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Anthropogenic aerosols impact cirrus clouds through ice nucleation, thereby changing the Earth's radiation budget. However, the magnitude and sign of anthropogenic forcing in cirrus clouds is still very uncertain depending on the treatments for ice-nucleating particles (INPs), the treatments for haze particle freezing, and the ice nucleation scheme. In this study, a new ice nucleation scheme (hereafter the HYBRID scheme) is developed to combine the best features of two previous ice nucleation schemes, so that global models are able to calculate the ice number concentration in both updrafts and downdrafts associated with gravity waves, and it has a robust sensitivity to the change of aerosol number. The scheme is applied in a box model, and the ice number concentrations (9.52±2.08 L−1) are somewhat overestimated but are in reasonable agreement with those from an adiabatic parcel model (9.40±2.31 L−1). Then, the forcing and cloud changes associated with changes in aircraft soot, sulfur emission, and all anthropogenic emissions between the preindustrial (PI) period and the present day (PD) are examined using the CESM/IMPACT global model with the HYBRID scheme. Aircraft soot emissions decrease the global average ice number concentration (Ni) by -1.0±2.4×107 m−2 (−1 %) (over the entire column) due to the inhibition of homogeneous nucleation and lead to a radiative forcing of -0.14±0.07 W m−2, while the increase in sulfur emissions increases the global average Ni by 7.3±2.9×107 m−2 (5 %) due to the increase in homogeneous nucleation and leads to a radiative forcing of -0.02±0.06 W m−2. The possible effects of aerosol and cloud feedbacks to the meteorological state in remote regions partly contribute to reduce the forcing and the change in Ni due to anthropogenic emissions. The radiative forcing due to all increased anthropogenic emissions from PI to PD is estimated to be -0.20±0.05 W m−2. If newly formed secondary organic aerosols (SOAs) act as INPs and inhibit homogeneous nucleation, the Ni formed from heterogeneous nucleation is increased. As a result, the inclusion of INPs from SOA increases the change in Ni to 12.0±2.3×107 m−2 (9 %) and increases (makes less negative) the anthropogenic forcing on cirrus clouds to -0.04±0.08 W m−2 from PI to PD.

Global aviation operations contribute to anthropogenic climate change via a complex set of processes that lead to a net surface warming. Of importance are aviation emissions of carbon dioxide (CO2), nitrogen oxides (NOx), water vapor, soot and sulfate aerosols, and increased cloudiness due to contrail formation. Aviation grew strongly over the past decades (1960–2018) in terms of activity, with revenue passenger kilometers increasing from 109 to 8269 billion km yr−1, and in terms of climate change impacts, with CO2 emissions increasing by a factor of 6.8–1034 Tg CO2 yr−1. Over the period 2013–2018, the growth rates in both terms show a marked increase. Here, we present a new comprehensive and quantitative approach for evaluating aviation climate forcing terms. Both radiative forcing (RF) and effective radiative forcing (ERF) terms and their sums are calculated for the years 2000–2018. Contrail cirrus, consisting of linear contrails and the cirrus cloudiness arising from them, yields the largest positive net (warming) ERF term followed by CO2 and NOx emissions. The formation and emission of sulfate aerosol yields a negative (cooling) term. The mean contrail cirrus ERF/RF ratio of 0.42 indicates that contrail cirrus is less effective in surface warming than other terms. For 2018 the net aviation ERF is +100.9 mW (mW) m−2 (5–95% likelihood range of (55, 145)) with major contributions from contrail cirrus (57.4 mW m−2), CO2 (34.3 mW m−2), and NOx (17.5 mW m−2). Non-CO2 terms sum to yield a net positive (warming) ERF that accounts for more than half (66%) of the aviation net ERF in 2018. Using normalization to aviation fuel use, the contribution of global aviation in 2011 was calculated to be 3.5 (4.0, 3.4) % of the net anthropogenic ERF of 2290 (1130, 3330) mW m−2. Uncertainty distributions (5%, 95%) show that non-CO2 forcing terms contribute about 8 times more than CO2 to the uncertainty in the aviation net ERF in 2018. The best estimates of the ERFs from aviation aerosol-cloud interactions for soot and sulfate remain undetermined. CO2-warming-equivalent emissions based on global warming potentials (GWP* method) indicate that aviation emissions are currently warming the climate at approximately three times the rate of that associated with aviation CO2 emissions alone. CO2 and NOx aviation emissions and cloud effects remain a continued focus of anthropogenic climate change research and policy discussions., Graphical abstract Image 1, Highlights • Global aviation warms Earth's surface through both CO2 and net non-CO2 contributions. • Global aviation contributes a few percent to anthropogenic radiative forcing. • Non-CO2 impacts comprise about 2/3 of the net radiative forcing. • Comprehensive and quantitative calculations of aviation effects are presented. • Data are made available to analyze past, present and future aviation climate forcing.

Secondary organic aerosol (SOA) is the largest component of global organic aerosol and plays a key role in determining the Earth’s radiation budget. A global chemistry model is developed to make SOA internally mixed with other aerosols based on the mechanism of formation, and includes a comprehensive organic nucleation scheme. Using an internal mixing state reduces the aerosol number, resulting in a large decrease in the cloud albedo effect of SOA. Organic nucleation is responsible for the decrease of 16% in the total radiative forcing associated with anthropogenic aerosols due to the change in the size distribution and number concentration of SOA. The radiative effect of SOA on cirrus clouds is estimated to be 0.31–0.35 W m− 2 using assumed and predicted size distributions. The formation mechanism of SOA is still needed to be improved according to the developing of experiments and measurements to reduce the uncertainty in the estimation of radiative effect of aerosols.

