Quantifying Prescribed-Fire Smoke Exposure Using Low-Cost Sensors and Satellites: Springtime Burning in Eastern Kansas.

Prescribed fires (fires intentionally set for mitigation purposes) produce pollutants, which have negative effects on human and animal health. One of the pollutants produced from fires is fine particulate matter (PM2.5). The Flint Hills (FH) region of Kansas experiences extensive prescribed burning each spring (March-May). Smoke from prescribed fires is often understudied due to a lack of monitoring in the rural regions where prescribed burning occurs, as well as the short duration and small size of the fires. Our goal was to attribute PM2.5 concentrations to the prescribed burning in the FH. To determine PM2.5 increases from local burning, we used low-cost PM2.5 sensors (PurpleAir) and satellite observations. The FH were also affected by smoke transported from fires in other regions during 2022. We separated the transported smoke from smoke from fires in eastern Kansas. Based on data from the PurpleAir sensors, we found the 24-hr median PM2.5 to increase by 3.0-5.3 µg m-3 (based on different estimates) on days impacted by smoke from fires in the eastern Kansas region compared to days unimpacted by smoke. The FH region was the most impacted by smoke PM2.5 compared to other regions of Kansas, as observed in satellite products and in situ measurements. Additionally, our study found that hourly PM2.5 estimates from a satellite-derived product aligned with our ground-based measurements. Satellite-derived products are useful in rural areas like the FH, where monitors are scarce, providing important PM2.5 estimates.

On Nucleation Pathways and Particle Size Distribution Evolutions in Stratospheric Aircraft Exhaust Plumes with H2SO4 Enhancement.

Stratospheric aerosol injection (SAI) is proposed as a means of reducing global warming and climate change impacts. Similar to aerosol enhancements produced by volcanic eruptions, introducing particles into the stratosphere would reflect sunlight and reduce the level of warming. However, uncertainties remain about the roles of nucleation mechanisms, ionized molecules, impurities (unevaporated residuals of injected precursors), and ambient conditions in the generation of SAI particles optimally sized to reflect sunlight. Here, we use a kinetic ion-mediated and homogeneous nucleation model to study the formation of H2SO4 particles in aircraft exhaust plumes with direct injection of H2SO4 vapor. We find that under the conditions that produce particles of desired sizes (diameter ∼200-300 nm), nucleation occurs in the nascent (t < 0.01 s), hot (T = 360-445 K), and dry (RH = 0.01-0.1%) plume and is predominantly unary. Nucleation on chemiions occurs first, followed by neutral new particle formation, which converts most of the injected H2SO4 vapor to particles. Coagulation in the aging and diluting plumes governs the subsequent evolution to a narrow (σg = 1.3) particle size distribution. Scavenging by exhaust soot is negligible, but scavenging by acid impurities or incomplete H2SO4 evaporation in the hot exhaust plume and enhanced background aerosols can matter. This research highlights the need to obtain laboratory and/or real-world experiment data to verify the model prediction.

Arctic warming by abundant fine sea salt aerosols from blowing snow.

The Arctic warms nearly four times faster than the global average, and aerosols play an increasingly important role in Arctic climate change. In the Arctic, sea salt is a major aerosol component in terms of mass concentration during winter and spring. However, the mechanisms of sea salt aerosol production remain unclear. Sea salt aerosols are typically thought to be relatively large in size but low in number concentration, implying that their influence on cloud condensation nuclei population and cloud properties is generally minor. Here we present observational evidence of abundant sea salt aerosol production from blowing snow in the central Arctic. Blowing snow was observed more than 20% of the time from November to April. The sublimation of blowing snow generates high concentrations of fine-mode sea salt aerosol (diameter below 300 nm), enhancing cloud condensation nuclei concentrations up to tenfold above background levels. Using a global chemical transport model, we estimate that from November to April north of 70° N, sea salt aerosol produced from blowing snow accounts for about 27.6% of the total particle number, and the sea salt aerosol increases the longwave emissivity of clouds, leading to a calculated surface warming of +2.30 W m-2 under cloudy sky conditions.

