Publications


Biomass burning aerosols in most climate models are too absorbing

Nature Communications Nature Research (part of Springer Nature) (2021)

H Brown, X Liu, R Pokhrel, S Murphy, Z Lu, R Saleh, T Mielonen, H Kokkola, T Bergman, G Myhre, R Skeie, D WATSON-PARRIS, P STIER, B Johnson, N Bellouin, M Schulz, V Vakkari, JP Beukes, PG van Zyl, S Liu, D Chand


Climate impacts of COVID‐19 induced emission changes

Geophysical Research Letters Wiley (2020) e2020GL091805

A Gettelman, R Lamboll, C Bardeen, P Forster

The COVID‐19 pandemic led to dramatic changes in economic activity in 2020. We use estimates of emissions changes for 2020 in two Earth System Models (ESMs) to simulate the impacts of the COVID‐19 economic changes. Ensembles of nudged simulations are used to separate small signals from meteorological variability. Reductions in aerosol and precursor emissions, chiefly Black Carbon (BC) and sulfate (SO4), led to reductions in total anthropogenic aerosol cooling through aerosol‐cloud interactions. The average overall Effective Radiative Forcing (ERF) peaks at +0.29±0.15 Wm−2 in spring 2020. Changes in cloud properties are smaller than observed changes during 2020. Impacts of these changes on regional land surface temperature range up to +0.3K. The peak impact of these aerosol changes on global surface temperature is very small (+0.03K). However, the aerosol changes are the largest contribution to radiative forcing and temperature changes as a result of COVID‐19 affected emissions, larger than ozone, CO2 and contrail effects.


An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin

Atmospheric Chemistry and Physics Copernicus GmbH 21 (2021) 1507-1563

J Redemann, R Wood, P Zuidema, SJ Doherty, B Luna, SE LeBlanc, MS Diamond, Y Shinozuka, IY Chang, AM da Silva, AM Fridlind, GR Carmichael, PE Saide, GA Ferrada, SG Howell, S Tanelli, TS L'Ecuyer, AM Dzambo, OO Sy, GM McFarquhar, M Kacarab, JPS Wong, JD Small-Griswold, KL Thornhill, D Noone

<jats:p>Abstract. Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June–October), aerosol particles reaching 3–5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ∼350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ∼100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced. </jats:p>


The CLoud–Aerosol–Radiation Interaction and Forcing: Year 2017 (CLARIFY-2017) measurement campaign

Atmospheric Chemistry and Physics Copernicus Publications 21 (2021) 1049-1084

SJ Abel, PA Barrett, N Bellouin, A Blyth, KN Bower, M Brooks, MI Cotterell, Z Cui, N Davies, B Dingley, P Field, P Formenti, H Gordon, R Herbert, B Johnson, AC Jones, JM Langridge, F Malavelle, F Peers, J Redemann, P Stier, JW Taylor, R Wood, H Wu

The representations of clouds, aerosols, and cloud–aerosol–radiation impacts remain some of the largest uncertainties in climate change, limiting our ability to accurately reconstruct past climate and predict future climate. The south-east Atlantic is a region where high atmospheric aerosol loadings and semi-permanent stratocumulus clouds are co-located, providing an optimum region for studying the full range of aerosol–radiation and aerosol–cloud interactions and their perturbations of the Earth's radiation budget. While satellite measurements have provided some useful insights into aerosol–radiation and aerosol–cloud interactions over the region, these observations do not have the spatial and temporal resolution, nor the required level of precision to allow for a process-level assessment. Detailed measurements from high spatial and temporal resolution airborne atmospheric measurements in the region are very sparse, limiting their use in assessing the performance of aerosol modelling in numerical weather prediction and climate models. CLARIFY-2017 was a major consortium programme consisting of five principal UK universities with project partners from the UK Met Office and European- and USA-based universities and research centres involved in the complementary ORACLES, LASIC, and AEROCLO-sA projects. The aims of CLARIFY-2017 were fourfold: (1) to improve the representation and reduce uncertainty in model estimates of the direct, semi-direct, and indirect radiative effect of absorbing biomass burning aerosols; (2) to improve our knowledge and representation of the processes determining stratocumulus cloud microphysical and radiative properties and their transition to cumulus regimes; (3) to challenge, validate, and improve satellite retrievals of cloud and aerosol properties and their radiative impacts; (4) to improve the impacts of aerosols in weather and climate numerical models. This paper describes the modelling and measurement strategies central to the CLARIFY-2017 deployment of the FAAM BAe146 instrumented aircraft campaign, summarizes the flight objectives and flight patterns, and highlights some key results from our initial analyses.


