A5088812284- Atmospheric chemistry and aerosols
- Air Quality Monitoring and Forecasting
- Air Quality and Health Impacts
- Atmospheric aerosols and clouds
- Atmospheric and Environmental Gas Dynamics
- Atmospheric Ozone and Climate
- Industrial Gas Emission Control
- Odor and Emission Control Technologies
- Oil, Gas, and Environmental Issues
- Spectroscopy and Laser Applications
- Water Quality Monitoring and Analysis
- Ocean Acidification Effects and Responses
- Catalysis and Oxidation Reactions
- Per- and polyfluoroalkyl substances research
- Oil Spill Detection and Mitigation
- Inorganic and Organometallic Chemistry
- Building Energy and Comfort Optimization
NOAA Chemical Sciences Laboratory
2024
Cooperative Institute for Research in Environmental Sciences
2024
University of Colorado Boulder
2024
University of Wisconsin–Madison
2020-2024
Dimethyl sulfide (DMS), emitted from the oceans, is most abundant biological source of sulfur to marine atmosphere. Atmospheric DMS oxidized condensable products that form secondary aerosols affect Earth's radiative balance by scattering solar radiation and serving as cloud condensation nuclei. We report atmospheric discovery a previously unquantified oxidation product, hydroperoxymethyl thioformate (HPMTF, HOOCH2SCHO), identified through global-scale airborne observations demonstrate it be...
Oceans emit large quantities of dimethyl sulfide (DMS) to the marine atmosphere. The oxidation DMS leads formation and growth cloud condensation nuclei (CCN) with consequent effects on Earth's radiation balance climate. quantitative assessment impact emissions CCN concentrations necessitates a detailed description in presence existing aerosol particles clouds. In unpolluted atmosphere, is efficiently oxidized hydroperoxymethyl thioformate (HPMTF), stable intermediate chemical trajectory...
Abstract The oxidation of carbonyl sulfide (OCS) is the primary, continuous source stratospheric sulfate aerosol particles, which can scatter shortwave radiation and catalyze heterogeneous reactions in stratosphere. While it has been estimated that dimethyl (DMS), emitted from surface ocean accounts for 8%–20% global OCS source, there no existing DMS mechanism relevant to marine atmosphere consistent with an this magnitude. We describe new laboratory measurements theoretical analyses provide...
Dimethyl sulfide (DMS; CH3SCH3), a biogenically produced trace gas emitted from the ocean, accounts for large fraction of natural sulfur released to marine atmosphere. The oxidation DMS in boundary layer (MBL), via hydrogen abstraction pathway, yields short-lived methylthiomethylperoxy radical (MSP; CH3SCH2OO). In remote MBL, unimolecular isomerization MSP outpaces bimolecular chemistry leading efficient formation hydroperoxymethyl thioformate (HPMTF; HOOCH2SCHO). Here, we report first...
Abstract. Oceanic emissions of dimethyl sulfide (CH3SCH3, DMS) have long been recognized to impact aerosol particle composition and size, the concentration cloud condensation nuclei (CCN), Earth's radiation balance. The oceanic methanethiol (CH3SH, MeSH), which is produced by same precursor as DMS, on volatile sulfur budget marine atmosphere largely unconstrained. Here we present direct flux measurements MeSH using eddy covariance (EC) method with a high-resolution proton-transfer-reaction...
Extension of laboratory results suggests that monoterpenes, a subset marine biogenic volatile organic compounds, might play competitive role in secondary aerosol formation the remote atmosphere, where oxidation dimethyl sulfide has traditionally been thought to dominate. However, current assessment monoterpenes atmosphere is limited by scarcity speciated monoterpene measurements and complete absence collocated particle chemical composition speciation. Here we present gas-phase with...
<p>The oxidation of carbonyl sulfide (OCS) is the primary, continuous source stratospheric sulfate aerosol particles, which can scatter shortwave radiation and catalyze heterogeneous reactions in stratosphere. While it has been estimated that dimethyl (DMS), emitted from surface ocean, accounts for 8-20% global OCS source, there no existing DMS mechanism relevant to marine atmosphere consistent with an this magnitude. We describe new laboratory measurements theoretical analyses...
The oxidation products of dimethyl sulfide (DMS) contribute to the production and growth cloud condensation nuclei (CCN) in marine boundary layer. Laboratory field measurements have demonstrated that DMS is oxidized by hydroxyl radicals (OH) forming stable intermediate hydroperoxymethyl thioformate (HPMTF) high yield. HPMTF both globally ubiquitous efficiently lost multiphase processes atmosphere. At present, there are no experimental aqueous reactions HPMTF. Prior modeling studies assumed...
