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38 records · Page 3

Tracking Aerosol Convection Interactions Experiment (TRACER) Field Campaign Report

Convective clouds serve a critical role in the Earth’s energy and water cycles through their transport of heat, moisture, momentum, and chemical species through the troposphere driving the global circulation (e.g., Hartmann et al. 1984, Del Genio et al. 2012, Su et al. 2014). On more local scales, convective clouds impact the atmospheric heating profile through diabatic heating effects, removal of water from the atmospheric column through precipitation, and conditioning of the local environment impacting further development of clouds (e.g., Sullivan and Voigt 2021). These critical roles underscore the importance of realistic representation of convective processes across scales of models from large-eddy simulation (LES), to convection-permitting models (CPM; e.g., Kendon et al. 2020, Marinescu et al. 2021), to numerical weather prediction (NWP) models used for operational weather forecasting, to Earth system models used to predict climate sensitivity (Sanderson et al. 2011, Sherwood et al. 2014, Tomassini et al. 2014, Zhao et al. 2016, Cronin et al. 2017). A key component of improving model representation of convective clouds is better quantification and parameterization of updraft microphysics and dynamics, including their interactions with the surrounding environment and storm organization (Bony et al. 2015, Hagos and Houze 2016, Donner et al. 2016, Morrison et al. 2020). Aerosol is an important environmental factor that could affect convective clouds and precipitation since cloud droplet and ice formation processes are initiated by it. Andrae et al. (2004) hypothesized that aerosols associated with increased biomass burning particles acting as cloud condensation nuclei (CCN) result in smaller and more monodisperse cloud droplets leading to suppression of warm rain formation, ultimately leading to more cloud water being lofted above the freezing level based on observations in the Amazon region. The subsequent increase in latent heat release increases the buoyancy of rising convective parcels invigorating the deep convection. This work was followed by a description of the theoretical basis for this “cold-phase invigoration” by Rosenfeld et al. (2008), who argued that it could have a significant effect for deep convective clouds with warm cloud-bases. Several modeling studies (e.g., Khain et al. 2005, 2009, van den Heever et al. 2006, Fan et al. 2007, 2009, 2012, Lee et al. 2008, Storer et al. 2010, Lebo et al. 2012, Storer and van den Heever 2013, Chen et al. 2020, Dagan et al. 2022) have investigated these aerosol-convection interactions and the environmental factors that influence their relative importance and magnitude. More recently, several studies have indicated that “warm-phase invigoration”, the enhancement of convection through condensational heating, also appears to play a role in enhancing both shallow cumuli (Seiki and Nakajima 2014, Saleeby et al 2015) and deeper tropical convection (Lebo and Seinfeld 2011, Khain et al. 2012, Sheffield et al 2015, Fan et al. 2018, Igel and van den Heever 2021), as well as Houston thunderstorms (Fan et al. 2007, 2020). However, still other studies have provided additional evidence of systematic biases in simulated convective outflow ice size distribution properties, which are consistent with a lack of poorly understood secondary ice production within convective updrafts (e.g., Fridlind et al. 2017). To help address these critical gaps in our understanding of cloud processes, aerosol processes and aerosol-cloud interactions, the Tracking Aerosol Convection Interactions Experiment was designed building upon efforts by the Aerosol, Cloud, Precipitation and Climate (ACPC) Initiative (http://acpcintiative.org/), a joint effort of the International Geosphere-Biosphere Programme (IGBP) and the World Climate Research Program (WCRP) that focused on resolving uncertainties in the interactions between aerosol and clouds towards better understanding the role that these interactions play in the climate system. The TRACER campaign was motivated by recommendations from a number of pilot studies undertaken by ACPC (van den Heever et al. 2017, Fridlind et al. 2019, Hu et al. 2019, Fan et al. 2020, Marinescu et al. 2021, Hernandez-Deckers et al. 2022) that pointed towards the southeastern Texas region as a locale where aerosol-convection interactions could be studied owing to the copious occurrence of isolated convection during the summer months accompanied by diverse and significant sources of aerosols from both anthropogenic and natural sources. The TRACER campaign began on 01 October 2021 and extended through 30 September 2022 with an intensive operational period (IOP) during June-September 2022. Three main sites (Table 1) were managed by the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility.

54 ENVIRONMENTAL SCIENCES↗

Contribution of expanded marine sulfur chemistry to the seasonal variability of dimethyl sulfide oxidation products and size-resolved sulfate aerosol

Marine emissions of dimethyl sulfide (DMS) and the subsequent formation of its oxidation products methanesulfonic acid (MSA) and sulfuric acid (H 2 SO 4 ) 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 path ways 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 (SO 2 ) mixing ratio by 40 % and enhances the sulfate aerosol ($SO^{2-}_{4}$) 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.

54 ENVIRONMENTAL SCIENCES↗