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All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Numerical case study of the aerosol–cloud interactions in warm boundary layer clouds over the eastern North Atlantic with an interactive chemistry module

The presence of warm boundary layer stratiform clouds over the eastern North Atlantic (ENA) region is commonly influenced by the Azores High, especially during the summer season. To investigate comprehensive aerosol–cloud interactions, this study employs the Weather Research and Forecasting model coupled with a chemistry component (WRF-Chem), incorporating aerosol chemical components that are relevant to the formation of cloud condensation nuclei (CCN) and accounting for aerosol spatiotemporal variation. This study focuses on aerosol indirect effects, particularly the long-range transport of aerosols, in the ENA region under three different weather regimes: a ridge with a surface high-pressure system, a post-trough with a surface high-pressure system, and a weak trough. The WRF-Chem simulations conducted at a near-large-eddy scale offer valuable insights into the model's performance, especially in terms of its ability to use high spatial resolution to capture mesoscale cloud features across various weather regimes. Our result shows that introducing 5 times more aerosols to either non-precipitating or precipitating clouds significantly increases ambient CCN numbers, resulting in, to varying degrees, higher liquid water path (LWP) values. The substantial aerosol–cloud interaction especially occurs in the precipitating clouds and demonstrates the susceptibility of the LWP to changes in CCN under different regimes. Conversely, thin, non-rain clouds at the edges of a cloud system are prone to evaporation, exhibiting an aerosol drying effect. The aerosols released during this process transition back to the accumulation mode, facilitating future activation. This dynamic behavior is not adequately represented in prescribed-aerosol simulations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Evaluation of E3SM Simulated Aerosols and Aerosol‐Cloud Interactions Across GCM and Convection‐Permitting Scales

This paper introduces an Earth system modeling testbed for predicting aerosols and aerosol‐cloud interactions (ACIs) at convection‐permitting scales. Using the Energy Exascale Earth System Model (E3SM) version 2 with a four‐mode Modal Aerosol Module, we conduct simulations at 3.25 km resolution on a regionally refined mesh (RRM) across four regions with distinct aerosol and cloud regimes. Results are compared with the standard 100 km E3SM configuration and evaluated against satellite, aircraft, and ground‐based observations. We find that increasing model resolution improves heavy precipitation simulation but amplifies positive bias in light drizzle at coarse resolution. These resolution‐induced changes affect cloud and aerosol properties to varying degrees across regions. Generally, cloud cover and liquid water path (LWP) show better agreement with satellite retrievals at 3.25 km, though surface‐based comparisons suggest otherwise. Aerosol composition remains poorly represented at both resolutions. The RRM increases Aitken mode aerosol number concentrations via enhanced new particle formation. However, accumulation mode aerosols are decreased at higher resolution as aerosol removals become more efficient. This partially contributes to fewer cloud condensation nuclei (CCN) and lower cloud droplet number concentrations (N d ), which produces larger model biases in some scenarios. These findings suggest that solely increasing horizontal resolution to kilometer scales is insufficient to broadly improve aerosol and cloud predictions without concurrent advancements in physical and chemical process representations. Nonetheless, the RRM moderately improves key ACI relationships such as CCN‐N d correlation, reflecting enhanced aerosol activation representation. The LWP‐N d relationship is also better captured by RRM, suggesting a better characterization of LWP adjustment.

Huang, Meng [Pacific Northwest National Laboratory↗
DOE OSTI2025

Advancing Aerosol Chemical Characterization and Vertical Profiling over the Southern Great Plains Using Uncrewed Aerial Sampling and Offline Aerosol Mass Spectrometry

