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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.

Accurate representation of aerosol optical properties is essential for the modeling and remote sensing of atmospheric aerosols. Although aerosol optical properties are strongly dependent upon the aerosol size distribution, the use of detailed aerosol microphysics schemes in global atmospheric models is inhibited by associated computational demands. Computationally efficient parameterizations for aerosol size are needed. In this study, airborne measurements over the United States (DISCOVER-AQ) and South Korea (KORUS-AQ) are interpreted with a global chemical transport model (GEOS-Chem) to investigate the variation in aerosol size when organic matter (OM) and sulfate–nitrate–ammonium (SNA) are the dominant aerosol components. The airborne measurements exhibit a strong correlation (r=0.83) between dry aerosol size and the sum of OM and SNA mass concentration (MSNAOM). A global microphysical simulation (GEOS-Chem-TOMAS) indicates that MSNAOM and the ratio between the two components (OM/SNA) are the major indicators for SNA and OM dry aerosol size. A parameterization of the dry effective radius (Reff) for SNA and OM aerosol is designed to represent the airborne measurements (R2=0.74; slope = 1.00) and the GEOS-Chem-TOMAS simulation (R2=0.72; slope = 0.81). When applied in the GEOS-Chem high-performance model, this parameterization improves the agreement between the simulated aerosol optical depth (AOD) and the ground-measured AOD from the Aerosol Robotic Network (AERONET; R2 from 0.68 to 0.73 and slope from 0.75 to 0.96). Thus, this parameterization offers a computationally efficient method to represent aerosol size dynamically.

Air quality network data in China and South Korea show very high year-round mass concentrations of coarse particulate matter (PM), as inferred by the difference between PM10 and PM2.5. Coarse PM concentrations in 2015 averaged 52 µg m−3 in the North China Plain (NCP) and 23 µg m−3 in the Seoul Metropolitan Area (SMA), contributing nearly half of PM10. Strong daily correlations between coarse PM and carbon monoxide imply a dominant source from anthropogenic fugitive dust. Coarse PM concentrations in the NCP and the SMA decreased by 21 % from 2015 to 2019 and further dropped abruptly in 2020 due to COVID-19 reductions in construction and vehicle traffic. Anthropogenic coarse PM is generally not included in air quality models but scavenges nitric acid to suppress the formation of fine particulate nitrate, a major contributor to PM2.5 pollution. GEOS-Chem model simulation of surface and aircraft observations from the Korea–United States Air Quality (KORUS-AQ) campaign over the SMA in May–June 2016 shows that consideration of anthropogenic coarse PM largely resolves the previous model overestimate of fine particulate nitrate. The effect is smaller in the NCP which has a larger excess of ammonia. Model sensitivity simulations for 2015–2019 show that decreasing anthropogenic coarse PM directly increases PM2.5 nitrate in summer, offsetting 80 % the effect of nitrogen oxide and ammonia emission controls, while in winter the presence of coarse PM increases the sensitivity of PM2.5 nitrate to ammonia and sulfur dioxide emissions. Decreasing coarse PM helps to explain the lack of decrease in wintertime PM2.5 nitrate observed in the NCP and the SMA over the 2015–2021 period despite decreases in nitrogen oxide and ammonia emissions. Continuing decrease of fugitive dust pollution means that more stringent nitrogen oxide and ammonia emission controls will be required to successfully decrease PM2.5 nitrate.

The NASA North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) ship and aircraft field campaign deployed to the western subarctic Atlantic between the years 2015 and 2018. One of the primary goals of NAAMES is to improve the understanding of aerosol–cloud interaction (ACI) over the Atlantic Ocean under different seasonal regimes. ACIs currently represent the largest source of uncertainty in global climate models. During three NAAMES field campaigns (NAAMES-1 in November 2015, NAAMES-2 in May 2016, and NAAMES-3 in September 2017), multiple 10 h science flights were conducted using the NASA C-130 aircraft to measure marine boundary layer aerosol and cloud properties. The standard flight pattern includes vertical spirals where the C-130 transitioned from high altitude to low altitude (and vice versa), collecting in situ measurements of aerosols, trace gases, clouds, and meteorological parameters as a function of altitude. We examine the data collected from 37 spirals during the three NAAMES field campaigns, and we present a comprehensive characterization of the vertical profiles of aerosol properties under different synoptic conditions and aerosol regimes. The vertical distribution of submicron aerosol particles exhibited strong seasonal variation, as well as elevated intra-seasonal variability depending on emission sources and aerosol processes in the atmospheric column. Pristine marine conditions and new particle formation were prevalent in the wintertime (NAAMES-1) due to low biogenic emissions from the surface ocean and reduced continental influence. Higher concentrations of submicron aerosol particles were observed in the spring (NAAMES-2) due to strong phytoplankton activity and the arrival of long-range-transported continental plumes in the free troposphere with subsequent entrainment into the marine boundary layer. Biomass burning from boreal wildfires was the main source of aerosol particles in the region during the late summer (NAAMES-3) in both the marine boundary layer and free troposphere.

Sustainable aviation fuels (SAFs) have different compositions compared to conventional petroleum jet fuels, particularly in terms of fuel sulfur and hydrocarbon content. These differences may change the amount and physicochemical properties of volatile and non-volatile particulate matter (nvPM) emitted by aircraft engines. In this study, we evaluate whether comparable nvPM measurement techniques respond similarly to nvPM produced by three blends of SAFs compared to three conventional fuels. Multiple SAF blends and conventional (Jet A-1) jet fuels were combusted in a V2527-A5 engine, while an additional conventional fuel (JP-8) was combusted in a CFM56-2C1 engine. We evaluated nvPM mass concentration measured by three real-time measurement techniques: photoacoustic spectroscopy, laser-induced incandescence, and the extinction-minus-scattering technique. Various commercial instruments were tested, including three laser-induced incandescence (LII) 300s, one photoacoustic extinctiometer (PAX), one micro soot sensor (MSS+), and two cavity-attenuated phase shift PMSSA (CAPS PMSSA) instruments. Mass-based emission indices (EIm) reported by these techniques were similar, falling within 30 % of their geometric mean for EIm above 100 mg per kg fuel (approximately 10 µg PM m−3 at the instrument); this geometric mean was therefore used as a reference value. Additionally, two integrative measurement techniques were evaluated: filter photometry and particle size distribution (PSD) integration. The commercial instruments used were one tricolor absorption photometer (TAP), one particle soot absorption photometer (PSAP), and two scanning mobility particle sizers (SMPSs). The TAP and PSAP were operated at 5 % and 10 % of their nominal flow rates, respectively, to extend the life of their filters. These techniques are used in specific applications, such as on board research aircraft to determine particulate matter (PM) emissions at cruise. EIm reported by the alternative techniques fell within approximately 50 % of the mean aerosol-phase EIm. In addition, we measured PM-number-based emission indices using PSDs and condensation particle counters (CPCs). The commercial instruments used included TSI SMPSs, a Cambustion differential mobility spectrometer (DMS500), and an AVL particle counter (APC), and the data also fell within approximately 50 % of their geometric mean. The number-based emission indices were highly sensitive to the accuracy of the sampling-line penetration functions applied as corrections. In contrast, the EIm data were less sensitive to those corrections since a smaller volume fraction fell within the size range where corrections were substantial. A separate, dedicated experiment also showed that the operating laser fluence used in the LII 300 laser-induced incandescence instrument for aircraft-engine nvPM measurement is adequate for a range of SAF blends investigated in this study. Overall, we conclude that all tested instruments are suitable for the measurement of nvPM emissions from the combustion of SAF blends in aircraft engines.

