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Armin Sorooshian

Publications and source records attributed to Armin Sorooshian.

At least 19 records

Summarizing Multiple Aspects of Triple Collocation Analysis in a Single Diagram

With the ongoing expansion of global observation networks, it is expected that we shall routinely analyze records of geophysical variables such as temperature from multiple collocated instruments. Validating datasets in this situation is not a trivial task because every observing system has its own bias and noise. Triple collocation is a general statistical framework to estimate the error characteristics in three or more observational-based datasets. In a triple colocation analysis, several metrics are routinely reported but traditional multiple-panel plots are not the most effective way to display information. A new formula of error variance is derived for connecting the key terms in the triple collocation theory. A diagram based on this formula is devised to facilitate triple collocation analysis of any data from observations, as illustrated using three aerosol optical depth datasets from the recent Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE). An observational-based skill score is also derived to evaluate the quality of three datasets by taking into account both error variance and correlation coefficient. Several applications are discussed and sample plotting routines are provided.

triple collocation↗

High Spectral Resolution Lidar – Generation 2 (HSRL-2) Retrievals of Ocean Surface Wind Speed: Methodology and Evaluation

Ocean surface wind speed (i.e., wind speed 10 m above sea level) is a critical parameter used by atmospheric models to estimate the state of the marine atmospheric boundary layer (MABL). Accurate surface wind speed measurements in diverse locations are required to improve characterization of MABL dynamics and assess how models simulate large-scale phenomena related to climate change and global weather patterns. To provide these measurements, this study introduces and evaluates a new surface wind speed data product from the NASA Langley Research Center nadir-viewing High Spectral Resolution Lidar – generation 2 (HSRL-2) using data collected as part of the NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) mission. The HSRL-2 can directly measure vertically resolved aerosol backscatter and extinction profiles without additional constraints or assumptions, enabling the instrument to accurately derive atmospheric attenuation and directly determine surface reflectance (i.e., surface backscatter). Also, the high horizontal spatial resolution of the HSRL-2 retrievals (0.5 s or ∼ 75 m along track) allows the instrument to probe the fine-scale spatial variability in surface wind speeds over time along the flight track and over breaks in broken cloud fields. A rigorous evaluation of these retrievals is performed by comparing coincident HSRL-2 and National Center for Atmospheric Research (NCAR) Airborne Vertical Atmosphere Profiling System (AVAPS) dropsonde data, owing to the joint deployment of these two instruments on the ACTIVATE King Air aircraft. These comparisons show correlations of 0.89, slopes of 1.04 and 1.17, and y intercepts of −0.13 and −1.05 m s−1 for linear and bisector regressions, respectively, and the overall accuracy is calculated to be 0.15 ± 1.80 m s−1. It is also shown that the dropsonde surface wind speed data most closely follow the HSRL-2 distribution of wave slope variance using the distribution proposed by Hu et al. (2008) rather than the ones proposed by Cox and Munk (1954) and Wu (1990) for surface wind speeds below 7 m s−1, with this category comprising most of the ACTIVATE data set. The retrievals are then evaluated separately for surface wind speeds below 7 m s−1 and between 7 and 13.3 m s−1 and show that the HSRL-2 retrieves surface wind speeds with a bias of ∼ 0.5 m s−1 and an error of ∼ 1.5 m s−1, a finding not apparent in the cumulative comparisons. Also, it is shown that the HSRL-2 retrievals are more accurate in the summer (−0.18 ± 1.52 m s−1) than in the winter (0.63 ± 2.07 m s−1), but the HSRL-2 is still able to make numerous (N=236) accurate retrievals in the winter. Overall, this study highlights the abilities and assesses the performance of the HSRL-2 surface wind speed retrievals, and it is hoped that further evaluation of these retrievals will be performed using other airborne and satellite data sets.

