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DOE OSTI2025

Implications of reduced-complexity aerosol thermodynamics on organic aerosol mass concentration and composition over North America

Atmospheric organic aerosol (OA) mass concentrations can be affected by water uptake through its impact on the gas–particle partitioning of semi-volatile compounds. Current chemical transport models (CTMs) neglect this process. We have implemented the Binary Activity Thermodynamics model coupled to a volatility basis set partitioning scheme in the GEOS-Chem CTM, providing an efficient reduced-complexity OA model that predicts relative-humidity-dependent mixing and partitioning thermodynamics, while limiting the impact on computational efficiency. We provide a quantitative assessment of this water-sensitive OA treatment, focusing on a subdomain over North America. The updated OA scheme predicts a spatiotemporal mean enhancement in surface-level OA mass concentration of 145 % for January 2019 and 76 % for July 2019 compared to GEOS-Chem's most advanced OA scheme. The temporal mean surface-level OA organic mass concentration can increase by up to ∼590 % for January 2019 and ∼280 % for July 2019, with the greatest enhancements occurring over the ocean. The updated OA scheme also quantifies the OA-associated water content. The simulations show how different OA precursors and related OA surrogates contribute and respond to water uptake, including that due to changes in temperature and relative humidity over the diurnal cycle in selected winter and summer months. These results are independent of future CTM improvements involving updates to chemical reaction schemes and emission inventories. Our water-sensitive OA scheme allows for a better representation of the seasonal and regional variations in OA mass concentration in CTMs.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Simulating organic aerosol in Delhi with WRF-Chem using the volatility-basis-set approach: exploring model uncertainty with a Gaussian process emulator

The nature and origin of organic aerosol in the atmosphere remain unclear. The gas–particle partitioning of semi-volatile organic compounds (SVOCs) that constitute primary organic aerosols (POAs) and the multigenerational chemical aging of SVOCs are particularly poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem (Weather Research and Forecasting model with Chemistry), can be a useful tool to describe emissions of POA and its chemical evolution. However, the evaluation of model uncertainty and the optimal model parameterization may be expensive to probe using only WRF-Chem simulations. Gaussian process emulators, trained on simulations from relatively few WRF-Chem simulations, are capable of reproducing model results and estimating the sources of model uncertainty within a defined range of model parameters. In this study, a WRF-Chem VBS parameterization is proposed; we then generate a perturbed parameter ensemble of 111 model runs, perturbing 10 parameters of the WRF-Chem model relating to organic aerosol emissions and the VBS oxidation reactions. This allowed us to cover the model's uncertainty space and to compare outputs from each run to aerosol mass spectrometer observations of organic aerosol concentrations and O:C ratios measured in New Delhi, India. The simulations spanned the organic aerosol concentrations measured with the aerosol mass spectrometer (AMS). However, they also highlighted potential structural errors in the model that may be related to unsuitable diurnal cycles in the emissions and/or failure to adequately represent the dynamics of the planetary boundary layer. While the structural errors prevented us from clearly identifying an optimized VBS approach in WRF-Chem, we were able to apply the emulator in the following two periods: the full period (1–29 May) and a subperiod period of 14:00–16:00 h LT (local time) on 1–29 May. The combination of emulator analysis and model evaluation metrics allowed us to identify plausible parameter combinations for the analyzed periods. We demonstrate that the methodology presented in this study can be used to determine the model uncertainty and to identify the appropriate parameter combination for the VBS approach and hence to provide valuable information to improve our understanding of OA production.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

The sources and diurnal variations of submicron aerosols in a coastal–rural environment near Houston, US