In this study we evaluate cloud properties simulated by the Community Atmosphere Model version 5 (CAM5) using in situ measurements from the HIAPER Pole-to-Pole Observations (HIPPO) campaign for the period of 2009 to 2011. The modeled wind and temperature are nudged towards reanalysis. Model results collocated with HIPPO flight tracks are directly compared with the observations, and model sensitivities to the representations of ice nucleation and growth are also examined. Generally, CAM5 is able to capture specific cloud systems in terms of vertical configuration and horizontal extension. In total, the model reproduces 79.8 % of observed cloud occurrences inside model grid boxes and even higher (94.3 %) for ice clouds (T ≤ −40 °C). The missing cloud occurrences in the model are primarily ascribed to the fact that the model cannot account for the high spatial variability of observed relative humidity (RH). Furthermore, model RH biases are mostly attributed to the discrepancies in water vapor, rather than temperature. At the micro-scale of ice clouds, the model captures the observed increase of ice crystal mean sizes with temperature, albeit with smaller sizes than the observations. The model underestimates the observed ice number concentration (Ni) and ice water content (IWC) for ice crystals larger than 75 µm in diameter. Modeled IWC and Ni are more sensitive to the threshold diameter for autoconversion of cloud ice to snow (Dcs), while simulated ice crystal mean size is more sensitive to ice nucleation parameterizations than to Dcs. Our results highlight the need for further improvements to the sub-grid RH variability and ice nucleation and growth in the model.

Observation-based studies have shown that the aerosol cloud lifetime effect or the increase of cloud liquid water path (LWP) with increased aerosol loading may have been overestimated in climate models. Here, we simulate shallow warm clouds on 27 May 2011 at the southern Great Plains (SGP) measurement site established by the Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) program using a single-column version of a global climate model (Community Atmosphere Model or CAM) and a cloud resolving model (CRM). The LWP simulated by CAM increases substantially with aerosol loading while that in the CRM does not. The increase of LWP in CAM is caused by a large decrease of the autoconversion rate when cloud droplet number increases. In the CRM, the autoconversion rate is also reduced, but this is offset or even outweighed by the increased evaporation of cloud droplets near the cloud top, resulting in an overall decrease in LWP. Our results suggest that climate models need to include the dependence of cloud top growth and the evaporation/condensation process on cloud droplet number concentrations.

Secondary organic aerosol (SOA) plays a significant role in the Earth system by altering its radiative balance. Here we use an Earth system model coupled with an explicit SOA formation module to estimate the response of SOA concentrations to changes in climate, anthropogenic emissions, and human land use in the future. We find that climate change is the major driver for SOA change under the representative concentration pathways for the 8.5 future scenario. Climate change increases isoprene emission rate by 18% with the effect of temperature increases outweighing that of the CO2 inhibition effect. Annual mean global SOA mass is increased by 25% as a result of climate change. However, anthropogenic emissions and land use change decrease SOA. The net effect is that future global SOA burden in 2100 is nearly the same as that of the present day. The SOA concentrations over the Northern Hemisphere are predicted to decline in the future due to the control of sulfur emissions.

Organic nucleation is an important source of atmospheric aerosol number concentration, especially in pristine continental regions and during the preindustrial period. Here, we improve on previous simulations that overestimate boundary layer nucleation in the tropics and add changes to climate and land use to evaluate climate forcing. Our model includes both pure organic nucleation and heteromolecular nucleation of sulfuric acid and organics and reproduces the profile of aerosol number concentration measured in the Amazon. Organic nucleation decreases the sum of the total aerosol direct and indirect radiative forcing by 12.5%. The addition of climate and land use change decreases the direct radiative forcing (−0.38 W m−2) by 6.3% and the indirect radiative forcing (−1.68 W m−2) by 3.5% due to the size distribution and number concentration change of secondary organic aerosol and sulfate. Overall, the total radiative forcing associated with anthropogenic aerosols is decreased by 16%., Organic nucleation is an important source of atmospheric aerosol number concentration, especially in pristine continental regions and during the preindustrial period. Here the authors find a 16% reduced radiative forcing associated with anthropogenic aerosols when including organic nucleation together with climate and land use change.

Marine stratocumulus clouds cover nearly one-quarter of the ocean surface and thus play an extremely important role in determining the global radiative balance. The semipermanent marine stratocumulus deck over the southeastern Atlantic Ocean is of particular interest, because of its interactions with seasonal biomass burning aerosols that are emitted in southern Africa. Understanding the impacts of biomass burning aerosols on stratocumulus clouds and the implications for regional and global radiative balance is still very limited. Previous studies have focused on assessing the magnitude of the warming caused by solar scattering and absorption by biomass burning aerosols over stratocumulus (the direct radiative effect) or cloud adjustments to the direct radiative effect (the semidirect effect). Here, using a nested modeling approach in conjunction with observations from multiple satellites, we demonstrate that cloud condensation nuclei activated from biomass burning aerosols entrained into the stratocumulus (the microphysical effect) can play a dominant role in determining the total radiative forcing at the top of the atmosphere, compared with their direct and semidirect radiative effects. Biomass burning aerosols over the region and period with heavy loadings can cause a substantial cooling (daily mean -8.05 W m-2), primarily as a result of clouds brightening by reducing the cloud droplet size (the Twomey effect) and secondarily through modulating the diurnal cycle of cloud liquid water path and coverage (the cloud lifetime effect). Our results highlight the importance of realistically representing the interactions of stratocumulus with biomass burning aerosols in global climate models in this region.

How much have aerosol particles slowed warming? Joyce Penner sets out priorities for a coordinated campaign of observations and modelling. How much have aerosol particles slowed warming? Joyce Penner sets out priorities for a coordinated campaign of observations and modelling.

Cirrus cloud seeding has been proposed as a possible technique that might thin cirrus clouds leading to reduced heating. The technique was shown to be viable in one model evaluation. Here we use an updated version of the Community Atmosphere Model version 5 (CAM5) and reevaluate whether seeding is a viable mechanism for cooling. We explore different model setups (with and without secondary organic aerosols acting as heterogeneous ice nuclei). None of the updated versions of the CAM5 lead to a significant amount of negative climate forcing and hence do not lead to cooling. We only calculate a net negative cloud forcing (−0.74 ± 0.25 W m−2) if we restrict the modeled subgrid-scale updraft velocity during nucleation to

Iron (Fe) oxides in aerosols are known to absorb sun light and heat the atmosphere. However, the radiative forcing (RF) of light-absorbing aerosols of pyrogenetic Fe oxides is ignored in climate models. For the first time, we use a global chemical transport model and a radiative transfer model to estimate the RF by light-absorbing aerosols of pyrogenetic Fe oxides. The model results suggest that strongly absorbing Fe oxides (magnetite) contribute a RF that is about 10% of the RF due to black carbon (BC) over East Asia. The seasonal average of the RF due to dark Fe-rich mineral particles over East Asia (0.4–1.0 W m−2) is comparable to that over major biomass burning regions. This additional warming effect is amplified over polluted regions where the iron and steel industries have been recently developed. These findings may have important implications for the projection of the climate change, due to the rapid growth in energy consumption of the heavy industry in newly developing countries.