Sanja Dmitrovic↗

Retrievals of Aerosol Optical Depth Over the Western North Atlantic Ocean During ACTIVATE

Aerosol optical depth was retrieved from two airborne remote sensing instruments, the Research Scanning Polarimeter (RSP) and Second Generation High Spectral Resolution Lidar (HSRL-2), during the National Aeronautics and Space Administration (NASA) Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE). The field campaign offers a unique opportunity to evaluate an extensive 3-year dataset under a wide range of meteorological conditions from two instruments on the same platform. However, a long-standing issue in atmospheric field studies is that there is a lack of reference datasets for properly validating field measurements and estimating their uncertainties. Here we address this issue by using the triple collocation method, in which a third collocated satellite dataset from the Moderate Resolution Imaging Spectroradiometer (MODIS) is introduced for comparison. HSRL-2 is found to provide a more accurate retrieval than RSP over the study region. The error standard deviation of HSRL-2 with respect to the ground truth is 0.027. Moreover, this approach enables us to develop a simple, yet efficient, quality control criterion for RSP data. The physical reasons for the differences in two retrievals are determined to be cloud contamination, aerosols near the surface, multiple aerosol layers, absorbing aerosols, non-spherical aerosols, and simplified retrieval assumptions. These results demonstrate the pathway for optimal aerosol retrievals by combining information from both lidars and polarimeters for future airborne and satellite missions.

Aerosol optical depth↗

Sea Salt Reactivity Over the Northwest Atlantic: an in-Depth Look Using the Airborne ACTIVATE Dataset

Chloride (Cl−) displacement from sea salt particles is an extensively studied phenomenon with implications for human health, visibility, and the global radiation budget. Past works have investigated Cl− depletion over the northwest Atlantic (NWA); however, an updated, multi-seasonal, and geographically expanded account of sea salt reactivity over the region is needed. This study uses chemically resolved mass concentrations and meteorological data from the airborne Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) to quantify seasonal, spatial, and meteorological trends in Cl− depletion and to explore the importance of quantifying (1) non-sea salt sources of Na+ and (2) mass concentrations of lost Cl− (instead of relative amounts displaced). Lost Cl− mass concentrations are lowest in December–February and March, moderate around Bermuda in June, and highest in May (median losses of 0.04, 0.04, 0.66, and 1.76µgm−3, respectively), with losses in May that are high enough to potentially accelerate tropospheric oxidation rates. Inorganic acidic species can account for all Cl− depletion in December–February, March, and June near Bermuda but none of the lost Cl− in May, suggesting that organic acids may be of importance for Cl− displacement in certain months. Contributions of dust to Na+ are not important seasonally but may cause relevant overestimates of lost Cl− in smoke and dust plumes. Higher percentages of Cl− depletion often do not correspond to larger mass concentrations of lost Cl−, so it is highly recommended to quantify the latter to place depletion reactions in context with their role in atmospheric oxidation and radiative forcing.

ACTIVATE↗

Maximizing the Volume of Collocated Data from Two Coordinated Suborbital Platforms

Suborbital (e.g., airborne) campaigns that carry advanced remote sensing and in situ payloads provide detailed observations of atmospheric processes, but can be challenging to use when it is necessary to geographically collocate data from multiple platforms that make repeated observations of a given geographic location at different altitudes. This study reports on a data collocation algorithm that maximizes the volume of collocated data from two coordinated suborbital platforms and demonstrates its value using data from the NASA Aerosol Cloud Meteorology Interactions Over the western Atlantic Experiment (ACTIVATE) suborbital mission. A robust data collocation algorithm is critical for the success of the ACTIVATE mission goal to develop new and improved remote sensing algorithms, and quantify their performance. We demonstrate the value of these collocated data to quantify the performance of a recently developed vertically resolved lidar + polarimeter–derived aerosol particle number concentration (Na ) product, resulting in a range-normalized mean absolute deviation (NMAD) of 9% compared to in situ measurements. We also show that this collocation algorithm increases the volume of collocated ACTIVATE data by 21% compared to using only nearest-neighbor finding algorithms alone. Additional to the benefits demonstrated within this study, the data files and routines produced by this algorithm have solved both the critical collocation and the collocation application steps for researchers who require collocated data for their own studies. This freely available and open-source collocation algorithm can be applied to future suborbital campaigns that, like ACTIVATE, use multiple platforms to conduct coordinated observations, e.g., a remote sensing aircraft together with in situ data collected from suborbital platforms.