Cloud adjustments dominate the overall negative aerosol radiative effects of biomass burning aerosols in UKESM1 climate model simulations over the south-eastern Atlantic

Atmospheric Chemistry and Physics Copernicus Publications 21 (2021) 17-33

H Che, P Stier, H Gordon, D Watson-Parris, L Deaconu

The South-eastern Atlantic Ocean (SEA) is semi-permanently covered by one of the most extensive stratocumulus cloud decks on the planet and experiences about one-third of the global biomass burning emissions from the southern Africa savannah region during the fire season. To get a better understanding of the impact of these biomass burning aerosols on clouds and radiation balance over the SEA, the latest generation of the UK Earth System Model (UKESM1) is employed. Measurements from the CLARIFY and ORACLES flight campaigns are used to evaluate the model, demonstrating that the model has good skill in reproducing the biomass burning plume. To investigate the underlying mechanisms in detail, the effects of biomass burning aerosols on the clouds are decomposed into radiative effects (via absorption and scattering) and microphysical effects (via perturbation of cloud condensation nuclei (CCN) and cloud microphysical processes). The July-August means are used to characterise aerosols, clouds and the radiation balance during the fire season. Results show around 65% of CCN at 0.2% supersaturation in the SEA domain can be attributed to biomass burning. The absorption effect of biomass burning aerosols is the most significant in affecting clouds and radiation. Near the continent, it increases the maximum supersaturation diagnosed by the activation scheme, while further from the continent it reduces the altitude of the maximum supersaturation. As a result, the cloud droplet number concentration responds with a similar pattern to the absorption effect of biomass burning aerosols. The microphysical effect, however, decreases the maximum supersaturation and increases the cloud droplets concentration over the ocean; although this change is relatively small. The liquid water path is also significantly increased over the SEA (mainly caused by the absorption effect of biomass burning aerosols) when biomass burning aerosols are above the stratocumulus cloud deck. The microphysical pathways lead to a slight increase in the liquid water path over the ocean. These changes in cloud properties indicate the significant role of biomass burning aerosols on clouds in this region. Among the effects of biomass burning aerosols on the radiation balance, the semi-direct radiative effects (rapid adjustments induced by biomass burning aerosols radiative effects) have a dominant cooling impact over the SEA, which offset the warming direct radiative effect (radiative forcing from biomass burning aerosol–radiation interactions) and lead to overall net cooling radiative effect in the SEA. However, the magnitude and the sign of the semi-direct effects are sensitive to the relative location of biomass burning aerosols and clouds, reflecting the critical task of the accurate modelling of the biomass burning plume and clouds in this region.


Description and evaluation of aerosol in UKESM1 and HadGEM3-GC3.1 CMIP6 historical simulations

Geoscientific Model Development Copernicus Publications 13 (2020) 6383-6423

C Jones, A Povey, C Scott, A Sellar, S Turnock, M Woodhouse, N Abraham, M Andrews, N Bellouin, J Browse, K Carslaw, M Dalvi, M Glover, D Grosvenor, B Johnson, A Jones, Z Kipling, J Palmiéri, C Reddington, S Rumbold, M Richardson, N Schutgens, P Stier, M Stringer, Y Tang

We document and evaluate the aerosol schemes as implemented in the physical and Earth system models, the Global Coupled 3.1 configuration of the Hadley Centre Global Environment Model version 3 (HadGEM3-GC3.1) and the United Kingdom Earth System Model (UKESM1), which are contributing to the sixth Coupled Model Intercomparison Project (CMIP6). The simulation of aerosols in the present-day period of the historical ensemble of these models is evaluated against a range of observations. Updates to the aerosol microphysics scheme are documented as well as differences in the aerosol representation between the physical and Earth system configurations. The additional Earth system interactions included in UKESM1 lead to differences in the emissions of natural aerosol sources such as dimethyl sulfide, mineral dust and organic aerosol and subsequent evolution of these species in the model. UKESM1 also includes a stratospheric–tropospheric chemistry scheme which is fully coupled to the aerosol scheme, while GC3.1 employs a simplified aerosol chemistry mechanism driven by prescribed monthly climatologies of the relevant oxidants. Overall, the simulated speciated aerosol mass concentrations compare reasonably well with observations. Both models capture the negative trend in sulfate aerosol concentrations over Europe and the eastern United States of America (US) although the models tend to underestimate sulfate concentrations in both regions. Interactive emissions of biogenic volatile organic compounds in UKESM1 lead to an improved agreement of organic aerosol over the US. Simulated dust burdens are similar in both models despite a 2-fold difference in dust emissions. Aerosol optical depth is biased low in dust source and outflow regions but performs well in other regions compared to a number of satellite and ground-based retrievals of aerosol optical depth. Simulated aerosol number concentrations are generally within a factor of 2 of the observations, with both models tending to overestimate number concentrations over remote ocean regions, apart from at high latitudes, and underestimate over Northern Hemisphere continents. Finally, a new primary marine organic aerosol source is implemented in UKESM1 for the first time. The impact of this new aerosol source is evaluated. Over the pristine Southern Ocean, it is found to improve the seasonal cycle of organic aerosol mass and cloud droplet number concentrations relative to GC3.1 although underestimations in cloud droplet number concentrations remain. This paper provides a useful characterisation of the aerosol climatology in both models and will facilitate understanding in the numerous aerosol–climate interaction studies that will be conducted as part of CMIP6 and beyond.


