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At least 793 records · Page 44
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Impact of phase state and non-ideal mixing on equilibration timescales of secondary organic aerosol partitioning

Abstract. Evidence has accumulated that secondary organic aerosols (SOAs) exhibit complex morphologies with multiple phases that can adopt amorphous semisolid or glassy phase states. However, experimental analysis and numerical modeling on the formation and evolution of SOA still often employ equilibrium partitioning with an ideal mixing assumption in the particle phase. Here we apply the kinetic multilayer model of gas–particle partitioning (KM-GAP) to simulate condensation of semi-volatile species into a core–shell phase-separated particle to evaluate equilibration timescales of SOA partitioning. By varying bulk diffusivity and the activity coefficient of the condensing species in the shell, we probe the complex interplay of mass transfer kinetics and the thermodynamics of partitioning. We found that the interplay of non-ideality and phase state can impact SOA partitioning kinetics significantly. The effect of non-ideality on SOA partitioning is slight for liquid particles but becomes prominent in semisolid or solid particles. If the condensing species is miscible with a low activity coefficient in the viscous shell phase, the particle can reach equilibrium with the gas phase long before the dissolution of concentration gradients in the particle bulk. For the condensation of immiscible species with a high activity coefficient in the semisolid shell, the mass concentration in the shell may become higher or overshoot its equilibrium concentration due to slow bulk diffusion through the viscous shell for excess mass to be transferred to the core phase. Equilibration timescales are shorter for the condensation of lower-volatility species into semisolid shell; as the volatility increases, re-evaporation becomes significant as desorption is faster for volatile species than bulk diffusion in a semisolid matrix, leading to an increase in equilibration timescale. We also show that the equilibration timescale is longer in an open system relative to a closed system especially for partitioning of miscible species; hence, caution should be exercised when interpreting and extrapolating closed-system chamber experimental results to atmosphere conditions. Our results provide a possible explanation for discrepancies between experimental observations of fast particle–particle mixing and predictions of long mixing timescales in viscous particles and provide useful insights into description and treatment of SOA in aerosol models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Photoaging of phenolic secondary organic aerosol in the aqueous phase: evolution of chemical and optical properties and effects of oxidants

Abstract. While gas-phase reactions are well established to have significant impacts on the mass concentration, chemical composition, and optical properties of secondary organic aerosol (SOA), the aqueous-phase aging of SOA remains poorly understood. In this study, we performed a series of long-duration photochemical aging experiments to investigate the evolution of the composition and light absorption of the aqueous SOA (aqSOA) from guaiacyl acetone (GA), a semivolatile phenolic carbonyl that is common in biomass burning smoke. The aqSOA was produced from reactions of GA with hydroxyl radical (•OH-aqSOA) or a triplet excited state of organic carbon (3C∗-aqSOA) and was then photoaged in water under conditions that simulate sunlight exposure in northern California for up to 48 h. The effects of increasing aqueous-phase •OH or 3C∗ concentration on the photoaging of the aqSOA were also studied. High-resolution aerosol mass spectrometry (HR-AMS) and UV–Vis spectroscopy were utilized to characterize the composition and the light absorptivity of the aqSOA and to track their changes during aging. Compared to •OH-aqSOA, the 3C∗-aqSOA is produced more rapidly and shows less oxidation, a greater abundance of oligomers, and higher light absorption. Prolonged photoaging promotes fragmentation and the formation of more volatile and less light-absorbing products. More than half of the initial aqSOA mass is lost, and substantial photobleaching occurs after 10.5 h of prolonged aging under simulated sunlight illumination for 3C∗-aqSOA and 48 h for •OH-aqSOA. By performing positive matrix factorization (PMF) analysis of the combined HR-AMS and UV–Vis spectral data, we resolved three generations of aqSOA with distinctly different chemical and optical properties. The first-generation aqSOA shows significant oligomer formation and enhanced light absorption at 340–400 nm. The second-generation aqSOA is enriched in functionalized GA species and has the highest mass absorption coefficients in 300–500 nm, while the third-generation aqSOA contains more fragmented products and is the least light absorbing. These results suggest that intermediately aged phenolic aqSOA is more light absorbing than other generations, and that the light absorptivity of phenolic aqSOA results from a competition between brown carbon (BrC) formation and photobleaching, which is dependent on aging time. Although photoaging generally increases the oxidation of aqSOA, a slightly decreased O/C of the •OH-aqSOA is observed after 48 h of prolonged photoaging with additional •OH exposure. This is likely due to greater fragmentation and evaporation of highly oxidized compounds. Increased oxidant concentration accelerates the transformation of aqSOA and promotes the decay of BrC chromophores, leading to faster mass reduction and photobleaching. In addition, compared with •OH, photoaging by 3C∗ produces more low-volatility functionalized products, which counterbalances part of the aqSOA mass loss due to fragmentation and evaporation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

