Search for: All records

Abstract. Dimethyl sulfide (DMS) is primarily emitted by marine phytoplankton and oxidized in the atmosphere to form methanesulfonic acid (MSA) and sulfate aerosols. Ice cores in regions affected by anthropogenic pollution show an industrial-era decline in MSA, which has previously been interpreted as indicating a decline in phytoplankton abundance. However, a simultaneous increase in DMS-derived sulfate (bioSO4) in a Greenland ice core suggests that pollution-driven oxidant changes caused the decline in MSA by influencing the relative production of MSA versus bioSO4. Here we use GEOS-Chem, a global chemical transport model, and a zero-dimensional box model over three time periods (preindustrial era, peak North Atlantic NOx pollution, and 21st century) to investigate the chemical drivers of industrial-era changes in MSA and bioSO4, and we examine whether four DMS oxidation mechanisms reproduce trends and seasonality in observations. We find that box model and GEOS-Chem simulations can only partially reproduce ice core trends in MSA and bioSO4 and that wide variation in model results reflects sensitivity to DMS oxidation mechanism and oxidant concentrations. Our simulations support the hypothesized increase in DMS oxidation by the nitrate radical over the industrial era, which increases bioSO4 production, but competing factors such as oxidation by BrO result in increased MSA production in some simulations, which is inconsistent with observations. To improve understanding of DMS oxidation, future work should investigate aqueous-phase chemistry, which produces 82 %–99 % of MSA and bioSO4 in our simulations, and constrain atmospheric oxidant concentrations, including the nitrate radical, hydroxyl radical, and reactive halogens. 

The intensity and frequency of wildfires in California (CA) have increased in recent years, causing significant damage to human health and property. In October 2007, a number of small fire events, collectively referred to as the Witch Creek Fire or Witch Fire started in Southern CA and intensified under strong Santa Ana winds. As a test of current mesoscale modeling capabilities, we use the Weather Research and Forecasting (WRF) model to simulate the 2007 wildfire event in terms of meteorological conditions. The main objectives of the present study are to investigate the impact of horizontal grid resolution and planetary boundary layer (PBL) scheme on the model simulation of meteorological conditions associated with a Mega fire. We evaluate the predictive capability of the WRF model to simulate key meteorological and fire-weather forecast parameters such as wind, moisture, and temperature. Results of this study suggest that more accurate predictions of temperature and wind speed relevant for better prediction of wildfire spread can be achieved by downscaling regional numerical weather prediction products to 1 km resolution. Furthermore, accurate prediction of near-surface conditions depends on the choice of the planetary boundary layer parameterization. The MYNN parameterization yields more accurate prediction as compared to the YSU parameterization. WRF simulations at 1 km resolution result in better predictions of temperature and wind speed than relative humidity during the 2007 Witch Fire. In summary, the MYNN PBL parameterization scheme with finer grid resolution simulations improves the prediction of near-surface meteorological conditions during a wildfire event. 

Abstract. Marine emissions of dimethyl sulfide (DMS) and the subsequent formation of its oxidation products methanesulfonic acid (MSA) and sulfuric acid (H2SO4) are well-known natural precursors of atmospheric aerosols, contributing to particle mass and cloud formation over ocean and coastal regions. Despite a long-recognized and well-studied role in the marine troposphere, DMS oxidation chemistry remains a work in progress within many current air quality and climate models, with recent advances exploring heterogeneous chemistry and uncovering previously unknown intermediate species. With the identification of additional DMS oxidation pathways and intermediate species that influence the eventual fate of DMS, it is important to understand the impact of these pathways on the overall sulfate aerosol budget and aerosol size distribution. In this work, we update and evaluate the DMS oxidation mechanism of the chemical transport model GEOS-Chem by implementing expanded DMS oxidation pathways in the model. These updates include gas- and aqueous-phase reactions, the formation of the intermediates dimethyl sulfoxide (DMSO) and methanesulfinic acid (MSIA), and cloud loss and aerosol uptake of the recently quantified intermediate hydroperoxymethyl thioformate (HPMTF). We find that this updated mechanism collectively decreases the global mean surface-layer gas-phase sulfur dioxide (SO2) mixing ratio by 40 % and enhances the sulfate aerosol (SO42-) mixing ratio by 17 %. We further perform sensitivity analyses exploring the contribution of cloud loss and aerosol uptake of HPMTF to the overall sulfur budget. Comparing modeled concentrations to available observations, we find improved biases relative to previous studies. To quantify the impacts of these chemistry updates on global particle size distributions and the mass concentration, we use the TwO-Moment Aerosol Sectional (TOMAS) aerosol microphysics module coupled to GEOS-Chem and find that changes in particle formation and growth affect the size distribution of aerosol. With this new DMS-oxidation scheme, the global annual mean surface-layer number concentration of particles with diameters smaller than 80 nm decreases by 16.8 %, with cloud loss processes related to HPMTF being mostly responsible for this reduction. However, the global annual mean number of particles larger than 80 nm (corresponding to particles capable of acting as cloud condensation nuclei, CCN) increases by 3.8 %, suggesting that the new scheme promotes seasonal particle growth to these sizes. 