Constraining the Twomey effect from satellite observations: issues and perspectives

ATMOSPHERIC CHEMISTRY AND PHYSICS Copernicus GmbH 20 (2020) 15079-15099

J Quaas, A Arola, B Cairns, M Christensen, H Deneke, AML Ekman, G Feingold, A Fridlind, E Gryspeerdt, O Hasekamp, Z Li, A Lipponen, P-L Ma, J Mulmenstadt, A Nenes, JE Penner, D Rosenfeld, R Schroedner, K Sinclair, O Sourdeval, P Stier, M Tesche, B van Diedenhoven, M Wendisch

© 2020 BMJ Publishing Group. All rights reserved. The Twomey effect describes the radiative forcing associated with a change in cloud albedo due to an increase in anthropogenic aerosol emissions. It is driven by the perturbation in cloud droplet number concentration (1Nd; ant) in liquid-water clouds and is currently understood to exert a cooling effect on climate. The Twomey effect is the key driver in the effective radiative forcing due to aerosol cloud interactions, but rapid adjustments also contribute. These adjustments are essentially the responses of cloud fraction and liquid water path to 1Nd; ant and thus scale approximately with it. While the fundamental physics of the influence of added aerosol particles on the droplet concentration (Nd) is well described by established theory at the particle scale (micrometres), how this relationship is expressed at the large-scale (hundreds of kilometres) perturbation, 1Nd; ant, remains uncertain. The discrepancy between process understanding at particle scale and insufficient quantification at the climate-relevant large scale is caused by co-variability of aerosol particles and updraught velocity and by droplet sink processes. These operate at scales on the order of tens of me-Tres at which only localised observations are available and at which no approach yet exists to quantify the anthropogenic perturbation. Different atmospheric models suggest diverse magnitudes of the Twomey effect even when applying the same anthropogenic aerosol emission perturbation. Thus, observational data are needed to quantify and constrain the Twomey effect. At the global scale, this means satellite data. There are four key uncertainties in determining 1Nd; ant, namely the quantification of (i) the cloud-Active aerosol the cloud condensation nuclei (CCN) concentrations at or above cloud base, (ii) Nd, (iii) the statistical approach for inferring the sensitivity of Nd to aerosol particles from the satellite data and (iv) uncertainty in the anthropogenic perturbation to CCN concentrations, which is not easily accessible from observational data. This review discusses deficiencies of current approaches for the different aspects of the problem and proposes several ways forward: in terms of CCN, retrievals of optical quantities such as aerosol optical depth suffer from a lack of vertical resolution, size and hygroscopicity information, non-direct relation to the concentration of aerosols, difficulty to quantify it within or below clouds, and the problem of insufficient sensitivity at low concentrations, in addition to retrieval errors. A future path forward can include utilising co-located polarimeter and lidar instruments, ideally including high-spectral-resolution lidar capability at two wavelengths to maximise vertically resolved size distribution information content. In terms of Nd, a key problem is the lack of operational retrievals of this quantity and the inaccuracy of the retrieval especially in broken-cloud regimes. As for the Nd-To-CCN sensitivity, key issues are the updraught distributions and the role of Nd sink processes, for which empirical assessments for specific cloud regimes are currently the best solutions. These considerations point to the conclusion that past studies using existing approaches have likely underestimated the true sensitivity and, thus, the radiative forcing due to the Twomey effect.


