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.

The total effect of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in anthropogenic radiative forcing on the climate. Correct characterization of intensive aerosol optical properties, particularly in conditions where absorbing aerosol is present, is a crucial factor in quantifying these effects. The southeast Atlantic Ocean (SEA), with seasonal biomass burning smoke plumes overlying and mixing with a persistent stratocumulus cloud deck, offers an excellent natural laboratory to make the observations necessary to understand the complexities of aerosol-cloud-radiation interactions. The first field deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in September of 2016 out of Walvis Bay, Namibia.Data collected during ORACLES-2016 are used to derive aerosol properties from an unprecedented number of simultaneous measurement techniques over this region. Here, we present results from six of the eight independent instruments or instrument combinations, all applied to measure or retrieve aerosol absorption and single-scattering albedo. Most but not all of the biomass burning aerosol was located in the free troposphere, in relative humidities typically ranging up to 60 %. We present the single-scattering albedo (SSA), absorbing and total aerosol optical depth (AAOD and AOD), and absorption, scattering, and extinction Ångström exponents (AAE, SAE, and EAE, respectively) for specific case studies looking at near-coincident and near-colocated measurements from multiple instruments, and SSAs for the broader campaign average over the month-long deployment. For the case studies, we find that SSA agrees within the measurement uncertainties between multiple instruments, though, over all cases, there is no strong correlation between values reported by one instrument and another. We also find that agreementPublished by Copernicus Publications on behalf of the European Geosciences Union. 9182 K. Pistone et al.: Biomass burning SSA intercomparisonbetween the instruments is more robust at higher aerosol loading (AOD 400 > 0.4).The campaign-wide average and range shows differences in the values measured by each instrument. We find the ORACLES-2016 campaign-average SSA at 500 nm (SSA 500 ) to be between 0.85 and 0.88, depending on the instrument considered (4STAR, AirMSPI, or in situ measurements), with the interquartile ranges for all instruments between 0.83 and 0.89. This is consistent with previous September values reported over the region (between 0.84 and 0.90 for SSA at 550nm). The results suggest that the differences observed in the campaign-average values may be dominated by instrument-specific spatial sampling differences and the natural physical variability in aerosol conditions over the SEA, rather than fundamental methodological differences.

Abstract. Nine Pandora spectrometer instruments (PSI) were installed at eight sites in South Korea as part of the KORUS-AQ (Korea U.S.-Air Quality) field study integrating information from ground, aircraft, and satellite measurements for validation of remote sensing air-quality studies. The PSI made direct-sun measurements of total vertical column NO 2 , C(NO 2 ), with high precision (0.05 DU, where 1 DU = 2.69 × 10 16 molecules cm −2 ) and accuracy (0.1 DU) that were retrieved using spectral fitting techniques. Retrieval of formaldehyde C(HCHO) total column amounts were also obtained at five sites using the recently improved PSI optics. The C(HCHO) retrievals have high precision, but possibly lower accuracy than for NO 2 because of uncertainty about the optimum spectral window for all ground-based and satellite instruments. PSI direct-sun retrieved values for C(NO 2 ) and C(HCHO) are always significantly larger than OMI (AURA satellite Ozone Monitoring Instrument) retrieved C(NO 2 ) and C(HCHO) for the OMI overpass local times (KST = 13.5 ± 0.5 h). In urban areas, PSI C(NO 2 ) 30-day running averages are at least a factor of two larger than OMI averages. Similar differences are seen for C(HCHO) in Seoul and nearby surrounding areas. Late afternoon values of C(HCHO) measured by PSI are even larger, implying that OMI early afternoon measurements underestimate the effect of poor air quality on human health. The primary cause of OMI underestimates is the large OMI field of view (FOV) that includes regions containing low values of pollutants. In relatively clean areas, PSI and OMI are more closely in agreement. C(HCHO) amounts were obtained for five sites,

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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 five-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 South-East Atlantic, where they interact with one of the largest subtropical stratocumulus 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, and 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 questions centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects; (b) effects of aerosol absorption on atmospheric circulation and clouds; (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 data set it produced.