Recent advancements in uncrewed aerial systems (UASs) and particulate matter (PM) analytical techniques have provided opportunities for atmospheric research. In this study, we deployed the Department of Energy’s fixed-wing ArcticShark UAS to examine PM 2.5 composition at varying altitudes─within and above the planetary boundary layer (PBL)─over the Southern Great Plains atmospheric observatory (SGP). A total of 22 flights were conducted across March, June, and August 2023. Composite filter samples were collected during each flight and analyzed with offline aerosol mass spectrometry (AMS), complemented by on-board real-time sensors and ground-based instrumentation, to provide a comprehensive view of regional aerosol characteristics. Results show clear vertical and seasonal differences in the aerosol composition. Relative to ground-level measurements, aloft samples exhibited shifts in the distribution of organic and inorganic PM, with the organic composition varying distinctly across seasons. Particulate organic nitrogen (ON) was elevated, with bulk compositions similar in March and June but strongly altered in August, likely driven by biomass burning and enhanced photochemical activity. Combined AMS and chemical ionization mass spectrometry analyses detected amines, amides, and amino acids. PM above the planetary boundary layer was enriched in oxidized organic aerosols, while ground-level PM contained higher nitrate and sulfate. Seasonal differences in aqueous-phase processing were also observed, which were strongest in March during persistent cloud cover and weaker in the drier August period, suggesting a shift from aqueous- to gas-phase SOA formation. In conclusion, these findings highlight the value of UAS in advancing PM measurements and vertical profiling of aerosol composition.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Impact of biomass burning aerosols on radiation, clouds, and precipitation over the Amazon: relative importance of aerosol–cloud and aerosol–radiation interactions

Biomass burning (BB) aerosols can influence regional and global climate through interactions with radiation, clouds, and precipitation. Here, we investigate the impact of BB aerosols on the energy balance and hydrological cycle over the Amazon Basin during the dry season. We performed simulations with a fully coupled meteorology–chemistry model, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), for a range of different BB emission scenarios to explore and characterize nonlinear effects and individual contributions from aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). The ARIs of BB aerosols tend to suppress low-level liquid clouds by local warming and increased evaporation and to facilitate the formation of high-level ice clouds by enhancing updrafts and condensation at high altitudes. In contrast, the ACIs of BB aerosol particles tend to enhance the formation and lifetime of low-level liquid clouds by providing more cloud condensation nuclei (CCN) and to suppress the formation of high-level ice clouds by reducing updrafts and condensable water vapor at high altitudes (>8 km). For scenarios representing the lower and upper limits of BB emission estimates for recent years (2002–2016), we obtained total regional BB aerosol radiative forcings of –0.2 and 1.5 W m –2 , respectively, showing that the influence of BB aerosols on the regional energy balance can range from modest cooling to strong warming. We find that ACIs dominate at low BB emission rates and low aerosol optical depth (AOD), leading to an increased cloud liquid water path (LWP) and negative radiative forcing, whereas ARIs dominate at high BB emission rates and high AOD, leading to a reduction of LWP and positive radiative forcing. In all scenarios, BB aerosols led to a decrease in the frequency of occurrence and rate of precipitation, caused primarily by ACI effects at low aerosol loading and by ARI effects at high aerosol loading. The dependence of precipitation reduction on BB aerosol loading is greater in a strong convective regime than under weakly convective conditions. Overall, our results show that ACIs tend to saturate at high aerosol loading, whereas the strength of ARIs continues to increase and plays a more important role in highly polluted episodes and regions. This should hold not only for BB aerosols over the Amazon, but also for other light-absorbing aerosols such as fossil fuel combustion aerosols in industrialized and densely populated areas. The importance of ARIs at high aerosol loading highlights the need for accurately characterizing aerosol optical properties in the investigation of aerosol effects on clouds, precipitation, and climate.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2005

Towards an A-train Aerosol Assimilation System: Assimilation of MODIS Aerosol Optical Thickness Retrievals into a Global Aerosol Transport and Radiation Model

To understand the role of atmospheric aerosols in Earth's climate system we ideally require a global, three-dimensional, and temporally continuous system of measurements. The view of aerosols provided by a single polar-orbiting satellite instrument (e.g., MODIS), while providing the greatest spatial coverage of any measurement system available, can offer only a single relevant observation per day of a particular location. Furthermore, the quantitative interpretation of those observations is subject to considerable uncertainty because of we do not know the aerosol optical properties or vertical profiles well enough. Ground-based and in situ measurements can provide missing detail about aerosol vertical and optical properties, but lack the spatial (and sometimes temporal) coverage desired. Chemical transport models treating the aerosol lifecycle complement this picture by providing three-dimensional, global, and continuous aerosol fields, but suffer from poor constraints on their initial conditions (e.g., the aerosol source, sink, and transformation mechanisms). Here we present a global, three- dimensional aerosol transport model and assimilation system. The model assimilates the MODIS aerosol optical thickness product to constrain its aerosol distributions and burdens. We provide an analysis of the model aerosol distributions as constrained by ground-based sun photometer measurements and aerosol products from other satellite measurements.

