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Due to their fast evolution and large natural variability in macro- and microphysical properties, the accurate representation of boundary layer clouds in current climate models remains a challenge. One of the regions with large intermodel spread in the Coupled Model Intercomparison Project Phase 6 ensemble is the western North Atlantic Ocean. Here, statistically representative in situ measurements can help to develop and constrain the parameterization of clouds in global models. To this end, we performed comprehensive measurements of boundary layer clouds, aerosol, trace gases, and radiation in the western North Atlantic Ocean during the NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) mission. In total, 174 research flights with 574 flight hours for cloud and precipitation measurements were performed with the HU-25 Falcon during three winter (February–March 2020, January–April 2021, and November 2021–March 2022) and three summer seasons (August–September 2020, May–June 2021, and May–June 2022). Here we present a statistical evaluation of 16 140 individual cloud events probed by the fast cloud droplet probe and the two-dimensional stereo cloud probe during 155 research flights in a representative and repetitive flight strategy allowing for robust statistical data analyses. We show that the vertical profiles of distributions of the liquid water content and the cloud droplet effective diameter (ED) increase with altitude in the marine boundary layer. Due to higher updraft speeds, higher cloud droplet number concentrations (Nliquid) were measured in winter compared to summer despite lower cloud condensation nucleus abundance. Flight cloud cover derived from statistical analysis of in situ data is reduced in summer and shows large variability. This seasonal contrast in cloud coverage is consistent with a dominance of a synoptic pattern in winter that favors conditions for the formation of stratiform clouds at the western edge of cyclones (post-cyclonic). In contrast, a dominant summer anticyclone is concomitant with the occurrence of shallow cumulus clouds and lower cloud coverage. The evaluation of boundary layer clouds and precipitation in the Nliquid ED phase space sheds light on liquid, mixed-phase, and ice cloud properties and helps to categorize the cloud data. Ice and liquid precipitation, often masked in cloud statistics by a high abundance of liquid clouds, is often observed throughout the cloud. The ACTIVATE in situ cloud measurements provide a wealth of cloud information useful for assessing airborne and satellite remote-sensing products, for global climate and weather model evaluations, and for dedicated process studies that address precipitation and aerosol–cloud interactions.

Agricultural and prescribed burning activities emit large amounts of trace gases and aerosols on regional to global scales. We present a compilation of emission factors (EFs) and emission ratios (ERs) from the eastern portion of the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign in 2019 in the United States, which sampled burning of crop residues and other prescribed fire fuels. FIREX-AQ provided comprehensive chemical characterization of 53 crop residue and 22 prescribed fires. Crop residues burned at different modified combustion efficiencies (MCE), with corn residue burning at higher MCE than other fuel types. Prescribed fires burned at lower MCE (<0.90) which is typical, while grasslands burned at lower MCE (0.90) than normally observed due to moist, green, growing season fuels. Most non-methane volatile organic compounds (NMVOCs) were significantly anticorrelated with MCE except for ethanol and NMVOCs that were measured with less certainty. We identified 23 species where crop residue fires differed by more than 50% from prescribed fires at the same MCE. Crop residue EFs were greater for species related to agricultural chemical use and fuel composition as well as oxygenated NMVOCs possibly due to the presence of metals such as potassium. Prescribed EFs were greater for monoterpenes (5×). FIREX-AQ crop residue average EFs generally agreed with the previous agricultural fire study in the US but had large disagreements with global compilations. FIREX-AQ observations show the importance of regionally-specific and fuel-specific EFs as first steps to reduce uncertainty in modeling the air quality impacts of fire emissions.

In-situ marine cloud droplet number concentrations (CDNCs), cloud condensation nuclei (CCN), and CCN proxies, based on particle sizes and optical properties, are accumulated from seven field campaigns: ACTIVATE; NAAMES; CAMP2EX; ORACLES; SOCRATES; MARCUS; and CAPRICORN2. Each campaign involves aircraft measurements, ship-based measurements, or both. Measurements collected over the North and Central Atlantic, Indo-Pacific, and Southern Oceans, represent a range of clean to polluted conditions in various climate regimes. With the extensive range of environmental conditions sampled, this data collection is ideal for testing satellite remote detection methods of CDNC and CCN in marine environments. Remote measurement methods are vital to expanding the available data in these difficult-to-reach regions of the Earth and improving our understanding of aerosolcloud interactions. The data collection includes particle composition and continental tracers to identify potential contributing CCN sources. Several of these campaigns include High Spectral Resolution Lidar (HSRL) and polarimetric imaging measurements and retrievals that will be the basis for the next generation of space-based remote sensors and, thus, can be utilized as satellite surrogates.

