Publications by authors named "Lukas Valin"

Single source contribution to ambient O and PM has been estimated with photochemical grid models to support policy demonstrations for National Ambient Air Quality Standards, regional haze, and permit related programs. Limited field data exists to evaluate model representation of the spatial extent and chemical composition of plumes emitted by specific facilities. New tropospheric column measurements of NO and in-plume chemical measurements downwind of specific facilities allows for photochemical model evaluation of downwind plume extent, grid resolution impacts on plume concentration gradients, and source attribution methods.

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Chemical mechanisms describe how emissions of gases and particles evolve in the atmosphere and are used within chemical transport models to evaluate past, current, and future air quality. Thus, a chemical mechanism must provide robust and accurate predictions of air pollutants if it is to be considered for use by regulatory bodies. In this work, we provide an initial evaluation of the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMMv1.

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The COVID-19 pandemic created an extreme natural experiment in which sudden changes in human behavior and economic activity resulted in significant declines in nitrogen oxide (NO ) emissions, immediately after strict lockdowns were imposed. Here we examined the impact of multiple waves and response phases of the pandemic on nitrogen dioxide (NO) dynamics and the role of meteorology in shaping relative contributions from different emission sectors to NO pollution in post-pandemic New York City. Long term (> 3.

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Understanding the local-scale spatial and temporal variability of ozone formation is crucial for effective mitigation. We combine tropospheric vertical column densities (VCD) of formaldehyde (HCHO) and nitrogen dioxide (NO), referred to as HCHO-VCD and NO-VCD, retrieved from airborne remote sensing and the TROPOspheric Monitoring Instrument (TROPOMI) with ground-based measurements to investigate changes in ozone precursors and the inferred chemical production regime on high-ozone days in May-August 2018 over two Northeast urban domains. Over New York City (NYC) and Baltimore/Washington D.

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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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Daytime onshore lake breezes are a critical factor controlling ozone abundance at coastal sites around Lake Michigan. Coastal counties along the western shore of Lake Michigan have historically observed high ozone episodes dating to the 1970s. We classified ozone episode days based on the extent or absence of the lake breeze (i.

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Satellite nitrogen dioxide (NO) measurements are used extensively to infer nitrogen oxide emissions and their trends, but interpretation can be complicated by background contributions to the NO column sensed from space. We use the step decrease of US anthropogenic emissions from the COVID-19 shutdown to compare the responses of NO concentrations observed at surface network sites and from satellites (Ozone Monitoring Instrument [OMI], Tropospheric Ozone Monitoring Instrument [TROPOMI]). After correcting for differences in meteorology, surface NO measurements for 2020 show decreases of 20% in March-April and 10% in May-August compared to 2019.

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Airborne and ground-based Pandora spectrometer NO column measurements were collected during the 2018 Long Island Sound Tropospheric Ozone Study (LISTOS) in the New York City/Long Island Sound region, which coincided with early observations from the Sentinel-5P TROPOspheric Monitoring Instrument (TROPOMI) instrument. Both airborne- and ground-based measurements are used to evaluate the TROPOMI NO Tropospheric Vertical Column (TrVC) product v1.2 in this region, which has high spatial and temporal heterogeneity in NO.

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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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NASA deployed the GeoTASO airborne UV-Visible spectrometer in May-June 2017 to produce high resolution (approximately 250 × 250 m) gapless NO datasets over the western shore of Lake Michigan and over the Los Angeles Basin. The results collected show that the airborne tropospheric vertical column retrievals compare well with ground-based Pandora spectrometer column NO observations (r=0.91 and slope of 1.

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Urban ozone (O) formation can be limited by NO, VOCs, or both, complicating the design of effective O abatement plans. A satellite-retrieved ratio of formaldehyde to NO (HCHO/NO), developed from theory and modeling, has previously been used to indicate O formation chemistry. Here, we connect this space-based indicator to spatiotemporal variations in O recorded by on-the-ground monitors over major U.

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Determining effective strategies for mitigating surface ozone (O) pollution requires knowledge of the relative ambient concentrations of its precursors, NO , and VOCs. The space-based tropospheric column ratio of formaldehyde to NO (FNR) has been used as an indicator to identify NO -limited versus NO -saturated O formation regimes. Quantitative use of this indicator ratio is subject to three major uncertainties: (1) the split between NO -limited and NO -saturated conditions may shift in space and time, (2) the ratio of the vertically integrated column may not represent the near-surface environment, and (3) satellite products contain errors.

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The Korea-United States Air Quality Study (KORUS-AQ) conducted during May-June 2016 offered the first opportunity to evaluate direct-sun observations of formaldehyde (HCHO) total column densities with improved Pandora spectrometer instruments. The measurements highlighted in this work were conducted both in the Seoul megacity area at the Olympic Park site (37.5232° N, 27.

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With the near-future launch of geostationary pollution monitoring satellite instruments over North America, East Asia, and Europe, the air quality community is preparing for an integrated global atmospheric composition observing system at unprecedented spatial and temporal resolutions. One of the ways that NASA has supported this community preparation is through demonstration of future space-borne capabilities using the Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) airborne instrument. This paper integrates repeated high-resolution maps from GeoTASO, ground-based Pandora spectrometers, and low Earth orbit measurements from the Ozone Mapping and Profiler Suite (OMPS), for case studies over two metropolitan areas: Seoul, South Korea on June 9, 2016 and Los Angeles, California on June 27, 2017.

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We describe ground and space-based measurements of spatial and temporal variation of NO(2) in four California metropolitan regions. The measurements of weekly cycles and trends over the years 2005-2008 observed both from the surface and from space are nearly identical to each other. Observed decreases in Los Angeles and the surrounding cities are 46% on weekends and 9%/year from 2005-2008.

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Methyl vinyl carbonyl oxide is an important intermediate in the reaction of isoprene and ozone and may be responsible for most of the (*)OH formed in isoprene ozonolysis. We use CBS-QB3 calculations and RRKM/master equation simulations to characterize all the pathways leading to the formation of this species, all the interconversions among its four possible conformers, and all of its irreversible isomerizations. Our calculations, like previous studies, predict (*)OH yields consistent with experiment if thermalized syn-methyl carbonyl oxides form (*)OH quantitatively.

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The vinoxy radical, a common intermediate in gas-phase alkene ozonolysis, reacts with O2 to form a chemically activated alpha-oxoperoxy species. We report CBS-QB3 energetics for O2 addition to the parent (*CH2CHO, 1a), 1-methylvinoxy (*CH2COCH3, 1b), and 2-methylvinoxy (CH3*CHCHO, 1c) radicals. CBS-QB3 predictions for peroxy radical formation agree with experimental data, while the G2 method systematically overestimates peroxy radical stability.

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