Secondary Organic Aerosol Formation from Volatile Chemical Product Emissions: Model Parameters and Contributions to Anthropogenic Aerosol.

Volatile chemical products (VCP) are an increasingly important source of hydrocarbon and oxygenated volatile organic compound (OVOC) emissions to the atmosphere, and these emissions are likely to play an important role as anthropogenic precursors for secondary organic aerosol (SOA). While the SOA from VCP hydrocarbons is often accounted for in models, the formation, evolution, and properties of SOA from VCP OVOCs remain uncertain. We use environmental chamber data and a kinetic model to develop SOA parameters for 10 OVOCs representing glycols, glycol ethers, esters, oxygenated aromatics, and amines. Model simulations suggest that the SOA mass yields for these OVOCs are of the same magnitude as widely studied SOA precursors (e.g., long-chain alkanes, monoterpenes, and single-ring aromatics), and these yields exhibit a linear correlation with the carbon number of the precursor. When combined with emissions inventories for two megacities in the United States (US) and a US-wide inventory, we find that VCP VOCs react with OH to form 0.8-2.5× as much SOA, by mass, as mobile sources. Hydrocarbons (terpenes, branched and cyclic alkanes) and OVOCs (terpenoids, glycols, glycol ethers) make up 60-75 and 25-40% of the SOA arising from VCP use, respectively. This work contributes to the growing body of knowledge focused on studying VCP VOC contributions to urban air pollution.

The Effects of Trash, Residential Biofuel, and Open Biomass Burning Emissions on Local and Transported PM2.5 and Its Attributed Mortality in Africa.

Long-term exposure to ambient fine particulate matter (PM2.5) is the second leading risk factor of premature death in Sub-Saharan Africa. We use GEOS-Chem to quantify the effects of (a) trash burning, (b) residential solid-fuel burning, and (c) open biomass burning (BB) (i.e., landscape fires) on ambient PM2.5 and PM2.5-attributable mortality in Africa. Using a series of sensitivity simulations, we excluded each of the three combustion sources in each of five African regions. We estimate that in 2017 emissions from these three combustion sources within Africa increased global ambient PM2.5 by 2%, leading to 203,000 (95% confidence interval: 133,000-259,000) premature mortalities yr-1 globally and 167,000 premature mortalities yr-1 in Africa. BB contributes more ambient PM2.5-related premature mortalities per year (63%) than residential solid-fuel burning (29%) and trash burning (8%). Open BB in Central Africa leads to the largest number of PM2.5-attributed mortalities inside the region, while trash burning in North Africa and residential solid-fuel burning in West Africa contribute the most regional mortalities for each source. Overall, Africa has a unique ambient air pollution profile because natural sources, such as windblown dust and BB, contribute strongly to ambient PM2.5 levels and PM2.5-related mortality. Air pollution policies may need to focus on taking preventative measures to avoid exposure to ambient PM2.5 from these less-controllable sources.

From the HOMEChem frying pan to the outdoor atmosphere: chemical composition, volatility distributions and fate of cooking aerosol.

Cooking organic aerosol (COA) is frequently observed in urban field studies. Like other forms of organic aerosol, cooking emissions partition between gas and particle phases; a quantitative understanding of the species volatility governing this partitioning is essential to model the transport and fate of COA. However, few cooking-specific volatility measurements are available, and COA is often assumed to be semi-volatile. We use measurements from a thermodenuder coupled to an aerosol chemical speciation monitor during the HOMEChem study to investigate the chemical components and volatility of near-source COA. We found that fresh emissions of COA have three chemical components: a biomass burning-like component (COABBOA), a lower volatility component associated with cooking oil (COAoil-2), and a higher volatility component associated with cooking oil (COAoil-1). We provide characteristic mass spectra and volatility profiles for these components. We develop a model to describe the partitioning of these emissions as they dilute through the house and outdoor atmosphere. We show that the total emissions from cooking can be misclassified in air quality studies that use semi-volatile emissions as a proxy for cooking aerosol, due to the presence of substantial mass in lower volatility bins of COA not generally represented in models. Primary emissions of COA can thus be not only primary sources of urban aerosol pollution, but also sources of semi-volatile organic compounds that undergo secondary chemistry in the atmosphere and contribute to ozone formation and secondary organic aerosol.