Aerosol properties were characterized at a rural site southwest of Houston from May to September 2022 during the intensive operation periods (IOPs) of the Tracking Aerosol Convection Interactions ExpeRiment (TRACER). Backward trajectory analysis reveals three major air mass types: marine air mass from the Gulf, urban air mass influenced by urban emissions, and regional air mass. Marine aerosols typically show a bimodal size distribution and have the lowest particle number and mass concentrations of PM 1 (particulate matter with an aerodynamic diameter of less than 1 µm), while aerosols from air masses strongly influenced by urban emissions exhibit the highest concentrations. Organic aerosol (OA) accounts for more than 50 % of PM 1 for urban and regional air masses, whereas sulfate is comparable to OA in marine air masses. Positive matrix factorization (PMF) analysis of aerosol mass spectra identifies 6 OA factors: hydrocarbon-like OA (HOA), OA from the oxidation of monoterpenes (MT-SOA), OA from the reactive uptake of isoprene epoxydiols by acidic sulfate particles (isoprene-SOA), oxygenated OA arising from shipping emissions (shipping-OOA), and two oxygenated OA factors with high O : C ratios (OOA1 and OOA2). OOA2 has the highest O : C ratio and exhibits elevated mass concentration in the afternoon. Similar diurnal variation of highly oxidized OA factors was commonly observed in the Houston area during previous studies and attributed to the SOA formation by photochemistry and mixing from aloft. Here, using air mass backward trajectories and a 1-D box model, we show the diurnal trend of OOA2 mass concentration is instead driven by changes in air mass arriving at the rural site. The air mass changes are likely caused by the shift between land breezes and sea/bay breezes. Within the same air mass type (e.g., either urban or marine air mass), OOA2 mass concentration is largely independent of wind direction and shows essentially no diurnal variation, suggesting OOA2 is related to aged OA with minimal influence by local emissions. This study helps identify the major sources of OA in the Houston region and highlights the impacts of both atmospheric chemistry and meteorology on aerosol properties in the coastal–rural environment.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Quantifying the impacts of marine aerosols over the southeast Atlantic Ocean using a chemical transport model: implications for aerosol–cloud interactions

The southeast Atlantic region, characterized by persistent stratocumulus clouds, has one of the highest uncertainties in aerosol radiative forcing and significant variability across climate models. In this study, we analyze the seasonally varying role of marine aerosol sources and identify key uncertainties in aerosol composition at cloud-relevant altitudes over the southeast Atlantic using the GEOS-Chem chemical transport model. We evaluate simulated aerosol optical depth (AOD) and speciated aerosol concentrations against those collected from ground observations and aircraft campaigns such as LASIC, ORACLES, and CLARIFY, conducted during 2017. The model consistently underestimates AOD relative to AERONET, particularly at remote locations like Ascension Island. However, when compared with aerosol mass concentrations from aircraft campaigns during the biomass burning period, it performs adequately at cloud-relevant altitudes, with a normalized mean bias (NMB) between -3.5 % (CLARIFY) and -7.5 % (ORACLES). At these altitudes, in the model, organic aerosols (63 %) dominate during the biomass burning period, while sulfate (41 %) prevails during austral summer, when dimethylsulfide (DMS) emissions peak in the model. Our findings indicate that marine sulfate can account for up to 69 % of total sulfate during the high-DMS period. Sensitivity analyses indicate that refining DMS emissions and oxidation chemistry may increase sulfate aerosol produced from marine sources, highlighting that there remains large uncertainty as to the role of DMS emissions in the marine boundary layer. Additionally, we find marine primary organic aerosol emissions may substantially increase total organic aerosol concentrations, particularly during austral summer. This study underscores the imperative need to refine marine emissions and their chemical transformations, as aerosols from marine sources are a major component of total aerosols at cloud-relevant altitudes and may impact uncertainties in aerosol radiative forcing over the southeast Atlantic.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Widespread 2013-2020 decreases and reduction challenges of organic aerosol in China

Abstract High concentrations of organic aerosol (OA) occur in Asian countries, leading to great health burdens. Clean air actions have resulted in significant emission reductions of air pollutants in China. However, long-term nation-wide trends in OA and their causes remain unknown. Here, we present both observational and model evidence demonstrating widespread decreases with a greater reduction in primary OA than in secondary OA (SOA) in China during the period of 2013 to 2020. Most of the decline is attributed to reduced residential fuel burning while the interannual variability in SOA may have been driven by meteorological variations. We find contrasting effects of reducing NO x and SO 2 on SOA production which may have led to slight overall increases in SOA. Our findings highlight the importance of clean energy replacements in multiple sectors on achieving air-quality targets because of high OA precursor emissions and fluctuating chemical and meteorological conditions.