Atmosphere↗

Overview and Statistical Analysis of Boundary Layer Clouds and Precipitation Over the Western North Atlantic Ocean

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 (N liquid ) 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 N liquid 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.

Aerosol↗

Spatially-Coordinated Airborne Data and Complementary Products for Aerosol, Gas, Cloud, and Meteorological Studies: the Nasa Activate Dataset

The NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) produced a unique dataset for research into aerosol–cloud–meteorology interactions, with applications extending from process-based studies to multi-scale model intercomparison and improvement as well as to remote-sensing algorithm assessments and advancements. ACTIVATE used two NASA Langley Research Center aircraft, a HU-25 Falcon and King Air, to conduct systematic and spatially coordinated flights over the northwest Atlantic Ocean, resulting in 162 joint flights and 17 other single-aircraft flights between 2020 and 2022 across all seasons. Data cover 574 and 592 cumulative flights hours for the HU-25 Falcon and King Air, respectively. The HU-25 Falcon conducted profiling at different level legs below, in, and just above boundary layer clouds (< 3 km) and obtained in situ measurements of trace gases, aerosol particles, clouds, and atmospheric state parameters. Under cloud-free conditions, the HU-25 Falcon similarly conducted profiling at different level legs within and immediately above the boundary layer. The King Air (the high-flying aircraft) flew at approximately ∼ 9 km and conducted remote sensing with a lidar and polarimeter while also launching dropsondes (785 in total). Collectively, simultaneous data from both aircraft help to characterize the same vertical column of the atmosphere. In addition to individual instrument files, data from the HU-25 Falcon aircraft are combined into “merge files” on the publicly available data archive that are created at different time resolutions of interest (e.g., 1, 5, 10, 15, 30, 60 s, or matching an individual data product's start and stop times). This paper describes the ACTIVATE flight strategy, instrument and complementary dataset products, data access and usage details, and data application notes. The data are publicly accessible through https://doi.org/10.5067/SUBORBITAL/ACTIVATE/DATA001 (ACTIVATE Science Team, 2020).

Aerosol Cloud meTeorology Interactions oVer the we↗

Uncertainty in Aerosol–Cloud Radiative Forcing Is Driven By Clean Conditions

Atmospheric aerosols and their impact on cloud properties remain the largest uncertainty in the human forcing of the climate system. By increasing the concentration of cloud droplets (Nd), aerosols reduce droplet size and increase the reflectivity of clouds (a negative radiative forcing). Central to this climate impact is the susceptibility of cloud droplet number to aerosol (β), the diversity of which explains much of the variation in the radiative forcing from aerosol–cloud interactions (RFaci) in global climate models. This has made measuring β a key target for developing observational constraints of the aerosol forcing.

Edward Gryspeerdt↗

Large-Eddy Simulations of Marine Boundary Layer Clouds Associated with Cold-Air Outbreaks during the ACTIVATE Campaign. Part II: Aerosol–Meteorology–Cloud Interaction