Geostationary satellite measurements of aerosol optical depth (AOD) over East Asia from the Geostationary Ocean Color Imager (GOCI) and Advanced Himawari Imager (AHI) instruments can augment surface monitoring of fine particulate matter (PM2.5) air quality, but this requires better understanding of the AOD–PM2.5 relationship. Here we use the GEOS-Chem chemical transport model to analyze the critical variables determining the AOD–PM2.5 relationship over East Asia by simulation of observations from satellite, aircraft, and ground-based datasets. This includes the detailed vertical aerosol profiling over South Korea from the KORUS-AQ aircraft campaign (May–June 2016) with concurrent ground-based PM2.5 composition, PM10, and AERONET AOD measurements. The KORUS-AQ data show that 550 nm AOD is mainly contributed by sulfate–nitrate–ammonium (SNA) and organic aerosols in the planetary boundary layer (PBL), despite large dust concentrations in the free troposphere, reflecting the optically effective size and high hygroscopicity of the PBL aerosols. We updated SNA and organic aerosol size distributions in GEOS-Chem to represent aerosol optical properties over East Asia by using in situ measurements of particle size distributions from KORUS-AQ. We find that SNA and organic aerosols over East Asia have larger size (number median radius of 0.11 µm with geometric standard deviation of 1.4) and 20 % larger mass extinction efficiency as compared to aerosols over North America (default setting in GEOS-Chem). Although GEOS-Chem is successful in reproducing the KORUS-AQ vertical profiles of aerosol mass, its ability to link AOD to PM2.5 is limited by under-accounting of coarse PM and by a large overestimate of nighttime PM2.5 nitrate. The GOCI–AHI AOD data over East Asia in different seasons show agreement with AERONET AODs and a spatial distribution consistent with surface PM2.5 network data. The AOD observations over North China show a summer maximum and winter minimum, opposite in phase to surface PM2.5. This is due to low PBL depths compounded by high residential coal emissions in winter and high relative humidity (RH) in summer. Seasonality of AOD and PM2.5 over South Korea is much weaker, reflecting weaker variation in PBL depth and lack of residential coal emissions.

Sustainable aviation fuels can reduce contrail ice numbers and radiative forcing by contrail cirrus. We measured apparent ice emission indices for fuels with varying aromatic content at altitude ranges of 9.1–9.8 and 11.4–11.6 km. Measurement data were collected during the ECLIF II/NDMAX flight experiment in January 2018. The fuels varied in both aromatic quantity and type. Between a sustainable aviation fuel blend and a reference fuel Jet A-1, a maximum reduction in apparent ice emission indices of 40 % was found. We show vertical ice number and extinction distributions for three different fuels and calculate representative contrail optical depths. Optical depths of contrails (0.5–3 min in age) were reduced by 40 % to 52 % for a sustainable aviation fuel compared to the reference fuel. Our measurements suggest that sustainable aviation fuels result in reduced ice particle numbers, extinction coefficients, optical depth and climate impact from contrails.

Nitrous acid (HONO) is an important precursor to hydroxyl radical (OH) that determines atmospheric oxidative capacity and thus impacts climate and air quality. Wildfire is not only a major direct source of HONO, it also results in highly polluted conditions that favor the heterogeneous formation of HONO from nitrogen oxides (NOx= NO + NO2) and nitrate on both ground and particle surfaces. However, these processes remain poorly constrained. To quantitatively constrain the HONO budget under various fire and/or smoke conditions, we combine a unique dataset of field concentrations and isotopic ratios (15N / 14N and 18O / 16O) of NOx and HONO with an isotopic box model. Here we report the first isotopic evidence of secondary HONO production in near-ground wildfire plumes (over a sample integration time of hours) and the subsequent quantification of the relative importance of each pathway to total HONO production. Most importantly, our results reveal that nitrate photolysis plays a minor role (<5 %) in HONO formation in daytime aged smoke, while NO2-to-HONO heterogeneous conversion contributes 85 %–95 % to total HONO production, followed by OH + NO (5 %–15 %). At nighttime, heterogeneous reduction of NO2 catalyzed by redox active species (e.g., iron oxide and/or quinone) is essential (≥ 75 %) for HONO production in addition to surface NO2 hydrolysis. Additionally, the 18O / 16O of HONO is used for the first time to constrain the NO-to-NO2 oxidation branching ratio between ozone and peroxy radicals. Our approach provides a new and critical way to mechanistically constrain atmospheric chemistry and/or air quality models on a diurnal timescale.

Arctic low clouds and the water they contain influence the evolution of the Arctic system through their effects on radiative fluxes, boundary layer mixing, stability, turbulence, humidity, and precipitation. Atmospheric models struggle to accurately simulate the occurrence and properties of Arctic low clouds, stemming from errors in both the simulated atmospheric state and the dependence of cloud properties on the atmospheric state. Knowledge of the contributions from these two factors to the model errors allows for the isolation of the process contributions to the model–observation differences. We analyze the differences between the Arctic System Reanalysis version 2 (ASR) and data taken during the September 2014 Arctic Radiation–IceBridge Sea and Ice Experiment (ARISE) airborne campaign conducted over the Beaufort Sea. The results show that ASR produces less total and liquid cloud water than observed along the flight track and is unable to simulate observed large in-cloud water content. Contributing to this bias, ASR is warmer by nearly 1.5 K and drier by 0.06 g kg−1 (relative humidity 4.3 % lower) than observed. Moreover, ASR produces cloud water over a much narrower range of thermodynamic conditions than shown in ARISE observations. Analyzing the ARISE–ASR differences by thermodynamic conditions, our results indicate that the differences are primarily attributed to disagreements in the cloud–thermodynamic relationships and secondarily (but importantly) to differences in the occurrence frequency of thermodynamic regimes. The ratio of the factors is about 2/3 to 1/3. Substantial sampling uncertainties are found within low-likelihood atmospheric regimes; sampling noise cannot be ruled out as a cause of observation–model differences, despite large differences. Thus, an important lesson from this analysis is that when comparing in situ airborne data and model output, one should not restrict the comparison to flight-track-only model output.