Colarco, P.↗
DOE OSTI2023

Earth System Model Aerosol–Cloud Diagnostics (ESMAC Diags) package, version 2: assessing aerosols, clouds, and aerosol–cloud interactions via field campaign and long-term observations

Abstract. Poor representations of aerosols, clouds, and aerosol–cloud interactions (ACIs) in Earth system models (ESMs) have long been the largest uncertainties in predicting global climate change. Huge efforts have been made to improve the representation of these processes in ESMs, and the key to these efforts is the evaluation of ESM simulations with observations. Most well-established ESM diagnostics packages focus on the climatological features; however, they lack process-level understanding and representations of aerosols, clouds, and ACIs. In this study, we developed the Earth System Model Aerosol–Cloud Diagnostics (ESMAC Diags) package to facilitate the routine evaluation of aerosols, clouds, and ACIs simulated the Energy Exascale Earth System Model (E3SM) from the US Department of Energy (DOE). This paper documents its version 2 functionality (ESMAC Diags v2), which has substantial updates compared with version 1 (Tang et al., 2022a). The simulated aerosol and cloud properties have been extensively compared with in situ and remote-sensing measurements from aircraft, ship, surface, and satellite platforms in ESMAC Diags v2. It currently includes six field campaigns and two permanent sites covering four geographical regions: the eastern North Atlantic, the central US, the northeastern Pacific, and the Southern Ocean. These regions produce frequent liquid- or mixed-phase clouds, with extensive measurements available from the DOE Atmospheric Radiation Measurement user facility and other agencies. ESMAC Diags v2 generates various types of single-variable and multivariable diagnostics, including percentiles, histograms, joint histograms, and heatmaps, to evaluate the model representation of aerosols, clouds, and ACIs. Select examples highlighting the capabilities of ESMAC Diags are shown using E3SM version 2 (E3SMv2). In general, E3SMv2 can reasonably reproduce many observed aerosol and cloud properties, with biases in some variables such as aerosol particle and cloud droplet sizes and number concentrations. The coupling of aerosol and cloud number concentrations may be too strong in E3SMv2, possibly indicating a bias in processes that control aerosol activation. Furthermore, the liquid water path response to a perturbed cloud droplet number concentration behaves differently in E3SMv2 and observations, which warrants further study to improve the cloud microphysics parameterizations in E3SMv2.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Aerosol Thermodynamics (Aerosol Liquid Water Concentration and Aerosol pH) at S2 during CoURAGE

These data report aerosol liquid water content (ALWC) and aerosol pH for the S2 (Mt. Airy) site during CoURAGE for April - June 2025. The ISORROPIA-II aerosol thermodynamic equilibrium model was used to compute ALWC and pH. The model was run in forward mode, with solids formation disabled (metastable mode), according to Pye et al. (Atmospheric Chemistry and Physics, 2020). Information about the model can be found at https://www.epfl.ch/labs/lapi/models-and-software/isorropia/, and in Fountoukis and Nenes (Atmospheric Chemistry and Physics, 2007). Inputs to the model were: (1) measured Temperature and relative humidity, both from the DoE ARM “metwxt” data products at S2, (2) aerosol chemical composition from the ARM ACSM, and (3) gas-phase ammonia concentrations. For ISORROPIA-II, ambient RH values above 0.995 were input to the model as 0.995; therefore, caution should be exercised interpreting ALWC when RH was above 0.995. Aerosol composition or NH3(g) concentrations below the LOD were input into the model as 0.5*LOD. Model runs were only conducted for data points at 30-min resolution with all three inputs (meteorology, ACSM, and NH3). If any of the three model inputs were missing, aerosol thermodynamic outputs are flagged as -999. Similarly, aerosol thermodynamic outputs are flagged as -999 if measured NH3(g) and aerosol ammonium (NH4+) were simultaneously below the respective LODs. The ALWC includes liquid water from inorganic aerosol components, calculated directly by ISORROPIA-II, as well as liquid water from organics, estimated from the ACSM organics assuming a kappa value of 0.12 according to Guo et al. (Atmospheric Chemistry and Physics, 2015).