Aerosol effects on micro/macrophysical properties of marine stratocumulus clouds over the western North Atlantic Ocean (WNAO) are investigated using in situ measurements and large-eddy simulations (LES) for two cold-air outbreak (CAO) cases (28 February and 1 March 2020) during the Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE). The LES is able to reproduce the vertical profiles of liquid water content (LWC), effective radius reff and cloud droplet number concentration Nc from fast cloud droplet probe (FCDP) in situ measurements for both cases. Furthermore, we show that aerosols affect cloud properties (N c , r eff , and LWC) via the prescribed bulk hygroscopicity of aerosols (¯k) and aerosol size distribution characteristics. N c , r eff , and liquid water path (LWP) are positively correlated to ¯κ and aerosol number concentration (N a ) while cloud fractional cover (CFC) is insensitive to ¯κ and aerosol size distributions for the two cases. The realistic changes to aerosol size distribution (number concentration, width, and the geometrical diameter) with the same meteorology state allow us to investigate aerosol effects on cloud properties without meteorological feedback. We also use the LES results to evaluate cloud properties from two reanalysis products, ERA5 and MERRA-2. Compared to LES, the ERA5 is able to capture the time evolution of LWP and total cloud coverage within the study domain during both CAO cases while MERRA-2 underestimates them.

Cloud forcing↗

A Cloud Detection Neural Network for Above-Aircraft Clouds Using Airborne Cameras

We introduce a method convolutional neural networks to detect the presence of clouds in airborne camera images. We quantify the performance of this Cloud Detection Neural Network (CDNN) using human-labeled validation data where we report a 96% accuracy in detecting clouds in testing datasets for both Zenith- viewing and Forward-viewing models. We assess our performance by comparing the flight-averaged cloud fraction of zenith and forward CDNN retrievals, with that of the prototype hyperspectral total-diffuse Sunshine Pyranometer (SPN-S) instrument’s cloud optical depth data. Comparison of the CDNN with the SPN-S on time specific intervals resulted in 93% accuracy for the zenith- viewing CDNN and 84% for the forward- viewing CDNN. The comparison of the CDNNs with the SPN-S on flight-averaged cloud fraction resulted in an agreement of 0.15 for the Forward CDNN and 0.07 for the Zenith CDNN. We then quantify the ability of the CDNN to identify the presence of clouds above the aircraft using a forward- looking camera mounted inside the aircraft cockpit compared to the use of an All- Sky upward-looking camera that is mounted outside the fuselage on top of the aircraft. We present results from the CDNN based on airborne imagery from the NASA Aerosol Cloud Meteorology Interactions Over the Western Atlantic Experiment (ACTIVATE) and the Clouds, Aerosol and Monsoon Processes- Philippines Experiment (CAMP2Ex). For CAMP2Ex 53% of flight dates had above- aircraft cloud fraction above 50%, while for ACTIVATE 52% and 54% of flight dates observed above-aircraft cloud fraction above 50% for 2020 and 2021, respectively.

Joseph D Nied↗

Impact of Meteorological Factors on the Mesoscale Morphology of Cloud Streets during a Cold-Air Outbreak over the Western North Atlantic

Postfrontal clouds (PFC) are ubiquitous in the marine boundary layer, and their morphology is essential to estimating the radiation budget in weather and climate models. Here we examine the roles of sea surface temperature (SST) and meteorological factors in controlling the mesoscale morphology and evolution of shallow clouds associated with a cold-air outbreak that occurred on 1 March 2020 during phase I of the Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE). Our results show that the simulated PFC structure and ambient conditions by the Weather Research and Forecasting (WRF) Model are generally consistent with observations from GOES-16 and dropsonde measurements. We also examine the thermodynamical and dynamical influences in the cloud mesoscale morphology using WRF sensitivity experiments driven by two meteorological forcing datasets with different domain-mean SST and spatial gradients, which lead to dissimilar values of hydrometeor water path and cloud core fraction. The SST from ERA5 leads to weaker stability and higher inversion height than the SST from FNL does. In addition, the use of large-scale meteorological forcings from ERA5 yields a distinctive time evolution of wind direction shear in the inner domain, which favors the formation and persistence of longer cloud rolls. Both factors contribute to a change in the time evolution of domain-mean water path and cloud core fraction of cloud streets. Our study takes advantage of the simulation driven by the differences between two large-scale forcing datasets to illustrate the importance of SST and wind direction shear in the cloud street morphology in a realistic scenario

Jingyi Chen↗

Measurement report: Closure Analysis of Aerosol–cloud Composition in Tropical Maritime Warm Convection

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.