We evaluate the sensitivity of the size calibrations of two commercially available, high-resolution optical particle sizers to changes in aerosol composition and complex refractive index (RI). The Droplet Measurement Technologies Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) and the TSI, Inc. Laser Aerosol Spectrometer (LAS) are two commonly used instruments for measuring the portion of the aerosol size distribution with diameters larger than nominally 60–90 nm. Both instruments illuminate particles with a laser and relate the single-particle light scattering intensity and count rate measured over a wide range of angles to the size-dependent particle concentration. While the optical block geometry and flow system are similar for each instrument, a significant difference between the two models is the laser wavelength (1054 nm for the UHSAS and 633 nm for the LAS) and intensity (about 100 times higher for the UHSAS), which may affect the way each instrument sizes non-spherical or absorbing aerosols. Here, we challenge the UHSAS and LAS with laboratory-generated, mobility-size-classified aerosols of known chemical composition to quantify changes in the optical size response relative to that of ammonium sulfate (RI of 1.52+0i at 532 nm) and NIST-traceable polystyrene latex spheres (PSLs with RI of 1.59+0i at 589 nm). Aerosol inorganic salt species are chosen to cover the real refractive index range of 1.32 to 1.78, while chosen light-absorbing carbonaceous aerosols include fullerene soot, nigrosine dye, humic acid, and fulvic acid standards. The instrument response is generally in good agreement with the electrical mobility diameter. However, large undersizing deviations are observed for the low-refractive-index fluoride salts and the strongly absorbing nigrosine dye and fullerene soot particles. Polydisperse size distributions for both fresh and aged wildfire smoke aerosols from the recent Fire Influence on Regional to Global Environments Experiment and Air Quality (FIREX-AQ) and the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex) airborne campaigns show good agreement between both optical sizers and contemporaneous electrical mobility sizing and particle time-of-flight mass spectrometric measurements. We assess the instrument uncertainties by interpolating the laboratory response curves using previously reported RIs and size distributions for multiple aerosol type classifications. These results suggest that, while the optical sizers may underperform for strongly absorbing laboratory compounds and fresh tailpipe emissions measurements, sampling aerosols within the atmospherically relevant range of refractive indices are likely to be sized to better than ±10 %–20 % uncertainty over the submicron aerosol size range when using instruments calibrated with ammonium sulfate.

In situ observations of spectrally resolved aerosol extinction coefficients (300–700 nm at ∼ 0.8 nm resolution) from the May–June 2016 Korea–United States Ocean Color (KORUS-OC) oceanographic field campaign are reported. Measurements were made with the custom-built Spectral Aerosol Extinction (SpEx) instrument that previously has been characterized only using laboratory-generated aerosols of known size and composition. Here, the performance of SpEx under realistic operating conditions in the field was assessed by comparison to extinction coefficients derived from commercial instruments that measured scattering and filter-based absorption coefficients at three discrete visible wavelengths. Good agreement was found between these two sets of extinction coefficients with slopes near unity for all three wavelengths within the SpEx measurement error (± 5 Mm−1). The meteorological conditions encountered during the cruise fostered diverse ambient aerosol populations with varying sizes and composition at concentrations spanning 2 orders of magnitude. The sampling inlet had a 50 % size cut of 1.3 µm diameter particles such that the in situ aerosol sampling suite deployed aboard ship measured fine-mode aerosols only. The extensive hyperspectral extinction data set acquired revealed that nearly all measured spectra exhibited curvature in logarithmic space, such that Ångström exponent (α) power law fits could lead to large errors compared to measured values. This problem was particularly acute for α values calculated over only visible wavelengths and then extrapolated to the UV, highlighting the need for measurements in this wavelength range. Second-order polynomial fits to the logarithmically transformed data provided a much better fit to the measured spectra than the linear fits of power laws. Building on previous studies that used total column aerosol optical depth observations to examine the information content of spectral curvature, the relationship between α and the second-order polynomial fit coefficients (a1 and a2) was found to depend on the wavelength range of the spectral measurement such that any given α maps into a line in (a1, a2) coefficient space with a slope of −2LN(λch), where λch is defined as the single wavelength that characterizes the wavelength range of the measured spectrum (i.e., the “characteristic wavelength”). Since the curvature coefficient values depend on λch, it must be taken into account when comparing values from spectra obtained from measurement techniques with different λch. Previously published work has shown that different bimodal size distributions of aerosols can exhibit the same α yet have differing spectral curvature with different (a1, a2). This implies that (a1, a2) contain more information about size distributions than α alone. Aerosol size distributions were not measured during KORUS-OC, and the data reported here were limited to the fine fraction, but the (a1, a2) maps obtained from the SpEx data set are consistent with the expectation that (a1, a2) may contain more information than α – a result that will be explored further with future SpEx and size distribution data sets.

This two-part study explores hyperspectral (300–700 nm) aerosol optical measurements obtained from in situ sampling methods employed during the May–June 2016 Korea–United States Ocean Color (KORUS-OC) cruise conducted in concert with the broader air quality campaign (KORUS-AQ). Part 1 focused on the hyperspectral measurement of extinction coefficients (σext) using the recently developed in situ Spectral Aerosol Extinction (SpEx) instrument and showed that second-order polynomials provided a better fit to the measured spectra than power law fits. Two dimensional mapping of the second-order polynomial coefficients (a1, a2) was used to explore the information content of the spectra. Part 2 expands on that work by applying a similar analytical approach to filter-based measurements of aerosol hyperspectral total absorption (σabs) and soluble absorption from filters extracted with either deionized water (σDI-abs) or methanol (σMeOH-abs). As was found for σext, second-order polynomials provided a better fit to all three absorption spectra sets. Averaging the measured σext from Part 1 over the filter sampling intervals in this work, hyperspectral single-scattering albedo (ω) was calculated. Water-soluble aerosol composition from the DI extracts was used to examine relationships with the various measured optical properties. In particular, both σDI-abs(365 nm) and σMeOH-abs(365 nm) were found to be best correlated with oxalate (C2O42-), but elevated soluble absorption was found from two chemically and optically distinct populations of aerosols. The more photochemically aged aerosols of those two groups exhibited partial spectra (i.e., the longer wavelengths of the spectral range were below detection) while the less-aged aerosol of the other group exhibited complete spectra across the wavelength range. The chromophores of these groups may have derived from different sources and/or atmospheric processes, such that photochemical age may have been only one factor contributing to the differences in the observed spectra. The differences in the spectral properties of these groups was evident in (a1, a2) maps. The results of the two-dimensional mapping shown in Parts 1 and 2 suggest that this spectral characterization may offer new methods to relate in situ aerosol optical properties to their chemical and microphysical characteristics. However, a key finding of this work is that mathematical functions (whether power laws or second-order polynomials) extrapolated from a few wavelengths or a subrange of wavelengths fail to reproduce the measured spectra over the full 300–700 nm wavelength range. Further, the σabs and ω spectra exhibited distinctive spectral features across the UV and visible wavelength range that simple functions and extrapolations cannot reproduce. These results show that in situ hyperspectral measurements provide valuable new data that can be probed for additional information relating in situ aerosol optical properties to the underlying physicochemical properties of ambient aerosols. It is anticipated that future studies examining in situ aerosol hyperspectral properties will not only improve our ability to use optical data to characterize aerosol physicochemical properties, but that such in situ tools will be needed to validate hyperspectral remote sensors planned for space-based observing platforms.

