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NASA NTRS2022

Characterizing Aerosol From Space With the MODerate Resolution Imaging Spectroradiometer (Modis) on the Terra and Aqua Satellites

Aerosols, the small, suspended liquid and solid particles in the atmosphere, have myriad effects on climate, weather, and air quality. When the NASA Earth-Observing System’s (EOS) Terra and Aqua satellites launched in 1999 and 2002, they each included many advanced sensors that have been used for aerosol research. In particular, the MODerate-resolution Imaging Spectroradiometer (MODIS) deployed on both satellites, has provided key data relating to aerosol loading and relative aerosol type on the global scale. Three different algorithms, known as “Dark Target”, “Deep Blue” and “MAIAC”, use different subsets of MODIS measurements and different assumptions to create various products such as Aerosol Optical Depth (AOD), fine mode fraction (FMF) and single scattering albedo (SSA). Although all three derive AOD in cloud-free conditions, each algorithm has different strengths and weaknesses in different areas of the globe and under different conditions. Here, we provide a short summary of each algorithm, description of products, and basic information about downloading and using the products. We also provide some examples of how MODIS aerosol products are used. Finally, we add a quick discussion about how these algorithms and products will continue after MODIS leaves orbit.

MODIS↗
NASA NTRSDate not supplied

Models, in Situ, and Remote Sensing of Aerosols (MIRA) International Working Group

There is a natural partitioning of scientific interest amongst three focus areas of aerosol research: modeling, in situ measurements, and remote sensing observations. The community benefits when these groups interact, with overall benefits towards advancing our understanding of climate, weather, and air quality. To this end, MIRA seeks to foster international collaborations across disciplines and regional boundaries and offers a complementary association with established international working groups. Within the present framework, MIRA has identified four initial focus areas, with opportunities to add more by the working group. One effort advances knowledge of the aerosol lidar ratio for different aerosol compositions and locations to improve backscatter lidar retrievals from satellites and ground-based instruments. Another effort seeks to improve aerosol optical parameters used by climate and radiative transfer models. A third effort focuses on harmonizing aerosol assimilation models with satellite measurement retrievals, and a fourth interest seeks to develop retrievals of aerosol Particulate Matter from remote sensing measurements. The presentation will provide an overview of MIRA and ways for the community to engage.

aerosols↗
NASA NTRSDate not supplied

Simulating Sulfate Aerosol Size in the Hunga Tonga Plume: Comparisons with Observations

Using the NASA GEOS Chemistry Climate Model (CCM) coupled to a detailed sectional aerosol microphysical model, we have simulated the January 2022 Hunga Tonga-Hunga Ha’apai (HTHH) plume. We have developed a version of the Global Modeling Initiative (GMI) chemistry mechanism to include the requisite sulfur chemistry and coupled it to the Community Aerosol and Radiation Model for Atmospheres (CARMA) sectional aerosol microphysics within the GEOS CCM. Our simulations focus on the lifecycle of stratospheric sulfur injected by the eruption–from the oxidation of the injected sulfur dioxide to the nucleation, growth, coagulation, hydration, and eventual settling of the volcanic sulfate aerosol particles. In order to constrain the simulated microphysics, we focus on comparing our model to observations with aerosol size information, namely in-situ particle counter observations and multi-wavelength satellite observations from OMPS-LP and SAGE-III. This eruption provides an interesting test case for our model; both the modeled gas-phase chemistry as well as the modeled aerosol microphysics are perturbed by the massive injection of water that accompanied the primary sulfur emissions from the eruption.

aerosols↗
NASA NTRS2023

The Mars Atmosphere Water Ice Aerosol Climatology by MRO/CRISM: 5 Mars Years of Observations