The annual cycle and sources of relevant aerosol precursor vapors in the central Arctic during the MOSAiC expedition

Abstract. In this study, we present and analyze the first continuous time series of relevant aerosol precursor vapors from the central Arctic (north of 80° N) during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. These precursor vapors include sulfuric acid (SA), methanesulfonic acid (MSA), and iodic acid (IA). We use FLEXPART simulations, inverse modeling, sulfur dioxide (SO2) mixing ratios, and chlorophyll a (chl a) observations to interpret the seasonal variability in the vapor concentrations and identify dominant sources. Our results show that both natural and anthropogenic sources are relevant for the concentrations of SA in the Arctic, but anthropogenic sources associated with Arctic haze are the most prevalent. MSA concentrations are an order of magnitude higher during polar day than during polar night due to seasonal changes in biological activity. Peak MSA concentrations were observed in May, which corresponds with the timing of the annual peak in chl a concentrations north of 75° N. IA concentrations exhibit two distinct peaks during the year, namely a dominant peak in spring and a secondary peak in autumn, suggesting that seasonal IA concentrations depend on both solar radiation and sea ice conditions. In general, the seasonal cycles of SA, MSA, and IA in the central Arctic Ocean are related to sea ice conditions, and we expect that changes in the Arctic environment will affect the concentrations of these vapors in the future. The magnitude of these changes and the subsequent influence on aerosol processes remains uncertain, highlighting the need for continued observations of these precursor vapors in the Arctic.

Boyer, Matthew↗
DOE OSTI2024

Secondary organic aerosols derived from intermediate-volatility n-alkanes adopt low-viscous phase state

Abstract. Secondary organic aerosol (SOA) derived from n-alkanes, as emitted from vehicles and volatile chemical products, is a major component of anthropogenic particulate matter, yet the chemical composition and phase state are poorly understood and thus poorly constrained in aerosol models. Here we provide a comprehensive analysis of n-alkane SOA by explicit gas-phase chemistry modeling, machine learning, and laboratory experiments to show that n-alkane SOA adopts low-viscous semi-solid or liquid states. Our study underlines the complex interplay of molecular composition and SOA viscosity: n-alkane SOA with a higher carbon number mostly consists of less functionalized first-generation products with lower viscosity, while the SOA with a lower carbon number contains more functionalized multigenerational products with higher viscosity. This study opens up a new avenue for analysis of SOA processes, and the results indicate few kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA formation in large-scale atmospheric models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Adiabatic and radiative cooling are both important causes of aerosol activation in simulated fog events in Europe

Aerosol–fog interactions affect the visibility in, and life cycle of, fog and are difficult to represent in weather and climate models. Here we explore processes that impact the simulation of fog droplet number concentrations (N d ) at sub-kilometer scale horizontal grid resolutions in the UK Met Office Unified Model. We modify the parameterization of aerosol activation to include droplet activation by radiative cooling in addition to adiabatic cooling and determine the relative importance of the two cooling mechanisms. We further test the sensitivity of simulated N d to: (a) interception of droplets by trees and buildings, (b) overestimation of updrafts in temperature inversions (which leads to artificially high N d values), and (c) potential mechanisms for droplet deactivation due to downward fluctuations in supersaturation. We evaluate our model against observations from the ParisFog and LANFEX field campaigns, building on evaluation described in the companion paper. Including radiative cooling in the activation mechanism improves how accurately we represent the liquid water path and the vertical structure of the fog in our LANFEX case study. However, with radiative cooling, the N d are overestimated for most of the ParisFog cases and for the LANFEX case. The time-averaged overestimate exceeds a factor of three (the normalized mean bias factor exceeds 2.0) in 4 out of 11 ParisFog cases. Our sensitivity studies demonstrate how these overestimates can be mitigated. Assuming the overestimate affects both radiative and adiabatic cooling, we find that although radiative cooling is more often the dominant source, both cooling sources can sometimes dominate activation.