Nitryl chloride (ClNO2) is a radical reservoir species that releases chlorine radicals upon photolysis. An integrated analysis of the impact of ClNO2 on regional photochemistry in the Seoul metropolitan area (SMA) during the Korea–United States Air Quality Study (KORUS-AQ) 2016 field campaign is presented. Comprehensive multiplatform observations were conducted aboard the NASA DC-8 and at two ground sites (Olympic Park, OP; Taehwa Research Forest, TRF), representing an urbanized area and a forested suburban region, respectively. Positive correlations between daytime Cl2 and ClNO2 were observed at both sites, the slope of which was dependent on O3 levels. The possible mechanisms are explored through box model simulations constrained with observations. The overall diurnal variations in ClNO2 at both sites appeared similar but the nighttime variations were systematically different. For about half of the observation days at the OP site the level of ClNO2 increased at sunset but rapidly decreased at around midnight. On the other hand, high levels were observed throughout the night at the TRF site. Significant levels of ClNO2 were observed at both sites for 4–5 h after sunrise. Airborne observations, box model calculations, and back-trajectory analysis consistently show that these high levels of ClNO2 in the morning are likely from vertical or horizontal transport of air masses from the west. Box model results show that chlorine-radical-initiated chemistry can impact the regional photochemistry by elevating net chemical production rates of ozone by ∼25 % in the morning.

Aerosol volume size distribution (VSD) retrievals from the Aerosol Robotic Network (AERONET) aerosol monitoring network were obtained during multiple DRAGON (Distributed Regional Aerosol Gridded Observational Network) campaigns conducted in Maryland, California, Texas and Colorado from 2011 to 2014. These VSD retrievals from the field campaigns were used to make comparisons with near-simultaneous in situ samples from aircraft profiles carried out by the NASA Langley Aerosol Group Experiment (LARGE) team as part of four campaigns comprising the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) experiments. For coincident (±1 h) measurements there were a total of 91 profile-averaged fine-mode size distributions acquired with the LARGE ultra-high sensitivity aerosol spectrometer (UHSAS) instrument matched to 153 AERONET size distributions retrieved from almucantars at 22 different ground sites. These volume size distributions were characterized by two fine-mode parameters, the radius of peak concentration (rpeak_conc) and the VSD fine-mode width (widthpeak_conc). The AERONET retrievals of these VSD fine-mode parameters, derived from ground-based almucantar sun photometer data, represent ambient humidity values while the LARGE aircraft spiral profile retrievals provide dried aerosol (relative humidity; RH  %) values. For the combined multiple campaign dataset, the average difference in rpeak_conc was 0.033±0.035 µm (ambient AERONET values were 15.8 % larger than dried LARGE values), and the average difference in widthpeak_conc was 0.042±0.039 µm (AERONET values were 25.7 % larger). For a subset of aircraft data, the LARGE data were adjusted to account for ambient humidification. For these cases, the AERONET–LARGE average differences were smaller, with rpeak_conc differing by 0.011±0.019 µm (AERONET values were 5.2 % larger) and widthpeak_conc average differences equal to 0.030±0.037 µm (AERONET values were 15.8 % larger).

Deep convective clouds are critically important to the distribution of atmospheric constituents throughout the troposphere but are difficult environments to study. The Deep Convective Clouds and Chemistry (DC3) study in 2012 provided the environment, platforms, and instrumentation to test oxidation chemistry around deep convective clouds and their impacts downwind. Measurements on the NASA DC-8 aircraft included those of the radicals hydroxyl (OH) and hydroperoxyl (HO2), OH reactivity, and more than 100 other chemical species and atmospheric properties. OH, HO2, and OH reactivity were compared to photochemical models, some with and some without simplified heterogeneous chemistry, to test the understanding of atmospheric oxidation as encoded in the model. In general, the agreement between the observed and modeled OH, HO2, and OH reactivity was within the combined uncertainties for the model without heterogeneous chemistry and the model including heterogeneous chemistry with small OH and HO2 uptake consistent with laboratory studies. This agreement is generally independent of the altitude, ozone photolysis rate, nitric oxide and ozone abundances, modeled OH reactivity, and aerosol and ice surface area. For a sunrise to midday flight downwind of a nighttime mesoscale convective system, the observed ozone increase is consistent with the calculated ozone production rate. Even with some observed-to-modeled discrepancies, these results provide evidence that a current measurement-constrained photochemical model can simulate observed atmospheric oxidation processes to within combined uncertainties, even around convective clouds. For this DC3 study, reduction in the combined uncertainties would be needed to confidently unmask errors or omissions in the model chemical mechanism.

Over the past 24 years, the AErosol RObotic NETwork (AERONET) program has provided highly accurate remote-sensing characterization of aerosol optical and physical properties for an increasingly extensive geographic distribution including all continents and many oceanic island and coastal sites. The measurements and retrievals from the AERONET global network have addressed satellite and model validation needs very well, but there have been challenges in making comparisons to similar parameters from in situ surface and airborne measurements. Additionally, with improved spatial and temporal satellite remote sensing of aerosols, there is a need for higher spatial-resolution ground-based remote-sensing networks. An effort to address these needs resulted in a number of field campaign networks called Distributed Regional Aerosol Gridded Observation Networks (DRAGONs) that were designed to provide a database for in situ and remote-sensing comparison and analysis of local to mesoscale variability in aerosol properties. This paper describes the DRAGON deployments that will continue to contribute to the growing body of research related to meso- and microscale aerosol features and processes. The research presented in this special issue illustrates the diversity of topics that has resulted from the application of data from these networks.

We present a detailed evaluation of remotely sensed aerosol microphysical properties obtained from an advanced, multi-wavelength high-spectral-resolution lidar (HSRL-2) during the 2013 NASA DISCOVER-AQ field campaign. Vertically resolved retrievals of fine-mode aerosol number, surface-area, and volume concentration as well as aerosol effective radius are compared to 108 collocated, airborne in situ measurement profiles in the wintertime San Joaquin Valley, California, and in summertime Houston, Texas. An algorithm for relating the dry in situ aerosol properties to those obtained by the HSRL at ambient relative humidity is discussed. We show that the HSRL-2 retrievals of ambient fine-mode aerosol surface-area and volume concentrations agree with the in situ measurements to within 25 and 10 %, respectively, once hygroscopic growth adjustments have been applied to the dry in situ data. Despite this excellent agreement for the microphysical properties, extinction and backscatter coefficients at ambient relative humidity derived from the in situ aerosol measurements using Mie theory are consistently smaller than those measured by the HSRL, with average differences of 31 ± 5 % and 53 ± 11 % for California and Texas, respectively. This low bias in the in situ estimates is attributed to the presence of coarse-mode aerosol that are detected by HSRL-2 but that are too large to be well sampled by the in situ instrumentation. Since the retrieval of aerosol volume is most relevant to current regulatory efforts targeting fine particle mass (PM2. 5), these findings highlight the advantages of an advanced 3β + 2α HSRL for constraining the vertical distribution of the aerosol volume or mass loading relevant for air quality.

Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10–23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout the aerosol size distribution. Using a core-shell mixing rule in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for modeling the time-varying mixing states of aerosols in future versions of ASP.

Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US). Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0–4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD) to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH). For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry–climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of ∼ 25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1–0.5 µm diameter dominates aerosol extinction.

Aircraft observations of meteorological, trace gas, and aerosol properties were made during May–September 2013 in the southeastern United States (US) under fair-weather, afternoon conditions with well-defined planetary boundary layer structure. Optical extinction at 532 nm was directly measured at relative humidities (RHs) of ∼ 15, ∼ 70, and ∼ 90 % and compared with extinction calculated from measurements of aerosol composition and size distribution using the κ-Köhler approximation for hygroscopic growth. The calculated enhancement in hydrated aerosol extinction with relative humidity, f(RH), calculated by this method agreed well with the observed f(RH) at ∼ 90 % RH. The dominance of organic aerosol, which comprised 65 ± 10 % of particulate matter with aerodynamic diameter f(RH) values of 1.43 ± 0.67 at 70 % RH and 2.28 ± 1.05 at 90 % RH. The subsaturated κ-Köhler hygroscopicity parameter κ for the organic fraction of the aerosol must have been κ = 0.05. This subsaturated κ value for the organic aerosol in the southeastern US is broadly consistent with field studies in rural environments. A new, physically based, single-parameter representation was developed that better described f(RH) than did the widely used gamma power-law approximation.

An instrumented NASA P-3B aircraft was used for airborne sampling of trace gases in a plume that had emanated from a small forest understory fire in Georgia, USA. The plume was sampled at its origin to derive emission factors and followed ∼ 13.6 km downwind to observe chemical changes during the first hour of atmospheric aging. The P-3B payload included a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS), which measured non-methane organic gases (NMOGs) at unprecedented spatiotemporal resolution (10 m spatial/0.1 s temporal). Quantitative emission data are reported for CO2, CO, NO, NO2, HONO, NH3, and 16 NMOGs (formaldehyde, methanol, acetonitrile, propene, acetaldehyde, formic acid, acetone plus its isomer propanal, acetic acid plus its isomer glycolaldehyde, furan, isoprene plus isomeric pentadienes and cyclopentene, methyl vinyl ketone plus its isomers crotonaldehyde and methacrolein, methylglyoxal, hydroxy acetone plus its isomers methyl acetate and propionic acid, benzene, 2,3-butanedione, and 2-furfural) with molar emission ratios relative to CO larger than 1 ppbV ppmV−1. Formaldehyde, acetaldehyde, 2-furfural, and methanol dominated NMOG emissions. No NMOGs with more than 10 carbon atoms were observed at mixing ratios larger than 50 pptV ppmV−1 CO. Downwind plume chemistry was investigated using the observations and a 0-D photochemical box model simulation. The model was run on a nearly explicit chemical mechanism (MCM v3.3) and initialized with measured emission data. Ozone formation during the first hour of atmospheric aging was well captured by the model, with carbonyls (formaldehyde, acetaldehyde, 2,3-butanedione, methylglyoxal, 2-furfural) in addition to CO and CH4 being the main drivers of peroxy radical chemistry. The model also accurately reproduced the sequestration of NOx into peroxyacetyl nitrate (PAN) and the OH-initiated degradation of furan and 2-furfural at an average OH concentration of 7.45 ± 1.07 × 106 cm−3 in the plume. Formaldehyde, acetone/propanal, acetic acid/glycolaldehyde, and maleic acid/maleic anhydride (tentatively identified) were found to be the main NMOGs to increase during 1 h of atmospheric plume processing, with the model being unable to capture the observed increase. A mass balance analysis suggests that about 50 % of the aerosol mass formed in the downwind plume is organic in nature.

In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites) and mass measurements of aerosol loading (PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type – such as composition, size, and hygroscopicity – and to the surrounding atmosphere, such as temperature, relative humidity (RH), and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in situ atmospheric profiling in the Baltimore, MD–Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs). The average black carbon concentrations were 240 ng m−3 in the lowest 1 km, decreasing to 35 ng m−3 in the free troposphere (above 3 km). Routine airborne sampling over six locations was used to evaluate the relative contributions of aerosol loading, composition, and relative humidity (the amount of water available for uptake onto aerosols) to variability in mixed-layer aerosol extinction. Aerosol loading (dry extinction) was found to be the predominant source, accounting for 88 % on average of the measured spatial variability in ambient extinction, with lesser contributions from variability in relative humidity (10 %) and aerosol composition (1.3 %). On average, changes in aerosol loading also caused 82 % of the diurnal variability in ambient aerosol extinction. However on days with relative humidity above 60 %, variability in RH was found to cause up to 62 % of the spatial variability and 95 % of the diurnal variability in ambient extinction. This work shows that extinction is driven to first order by aerosol mass loadings; however, humidity-driven hydration effects play an important secondary role. This motivates combined satellite–modeling assimilation products that are able to capture these components of the aerosol optical depth (AOD)–PM2.5 link. Conversely, aerosol hygroscopicity and SSA play a minor role in driving variations both spatially and throughout the day in aerosol extinction and therefore AOD. However, changes in aerosol hygroscopicity from day to day were large and could cause a bias of up to 27 % if not accounted for. Thus it appears that a single daily measurement of aerosol hygroscopicity can be used for AOD-to-PM2.5 conversions over the study region (on the order of 1400 km2). This is complimentary to the results of Chu et al. (2015), who determined that the aerosol vertical distribution from "a single lidar is feasible to cover the range of 100 km" in the same region.

We introduce a new instrument for the measurement of in situ ambient aerosol extinction over the 300–700 nm wavelength range, the spectral aerosol extinction (SpEx) instrument. This measurement capability is envisioned to complement existing in situ instrumentation, allowing for simultaneous measurement of the evolution of aerosol optical, chemical, and physical characteristics in the ambient environment. In this work, a detailed description of the instrument is provided along with characterization tests performed in the laboratory. Measured spectra of NO2 and polystyrene latex spheres (PSLs) agreed well with theoretical calculations. Good agreement was also found with simultaneous aerosol extinction measurements at 450, 530, and 630 nm using CAPS PMex instruments in a series of 22 tests including nonabsorbing compounds, dusts, soot, and black and brown carbon analogs. SpEx measurements are expected to help identify the presence of ambient brown carbon due to its 300 nm lower wavelength limit compared to measurements limited to longer UV and visible wavelengths. Extinction spectra obtained with SpEx contain more information than can be conveyed by a simple power law fit (typically represented by Ångström exponents). Planned future improvements aim to lower detection limits and ruggedize the instrument for mobile operation.