We use near-infrared spectra returned from the Compact Reconnaissance Imaging Spectrometer for Mars (CRISM) aboard the Mars Reconnaissance Orbiter (MRO) to provide retrievals of the column-integrated optical depth of water ice aerosols for more than 5 Martian years between Mars Year (MY) 28 at Ls = 112° (27 September 2006) and MY 33 at Ls = 213° (30 August 2016). We have developed a radiative transfer model for this purpose that retrieves aerosol opacity from the water ice aerosol feature near 3.3 μm using CRISM hyperspectral observations for the first time. The resulting retrievals well depict the main features in the water ice aerosol climatology with repeatable patterns every Martian year. The aphelion cloud belt (ACB) is observed between 10°S and 30°N, with peak optical depth around Ls = 90°. Apart from the global dust storm during MY 28, modest interannual variability in the water ice aerosol optical depth is observed in the ACB. The north polar hood is observed at latitudes poleward of 45°N throughout northern spring and summer seasons and reappears in northern winter. The south polar hood is observed in early to mid-southern autumn, reaching latitudes around 60°S, and re-emerging during southern winter between 45°S and 60°S. A lack of water ice aerosols is repeatedly seen in the southern hemisphere throughout southern spring and summer. High optical depth in the ACB is observed over the volcanoes of Olympus Mons, Elysium, and the Tharsis bulge, as well as over Hellas Basin.

Mars↗
NASA NTRSDate not supplied

Airborne High Spectral Resolution Lidar Measurements of Aerosols over Major Metropolitan Areas

NASA Langley Research Center airborne High Spectral Resolution Lidars have participated in several NASA field missions designed to study air quality over major metropolitan regions. Data from these instruments reveal the temporal and spatial variabilities of aerosol distributions over these urban areas, quantify aerosol backscatter, extinction, and depolarization near the surface, and provide additional relevant information regarding aerosol optical thickness, mixed layer height, and aerosol type. We show that measurements of surface PM2.5 concentrations typically are more directly related to coincident near-surface measurements of aerosol extinction than coincident measurements of aerosol optical thickness.

lidar↗
NASA NTRSDate not supplied

AERACEPT (Aerosol Rapid Analysis Combined Entry Probe/sonde Technology): Enabling Technology for Planetary Atmospheric Science Probes

Aerosols –clouds, hazes, and dusts –are a key part of planetary mass and energy balance, but difficult to study remotely. Current technology limits in situ measurements to once-in-a-lifetime flagship missions, which is not enough to characterize such highly dynamic systems. AERACEPT (AErosol Rapid Analysis Combined Entry Probe/sonde Technology) is an early-stage technology allowing asingle aeroshell body toact as both anentry vehicle and aerosol-samplingpassivedescent sonde, using the aeroshell’sown velocityto drive aerosol capture and separationthrough a series of embedded inlets.It takes advantage ofrecently developed thermal protection materials (3D-CC and 3MDCP)in combination withheritage aerosol sampling technologies fromboth planetary and airborne science (high-speed inlets and particle separation). By eliminating the need for heat shield separation, deployable parachutes, ordescent control, AERACEPT reducesthe mass, volume, and complexity ofplanetary aerosol sampling. Verifying AERACEPT’s performance involves modeling interdependencies between the size and geometry of the sampling inlets, the material response of the hypersonic phase of entry, the thermal conditions throughout the probe’s descent, the subsonic flow and particle sampling efficiency, the needed amount of sample, andthe cadence at which the sample can be analyzed. AERACEPT’s current predictions, using the Nephele Venus cloud mission concept (sampling between 63km to 39km, all subsonic) indicates AERACEPT can obtain >20 μL of particle material (roughly 10x the limit of detection) from droplets larger than 0.2 μm, with sample heating limited to <15 K above ambient. Validation testing for the thermal material response model has recently been performed at the UIUC Plasmatron facility, and for the flow and particle capture models is planned for this fall at the Ames Fluid Mechanics Laboratory.

AERACEPT↗
NASA NTRS2026

Satellite Optical Remote Sensing of Clouds and Aerosols: From Particle Single-Scattering and Gaseous Absorption Through Radiative Transfer to Retrieval Products

Clouds and aerosols are fundamental regulators of Earth’s radiation budget and climate system, influencing both solar and terrestrial radiation through scattering, absorption, and emission processes. Accurate characterization of their physical and radiative properties from space requires a rigorous understanding of particle single-scattering, gaseous absorption, and radiative transfer in the atmosphere, as well as reliable inversion methods. This review synthesizes the physical foundations and algorithmic implementations of satellite-based passive optical remote sensing of clouds and aerosols, spanning the ultraviolet to thermal infrared spectral range. Beginning with electromagnetic scattering theory and state-of-the-art methods for computing single-scattering by nonspherical particles and computationally efficient methods for accounting for atmospheric absorption, we discuss the radiative transfer framework underpinning cloud and aerosol retrievals. The connection between single-scattering and multiple-scattering is rigorously formulated. We then summarize operational and research-grade retrieval techniques, including cloud masking and thermodynamic phase determination, CO₂ slicing for cloud-top pressure, the Nakajima-King shortwave bi-spectral, and infrared split-window approaches for cloud optical thickness and effective particle size, inversion algorithms for determining aerosol properties from multi-spectral and/or multi-angle radiometric and polarimetric measurements, and active-passive sensing synergy. Examples of the global cloud and aerosol climatologies are illustrated using observations from the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Multi-angle Imaging SpectroRadiometer (MISR). Furthermore, the unique strengths of active remote sensing techniques based on spaceborne lidar observations are briefly elaborated in the context of studying ice clouds composed of randomly and horizontally oriented ice crystals, which is a significant challenge for conventional passive remote sensing techniques. By connecting physical theory to practical retrievals, this review highlights both the maturity of current methodologies and the remaining challenges in reducing uncertainties in particle morphology, vertical structure, absorption, and aerosol-cloud interactions. Furthermore, the impact of artificial intelligence (AI) on atmospheric remote sensing is briefly addressed.

Aerosols↗
DOE OSTI2018

Cloud, Aerosol, and Complex Terrain Interactions (CACTI) Science Plan

General circulation models and downscaled regional models exhibit persistent biases in deep convective initiation location and timing, cloud top height, stratiform area and precipitation fraction, and anvil coverage. Despite important impacts on the distribution of atmospheric heating, moistening, and momentum, nearly all climate models fail to represent convective organization, while system evolution is not represented at all. Improving representation of convective systems in models requires characterization of their predictability as a function of environmental conditions, and this characterization depends on observing many cases of convective initiation, non-initiation, organization, and non-organization. The Cloud, Aerosol, and Complex Terrain Interactions (CACTI) experiment in the Sierras de Córdoba mountain range of north-central Argentina is designed to improve understanding of cloud life cycle and organization in relation to environmental conditions so that cumulus, microphysics, and aerosol parameterizations in multiscale models can be improved. The Sierras de Córdoba range has a high frequency of orographic boundary-layer clouds, many reaching congestus depths, many initiating into deep convection, and some organizing into mesoscale systems uniquely observable from a single fixed site. Some systems even grow upscale to become among the deepest, largest, and longest-lived in the world. These systems likely contribute to an observed regional trend of increasing extreme rainfall, and poor prediction of them likely contributes to a warm, dry bias in climate models downstream of the Sierras de Córdoba range in a key agricultural region. Many environmental factors influence the convective life cycle in this region, including orographic, low-level jet, and frontal circulations, surface fluxes, synoptic vertical motions influenced by the Andes, cloud detrainment, and aerosol properties. Local and long-range transport of smoke resulting from biomass burning as well as blowing dust are common in the austral spring, while changes in land surface properties as the wet season progresses impact surface fluxes and boundary-layer evolution on daily and seasonal time scales that feed back to cloud and rainfall generation. This range of environmental conditions and cloud properties coupled with a high frequency of events makes this an ideal location for improving our understanding of cloud-environment interactions. The following primary science questions will be addressed through coordinated first U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF1), mobile C-band Scanning ARM Precipitation Radar (C-SAPR2), ARM Aerial Facility (AAF) Gulfstream-1 (G-1), and guest instrument observations: How are the properties and life cycles of orographically generated cumulus humulis, mediocris, and congestus clouds affected by environmental kinematics, thermodynamics, aerosols, and surface properties? How do these cloud types alter these environmental conditions? How do environmental kinematics, thermodynamics, and aerosols impact deep convective initiation, upscale growth, and mesoscale organization? How are soil moisture, surface fluxes, and aerosol properties altered by deep convective precipitation events and seasonal accumulation of precipitation? This multi-faceted experiment involves a long-term 7-month extended operational period (EOP, 1 October, 2018–30 April, 2019) as well as a 1.5-month intensive operational period (IOP, 30 October–13 December) that will include G-1 observations coinciding with the international multi-agency Remote Sensing of Electrification, Lightning, and Meso-scale/Micro-scale Processes with Adaptive Ground Observations (RELAMPAGO) field campaign.

Convection, Andes, Argentina, cloud life cycle, cl↗
DOE OSTI2019

Production of Secondary Organic Aerosol During Aging of Biomass Burning Smoke From Fresh Fuels and Its Relationship to VOC Precursors

After smoke from burning biomass is emitted into the atmosphere, chemical and physical processes change the composition and amount of organic aerosol present in the aged, diluted plume. During the fourth Fire Lab at Missoula Experiment, we performed smog-chamber experiments to investigate formation of secondary organic aerosol (SOA) and multiphase oxidation of primary organic aerosol (POA). We simulated atmospheric aging of diluted smoke from a variety of biomass fuels while measuring particle composition using high-resolution aerosol mass spectrometry. We quantified SOA formation using a tracer ion for low-volatility POA as a reference standard (akin to a naturally occurring internal standard). We report these smoke aging experiments revealed variable organic aerosol (OA) enhancements, even for smoke from similar fuels and aging mechanisms. This variable OA enhancement correlated well with measured differences in the amounts of emitted volatile organic compounds (VOCs) that could subsequently be oxidized to form SOA. For some aging experiments, we were able to predict the SOA production to within a factor of 2 using a fuel-specific VOC emission inventory that was scaled by burn-specific toluene measurements. For fires of coniferous fuels that were dominated by needle burning, volatile biogenic compounds were the dominant precursor class. For wiregrass fires, furans were the dominant SOA precursors. We used a POA tracer ion to calculate the amount of mass lost due to gas-phase oxidation and subsequent volatilization of semivolatile POA. Less than 5% of the POA mass was lost via multiphase oxidation-driven evaporation during up to 2 hr of equivalent atmospheric oxidation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Pathways of sulfate enhancement by natural and anthropogenic mineral aerosols in China

China, the world’s largest consumer of coal, emits approximately 30 million tons of sulfur dioxide (SO₂) per year. SO₂ is subsequently oxidized to sulfate in the atmosphere. However, large gaps exist between model-predicted and measured sulfate levels in China. Long-term field observations and numerical simulations were integrated to investigate the effect of mineral aerosols on sulfate formation. We found that mineral aerosols contributed a nationwide average of approximately 22% to sulfate production in 2006. The increased sulfate concentration was approximately 2 μg m⁻³ in the entire China. In East China and the Sichuan Basin, the increments reached 6.3 μg m⁻³ and 7.3 μg m⁻³, respectively. Mineral aerosols led to faster SO₂ oxidation through three pathways. First, more SO₂ was dissolved as cloud water alkalinity increased due to water-soluble mineral cations. Sulfate production was then enhanced through the aqueous-phase oxidation of S(IV) (dissolved sulfur in oxidation state +4). The contribution to the national sulfate production was 5%. Second, sulfate was enhanced through S(IV) catalyzed oxidation by transition metals. The contribution to the annual sulfate production was 8%, with 19% during the winter that decreased to 2% during the summer. Third, SO₂ reacts on the surface of mineral aerosols to produce sulfate. The contribution to the national average sulfate concentration was 9% with 16% during the winter and a negligible effect during the summer. The inclusion of mineral aerosols does resolve model discrepancies with sulfate observations in China, especially during the winter. These three pathways, which are not fully considered in most current chemistry-climate models, will significantly impact assessments regarding the effects of aerosol on climate change in China.

Huang, Xin↗
DOE OSTI2017

Retrieval of water vapor column abundance and aerosol properties from ChemCam passive sky spectroscopy

In this work, we derive water vapor column abundances and aerosol properties from Mars Science Laboratory (MSL) ChemCam passive mode observations of scattered sky light. This paper covers the methodology and initial results for water vapor and also provides preliminary results for aerosols. The data set presented here includes the results of 113 observations spanning from Mars Year 31 L s = 291° (March 30, 2013) to Mars Year 33 L s = 127° (March 24, 2016). Each ChemCam passive sky observation acquires spectra at two different elevation angles. We fit these spectra with a discrete-ordinates multiple scattering radiative transfer model, using the correlated-k approximation for gas absorption bands. The retrieval proceeds by first fitting the continuum of the ratio of the two elevation angles to solve for aerosol properties, and then fitting the continuum-removed ratio to solve for gas abundances. The final step of the retrieval makes use of the observed CO 2 absorptions and the known CO 2 abundance to correct the retrieved water vapor abundance for the effects of the vertical distribution of scattering aerosols and to derive an aerosol scale height parameter. Our water vapor results give water vapor column abundance with a precision of ±0.6 precipitable microns and systematic errors no larger than ±0.3 precipitable microns, assuming uniform vertical mixing. The ChemCam-retrieved water abundances show, with only a few exceptions, the same seasonal behavior and the same timing of seasonal minima and maxima as the TES, CRISM, and REMS-H data sets that we compare them to. However ChemCam-retrieved water abundances are generally lower than zonal and regional scale from-orbit water vapor data, while at the same time being significantly larger than pre-dawn REMS-H abundances. Pending further analysis of REMS-H volume mixing ratio uncertainties, the differences between ChemCam and REMS-H pre-dawn mixing ratios appear to be much too large to be explained by large scale circulations and thus they tend to support the hypothesis of substantial diurnal interactions of water vapor with the surface. Our preliminary aerosol results, meanwhile, show the expected seasonal pattern in dust particle size but also indicate a surprising interannual increase in water–ice cloud opacities.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2016

Total and regional deposition of inhaled aerosols in supine healthy subjects and subjects with mild-to-moderate COPD

Despite substantial development of sophisticated subject-specific computational models of aerosol transport and deposition in human lungs, experimental validation of predic- tions from these new models is sparse. We collected aerosol retention and exhalation profiles in seven healthy volunteers and six subjects with mild-to-moderate COPD (FEV1 ¼ 50–80%predicted) in the supine posture. Total deposition was measured during continuous breathing of 1 and 2.9 mm-diameter particles (tidal volume of 1 L, flow rate of 0.3 L/s and 0.75 L/s). Bolus inhalations of 1 mm particles were performed to penetration volumes of 200, 500 and 800 mL (flow rate of 0.5 L/s). Aerosol bolus dispersion (H), deposition, and mode shift (MS) were calculated from these data. There was no significant difference in total deposition between healthy subjects and those with COPD. Total deposition increased with increasing particle size and also with increasing flow rate. Similarly, there was no significant difference in aerosol bolus deposition between subject groups. Yet, the rate of increase in dispersion and of decrease in MS with increasing penetration volume was higher in subjects with COPD than in healthy volunteers (H: 0.79870.205 vs. 0.52770.122 mL/mL, p¼ 0.01; MS: - 0.27170.129 vs. - 0.145 70.076 mL/mL, p¼ 0.05) indicating larger ventilation inhomogeneities (based on H) and increased flow sequencing (based on MS) in the COPD than in the healthy group. In conclusion, in the supine posture, deposition appears to lack sensitivity for assessing the effect of lung morphology and/or ventilation distribution alteration induced by mild-to- moderate lung disease on the fate of inhaled aerosols. However, other parameters such as aerosol bolus dispersion and mode shift may be more sensitive parameters for evaluating models of lungs with moderate disease.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Tutorial: Langevin Dynamics methods for aerosol particle trajectory simulations and collision rate constant modeling