Ghosh, Pratapaditya [Carnegie Mellon University, P↗
DOE OSTI2025

The diurnal susceptibility of subtropical clouds to aerosols

The diurnal susceptibility of clouds and their radiative properties to aerosols is examined during their Lagrangian transition from subtropical stratocumulus to shallow cumulus regimes. Using large-eddy simulations, we analyze the six-day evolution of an air mass along a 3800 km observed trajectory from the coast of Peru toward the equator. Pristine and polluted scenarios are simulated with forcing imposed from weather reanalysis. The polluted scenario exhibits stronger diurnal variations in cloud water, cloud fraction, and albedo, with enhanced nighttime entrainment and suppressed precipitation. The overall response of cloud properties and outgoing shortwave radiation to droplet number concentration follows a distinct diurnal pattern: strong positive cloud adjustments dominate at night and in the morning, while weak negative adjustments prevail in the afternoon. This cycle is driven by the competition between precipitation suppression, which enhances cloud water and coverage, and entrainment drying, which depletes them. In polluted conditions, enhanced entrainment leads to a deeper and more decoupled boundary layer that cannot be sustained by surface fluxes in the afternoon, resulting in negative cloud adjustments. The enhanced entrainment rate under polluted conditions is caused by the reduced sedimentation of cloud and precipitation water from the entrainment zone. While the Twomey effect dominates the diurnal average albedo response, the diurnal variation in the competing cloud adjustments lead to a near-neutral net susceptibility in the afternoon, highlighting the critical role of diurnally varying processes in aerosol-cloud interactions.

Geosciences↗
DOE OSTI2025

Steady-state mixing state of black carbon aerosols from a particle-resolved model

Abstract. Black carbon (BC) exerts a notable warming effect due to its strong light absorption, largely influenced by its “mixing state”. However, due to computational constraints, the mixing state is challenging to accurately represent in large-scale models. In this study, we employ a particle-resolved model to simulate the evolution of BC mixing state based on field observation. Our result shows that aerosol compositions, coating thickness (CT) distribution, and optical properties of BC aerosols all exhibit a tendency toward a steady state with a characteristic timescale of less than 1 d, considerably shorter than the BC atmospheric lifetime. The rapid attainment of a steady state suggests that it is reasonable to disregard this pre-steady-state period and instead concentrate on the average properties of BC across extensive spatial and temporal scales. The distribution of CT follows an exponential linear distribution and can be characterized by a single slope parameter k. This distribution is independent of the BC core's distribution. In the model simulation, the mean CT, equivalent to the 1/k, is 62 nm, which is consistent with the statistical results indicating a mean CT of 63 nm. Utilizing the slope parameter k, which effectively characterizes the CT distribution under the steady-state simplifying assumption, the BC absorption enhancement closely corresponds to the results obtained via the particle-resolved method. This study simplifies the BC mixing state description and yields a precise evaluation of the BC optical properties, which has the potential utility for modeling efforts in the refinement of the assessment of BC's radiative effects.

