Summary (149 words of referenced text): 46The climate impact of aerosols is highly uncertain owing primarily to their poorly quantified 47 influence on cloud properties. During 2014-15, a fissure eruption in Holuhraun (Iceland) 48 emitted huge quantities of sulphur dioxide, resulting in significant reductions in liquid cloud 49 droplet size. Using satellite observations and detailed modelling, we estimate a global mean 50 radiative forcing from the resulting aerosol-induced cloud brightening for the time of the 51 eruption of around -0.2 W.m -2 . Changes in cloud amount or liquid water path are 52 undetectable, indicating that these aerosol-cloud indirect effects are modest. It supports the 53 idea that cloud systems are well buffered against aerosol changes as only impacts on cloud 54 effective radius appear relevant from a climate perspective, thus providing a strong constraint 55 on aerosol-cloud interactions. This result will reduce uncertainties in future climate 56 projections as we are able to reject the results from climate models with an excessive liquid 57 water path response. 58 59Main Text: (3103 words of referenced text, including concluding paragraph) 60 The 2014-15 eruption at Holuhraun (486 words of referenced text): 61Anthropogenic emissions that affect climate are not just confined to greenhouse gases. 62Sulphur dioxide and other pollutants form atmospheric aerosols that can scatter and absorb 63 sunlight and can influence the properties of clouds, modulating the Earth-atmosphere energy 64 balance. Aerosols act as cloud condensation nuclei (CCN); an increase in CCN translates into 65 a higher number of smaller, more reflective cloud droplets that scatter more sunlight back to 66 space 1 (the ÔfirstÕ indirect effect of aerosols). Smaller cloud droplets decrease the efficiency 67 of collision-coalescence processes that are pivotal in rain initiation, thus aerosol-influenced 68 clouds may retain more liquid water and extend coverage/lifetime 2,3 (the ÔsecondÕ or Ôcloud 69 lifetimeÕ indirect effect). Aerosols usually co-vary with key environmental variables making 70 it difficult to disentangle aerosol-cloud impacts from meteorological variability [4][5][6] . 71Additionally, clouds themselves are complex transient systems subject to dynamical 72 feedbacks (e.g. cloud top entrainment/evaporation, invigoration of convection) which 73 influence cloud response [7][8][9][10][11][12] . These aspects present great challenges in evaluating and 74 constraining aerosol-cloud interactions (ACI) in General Circulation Models (GCM) 13-17 , 75 with particular contentious debate surrounding the relative importance of these feedback 76 mechanisms. 77Nonetheless, anthropogenic aerosol emissions are thought to cool the Earth via indirect 78 effects 17 , but the uncertainty ranges from -1.2 to -0.0 W.m -2 (90% confidence interval) due to 79 i) a lack of characterization of the pre-industrial aerosol state 15,18,19 , and ii) model parametric 80 and structural errors in representing cloud responses to aerosol chan...

Abstract. In situ measurements of ice crystal concentrations and sizes made with aircraft instrumentation over the past two decades have often indicated the presence of numerous relatively small (< 50 µm diameter) crystals in cirrus clouds. Further, these measurements frequently indicate that small crystals account for a large fraction of the extinction in cirrus clouds. The fact that the instruments used to make these measurements, such as the Forward Scattering Spectrometer Probe (FSSP) and the Cloud Aerosol Spectrometer (CAS), ingest ice crystals into the sample volume through inlets has led to suspicion that the indications of numerous small-crystals could be artifacts of large-crystal shattering on the instrument inlets. We present new aircraft measurements in anvil cirrus sampled during the Tropical Composition, Cloud, and Climate Coupling (TC4) campaign with the 2-Dimensional Stereo (2D-S) probe, which detects particles as small as 10 µm. The 2D-S has detector "arms" instead of an inlet tube. Since the 2D-S probe surfaces are much further from the sample volume than is the case for the instruments with inlets, it is expected that 2D-S will be less susceptible to shattering artifacts. In addition, particle interarrival times are used to identify and remove shattering artifacts that occur even with the 2D-S probe. The number of shattering artifacts identified by the 2D-S interarrival time analysis ranges from a negligible contribution to an order of magnitude or more enhancement in apparent ice concentration over the natural ice concentration, depending on the abundance of large crystals and the natural small-crystal concentration. The 2D-S measurements in tropical anvil cirrus suggest that natural small-crystal concentrations are typically one to two orders of magnitude lower than those inferred from CAS. The strong correlation between the CAS/2D-S raCorrespondence to: E. J. Jensen (eric.j.jensen@nasa.gov) tio of small-crystal concentrations and large-crystal concentration suggests that the discrepancy is likely caused by shattering of large crystals on the CAS inlet. We argue that past measurements with CAS in cirrus with large crystals present may contain errors due to crystal shattering, and past conclusions derived from these measurements may need to be revisited. Further, we present correlations between CAS spurious concentration and 2D-S large-crystal mass from spatially uniform anvil cirrus sampling periods as an approximate guide for estimating quantitative impact of large-crystal shattering on CAS concentrations in previous datasets. We use radiative transfer calculations to demonstrate that in the maritime anvil cirrus sampled during TC4, small crystals indicated by 2D-S contribute relatively little cloud extinction, radiative forcing, or radiative heating in the anvils, regardless of anvil age or vertical location in the clouds. While 2D-S ice concentrations in fresh anvil cirrus may often exceed 1 cm −3 , and are observed to exceed 10 cm −3 in turrets, they are typically 0.1 cm −3 and rarely ex...

