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International audience; Tropospheric anthropogenic aerosols contribute the second-largest forcing to climate change, but with high uncertainty owing to their spatio-temporal variability and complicated optical properties. In this Review, we synthesize understanding of aerosol observations and their radiative and climate effects. Aerosols offset about one-third of the warming effect by anthropogenic greenhouse gases. Yet, in regions and seasons where the absorbing aerosol fraction is high — such as South America and East and South Asia — substantial atmospheric warming can occur. The internal mixing and the vertical distribution of aerosols, which alters both the direct effect and aerosol-cloud interactions, might further enhance this warming. Despite extensive research in aerosol-cloud interactions, there is still at least a 50% spread in total aerosol forcing estimates. This ongoing uncertainty is linked, in part, to the poor measurement of anthropogenic and natural aerosol absorption, as well as the little-understood effects of aerosols on clouds. Next-generation, space-borne, multi-angle polarization and active remote sensing, combined with in situ observations, offer opportunities to better constrain aerosol scattering, absorption and size distribution, thus, improving models to refine estimates of aerosol forcing and climate effects.

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.

We have implemented a parameterization for forming ice in large‐scale cirrus clouds that accounts for the changes in updrafts associated with a spectrum of waves acting within each time step in the model. This allows us to account for the frequency of homogeneous and heterogeneous freezing events that occur within each time step of the model and helps to determine more realistic ice number concentrations as well as changes to ice number concentrations. The model is able to fit observations of ice number at the lowest temperatures in the tropical tropopause but is still somewhat high in tropical latitudes with temperatures between 195°K and 215°K. The climate forcings associated with different representations of heterogeneous ice nuclei (IN or INPs) are primarily negative unless large additions of IN are made, such as when we assumed that all aircraft soot acts as an IN. However, they can be close to zero if it is assumed that all background dust can act as an INP irrespective of how much sulfate is deposited on these particles. Our best estimate for the forcing of anthropogenic aircraft soot in this model is −0.2 ± 0.06 W/m2, while that from anthropogenic fossil/biofuel soot is −0.093 ± 0.033 W/m2. Natural and anthropogenic open biomass burning leads to a net forcing of −0.057 ± 0.05 W/m2., Key Points A new version of the CAM/IMPACT atmospheric model that includes gravity waves and the effect of aerosols on cirrus clouds is presentedThe best representation of the particles that act as ice nuclei results in a climate forcing of −0.2 W/m2 for aircraft sootThe use of all dust particles as ice nuclei lowers this forcing to near zero

Significance Secondary organic aerosol (SOA) forms via a variety of processes and plays a key role in climate change and air quality. Recent measurements indicate that most SOA exists as an internal mixture with other aerosols. This study examines the radiative effect of using a mixing state for SOA that depends on the process of formation, based on an explicit mechanism for the chemical production of SOA. The radiative forcing of SOA in the future is estimated using this approach. A surprising result is that the contribution of SOA to radiative forcing increases substantially (becomes more negative) in the future even though the increase of its burden is slight., Secondary organic aerosol (SOA) nearly always exists as an internal mixture, and the distribution of this mixture depends on the formation mechanism of SOA. A model is developed to examine the influence of using an internal mixing state based on the mechanism of formation and to estimate the radiative forcing of SOA in the future. For the present day, 66% of SOA is internally mixed with sulfate, while 34% is internally mixed with primary soot. Compared with using an external mixture, the direct effect of SOA is decreased due to the decrease in total aerosol surface area and the increase of absorption efficiency. Aerosol number concentrations are sharply reduced, and this is responsible for a large decrease in the cloud albedo effect. Internal mixing decreases the radiative effect of SOA by a factor of >4 compared with treating SOA as an external mixture. The future SOA burden increases by 24% due to CO2 increases and climate change, leading to a total (direct plus cloud albedo) radiative forcing of −0.05 W m−2. When the combined effects of changes in climate, anthropogenic emissions, and land use are included, the SOA forcing is −0.07 W m−2, even though the SOA burden only increases by 6.8%. This is caused by the substantial increase of SOA associated with sulfate in the Aitken mode. The Aitken mode increase contributes to the enhancement of first indirect radiative forcing, which dominates the total radiative forcing.