Vapors Are Lost to Walls, Not to Particles on the Wall: Artifact-Corrected Parameters from Chamber Experiments and Implications for Global Secondary Organic Aerosol.

Atmospheric models of secondary organic aerosol (OA) (SOA) typically rely on parameters derived from environmental chambers. Chambers are subject to experimental artifacts, including losses of (1) particles to the walls (PWL), (2) vapors to the particles on the wall (V2PWL), and (3) vapors to the wall directly (VWL). We present a method for deriving artifact-corrected SOA parameters and translating these to volatility basis set (VBS) parameters for use in chemical transport models (CTMs). Our process involves combining a box model that accounts for chamber artifacts (Statistical Oxidation Model with a TwO-Moment Aerosol Sectional model (SOM-TOMAS)) with a pseudo-atmospheric simulation to develop VBS parameters that are fit across a range of OA mass concentrations. We found that VWL led to the highest percentage change in chamber SOA mass yields (high NOx: 36-680%; low NOx: 55-250%), followed by PWL (high NOx: 8-39%; low NOx: 10-37%), while the effects of V2PWL are negligible. In contrast to earlier work that assumed that V2PWL was a meaningful loss pathway, we show that V2PWL is an unimportant SOA loss pathway and can be ignored when analyzing chamber data. Using our updated VBS parameters, we found that not accounting for VWL may lead surface-level OA to be underestimated by 24% (0.25 µg m-3) as a global average or up to 130% (9.0 µg m-3) in regions of high biogenic or anthropogenic activity. Finally, we found that accurately accounting for PWL and VWL improves model-measurement agreement for fine mode aerosol mass concentrations (PM2.5) in the GEOS-Chem model.

Disparities in Air Pollutants Across Racial, Ethnic, and Poverty Groups at US Public Schools.

We investigate socioeconomic disparities in air quality at public schools in the contiguous US using high resolution estimates of fine particulate matter (PM2.5) and nitrogen dioxide (NO2) concentrations. We find that schools with higher proportions of people of color (POC) and students eligible for the federal free or reduced lunch program, a proxy for poverty level, are associated with higher pollutant concentrations. For example, we find that the median annual NO2 concentration for White students, nationally, was 7.7 ppbv, compared to 9.2 ppbv for Black and African American students. Statewide and regional disparities in pollutant concentrations across racial, ethnic, and poverty groups are consistent with nationwide results, where elevated NO2 concentrations were associated with schools with higher proportions of POC and higher levels of poverty. Similar, though smaller, differences were found in PM2.5 across racial and ethnic groups in most states. Racial, ethnic, and economic segregation across the rural-urban divide is likely an important factor in pollution disparities at US public schools. We identify distinct regional patterns of disparities, highlighting differences between California, New York, and Florida. Finally, we highlight that disparities exist not only across urban and non-urban lines but also within urban environments.

Process-Level Modeling Can Simultaneously Explain Secondary Organic Aerosol Evolution in Chambers and Flow Reactors.

Secondary organic aerosol (SOA) data gathered in environmental chambers (ECs) have been used extensively to develop parameters to represent SOA formation and evolution. The EC-based parameters are usually constrained to less than one day of photochemical aging but extrapolated to predict SOA aging over much longer timescales in atmospheric models. Recently, SOA has been increasingly studied in oxidation flow reactors (OFRs) over aging timescales of one to multiple days. However, these OFR data have been rarely used to validate or update the EC-based parameters. The simultaneous use of EC and OFR data is challenging because the processes relevant to SOA formation and evolution proceed over very different timescales, and both reactor types exhibit distinct experimental artifacts. In this work, we show that a kinetic SOA chemistry and microphysics model that accounts for various processes, including wall losses, aerosol phase state, heterogeneous oxidation, oligomerization, and new particle formation, can simultaneously explain SOA evolution in EC and OFR experiments, using a single consistent set of SOA parameters. With α-pinene as an example, we first developed parameters by fitting the model output to the measured SOA mass concentration and oxygen-to-carbon (O:C) ratio from an EC experiment (<1 day of aging). We then used these parameters to simulate SOA formation in OFR experiments and found that the model overestimated SOA formation (by a factor of 3-16) over photochemical ages ranging from 0.4 to 13 days, when excluding the abovementioned processes. By comprehensively accounting for these processes, the model was able to explain the observed evolution in SOA mass, composition (i.e., O:C), and size distribution in the OFR experiments. This work suggests that EC and OFR SOA data can be modeled consistently, and a synergistic use of EC and OFR data can aid in developing more refined SOA parameters for use in atmospheric models.

Heterogeneous Nucleation Drives Particle Size Segregation in Sequential Ozone and Nitrate Radical Oxidation of Catechol.

Secondary organic aerosol formation via condensation of organic vapors onto existing aerosol transforms the chemical composition and size distribution of ambient aerosol, with implications for air quality and Earth's radiative balance. Gas-to-particle conversion is generally thought to occur on a continuum between equilibrium-driven partitioning of semivolatile molecules to the pre-existing mass size distribution and kinetic-driven condensation of low volatility molecules to the pre-existing surface area size distribution. However, we offer experimental evidence in contrast to this framework. When catechol is sequentially oxidized by O3 and NO3 in the presence of (NH4)2SO4 seed particles with a single size mode, we observe a bimodal organic aerosol mass size distribution with two size modes of distinct chemical composition with nitrocatechol from NO3 oxidation preferentially condensing onto the large end of the pre-existing size distribution (∼750 nm). A size-resolved chemistry and microphysics model reproduces the evolution of the two distinct organic aerosol size modes─heterogeneous nucleation to an independent, nitrocatechol-rich aerosol phase.

Estimated Mortality and Morbidity Attributable to Smoke Plumes in the United States: Not Just a Western US Problem.

As anthropogenic emissions continue to decline and emissions from landscape (wild, prescribed, and agricultural) fires increase across the coming century, the relative importance of landscape-fire smoke on air quality and health in the United States (US) will increase. Landscape fires are a large source of fine particulate matter (PM2.5), which has known negative impacts on human health. The seasonal and spatial distribution, particle composition, and co-emitted species in landscape-fire emissions are different from anthropogenic sources of PM2.5. The implications of landscape-fire emissions on the sub-national temporal and spatial distribution of health events and the relative health importance of specific pollutants within smoke are not well understood. We use a health impact assessment with observation-based smoke PM2.5 to determine the sub-national distribution of mortality and the sub-national and sub-annual distribution of asthma morbidity attributable to US smoke PM2.5 from 2006 to 2018. We estimate disability-adjusted life years (DALYs) for PM2.5 and 18 gas-phase hazardous air pollutants (HAPs) in smoke. Although the majority of large landscape fires occur in the western US, we find the majority of mortality (74%) and asthma morbidity (on average 75% across 2006-2018) attributable to smoke PM2.5 occurs outside the West, due to higher population density in the East. Across the US, smoke-attributable asthma morbidity predominantly occurs in spring and summer. The number of DALYs associated with smoke PM2.5 is approximately three orders of magnitude higher than DALYs associated with gas-phase smoke HAPs. Our results indicate awareness and mitigation of landscape-fire smoke exposure is important across the US.

Quantifying the Health Benefits of Face Masks and Respirators to Mitigate Exposure to Severe Air Pollution.

Familiarity with the use of face coverings to reduce the risk of respiratory disease has increased during the coronavirus pandemic; however, recommendations for their use outside of the pandemic remains limited. Here, we develop a modeling framework to quantify the potential health benefits of wearing a face covering or respirator to mitigate exposure to particulate air pollution. This framework accounts for the wide range of available face coverings and respirators, fit factors and efficacy, air pollution characteristics, and exposure-response data. Our modeling shows that N95 respirators offer robust protection against different sources of particulate matter, reducing exposure by more than a factor of 14 when worn with a leak rate of 5%. Synthetic-fiber masks offer less protection with a strong dependence on aerosol size distribution (protection factors ranging from 4.4 to 2.2), while natural-fiber and surgical masks offer reductions in the exposure of 1.9 and 1.7, respectively. To assess the ability of face coverings to provide population-level health benefits to wildfire smoke, we perform a case study for the 2012 Washington state fire season. Our models suggest that although natural-fiber masks offer minor reductions in respiratory hospitalizations attributable to smoke (2%-11%) due to limited filtration efficiency, N95 respirators and to a lesser extent surgical and synthetic-fiber masks may lead to notable reductions in smoke-attributable hospitalizations (22%-39%, 9%-24%, and 7%-18%, respectively). The filtration efficiency, bypass rate, and compliance rate (fraction of time and population wearing the device) are the key factors governing exposure reduction potential and health benefits during severe wildfire smoke events.