Aerosol Liquid Water Content↗
NASA NTRS2015

The Two-Column Aerosol Project: Phase I - Overview and Impact of Elevated Aerosol Layers on Aerosol Optical Depth

The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere be tween and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2).These layer s contributed up to 60 of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. In addition, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed.

aerosols↗
NASA NTRS1989

SAGE II aerosol data validation based on retrieved aerosol model size distribution from SAGE II aerosol measurements

Consideration is given to aerosol correlative measurements experiments for the Stratospheric Aerosol and Gas Experiment (SAGE) II, conducted between November 1984 and July 1986. The correlative measurements were taken with an impactor/laser probe, a dustsonde, and an airborne 36-cm lidar system. The primary aerosol quantities measured by the ground-based instruments are compared with those calculated from the aerosol size distributions from SAGE II aerosol extinction measurements. Good agreement is found between the two sets of measurements.

Wang, Pi-Huan↗
NASA NTRS1998

Vertical Profiles of Cloud Condensation Nuclei, Condensation Nuclei, Optical Aerosol, Aerosol Optical Properties, and Aerosol Volatility Measured from Balloons

Under the support of this grant a balloon-borne gondola containing a variety of aerosol instruments was developed and flown from Laramie, Wyoming, (41 deg N, 105 deg W) and from Lauder, New Zealand (45 deg S, 170 deg E). The gondola includes instruments to measure the concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), optically detectable aerosol (OA.) (r greater than or equal to 0.15 - 2.0 microns), and optical scattering properties using a nephelometer (lambda = 530 microns). All instruments sampled from a common inlet which was heated to 40 C on ascent and to 160 C on descent. Flights with the CN counter, OA counter, and nephelometer began in July 1994. The CCN counter was added in November 1994, and the engineering problems were solved by June 1995. Since then the flights have included all four instruments, and were completed in January 1998. Altogether there were 20 flights from Laramie, approximately 5 per year, and 2 from Lauder. Of these there were one or more engineering problems on 6 of the flights from Laramie, hence the data are somewhat limited on those 6 flights, while a complete data set was obtained from the other 14 flights. Good CCN data are available from 12 of the Laramie flights. The two flights from Lauder in January 1998 were successful for all measurements. The results from these flights, and the development of the balloon-bome CCN counter have formed the basis for five conference presentations. The heated and unheated CN and OA measurements have been used to estimate the mass fraction of the aerosol volatile, while comparisons of the nephelometer measurements were used to estimate the light scattering, associated with the volatile aerosol. These estimates were calculated for 0.5 km averages of the ascent and descent data between 2.5 km and the tropopause, near 11.5 km.

Deshler, T.↗
NASA NTRS2001

Overview of ACE-Asia Spring 2001 Investigations on Aerosol Radiative Effects and Related Aerosol Properties

A primary, ACE-Asia objective was to quantify the interactions between aerosols and radiation in the Asia-Pacific region. Toward this end, radiometric and related aerosol measurements were made from ocean, land, air and space platforms. Models that predict aerosol fields guided the measurements and are helping integrate and interpret results. Companion overview's survey these measurement and modeling components. Here we illustrate how these components were combined to determine aerosol radiative. impacts and their relation to aerosol properties. Because clouds can obscure or change aerosol direct radiative effects, aircraft and ship sorties to measure these effects depended on predicting and finding cloud-free areas and times with interesting aerosols present. Pre-experiment satellite cloud climatologies, pre-flight aerosol and cloud forecasts, and in-flight guidance from satellite imagery all helped achieve this. Assessments of aerosol regional radiative impacts benefit from the spatiotemporal coverage of satellites, provided satellite-retrieved aerosol properties are accurate. Therefore, ACE-Asia included satellite retrieval tests, as part of many comparisons to judge the consistency (closure) among, diverse measurements. Early results include: (1) Solar spectrally resolved and broadband irradiances and optical depth measurements from the C-130 aircraft and at Kosan, Korea yielded aerosol radiative forcing efficiencies, permitting comparisons between efficiencies of ACE-Asia and INDOEX aerosols, and between dust and "pollution" aerosols. Detailed results will be presented in separate papers. (2) Based on measurements of wavelength dependent aerosol optical depth (AOD) and single scattering albedo the estimated 24-h a average aerosol radiative forcing efficiency at the surface for photosynthetically active radiation (400 - 700 nm) in Yulin, China is approx. 30 W sq m per AOD(500 nm). (3) The R/V Brown cruise from Honolulu to Sea of Japan sampled an aerosol optical depth gradient, with AOD(500 nm) extremes from 0.1 to 1.1. On the Pacific transit from Honolulu to Hachijo AOD(500 nm) averaged 0.2, including increases to 0.4 after several storms, suggesting the strong impact of wind-generated seasalt. The AOD maximum, found in the Sea of Japan, was influenced by dust and anthropogenic sources. (4) In Beijing, single scattering albedo retrieved from AERONET sun-sky radiometry yielded midvisible SSA=0.88 with strong wavelength dependence, suggesting a significant black carbon component. SSA retrieved during dust episodes was approx. 0.90 and variable but wavelength neutral reflecting the presence of urban haze with the dust. Downwind at Anmyon Island SSA was considerably higher, approx. 0.94, but wavelength neutral for dust episodes and spectrally dependent during non dust periods. (5) Satellite retrievals show major aerosol features moving from Asia over the Pacific; however, determining seasonal-average aerosol effects is hampered by sampling frequency and large-scale cloud systems that obscure key parts of aerosol patterns. Preliminary calculations using, satellite-retrieved AOD fields and initial ACE-Asia aerosol properties (including sulfates, soot, and dust) yield clear-sky aerosol radiative effects in the seasonal-average ACE-Asia plume exceeding those of manmade greenhouse gases. Quantifying all-sky direct aerosol radiative effects is complicated by the need to define the height of absorbing aerosols with respect to cloud decks.