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.

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.

A modest operational program of systematic aircraft measurements can resolve key satellite aerosol data record limitations. Satellite observations provide frequent global aerosol amount maps but offer only loose aerosol property constraints needed for climate and air quality applications. We define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ. The flight program could characterize major aerosol airmass types statistically, at a level of detail unobtainable from space. It would 1) enhance satellite aerosol retrieval products with better climatology assumptions and 2) improve translation between satellite-retrieved optical properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space; improve aerosol constraints on climate modeling; help interrelate remote sensing, in situ, and modeling aerosol-type definitions; and contribute to future satellite aerosol missions. Fifteen required variables are identified and four payload options of increasing ambition are defined to constrain these quantities. “Option C” could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable, even if aerosol loading varies.

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.

There is growing interest in the formation of secondary organic aerosol (SOA) through condensed aqueous-phase reactions. In this study, we use a global model (IMPACT) to investigate the potential formation of SOA in the aqueous phase. We compare results from several multiphase process schemes with detailed aqueous-phase reactions to schemes that use a first-order gas-to-particle formation rate based on uptake coefficients. The predicted net global SOA production rate in cloud water ranges from 13.1 Tg yr−1 to 46.8 Tg yr−1 while that in aerosol water ranges from −0.4 Tg yr−1 to 12.6 Tg yr−1. The predicted global burden of SOA formed in the aqueous phase ranges from 0.09 Tg to 0.51 Tg. A sensitivity test to investigate two representations of cloud water content from two global models shows that increasing cloud water by an average factor of 2.7 can increase the net SOA production rate in cloud water by a factor of 4 at low altitudes (below approximately 900 hPa). We also investigated the importance of including dissolved Fe chemistry in cloud water aqueous reactions. Adding these reactions increases the formation rate of aqueous-phase OH by a factor of 2.6 and decreases the amount of global aqueous SOA formed by 31%. None of the mechanisms discussed here is able to provide a best fit for all observations. Rather, the use of an uptake coefficient method for aerosol water and a multi-phase scheme for cloud water provides the best fit in the Northern Hemisphere and the use of multiphase process scheme for aerosol and cloud water provides the best fit in the tropics. The model with Fe chemistry underpredicts oxalate measurements in all regions. Finally, the comparison of oxygen-to-carbon (O / C) ratios estimated in the model with those estimated from measurements shows that the modeled SOA has a slightly higher O / C ratio than the observed SOA for all cases.

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.

Under the Federal Aviation Administration’s (FAA) Aviation Climate Change Research Initiative (ACCRI), non-CO2 climatic impacts of commercial aviation are assessed for current (2006) and for future (2050) baseline and mitigation scenarios. The effects of the non-CO2 aircraft emissions are examined using a number of advanced climate and atmospheric chemistry transport models. Radiative forcing (RF) estimates for individual forcing effects are provided as a range for comparison against those published in the literature. Preliminary results for selected RF components for 2050 scenarios indicate that a 2% increase in fuel efficiency and a decrease in NOx emissions due to advanced aircraft technologies and operational procedures, as well as the introduction of renewable alternative fuels, will significantly decrease future aviation climate impacts. In particular, the use of renewable fuels will further decrease RF associated with sulfate aerosol and black carbon. While this focused ACCRI program effort has yielded significant new knowledge, fundamental uncertainties remain in our understanding of aviation climate impacts. These include several chemical and physical processes associated with NOx–O3–CH4 interactions and the formation of aviation-produced contrails and the effects of aviation soot aerosols on cirrus clouds as well as on deriving a measure of change in temperature from RF for aviation non-CO2 climate impacts—an important metric that informs decision-making.