Zhang, Zhouyang↗
DOE OSTI2025

A new method for diagnosing effective radiative forcing from aerosol–cloud interactions in climate models

Aerosol–cloud interactions (ACIs) are a leading source of uncertainty in estimates of the historical effective radiative forcing (ERF). One reason for this uncertainty is the difficulty in estimating the ERF from aerosol–cloud interactions (ERFaci) in climate models, which typically requires multiple calls to the radiation code. Most commonly used methods also cannot disentangle the contributions from different processes to ERFaci. Here, we develop a new, computationally efficient method for estimating the shortwave (SW) ERFaci from liquid clouds using histograms of monthly averaged cloud fraction partitioned by cloud droplet effective radius (r e ) and liquid water path (LWP). Multiplying the histograms with SW cloud radiative kernels gives the total SW ERFaci from liquid clouds, which can be decomposed into contributions from the Twomey effect, LWP adjustments, and cloud fraction (CF) adjustments. We test the method with data from five CMIP6-era models, using the Moderate Resolution Imaging Spectroradiometer (MODIS) satellite instrument simulator to generate the histograms. Our method gives similar total SW ERFaci estimates to other established methods in regions of prevalent liquid cloud and indicates that the Twomey effect, LWP adjustments, and CF adjustments have contributed -0.34 ± 0.23, -0.22 ± 0.13, and -0.09 ± 0.11 W m -2 , respectively, to the effective radiative forcing of the climate since 1850 in the ensemble mean (95 % confidence). These results demonstrate that widespread adoption of a MODIS r e –LWP joint histogram diagnostic would allow the SW ERFaci and its components to be quickly and accurately diagnosed from climate model outputs, a crucial step for reducing uncertainty in the historical ERF.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Impacts of sea ice leads on sea salt aerosols and atmospheric chemistry in the Arctic

Abstract. The processes contributing to Arctic cold-season (November–April) sea salt aerosols (SSAs) remain uncertain. Observations from coastal Alaska suggest that emissions from open leads in sea ice, which are not included in climate models, may play a dominant role. Their Arctic-wide significance has not yet been quantified. Here, we create an emission parameterization of SSAs from leads by combining satellite data of lead area (the Advanced Microwave Scanning Radiometer–Earth Observation System (AMSR-E) product) and a chemical transport model (GEOS-Chem) to quantify pan-Arctic SSA emissions from leads during the cold season from 2002 to 2008 and to predict their impacts on atmospheric chemistry, evaluating the results of our simulated SSAs against in situ observations. The AMSR-E product detects large leads with certainty (> 3 km in size), and, hence, our study is limited to quantifying emissions from large leads. Lead emissions vary seasonally and interannually. Simulated total monthly SSA emissions increase by 1.1 %–1.8 % (≥60° N latitude) and 5.6 %–7.5 % (≥75° N) for the 2002–2008 cold seasons. SSA concentrations primarily increase at the location of leads, where standard model concentrations are low. GEOS-Chem overestimates SSA concentrations at Arctic sites compared to ground observations, even when lead emissions are not included, suggesting underestimation of SSA sinks and/or uncertainties in SSA emissions from blowing snow and the open ocean. Multi-year monthly mean surface bromine atom (Br) concentrations increase by 2.8 %–8.8 % due to SSAs from leads for the 2002–2008 cold seasons. Changes in ozone concentrations are negligible. While leads contribute < 10 % to Arctic-wide SSA emissions in the years 2002–2008, these emissions occur in regions of low background aerosol concentrations. Leads may increase in frequency under future climate change, which could increase SSA emissions from leads.

Emme, Erin J. (ORCID:0000000268406352)↗
DOE OSTI2025

Merged aerosol size distribution from SMPS and OPC for SAIL

This dataset contains merged aerosol number size distribution data for the Surface Atmosphere Integrated Field Laboratory (SAIL) campaign. The merged size distribution data were constructed by combining measurements from a scanning-mobility particle sizer (SMPS) and an optical particle counter (OPC), covering a size range of 0.01–35 µm. The merging methodology follows the approach described by Hand and Kreidenweis (2002) and Marinescu et al. (2019). All aerosol data from the ARM archive were corrected to standard temperature (273.15 K) and pressure (101.3 kPa).

merged size distribution↗
DOE OSTI2025

Source apportionment of aerosols at the White River IMPROVE site near the SAIL site