The indirect effect of aircraft soot on cirrus clouds is subject to large uncertainties due to uncertainty in the effectiveness of aircraft soot acting as heterogeneous ice nuclei (IN) and the complexity caused by background ice nucleation, which introduces two major competing ice nucleation mechanisms: homogeneous freezing that generally produces more abundant ice particles and heterogeneous nucleation that generally produces fewer ice particles. In this paper, we used the coupled Community Atmosphere Model version 5.2 (CAM5)/IMPACT model to estimate the climate impacts of aircraft soot acting as IN in large-scale cirrus clouds. We assume that only the aircraft soot particles that are preactivated in persistent contrail cirrus clouds are efficient IN. Further, we assume that these particles lose their ability to act as efficient IN when they become coated with three monolayers of sulfate. We varied the background number concentration of sulfate aerosols allowed to act as homogeneous ice nucleation sites as well as the dust concentrations that act as heterogeneous ice nuclei to examine the sensitivity of the forcing by aircraft soot to the background atmosphere. The global average effect can range from a high negative (cooling) rate, −0.35 W m−2, for the high sulfate/low dust case to a positive (warming) rate, +0.09 W m−2, for the low sulfate/low dust case (default CAM5 setup) when approximately 0.6% of total aviation soot acts as IN. The net negative forcing is caused by the addition of IN to a background atmosphere that is dominated by homogeneous nucleation (mainly in the tropic Indian Ocean, Central America, and North Atlantic Ocean). The forcings can be all positive, about +0.11 to +0.21 W m−2, when the background atmosphere is dominated by pure heterogeneous ice nucleation.

Injection of powdered activated carbon (PAC) adsorbents into the flue gas of coal fired power plants with electrostatic precipitators (ESPs) is the most mature technology to control mercury emissions for coal combustion. However, the PAC itself can penetrate ESPs to emit into the atmosphere. These emitted PACs have similar size and optical properties to submicron black carbon (BC) and thus could increase BC radiative forcing unintentionally. The present paper estimates, for the first time, the potential emission of PAC together with their climate forcing. The global average maximum potential emissions of PAC is 98.4 Gg/yr for the year 2030, arising from the assumed adoption of the maximum potential PAC injection technology, the minimum collection efficiency, and the maximum PAC injection rate. These emissions cause a global warming of 2.10 mW m(-2) at the top of atmosphere and a cooling of -2.96 mW m(-2) at the surface. This warming represents about 2% of the warming that is caused by BC from direct fossil fuel burning and 0.86% of the warming associated with CO2 emissions from coal burning in power plants. Its warming is 8 times more efficient than the emitted CO2 as measured by the 20-year-integrated radiative forcing per unit of carbon input (the 20-year Global Warming Potential).

Organic aerosols (OA) play an important role in climate change. However, very few calculations of global OA radiative forcing include secondary organic aerosol (SOA) or the light-absorbing part of OA (brown carbon). Here we use a global model to assess the radiative forcing associated with the change in primary organic aerosol (POA) and SOA between present-day and preindustrial conditions in both the atmosphere and the land snow/sea ice. Anthropogenic emissions are shown to substantially influence the SOA formation rate, causing it to increase by 29 Tg/yr (93%) since preindustrial times. We examine the effects of varying the refractive indices, size distributions for POA and SOA, and brown carbon fraction in SOA. The increase of SOA exerts a direct forcing ranging from −0.12 to −0.31 W m−2 and a first indirect forcing in warm-phase clouds ranging from −0.22 to −0.29 W m−2, with the range due to different assumed SOA size distributions and refractive indices. The increase of POA since preindustrial times causes a direct forcing varying from −0.06 to −0.11 W m−2, when strongly and weakly absorbing refractive indices for brown carbon are used. The change in the total OA exerts a direct forcing ranging from −0.14 to −0.40 W m−2. The atmospheric absorption from brown carbon ranges from +0.22 to +0.57 W m−2, which corresponds to 27%~70% of the black carbon (BC) absorption predicted in the model. The radiative forcing of OA deposited in land snow and sea ice ranges from +0.0011 to +0.0031 W m−2 or as large as 24% of the forcing caused by BC in snow and ice simulated by the model.

Atmospheric deposition of reactive nitrogen (N) species from air pollutants is a significant source of exogenous nitrogen in marine ecosystems. Here we use an atmospheric chemical transport model to investigate the supply of soluble organic nitrogen (ON) from anthropogenic sources to the ocean. Comparisons of modeled deposition with observations at coastal and marine locations show good overall agreement for inorganic nitrogen and total soluble nitrogen. However, previous modeling approaches result in significant underestimates of the soluble ON deposition if the model only includes the primary soluble ON and the secondary oxidized ON in gases and aerosols. Our model results suggest that including the secondary reduced ON in aerosols as a source of soluble ON contributes to an improved prediction of the deposition rates (g N m−2 yr−1). The model results show a clear distinction in the vertical distribution of soluble ON in aerosols between different processes from the primary sources and the secondary formation. The model results (excluding the biomass burning and natural emission changes) suggest an increase in soluble ON outflow from atmospheric pollution, in particular from East Asia, to the oceans in the twentieth century. These results highlight the necessity of improving the process-based quantitative understanding of the chemical reactions of inorganic nitrogen species with organics in aerosol and cloud water.

