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Lee Thornhill

Publications and source records attributed to Lee Thornhill.

Rapid Cloud Removal of Dimethyl Sulfide Oxidation Products Limits SO 2 and Cloud Condensation Nuclei Production in the Marine Atmosphere

Oceans emit large quantities of dimethyl sulfide (DMS) to the marine atmosphere. The oxidation of 60 DMS leads to the formation and growth of cloud condensation nuclei (CCN) with consequent effects on Earth’s radiation balance and climate. Quantitative assessment of the impact of DMS emissions on CCN concentrations necessitates a detailed description of the oxidation of DMS in the presence of existing aerosol particles and clouds. In the unpolluted marine atmosphere, DMS is efficiently oxidized to hydroperoxymethyl thioformate (HPMTF), a stable intermediate in the chemical trajectory towards sulfur dioxide (SO 2 ) and ultimately sulfate aerosol (Veres et al. 2020). Using direct airborne flux measurements, we demonstrate that irreversible loss of HPMTF to clouds in the marine boundary layer determines the HPMTF lifetime (τ HPMTF < 2 hours) and terminates DMS oxidation to SO 2 in the cloudy marine boundary layer. When accounting for HPMTF cloud loss in a global chemical transport model, we show that SO 2 production from DMS is reduced by 35% globally and near surface (0-3km) SO 2 concentrations over the ocean are lowered by 24%. This large, previously unconsidered loss process for volatile sulfur accelerates the timescale for conversion of DMS to sulfate, while limiting new particle formation in the marine atmosphere and changing the dynamics of aerosol growth. This loss process potentially reduces the spatial scale over which DMS emissions contribute to aerosol production and growth and weakens the link between DMS emission and marine CCN production with subsequent implications for cloud formation, radiative forcing, and climate.

dimethyl sulfide↗

On Assessing ERA5 and MERRA2 Representations of Cold-Air Outbreaks Across the Gulf Stream

The warm Gulf Stream sea surface temperatures (SSTs) strongly impact the evolution of winter clouds behind atmospheric cold fronts. Such cloud evolution remains challenging to model. The Gulf Stream is too wide within the ERA5 and MERRA2 reanalyses, affecting the turbulent surface fluxes. Known problems within the ERA5 boundary layer (too-dry and too-cool with too strong westerlies), ascertained primarily from ACTIVATE 2020 campaign aircraft dropsondes and secondarily from older buoy measurements, reinforce surface flux biases. In contrast, MERRA2 winter surface winds and air-sea temperature/humidity differences are slightly too weak, producing surface fluxes that are too low. Reanalyses boundary layer heights in the strongly-forced winter cold-air-outbreak regime are realistic, whereas late-summer quiescent stable boundary layers are too shallow. Nevertheless, the reanalysis biases are small, and reanalyses adequately support their use for initializing higher-resolution cloud process modeling studies of cold-air outbreaks.

Gulf stream↗

TPSAS-NF1676L-22701-DND

The next generation of aerosol satellite instruments will include multi-spectral polarimetric measurements to retrieval aerosol size distribution and refractive index (Hasekamp et al., 2011; NRC, 2007). Refractive index is the “only means of constraining aerosol chemical composition from space” for passive sensors (Mischenko et al., 2007). A number of methods have been developed to derive refractive index from combined optical and electrical mobility sizing instruments (e.g., the “Alignment Method” of Hand and Kreidenweis, 2002). In this work, we evaluate the sensitivity of two, commercially-available, high-resolution optical particle counters for determining the size-resolved refractive index of laboratory-generated aerosols when used with a modified form of the Alignment Method.

Stephen Zimmerman↗

TPSAS-NF1676L-23266-DND

Currently, near-surface air quality information (e.g. PM_2.5) must be inferred from column-integrated quantities (i.e. Aerosol Optical Thickness – AOT) obtained by passive remote sensing from downward-looking satellite instruments. Such retrievals must address the following questions: What do we use for the height of the aerosols? Mixed Layer (ML) height? Can we assume that near-surface aerosol extinction is about the same as the mean aerosol extinction in the ML? How well is near-surface extinction related to surface PM_2.5? How well can column AOT be used to infer near-surface aerosol extinction and PM_2.5?