Improved estimates of preindustrial biomass burning reduce the magnitude of aerosol climate forcing in the Southern Hemisphere.

Fire plays a pivotal role in shaping terrestrial ecosystems and the chemical composition of the atmosphere and thus influences Earth's climate. The trend and magnitude of fire activity over the past few centuries are controversial, which hinders understanding of preindustrial to present-day aerosol radiative forcing. Here, we present evidence from records of 14 Antarctic ice cores and 1 central Andean ice core, suggesting that historical fire activity in the Southern Hemisphere (SH) exceeded present-day levels. To understand this observation, we use a global fire model to show that overall SH fire emissions could have declined by 30% over the 20th century, possibly because of the rapid expansion of land use for agriculture and animal production in middle to high latitudes. Radiative forcing calculations suggest that the decreasing trend in SH fire emissions over the past century largely compensates for the cooling effect of increasing aerosols from fossil fuel and biofuel sources.

Associations Between Wildfire-Related PM2.5 and Intensive Care Unit Admissions in the United States, 2006-2015.

Wildfire smoke is a growing public health concern in the United States. Numerous studies have documented associations between ambient smoke exposure and severe patient outcomes for single-fire seasons or limited geographic regions. However, there are few national-scale health studies of wildfire smoke in the United States, few studies investigating Intensive Care Unit (ICU) admissions as an outcome, and few specifically framed around hospital operations. This study retrospectively examined the associations between ambient wildfire-related PM2.5 at a hospital ZIP code with total hospital ICU admissions using a national-scale hospitalization data set. Wildfire smoke was characterized using a combination of kriged PM2.5 monitor observations and satellite-derived plume polygons from National Oceanic and Atmospheric Administration's Hazard Mapping System. ICU admissions data were acquired from Premier, Inc. and encompass 15%-20% of all U.S. ICU admissions during the study period. Associations were estimated using a distributed-lag conditional Poisson model under a time-stratified case-crossover design. We found that a 10 µg/m3 increase in daily wildfire PM2.5 was associated with a 2.7% (95% CI: 1.3, 4.1; p = 0.00018) increase in ICU admissions 5 days later. Under stratification, positive associations were found among patients aged 0-20 and 60+, patients living in the Midwest Census Region, patients admitted in the years 2013-2015, and non-Black patients, though other results were mixed. Following a simulated severe 7-day 120 µg/m3 smoke event, our results predict ICU bed utilization peaking at 131% (95% CI: 43, 239; p < 10-5) over baseline. Our work suggests that hospitals may need to preposition vital critical care resources when severe smoke events are forecast.

Quantifying Proximity, Confinement, and Interventions in Disease Outbreaks: A Decision Support Framework for Air-Transported Pathogens.

The inability to communicate how infectious diseases are transmitted in human environments has triggered avoidance of interactions during the COVID-19 pandemic. We define a metric, Effective ReBreathed Volume (ERBV), that encapsulates how infectious pathogens, including SARS-CoV-2, transport in air. ERBV separates environmental transport from other factors in the chain of infection, allowing quantitative comparisons among situations. Particle size affects transport, removal onto surfaces, and elimination by mitigation measures, so ERBV is presented for a range of exhaled particle diameters: 1, 10, and 100 µm. Pathogen transport depends on both proximity and confinement. If interpersonal distancing of 2 m is maintained, then confinement, not proximity, dominates rebreathing after 10-15 min in enclosed spaces for all but 100 µm particles. We analyze strategies to reduce this confinement effect. Ventilation and filtration reduce person-to-person transport of 1 µm particles (ERBV1) by 13-85% in residential and office situations. Deposition to surfaces competes with intentional removal for 10 and 100 µm particles, so the same interventions reduce ERBV10 by only 3-50%, and ERBV100 is unaffected. Prior knowledge of size-dependent ERBV would help identify transmission modes and effective interventions. This framework supports mitigation decisions in emerging situations, even before other infectious parameters are known.