Constraint on precipitation response to climate change by combination of atmospheric energy and water budgets

npj Climate and Atmospheric Science Springer Nature 3 (2020) 34

G Dagan, P Stier

Global mean precipitation is expected to increase with increasing temperatures, a process which is fairly well understood. In contrast, local precipitation changes, which are key for society and ecosystems, demonstrate a large spread in predictions by climate models, can be of both signs and have much larger magnitude than the global mean change. Previously, two top-down approaches to constrain precipitation changes were proposed, using either the atmospheric water or energy budget. Here, using an ensemble of 27 climate models, we study the relative importance of these two budgetary constraints and present analysis of the spatial scales at which they hold. We show that specific geographical locations are more constrained by either one of the budgets and that the combination of water and energy budgets provides a significantly stronger constraint on the spatial scale of precipitation changes under anthropogenic climate change (on average about 3000 km, above which changes in precipitation approach the global mean change). These results could also provide an objective way to define the scale of ‘regional’ climate change.


Aerosol forcing masks and delays the formation of the North-Atlantic warming hole by three decades

Geophysical Research Letters American Geophysical Union 47 (2020) e2020GL090778

G Dagan, P Stier, D Watson-Parris

The North-Atlantic warming hole (NAWH) is referred to as a reduced warming, or even cooling, of the North-Atlantic during an anthropogenic-driven global warming. A NAWH is predicted by climate models during the 21st century and its pattern is already emerging in observations. Despite the known key role of the North-Atlantic surface temperatures in setting the Northern-Hemisphere climate, the mechanisms behind the NAWH are still not fully understood. Using state-of-the-art climate models, we show that anthropogenic aerosol forcing opposes the formation of the NAWH (by leading to a local warming) and delays its emergence by about 30 years. In agreement with previous studies, we also demonstrate that the relative warming of the North-Atlantic under aerosol forcing is due to changes in ocean heat fluxes, rather than air-sea fluxes. These results suggest that the predicted reduction in aerosol forcing during the 21st century may accelerate the formation of the NAWH.


The Southern Hemisphere midlatitude circulation response to rapid adjustments and sea surface temperature driven feedbacks

Journal of Climate American Meteorological Society 33 (2020) 9673-9690

T Wood, A Maycock, P Forster, T Richardson, T Andrews, O Boucher, G Myhre, B Samset, A Kirkevåg, J Lamarque, J MüLmenstädt, D Olivié, T Takemura, D Watson-Parris

Rapid adjustments-the response of meteorology to external forcing while sea surface temperatures (SST) and sea ice are held fixed-can affect the midlatitude circulation and contribute to long-term forced circulation responses in climate simulations. This study examines rapid adjustments in the Southern Hemisphere (SH) circulation using nine models from the Precipitation Driver and Response Model Intercomparison Project (PDRMIP), which perform fixed SST and coupled ocean experiments for five perturbations: a doubling of carbon dioxide (2xCO2), a tripling of methane (3xCH4), a fivefold increase in sulfate aerosol (5xSO4), a tenfold increase in black carbon aerosol (10xBC), and a 2% increase in solar constant (2%Sol). In the coupled experiments, the SH eddy-driven jet shifts poleward and strengthens for forcings that produce global warming (and vice versa for 5xSO4), with the strongest response found in austral summer. In austral winter, the responses project more strongly onto a change in jet strength. For 10xBC, which induces strong shortwave absorption, the multimodel mean (MMM) rapid adjustment in DJF jet latitude is ∼75% of the change in the coupled simulations. For the other forcings, which induce larger SST changes, the effect of SST-mediated feedbacks on the SH circulation is larger than the rapid adjustment. Nevertheless, for these perturbations the magnitude of the MMM jet shift due to the rapid adjustment is still around 20%-30% of that in the coupled experiments. The results demonstrate the need to understand the mechanisms for rapid adjustments in the midlatitude circulation, in addition to the effect of changing SSTs.


