphere; and 3) developing improved predictive capability across a range of spatial and temporal scales

Vertical profiles of light absorption and scattering associated with black carbon particle fractions in the springtime Arctic above 79◦ N

Despite the potential importance of black carbon (BC) for radiative forcing of the Arctic atmosphere, ver- tically resolved measurements of the particle light scatter- ing coefficient (σsp ) and light absorption coefficient (σap ) in the springtime Arctic atmosphere are infrequent, espe- cially measurements at latitudes at or above 80◦ N. Here, re- lationships among vertically distributed aerosol optical prop- erties (σap, σsp and single scattering albedo or SSA), par- ticle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9 and 83.4◦ N from near the surface to 500 hPa. Airborne data collected during April 2015 are combined with ground- based observations from the observatory at Alert, Nunavut and simulations from the Goddard Earth Observing Sys- tem (GEOS) model, GEOS-Chem, coupled with the TwO- Moment Aerosol Sectional (TOMAS) model (collectively GEOS-Chem–TOMAS; Kodros et al., 2018) to further our knowledge of the effects of BC on light absorption in the Arctic troposphere. The results are constrained for σsp less than 15 Mm−1, which represent 98 % of the observed σsp, be- cause the single scattering albedo (SSA) has a tendency to be lower at lower σsp, resulting in a larger relative contribution to Arctic warming. At 18.4 m2 g−1, the average BC mass ab- sorption coefficient (MAC) from the combined airborne and Alert observations is substantially higher than the two aver- aged modelled MAC values (13.6 and 9.1 m2 g−1) for two different internal mixing assumptions, the latter of which is based on previous observations. The higher observed MAC value may be explained by an underestimation of BC, the presence of small amounts of dust and/or possible differences in BC microphysics and morphologies between the obser- vations and model. In comparing the observations and simulations, we present σap and SSA, as measured, and σap/2 and the corresponding SSA to encompass the lower modelled MAC that is more consistent with accepted MAC values. Me- dian values of the measured σap, rBC and the organic com- ponent of particles all increase by a factor of 1.8 ± 0.1, going from near-surface to 750 hPa, and values higher than the sur- face persist to 600 hPa. Modelled BC, organics and σap agree with the near-surface measurements but do not reproduce the higher values observed between 900 and 600 hPa. The dif- ferences between modelled and observed optical properties follow the same trend as the differences between the mod- elled and observed concentrations of the carbonaceous com- ponents (black and organic). Model-observation discrepan- cies may be mostly due to the modelled ejection of biomass burning particles only into the boundary layer at the sources. For the assumption of the observed MAC value, the SSA range between 0.88 and 0.94, which is significantly lower than other recent estimates for the Arctic, in part reflecting the constraint of σsp < 15 Mm−1. The large uncertainties in measuring optical properties and BC, and the large differ- ences between measured and modelled values here and in the literature, argue for improved measurements of BC and light absorption by BC and more vertical profiles of aerosol chemistry, microphysics and other optical properties in the Arctic

Current model capabilities for simulating black carbon and sulfate concentrations in the Arctic atmosphere: a multi-model evaluation using a comprehensive measurement data set

The concentrations of sulfate, black carbon (BC) and other aerosols in the Arctic are characterized by high values in late winter and spring (so-called Arctic Haze) and low values in summer. Models have long been struggling to capture this seasonality and especially the high concentrations associated with Arctic Haze. In this study, we evaluate sulfate and BC concentrations from eleven different models driven with the same emission inventory against a comprehensive pan-Arctic measurement data set over a time period of 2 years (2008–2009). The set of models consisted of one Lagrangian particle dispersion model, four chemistry transport models (CTMs), one atmospheric chemistry-weather forecast model and five chemistry climate models (CCMs), of which two were nudged to meteorological analyses and three were running freely. The measurement data set consisted of surface measurements of equivalent BC (eBC) from five stations (Alert, Barrow, Pallas, Tiksi and Zeppelin), elemental carbon (EC) from Station Nord and Alert and aircraft measurements of refractory BC (rBC) from six different campaigns. We find that the models generally captured the measured eBC or rBC and sulfate concentrations quite well, compared to previous comparisons. However, the aerosol seasonality at the surface is still too weak in most models. Concentrations of eBC and sulfate averaged over three surface sites are underestimated in winter/spring in all but one model (model means for January–March underestimated by 59 and 37 % for BC and sulfate, respectively), whereas concentrations in summer are overestimated in the model mean (by 88 and 44 % for July–September), but with overestimates as well as underestimates present in individual models. The most pronounced eBC underestimates, not included in the above multi-site average, are found for the station Tiksi in Siberia where the measured annual mean eBC concentration is 3 times higher than the average annual mean for all other stations. This suggests an underestimate of BC sources in Russia in the emission inventory used. Based on the campaign data, biomass burning was identified as another cause of the modeling problems. For sulfate, very large differences were found in the model ensemble, with an apparent anti-correlation between modeled surface concentrations and total atmospheric columns. There is a strong correlation between observed sulfate and eBC concentrations with consistent sulfate/eBC slopes found for all Arctic stations, indicating that the sources contributing to sulfate and BC are similar throughout the Arctic and that the aerosols are internally mixed and undergo similar removal. However, only three models reproduced this finding, whereas sulfate and BC are weakly correlated in the other models. Overall, no class of models (e.g., CTMs, CCMs) performed better than the others and differences are independent of model resolution

Intercomparison and evaluation of global aerosol microphysical properties among AeroCom models of a range of complexity

Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multi-model-mean data set simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the individual global aerosol microphysics models are performing well, although the large model diversity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation and growth (e.g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions