Project description:By producing a first-of-its-kind, decadal-scale wildfire plume rise climatology in the Western U.S. and Canada, we identify trends toward enhanced plume top heights, aerosol loading aloft, and near-surface smoke injection throughout the American West. Positive and significant plume trends suggest a growing impact of Western US wildfires on air quality at the local to continental scales and support the notion that wildfires may have an increasing impact on regional climate. Overlap of identified trends with regions of increasing wildfire emissions and burn severity suggests a link to climate driven trends toward enhanced wildfire activity. Further, time series of plume activity point to a possible acceleration of trends over recent years, such that the future impacts to air quality and regional climate may exceed those suggested by a linear fit to the multi-decadal data. These findings have significant implications for human health and exacerbate concern for the climate-wildfire connection.
Project description:Wildfire area has been increasing in most ecoregions across the western United States, including snow-dominated regions. These fires modify snow accumulation, ablation, and duration, but the sign and magnitude of these impacts can vary substantially between regions. This study compares spatiotemporal patterns of western United States wildfires between ecoregions and snow zones. Results demonstrate significant increases in wildfire area from 1984 to 2020 throughout the West, including the Sierra Nevada, Cascades, Basin and Range, and Northern to Southern Rockies. In the late snow zone, where mean annual snow-free date is in May or later, 70% of ecoregions experienced significant increases in wildfire area since 1984. The distribution of burned area shifted from earlier melt zones to later-melt snow zones in several ecoregions, including the Southern Rockies, where the area burned in the late snow zone during 2020 exceeded the total burned area over the previous 36 y combined. Snow measurements at a large Southern Rockies fire revealed that burning caused lower magnitude and earlier peak snow-water equivalent as well as an 18-24 d estimated advance in snow-free dates. Latitude, a proxy for solar radiation, is a dominant driver of snow-free date, and fire advances snow-free timing through a more-positive net shortwave radiation balance. This loss of snow can reduce both ecosystem water availability and streamflow generation in a region that relies heavily on mountain snowpack for water supply.
Project description:Recent field observations have shown that the atmospheric plumes of quiescently degassing volcanoes are chemically very active, pointing to the role of chemical cycles involving halogen species and heterogeneous reactions on aerosol particles that have previously been unexplored for this type of volcanic plumes. Key features of these measurements can be reproduced by numerical models such as the one employed in this study. The model shows sustained high levels of reactive bromine in the plume, leading to extensive ozone destruction, that, depending on plume dispersal, can be maintained for several days. The very high concentrations of sulfur dioxide in the volcanic plume reduces the lifetime of the OH radical drastically, so that it is virtually absent in the volcanic plume. This would imply an increased lifetime of methane in volcanic plumes, unless reactive chlorine chemistry in the plume is strong enough to offset the lack of OH chemistry. A further effect of bromine chemistry in addition to ozone destruction shown by the model studies presented here, is the oxidation of mercury. This relates to mercury that has been coemitted with bromine from the volcano but also to background atmospheric mercury. The rapid oxidation of mercury implies a drastically reduced atmospheric lifetime of mercury so that the contribution of volcanic mercury to the atmospheric background might be less than previously thought. However, the implications, especially health and environmental effects due to deposition, might be substantial and warrant further studies, especially field measurements to test this hypothesis.
Project description:Since their introduction two decades ago, Community Wildfire Protection Plans (CWPPs) have become a common planning tool for improving community preparedness and risk mitigation in fire-prone regions, and for strengthening coordination among federal and state land management agencies, local government, and residents. While CWPPs have been the focus of case studies, there are limited large-scale studies to understand the extent of, and factors responsible for, variation in stakeholder participation-a core element of the CWPP model. This article describes the scale and scope of participation in CWPPs across the western United States. We provide a detailed account of participants in over 1,000 CWPPs in 11 states and examine how levels of participation and stakeholder diversity vary as a function of factors related to planning process, planning context, and the broader geographic context in which plans were developed. We find that CWPPs vary substantially both by count and diversity of participants and that the former varies as a function of the geographic scale of the plan, while the latter varies largely as a function of the diversity of landowners within the jurisdiction. More than half of participants represented local interests, indicating a high degree of local engagement in hazard mitigation. Surprisingly, plan participation and diversity were unrelated to wildfire hazard. These findings suggest that CWPPs have been largely successful in their intent to engage diverse stakeholders in preparing for and mitigating wildfire risk, but that important challenges remain. We discuss the implications of this work and examine how the planning process and context for CWPPs may be changing.
Project description:Increases in vapor pressure deficit (VPD) have been hypothesized as the primary driver of future fire changes. The Coupled Model Intercomparison Project Phase 5 (CMIP5) models agree that western U.S. surface temperatures and associated dryness of air as defined by the VPD will increase in the 21st century for Representative Concentration Pathways (RCPs) 4.5 and 8.5. However, we find that averaged over seasonal and regional scales, other environmental variables demonstrated to be relevant to flammability, moisture abundances, and aridity-such as precipitation, evaporation, relative humidity, root zone soil moisture, and wind speed-can be used to explain observed variance in wildfire burn area as well or better than VPD. However, the magnitude and sign of the change of these variables in the 21st century are less certain than the predicted changes in VPD. Our work demonstrates that when objectively selecting environmental variables to maximize predictive skill of linear regressions (minimize square error on unseen data) VPD is not always selected and when it is not, the magnitude of future increases in burn area becomes less certain. Hence, this work shows that future burn area predictions are sensitive to what environmental predictors are chosen to drive burn area.
Project description:The evolution of organic aerosol (OA) and brown carbon (BrC) in wildfire plumes, including the relative contributions of primary versus secondary sources, has been uncertain in part because of limited knowledge of the precursor emissions and the chemical environment of smoke plumes. We made airborne measurements of a suite of reactive trace gases, particle composition, and optical properties in fresh western US wildfire smoke in July through August 2018. We use these observations to quantify primary versus secondary sources of biomass-burning OA (BBPOA versus BBSOA) and BrC in wildfire plumes. When a daytime wildfire plume dilutes by a factor of 5 to 10, we estimate that up to one-third of the primary OA has evaporated and subsequently reacted to form BBSOA with near unit yield. The reactions of measured BBSOA precursors contribute only 13 ± 3% of the total BBSOA source, with evaporated BBPOA comprising the rest. We find that oxidation of phenolic compounds contributes the majority of BBSOA from emitted vapors. The corresponding particulate nitrophenolic compounds are estimated to explain 29 ± 15% of average BrC light absorption at 405 nm (BrC Abs405) measured in the first few hours of plume evolution, despite accounting for just 4 ± 2% of average OA mass. These measurements provide quantitative constraints on the role of dilution-driven evaporation of OA and subsequent radical-driven oxidation on the fate of biomass-burning OA and BrC in daytime wildfire plumes and point to the need to understand how processing of nighttime emissions differs.
Project description:Wildfire emissions are a key contributor of carbonaceous aerosols and trace gases to the atmosphere. Induced by buoyant lifting, smoke plumes can be injected into the free troposphere and lower stratosphere, which by consequence significantly affects the magnitude and distance of their influences on air quality and radiation budget. However, the vertical allocation of emissions when smoke escapes the planetary boundary layer (PBL) and the mechanism modulating it remain unclear. We present an inverse modeling framework to estimate the wildfire emissions, with their temporal and vertical evolution being constrained by assimilating aerosol extinction profiles observed from the airborne Differential Absorption Lidar-High Spectral Resolution Lidar during the Fire Influence on Regional to Global Environments and Air Quality field campaign. Three fire events in the western U.S., which exhibit free-tropospheric injections are examined. The constrained smoke emissions indicate considerably larger fractions of smoke injected above the PBL (f >PBL, 80%-94%) versus the column total, compared to those estimated by the WRF-Chem model using the default plume rise option (12%-52%). The updated emission profiles yield improvements for the simulated vertical structures of the downwind transported smoke, but limited refinement of regional smoke aerosol optical depth distributions due to the spatiotemporal coverage of flight observations. These results highlight the significance of improving vertical allocation of fire emissions on advancing the modeling and forecasting of the environmental impacts of smoke.