This report is the response to a request by the Committee on Space Research of the International Council for Science to prepare a roadmap on observation and integrated Earth-system science for the coming ten years. Its focus is on the combined use of observations and modelling to address the functioning, predictability and projected evolution of interacting components of the Earth system on timescales out to a century or so. It discusses how observations support integrated Earth-system science and its applications, and identifies planned enhancements to the contributing observing systems and other requirements for observations and their processing. All types of observation are considered, but emphasis is placed on those made from space.\ud \ud The origins and development of the integrated view of the Earth system are outlined, noting the interactions between the main components that lead to requirements for integrated science and modelling, and for the observations that guide and support them. What constitutes an Earth-system model is discussed. Summaries are given of key cycles within the Earth system.\ud \ud The nature of Earth observation and the arrangements for international coordination essential for effective operation of global observing systems are introduced. Instances are given of present types of observation, what is already on the roadmap for 2016–2025 and some of the issues to be faced. Observations that are organised on a systematic basis and observations that are made for process understanding and model development, or other research or demonstration purposes, are covered. Specific accounts are given for many of the variables of the Earth system.\ud \ud The current status and prospects for Earth-system modelling are summarized. The evolution towards applying Earth-system models for environmental monitoring and prediction as well as for climate simulation and projection is outlined. General aspects of the improvement of models, whether through refining the representations of processes that are already incorporated or through adding new processes or components, are discussed. Some important elements of Earth-system models are considered more fully.\ud \ud Data assimilation is discussed not only because it uses observations and models to generate datasets for monitoring the Earth system and for initiating and evaluating predictions, in particular through reanalysis, but also because of the feedback it provides on the quality of both the observations and the models employed. Inverse methods for surface-flux or model-parameter estimation are also covered. Reviews are given of the way observations and the processed datasets based on them are used for evaluating models, and of the combined use of observations and models for monitoring and interpreting the behaviour of the Earth system and for predicting and projecting its future.\ud \ud A set of concluding discussions covers general developmental needs, requirements for continuity of space-based observing systems, further long-term requirements for observations and other data, technological advances and data challenges, and the importance of enhanced international co-operation.

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).

We use a single aerosol model to explore the effects of the differing meteorological fields from the NCAR CAM5 and GFDL AM3 models. We simulate the global distributions of sulfate, black carbon, organic matter, dust and sea salt using the University of Michigan IMPACT model and use these fields to calculate aerosol direct and indirect forcing, thereby isolating the impacts of the differing meteorological fields. Over all, the IMPACT-AM3 model predicts larger burdens and longer aerosol lifetimes than the IMPACT-CAM5 model. However, the IMPACT-CAM5 simulations transport more black carbon to the polar regions and more dust from Asia towards North America. These differences can mainly be attributed to differences in: (1) the vertical cloud mass flux and large-scale precipitation fields which determine the wet deposition of aerosols; (2) the in-cloud liquid water content and the cloud coverage which determine the wet aqueous phase production of sulfate. The burden, lifetime and global distribution, especially black carbon in polar regions, are strongly affected by choice of the parameters used for wet deposition. The total annual mean aerosol optical depth (AOD) at 550 nm ranges from 0.087 to 0.122 for the IMPACT-AM3 model and from 0.138 to 0.186 for the IMPACT-CAM5 model (range is due to different parameters used for wet deposition). Even though IMPACT-CAM5 has smaller aerosol burdens, its AOD is larger due to the much higher relative humidity in CAM5 which leads to more hygroscopic growth. The corresponding global annual average anthropogenic and all-sky aerosol direct forcing at the top of the atmosphere ranges from −0.25 W m−2 to −0.30 W m−2 for IMPACT-AM3 and from −0.48 W m−2 to −0.64 W m−2 for IMPACT-CAM5. The global annual average anthropogenic 1st aerosol indirect effect at the top of the atmosphere ranges from −1.26 W m−2 to −1.44 W m−2 for IMPACT-AM3 and from −1.74 W m−2 to −1.77 W m−2 for IMPACT-CAM5.

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.