Richard Ferrare↗

Airborne High Spectral Resolution Lidar-2 Measurements of Enhanced Depolarization in Marine Aerosols

Airborne NASA Langley Research Center (LaRC) High Spectral Resolution Lidar-2 (HSRL-2) measurements acquired during the recent NASA EVS-3 Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE) revealed enhanced particulate linear depolarization associated with aerosols within the marine boundary layer. These HSRL-2 observations were acquired off the east coast of the United States in February and March 2020 when this lidar was deployed on the NASA LaRC UC-12 aircraft. HSRL-2 measured profiles of aerosol backscattering, extinction,and depolarization at 355 and 532nm and aerosol backscattering and depolarization at 1064nm. Typically HSRL-2 measures low (<5%) linear particulate depolarization associated with marine sea salt aerosols. However, during several ACTIVATE flights, particularly those that occurred with outbreaks of cold, dry air, linear particulate depolarization exceeded 15-20% (532nm) for aerosols within a few hundred meters above the surface. These high values indicated that these particles were nonspherical. Elevated depolarization values were also observed at 355 and 1064 nm. HSRL-2 measured aerosol extinction/backscatter ratio (“lidar ratio”) values around 20-25 sr (355 and 532 nm) that are typically associated with sea salt particles. Coincident measurements of relative humidity from dropsondes released from the UC-12and in situ Diode Laser Hygrometer (DLH) measurements flown on the NASA HU-25 aircraft showed that highest depolarization values of these nonspherical particles were found when the relative humidity (RH)was below 50-60%.These lidar observations of elevated depolarization associated with sea salt aerosol are consistent with previous lidar measurements of sea salt aerosols in dry conditions. We discuss these HSRL-2 measurements also in the context of coincident airborne in situ measurements of particle size and composition acquired on the HU-25 aircraft. We also found that CALIOP satellite measurements observed elevated depolarization during some similar cold air outbreaks. In such cases, the operational CALIOP algorithms attributed the elevated depolarization to nonspherical dust particles rather than the more likely scenario of nonspherical sea salt particles associated with low RH.

aerosols↗

Observation of Trace Gases Seasonal Variability in the Marine Boundary Layer over the Atlantic Ocean during the ACTIVATE Field Campaign

High resolution in-situ measurements of carbon monoxide (CO), carbon dioxide (CO2), methane (CH4), and water vapor (H2O) were made onboard the NASA HU-25 aircraft during the ACTIVATE (Aerosol Cloud meteorology Interactions oVer the western Atlantic Experiment) campaign during 2020 and 2021 in different seasons (winter through summer) over the mid-latitude western Atlantic Ocean. As most of the flights focused on the marine boundary layer (MBL) during the campaign, these trace gas observations are an excellent data set to examine seasonal variability of trace gas background values in the MBL without the influence of localized point sources. We will describe the variability of these trace gases in the MBL background by filtering out concentrated point sources using back trajectory analysis along with trace gas ratios. Additionally, the ocean is a significant sink of anthropogenic CO2 capturing about one quarter of total anthropogenic carbon. By looking at the MBL CO2 variation as a function of season, we discuss observed changes in CO2 uptake over the ocean. These high accuracy observations of trace gas backgrounds in the MBL along with characterizing seasonal effects on oceanic sequestering of anthropogenic CO2 will improve the understanding of seasonal variations and change in climate and inverse modelling over the ocean.

Yonghoon Choi↗

Exploring the Continuum of Stratiform and Cumulus Cloudiness: Observational Insights Related to Marine Boundary Layer Clouds

Low-level marine clouds take on a wide range of morphological states owing to external forcing and internal feedbacks. Rarely are shallow marine clouds adequately described by a single simplified framework but instead exhibit features that partially conform to several states that could be considered “limiting”. Perhaps the most apparent dichotomy is whether to consider shallow clouds as existing within a surface-driven mixed layer or as convective “plume” elements positioned on top. Do the rules that govern the limiting cases transition smoothly through the hybrid scenarios found in nature, or are there particular regions of attraction or repulsion?We have identified 3 ”axes” along which to investigate how the energetics, thermodynamics and cloud macro structure relate to the intermediate spaces between idealizations.

Ewan Crosbie↗