Ewan Crosbie↗

The Impact of Sampling Strategy on the Cloud Droplet Number Concentration Estimated From Satellite Data

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.

Edward Gryspeerdt↗

Seasonal Updraft Speeds Change Cloud Droplet Number Concentrations in Low Level Clouds Over the Western North Atlantic

To determine the impact of dynamic and aerosol processes on marine low clouds, we examine the seasonal impact of updraft speed w and cloud condensation nuclei concentration at 0.43 % supersaturation () on the cloud droplet number concentration (N(C)) of low-level clouds over the western North Atlantic Ocean. Aerosol and cloud properties were measured with instruments on board the NASA LaRC Falcon HU-25 during the ACTIVATE (Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment) mission in summer (August) and winter (February–March) 2020. The data are grouped into different loadings, and the density functions of NC and w near the cloud bases are compared. For low updrafts (w < 1.3 m s−1), NC in winter is mainly limited by the updraft speed and in summer additionally by aerosols. At larger updrafts (w > 3 m s−1), NC is impacted by the aerosol population, while at clean marine conditions cloud nucleation is aerosol-limited, and for high it is influenced by aerosols and updraft. The aerosol size distribution in winter shows a bimodal distribution in clean marine environments, which transforms to a unimodal distribution in high due to chemical and physical aerosol processes, whereas unimodal distributions prevail in summer, with a significant difference in their aerosol concentration and composition. The increase of is accompanied with an increase of organic aerosol and sulfate compounds in both seasons. We demonstrate that NC can be explained by cloud condensation nuclei activation through upwards processed air masses with varying fractions of activated aerosols. The activation highly depends on w and thus supersaturation between the different seasons, while the aerosol size distribution additionally affects NC within a season. Our results quantify the seasonal influence of w and on NC and can be used to improve the representation of low marine clouds in models.

Simon Kirschler↗

Polarimeter + Lidar–Derived Aerosol Particle Number Concentration

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).

RSP↗

Identifying Chemical Aerosol Signatures Using Optical Suborbital Observations: How Much Can Optical Properties Tell us about Aerosol Composition?

Improvements in air quality and Earth’s climate predictions require improvements of the aerosol speciation in chemical transport models, using observational constraints. Aerosol speciation (e.g., organic aerosols, black carbon, sulfate, nitrate, ammonium, dust or sea salt) is typically determined using in situ instrumentation. Continuous, routine surface network aerosol composition measurements are not uniformly widespread over the globe. Satellites, on the other hand, can provide a maximum coverage of the horizontal and vertical atmosphere but observe aerosol optical properties (and not aerosol speciation) based on remote sensing instrumentation. Combinations of satellite-derived aerosol optical properties can inform on air mass aerosol types (AMTs e.g., clean marine, dust, polluted continental). However, these AMTs are subjectively defined, might often be misclassified and are hard to relate to the critical parameters that need to be refined in models. In this paper, we derive AMTs that are more directly related to sources and hence to speciation. They are defined, characterized, and derived using simultaneous in situ gas-phase, chemical and optical instruments on the same aircraft during the Study of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS, US, summer of 2013). First, we prescribe well-informed AMTs that display distinct aerosol chemical and optical signatures to act as a training AMT dataset. These in situ observations reduce the errors and ambiguities in the selection of the AMT training dataset. We also investigate the relative skill of various combinations of aerosol optical properties to define AMTs and how much these optical properties can capture dominant aerosol speciation. We find distinct optical signatures for biomass burning (from agricultural or wildfires), biogenic and dust-influence AMTs. Useful aerosol optical properties to characterize these signatures are the extinction angstrom exponent (EAE), the single scattering albedo, the difference of single scattering albedo in two wavelengths, the absorption coefficient, the absorption angstrom exponent (AAE), and the real part of the refractive index (RRI). We find that all four AMTs studied when prescribed using mostly airborne in situ gas measurements, can be successfully extracted from at least three combinations of airborne in situ aerosol optical properties (e.g., EAE, AAE and RRI) over the US during SEAC4RS. However, we find that the optically based classifications for BB from agricultural fires and polluted dust include a large percentage of misclassifications that limit the usefulness of results relating to those classes. The technique and results presented in this study are suitable to develop a representative, robust and diverse source-based AMT database. This database could then be used for widespread retrievals of AMTs using existing and future remote sensing suborbital instruments/networks. Ultimately, it has the potential to provide a much broader observational aerosol data set to evaluate chemical transport and air quality models than is currently available by direct in situ measurements. This study illustrates how essential it is to explore existing airborne datasets to bridge chemical and optical signatures of different AMTs, before the implementation of future spaceborne missions (e.g., the next generation of Earth Observing System (EOS) satellites addressing Aerosol, Cloud, Convection and Precipitation (ACCP) designated observables).