Chen, Qi (ORCID:0000000335598914)↗

DOE OSTI2025

Burning conditions and transportation pathways determine biomass-burning aerosol properties in the Ascension Island marine boundary layer

Abstract. African biomass-burning aerosol (BBA) in the southeast Atlantic Ocean (SEA) marine boundary layer (MBL) is an important contributor to Earth's radiation budget, yet its representation remains poorly constrained in regional and global climate models. Data from the Layered Atlantic Smoke Interactions with Clouds (LASIC) field campaign on Ascension Island (7.95° S, 14.36° W) provide insight into how burning conditions, fuel type, transport pathways, and atmospheric processing affect the chemical, microphysical, and optical properties of BBA between June and September 2017. A total of 10 individual plume events characterize the seasonal evolution of the BBA properties. Early-season inefficient fires, determined by low refractory black carbon to above-background carbon monoxide mixing ratios (rBC : ΔCO), led to enhanced concentrations of organic- and sulfate-rich aerosols. Mid-season efficient fires, determined by higher rBC : ΔCO values, led to rBC-enriched BBA. A mix of efficient and inefficient fires later in the season resulted in conflicting BBA properties. Prolonged transport (∼ 10 d) through the MBL and lower free troposphere (FT) facilitated chemical and aqueous-phase processing, which led to a reduction in organic aerosol mass concentrations. This resulted in lower organic aerosol (OA) to rBC (OA : rBC) mass ratios (2–5) in the MBL compared to higher values (5–15) in the nearby FT. These atmospheric and cloud oxidation processes yield more light-absorbing BBA and explain the notably low single-scattering albedo at 530 nm (SSA530) values (< 0.80) observed in the MBL. This study establishes a robust correlation between SSA530 and OA : rBC across the MBL and FT, underscoring the dependency of optical properties on chemical composition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Modeling the smoky troposphere of the southeast Atlantic: a comparison to ORACLES airborne observations from September of 2016

The southeast Atlantic is home to well-defined smoke outflow from Africa coinciding vertically with extensive marine boundary-layer cloud decks, both reaching their climatological maxima in spatial extent around September. A framework is put forth for evaluating the performance of a range of global and regional aerosol models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016. The sparse airborne observations are first aggregated into 2o grid boxes and into three vertical layers: the cloud-topped marine boundary layer (MBL), the layer from cloud top to 3 km, and the 3-6 km layer. Aerosol extensive properties simulated for the entire study region for all September suggest that the 2016 ORACLES observations are reasonably representative of the regional monthly average, with systematic deviations of 30% or less. All six models typically place the bottom of the smoke layer at lower altitudes than do the airborne lidar observations by 300-1400 m, whereas model aerosol top heights are within 0-500 m of the observations. All but one of the models that report carbonaceous aerosol masses underestimate the ratio of particulate extinction to the masses, a proxy for mass extinction efficiency, in 3-6 km. Notable findings on individual models include that WRF-CAM5 predicts the mass of black carbon and organic aerosols with minor (~10% or less) biases. GEOS-5 overestimates the carbonaceous particle masses in the MBL by a factor of 3-6. Extinction coefficients in the free troposphere (FT) and above-cloud aerosol optical depth (ACAOD) are 10-30% lower in WRF-CAM5, 30-50% lower in GEOS-5, 10-40% higher in GEOS-Chem, 10-20% higher in EAM-E3SM except for the practically unbiased 3-6 km extinction, and 20-70% lower in the Unified Model, than the airborne in situ, lidar and sunphotometer measurements. ALADIN-Climate also underestimates the ACAOD, by 30%. GEOS-5 and GEOS-Chem predict carbon monoxide in the MBL with small (10% or less) negative biases, despite their overestimates of carbonaceous aerosol masses. Overall, this study highlights a new approach to utilizing airborne aerosol measurements for model diagnosis.

Shinozuka, Yohei↗

NASA NTRS2020

Modeling the smoky troposphere of the southeast Atlantic: a comparison to ORACLES airborne observations from September of 2016

In the southeast Atlantic, well-defined smoke plumes from Africa advect over marine boundary layer cloud decks; both are most extensive around September, when most of the smoke resides in the free troposphere. A framework is put forth for evaluating the performance of a range of global and regional atmospheric composition models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016. A strength of the comparison is a focus on the spatial distribution of a wider range of aerosol composition and optical properties than has been done previously. The sparse airborne observations are aggregated into approximately 2° grid boxes and into three vertical layers: 3–6 km, the layer from cloud top to 3 km, and the cloud-topped marine boundary layer. Simulated aerosol extensive properties suggest that the flight-day observations are reasonably representative of the regional monthly average, with systematic deviations of 30 % or less. Evaluation against observations indicates that all models have strengths and weaknesses, and there is no single model that is superior to all the others in all metrics evaluated. Whereas all six models typically place the top of the smoke layer within 0–500 m of the airborne lidar observations, the models tend to place the smoke layer bottom 300–1400 m lower than the observations. A spatial pattern emerges, in which most models underestimate the mean of most smoke quantities (black carbon, extinction, carbon monoxide) on the diagonal corridor between 16° S, 6° E, and 10° S, 0° E, in the 3–6 km layer, and overestimate them further south, closer to the coast, where less aerosol is present. Model representations of the above-cloud aerosol optical depth differ more widely. Most models overestimate the organic aerosol mass concentrations relative to those of black carbon, and with less skill, indicating model uncertainties in secondary organic aerosol processes. Regional-mean free-tropospheric model ambient single scattering albedos vary widely, between 0.83 and 0.93 compared with in situ dry measurements centered at 0.86, despite minimal impact of humidification on particulate scattering. The modeled ratios of the particulate extinction to the sum of the black carbon and organic aerosol mass concentrations (a mass extinction efficiency proxy) are typically too low and vary too little spatially, with significant inter-model differences. Most models overestimate the carbonaceous mass within the offshore boundary layer. Overall, the diversity in the model biases suggests that different model processes are responsible. The wide range of model optical properties requires further scrutiny because of their importance for radiative effect estimates.

Yohei Shinozuka↗

DOE OSTI2024

Capturing the Relative‐Humidity‐Sensitive Gas–Particle Partitioning of Organic Aerosols in a 2D Volatility Basis Set

Abstract Aerosol water affects the physicochemical properties and mass concentration of organic aerosols (OA), but it is typically omitted by air quality, weather, and climate models. We compare two classes of simplified models to estimate the OA water uptake and gas–particle partitioning of organic compounds. One class uses a single‐hygroscopicity‐parameter (κ) approach while the other is based on the reduced‐complexity Binary Activity Thermodynamics (BAT) model. We show that a BAT‐based two‐dimensional volatility basis set (VBS) model always predicts a higher OA mass concentration at elevated relative humidity (RH), for example, ∼16% at 80% RH, than any variation of theκ‐based method considered—even when BAT‐VBS predicts a lower water uptake. The main reason being that the BAT‐VBS model captures variations in effective saturation mass concentration of organics (C*) with RH, a feature that other VBS methods lack. The BAT‐VBS framework offers an efficient, RH‐sensitive treatment for reduced‐complexity OA modeling.