Mixed-phase clouds (clouds that consist of both cloud droplets and ice crystals) are frequently present in the Earth’s atmosphere and influence the Earth’s energy budget through their radiative properties, which are highly dependent on the cloud water phase. In this study, the phase partitioning of cloud water is compared among six global climate models (GCMs) and with Cloud and Aerosol Lidar with Orthogonal Polarization retrievals. It is found that the GCMs predict vastly different distributions of cloud phase for a given temperature, and none of them are capable of reproducing the spatial distribution or magnitude of the observed phase partitioning. While some GCMs produced liquid water paths comparable to satellite observations, they all failed to preserve sufficient liquid water at mixed-phase cloud temperatures. Our results suggest that validating GCMs using only the vertically integrated water contents could lead to amplified differences in cloud radiative feedback. The sensitivity of the simulated cloud phase in GCMs to the choice of heterogeneous ice nucleation parameterization is also investigated. The response to a change in ice nucleation is quite different for each GCM, and the implementation of the same ice nucleation parameterization in all models does not reduce the spread in simulated phase amongmore » GCMs. The results suggest that processes subsequent to ice nucleation are at least as important in determining phase and should be the focus of future studies aimed at understanding and reducing differences among the models.« less

[1] Observational evidence demonstrates that marine organic aerosols (MOA) are able to act as ice nuclei. MOA explains a substantial portion of the submicron marine aerosol, so that they have the potential to effectively influence marine cloud microphysics and cloud radiative forcing. This study provides the first evaluation of the radiative forcing and climatic impact of marine organic aerosols as ice nuclei on a global scale. MOA is implemented into a coupled aerosol and general circulation model. It is found that MOA contributes to more ice formation than dust or black carbon/organic matter in mixed-phase clouds. They also have a significant impact on the ice water path in the Southern Hemisphere and therefore could be an important missing source of ice nuclei in current models. The addition of MOA as natural heterogeneous ice nuclei reduces the magnitude of the total top-of-atmosphere anthropogenic aerosol forcing by as much as 0.3 W/m2.

Accurate and stable numerical discretization of the equations for the nonhydrostatic atmosphere is required, for example, to resolve interactions between clouds and aerosols in the atmosphere. Here the authors present a modification of the hydrostatic control-volume approach for solving the nonhydrostatic Euler equations with a Lagrangian vertical coordinate. A scheme with low numerical diffusion is achieved by introducing a low Mach number approximate Riemann solver (LMARS) for atmospheric flows. LMARS is a flexible way to ensure stability for finite-volume numerical schemes in both Eulerian and vertical Lagrangian configurations. This new approach is validated on test cases using a 2D (x–z) configuration.

Fossil fuel black carbon and organic matter (ffBC/OM) are often emitted together with sulfate, which coats the surface of these particles and changes their hygroscopicity. Observational studies at cirrus temperatures (≈−40 °C) show that the hygroscopicity of soot particles can modulate their ice nucleation ability. Here, we implement a scheme for 3 categories of soot (hydrophobic, hydrophilic and hygroscopic) on the basis of laboratory data and specify their ability to act as ice nuclei at mixed-phase temperatures by extrapolating the observations using a published deposition/condensation/immersion freezing parameterization. The new scheme results in significant changes to anthropogenic forcing in mixed-phase clouds. The net forcing in our offline model studies varies from 0.111 to 1.059 W m−2 depending on the ice nucleation capability of hygroscopic soot particles. The total anthropogenic cloud forcing and whole-sky forcing with the new scheme are 0.06 W m−2 and −2.45 W m−2, respectively, but could be more positive (by about 1.17 W m−2) if hygroscopic soot particles are allowed to nucleate ice particles. The change in liquid water path dominates the anthropogenic forcing in mixed-phase clouds.

Observation-based studies have shown that the aerosol cloud lifetime effect or the increase of cloud liquid water (LWP) with increased aerosol loading may have been overestimated in climate models. Here, we simulate shallow warm clouds on 05/27/2011 at the Southern Great Plains (SGP) measurement site established by Department of Energy's Atmospheric Radiation Measurement (ARM) Program using a single column version of a global climate model (CAM5.3) and a cloud resolving model (CRM). The LWP simulated by CAM increases substantially with aerosol loading while that in the CRM does not. The increase of LWP in CAM is caused by a large decrease of the autoconversion rate when cloud droplet number increases. In the CRM, the autoconversion rate is also reduced, but this is offset or even outweighed by the increased evaporation of cloud droplets near cloud top, resulting in an overall decrease in LWP. Our results suggest that climate models need to include the dependence of cloud top growth and the evaporation/condensation process on cloud droplet number concentrations.

We examine the formation of nitrate and ammonium on five types of externally mixed pre-existing aerosols using the hybrid dynamic method in a global chemistry transport model. The model developed here predicts a similar spatial pattern of total aerosol nitrate and ammonium to that of several pioneering studies, but separates the effects of nitrate and ammonium on pure sulfate, biomass burning, fossil fuel, dust and sea salt aerosols. Nitrate and ammonium boost the scattering efficiency of sulfate and organic matter but lower the extinction of sea salt particles since the hygroscopicity of a mixed nitrate-ammonium-sea salt particle is less than that of pure sea salt. The direct anthropogenic forcing of particulate nitrate and ammonium at the top of the atmosphere (TOA) is estimated to be −0.12 W m−2. Nitrate, ammonium and nitric acid gas also affect aerosol activation and the reflectivity of clouds. The first aerosol indirect forcing by anthropogenic nitrate (gas plus aerosol) and ammonium is estimated to be −0.09 W m−2 at the TOA, almost all of which is due to condensation of nitric acid gas onto growing droplets (−0.08 W m−2).