Chemical components of organic aerosol (OA) selectively absorb light at short wavelengths. In this study, the prevalence, sources, and optical importance of this so-called brown carbon (BrC) aerosol component are investigated throughout the North American continental tropospheric column during a summer of extensive biomass burning. Spectrophotometric absorption measurements on extracts of bulk aerosol samples collected from an aircraft over the central USA were analyzed to directly quantify BrC abundance. BrC was found to be prevalent throughout the 1 to 12 km altitude measurement range, with dramatic enhancements in biomass-burning plumes. BrC to black carbon (BC) ratios, under background tropospheric conditions, increased with altitude, consistent with a corresponding increase in the absorption Ångström exponent (AAE) determined from a three-wavelength particle soot absorption photometer (PSAP). The sum of inferred BC absorption and measured BrC absorption at 365 nm was within 3 % of the measured PSAP absorption for background conditions and 22 % for biomass burning. A radiative transfer model showed that BrC absorption reduced top-of-atmosphere (TOA) aerosol forcing by ~ 20 % in the background troposphere. Extensive radiative model simulations applying this study background tropospheric conditions provided a look-up chart for determining radiative forcing efficiencies of BrC as a function of a surface-measured BrC : BC ratio and single scattering albedo (SSA). The chart is a first attempt to provide a tool for better assessment of brown carbon's forcing effect when one is limited to only surface data. These results indicate that BrC is an important contributor to direct aerosol radiative forcing.

During the July 2011 Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) field experiment in Maryland, significant enhancements in Aerosol Robotic Network (AERONET) sun–sky radiometer measured aerosol optical depth (AOD) were observed in the immediate vicinity of non-precipitating cumulus clouds on some days. Both measured Ångström exponents and aerosol size distribution retrievals made before, during and after cumulus development often suggest little change in fine mode particle size; therefore, implying possible new particle formation in addition to cloud processing and humidification of existing particles. In addition to sun–sky radiometer measurements of large enhancements of fine mode AOD, lidar measurements made from both ground-based and aircraft-based instruments during the experiment also measured large increases in aerosol signal at altitudes associated with the presence of fair weather cumulus clouds. These data show modifications of the aerosol vertical profile as a result of the aerosol enhancements at and below cloud altitudes. The airborne lidar data were utilized to estimate the spatial extent of these aerosol enhancements, finding increased AOD, backscatter and extinction out to 2.5 km distance from the cloud edge. Furthermore, in situ measurements made from aircraft vertical profiles over an AERONET site during the experiment also showed large increases in aerosol scattering and aerosol volume after cloud formation as compared to before. The 15-year AERONET database of AOD measurements at the Goddard Space Flight Center (GSFC), Maryland site, was investigated in order to obtain a climatological perspective of this phenomenon of AOD enhancement. Analysis of the diurnal cycle of AOD in summer showed significant increases in AOD from morning to late afternoon, corresponding to the diurnal cycle of cumulus development.

Retrievals of aerosol microphysical properties (effective radius, volume and surface-area concentrations) and aerosol optical properties (complex index of refraction and single-scattering albedo) were obtained from a hybrid multiwavelength lidar data set for the first time. In July 2011, in the Baltimore–Washington DC region, synergistic profiling of optical and microphysical properties of aerosols with both airborne (in situ and remote sensing) and ground-based remote sensing systems was performed during the first deployment of DISCOVER-AQ. The hybrid multiwavelength lidar data set combines ground-based elastic backscatter lidar measurements at 355 nm with airborne High-Spectral-Resolution Lidar (HSRL) measurements at 532 nm and elastic backscatter lidar measurements at 1064 nm that were obtained less than 5 km apart from each other. This was the first study in which optical and microphysical retrievals from lidar were obtained during the day and directly compared to AERONET and in situ measurements for 11 cases. Good agreement was observed between lidar and AERONET retrievals. Larger discrepancies were observed between lidar retrievals and in situ measurements obtained by the aircraft and aerosol hygroscopic effects are believed to be the main factor in such discrepancies.

During the NASA DISCOVER-AQ campaign over the US Baltimore, MD–Washington, D.C., metropolitan area in July 2011, the NASA P-3B aircraft performed extensive profiling of aerosol optical, chemical, and microphysical properties. These in situ profiles were coincident with ground-based remote sensing (AERONET) and in situ (PM2.5) measurements. Here, we use this data set to study the correlation between the PM2.5 observations at the surface and the column integrated measurements. Aerosol optical depth (AOD550 nm) calculated with the extinction (550 nm) measured during the in situ profiles was found to be strongly correlated with the volume of aerosols present in the boundary layer (BL). Despite the strong correlation, some variability remains, and we find that the presence of aerosol layers above the BL (in the buffer layer – BuL) introduces significant uncertainties in PM2.5 estimates based on column-integrated measurements (overestimation of PM2.5 by a factor of 5). This suggests that the use of active remote sensing techniques would dramatically improve air quality retrievals. Indeed, the relationship between the AOD550 nm and the PM2.5 is strongly improved by accounting for the aerosol present in and above the BL (i.e., integrating the aerosol loading from the surface to the top of the BuL). Since more than 15% of the AOD values observed during DISCOVER-AQ are dominated by aerosol water uptake, the f(RH)amb (ratio of scattering coefficient at ambient relative humidity (RH) to scattering coefficient at low RH; see Sect. 3.2) is used to study the impact of the aerosol hygroscopicity on the PM2.5 retrievals. The results indicate that PM2.5 can be predicted within a factor up to 2 even when the vertical variability of the f(RH)amb is assumed to be negligible. Moreover, f(RH = 80%) and RH measurements performed at the ground may be used to estimate the f(RH)amb during dry conditions (RHBL < 55%).

