Publications by authors named "Millet D"

Ethane is the most abundant non-methane hydrocarbon in the troposphere, where it impacts ozone and reactive nitrogen and is a key tracer used for partitioning emitted methane between anthropogenic and natural sources. However, quantification has been challenged by sparse observations. Here, we present a satellite-based measurement of tropospheric ethane and demonstrate its utility for fossil-fuel source quantification.

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Indirect nitrous oxide (NO) emissions from streams and rivers are a poorly constrained term in the global NO budget. Current models of riverine NO emissions place a strong focus on denitrification in groundwater and riverine environments as a dominant source of riverine NO, but do not explicitly consider direct NO input from terrestrial ecosystems. Here, we combine NO isotope measurements and spatial stream network modeling to show that terrestrial-aquatic interactions, driven by changing hydrologic connectivity, control the sources and dynamics of riverine NO in a mesoscale river network within the U.

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The hydroxyl radical (OH) is the central oxidant in Earth's troposphere, but its temporal variability is poorly understood. We combine 2012-2020 satellite-based isoprene and formaldehyde measurements to identify coherent OH changes over temperate and tropical forests with attribution to emission trends, biotic stressors, and climate. We identify a multiyear OH decrease over the Southeast United States and show that with increasingly hot/dry summers the regional chemistry could become even less oxidizing depending on competing temperature/drought impacts on isoprene.

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Schools may have important impacts on children's exposure to ambient air pollution, yet ambient air quality at schools is not consistently tracked. We characterize ambient air quality at home and school locations in the United States using satellite-based empirical model (i.e.

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The Lake Michigan Ozone Study 2017 (LMOS 2017) was a collaborative multiagency field study targeting ozone chemistry, meteorology, and air quality observations in the southern Lake Michigan area. The primary objective of LMOS 2017 was to provide measurements to improve air quality modeling of the complex meteorological and chemical environment in the region. LMOS 2017 science questions included spatiotemporal assessment of nitrogen oxides (NO = NO + NO) and volatile organic compounds (VOC) emission sources and their influence on ozone episodes; the role of lake breezes; contribution of new remote sensing tools such as GeoTASO, Pandora, and TEMPO to air quality management; and evaluation of photochemical grid models.

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Each year, millions of premature deaths worldwide are caused by exposure to outdoor air pollution, especially fine particulate matter (PM2.5). Designing policies to reduce these deaths relies on air quality modeling for estimating changes in PM2.

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The Arctic is a climatically sensitive region that has experienced warming at almost 3 times the global average rate in recent decades, leading to an increase in Arctic greenness and a greater abundance of plants that emit biogenic volatile organic compounds (BVOCs). These changes in atmospheric emissions are expected to significantly modify the overall oxidative chemistry of the region and lead to changes in VOC composition and abundance, with implications for atmospheric processes. Nonetheless, observations needed to constrain our current understanding of these issues in this critical environment are sparse.

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Purpose: To probabilistically forecast needed anti-vascular endothelial growth factor (anti-VEGF) treatment frequency using volumetric spectral domain-optical coherence tomography (SD-OCT) biomarkers in neovascular age-related macular degeneration from real-world settings.

Methods: SD-OCT volume scans were segmented with a custom deep-learning-based analysis pipeline. Retinal thickness and reflectivity values were extracted for the central and the four inner Early Treatment Diabetic Retinopathy Study (ETDRS) subfields for six retinal layers (inner retina, outer nuclear layer, inner segments [IS], outer segments [OS], retinal pigment epithelium-drusen complex [RPEDC] and the choroid).

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Formic acid (HCOOH) is an important component of atmospheric acidity but its budget is poorly understood, with prior observations implying substantial missing sources. Here we combine pole-to-pole airborne observations from the Atmospheric Tomography Mission (ATom) with chemical transport model (GEOS-Chem CTM) and back trajectory analyses to provide the first global in-situ characterization of HCOOH in the remote atmosphere. ATom reveals sub-100 ppt HCOOH concentrations over most of the remote oceans, punctuated by large enhancements associated with continental outflow.

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The widespread and rapid social and economic changes from Covid-19 response might be expected to dramatically improve air quality. However, national monitoring data from the US Environmental Protection Agency for criteria pollutants (PM, ozone, NO, CO, PM) provide inconsistent support for that expectation. Specifically, during stay-at-home orders, average PM levels were slightly higher (~10% of its multi-year interquartile range [IQR]) than expected; average ozone, NO, CO, and PM levels were slightly lower (~30%, ~20%, ~27%, and ~1% of their IQR, respectively) than expected.

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Eddy covariance (EC) measurements of ecosystem-atmosphere carbon dioxide (CO) exchange provide the most direct assessment of the terrestrial carbon cycle. Measurement biases for open-path (OP) CO concentration and flux measurements have been reported for over 30 years, but their origin and appropriate correction approach remain unresolved. Here, we quantify the impacts of OP biases on carbon and radiative forcing budgets for a sub-boreal wetland.