Here we explore light absorption by snowpack containing black carbon (BC) particles residing within ice grains. Basic considerations of particle volumes and BC/snow mass concentrations show that there are generally 0.05–109 BC particles for each ice grain. This suggests that internal BC is likely distributed as multiple inclusions within ice grains, and thus the dynamic effective medium approximation (DEMA) (Chýlek and Srivastava, 1983) is a more appropriate optical representation for BC/ice composites than coated-sphere or standard mixing approximations. DEMA calculations show that the 460 nm absorption cross-section of BC/ice composites, normalized to the mass of BC, is typically enhanced by factors of 1.8–2.1 relative to interstitial BC. BC effective radius is the dominant cause of variation in this enhancement, compared with ice grain size and BC volume fraction. We apply two atmospheric aerosol models that simulate interstitial and within-hydrometeor BC lifecycles. Although only ~2% of the atmospheric BC burden is cloud-borne, 71–83% of the BC deposited to global snow and sea-ice surfaces occurs within hydrometeors. Key processes responsible for within-snow BC deposition are development of hydrophilic coatings on BC, activation of liquid droplets, and subsequent snow formation through riming or ice nucleation by other species and aggregation/accretion of ice particles. Applying deposition fields from these aerosol models in offline snow and sea-ice simulations, we calculate that 32–73% of BC in global surface snow resides within ice grains. This fraction is smaller than the within-hydrometeor deposition fraction because meltwater flux preferentially removes internal BC, while sublimation and freezing within snowpack expose internal BC. Incorporating the DEMA into a global climate model, we simulate increases in BC/snow radiative forcing of 43–86%, relative to scenarios that apply external optical properties to all BC. We show that snow metamorphism driven by diffusive vapor transfer likely proceeds too slowly to alter the mass of internal BC while it is radiatively active, but neglected processes like wind pumping and convection may play much larger roles. These results suggest that a large portion of BC in surface snowpack may reside within ice grains and increase BC/snow radiative forcing, although measurements to evaluate this are lacking. Finally, previous studies of BC/snow forcing that neglected this absorption enhancement are not necessarily biased low, because of application of absorption-enhancing sulfate coatings to hydrophilic BC, neglect of coincident absorption by dust in snow, and implicit treatment of cloud-borne BC resulting in longer-range transport.

Refractory black carbon aerosols (rBC) emitted by biomass burning (fires) and fossil fuel combustion, affect global climate and atmospheric chemistry. In the Southern Hemisphere (SH), rBC is transported in the atmosphere from low- and mid-latitudes to Antarctica and deposited to the polar ice sheet preserving a history of emissions and atmospheric transport. Here, we present two high-resolution Antarctic rBC ice core records drilled from the West Antarctic Ice Sheet divide and Law Dome on the periphery of the East Antarctic ice sheet. Separated by ~3500 km, the records span calendar years 1850–2001 and reflect the rBC distribution over the Indian and Pacific ocean sectors of the Southern Ocean. Concentrations of rBC in the ice cores displayed significant variability at annual to decadal time scales, notably in ENSO-QBO and AAO frequency bands. The delay observed between rBC and ENSO variability suggested that ENSO does not directly affect rBC transport, but rather continental hydrology, subsequent fire regimes, and aerosol emissions. From 1850 to 1950, the two ice core records were uncorrelated but were highly correlated from 1950 to 2002 (cross-correlation coefficient at annual resolution: r = 0.54, p < 0.01) due to a common decrease in rBC variability. The decrease in ice-core rBC from the 1950s to late 1980s displays similarities with inventories of SH rBC grass fires and biofuel emissions, which show reduced emission estimates over that period.

Refractory black carbon aerosols (rBC) from biomass burning and fossil fuel combustion are deposited to the Antarctic ice sheet and preserve a history of emissions and long-range transport from low- and mid-latitudes. Antarctic ice core rBC records may thus provide information with respect to past combustion aerosol emissions and atmospheric circulation. Here, we present six East Antarctic ice core records of rBC concentrations and fluxes covering the last two centuries with approximately annual resolution (cal. yr. 1800 to 2000). The ice cores were drilled in disparate regions of the high East Antarctic ice sheet, at different elevations and net snow accumulation rates. Annual rBC concentrations were log-normally distributed and geometric means of annual concentrations ranged from 0.10 to 0.18 μg kg−1. Average rBC fluxes were determined over the time periods 1800 to 2000 and 1963 to 2000 and ranged from 3.4 to 15.5 μg m−2 a−1 and 3.6 to 21.8 μg m−2 a−1, respectively. Geometric mean concentrations spanning 1800 to 2000 increased linearly with elevation at a rate of 0.025 μg kg−1/500 m. Spectral analysis of the records revealed significant decadal-scale variability, which at several sites was comparable to decadal ENSO variability.

A recent study showed that aerosol-induced feedbacks between microphysics and dynamics predominantly determined the cloud-mass response to aerosols in thin clouds with liquid-water path (LWP) of ∼50 g m −2 or less; in this paper, cloud mass represents the time- and area-averaged LWP and LWP is the column-integrated cloud liquid content (LWC); LWC is the mass of cloud liquid per unit volume of air. This is contrary to studies which have shown that aerosol-induced inefficient conversion and sedimentation play an important role in the determination of the effect of aerosols on cloud mass. These studies are generally based on clouds with LWP >50 g m −2 . Hence, it is important to understand whether the role of aerosol-induced feedbacks in the effect of aerosols on cloud mass depends on the level of LWP. Pairs of numerical experiments for high and low-aerosol cases are run for four cases of stratiform clouds with different LWPs. All of these cases show that the role of condensation or evaporation of cloud liquid in the cloud-mass response to aerosol is more important than that of conversion of cloud liquid to rain and sedimentation (or precipitation). This indicates that focusing only on parameterization of autoconversion and sedimentation to represent aerosol effects on cloud mass in climate models can be misleading. Also, this study finds that the effect of aerosol-induced sedimentation suppression on the cloud-mass response to aerosol becomes less important as LWP lowers. Instead, the effect of aerosol-induced changes in condensation or evaporation on the cloud-mass response becomes more important with the decreasing LWP. These changes in condensation (and associated changes in evaporation) are caused by interactions (or feedbacks) among aerosol, droplet surface area, supersaturation, and instability around cloud base.