An AeroCom–AeroSat study: intercomparison of satellite AOD datasets for aerosol model evaluation

Atmospheric Chemistry and Physics Copernicus GmbH 20 (2020) 12431-12457

N Schutgens, AM Sayer, A Heckel, C Hsu, H Jethva, G de Leeuw, PJT Leonard, RC Levy, A Lipponen, A Lyapustin, P North, T Popp, C Poulsen, V Sawyer, L Sogacheva, G Thomas, O Torres, Y Wang, S Kinne, M Schulz, P Stier

<jats:p>Abstract. To better understand and characterize current uncertainties in the important observational constraint of climate models of aerosol optical depth (AOD), we evaluate and intercompare 14 satellite products, representing nine different retrieval algorithm families using observations from five different sensors on six different platforms. The satellite products (super-observations consisting of 1∘×1∘ daily aggregated retrievals drawn from the years 2006, 2008 and 2010) are evaluated with AErosol RObotic NETwork (AERONET) and Maritime Aerosol Network (MAN) data. Results show that different products exhibit different regionally varying biases (both under- and overestimates) that may reach ±50 %, although a typical bias would be 15 %–25 % (depending on the product). In addition to these biases, the products exhibit random errors that can be 1.6 to 3 times as large. Most products show similar performance, although there are a few exceptions with either larger biases or larger random errors. The intercomparison of satellite products extends this analysis and provides spatial context to it. In particular, we show that aggregated satellite AOD agrees much better than the spatial coverage (often driven by cloud masks) within the 1∘×1∘ grid cells. Up to ∼50 % of the difference between satellite AOD is attributed to cloud contamination. The diversity in AOD products shows clear spatial patterns and varies from 10 % (parts of the ocean) to 100 % (central Asia and Australia). More importantly, we show that the diversity may be used as an indication of AOD uncertainty, at least for the better performing products. This provides modellers with a global map of expected AOD uncertainty in satellite products, allows assessment of products away from AERONET sites, can provide guidance for future AERONET locations and offers suggestions for product improvements. We account for statistical and sampling noise in our analyses. Sampling noise, variations due to the evaluation of different subsets of the data, causes important changes in error metrics. The consequences of this noise term for product evaluation are discussed. </jats:p>


Overview: The CLoud-Aerosol-Radiation Interaction and Forcing: Year-2017 (CLARIFY-2017) measurement campaign

Atmospheric Chemistry and Physics Discussions European Geosciences Union (2020)

JM Haywood, SJ Abel, P Barrett, N Bellouin, A Blyth, K Bower, M Brooks, K Carslaw, H Che, M Cotterell, N Davies, B Dingley, P Field, H Gordon, M de Graaf, A Jones, J Langridge, F Malavelle, D Partridge, F Peers, J Reedemann, K Szpek, J Taylor, D Watson-Parris, P Zuidema

The representation of clouds, aerosols and cloud-aerosol-radiation impacts remain some of the largest uncertainties in climate change, limiting our ability to accurately reconstruct and predict future climate. The south-east Atlantic is a region where high atmospheric aerosol loadings and semi-permanent stratocumulus clouds are co-located, providing a natural laboratory for studying the full range of aerosol-radiation and aerosol-cloud interactions and their perturbations of the Earth’s radiation budget. While satellite measurements have provided some useful insights into aerosol-radiation and aerosol cloud interactions over the region, these observations do not have the spatial and temporal resolution, nor the required level of precision to allow for a process level assessment. Detailed measurements from high spatial and temporal resolution airborne atmospheric measurements in the region are very sparse, limiting their use in assessing the performance of aerosol modelling in numerical weather prediction and climate models. CLARIFY-2017 was a major consortium programme consisting of 5 principal UK universities with project partners from the UK Met Office and European and USA-based universities and research centres involved in the complementary ORACLES, LASIC and AEROCLO-sA projects. The aims of CLARIFY-2017 were four-fold; (1) to improve the representation and reduce uncertainty in model estimates of the direct, semi-direct and indirect radiative effect of absorbing biomass burning aerosols; (2) improve our knowledge and representation of the processes determining stratocumulus cloud microphysical and radiative properties and their transition to cumulus regimes; (3) challenge, validate and improve satellite retrievals of cloud and aerosol properties and their radiative impacts; (4) improve numerical models of cloud and aerosol and their impacts on radiation, weather and climate. This paper describes the modelling and measurement strategies central to the CLARIFY-2017 deployment of the FAAM BAe146 instrumented aircraft campaign, summarises the flight objectives and flight patterns, and highlights some key results from our initial analyses.