The NOAA/NASA Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) experiment was a multi-agency, inter-disciplinary research effort to: (a) obtain detailed measurements of trace gas and aerosol emissions from wildfires and prescribed fires using aircraft, satellites and ground-based instruments, (b) make extensive suborbital remote sensing measurements of fire dynamics, (c) assess local, regional, and global modeling of fires, and (d) strengthen connections to observables on the ground such as fuels and fuel consumption and satellite products such as burned area and fire radiative power. From Boise, ID western wildfires were studied with the NASA DC-8 and two NOAA Twin Otter aircraft. The high-altitude NASA ER-2 was deployed from Palmdale, CA to observe some of these fires in conjunction with satellite overpasses and the other aircraft. Further research was conducted on three mobile laboratories and ground sites, and 17 different modeling forecast and analyses products for fire, fuels and air quality and climate implications. From Salina, KS the DC-8 investigated 87 smaller fires in the Southeast with remote and in-situ data collection. Sampling by all platforms was designed to measure emissions of trace gases and aerosols with multiple transects to capture the chemical transformation of these emissions and perform remote sensing observations of fire and smoke plumes under day and night conditions. The emissions were linked to fuels consumed and fire radiative power using orbital and suborbital remote sensing observations collected during overflights of the fires and smoke plumes and ground sampling of fuels.

Fires emit sufficient sulfur to affect local and regional air quality and climate. This study analyzes SO2 emission factors and variability in smoke plumes from US wildfires and agricultural fires, as well as their relationship to sulfate and hydroxymethanesulfonate (HMS) formation. Observed SO2 emission factors for various fuel types show good agreement with the latest reviews of biomass burning emission factors, producing an emission factor range of 0.47–1.2 g SO2 kg^(−1) C. These emission factors vary with geographic location in a way that suggests that deposition of coal burning emissions and application of sulfur-containing fertilizers likely play a role in the larger observed values, which are primarily associated with agricultural burning. A 0-D box model generally reproduces the observed trends of SO2 and total sulfate (inorganic + organic) in aging wildfire plumes. In many cases, modeled HMS is consistent with the observed organosulfur concentrations. However, a comparison of observed organosulfur and modeled HMS suggests that multiple organosulfur compounds are likely responsible for the observations but that the chemistry of these compounds yields similar production and loss rates as that of HMS, resulting in good agreement with the modeled results. We provide suggestions for constraining the organosulfur compounds observed during these flights, and we show that the chemistry of HMS can allow organosulfur to act as an S(IV) reservoir under conditions of pH > 6 and liquid water content >10^(−7) g sm^(−3). This can facilitate long-range transport of sulfur emissions, resulting in increased SO2 and eventually sulfate in transported smoke.