This data set contains source apportionment results at the White River IMPROVE site (39.1536, -106.8209), which is about 30 km north of the Surface Atmosphere Integrated Field Laboratory (SAIL) Campaign site. The IMPROVE network (Malm et al. 1994) collected 24-hour aerosol filter samples every three days over several decades at this site. Chemical concentrations in the PM2.5 fraction of 19 elements (Al, As, Br, Ca, Cl, Cr, Cu, Fe, K, Mg, Mn, Na, Ni, Pb, Se, Si, Ti, V, and Zn), along with nitrate, sulfate, elemental carbon (EC), organic carbon (OC), and calculated coarse mass concentrations (PM10−PM2.5 mass concentrations), from 2014 to 2023, were used as input for the PMF analysis. PMF was performed using EPA PMF 5.0 (Norris et al. 2014). A five-factor solution was chosen as the optimal solution. These factors were identified as coarse dust, fine dust, biomass burning, sulfate-dominated, and nitrate-dominated sources. This data set is useful for understanding aerosol sources and their long-term variability near this region.

biomass burning↗
DOE OSTI2021

Aerosol-Based Method Seals the Deal for Tighter New Homes

What if an aerosol-based sealing method could tighten new home envelopes more quickly and effectively than traditional sealing methods? The method involves pressurizing an entire building while dispersing an aerosol sealant "fog" to the building interior. As air escapes the building through leaks in the envelope, sealant particles are carried to the leaks where they make contact and stick, sealing the leaks. A standard blower door and connected laptop facilitate the sealing process and provide real-time feedback and a permanent record of the sealing. The technology is thus capable of simultaneously measuring, locating, and automatically sealing leaks in a building. In fact, hundreds of linear feet of narrow leaks can be sealed simultaneously, reducing the time needed for manual inspection and sealing. To investigate the use of this method in new homes, the Center for Energy and Environment and partners worked with builders who performed the technique on 11 homes in California and 15 homes in Minnesota.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2022

Using the Black Carbon Particle Mixing State to Characterize the Lifecycle of Biomass Burning Aerosols

The lifecycle of black carbon (BC)-containing particles from biomass burns is examined using aircraft and surface observations of BC mixing state for plume ages from ~15 minutes to 10 days. Because BC is non-volatile and chemically inert, changes in the mixing state of BC-containing particles are driven solely by changes in particle coating, which is mainly secondary organic aerosol (SOA). The coating mass initially increases rapidly (k = 0.84 hr-1), then remains growth relatively constant for 1 to 2 days as plume dilution no longer supports further growth, then decreases slowly until only ~30 % of the maximum coating mass remains after 10 days, (kloss = 0.011 hr-1). The mass ratio of coating-to-core for a BC-containing particle with a 100 nm mass- equivalent diameter BC core reaches a maximum of ~20 after a few hours and drops to ~5 after 10 days of aging. The initial increase in coating mass can be used to determine SOA formation rates. The slow loss of coating material, not captured in global models, comprises the dominant fraction of the lifecycle of these particles. Coating-to-core mass ratios of BC particles in the stratosphere are much greater than those in the free troposphere indicating a different lifecycle.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Photolysis Controls Atmospheric Budgets of Biogenic Secondary Organic Aerosol

Secondary organic aerosol (SOA) accounts for a large fraction of tropospheric particulate matter. While SOA production rates and mechanisms have been extensively investigated, loss pathways remain uncertain. Most large-scale chemistry and transport models account for mechanical deposition of SOA, but not chemical losses, such as photolysis. There is also a paucity of laboratory measurements of SOA photolysis, which limits how well photolytic losses can be modeled. Here we show, through a combined experimental and modeling approach, that photolytic loss of SOA mass significantly alters SOA budget predictions. Using environmental chamber experiments, we find that SOA produced from several biogenic volatile organic compounds (VOCs) undergoes photolysis-induced mass loss at rates between 0 and 2.2% ± 0.4% of nitrogen dioxide (NO 2 ) photolysis, equivalent to average atmospheric lifetimes as short as 10 hours. We incorporate our photolysis rates into a regional chemical transport model to test the sensitivity of predicted SOA mass concentrations to photolytic losses. The addition of photolysis at rates consistent with our experimental conditions causes a ~50% reduction in biogenic SOA loadings over the Amazon, indicating that photolysis exerts a substantial control over the atmospheric SOA lifetime, with a likely dependence upon SOA molecular composition and thus production mechanisms.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Enhanced Detection of Primary Biological Aerosol Particles Using Machine Learning and Single-Particle Measurement