Russell, Philip B.↗
NASA NTRS2000

Retrieving the Vertical Structure of the Effective Aerosol Complex Index of Refraction from a Combination of Aerosol in Situ and Remote Sensing Measurements During TARFOX

The largest uncertainty in estimates of the effects of atmospheric aerosols on climate stems from uncertainties in the determination of their microphysical properties, including the aerosol complex index of refraction, which in turn determines their optical properties. A novel technique is used to estimate the aerosol complex index of refraction in distinct vertical layers from a combination of aerosol in situ size distribution and remote sensing measurements during the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX). In particular, aerosol backscatter measurements using the NASA Langley LASE (Lidar Atmospheric Sensing Experiment) instrument and in situ aerosol size distribution data are utilized to derive vertical profiles of the "effective" aerosol complex index of refraction at 815 nm (i.e., the refractive index that would provide the same backscatter signal in a forward calculation on the basis of the measured in situ particle size distributions for homogeneous, spherical aerosols). A sensitivity study shows that this method yields small errors in the retrieved aerosol refractive indices, provided the errors in the lidar-derived aerosol backscatter are less than 30% and random in nature. Absolute errors in the estimated aerosol refractive indices are generally less than 0.04 for the real part and can be as much as 0.042 for the imaginary part in the case of a 30% error in the lidar-derived aerosol backscatter. The measurements of aerosol optical depth from the NASA Ames Airborne Tracking Sunphotometer (AATS-6) are successfully incorporated into the new technique and help constrain the retrieved aerosol refractive indices. An application of the technique to two TARFOX case studies yields the occurrence of vertical layers of distinct aerosol refractive indices. Values of the estimated complex aerosol refractive index range from 1.33 to 1.45 for the real part and 0.001 to 0.008 for the imaginary part. The methodology devised in this study provides, for the first time, a complete set of vertically resolved aerosol size distribution and refractive index data. yielding the vertical distribution of aerosol optical properties required for the determination of aerosol-induced radiative flux changes.

Redemann, J.↗
NASA NTRS2004

Aerosol Optical Properties Measured Onboard the Ronald H. Brown During ACE Asia as a Function of Aerosol Chemical Composition and Source Region

During the ACE Asia intensive field campaign conducted in the spring of 2001 aerosol properties were measured onboard the R/V Ronald H. Brown to study the effects of the Asian aerosol on atmospheric chemistry and climate in downwind regions. Aerosol properties measured in the marine boundary layer included chemical composition; number size distribution; and light scattering, hemispheric backscattering, and absorption coefficients. In addition, optical depth and vertical profiles of aerosol 180 deg backscatter were measured. Aerosol within the ACE Asia study region was found to be a complex mixture resulting from marine, pollution, volcanic, and dust sources. Presented here as a function of air mass source region are the mass fractions of the dominant aerosol chemical components, the fraction of the scattering measured at the surface due to each component, mass scattering efficiencies of the individual components, aerosol scattering and absorption coefficients, single scattering albedo, Angstrom exponents, optical depth, and vertical profiles of aerosol extinction. All results except aerosol optical depth and the vertical profiles of aerosol extinction are reported at a relative humidity of 55 +/- 5%. An over-determined data set was collected so that measured and calculated aerosol properties could be compared, internal consistency in the data set could be assessed, and sources of uncertainty could be identified. By taking into account non-sphericity of the dust aerosol, calculated and measured aerosol mass and scattering coefficients agreed within overall experimental uncertainties. Differences between measured and calculated aerosol absorption coefficients were not within reasonable uncertainty limits, however, and may indicate the inability of Mie theory and the assumption of internally mixed homogeneous spheres to predict absorption by the ACE Asia aerosol. Mass scattering efficiencies of non-sea salt sulfate aerosol, sea salt, submicron particulate organic matter, and dust found for the ACE Asia aerosol are comparable to values estimated for ACE 1, Aerosols99, and INDOEX. Unique to the ACE Asia aerosol was the large mass fractions of dust, the dominance of dust in controlling the aerosol optical properties, and the interaction of dust with soot aerosol.