Quantifying the sensitivity of aerosol optical properties to the parameterizations of physico-chemical processes during the 2010 Russian wildfires and heatwave

Atmospheric Chemistry and Physics Copernicus Publications 20 (2020) 9679-9700

L Palacios-Peña, P Stier, R Lorente-Plazas, P Jiménez-Guerrero

The impact of aerosol–radiation and aerosol–cloud interactions on the radiative forcing is subject to large uncertainties. This is caused by the limited understanding of aerosol optical properties and the role of aerosols as cloud condensation/ice nuclei (CCN/IN). On the other hand, aerosol optical properties and vertical distribution are highly related, and their uncertainties come from different processes. This work attempts to quantify the sensitivity of aerosol optical properties (i.e. aerosol optical depth; AOD) and their vertical distribution (using the extinction coefficient, backscatter coefficient, and concentrations' species profiles) to key processes. In order to achieve this objective, sensitivity tests have been carried out, using the WRF-Chem regional fully coupled model by modifying the dry deposition, sub-grid convective transport, relative humidity, and wet scavenging. The 2010 Russian heatwave–wildfires episode has been selected as case study. <br></br> Results indicate that AOD is sensitive to these key processes in the following order of importance: (1) modification of relative humidity, causing AOD differences of up to 0.6; (2) modification of vertical convection transport with AOD differences around −0.4; and (3) the dry deposition with AOD absolute differences of up to −0.35 and 0.3. Moreover, these AOD changes exhibit a nonlinear response. Both an increase and a decrease in the RH result in higher AOD values. On the other hand, both the increase and offset of the sub-grid convective transport lead to a reduction in the AOD over the fire area. In addition, a similar nonlinear response is found when reducing the dry deposition velocity; in particular, for the accumulation mode where the concentration of several species increases (while a decrease might be expected). These nonlinear responses are highly dependent on the equilibrium of the thermodynamics system sulfate–nitrate–SOA (secondary organic aerosol). In this sense, small changes in the concentration of one species can strongly affect others, finally affecting aerosol optical properties. Changes in this equilibrium could come from modifications in relative humidity, dry deposition, or vertical convective transport. By itself, dry deposition also presents a high uncertainty influencing the AOD representation.


The hemispheric contrast in cloud microphysical properties constrains aerosol forcing

Proceedings of the National Academy of Sciences National Academy of Sciences 117 (2020) 18998-19006

IL McCoy, D McCoy, R Wood, L Regayre, D Watson-Parris, DP Grosvenor, JP Mulcahy, Y Hu, FAM Bender, PR Field, KS Carslaw, H Gordon

The change in planetary albedo due to aerosol−cloud interactions during the industrial era is the leading source of uncertainty in inferring Earth’s climate sensitivity to increased greenhouse gases from the historical record. The variable that controls aerosol−cloud interactions in warm clouds is droplet number concentration. Global climate models demonstrate that the present-day hemispheric contrast in cloud droplet number concentration between the pristine Southern Hemisphere and the polluted Northern Hemisphere oceans can be used as a proxy for anthropogenically driven change in cloud droplet number concentration. Remotely sensed estimates constrain this change in droplet number concentration to be between 8 cm−3 and 24 cm−3. By extension, the radiative forcing since 1850 from aerosol−cloud interactions is constrained to be −1.2 W⋅m−2 to −0.6 W⋅m−2. The robustness of this constraint depends upon the assumption that pristine Southern Ocean droplet number concentration is a suitable proxy for preindustrial concentrations. Droplet number concentrations calculated from satellite data over the Southern Ocean are high in austral summer. Near Antarctica, they reach values typical of Northern Hemisphere polluted outflows. These concentrations are found to agree with several in situ datasets. In contrast, climate models show systematic underpredictions of cloud droplet number concentration across the Southern Ocean. Near Antarctica, where precipitation sinks of aerosol are small, the underestimation by climate models is particularly large. This motivates the need for detailed process studies of aerosol production and aerosol−cloud interactions in pristine environments. The hemispheric difference in satellite estimated cloud droplet number concentration implies preindustrial aerosol concentrations were higher than estimated by most models.


Cloudy-sky contributions to the direct aerosol effect

Atmospheric Chemistry and Physics Copernicus GmbH 20 (2020) 8855-8865

G Myhre, BH Samset, CW Mohr, K Alterskjær, Y Balkanski, N Bellouin, M Chin, J Haywood, Ø Hodnebrog, S Kinne, G Lin, MT Lund, JE Penner, M Schulz, N Schutgens, RB Skeie, P Stier, T Takemura, K Zhang

The radiative forcing of the aerosol&#x2013;radiation interaction can be decomposed into clear-sky and cloudy-sky portions. Two sets of multi-model simulations within Aerosol Comparisons between Observations and Models (AeroCom), combined with observational methods, and the time evolution of aerosol emissions over the industrial era show that the contribution from cloudy-sky regions is likely weak. A mean of the simulations considered is 0.01&#xB1;0.1&#x2009;W&#x2009;m&#x2212;2. Multivariate data analysis of results from AeroComPhase&#xA0;II shows that many factors influence the strength of the cloudy-sky contribution to the forcing of the aerosol&#x2013;radiation interaction. Overall, single-scattering albedo of anthropogenic aerosols and the interaction of aerosols with the short-wave cloud radiative effects are found to be important factors. A more dedicated focus on the contribution from the cloud-free and cloud-covered sky fraction, respectively, to the aerosol&#x2013;radiation interaction will benefit the quantification of the radiative forcing and its uncertainty range.