Desert dust plays an important role in the climate system through its impact on Earth¿s radiative budget and its role in the biogeochemical cycle as a source of iron in highnutrient- low-chlorophyll regions. A large degree of diversity exists between the many global models that simulate the dust cycle to estimate its impact on climate. We present the results of a broad intercomparison of a total of 15 global aerosol models within the AeroCom project. Each model is compared to observations focusing on variables responsible for the uncertainties in estimating the direct radiative effect and the dust impact on the biogeochemical cycle, i.e., aerosol optical depth (AOD) and dust deposi10 tion. Additional comparisons to Angstro¨m Exponent (AE), coarse mode AOD and dust surface concentration are included to extend the assessment of model performance. These datasets form a benchmark data set which is proposed for model inspection and future dust model developments. In general, models perform better in simulating climatology of vertically averaged integrated parameters (AOD and AE) in dusty sites 15 than they do with total deposition and surface concentration. Almost all models overestimate deposition fluxes over Europe, the Indian Ocean, the Atlantic Ocean and ice core data. Differences among the models arise when simulating deposition at remote sites with low fluxes over the Pacific and the Southern Atlantic Ocean. This study also highlights important differences in models ability to reproduce the deposition flux over Antarctica. The cause of this discrepancy could not be identified but different dust regimes at each site and issues with data quality should be considered. Models generally simulate better surface concentration at stations downwind of the main sources than at remote ones. Likewise, they simulate better surface concentration at stations affected by Saharan dust than at stations affected by Asian dust. Most models simulate the gradient in AOD and AE between the different dusty regions, however the seasonality and magnitude of both variables is better simulated at African stations than Middle East ones. The models also reproduce the dust transport across the Atlantic in terms of both AOD and AE; they simulate the offshore transport of West Africa throughout the year and limit the transport across the Atlantic to the summer months, yet overestimating the AOD and transporting too fine particles. However, most of the models do not reproduce the southward displacement of the dust cloud during the winter responsible of the transport of dust into South America. Based on the dependency of AOD on aerosol 5 burden and size distribution we use model data bias with respect to AOD and AE and infer on the over/under estimation of the dust emissions. According to this we suggest the emissions in the Sahara be between 792 and 2271 Tg/yr and the one in the Middle East between 376 and 526 Tg/yr., JRC.DDG.H.2-Climate change and air quality

Satellite-based estimates of the aerosol indirect effect (AIE) are consistently smaller than the estimates from global aerosol models, and, partly as a result of these differences, the assessment of this climate forcing includes large uncertainties. Satellite estimates typically use the present-day (PD) relationship between observed cloud drop number concentrations ( N c ) and aerosol optical depths (AODs) to determine the preindustrial (PI) values of N c . These values are then used to determine the PD and PI cloud albedos and, thus, the effect of anthropogenic aerosols on top of the atmosphere radiative fluxes. Here, we use a model with realistic aerosol and cloud processes to show that empirical relationships for ln( N c ) versus ln(AOD) derived from PD results do not represent the atmospheric perturbation caused by the addition of anthropogenic aerosols to the preindustrial atmosphere. As a result, the model estimates based on satellite methods of the AIE are between a factor of 3 to more than a factor of 6 smaller than model estimates based on actual PD and PI values for N c . Using ln( N c ) versus ln(AI) (Aerosol Index, or the optical depth times angstrom exponent) to estimate preindustrial values for N c provides estimates for N c and forcing that are closer to the values predicted by the model. Nevertheless, the AIE using ln( N c ) versus ln(AI) may be substantially incorrect on a regional basis and may underestimate or overestimate the global average forcing by 25 to 35%.

Satellite observations are analyzed to examine the correlations between aerosols and the tropical tropopause layer (TTL) temperature and water vapor. This study focuses on two regions, both of which are important pathways for the mass transport from the troposphere to the stratosphere and over which Asian pollution prevails: South and East Asia during boreal summer and the Maritime Continent during boreal winter. Using the upper-tropospheric carbon monoxide measurements from the Aura Microwave Limb Sounder as a proxy of aerosols to classify ice clouds as polluted or clean, the authors find that polluted clouds have a smaller ice effective radius and a higher temperature and specific humidity near the tropopause than clean clouds. The increase in water vapor appears to be related to the increase in temperature, as a result of increased aerosols. Meteorological differences between the clouds cannot explain the differences in temperature and water vapor for the polluted and clean clouds. The authors hypothesize that aerosol semidirect radiative heating and/or changes in cirrus radiative heating, resulting from aerosol microphysical effects on clouds, may contribute to the increased TTL temperature and thus increased water vapor in the polluted clouds.

Cirrus clouds cover approximately 20–25% of the globe and thus play an important role in the Earth's radiation budget. Therefore the effect of aerosols on cirrus clouds can have a substantial impact on global radiative forcing if either the ice-water path (IWP) and/or the cloud ice number concentration (CINC) changes. This study examines the aerosol indirect effect (AIE) through changes in the CINC and IWP for a cirrus cloud case. We use a cloud-system resolving model (CSRM) coupled with a double-moment representation of cloud microphysics. Intensified interactions among CINC, deposition and dynamics play a critical role in increasing the IWP as aerosols increase. Increased IWP leads to a smaller change in the outgoing LW radiation relative to that for the SW radiation for increasing aerosols. Increased aerosols lead to increased CINC, providing increased surface area for water vapor deposition. The increased deposition causes depositional heating which produces stronger updrafts, and leads to the increased IWP. The conversion of ice crystals to aggregates through autoconversion and accretion plays a negligible role in the IWP response to aerosols, and the sedimentation of aggregates is negligible. The sedimentation of ice crystals plays a more important role in the IWP response to aerosol increases than the sedimentation of aggregates, but not more than the interactions among the CINC, deposition and dynamics.

We present a sensitivity study of the effects of spatial and temporal resolution of atmospheric relative humidity (RH) on calculated aerosol optical thickness (AOT) and the aerosol direct radiative effects (DRE) in a global model. We carry out different modeling experiments using the same aerosol fields simulated in the Global Modeling Initiative (GMI) model at a resolution of 2° latitude by 2.5° longitude, using time-averaged fields archived every three hours by the Goddard Earth Observation System Version 4 (GEOS-4), but we change the horizontal and temporal resolution of the relative humidity fields. We find that, on a global average, the AOT calculated using RH at a 1°×1.25° horizontal resolution is 11% higher than that using RH at a 2°×2.5° resolution, and the corresponding DRE at the top of the atmosphere is 8–9% and 15% more negative (i.e., more cooling) for total aerosols and anthropogenic aerosol alone, respectively, in the finer spatial resolution case. The difference is largest over surface escarpment regions (e.g. >200% over the Andes Mountains) where RH varies substantially with surface terrain. The largest zonal mean AOT difference occurs at 50–60° N (16–21%), where AOT is also relatively larger. A similar impact is also found when the time resolution of RH is increased. This increase of AOT and aerosol cooling with the increase of model resolution is due to the highly non-linear relationship between RH and the aerosol mass extinction efficiency (MEE) at high RH (>80%). Our study is a specific example of the uncertainty in model results highlighted by multi-model comparisons such as AeroCom, and points out one of the many inter-model differences that can contribute to the overall spread among models.