Accurately identifying primary biological aerosol particles (PBAPs) using analytical techniques poses inherent challenges due to their resemblance to other atmospheric carbonaceous particles. Here, we present a study of an enhanced method for detecting PBAPs by combining single-particle measurement with advanced supervised machine learning (SML) techniques. We analyzed ambient particles from a variety of environments and lab-generated standards, focusing on chemical composition for traditional rule-based and clustering approaches and incorporating morphological features into the SML approaches, neural networks and XGBoost, for improved accuracy. This study demonstrates that SML methods outperform traditional methods in quantifying PBAPs, achieving significant improvements in precision, recall, F1-score, and accuracy, leading to an increased number of detected PBAPs by at least 19%. The adaptability of the proposed XGBoost-based SML model is showcased in comparison to traditional methods in categorizing PBAPs for blind data sets from different geographical locations. Two field case studies were investigated, over agricultural land and Amazonia rain forest, representing relatively low and high concentrations of PBAPs, respectively, where XGBoost consistently detected up to 3.5 times more PBAPs than traditional methods. Precise detection of PBAPs in the atmosphere could significantly improve the prediction of climatic impacts by them.

42 ENGINEERING↗
DOE OSTI2021

Liquid Containing Clouds at the North Slope of Alaska Demonstrate Sensitivity to Local Industrial Aerosol Emissions

Abstract Cloud condensation nucleus control alter cloud solar albedo through cloud droplet size. Here, we leverage anthropogenic emissions at the North Slope of Alaska as a natural laboratory to study relationships between aerosols and Arctic liquid‐containing clouds. Averaging 14 years of MODIS observations, we found a reduction in temporally averaged cloud effective radius ( ) of up to 1.0 μm related to localized pollution. Pronounced regional gradients in cloud frequency of occurrence and liquid water path prohibit the detection of potential changes of these variables. Observed changes of alter radiative fluxes and increase cloud‐reflected shortwave radiation by up to 0.8 W m − 2 in the Prudhoe Bay area for the period covered by observations (April–September). Due to the frequent occurrence of liquid‐containing clouds, this implies that enhanced local emissions in Arctic regions can impact climate processes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

A 1D Model for Nucleation of Ice From Aerosol Particles: An Application to a Mixed‐Phase Arctic Stratus Cloud Layer

Abstract Mixed‐phase clouds (MPCs) have been identified as significant contributors to uncertainties in climate projections, attributable to model representation of processes controlling the formation and loss of supercooled water droplets and ice particles from the atmosphere. Arctic MPCs are commonly widespread and long‐lived, with sustained ice crystal formation processes that challenge current understanding. This study examines the ice‐nucleating particle (INP) reservoir dynamics governing immersion‐mode heterogeneous freezing in an observed case of Arctic MPCs using a simplified 1D aerosol‐cloud model. The model setup includes prescribed dynamical forcings and thermodynamic profiles, and represents INPs as multicomponent and polydisperse particle size distributions. Diagnostic and prognostic approaches to immersion freezing parameterization are compared, including time‐independent (singular) number‐ and surface area‐based descriptions and a time‐dependent description following classical nucleation theory (CNT). The choice of freezing parameterization defines the size of the INP reservoir. The CNT‐based description yields an orders of magnitude larger INP reservoir than the singular parameterizations, which is the dominant factor for sustained ice crystal formation. The efficiency of the freezing process and cloud cooling are of secondary importance. A diagnostic treatment neglecting INP loss is only accurate when the INP reservoir size is large and INP depletion weak. Since a larger INP reservoir sustains ice crystal formation substantially longer, and ice water path scales with ice crystal concentrations for the conditions considered, resolving the source of differences in INP reservoir dynamics due to model implementation is a high priority for advancing climate model physics.

54 ENVIRONMENTAL SCIENCES↗