Abstract. Determining the direct aerosol radiative effect (DARE) of absorbing aerosols above clouds from satellite observations alone is a challenging task, in part because the radiative signal of the aerosol layer is not easily untangled from that of the clouds below. In this study, we use aircraft measurements from the NASA ObseRvations of CLouds above Aerosols and their intEractionS (ORACLES) project in the southeastern Atlantic to derive it with as few assumptions as possible. This is accomplished by using spectral irradiance measurements (Solar Spectral Flux Radiometer, SSFR) and aerosol optical depth (AOD) retrievals (Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research, 4STAR) during vertical profiles (spirals) that minimize the albedo variability of the underlying cloud field – thus isolating aerosol radiative effects from those of the cloud field below. For two representative cases, we retrieve spectral aerosol single scattering albedo (SSA) and the asymmetry parameter (g) from these profile measurements and calculate DARE given the albedo range measured by SSFR on horizontal legs above clouds. For mid-visible wavelengths, we find SSA values from 0.80 to 0.85 and a significant spectral dependence of g. As the cloud albedo increases, the aerosol increasingly warms the column. The transition from a cooling to a warming top-of-aerosol radiative effect occurs at an albedo value (critical albedo) just above 0.2 in the mid-visible wavelength range. In a companion paper, we use the techniques introduced here to generalize our findings to all 2016 and 2017 measurements and parameterize aerosol radiative effects.

The flow rate of the Lower Jordan River has changed dramatically during the second half of the 20th century. The diversion of its major natural sources reduced its flow rate and led to drying events during the drought years of 2000 and 2001. Under these conditions of low flow rates, the potential influence of external sources on the river discharge and chemical composition became significant. Our measurements show that the concentrations of chloride, calcium, and sodium in the river water decrease along the first 20-km section, while sulfate and magnesium concentrations increase. These variations were addressed by a recent geochemical study, suggesting that ground water inflow plays a major role. To further examine the role of ground water, we applied mass-balance calculations, using detailed flow rate measurements, water samplings, and chemical analyses along the northern (upstream) part of the river. Our flow-rate measurements showed that the river base-flow during 2000 and 2001 was 500 to 1100 L s(-1), which is about 40 times lower than the historical flow rates. Our measurements and calculations indicate that ground water input was 20 to 80% of the river water flow, and 20 to 50% of its solute mass flow. This study independently identifies the composition of possible end-members. These end-members contain high sulfate concentration and have similar chemical characteristics as were found in agricultural drains and in the "saline" Yarmouk River. Future regional development plans that include the river flow rate and chemistry should consider the interactions between the river and its shallow ground water system.

Abstract. In southern Africa, widespread agricultural fires produce substantial biomass burning (BB) emissions over the region. The seasonal smoke plumes associated with these emissions are then advected westward over the persistent stratocumulus cloud deck in the southeast Atlantic (SEA) Ocean, resulting in aerosol effects which vary with time and location. Much work has focused on the effects of these aerosol plumes, but previous studies have also described an elevated free tropospheric water vapor signal over the SEA. Water vapor influences climate in its own right, and it is especially important to consider atmospheric water vapor when quantifying aerosol–cloud interactions and aerosol radiative effects. Here we present airborne observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign over the SEA Ocean. In observations collected from multiple independent instruments on the NASA P-3 aircraft (from near-surface to 6–7 km), we observe a strongly linear correlation between pollution indicators (carbon monoxide (CO) and aerosol loading) and atmospheric water vapor content, seen at all altitudes above the boundary layer. The focus of the current study is on the especially strong correlation observed during the ORACLES-2016 deployment (out of Walvis Bay, Namibia), but a similar relationship is also observed in the August 2017 and October 2018 ORACLES deployments. Using reanalyses from the European Centre for Medium-Range Weather Forecasts (ECMWF) and Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), and specialized WRF-Chem simulations, we trace the plume–vapor relationship to an initial humid, smoky continental source region, where it mixes with clean, dry upper tropospheric air and then is subjected to conditions of strong westward advection, namely the southern African easterly jet (AEJ-S). Our analysis indicates that air masses likely left the continent with the same relationship between water vapor and carbon monoxide as was observed by aircraft. This linear relationship developed over the continent due to daytime convection within a deep continental boundary layer (up to ∼5–6 km) and mixing with higher-altitude air, which resulted in fairly consistent vertical gradients in CO and water vapor, decreasing with altitude and varying in time, but this water vapor does not originate as a product of the BB combustion itself. Due to a combination of conditions and mixing between the smoky, moist continental boundary layer and the dry and fairly clean upper-troposphere air above (∼6 km), the smoky, humid air is transported by strong zonal winds and then advected over the SEA (to the ORACLES flight region) following largely isentropic trajectories. Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT) back trajectories support this interpretation. This work thus gives insights into the conditions and processes which cause water vapor to covary with plume strength. Better understanding of this relationship, including how it varies spatially and temporally, is important to accurately quantify direct, semi-direct, and indirect aerosol effects over this region.