Geology↗

DOE OSTI2023

TRACER-CAT Laser only SP-AMS measurements

Composition of black carbon containing aerosol was measured using laser-only soot particle aerosol mass spectrometer. This was done as part of TRACER-CAT in July 2022 at the La Porte, TX field site. Dataset includes the time series of black carbon (HRBC), organic aerosol (HROrg), sulfate (HRSO4), nitrate (HRNO3), chloride (HRChl), ammonium (HRNH4).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Contemporary sources dominate carbonaceous aerosol on the North Slope of Alaska

As the Arctic continues to change and warm rapidly, it is increasingly important to understand the organic carbon (OC) contribution to Arctic aerosol. Biogenic sources of primary and secondary OC in the Arctic will be impacted by climate change, including warming temperatures and earlier snow and ice melt. Here, this study focuses on identifying potential sources and regional influences on the seasonal concentration of organic aerosol through analysis of chemical and isotopic composition. Aerosol samples were collected at two sites on the North Slope of Alaska ($Utqia\dot{g}vik$, UQK, and Oliktok Point, OLK, which is in an Arctic oilfield) over three summers from 2015 to 2017. The elemental carbon (EC) trends at each site were used to understand local combustion influences. Local sources drove EC concentrations at Oliktok Point, where high EC was attributed to oil and gas extraction activity, including diesel combustion emissions. $Utqia\dot{g}vik$ had very low EC in the summer. OC was more similar in concentration and well correlated between the two sites with high contributions of contemporary carbon by radiocarbon apportionment (UQK = 74%, OLK = 63%), which could include both marine and terrestrial sources of contemporary carbon (e.g. primary and secondary biogenic, biomass burning and/or associated SOA, and bioaerosols). OC concentrations are strongly correlated to maximum ambient temperatures on the NSA during the summer, which may have implications for predicting future OC aerosol concentrations in a warming Arctic. Biomass burning was determined to be an episodic influence at both sites, based on interpretation of combined aerosol composition, air mass trajectories, and remote sensing of smoke plumes. The results from this study overall strongly suggests contribution from regional sources of contemporary organic aerosol on the NSA, but additional analysis is needed to better constrain contributions from both biogenic sources (terrestrial and/or marine) and bioaerosol to better understand temperature-related aerosol processes in the Arctic.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Dilution impacts on smoke aging: evidence in Biomass Burning Observation Project (BBOP) data

Abstract. Biomass burning emits vapors and aerosols into the atmosphere that can rapidly evolve as smoke plumes travel downwind and dilute, affecting climate- and health-relevant properties of the smoke. To date, theory has been unable to explain observed variability in smoke evolution. Here, we use observational data from the Biomass Burning Observation Project (BBOP) field campaign and show that initial smoke organic aerosol mass concentrations can help predict changes in smoke aerosol aging markers, number concentration, and number mean diameter between 40–262 nm. Because initial field measurements of plumes are generally >10 min downwind, smaller plumes will have already undergone substantial dilution relative to larger plumes and have lower concentrations of smoke species at these observations closest to the fire. The extent to which dilution has occurred prior to the first observation is not a directly measurable quantity. We show that initial observed plume concentrations can serve as a rough indicator of the extent of dilution prior to the first measurement, which impacts photochemistry, aerosol evaporation, and coagulation. Cores of plumes have higher concentrations than edges. By segregating the observed plumes into cores and edges, we find evidence that particle aging, evaporation, and coagulation occurred before the first measurement. We further find that on the plume edges, the organic aerosol is more oxygenated, while a marker for primary biomass burning aerosol emissions has decreased in relative abundance compared to the plume cores. Finally, we attempt to decouple the roles of the initial concentrations and physical age since emission by performing multivariate linear regression of various aerosol properties (composition, size) on these two factors.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2020

How emissions uncertainty influences the distribution and radiative impacts of smoke from fires in North America

Fires and the aerosols that they emit impact air quality, health, and climate, but the abundance and properties of carbonaceous aerosol (both black carbon and organic carbon) from biomass burning (BB) remain uncertain and poorly constrained. We aim to explore the uncertainties associated with fire emissions and their air quality and radiative impacts from underlying dry matter consumed and emissions factors. To investigate this, we compare model simulations from a global chemical transport model, GEOS-Chem, driven by a variety of fire emission inventories with surface and airborne observations of black carbon (BC) and organic aerosol (OA) concentrations and satellite-derived aerosol optical depth (AOD). We focus on two fire-detection-based and/or burned-area-based (FD-BA) inventories using burned area and active fire counts, respectively, i.e., the Global Fire Emissions Database version 4 (GFED4s) with small fires and the Fire INventory from NCAR version 1.5 (FINN1.5), and two fire radiative power (FRP)-based approaches, i.e., the Quick Fire Emission Dataset version 2.4 (QFED2.4) and the Global Fire Assimilation System version 1.2 (GFAS1.2). We show that, across the inventories, emissions of BB aerosol (BBA) differ by a factor of 4 to 7 over North America and that dry matter differences, not emissions factors, drive this spread. We find that simulations driven by QFED2.4 generally overestimate BC and, to a lesser extent, OA concentrations observations from two fire-influenced aircraft campaigns in North America (ARCTAS and DC3) and from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network, while simulations driven by FINN1.5 substantially underestimate concentrations. The GFED4s and GFAS1.2-driven simulations provide the best agreement with OA and BC mass concentrations at the surface (IMPROVE), BC observed aloft (DC3 and ARCTAS), and AOD observed by MODIS over North America. We also show that a sensitivity simulation including an enhanced source of secondary organic aerosol (SOA) from fires, based on the NOAA Fire Lab 2016 experiments, produces substantial additional OA; however, the spread in the primary emissions estimates implies that this magnitude of SOA can be neither confirmed nor ruled out when comparing the simulations against the observations explored here. Given the substantial uncertainty in fire emissions, as represented by these four emission inventories, we find a sizeable range in 2012 annual BBA PM2.5 population-weighted exposure over Canada and the contiguous US (0.5 to 1.6 µg/cu. m). We also show that the range in the estimated global direct radiative effect of carbonaceous aerosol from fires (−0.11 to −0.048 W/sq. m) is large and comparable to the direct radiative forcing of OA (−0.09 W/sq. m) estimated in the Fifth Assessment Report (AR5) of the Intergovernmental Panel on Climate Change (IPCC). Our analysis suggests that fire emissions uncertainty challenges our ability to accurately characterize the impact of smoke on air quality and climate.

North America↗

NASA NTRS2015

Implementing Marine Organic Aerosols Into the GEOS-Chem Model

Marine-sourced organic aerosols (MOA) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem model. The implemented emission scheme improved the large under-prediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOA observed during the summertime at an inland site near Paris, France. Our study shows that MOA have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having > 10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly-emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.

Aerosols↗

DOE OSTI2023

TRACER-MAP AMS Measurement

Aerosol composition was measured by using the high resolution time-of-flight aerosol mass spectrometer (HR ToF-AMS). The data were collected at five different sites (AMF1, Aldine, University of Houston (UH), Jones Forest (JF), San Jacinto Battleground (BG)) from July to August, 2022. Dataset includes time series of five species of aerosol composition: Organic, sulfate (SO4), nitrate (NO3), ammonium (NH4), chlorine (Chl)

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Dependence of Deep Convective Cell Properties on Meteorological and Aerosol Conditions during TRACER