Quinn, P. K.↗
NASA NTRS2000

Retrieving the Vertical Structure of the Effective Aerosol Complex Index of Refraction from a Combination of Aerosol in Situ and Remote Sensing Measurements During TARFOX

The largest uncertainty in estimates of the effects of atmospheric aerosols on climate stems from uncertainties in the determination of their microphysical properties, including the aerosol complex index of refraction, which in turn determines their optical properties. A novel technique is used to estimate the aerosol complex index of refraction in distinct vertical layers from a combination of aerosol in situ size distribution and remote sensing measurements during the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX). In particular, aerosol backscatter measurements using the NASA Langley LASE (Lidar Atmospheric Sensing Experiment) instrument and in situ aerosol size distribution data are utilized to derive vertical profiles of the 'effective' aerosol complex index of refraction at 815 nm (i.e., the refractive index that would provide the same backscatter signal in a forward calculation on the basis of the measured in situ particle size distributions for homogeneous, spherical aerosols). A sensitivity study shows that this method yields small errors in the retrieved aerosol refractive indices, provided the errors in the lidar derived aerosol backscatter are less than 30% and random in nature. Absolute errors in the estimated aerosol refractive indices are generally less than 0.04 for the real part and can be as much as 0.042 for the imaginary part in the case of a 30% error in the lidar-derived aerosol backscatter. The measurements of aerosol optical depth from the NASA Ames Airborne Tracking Sunphotometer (AATS-6) are successfully incorporated into the new technique and help constrain the retrieved aerosol refractive indices. An application of the technique to two TARFOX case studies yields the occurrence of vertical layers of distinct aerosol refractive indices. Values of the estimated complex aerosol refractive index range from 1.33 to 1.45 for the real part and 0.001 to 0.008 for the imaginary part. The methodology devised in this study provides, for the first time a complete set of vertically resolved aerosol size distribution and refractive index data, yielding the vertical distribution of aerosol optical properties required for the determination of aersol-induced radiative flux changes

Redemann, J.↗
DOE OSTI2024

62°S Witnesses the Transition of Boundary Layer Marine Aerosol Pattern Over the Southern Ocean (50°S–68°S, 63°E– 150°E) During the Spring and Summer: Results From MARCUS (I)

The Atmospheric Radiation Measurement Mobile Facility-2 was installed onboard the research vessel Aurora Australis to measure aerosol properties during the 2017-2018 Measurement of Aerosols, Radiation, and CloUds over the pristine Southern ocean (MARCUS) Experiment, providing unique data on aerosols latitudinal and seasonal variation, including south of 60 degrees S where previous observations are scarce. Data from a Cloud Condensation Nuclei (CCN) counter and Ultra-High-Sensitivity Aerosol Spectrometer show that both the number concentration (N-CCN) and size distribution of CCN-active aerosols, with diameters (D) between 60 nm < D < 1,000 nm are different over the North Southern Ocean (NSO) (50 degrees S-60 degrees S) and the South Southern Ocean (SSO) (62 degrees S-68 degrees S). The average NSO N-CCN at 0.2% and 0.5% supersaturation were 28% and 49% less than that over the SSO. This increase of CCN over the SSO is caused by the increase of aerosols with 60 nm < D < 200 nm, consistent with calculations of Aerosol Scattering Angstrom Exponents derived from a nephelometer. Aerosol hygroscopicity growth factor measured by the Hygroscopic Tandem Differential Mobility Analyzer stayed close to 1.41 for aerosols with 50 nm < D < 250 nm over the SSO, but increased from 1.30 to 1.67 over the NSO, indicating different chemical compositions. Both CCN and Ice Nucleating Particles (INPs) showed a stronger variation with season than with latitude. The variation of heat-labile and presumably proteinacous INPs suggests an increase of ice nucleating-active microbes in summer.