The use of alternative fuels for aviation is likely to increase due to concerns over fuel security, price stability, and the sustainability of fuel sources. Concurrent reductions in particulate emissions from these alternative fuels are expected because of changes in fuel composition including reduced sulfur and aromatic content. The NASA Alternative Aviation Fuel Experiment (AAFEX) was conducted in January–February 2009 to investigate the effects of synthetic fuels on gas-phase and particulate emissions. Standard petroleum JP-8 fuel, pure synthetic fuels produced from natural gas and coal feedstocks using the Fischer–Tropsch (FT) process, and 50% blends of both fuels were tested in the CFM-56 engines on a DC-8 aircraft. To examine plume chemistry and particle evolution with time, samples were drawn from inlet probes positioned 1, 30, and 145 m downstream of the aircraft engines. No significant alteration to engine performance was measured when burning the alternative fuels. However, leaks in the aircraft fuel system were detected when operated with the pure FT fuels as a result of the absence of aromatic compounds in the fuel. Dramatic reductions in soot emissions were measured for both the pure FT fuels (reductions in mass of 86% averaged over all powers) and blended fuels (66%) relative to the JP-8 baseline with the largest reductions at idle conditions. At 7% power, this corresponds to a reduction from 7.6 mg kg−1 for JP-8 to 1.2 mg kg−1 for the natural gas FT fuel. At full power, soot emissions were reduced from 103 to 24 mg kg−1 (JP-8 and natural gas FT, respectively). The alternative fuels also produced smaller soot (e.g., at 85% power, volume mean diameters were reduced from 78 nm for JP-8 to 51 nm for the natural gas FT fuel), which may reduce their ability to act as cloud condensation nuclei (CCN). The reductions in particulate emissions are expected for all alternative fuels with similar reductions in fuel sulfur and aromatic content regardless of the feedstock. As the plume cools downwind of the engine, nucleation-mode aerosols form. For the pure FT fuels, reductions (94% averaged over all powers) in downwind particle number emissions were similar to those measured at the exhaust plane (84%). However, the blended fuels had less of a reduction (reductions of 30–44%) than initially measured (64%). The likely explanation is that the reduced soot emissions in the blended fuel exhaust plume results in promotion of new particle formation microphysics, rather than coating on pre-existing soot particles, which is dominant in the JP-8 exhaust plume. Downwind particle volume emissions were reduced for both the pure (79 and 86% reductions) and blended FT fuels (36 and 46%) due to the large reductions in soot emissions. In addition, the alternative fuels had reduced particulate sulfate production (near zero for FT fuels) due to decreased fuel sulfur content. To study the formation of volatile aerosols (defined as any aerosol formed as the plume ages) in more detail, tests were performed at varying ambient temperatures (−4 to 20 °C). At idle, particle number and volume emissions were reduced linearly with increasing ambient temperature, with best fit slopes corresponding to −8 × 1014 particles (kg fuel)−1 °C−1 for particle number emissions and −10 mm3 (kg fuel)−1 °C−1 for particle volume emissions. The temperature dependency of aerosol formation can have large effects on local air quality surrounding airports in cold regions. Aircraft-produced aerosols in these regions will be much larger than levels expected based solely on measurements made directly at the engine exit plane. The majority (90% at idle) of the volatile aerosol mass formed as nucleation-mode aerosols, with a smaller fraction as a soot coating. Conversion efficiencies of up to 2.8% were measured for the partitioning of gas-phase precursors (unburned hydrocarbons and SO2) to form volatile aerosols. Highest conversion efficiencies were measured at 45% power.

Contrails and contrail-induced cirrus clouds are identified as the most uncertain components in determining aviation impacts on global climate change. Parameters affecting contrail ice particle formation immediately after the engine exit plane (< 5 s in plume age) may be critical to ice particle properties used in large-scale models predicting contrail radiative forcing. Despite this, detailed understanding of these parametric effects is still limited. In this paper, we present results from recent laboratory and modeling studies conducted to investigate the effects of water and soot emissions and ambient conditions on near-field formation of contrail ice particles and ice particle properties. The Particle Aerosol Laboratory (PAL) at the NASA Glenn Research Center and the Aerodyne microphysical parcel model for contrail ice particle formation were employed. Our studies show that exhaust water concentration has a significant impact on contrail ice particle formation and properties. When soot particles were introduced, ice particle formation was observed only when exhaust water concentration was above a critical level. When no soot or sulfuric acid was introduced, no ice particle formation was observed, suggesting that ice particle formation from homogeneous nucleation followed by homogeneous freezing of liquid water was unfavorable. Soot particles were found to compete for water vapor condensation, and higher soot concentrations emitted into the chamber resulted in smaller ice particles being formed. Chamber conditions corresponding to higher cruising altitudes were found to favor ice particle formation. The microphysical model captures trends of particle extinction measurements well, but discrepancies between the model and the optical particle counter measurements exist as the model predicts narrower ice particle size distributions and ice particle sizes nearly a factor of two larger than measured. These discrepancies are likely due to particle loss and scatter during the experimental sampling process and the lack of treatment of turbulent mixing in the model. Our combined experimental and modeling work demonstrates that formation of contrail ice particles can be reproduced in the NASA PAL facility, and the parametric understanding of the ice particle properties from the model and experiments can potentially be used in large-scale models to provide better estimates of the impact of aviation contrails on climate change.

The NASA DC-8 aircraft characterized the aerosol properties, chemical composition, and cloud condensation nuclei (CCN) concentrations of the summertime Arctic during the 2008 NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. Air masses characteristic of fresh and aged biomass burning, boreal forest, Arctic background, and anthropogenic industrial pollution were sampled. Observations were spatially extensive (50–85° N and 40–130° W) and exhibit significant variability in aerosol and CCN concentrations. The chemical composition was dominated by highly oxidized organics (66–94% by volume), with a water-soluble mass fraction of more than 50%. The aerosol hygroscopicity parameter, κ, ranged between κ = 0.08–0.32 for all air mass types. Industrial pollution had the lowest κ of 0.08 ± 0.01, while the Arctic background had the highest and most variable κ of 0.32 ± 0.21, resulting from a lower and more variable organic fraction. Both fresh and aged (long-range transported) biomass burning air masses exhibited remarkably similar κ (0.18 ± 0.13), consistent with observed rapid chemical and physical aging of smoke emissions in the atmosphere, even in the vicinity of fresh fires. The organic hygroscopicity (κorg) was parameterized by the volume fraction of water-soluble organic matter (εWSOM), with a κ = 0.12, such that κorg = 0.12εWSOM. Assuming bulk (size-independent) composition and including the κorg parameterization enabled CCN predictions to within 30% accuracy for nearly all environments sampled. The only exception was for industrial pollution from Canadian oil sands exploration, where an external mixture and size-dependent composition was required. Aerosol mixing state assumptions (internal vs. external) in all other environments did not significantly affect CCN predictions; however, the external mixing assumption provided the best results, even though the available observations could not determine the true degree of external mixing and therefore may not always be representative of the environments sampled. No correlation was observed between κorg and O : C. A novel correction of the CCN instrument supersaturation for water vapor depletion, resulting from high concentrations of CCN, was also employed. This correction was especially important for fresh biomass burning plumes where concentrations exceeded 1.5×104 cm−3 and introduced supersaturation depletions of &geq;25%. Not accounting for supersaturation depletion in these high concentration environments would therefore bias CCN closure up to 25% and inferred κ by up to 50%.

Actinic flux, as well as aerosol chemical and optical properties, were measured aboard the NASA DC-8 aircraft during the ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) mission in Spring and Summer 2008. These measurements were used in a radiative transfer code to retrieve spectral (350–550 nm) aerosol single scattering albedo (SSA) for biomass burning plumes encountered on 17 April and 29 June. Retrieved SSA values were subsequently used to calculate the absorption Angstrom exponent (AAE) over the 350–500 nm range. Both plumes exhibited enhanced spectral absorption with AAE values that exceeded 1 (6.78 &pm; 0.38 for 17 April and 3.34 &pm; 0.11 for 29 June). This enhanced absorption was primarily due to organic aerosol (OA) which contributed significantly to total absorption at all wavelengths for both 17 April (57.7%) and 29 June (56.2%). OA contributions to absorption were greater at UV wavelengths than at visible wavelengths for both cases. Differences in AAE values between the two cases were attributed to differences in plume age and thus to differences in the ratio of OA and black carbon (BC) concentrations. However, notable differences between AAE values calculated for the OA (AAEOA) for 17 April (11.15 &pm; 0.59) and 29 June (4.94 &pm; 0.19) suggested differences in the plume AAE values might also be due to differences in organic aerosol composition. The 17 April OA was much more oxidized than the 29 June OA as denoted by a higher oxidation state value for 17 April (&plus;0.16 vs. −0.32). Differences in the AAEOA, as well as the overall AAE, were thus also possibly due to oxidation of biomass burning primary organic aerosol in the 17 April plume that resulted in the formation of OA with a greater spectral-dependence of absorption.

