Cloud drop condensation nuclei (CCN) and ice nuclei (IN) particles determine to a large extent cloud microstructure and, consequently, cloud albedo and the dynamic response of clouds to aerosol-induced changes to precipitation. This can modify the reflected solar radiation and the thermal radiation emitted to space. Measurements of tropospheric CCN and IN over large areas have not been possible and can be only roughly approximated from satellite-sensor-based estimates of optical properties of aerosols. Our lack of ability to measure both CCN and cloud updrafts precludes disentangling the effects of meteorology from those of aerosols and represents the largest component in our uncertainty in anthropogenic climate forcing. Ways to improve the retrieval accuracy include multiangle and multipolarimetric passive measurements of the optical signal and multispectral lidar polarimetric measurements. Indirect methods include proxies of trace gases, as retrieved by hyperspectral sensors. Perhaps the most promising emerging direction is retrieving the CCN properties by simultaneously retrieving convective cloud drop number concentrations and updraft speeds, which amounts to using clouds as natural CCN chambers. These satellite observations have to be constrained by in situ observations of aerosol-cloud-precipitation-climate (ACPC) interactions, which in turn constrain a hierarchy of model simulations of ACPC. Since the essence of a general circulation model is an accurate quantification of the energy and mass fluxes in all forms between the surface, atmosphere and outer space, a route to progress is proposed here in the form of a series of box flux closure experiments in the various climate regimes. A roadmap is provided for quantifying the ACPC interactions and thereby reducing the uncertainty in anthropogenic climate forcing.

We present an overview of the background, scientific goals, and execution of the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project of April 2008. We then summarize airborne measurements, made in the troposphere of the Alaskan Arctic, of aerosol particle size distributions, composition, and optical properties and discuss the sources and transport of the aerosols. The aerosol data were grouped into four categories based on gas-phase composition. First, the background troposphere contained a relatively diffuse, sulfate-rich aerosol extending from the top of the sea-ice inversion layer to 7.4 km altitude. Second, a region of depleted (relative to the background) aerosol was present within the surface inversion layer over sea-ice. Third, layers of dense, organic-rich smoke from open biomass fires in southern Russia and southeastern Siberia were frequently encountered at all altitudes from the top of the inversion layer to 7.1 km. Finally, some aerosol layers were dominated by components originating from fossil fuel combustion. <br></br> Of these four categories measured during ARCPAC, the diffuse background aerosol was most similar to the average springtime aerosol properties observed at a long-term monitoring site at Barrow, Alaska. The biomass burning (BB) and fossil fuel layers were present above the sea-ice inversion layer and did not reach the sea-ice surface during the course of the ARCPAC measurements. The BB aerosol layers were highly scattering and were moderately hygroscopic. On average, the layers produced a noontime net heating of ~0.1 K day^&minus;1 between 3 and 7 km and a slight cooling at the surface. The ratios of particle mass to carbon monoxide (CO) in the BB plumes, which had been transported over distances >5000 km, were comparable to the high end of literature values derived from previous measurements in wildfire smoke. These ratios suggest minimal precipitation scavenging and removal of the BB particles between the time they were emitted and the time they were observed in dense layers above the sea-ice inversion layer

Atmospheric iodine monoxide (IO) is a radical that catalytically destroys heat trapping ozone and reacts further to form aerosols. Here, we report the detection of IO in the tropical free troposphere (FT). We present vertical profiles from airborne measurements over the Pacific Ocean that show significant IO up to 9.5 km altitude and locate, on average, two-thirds of the total column above the marine boundary layer. IO was observed in both recent deep convective outflow and aged free tropospheric air, suggesting a widespread abundance in the FT over tropical oceans. Our vertical profile measurements imply that most of the IO signal detected by satellites over tropical oceans could originate in the FT, which has implications for our understanding of iodine sources. Surprisingly, the IO concentration remains elevated in a transition layer that is decoupled from the ocean surface. This elevated concentration aloft is difficult to reconcile with our current understanding of iodine lifetimes and may indicate heterogeneous recycling of iodine from aerosols back to the gas phase. Chemical model simulations reveal that the iodine-induced ozone loss occurs mostly above the marine boundary layer (34%), in the transition layer (40%) and FT (26%) and accounts for up to 20% of the overall tropospheric ozone loss rate in the upper FT. Our results suggest that the halogen-driven ozone loss in the FT is currently underestimated. More research is needed to quantify the widespread impact that iodine species of marine origin have on free tropospheric composition, chemistry, and climate.atmospheric chemistry | oxidative capacity | halogens | heterogeneous chemistry | air-sea exchange R eactive iodine impacts atmospheric chemistry in several ways. Catalytic reaction cycles involving iodine atoms and iodine monoxide (IO; I x = I + IO) destroy tropospheric ozone, which is a primary source for OH radicals (1, 2). Halogens contribute ∼45% of the ozone loss in the remote tropical marine boundary layer (MBL) (2-4). IO further affects the oxidative capacity of the atmosphere through fast reactions with HO 2 radicals and the resulting changes in HO x (HO x = OH + HO 2 ) (1, 2). Iodine also affects NO x (NO x = NO + NO 2 ) by oxidizing NO to NO 2 (1-4). Additionally, bromine atom recycling by IO increases ozone destruction and mercury oxidation rates in the MBL, resulting in higher mercury deposition rates to ecosystems and increased availability to the food chain (2, 5, 6). Finally, in coastal regions, the formation of ultrafine aerosol particles from iodine oxides can be a source of cloud condensation nuclei that can modify Earth's albedo and thus, the radiative budget of the atmosphere (2, 7).Oceans are the main source of iodine to the atmosphere. Most current knowledge of iodine sources and chemistry is based on measurements in the MBL (3,(8)(9)(10)(11)(12)(13). IO observations at coastal MBL sites primarily link iodine sources to macroalgae (8-10). More recent studies have measured IO at open ocean sites (3, 11-13), suggesting that ther...