Deep convective cells significantly influence Earth’s energy balance and water cycle. However, their accurate representation in numerical models remains challenging due to their small spatiotemporal scales and limited observational constraints. This study examines over ∼400 deep convective cells near Houston, observed by a dual-polarization C-band radar during the Tracking Aerosol Convection Interactions Experiment (TRACER) intensive observation period (June–September 2022). Cells are categorized by lifetime into short-lived (<40 min), intermediate-lived (40–80 min), and long-lived (80+ min) groups. Long-lived cells were broader (∼13.2 km at 2–4-km height) and deeper (∼11.4 km) than short-lived cells (∼6.4-km width, ∼7.31-km height). Using random forest (RF) modeling and correlation analyses, precipitable water vapor (PWV), 2–6-km lapse rate, 0–8-km bulk shear, and fine aerosol mass concentration (Mass_f) are identified as key predictors of cell lifetime. Higher PWV is associated with significantly longer convective cell lifetimes compared to the low-PWV group, particularly within low 2–6-km temperature lapse rate (LR_26km), moderate-to-higher 0–8-km bulk shear (BS_08km), and low-to-moderate Mass_f environments. RF analysis also identifies low-level (0–2 km) equivalent potential temperature, PWV, Mass_f, and surface latent heat flux as key predictors for cell width and height. Short-lived cells have higher aerosol number concentrations (500–1000-nm size range), linked to onshore wind conditions and marine aerosols; however, their low concentration suggests the sensitivity may reflect associated meteorological regimes rather than a direct aerosol effect. Long-lived cells have higher concentrations of organic and sulfate aerosols, while short-lived cells exhibit higher black carbon concentrations. These results highlight the intricate dependence of convective cell lifetimes and structure on environmental moisture, thermodynamics, wind shear, and aerosol characteristics.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2018

Can Semi-Volatile Organic Aerosols Lead to Fewer Cloud Particles?

The impact of condensing organic aerosols on activated cloud number concentration is examined in a new aerosol microphysics box model, MATRIX-VBS. The model includes the volatility-basis set (VBS) framework coupled with the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) that resolves aerosol mass and number concentrations and aerosol mixing state. By including the condensation of organic aerosols, the new model produces less activated particles compared to the original model, which treats organic aerosols as non-volatile. Parameters such as aerosol chemical composition, mass and number concentrations, and particle sizes which affect activated cloud number concentration are thoroughly tested via a suite of Monte-Carlo simulations. Results show that by considering semi-volatile organics in MATRIX-VBS, there is lower activated particle number concentration, except in cases with low cloud updrafts, in clean environment at above freezing temperatures, and in polluted environments at high temperature (310K) and extremely low humidity conditions.

Gao, Chloe Y.↗

DOE OSTI2025

Uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effects

We used the CAM5 model to examine how different particle-bound polycyclic aromatic hydrocarbon (PAH) degradation approaches affect the spatial distribution of benzo(a)pyrene (BaP). Three approaches were evaluated: NOA (no effect of OA coatings state on BaP), shielded (viscous OA coatings shield BaP from oxidation under cool and dry conditions) and ROI-T (viscous OA coatings slow BaP oxidation in response to temperature and humidity). Results show that BaP concentrations vary seasonally, influenced by emissions, deposition, transport and degradation approach, all of which are influenced by meteorological conditions. All simulations predict higher population-weighted global average (PWGA) fresh BaP concentrations during December–January–February (DJF) compared to June–July–August (JJA), due to increased emissions from household activities and reduced removal processes during colder months. The shielded and ROI-T approaches, which account for OA coatings, result in 2–6 times higher BaP concentrations in DJF compared to NOA. The shielded simulation predicts the highest PWGA fresh BaP concentration (1.3 ng m −3 ), with 90 % of BaP protected from oxidation. In contrast, the ROI-T approach forecasts lower concentrations in middle to low latitudes, as it assumes less effective OA coatings under warmer, more humid conditions. Evaluations against observed BaP concentrations show the shielded approach performs best, with a normalized mean bias (NMB) within ± 20 %. The combined incremental lifetime cancer risk (ILCR) for both fresh and oxidized PAHs is similar across simulations, emphasizing the importance of considering both forms in health risk assessments. This study highlights the critical role of accurate degradation approaches in PAH modeling.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