In the spring of 2008 NASA and NOAA funded the ARCTAS and ARCPAC field campaigns as contributions to POLARCAT, a core IPY activity. During the campaigns the NASA DC-8, P-3B and NOAA WP-3D aircraft conducted over 160 h of in-situ sampling between 0.1 and 12 km throughout the Western Arctic north of 55° N (i.e. Alaska to Greenland). All aircraft were equipped with multiple wavelength measurements of aerosol optics, trace gas and aerosol chemistry measurements, as well as direct measurements of the aerosol size distributions and black carbon mass. Late April of 2008 proved to be exceptional in terms of Asian biomass burning emissions transported to the Western Arctic. Though these smoke plumes account for only 11–14 % of the samples within the Western Arctic domain, they account for 42–47 % of the total burden of black carbon. Dust was also commonly observed but only contributes to 4–12 % and 3–8 % of total light absorption at 470 and 530 nm wavelengths above 6 km. Below 6 km, light absorption by carbonaceous aerosol derived from urban/industrial and biomass burning emissions account for 97–99 % of total light absorption by aerosol. Stratifying the data to reduce the influence of dust allows us to determine mass absorption efficiencies for black carbon of 11.2±0.8, 9.5±0.6 and 7.4±0.7 m2 g−1 at 470, 530 and 660 nm wavelengths. These estimates are consistent with 35–80 % enhancements in 530 nm absorption due to clear or slightly absorbing coatings of pure black carbon particulate. Assuming a 1/λ wavelength dependence for BC absorption, and assuming that refractory aerosol (420 °C, τ = 0.1 s) in low-dust samples is dominated by brown carbon, we derive mass absorption efficiencies for brown carbon of 0.83±0.15 and 0.27±0.08 m2 g−1 at 470 and 530 nm wavelengths. Estimates for the mass absorption efficiencies of Asian dust are 0.034 m2 g−1 and 0.017 m2 g−1. However the absorption efficiency estimates for dust are highly uncertain due to the limitations imposed by PSAP instrument noise. In-situ ARCTAS/ARCPAC measurements during the IPY provide valuable constraints for absorbing aerosol over the Western Arctic, species which are currently poorly simulated over a region that is critically under-sampled.

As part of the international project entitled "African Monsoon Multidisciplinary Analysis (AMMA)", NAMMA (NASA AMMA) aimed to gain a better understanding of the relationship between the African Easterly Waves (AEWs), the Sahara Air Layer (SAL), and tropical cyclogenesis. The NAMMA airborne field campaign was based out of the Cape Verde Islands during the peak of the hurricane season, i.e., August and September 2006. Multiple Sahara dust layers were sampled during 62 encounters in the eastern portion of the hurricane main development region, covering both the eastern North Atlantic Ocean and the western Saharan desert (i.e., 5–22° N and 10–35° W). The centers of these layers were located at altitudes between 1.5 and 3.3 km and the layer thickness ranged from 0.5 to 3 km. Detailed dust microphysical and optical properties were characterized using a suite of in-situ instruments aboard the NASA DC-8 that included a particle counter, an Ultra-High Sensitivity Aerosol Spectrometer, an Aerodynamic Particle Sizer, a nephelometer, and a Particle Soot Absorption Photometer. The NAAMA sampling inlet has a size cut (i.e., 50% transmission efficiency size) of approximately 4 μm in diameter for dust particles, which limits the representativeness of the NAMMA observational findings. The NAMMA dust observations showed relatively low particle number densities, ranging from 268 to 461 cm−3, but highly elevated volume density with an average at 45 μm3 cm−3. NAMMA dust particle size distributions can be well represented by tri-modal lognormal regressions. The estimated volume median diameter (VMD) is averaged at 2.1 μm with a small range of variation regardless of the vertical and geographical sampling locations. The Ångström Exponent assessments exhibited strong wavelength dependence for absorption but a weak one for scattering. The single scattering albedo was estimated at 0.97 ± 0.02. The imaginary part of the refractive index for Sahara dust was estimated at 0.0022, with a range from 0.0015 to 0.0044. Closure analysis showed that observed scattering coefficients are highly correlated with those calculated from spherical Mie-Theory and observed dust particle size distributions. These values are generally consistent with literature values reported from studies with similar particle sampling size range.

In-situ airborne measurements of trace gases, aerosol size distributions, chemistry and optical properties were conducted over Mexico and the Eastern North Pacific during MILAGRO and INTEX-B. Heterogeneous reactions between secondary aerosol precursor gases and mineral dust lead to sequestration of sulfur, nitrogen and chlorine in the supermicrometer particulate size range. Simultaneous measurements of aerosol size distributions and weak-acid soluble calcium result in an estimate of 11 wt% of CaCO3 for Asian dust. During transport across the North Pacific, ~5–30% of the CaCO3 is converted to CaSO4 or Ca(NO3)2 with an additional ~4% consumed through reactions with HCl. The 1996 to 2008 record from the Mauna Loa Observatory confirm these findings, indicating that, on average, 19% of the CaCO3 has reacted to form CaSO4 and 7% has reacted to form Ca(NO3)2 and ~2% has reacted with HCl. In the nitrogen-oxide rich boundary layer near Mexico City up to 30% of the CaCO3 has reacted to form Ca(NO3)2 while an additional 8% has reacted with HCl. These heterogeneous reactions can result in a ~3% increase in dust solubility which has an insignificant effect on their optical properties compared to their variability in-situ. However, competition between supermicrometer dust and submicrometer primary aerosol for condensing secondary aerosol species led to a 25% smaller number median diameter for the accumulation mode aerosol. A 10–25% reduction of accumulation mode number median diameter results in a 30–70% reduction in submicrometer light scattering at relative humidities in the 80–95% range. At 80% RH submicrometer light scattering is only reduced ~3% due to a higher mass fraction of hydrophobic refractory components in the dust-affected accumulation mode aerosol. Thus reducing the geometric mean diameter of the submicrometer aerosol has a much larger effect on aerosol optical properties than changes to the hygroscopic:hydrophobic mass fractions of the accumulation mode aerosol. In the presence of dust, nitric acid concentrations are reduced to y as a fraction of total nitrogen (NOy plus particulate nitrate), is reduced from >85% to 60–80% in the presence of dust. These observations support previous model studies which predict irreversible sequestration of reactive nitrogen species through heterogeneous reactions with mineral dust during long-range transport.