Cloud droplet chemical composition is a key observable property that can aid understanding of how aerosols and clouds interact. As part of the Clouds, Aerosols and Monsoon Processes – Philippines Experiment (CAMP2Ex), three case studies were analyzed involving collocated airborne sampling of relevant clear and cloudy air masses associated with maritime warm convection. Two of the cases represented a polluted marine background, with signatures of transported East Asian regional pollution, aged over water for several days, while the third case comprised a major smoke transport event from Kalimantan fires. Sea salt was a dominant component of cloud droplet composition, in spite of fine particulate enhancement from regional anthropogenic sources. Furthermore, the proportion of sea salt was enhanced relative to sulfate in rainwater and may indicate both a propensity for sea salt to aid warm rain production and an increased collection efficiency of large sea salt particles by rain in subsaturated environments. Amongst cases, as precipitation became more significant, so too did the variability in the sea salt to (non-sea salt) sulfate ratio. Across cases, nitrate and ammonium were fractionally greater in cloud water than fine-mode aerosol particles; however, a strong covariability in cloud water nitrate and sea salt was suggestive of prior uptake of nitrate on large salt particles. A mass-based closure analysis of non-sea salt sulfate compared the cloud water air-equivalent mass concentration to the concentration of aerosol particles serving as cloud condensation nuclei for droplet activation. While sulfate found in cloud was generally constrained by the sub-cloud aerosol concentration, there was significant intra-cloud variability that was attributed to entrainment – causing evaporation of sulfate-containing droplets –and losses due to precipitation. In addition, precipitation tended to promote mesoscale variability in the sub-cloud aerosol through a combination of removal, convective downdrafts, and dynamically driven convergence. Physical mechanisms exerted such strong control over the cloud water compositional budget that it was not possible to isolate any signature of chemical production/loss using in-cloud observations. The cloud-free environment surrounding the non-precipitating smoke case indicated sulfate enhancement compared to convective mixing quantified by a stable gas tracer; however, this was not observed in the cloud water (either through use of ratios or the mass closure), perhaps implying that the warm convective cloud timescale was too short for chemical production to be a leading-order budgetary term and because precursors had already been predominantly exhausted. Closure of other species was truncated by incomplete characterization of coarse aerosol (e.g., it was found that only 10 %–50% of sea salt mass found in cloud was captured during clear-air sampling) and unmeasured gasphase abundances affecting closure of semi-volatile aerosol species (e.g., ammonium, nitrate and organic) and soluble volatile organic compound contributions to total organic carbon in cloud water.

Cloud droplet number concentration (Nd) is of central importance to observation-based estimates of aerosol indirect effects, being used to quantify both the cloud sensitivity to aerosol and the base state of the cloud. However, the derivation of Nd from satellite data depends on a number of assumptions about the cloud and the accuracy of the retrievals of the cloud properties from which it is derived, making it prone to systematic biases. A number of sampling strategies have been proposed to address these biases by selecting the most accurate Nd retrievals in the satellite data. This work compares the impact of these strategies on the accuracy of the satellite retrieved Nd, using a selection of in situ measurements. In stratocumulus regions, the MODIS Nd retrieval is able to achieve a high precision (r2 of 0.5–0.8). This is lower in other cloud regimes but can be increased by appropriate sampling choices. Although the Nd sampling can have significant effects on the Nd climatology, it produces only a 20 % variation in the implied radiative forcing from aerosol–cloud interactions, with the choice of aerosol proxy driving the overall uncertainty. The results are summarised into recommendations for using MODIS Nd products and appropriate sampling.

In this study, we propose a simple method to derive vertically resolved aerosol particle number concentration (Na) using combined polarimetric and lidar remote sensing observations. This method relies on accurate polarimeter retrievals of the fine-mode column-averaged aerosol particle extinction cross section and accurate lidar measurements of vertically resolved aerosol particle extinction coefficient such as those provided by multiwavelength high spectral resolution lidar. We compare the resulting lidar + polarimeter vertically resolved N(a) product to in situ N(a) data collected by airborne instruments during the NASA aerosol cloud meteorology interactions over the western Atlantic experiment (ACTIVATE). Based on all 35 joint ACTIVATE flights in 2020, we find a total of 32 collocated in situ and remote sensing profiles that occur on 11separate days, which contain a total of 322 cloud-free vertically resolved altitude bins of 150 m resolution. We demonstrate that the lidar + polarimeter N(a) agrees to within 106% for 90% of the 322 vertically resolved points. We also demonstrate similar agreement to within 121% for the polarimeter-derived column-averaged N(a). We find that the range-normalized mean absolute deviation (NMAD) for the polarimeter-derived column-averaged Na is 21%, and the NMAD for the lidar + polarimeter-derived vertically resolved Na is 16%. Taken together, these findings suggest that the error in the polarimeter-only column-averaged N(a) and the lidar + polarimeter vertically resolved N(a) are of similar magnitude and represent a significant improvement upon current remote sensing estimates of N(a).