The Langevin Dynamics (LD) method (also known in the literature as Brownian Dynamics) is routinely used to simulate aerosol particle trajectories for transport rate constant calculations as well as to understand aerosol particle transport in internal and external fluid flows. This tutorial intends to explain the methodological details of setting up a LD simulation of a population of aerosol particles and to deduce rate constants from an ensemble of classical trajectories. We discuss the applicability and limitations of the translational Langevin equation to model the combined stochastic and deterministic motion of particles in fields of force or fluid flow. The drag force and stochastic “diffusion” force terms that appear in the Langevin equation are discussed elaborately, along with a summary of common forces relevant to aerosol systems (electrostatic, gravity, van der Waals, …); a commonly used first order and a fourth order Runge-Kutta time stepping schemes for linear stochastic ordinary differential equations are presented. A MATLAB® implementation of a LD code for simulating particle settling under gravity using the first order scheme is included for illustration. Scaling analysis of aerosol transport processes and the selection of timestep and domain size for trajectory simulations are demonstrated through two specific aerosol processes: particle diffusion charging and coagulation. Fortran® implementations of the first order and fourth order time-stepping schemes are included for simulating the 3D motion of a particle in a periodic domain. Lastly, potential applications and caveats to the usage of LD are included as a summary.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Molecular Specificity and Proton Transfer Mechanisms in Aerosol Prenucleation Clusters Relevant to New Particle Formation

Atmospheric aerosol particles influence Earth’s radiative energy balance and cloud properties either directly through interacting with the solar radiation or indirectly through acting as cloud condensation nuclei (CCN), thus impacting Earth’s climate change, air quality, and human health. Regarding both the important scientific and overarching practical implications of aerosols, the past two decades have seen an extensive research effort, with emphasis on the chemical compositions and underlying mechanisms of aerosol formation. New particle formation (NPF) has been recognized as an important pathway, contributing up to 50% of atmospheric aerosols. Nowadays, the general consensus in NPF is that it proceeds via two distinct stages—the nucleation from gaseous precursors to form critical nuclei of sub-1–2 nanometer size, and the subsequent growth into large particles. However, a fundamental understanding of both the NPF process and the molecular-level characterization of the critical size aerosol clusters is still largely missing, hampering the development of reliable and predictive aerosol nucleation and climate models.

Hou, Gao-Lei↗
DOE OSTI2025

Secondhand Exposure to Simulated Cannabis Vaping Aerosols

Emissions from cannabis vaping degrade indoor air quality and expose non-users to secondhand pollutants. We investigated how the vaping mixture composition affects indoor aerosol characteristics and exposures. Simulated cannabis vaping aerosol was produced by flash evaporation in a 20 m3 chamber of mixtures containing terpenoids, cannabinoids, cannabis extract constituents, and the adulterant vitamin E acetate (VEA). Aerosol time- and size-resolved concentrations (8 nm-2.5 μm at 1 Hz) were measured, and a dosimetry model was used to evaluate the intake of secondhand aerosols. The results showed peak particle number (PN) concentrations between 0.7 × 106 and 13 × 106 cm-3 and peak mass concentration (PM1.0) between 65 and 1191 μg m-3 at t = 5 min after emission. Concentrations decreased to 21-57% of peak PN and 33-69% of peak PM1.0 at t = 60 min. The PM1.0 yield was 0.06 for a terpenoid-only mixture, 0.22-0.36 for tetrahydrocannabinol (THC)-terpenoid mixtures, and >1 for mixtures containing high concentrations of cannabidiol (CBD) or VEA. For intake deposition, the highest aerosol fraction was deposited in the pulmonary region, followed by the tracheobronchial and head regions. Deposition increased in the presence of THC, CBD, or VEA, with aerosols <100 nm contributing the majority of particles deposited in all regions.

Tang, Xiaochen↗
DOE OSTI2016

Sulfur Dioxide Accelerates the Heterogeneous Oxidation Rate of Organic Aerosol by Hydroxyl Radicals