Assessing California wintertime precipitation responses to various climate drivers

Journal of Geophysical Research: Atmospheres American Geophysical Union 125 (2020) e2019JD031736

RJ Allen, J-F Lamarque, D Watson-Parris, D Olivie

Understanding how drivers of climate change affect precipitation remains an important area of research. Although several robust precipitation responses have been identified under continued increases in greenhouse gases (GHGs), considerable uncertainty remains. This is particularly the case at regional scales, including the West Coast of the United States and California. Here, we exploit idealized, single forcing simulations from the Precipitation Driver Response Model Intercomparison Project (PDRMIP) to address how climate drivers impact California wintertime precipitation. Consistent with recent work, GHGs including carbon dioxide and methane, as well as solar forcing, yield a robust increase in California wintertime precipitation. We also find robust California precipitation responses to aerosols but with opposite responses for sulfate versus black carbon aerosol. Sulfate aerosol increases California wintertime precipitation, whereas black carbon reduces it. Moreover, California precipitation is more sensitive to aerosols, particularly regional emissions from Europe and Asia, than to GHGs. These precipitation responses are consistent with shifts in the jet stream and altered moisture fluxes. Although the idealized nature of PDRMIP simulations precludes a formal attribution, our results suggest that aerosols can perturb precipitation and fresh water resources along the West Coast of the United States.


The significant role of biomass burning aerosols in clouds and radiation in the South-eastern Atlantic Ocean

Atmospheric Chemistry and Physics Copernicus Publications (2020)

H Che, P Stier, H Gordon, D Watson-Parris, L Deaconu

The South-eastern Atlantic Ocean (SEA) is semi-permanently covered by one of the most extensive stratocumulus cloud decks on the planet and experiences about one-third of the global biomass burning emissions from the southern Africa savannah region during the fire season. To get a better understanding of the impact of these biomass burning aerosols on clouds and radiation balance over the SEA, the latest generation of the UK Earth System Model (UKESM1) is employed. Measurements from the CLARIFY and ORACLES flight campaigns are used to evaluate the model, demonstrating that the model has good skill in reproducing the biomass burning plume. To investigate the underlying mechanisms in detail, the effects of biomass burning aerosols on the clouds are decomposed into radiative effects (via absorption and scattering) and microphysical effects (via perturbation of cloud condensation nuclei (CCN) and cloud microphysical processes). The July–August means are used to characterise aerosols, clouds and the radiation balance during the fire season. Results show around 68 % of CCN at 0.2 % supersaturation in the SEA domain can be attributed to biomass burning. The absorption effect of biomass burning aerosols is the most significant in affecting clouds and radiation. Near the continent it increases the maximum supersaturation diagnosed by the activation scheme, while further from the continent it reduces the altitude of the maximum supersaturation. As a result, the cloud droplet number concentration shows a similar pattern. The microphysical effect of biomass burning aerosols decreases the maximum supersaturation and increases the cloud droplets concentration over the ocean; however, this change is relatively small. The liquid water path is also significantly increased over the SEA (mainly caused by the absorption effect of biomass burning aerosols) when biomass burning aerosols are above the stratocumulus cloud deck. The microphysical pathways lead to a slight increase in the liquid water path over the ocean. These changes in cloud properties indicate the significant role of biomass burning aerosols on clouds in this region. Among the effects of biomass burning aerosols on radiation balance, the semi-direct radiative effects (rapid adjustments induced by biomass burning aerosols radiative effects) have a dominant cooling impact over the SEA, which offset the warming direct radiative effect (radiative forcing from biomass burning aerosol–radiation interactions). However, the magnitude and the sign of the semi-direct effects are dependent on the relative location of biomass burning aerosols and clouds. The net biomass burning aerosols radiative effect shows a negative cooling effect in the SEA, indicating the significant role of biomass burning aerosols in affecting the regional radiation balance and climate.