Meloe S F Kacenelenbogen↗

Opportunistic Experiments to Constrain Aerosol Effective Radiative Forcing

Aerosol-cloud interactions (ACI) are considered to be the most uncertain driver of present-day radiative forcing due to human activities. The non-linearity of cloud-state changes to aerosol perturbations make it challenging to attribute causality in observed relationships of aerosol radiative forcing. Using correlations to infer causality can be challenging when meteorological variability also drives both aerosol and cloud changes independently. Natural and anthropogenic aerosol perturbations from well defined sources provide ‘opportunistic experiments’ (also known as natural experiments) to investigate ACI in cases where causality may be more confidently inferred. These perturbations cover a wide range of locations and spatio-temporal scales, including point sources such as volcanic eruptions or industrial sources, plumes from biomass burning or forest fires, and tracks from individual ships or shipping corridors.We review the different experimental conditions and conduct a synthesis of the available satellite data sets and field campaigns to place these opportunistic experiments on a common footing, facilitating new insights and a clearer understanding of key uncertainties in aerosol radiative forcing. Cloud albedo perturbations are strongly sensitive to background meteorological conditions. Strong liquid water path increases due to aerosol perturbations are largely ruled out by averaging across experiments. Opportunistic experiments have significantly improved process-level understanding of ACI, but it remains unclear how reliably the relationships found can be scaled to the global level, thus demonstrating a need for deeper investigation in order to improve assessments of aerosol radiative forcing and climate change.

Matthew W Christensen↗

An Overview of Atmospheric Features Over the Western North Atlantic Ocean and North American East Coast – Part 1: Analysis of Aerosols, Gases, and Wet Deposition Chemistry

The Western North Atlantic Ocean (WNAO) and adjoining East Coast of North America are of great importance for atmospheric research and have been extensively studied for several decades. This broad region exhibits complex meteorological features and a wide range of conditions associated with gas and particulate species from many sources regionally and other continents. As Part 1 of a 2‐part paper series, this work characterizes quantities associated with atmospheric chemistry, including gases, aerosols, and wet deposition, by analyzing available satellite observations, ground‐based data, model simulations, and reanalysis products. Part 2 provides insight into the atmospheric circulation, boundary layer variability, three‐dimensional cloud structure, properties, and precipitation over the WNAO domain. Key results include spatial and seasonal differences in composition along the North American East Coast and over the WNAO associated with varying sources of smoke and dust and meteorological drivers such as temperature, moisture, and precipitation. Spatial and seasonal variations of tropospheric carbon monoxide and ozone highlight different pathways towards the accumulation of these species in the troposphere. Spatial distributions of speciated aerosol optical depth and vertical profiles of aerosol mass mixing ratios show a clear seasonal cycle highlighting the influence of different sources in addition to the impact of intercontinental transport. Analysis of long‐term climate model simulations of aerosol species and satellite observations of carbon monoxide confirm that there has been a significant decline in recent decades among anthropogenic constituents owing to regulatory activities.

ACTIVATE↗