The regional haze over the southeast (SE) Atlantic Ocean induced by biomass burning in southern Africa can be problematic for passive imager-based retrievals of the underlying quasi-permanent marine boundary layer (MBL) clouds and for estimates of top-of-atmosphere (TOA) aerosol direct radiative effect (DRE). Here an algorithm is introduced to simultaneously retrieve above-cloud aerosol optical thickness (AOT), the cloud optical thickness (COT), and cloud effective particle radius (CER) of the underlying MBL clouds while also providing pixel-level estimates of retrieval uncertainty. This approach utilizes reflectance measurements at six Moderate Resolution Imaging Spectroradiometer (MODIS) channels from the visible to the shortwave infrared. Retrievals are run under two aerosol model assumptions on 8 years (2006)(2007)(2008)(2009)(2010)(2011)(2012)(2013) of June-October Aqua MODIS data over the SE Atlantic, from which a regional cloud and above-cloud aerosol climatology is produced. The cloud retrieval methodology is shown to yield COT and CER consistent with those from the MODIS operational cloud product (MOD06) when forcing AOT to zero, while the full COT-CER-AOT retrievals that account for the above-cloud aerosol attenuation increase regional monthly mean COT and CER by up to 9% and 2%, respectively. Retrieved AOT is roughly 3 to 5 times larger than the collocated 532 nm Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) retrievals, though closer agreement is observed with the CALIOP 1064 nm retrievals, a result consistent with previous case study analyses. Regional cloudy-sky above-cloud aerosol DRE calculations are also performed that illustrate the importance of the aerosol model assumption and underlying cloud retrievals.

The Atlantic Multidecadal Oscillation (AMO) is characterized by a horseshoe pattern of sea surface temperature (SST) anomalies and has a wide range of climatic impacts. While the tropical arm of AMO is responsible for many of these impacts, it is either too weak or completely absent in many climate model simulations. Here we show, using both observational and model evidence, that the radiative effect of positive low cloud and dust feedbacks is strong enough to generate the tropical arm of AMO, with the low cloud feedback more dominant. The feedbacks can be understood in a consistent dynamical framework: weakened tropical trade wind speed in response to a warm middle latitude SST anomaly reduces dust loading and low cloud fraction over the tropical Atlantic, which warms the tropical North Atlantic SST. Together they contribute to the appearance of the tropical arm of AMO. Most current climate models miss both the critical wind speed response and two positive feedbacks though realistic simulations of them may be essential for many climatic studies related to the AMO.

Moderate Resolution Imaging Spectroradiometer (MODIS) retrieves cloud droplet effective radius (r e) and optical thickness (τ) by projecting observed cloud reflectances onto a precomputed look‐up table (LUT). When observations fall outside of the LUT, the retrieval is considered “failed” because no combination of τ and r e within the LUT can explain the observed cloud reflectances. In this study, the frequency and potential causes of failed MODIS retrievals for marine liquid phase (MLP) clouds are analyzed based on 1 year of Aqua MODIS Collection 6 products and collocated CALIOP and CloudSat observations. The retrieval based on the 0.86 µm and 2.1 µm MODIS channel combination has an overall failure rate of about 16% (10% for the 0.86 µm and 3.7 µm combination). The failure rates are lower over stratocumulus regimes and higher over the broken trade wind cumulus regimes. The leading type of failure is the “r e too large” failure accounting for 60%–85% of all failed retrievals. The rest is mostly due to the “r e too small” or τ retrieval failures. Enhanced retrieval failure rates are found when MLP cloud pixels are partially cloudy or have high subpixel inhomogeneity, are located at special Sun‐satellite viewing geometries such as sunglint, large viewing or solar zenith angles, or cloudbow and glory angles, or are subject to cloud masking, cloud overlapping, and/or cloud phase retrieval issues. The majority (more than 84%) of failed retrievals along the CALIPSO track can be attributed to at least one or more of these potential reasons. The collocated CloudSat radar reflectivity observations reveal that the remaining failed retrievals are often precipitating. It remains an open question whether the extremely large r e values observed in these clouds are the consequence of true cloud microphysics or still due to artifacts not included in this study.

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The bispectral method retrieves cloud optical thickness (τ) and cloud droplet effective radius (re) simultaneously from a pair of cloud reflectance observations, one in a visible or near‐infrared (VIS/NIR) band and the other in a shortwave infrared (SWIR) band. A cloudy pixel is usually assumed to be horizontally homogeneous in the retrieval. Ignoring subpixel variations of cloud reflectances can lead to a significant bias in the retrieved τ and re. In the literature, the retrievals of τ and re are often assumed to be independent and considered separately when investigating the impact of subpixel cloud reflectance variations on the bispectral method. As a result, the impact on τ is contributed only by the subpixel variation of VIS/NIR band reflectance and the impact on re only by the subpixel variation of SWIR band reflectance. In our new framework, we use the Taylor expansion of a two‐variable function to understand and quantify the impacts of subpixel variances of VIS/NIR and SWIR cloud reflectances and their covariance on the τ and re retrievals. This framework takes into account the fact that the retrievals are determined by both VIS/NIR and SWIR band observations in a mutually dependent way. In comparison with previous studies, it provides a more comprehensive understanding of how subpixel cloud reflectance variations impact the τ and re retrievals based on the bispectral method. In particular, our framework provides a mathematical explanation of how the subpixel variation in VIS/NIR band influences the re retrieval and why it can sometimes outweigh the influence of variations in the SWIR band and dominate the error in re retrievals, leading to a potential contribution of positive bias to the re retrieval. We test our framework using synthetic cloud fields from a large‐eddy simulation and real observations from Moderate Resolution Imaging Spectroradiometer. The predicted results based on our framework agree very well with the numerical simulations. Our framework can be used to estimate the retrieval uncertainty from subpixel reflectance variations in operational satellite cloud products and to help understand the differences in τ and re retrievals between two instruments.

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.