Cirrus clouds have a net warming effect on the atmosphere and cover about 30% of the Earth's area. Aerosol particles initiate ice formation in the upper troposphere through modes of action that include homogeneous freezing of solution droplets, heterogeneous nucleation on solid particles immersed in a solution, and deposition nucleation of vapor onto solid particles. Here, we examine the possible change in ice number concentration from anthropogenic soot originating from surface sources of fossil fuel and biomass burning, from anthropogenic sulfate aerosols, and from aircraft that deposit their aerosols directly in the upper troposphere. We use a version of the aerosol model that predicts sulfate number and mass concentrations in 3-modes and includes the formation of sulfate aerosol through homogeneous binary nucleation as well as a version that only predicts sulfate mass. The 3-mode version best represents the Aitken aerosol nuclei number concentrations in the upper troposphere which dominated ice crystal residues in the upper troposphere. Fossil fuel and biomass burning soot aerosols with this version exert a radiative forcing of −0.3 to −0.4 Wm−2 while anthropogenic sulfate aerosols and aircraft aerosols exert a forcing of −0.01 to 0.04 Wm−2 and −0.16 to −0.12 Wm−2, respectively, where the range represents the forcing from two parameterizations for ice nucleation. The sign of the forcing in the mass-only version of the model depends on which ice nucleation parameterization is used and can be either positive or negative. The magnitude of the forcing in cirrus clouds can be comparable to the forcing exerted by anthropogenic aerosols on warm clouds, but this forcing has not been included in past assessments of the total anthropogenic radiative forcing of climate.

The number concentration of cloud condensation nuclei (CCN) formed as a result of anthropogenic emissions is a key uncertainty in the study of aerosol indirect forcing and global climate change. Here, we use a global aerosol model that includes an empirical boundary layer nucleation mechanism, the use of primary-emitted sulfate particles to represent sub-grid scale nucleation, as well as binary homogeneous nucleation to explore how nucleation affects the CCN concentration and the first aerosol indirect effect (AIE). The inclusion of the boundary layer nucleation scheme increases the global average CCN concentrations in the boundary layer by 31.4% when no primary-emitted sulfate particles are included and by 5.3% when they are included. Particle formation with the boundary layer nucleation scheme decreases the first indirect forcing over ocean, and increases the first indirect forcing over land when primary sulfate particles are included. This suggests that whether particle formation from aerosol nucleation increases or decreases aerosol indirect effects largely depends on the relative change of primary particles and SO2 emissions from the preindustrial to the present day atmosphere. Including primary-emitted sulfate particle significantly increases both the anthropogenic fraction of CCN concentrations and the first aerosol indirect forcing. The forcing from various treatments of aerosol nucleation ranges from −1.22 to −2.03 w/m2. This large variation shows the importance of better quantifying aerosol nucleation mechanisms for the prediction of CCN concentrations and aerosol indirect effects.

The uptake of water by contrails in ice-supersaturated air and the release of water after ice particle advection and sedimentation dehydrates the atmosphere at flight levels and redistributes humidity mainly to lower levels. The dehydration is investigated by coupling a plume-scale contrail model with a global aerosol–climate model. The contrail model simulates all the individual contrails forming from global air traffic for meteorological conditions as defined by the climate model. The computed contrail cirrus properties compare reasonably with theoretical concepts and observations. The mass of water in aged contrails may exceed 106 times the mass of water emitted from aircraft. Many of the ice particles sediment and release water in the troposphere, on average 700 m below the mean flight levels. Simulations with and without coupling are compared. The drying at contrail levels causes thinner and longer-lived contrails with about 15 % reduced contrail radiative forcing (RF). The reduced RF from contrails is on the order of 0.06 W m−2, slightly larger than estimated earlier because of higher soot emissions. For normal traffic, the RF from dehydration is small compared to interannual variability. A case with emissions increased by 100 times is used to overcome statistical uncertainty. The contrails impact the entire hydrological cycle in the atmosphere by reducing the total water column and the cover by high- and low-level clouds. For normal traffic, the dehydration changes contrail RF by positive shortwave and negative longwave contributions on the order of 0.04 W m−2, with a small negative net RF. The total net RF from contrails and dehydration remains within the range of previous estimates.

The IPCC has stressed the importance of producing unbiased estimates of the uncertainty in indirect aerosol forcing, in order to give policy makers as well as research managers an understanding of the most important aspects of climate change that require refinement. In this study, we use 3-D meteorological fields together with a radiative transfer model to examine the spatially-resolved uncertainty in estimates of the first indirect aerosol forcing. The global mean forcing calculated in the reference case is -1.30 Wm-2. Uncertainties in the indirect forcing associated with aerosol and aerosol precursor emissions, aerosol mass concentrations from different chemical transport models, aerosol size distributions, the cloud droplet parameterization, the representation of the in-cloud updraft velocity, the relationship between effective radius and volume mean radius, cloud liquid water content, cloud fraction, and the change in the cloud drop single scattering albedo due to the presence of black carbon are calculated. The aerosol burden calculated by chemical transport models and the cloud fraction are found to be the most important sources of uncertainty. Variations in these parameters cause an underestimation or overestimation of the indirect forcing compared to the base case by more than 0.6 Wm-2. Uncertainties associated with aerosol and aerosol precursor emissions, uncertainties in the representation of the aerosol size distribution (including the representation of the pre-industrial size distribution), and uncertainties in the representation of cloud droplet spectral dispersion effect cause uncertainties in the global mean forcing of 0.2~0.6 Wm-2. There are significant regional differences in the uncertainty associated with the first indirect forcing with the largest uncertainties in industrial regions (North America, Europe, East Asia) followed by those in the major biomass burning regions.