Niu, Qing↗
NASA NTRSDate not supplied

Impacts of Aerosol and Cloud Variability on Satellite-Derived All-skies Direct Aerosol Radiative Effects (DARE) over the North and Southeast Atlantic

The Top-of-Atmosphere (TOA) Shortwave (SW) Direct Aerosol Radiative Effect (DARE) in all-sky conditions (i.e., aerosols in clear skies and aerosols above and below all types of clouds) is the global change in upwelling radiative flux due to aerosols. It is one of the strongest indicators of global climate change due to aerosols. SW DARE at TOA depends on the Earth’s surface albedo, cloud fraction, cloud optical properties, and aerosol optical properties, which are all challenging to accurately characterize from space. The overarching goals of our project are to provide state-of-the-art observational all-sky TOA SW DARE, along with guidance on which aerosol and/or cloud properties are the most important to measure, and at which spatio-temporal scales, for accurate DARE observations. We compute all-sky DARE based on state-of-the-art cloud and aerosol retrieval algorithms from CALIOP (Cloud–Aerosol Lidar with Orthogonal Polarization) and MODIS (Moderate Resolution Imaging spectroradiometer) satellite sensors, as well as aerosol intensive properties from MERRA-2 (Modern-Era Retrospective Analysis for Research and Applications, version 2) simulations over three specific regions of the Atlantic Ocean from 2012 to 2016. In this symposium, we present a characterization of the cloud and aerosol optical and physical properties and the observational TOA SW DARE along three individual satellite tracks in the Southeast Atlantic region -- on September 18 and 20, 2016 and August 13, 2017. We then quantify the impact of assuming homogeneous cloud or aerosol fields in space-based TOA SW DARE calculations. And, finally, the resulting space-based all-skies aerosol vertical distribution and DARE calculations are evaluated using remote sensing observations from coincident suborbital flights from the NASA ORACLES (the ObseRvations of Aerosols above CLouds and their intEractionS, ORACLES field campaign) field campaign. The NASA Atmospheric Observing System (AOS) mission addresses the NASA Aerosol, Cloud, Convection and Precipitation (ACCP) designated observables and proposes, as one of its aerosol objectives, to reduce uncertainties in estimates of global mean all-sky SW DARE at TOA. Well characterizing clouds, aerosol vertical distributions, aerosol types and associated all-skies DARE over the Atlantic Ocean will inform the AOS community on where, when, how, and how often the satellite retrievals should be performed to estimate DARE and reduce all-skies DARE uncertainties most accurately. These comprehensive characterizations will also identify the key regions and times when the AOS (or other ACCP-related) suborbital missions should be conducted to evaluate and improve the AOS space-based observations and retrievals.

aerosol↗
DOE OSTI2023

Assessing the link between aerosol mixing state, structure and composition and their optical properties: Ascension Island as a testbed for the South‐East Atlantic aerosol regimes

