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Creators/Authors contains: "Gold, A"

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  1. Ion mobility spectrometry (IMS) using Structures for Lossless Ion Manipulations (SLIM) is an emerging powerful tool for rapid isomer separations. This technology offers high mobility resolution due to prolonged ion mobility path lengths that are achieved on a small form factor separation device. In this work, we interface SLIM IMS separation with a chemical ionization source, which allows one to sample from the gas- and particle-phases directly. As such, one can monitor dynamic isomer populations in ambient air in real-time without prior sample preparation. This technology opens the door to new possibilities in atmospheric chemistry where isomer distribution is expected to play a key role in gas phase processes and in the formation of organic aerosols. The CI-IMS-TOF instrument built by TOFWERK produces ions via a two-step chemical ionization process, which involves 1) producing reagent ions and 2) ionizing neutral analyte molecules via the reagent ions through either charge transfer or adduct formation. Once generated, these secondary ions travel into the SLIM IMS region, where a series of DC- and AC-electrodes on printed circuit boards create a traveling wave driving force. As the ions travel through the helium buffer gas, they separate based on their rotationally averaged collision cross-sections. In the present work, various experiments were performed using an aerosol flow tube reactor and an atmospheric simulation chamber to recreate atmospheric conditions. Gas-phase oxidation of isoprene was used to explore the capabilities of the CI-SLIM IMS-MS under atmospheric relevant conditions. Firstly, the most important oxidation products produced from the OH-oxidation of isoprene were used including methacrolein, methyl vinyl ketone, isoprene epoxy diols (IEPOX), isoprene hydroxy hydroperoxide (1,2 and 4,3-ISOPOOH), and other C5H10O3 reactive uptake products as a single component or as a mixture to first evaluate the capabilities of the CI-SLIM IMS-MS at resolving the different isomers. Secondly, the reactive uptake of IEPOX onto acidic particles and OH-initiated oxidation (low and high NO regimes) of isoprene were studied to characterize the dynamic of the isomers generated within the simulation chamber under various environmental conditions. Results will be presented to demonstrate the capabilities of the newly developed CI-SLIM IMS-MS at resolving isomers in real time. How to cite: Riva, M., Gerber, S., Claflin, M., Mettke, P., Frauenheim, M., Rice, R., Gold, A., Surratt, J., Yatsyna, V., Graf, S., Canagaratna, M., Herrmann, H., Rohner, U., Kamrath, M., and Lopez-Hilfiker, F.: Real-time monitoring of dynamic isomer populations with CI-SLIM IMS-MS, EGU General Assembly 2024, Vienna, Austria, 14–19 Apr 2024, EGU24-6074, https://doi.org/10.5194/egusphere-egu24-6074, 2024. 
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  2. null (Ed.)
    Narragansett Bay (Rhode Island, USA) is an estuary undergoing changes from a combination of rising water temperatures, nutrient fluxes, and human uses. In this study, we created an ecosystem food web model and evaluated its ability to predict functional group biomasses. Specifically, we used Ecopath to construct 2 mass-balanced models covering different time periods in Narragansett Bay: a historical model using data from 1994-1998 and a present-day model that represents 2014-2018. With the historical model as a starting point, we used Ecosim fit to time series data and projected forward to present-day values, forcing the model with both phytoplankton biomass and fishing mortality. The biomass of most mid- and upper trophic level groups increased by 2018, with the exception of carnivorous benthos, which experienced a large decline. There were changes in the composition of fisheries, with a large increase in recreational benthivorous fish landings and a decrease in commercial landings of planktivorous fish and suspension feeding benthos. The inclusion of fishing mortality and phytoplankton biomass as forcing functions, as well as adjusting the vulnerability levels of prey, greatly improved our model fits for all functional groups with the exception of gelatinous zooplankton. Our ecosystem model was able to correctly predict the direction of change for all fish and fished invertebrate groups with a relatively high degree of precision, particularly for the upper trophic levels. Thus, this ecosystem model is broadly applicable and suitable to project trends in the Narragansett Bay food web associated with localized and adaptive ecosystem-based management. 
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  3. Abstract Inundation of coastal stormwater networks by tides is widespread due to sea‐level rise (SLR). The water quality risks posed by tidal water rising up through stormwater infrastructure (pipes and catch basins), out onto roadways, and back out to receiving water bodies is poorly understood but may be substantial given that stormwater networks are a known source of fecal contamination. In this study, we (a) documented temporal variation in concentrations ofEnterococcusspp. (ENT), the fecal indicator bacteria standard for marine waters, in a coastal waterway over a 2‐month period and more intensively during two perigean spring tide periods, (b) measured ENT concentrations in roadway floodwaters during tidal floods, and (c) explained variation in ENT concentrations as a function of tidal inundation, antecedent rainfall, and stormwater infrastructure using a pipe network inundation model and robust linear mixed effect models. We find that ENT concentrations in the receiving waterway vary as a function of tidal stage and antecedent rainfall, but also site‐specific characteristics of the stormwater network that drains to the waterway. Tidal variables significantly explain measured ENT variance in the waterway, however, runoff drove higher ENT concentrations in the receiving waterway. Samples of floodwaters on roadways during both perigean spring tide events were limited, but all samples exceeded the threshold for safe public use of recreational waters. These results indicate that inundation of stormwater networks by tides could pose public health hazards in receiving water bodies and on roadways, which will likely be exacerbated in the future due to continued SLR. 
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