Reducing the aerosol forcing uncertainty using observational constraints on warm rain processes

Science Advances (2020)

J Mülmenstädt, C Nam, M Salzmann, J Kretzschmar, TS L’Ecuyer, U Lohmann, P-L Ma, G Myhre, D Neubauer, P STIER, K Suzuki, M Wang, J Quaas


Constraining uncertainty in aerosol direct forcing

Geophysical Research Letters American Geophysical Union 47 (2020) e2020GL087141

D Watson-Parris, N Bellouin, L Deaconu, N Schutgens, M Yoshioka, L Regayre, K Pringle, J Johnson, C Smith, K Carslaw, P Stier

The uncertainty in present-day anthropogenic forcing is dominated by uncertainty in the strength of the contribution from aerosol. Much of the uncertainty in the direct aerosol forcing can be attributed to uncertainty in the anthropogenic fraction of aerosol in the present-day atmosphere, due to a lack of historical observations. Here we present a robust relationship between total present-day aerosol optical depth and the anthropogenic contribution across three multi-model ensembles and a large single-model perturbed parameter ensemble. Using observations of aerosol optical depth, we determine a reduced likely range of the anthropogenic component and hence a reduced uncertainty in the direct forcing of aerosol.


Constraining the Twomey effect from satellite observations: issues and perspectives

Atmospheric Chemistry and Physics Discussions European Geosciences Union 20 (2020) 23

J Quaas, A Antti, B Cairns, M Christensen, H Deneke, AML Ekman, G Feingold, A Fridlind, E Gryspeerdt, O Hasekamp, Z Li, A Lipponen, P-L Ma, J Muelmenstaedt, A Nenes, J Penner, D Rosenfeld, R Schroedner, K Sinclair, O Sourdeval, P Stier, M Tesche, B van Dieedenhoven, M Wendisch

The Twomey effect describes the radiative forcing associated with a change in cloud albedo due to an increase in anthropogenic aerosol emissions. It is driven by the perturbation in cloud droplet number concentration (ΔNd, ant) in liquid-water clouds and is currently understood to exert a cooling effect on climate. The Twomey effect is the key driver in the effective radiative forcing due to aerosol–cloud interactions, but rapid adjustments also contribute. These adjustments are essentially the responses of cloud fraction and liquid water path to ΔNd, ant and thus scale approximately with it. While the fundamental physics of the influence of added aerosol particles on the droplet concentration (Nd) is well described by established theory at the particle scale (micrometres), how this relationship is expressed at the large-scale (hundreds of kilometres) perturbation, ΔNd, ant, remains uncertain. The discrepancy between process understanding at particle scale and insufficient quantification at the climate-relevant large scale is caused by co-variability of aerosol particles and updraught velocity and by droplet sink processes. These operate at scales on the order of tens of metres at which only localised observations are available and at which no approach yet exists to quantify the anthropogenic perturbation. Different atmospheric models suggest diverse magnitudes of the Twomey effect even when applying the same anthropogenic aerosol emission perturbation. Thus, observational data are needed to quantify and constrain the Twomey effect. At the global scale, this means satellite data. There are four key uncertainties in determining ΔNd, ant, namely the quantification of (i) the cloud-active aerosol – the cloud condensation nuclei (CCN) concentrations at or above cloud base, (ii) Nd, (iii) the statistical approach for inferring the sensitivity of Nd to aerosol particles from the satellite data and (iv) uncertainty in the anthropogenic perturbation to CCN concentrations, which is not easily accessible from observational data. This review discusses deficiencies of current approaches for the different aspects of the problem and proposes several ways forward: in terms of CCN, retrievals of optical quantities such as aerosol optical depth suffer from a lack of vertical resolution, size and hygroscopicity information, non-direct relation to the concentration of aerosols, difficulty to quantify it within or below clouds, and the problem of insufficient sensitivity at low concentrations, in addition to retrieval errors. A future path forward can include utilising co-located polarimeter and lidar instruments, ideally including high-spectral-resolution lidar capability at two wavelengths to maximise vertically resolved size distribution information content. In terms of Nd, a key problem is the lack of operational retrievals of this quantity and the inaccuracy of the retrieval especially in broken-cloud regimes. As for the Nd-to-CCN sensitivity, key issues are the updraught distributions and the role of Nd sink processes, for which empirical assessments for specific cloud regimes are currently the best solutions. These considerations point to the conclusion that past studies using existing approaches have likely underestimated the true sensitivity and, thus, the radiative forcing due to the Twomey effect.

Pages