Project description:SignificanceLarge wildfires have been observed to inject smoke into the stratosphere, raising questions about their potential to affect the stratospheric ozone layer that protects life on Earth from biologically damaging ultraviolet radiation. Multiple observations of aerosol and NO2 concentrations from three independent satellite instruments are used here together with model calculations to identify decreases in stratospheric NO2 concentrations following major Australian 2019 through 2020 wildfires. The data confirm that important chemistry did occur on the smoke particle surfaces. The observed behavior in NO2 with increasing particle concentrations is a marker for surface chemistry that contributes to midlatitude ozone depletion. The results indicate that increasing wildfire activity in a warming world may slow the recovery of the ozone layer.
Project description:Outdoor ozone transported indoors initiates oxidative chemistry, forming volatile organic products. The influence of ozone chemistry on indoor air composition has not been directly quantified in normally occupied residences. Here, we explore indoor ozone chemistry in a house in California with two adult inhabitants. We utilize space- and time-resolved measurements of ozone and volatile organic compounds (VOCs) acquired over an 8-wk summer campaign. Despite overall low indoor ozone concentrations (mean value of 4.3 ppb) and a relatively low indoor ozone decay constant (1.3 h-1), we identified multiple VOCs exhibiting clear contributions from ozone-initiated chemistry indoors. These chemicals include 6-methyl-5-hepten-2-one (6-MHO), 4-oxopentanal (4-OPA), nonenal, and C8-C12 saturated aldehydes, which are among the commonly reported products from laboratory studies of ozone interactions with indoor surfaces and with human skin lipids. These VOCs together accounted for ≥12% molecular yield with respect to house-wide consumed ozone, with the highest net product yield for nonanal (≥3.5%), followed by 6-MHO (2.7%) and 4-OPA (2.6%). Although 6-MHO and 4-OPA are prominent ozonolysis products of skin lipids (specifically squalene), ozone reaction with the body envelopes of the two occupants in this house are insufficient to explain the observed yields. Relatedly, we observed that ozone-driven chemistry continued to produce 6-MHO and 4-OPA even after the occupants had been away from the house for 5 d. These observations provide evidence that skin lipids transferred to indoor surfaces made substantial contributions to ozone reactivity in the studied house.
Project description:This study aimed to better understand and quantify the influence of ventilation strategies on occupant-related indoor air chemistry. The oxidation of human skin oil constituents was studied in a continuously ventilated climate chamber at two air exchange rates (1 h-1 and 3 h-1 ) and two initial ozone mixing ratios (30 and 60 ppb). Additional measurements were performed to investigate the effect of intermittent ventilation ("off" followed by "on"). Soiled t-shirts were used to simulate the presence of occupants. A time-of-flight-chemical ionization mass spectrometer (ToF-CIMS) in positive mode using protonated water clusters was used to measure the oxygenated reaction products geranyl acetone, 6-methyl-5-hepten-2-one (6-MHO) and 4-oxopentanal (4-OPA). The measurement data were used in a series of mass balance models accounting for formation and removal processes. Reactions of ozone with squalene occurring on the surface of the t-shirts are mass transport limited; ventilation rate has only a small effect on this surface chemistry. Ozone-squalene reactions on the t-shirts produced gas-phase geranyl acetone, which was subsequently removed almost equally by ventilation and further reaction with ozone. About 70% of gas-phase 6-MHO was produced in surface reactions on the t-shirts, the remainder in secondary gas-phase reactions of ozone with geranyl acetone. 6-MHO was primarily removed by ventilation, while further reaction with ozone was responsible for about a third of its removal. 4-OPA was formed primarily on the surfaces of the shirts (~60%); gas-phase reactions of ozone with geranyl acetone and 6-MHO accounted for ~30% and ~10%, respectively. 4-OPA was removed entirely by ventilation. The results from the intermittent ventilation scenarios showed delayed formation of the reaction products and lower product concentrations compared to continuous ventilation.