Marine phytoplankton are primary producers in ocean ecosystems and emit dimethyl sulfide (DMS) into the atmosphere. DMS emissions are the largest biological source of atmospheric sulfur and are one of the largest uncertainties in global climate modeling. DMS is oxidized to methanesulfonic acid (MSA), sulfur dioxide, and hydroperoxymethyl thioformate, all of which can be oxidized to sulfate. Ice core records of MSA are used to investigate past DMS emissions but rely on the implicit assumption that the relative yield of oxidation products from DMS remains constant. However, this assumption is uncertain because there are no long-term records that compare MSA to other DMS oxidation products. Here, we share the first long-term record of both MSA and DMS-derived biogenic sulfate concentration in Greenland ice core samples from 1200 to 2006 CE. While MSA declines on average by 0.2 µg S kg^–1over the industrial era, biogenic sulfate from DMS increases by 0.8 µg S kg^–1. This increasing biogenic sulfate contradicts previous assertions of declining North Atlantic primary productivity inferred from decreasing MSA concentrations in Greenland ice cores over the industrial era. The changing ratio of MSA to biogenic sulfate suggests that trends in MSA could be caused by time-varying atmospheric chemistry and that MSA concentrations alone should not be used to infer past primary productivity. 

Abstract In situ observations and output from a numerical model are utilized to examine three dust outbreaks that occurred in the northwestern Sonoran Desert. Via analysis of these events, it is shown that trapped waves generated in the lee of an upwind mountain range produced high surface wind speeds along the desert floor and the observed dust storms. Based on analysis of observational and model output, general characteristics of dust outbreaks generated by trapped waves are suggested, including dust-layer depths and concentrations that are dependent upon wave phase and height above the surface, emission and transport associated with the presence of a low-level jet, and wave-generated high wind speeds and thus emission that occurs far downwind of the wave source. Trapped lee waves are ubiquitous in Earth’s atmosphere and thus it is likely that the meteorological aspects of the dust storms examined here are also relevant to understanding dust in other regions. These dust outbreaks occurred near the Salton Sea, an endorheic inland body of water that is rapidly drying due to changes in water-use management. As such, these findings are also relevant in terms of understanding how future changes in size of the Salton Sea will impact dust storms and air quality there. Significance Statement Dust storms are ubiquitous in Earth’s atmosphere, yet the physical processes underlying dust emission and subsequent transport are not always understood, in part due to the wide variety of meteorological processes that can generate high winds and dust. Here we use in situ measurements and numerical modeling to demonstrate that vertically trapped atmospheric waves generated by air flowing over a mountain are one such mechanism that can produce dust storms. We suggest several features of these dust outbreaks that are specific to their production by trapped waves. As the study area is a region undergoing rapid environmental change, these results are relevant in terms of predicting future dust there. 

Nuclear reactions play a crucial role in determining the nucleosynthesis that occurs in astrophysical events. The rates of many reactions that significantly impact certain nucleosynthesis processes can not be currently measured via direct means. These reactions must be constrained in another manner, such as determining the level energies and other structure properties of the compound nuclei. In order to measure level energies of nuclei relevant to nuclear astrophysics, the Enge split-pole spectrograph has been installed and commissioned at the University of Notre Dame’s Nuclear Science Laboratory. The first scientific measurement has also been performed. Structure properties of⁵⁸Cu were measured via the reaction⁵⁸Ni(³He,t)⁵⁸Cu to provide the first experimental constraint of the⁵⁷Ni(p,γ)⁵⁸Cu reaction rate, which impacts the production of of⁴⁴Ti,⁵⁷Fe, and⁵⁹Ni in core-collapse supernovae. Preliminary analysis of this measurement confirms the level energies of states in⁵⁸Cu that could lead to significant resonances in the⁵⁷Ni(p,γ)⁵⁸Cu reaction rate, while suggesting the presence of additional states that have not been previously observed but could also lead to significant resonances. 

Precise measurements of nuclear beta decays provide a unique insight into the Standard Model due to their connection to the electroweak interaction. These decays help constrain the unitarity or non-unitarity of the Cabibbo–Kobayashi–Maskawa (CKM) quark mixing matrix, and can uniquely probe the existence of exotic scalar or tensor currents. Of these decays, superallowed mixed mirror transitions have been the least well-studied, in part due to the absence of data on their Fermi to Gamow-Teller mixing ratios (ρ). At the Nuclear Science Laboratory (NSL) at the University of Notre Dame, the Superallowed Transition Beta-Neutrino Decay Ion Coincidence Trap (St. Benedict) is being constructed to determine the ρ for various mirror decays via a measurement of the beta–neutrino angular correlation parameter (aβν) to a relative precision of 0.5%. In this work, we present an overview of the St. Benedict facility and the impact it will have on various Beyond the Standard Model studies, including an expanded sensitivity study of ρ for various mirror nuclei accessible to the facility. A feasibility evaluation is also presented that indicates the measurement goals for many mirror nuclei, which are currently attainable in a week of radioactive beam delivery at the NSL.