Particle Size Distribution Dynamics Can Help Constrain the Phase State of Secondary Organic Aerosol.

Particle phase state is a property of atmospheric aerosols that has important implications for the formation, evolution, and gas/particle partitioning of secondary organic aerosol (SOA). In this work, we use a size-resolved chemistry and microphysics model (Statistical Oxidation Model coupled to the TwO Moment Aerosol Sectional (SOM-TOMAS)), updated to include an explicit treatment of particle phase state, to constrain the bulk diffusion coefficient (Db) of SOA produced from α-pinene ozonolysis. By leveraging data from laboratory experiments performed in the absence of a seed and under dry conditions, we find that the Db for SOA can be constrained ((1-7) × 10-15 cm2 s-1 in these experiments) by simultaneously reproducing the time-varying SOA mass concentrations and the evolution of the particle size distribution. Another version of our model that used the predicted SOA composition to calculate the glass-transition temperature, viscosity, and, ultimately, Db (∼10-15 cm2 s-1) of the SOA was able to reproduce the mass and size distribution measurements when we included oligomer formation (oligomers accounted for about a fifth of the SOA mass). Our work highlights the potential of a size-resolved SOA model to constrain the particle phase state of SOA using historical measurements of the evolution of the particle size distribution.

Differential Cardiopulmonary Health Impacts of Local and Long-Range Transport of Wildfire Smoke.

We estimated cardiopulmonary morbidity and mortality associated with wildfire smoke (WFS) fine particulate matter (PM2.5) in the Front Range of Colorado from 2010 to 2015. To estimate WFS PM2.5, we developed a daily kriged PM2.5 surface at a 15  × 15 km resolution based on the Environmental Protection Agency Air Quality System monitors for the western United States; we subtracted out local seasonal-average PM2.5 of nonsmoky days, identified using satellite-based smoke plume estimates, from the local daily estimated PM2.5 if smoke was identified by National Oceanic and Atmospheric Administration's Hazard Mapping System. We implemented time-stratified case-crossover analyses to estimate the effect of a 10 µg/m3 increase in WFS PM2.5 with cardiopulmonary hospitalizations and deaths using single and distributed lag models for lags 0-5 and distinct annual impacts based on local and long-range smoke during 2012, and long-range transport of smoke in 2015. A 10 µg/m3 increase in WFS was associated with all respiratory, asthma, and chronic obstructive pulmonary disease hospitalizations for lag day 3 and hospitalizations for ischemic heart disease at lag days 2 and 3. Cardiac arrest deaths were associated with WFS PM2.5 at lag day 0. For 2012 local wildfires, asthma hospitalizations had an inverse association with WFS PM2.5 (OR: 0.716, 95% CI: 0.517-0.993), but a positive association with WFS PM2.5 during the 2015 long-range transport event (OR: 1.455, 95% CI: 1.093-1.939). Cardiovascular mortality was associated with the 2012 long-range transport event (OR: 1.478, 95% CI: 1.124-1.944).

Outdoor air pollution in India is not only an urban problem.

Urban outdoor air pollution in the developing world, mostly due to particulate matter with diameters smaller than 2.5 µm (PM2.5), has been highlighted in recent years. It leads to millions of premature deaths. Outdoor air pollution has also been viewed mostly as an urban problem. We use satellite-derived demarcations to parse India's population into urban and nonurban regions, which agrees with the census data. We also use the satellite-derived surface PM2.5 levels to calculate the health impacts in the urban and nonurban regions. We show that outdoor air pollution is just as severe in nonurban regions as in the urban regions of India, with implications to monitoring, regulations, health, and policy.