Abstract. Dimethyl sulfide (DMS) is the major sulfur species emitted from ocean. The gas-phase oxidation of DMS by hydroxyl radicals proceeds through stable, soluble intermediate hydroperoxymethyl thioformate (HPMTF), eventually forming carbonyl (OCS) and dioxide (SO2). Recent work has shown that HPMTF efficiently lost to marine boundary layer (MBL) clouds, thus arresting OCS SO2 production their contributions new-particle formation growth events. To date, no long-term field studies exist...
Abstract. Hydroxyl radical (OH) reactivity, which is the inverse lifetime of OH radical, provides information on burden air pollutants, since almost all pollutants react with OH. reactivity measurements from field experiments can help to identify gaps in measurement individual reactants and serve as a proxy for potential formation secondary including ozone particles. However, not regularly measured specifically airborne platforms due technical complexity instruments and/or need careful...
The oxidation products of dimethyl sulfide (DMS) contribute to the production and growth cloud condensation nuclei (CCN) in marine boundary layer. Recent work demonstrates that DMS is oxidized by OH radicals stable intermediate hydroperoxymethyl thioformate (HPMTF), which both globally ubiquitous efficiently lost multiphase processes atmosphere. At present, there are no experimental measurements reactive uptake HPMTF aerosol particles, limiting model implementation chemistry. Using an...
Multifunctional organic nitrates derived from biogenic volatile compounds are important for understanding ozone and secondary aerosol production oxidation reactions in the presence of nitrogen oxides. Their measurement is challenging, part because quantification these difficult time consuming due to techniques required synthesize purify authentic standards. We describe a novel online synthesis separation technique demonstrate its use calibration chemical ionization mass spectrometer using...
Abstract. Dimethyl sulfide (DMS) is the major sulfur species emitted from ocean. The gas-phase oxidation of DMS by hydroxyl radicals proceeds through stable, soluble intermediate hydroperoxymethyl thioformate (HPMTF), eventually forming carbonyl (OCS) and dioxide (SO2). Recent work has shown that HPMTF efficiently lost to marine boundary layer (MBL) clouds, thus arresting OCS SO2 production their contributions new particle formation growth events. To date, no long-term field studies exist...
Abstract. Oceanic emissions of dimethyl sulfide (CH3SCH3, DMS) have long been recognized to impact aerosol particle composition and size, the concentration cloud condensation nuclei (CCN), Earth’s radiation balance. The oceanic methanethiol (CH3SH, MeSH), which is produced by same precursor as DMS, on volatile sulfur budget marine atmosphere largely unconstrained. Here we present direct flux measurements MeSH using eddy covariance (EC) method with a high-resolution proton-transfer-reaction...
We present an examination of the 248 nm VUV (vacuum ultraviolet) laser photolysis ozone (O3) and methylamine (CH3NH2) mixture as means to produce aminomethanol (NH2CH2OH). Aminomethanol is predicted be direct interstellar precursor glycine therefore important target for detection in medium. However, due its high reactivity under terrestrial conditions, evades gas-phase spectral detection. The insertion O(1D) into one proposed pathway form aminomethanol. this formation highly exothermic...
Sea spray aerosol (SSA) formed after wave breaking at the ocean surface influences our climate by scattering incoming solar radiation and acting as cloud condensation nuclei. Furthermore, they provide a microenvironment for aqueous phase chemistry, selective uptake of surfactants, gas-to-particle partitioning compounds providing an acidic pH air-water interface (Angle et al., 2022). Despite these known effects, crucial question remains unanswered: which volatile organic (VOCs) are emitted...
Abstract. Hydroxyl radical OH reactivity, which is the inverse lifetime of radical, provides information on burden air pollutants, since almost all pollutants react with OH. reactivity measurements from field experiments can help to identify gaps in measurement individual reactants and serve as a proxy for potential formation secondary including ozone particles. However, not regularly measured specifically airborne platforms due technical complexity instruments and/or need careful...
Sea spray aerosols (SSA) represent one of the largest sources atmospheric particles since over two-thirds Earth’s surface is covered by oceans. They play an important role in climate and chemistry, however, despite this a series knowledge gaps hinder us from constraining their relevance. One critical question why physicochemical properties nascent generated in the laboratory are so different those measured ambient marine atmosphere. For...