Global modeling of ice clouds and the effects of aerosol-related ice nuclei (IN) changes on clouds and climate remains a significant challenge. Here, we describe a parameterization that accounts for the effects of homogeneous ice nucleation as well as two different modes of heterogeneous nucleation in the upper troposphere. The parameterization treats homogeneous nucleation by sulfate aerosol, deposition nucleation as described by the MEYERS et al. (1992) formulation, and immersion nucleation by soot aerosol. Besides air mass temperature and updraft velocity, number concentration of pure sulfate aerosol acting through homogeneous ice nucleation and number concentration of soot aerosol as heterogeneous ice nuclei are explicitly included in the parameterization so that the indirect effect of aerosols on the cirrus clouds (i.e. the effect of increases in aerosol number concentrations) can be described in a global model. In addition the transition from the heterogeneous to homogeneous-dominated nucleation and the competition between homogeneous and heterogeneous nucleation in the transition regime are considered in the parameterization. The parameterization is compared to the results from air parcel model simulations of uplifting and adiabatically cooling clouds and to other recently developed ice nucleation parameterizations.

An adaptive grid dynamical core for a global atmospheric climate model has been developed. Adaptations allow a smooth transition from hydrostatic to non-hydrostatic physics at small resolution. The adaptations use a parallel program library for block-wise adaptive grids on the sphere. This library also supports the use of a reduced grid with coarser resolution in the longitudinal direction as the poles are approached. This permits the use of a longer time step since the CFL number restriction (CFL < 1) in a regular longitude-latitude grid is most severe in the zonal direction at high latitudes. Several tests show that our modelling procedures are stable and accurate.

Aerosols exert myriad influences on the earth's environment and climate, and on human health. The complexity of aerosol-related processes requires that information gathered to improve our understanding of climate change must originate from multiple sources, and that effective strategies for data integration need to be established. While a vast array of observed and modeled data are becoming available, the aerosol research community currently lacks the necessary tools and infrastructure to reap maximum scientific benefit from these data. Spatial and temporal sampling differences among a diverse set of sensors, nonuniform data qualities, aerosol mesoscale variabilities, and difficulties in separating cloud effects are some of the challenges that need to be addressed. Maximizing the long-term benefit from these data also requires maintaining consistently well-understood accuracies as measurement approaches evolve and improve. Achieving a comprehensive understanding of how aerosol physical, chemical, and radiative processes impact the earth system can be achieved only through a multidisciplinary, inter-agency, and international initiative capable of dealing with these issues. A systematic approach, capitalizing on modern measurement and modeling techniques, geospatial statistics methodologies, and high-performance information technologies, can provide the necessary machinery to support this objective. We outline a framework for integrating and interpreting observations and models, and establishing an accurate, consistent, and cohesive long-term record, following a strategy whereby information and tools of progressively greater sophistication are incorporated as problems of increasing complexity are tackled. This concept is named the Progressive Aerosol Retrieval and Assimilation Global Observing Network (PARAGON). To encompass the breadth of the effort required, we present a set of recommendations dealing with data interoperability; measurement and model integration; multisensor synergy; data summarization and mining; model evaluation; calibration and validation; augmentation of surface and in situ measurements; advances in passive and active remote sensing; and design of satellite missions. Without an initiative of this nature, the scientific and policy communities will continue to struggle with understanding the quantitative impact of complex aerosol processes on regional and global climate change and air quality.

Given the breadth and complexity of available data, constructing a measurement-based description of global tropospheric aerosols that will effectively confront and constrain global three-dimensional models is a daunting task. Because data are obtained from multiple sources and acquired with nonuniform spatial and temporal sampling, scales, and coverage, protocols need to be established that will organize this vast body of knowledge. Currently, there is no capability to assemble the existing aerosol data into a unified, interoperable whole. Technology advancements now being pursued in high-performance distributed computing initiatives can accomplish this objective. Once the data are organized, there are many approaches that can be brought to bear upon the problem of integrating data from different sources. These include data-driven approaches, such as geospatial statistics formulations, and model-driven approaches, such as assimilation or chemical transport modeling. Establishing a data interopera...

Anthropogenic aerosols enhance cloud reflectivity by increasing the number concentration of cloud droplets, leading to a cooling effect on climate known as the indirect aerosol effect. Observational support for this effect is based mainly on evidence that aerosol number concentrations are connected with droplet concentrations, but it has been difficult to determine the impact of these indirect effects on radiative forcing1,2,3. Here we provide observational evidence for a substantial alteration of radiative fluxes due to the indirect aerosol effect. We examine the effect of aerosols on cloud optical properties using measurements of aerosol and cloud properties at two North American sites that span polluted and clean conditions—a continental site in Oklahoma with high aerosol concentrations, and an Arctic site in Alaska with low aerosol concentrations. We determine the cloud optical depth required to fit the observed shortwave downward surface radiation. We then use a cloud parcel model to simulate the cloud optical depth from observed aerosol properties due to the indirect aerosol effect. From the good agreement between the simulated indirect aerosol effect and observed surface radiation, we conclude that the indirect aerosol effect has a significant influence on radiative fluxes.

Significant progress has been made in understanding how aerosols affect climate change, but big unknowns must still be addressed.

The component of the indirect aerosol effect related to changes in precipitation efficiency (the second indirect or Albrecht effect) is presently evaluated in climate models by taking the difference in net irradiance between a present-day and a preindustrial simulation using fixed sea surface temperatures (SSTs). This approach gives a “quasi forcing,” which differs from a pure forcing in that fields other than the initially perturbed quantity have been allowed to vary. It is routinely used because, in contrast to the first indirect (Twomey) effect, there is no straightforward method of calculating a pure forcing for the second indirect effect. This raises the question of whether evaluation of the second indirect effect in this manner is adequate as an indication of the likely effect of this perturbation on the global-mean surface temperature. An atmospheric global climate model (AGCM) is used to compare the evaluation of different radiative perturbations as both pure forcings (when available) and...