Forest and savanna fires are a major source of pollution over the globe. Such fire events emit to the atmosphere a considerable amount of “fluffy” fractal black looking particles that are often referred to as black carbon (BC) or soot aerosols. In fact, BC particles (aerosols) emitted from savanna and agricultural fires over the African continent play an important role in the region’s and the global climate. These fires occur each year between July and October, which is referred to as the biomass burning (BB) season and are considered among the globe's largest man-made emission sources of BC particles. However, during these fire events, not only BC particles are emitted, but also other types of particles and gases that can interact with each other to create new particles, generating a slew of particles often generally referred to as BB aerosols. Although the majority of the fire emissions occur inland in the sub-Saharan part of Africa, their effect reaches far beyond the continent due to the prevailing easterly winds, which transport those aerosols over the South-East Atlantic (SEA) ocean, off the west-coast of Africa. The reason why these particles are so important to the regional and global climate is that they absorb sunlight radiation, which overall warms the climate. However, the magnitude of this warming effect is highly uncertain and depends upon a multitude of aspects. Our overarching goal for this project was to better understand the changes in the aerosol properties as they transport from fire sources downstream toward the ocean and how this can eventually affect the earth's radiative budget in terms of warming or cooling. Following the above, our work here was focused on the investigation of the African BB aerosol plumes mixing state (mixing of BB aerosols and other aerosol types), composition and size distribution as they transport from the African continent towards the SEA ocean, and their link with some of the commonly measurable bulk optical properties such as mass absorption coefficient (MAC) and single scattering albedo (SSA). We utilized three field missions that were conducted over the SEA ocean between 2016 and 2018. Specifically, we used (1) ground-based measurements from the DOE ARM Mobile Facility (AMF1), which was deployed at Ascension Island (ASI) for the LASIC (Layered Atlantic Smoke Interactions with Clouds) campaign between June 2016 and October 2017, (2) airborne measurements from the UK CLARIFY (Clouds and Aerosol Radiative impacts and Forcing) campaign during Aug-Sep-2017, and (3) airborne measurements from the ORACLES (Observations of Aerosols above Clouds and their interactions) campaign during Aug-2017, and Sep-Oct-2018. The three campaigns cover a relatively large region, from the western African coast on the east towards Ascension Island in the middle of the SEA to the west. We used the data gathered by these campaigns to find how BB properties and composition change from near emission sources (the ORACLES campaign flights) downstream (the CLARIFY flights and the ground based LASIC measurements). We used particle trajectory following methodologies to connect the measurements from the different campaigns, which allowed us to follow a certain aerosol plume (airmass) from near-source towards Ascension Island. We found out that atmospheric aging processes governed by the UV light from the sun (photochemistry) and cloud processes (aqueous chemistry) govern the changes seen in the particle composition during the transport were more dominant in dictating aerosol composition than specific emission composition or source types. We assessed how aerosol optical properties change during the BB season and what are the main drivers of this change. We found that the enhanced ratio of BC to CO is well correlated with single scattering albedo (SSA) and mass absorption coefficient (MACBC), providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic Ocean. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/CO from June to August is likely to be caused by burning becoming more flaming (hot fires), and the decrease in BC/CO in September and October may be caused by smoldering (colder) fires. We found that aerosol hygroscopicity increases with decreasing altitude below 2km, and that enhanced BB hygroscopicity at lower altitudes is mainly due to a lower organic aerosol (OA) fraction, increased sulfate fraction, and greater hygroscopicity parameter of OA at lower altitudes.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2010

Identifying Aerosol Type/Mixture from Aerosol Absorption Properties Using AERONET

Aerosols are generated in the atmosphere through anthropogenic and natural mechanisms. These sources have signatures in the aerosol optical and microphysical properties that can be used to identify the aerosol type/mixture. Spectral aerosol absorption information (absorption Angstrom exponent; AAE) used in conjunction with the particle size parameterization (extinction Angstrom exponent; EAE) can only identify the dominant absorbing aerosol type in the sample volume (e.g., black carbon vs. iron oxides in dust). This AAE/EAE relationship can be expanded to also identify non-absorbing aerosol types/mixtures by applying an absorption weighting. This new relationship provides improved aerosol type distinction when the magnitude of absorption is not equal (e.g, black carbon vs. sulfates). The Aerosol Robotic Network (AERONET) data provide spectral aerosol optical depth and single scattering albedo - key parameters used to determine EAE and AAE. The proposed aerosol type/mixture relationship is demonstrated using the long-term data archive acquired at AERONET sites within various source regions. The preliminary analysis has found that dust, sulfate, organic carbon, and black carbon aerosol types/mixtures can be determined from this AAE/EAE relationship when applying the absorption weighting for each available wavelength (Le., 440, 675, 870nm). Large, non-spherical dust particles absorb in the shorter wavelengths and the application of 440nm wavelength absorption weighting produced the best particle type definition. Sulfate particles scatter light efficiently and organic carbon particles are small near the source and aggregate over time to form larger less absorbing particles. Both sulfates and organic carbon showed generally better definition using the 870nm wavelength absorption weighting. Black carbon generation results from varying combustion rates from a number of sources including industrial processes and biomass burning. Cases with primarily black carbon showed improved definition in the 870nm wavelength absorption weighting due to the increased absorption in the near-infrared wavelengths, while the 440nm wavelength provided better definition when black carbon mixed with dust. Utilization of this particle type scheme provides necessary information for remote sensing applications, which needs a priori knowledge of aerosol type to model the retrieved properties especially over semi-bright surfaces. In fact, this analysis reveals that the aerosol types occurred in mixtures with varying magnitudes of absorption and requires the use of more than one assumed aerosol mixture model. Furthermore, this technique will provide the aerosol transport model community a data set for validating aerosol type.

Giles, D. M.↗