Abstract. We introduce a new spectral method for the retrieval of optical thickness and effective radius from cloud transmittance that relies on the spectral slope of the normalized transmittance between 1565 nm and 1634 nm, and on cloud transmittance at a visible wavelength. The standard dual-wavelength technique, which is traditionally used in reflectance-based retrievals, is ill-suited for transmittance because it lacks sensitivity to effective radius, especially for optically thin clouds. Using the spectral slope rather than the transmittance itself enhances the sensitivity of transmittance observations with respect to the effective radius. This is demonstrated by applying it to the moderate spectral resolution observations from the Solar Spectral Flux Radiometer (SSFR) and Shortwave Spectroradiometer (SWS), and by examining the retrieval uncertainties of the standard and the spectral method for data from the DOE ARM Southern Great Plains (SGP) site and a NOAA ship cruise (ICEALOT). The liquid water path (LWP) is derived from the retrieved optical thickness and effective radius, based on two different assumptions about the cloud vertical profile, and compared to the simultaneous observations from a microwave radiometer. Optical thickness and effective radius is also compared to MODIS retrievals. In general, the effective radius uncertainties were much larger for the standard retrieval than for the spectral retrieval, particularly for thin clouds. When defining 2 µm as upper limit for the tolerable uncertainty of the effective radius, the standard method returned only very few valid retrievals for clouds with an optical thickness below 25. For the analyzed ICEALOT data (mean optical thickness 23), the Correspondence to: P. J. McBride (patrick.mcbride@colorado.edu) spectral method provided valid retrievals for 84 % of the data (24 % for the standard method). For the SGP data (mean optical thickness 44), both methods provided a high return of 90 % for the spectral method and 78 % for the standard method.

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[1] Haywood et al. (2004) show that an aerosol layer above a cloud can cause a bias in the retrieved cloud optical thickness and effective radius. Monitoring for this potential bias is difficult because space-based passive remote sensing cannot unambiguously detect or characterize aerosol above cloud. We show that cloud retrievals from aircraft measurements above cloud and below an overlying aerosol layer are a means to test this bias. The data were collected during the Intercontinental Chemical Transport Experiment (INTEX-A) study based out of Portsmouth, New Hampshire, United States, above extensive, marine stratus cloud banks affected by industrial outflow. Solar Spectral Flux Radiometer (SSFR) irradiance measurements taken along a lower level flight leg above cloud and below aerosol were unaffected by the overlying aerosol. Along upper level flight legs, the irradiance reflected from cloud top was transmitted through an aerosol layer. We compare SSFR cloud retrievals from below-aerosol legs to satellite retrievals from the Moderate Resolution Imaging Spectroradiometer (MODIS) in order to detect an aerosol-induced bias. In regions of small variation in cloud properties, we find that SSFR and MODIS-retrieved cloud optical thickness compares within the uncertainty range for each instrument while SSFR effective radius tend to be smaller than MODIS values (by 1-2 mm) and at the low end of MODIS uncertainty estimates. In regions of large variation in cloud properties, differences in SSFR and MODIS-retrieved cloud optical thickness and effective radius can reach values of 10 and 10 mm, respectively. We include aerosols in forward modeling to test the sensitivity of SSFR cloud retrievals to overlying aerosol layers. We find an overlying absorbing aerosol layer biases SSFR cloud retrievals to smaller effective radii and optical thickness while nonabsorbing aerosols had no impact.

[1] Airborne measurements of the ratio of spectral upward and downward irradiances (so-called spectral albedo) are used to derive the areal spectral surface albedo in the wavelength range from 330 to 1670 nm. The data were collected over different sea and land surfaces in cloudless atmospheric conditions during three field campaigns. Measurements from the Albedometer (developed at IfT) and the NASA Solar Spectral Flux Radiometer (SSFR) are employed. Spectral radiative transfer calculations show that atmospheric scattering and absorption within the layer beneath the flight level considerably contribute to the airborne albedo measurements reported here, even for low flight altitudes (0.2-0.5 km). To remove this atmospheric masking, a nonlinear extrapolation of the airborne albedo measurements to the ground is performed. The nonlinearity is due to the vertically inhomogeneous distribution of the particle microphysical properties. This fact underlines the importance of aerosol profile measurements for the proper correction of atmospheric masking. Examples of the extrapolated areal spectral surface albedos are discussed in terms of their solar zenith angle dependence, their small-scale, and general variability. Finally, typical areal spectral surface albedos for different sea and land surfaces, as derived from the three measurement campaigns, are supplied in parameterized form for use in radiative transfer applications.

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.