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Article Synopsis
  • The Lake Michigan Ozone Study 2017 (LMOS 2017) focused on understanding ozone pollution in the Lake Michigan region through various sampling methods, including ground-based, airborne, and maritime approaches.
  • Two key sampling sites in Zion, Illinois, and Sheboygan, Wisconsin, were chosen for their unique positions to study both less processed and aged air parcels during high-ozone events.
  • The results indicated significant ozone concentrations during several multi-day periods, with local vehicle traffic and large point sources contributing minimally (under 15%) to the pollution levels, leading to discussions on future research methods and model comparisons.
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Article Synopsis
  • The global oxidation capacity, measured by hydroxyl radicals (OH), affects the lifespan of gases like methane and carbon monoxide, with models generally underestimating their lifetimes due to excessive OH levels.
  • Observations from NASA's ATom campaign provide insights into remote ocean oxidation capacity, showing that the GEOS-Chem model accurately reflects remote OH profiles but struggles with seasonal NO estimates.
  • The study reveals an unexplained enhancement of OH reactivity below 3 km during ATom-1, indicating potential missing reactive VOCs that existing models fail to account for.
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Isoprene is emitted from the biosphere into the atmosphere, and may strengthen the defense mechanisms of plants against oxidative and thermal stress. Once in the atmosphere, isoprene is rapidly oxidized, either to isoprene-hydroxy-hydroperoxides (ISOPOOH) at low levels of nitrogen oxides, or to methyl vinyl ketone (MVK) and methacrolein at high levels. Here we combine uptake rates and deposition velocities that we obtained in laboratory experiments with observations in natural forests to show that 1,2-ISOPOOH deposits rapidly into poplar leaves.

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Article Synopsis
  • The study uses airborne measurements across different seasons to analyze methane emissions in the US Corn Belt and Upper Midwest, focusing on natural and anthropogenic sources.
  • It finds that wetlands are the largest methane source, while livestock contribute significantly as the major human-related source, with implications for emission management.
  • The research highlights discrepancies in methane estimates from different agricultural practices and suggests improvements in management strategies for livestock to effectively mitigate emissions.
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Peatlands are among the largest natural sources of atmospheric methane (CH) worldwide. Peatland emissions are projected to increase under climate change, as rising temperatures and shifting precipitation accelerate microbial metabolic pathways favorable for CH production. However, how these changing environmental factors will impact peatland emissions over the long term remains unknown.

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Nitrous oxide (NO), like carbon dioxide, is a long-lived greenhouse gas that accumulates in the atmosphere. Over the past 150 years, increasing atmospheric NO concentrations have contributed to stratospheric ozone depletion and climate change, with the current rate of increase estimated at 2 per cent per decade. Existing national inventories do not provide a full picture of NO emissions, owing to their omission of natural sources and limitations in methodology for attributing anthropogenic sources.

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Isoprene is the dominant non-methane organic compound emitted to the atmosphere. It drives ozone and aerosol production, modulates atmospheric oxidation and interacts with the global nitrogen cycle. Isoprene emissions are highly uncertain, as is the nonlinear chemistry coupling isoprene and the hydroxyl radical, OH-its primary sink.

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Natural emissions of air pollutants from the surface play major roles in air quality and climate change. In particular, nitrogen oxides (NO) emitted from soils contribute ~15% of global NO emissions, sea salt aerosols are a major player in the climate and chemistry of the marine atmosphere, and biogenic emissions are the dominant source of non-methane volatile organic compounds at the global scale. These natural emissions are often estimated using nonlinear parameterizations, which are sensitive to the horizontal resolutions of inputted meteorological and ancillary data.

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Rapid Arctic warming, a lengthening growing season, and the increasing abundance of biogenic volatile-organic-compound-emitting shrubs are all anticipated to increase atmospheric biogenic volatile organic compounds (BVOCs) in the Arctic atmosphere, with implications for atmospheric oxidation processes and climate feedbacks. Quantifying these changes requires an accurate understanding of the underlying processes driving BVOC emissions in the Arctic. While boreal ecosystems have been widely studied, little attention has been paid to Arctic tundra environments.

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Wetlands represent the dominant natural source of methane (CH) to the atmosphere. Thus, substantial effort has been spent examining the CH budgets of global wetlands continuous ecosystem-scale measurements using the eddy covariance (EC) technique. Robust error characterization for such measurements, however, remains a major challenge.

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India is an air pollution mortality hot spot, but regional emissions are poorly understood. We present a high-resolution nested chemical transport model (GEOS-Chem) simulation for the Indian subcontinent and use it to interpret formaldehyde (HCHO) observations from two satellite sensors (OMI and GOME-2A) in terms of constraints on regional volatile organic compound (VOC) emissions. We find modeled biogenic VOC emissions to be overestimated by ~30-60% for most locations and seasons, and derive a best estimate biogenic flux of 16 Tg C/year subcontinent-wide for year 2009.

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Isoprene is the atmosphere's most important non-methane organic compound, with key impacts on atmospheric oxidation, ozone, and organic aerosols. In-situ isoprene measurements are sparse, and satellite-based constraints have employed an indirect approach using its oxidation product formaldehyde, which is affected by non-isoprene sources plus uncertainty and spatial smearing in the isoprene-formaldehyde relationship. Direct global isoprene measurements are therefore needed to better understand its sources, sinks, and atmospheric impacts.

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We apply a high-resolution chemical transport model (GEOS-Chem CTM) with updated treatment of volatile organic compounds (VOCs) and a comprehensive suite of airborne datasets over North America to (i) characterize the VOC budget and (ii) test the ability of current models to capture the distribution and reactivity of atmospheric VOCs over this region. Biogenic emissions dominate the North American VOC budget in the model, accounting for 70 % and 95 % of annually emitted VOC carbon and reactivity, respectively. Based on current inventories anthropogenic emissions have declined to the point where biogenic emissions are the dominant summertime source of VOC reactivity even in most major North American cities.

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