Although the characteristics of biomass burning events and the ambient ecosystem determine emitted smoke composition, the conditions that modulate the partitioning of black carbon (BC) and brown carbon (BrC) formation are not well understood, nor are the spatial or temporal frequency of factors driving smoke particle evolution, such as hydration, coagulation, and oxidation, all of which impact smoke radiative forcing. In situ data from surface observation sites and aircraft field campaigns offer deep insight into the optical, chemical, and microphysical traits of biomass burning (BB) smoke aerosols, such as single scattering albedo (SSA) and size distribution, but cannot by themselves provide robust statistical characterization of both emitted and evolved particles. Data from the NASA Earth Observing System’s Multi-Angle Imaging SpectroRadiometer (MISR) instrument can provide at least a partial picture of BB particle properties and their evolution downwind, once properly validated. Here we use in situ data from the joint NOAA/NASA 2019 Fire Influence on Regional to Global Environments Experiment-Air Quality (FIREX-AQ) field campaign to assess the strengths and limitations of MISR-derived constraints on particle size, shape, light-absorption, and its spectral slope, as well as plume height and associated wind vectors. Based on the satellite observations, we also offer inferences about aging mechanisms effecting downwind particle evolution, such as gravitational settling, oxidation, secondary particle formation, and the combination of particle aggregation and condensational growth. This work builds upon our previous study, adding confidence to our interpretation of the remote-sensing data based on an expanded suite of in situ measurements for validation. The satellite and in situ measurements offer similar characterizations of particle property evolution as a function of smoke age for the 06 August Williams Flats Fire, and most of the key differences in particle size and absorption can be attributed to differences in sampling and changes in the plume geometry between sampling times. Whereas the aircraft data provide validation for the MISR retrievals, the satellite data offer a spatially continuous mapping of particle properties over the plume, which helps identify trends in particle property downwind evolution that are ambiguous in the sparsely sampled aircraft transects. The MISR data record is more than two decades long, offering future opportunities to study regional wildfire plume behavior statistically, where aircraft data are limited or entirely lacking.

We present ground‐based, advected aircraft engine emissions from flights taking off at Los Angeles International Airport. 275 discrete engine take‐off plumes were observed on 18 and 25 May 2014 at a distance of 400 m downwind of the runway. CO2 measurements are used to convert the aerosol data into plume‐average emissions indices that are suitable for modelling aircraft emissions. Total and non‐volatile particle number EIs are of order 1016‐1017 kg‐1 and 1014‐1016 kg‐1, respectively. Black‐carbon‐equivalent particle mass EIs vary between 175‐941 mg kg‐1 (except for the GE GEnx engines at 46 mg kg‐1). Aircraft tail numbers recorded for each take‐off event are used to incorporate aircraft‐ and engine‐specific parameters into the data set. Data acquisition and processing follow standard methods for quality assurance. A unique aspect of the data set is the mapping of aerosol concentration time series to integrated plume EIs, aircraft and engine specifications, and manufacturer‐reported engine emissions certifications. The integrated data enable future studies seeking to understand and model aircraft emissions and their impact on air quality.

Aviation aerosol emissions have a disproportionately large climatic impact because they are emitted high in the relatively pristine upper troposphere where they can form linear contrails and influence cirrus clouds. Research aircraft from NASA, DLR, and NRC Canada made airborne measurements of gaseous and aerosol composition and contrail microphysical properties behind the NASA DC-8 aircraft at cruise altitudes. The DC-8 CFM-56-2C engines burned traditional medium-sulfur Jet A fuel as well as a low-sulfur Jet A fuel and a 50:50 biofuel blend. Substantial, two-to-three-fold emissions reductions are found for both particle number and mass emissions across the range of cruise thrust operating conditions. These observations provide direct and compelling evidence for the beneficial impacts of biojet fuel blending under real-world conditions.

The next generation of aerosol satellite instruments will include multi-spectral polarimetric measurements to retrieval aerosol size distribution and refractive index (Hasekamp et al., 2011; NRC, 2007). Refractive index is the “only means of constraining aerosol chemical composition from space” for passive sensors (Mischenko et al., 2007). A number of methods have been developed to derive refractive index from combined optical and electrical mobility sizing instruments (e.g., the “Alignment Method” of Hand and Kreidenweis, 2002). In this work, we evaluate the sensitivity of two, commercially-available, high-resolution optical particle counters for determining the size-resolved refractive index of laboratory-generated aerosols when used with a modified form of the Alignment Method.