There remains considerable uncertainty in how anthropogenic gas phase emissions alter the oxidative aging of organic aerosols in the troposphere. Here we observe a 10-20 fold acceleration in the effective heterogeneous OH oxidation rate of organic aerosol in the presence of SO 2 . This acceleration originates from the radical chain reactions propagated by alkoxy radicals, which are formed efficiently inside the particle by the reaction of peroxy radicals with SO 2 . As the OH approaches atmospheric concentrations, the radical chain length increases, transforming the aerosol at rates predicted to be up to 10 times the OH-aerosol collision frequency. Model predictions, constrained by experiments over orders of magnitude changes in [OH] and [SO 2 ], suggest that in polluted regions the heterogeneous processing of organic aerosols by OH ([SO 2 ] ≥ 40 ppb) occur on similar time scales as analogous gas-phase oxidation reactions. These results provide evidence for a previously unidentified mechanism by which organic aerosol oxidation is enhanced by anthropogenic gas phase emissions. (Chemical Equation Presented).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Climate Forcing and Trends of Organic Aerosols in the Community Earth System Model (CESM2)

The Community Earth System Model version 2 (CESM2) includes three main atmospheric configurations: the Community Atmosphere Model version 6 (CAM6) with simplified chemistry and a simplified organic aerosol (OA) scheme, CAM6 with comprehensive tropospheric and stratospheric chemistry representation (CAM6-chem), and the Whole Atmosphere Community Climate Model version 6 (WACCM6). Both, CAM6-chem and WACCM6 include a more comprehensive secondary organic aerosols (SOA) approach using the volatility basis set (vbs) scheme and prognostic stratospheric aerosols. This paper describes the different OA schemes available in the different atmospheric configurations of CESM2 and discusses differences in aerosol burden and resulting climate forcings. Derived OA burden and trends differ due to differences in OA formation using the different approaches. Regional differences in Aerosol Optical Depth with larger values using the comprehensive approach occur over SOA source regions. Stronger increasing SOA trends between 1960 and 2015 in WACCM6 compared to CAM6 are due to increasing biogenic emissions aligned with increasing surface temperatures. Using the comprehensive SOA approach further leads to improved comparisons to aircraft observations and SOA formation of ˜143 Tg/yr. We further use WACCM6 to identify source contributions of OA from biogenic, fossil fuel, and biomass burning emissions, to quantify SOA amounts and trends from these sources. Increasing SOA trends between 1960 and 2015 are the result of increasing biogenic emissions aligned with increasing surface temperatures. Biogenic emissions are at least two thirds of the total SOA burden. In addition, SOA source contributions from fossil fuel emissions become more important, with largest values over Southeast Asia. The estimated total anthropogenic forcing of OA in WACCM6 for 1995–2010 conditions is -0.43 W/m2, mostly from the aerosol direct effect.

Tilmes, S↗
DOE OSTI2024

Long-Term Trends in Aerosols, Low Clouds, and Large-Scale Meteorology Over the Western North Atlantic From 2003 to 2020

Here, a continuous decrease in aerosols over the Western North Atlantic Ocean (WNAO) on a decadal timescale provides a long-term benchmark to evaluate how various natural and anthropogenic processes affect the manifestation of aerosol-cloud interactions in this region. Furthermore, the WNAO serves as a natural laboratory with diverse aerosol sources, marine boundary layer clouds more variable than those in marine stratocumulus deck regions, and unique flow regimes established by the Gulf Stream and the semi-permanent Bermuda High. We investigate how satellite-retrieved macrophysical and microphysical properties of low clouds and the surface shortwave irradiance changed from 2003 to 2020, in tandem with this aerosol decrease. The decadal changes in large-scale meteorology related to the North Atlantic Oscillation (NAO) are also examined. We find a reduction in low-cloud optical thickness, accompanied by fewer and larger cloud droplets, yet observe no significant changes in low-cloud fraction and liquid water path. Despite the reduction in low-cloud optical thickness together with aerosol decrease, a corresponding increase in the trends of surface shortwave irradiance, also known as surface brightening, is lacking. This absence of brightening is potentially related to concomitant changes found in large-scale meteorology associated with NAO—Bermuda High strengthening, sea surface warming, and atmospheric moistening— as well as an increase in high-level cloud fraction that can counteract the surface brightening. Ultimately, our findings suggest that spatial patterns of decadal meteorological variability introduce complexities in the surface cloud radiative effect over the WNAO, thereby complicating the isolation and examination of aerosol-cloud interactions.

54 ENVIRONMENTAL SCIENCES↗