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Wood, Robert (ORCID:0000000214013828)

Publications and source records attributed to Wood, Robert (ORCID:0000000214013828).

Exploring ship track spreading rates with a physics-informed Langevin particle parameterization

Abstract. The rate at which aerosols spread from a point source injection, such as from a ship or other stationary pollution source, is critical for accurately representing subgrid plume spreading in a climate model. Such climate model results will guide future decisions regarding the feasibility and application of large-scale intentional marine cloud brightening (MCB). Prior modeling studies have shown that the rate at which ship plumes spread may be strongly dependent on meteorological conditions, such as precipitating versus non-precipitating boundary layers and shear. In this study, we apply a Lagrangian particle model (PM-ABL v1.0), governed by a Langevin stochastic differential equation, to create a simplified framework for predicting the rate of spreading from a ship-injected aerosol plume in sheared, precipitating, and non-precipitating boundary layers. The velocity and position of each stochastic particle is predicted with the acceleration of each particle being driven by the turbulent kinetic energy, dissipation rate, momentum variance, and mean wind. These inputs to the stochastic particle velocity equation are derived from high-fidelity large-eddy simulations (LES) equipped with a prognostic aerosol–cloud microphysics scheme (UW-SAM) to simulate an aerosol injection from a ship into a cloud-topped marine boundary layer. The resulting spreading rate from the reduced-order stochastic model is then compared to the spreading rate in the LES. The stochastic particle velocity representation is shown to reasonably reproduce spreading rates in sheared, precipitating, and non-precipitating cases using domain-averaged turbulent statistics from the LES.

54 ENVIRONMENTAL SCIENCES↗

Abrupt reduction in shipping emission as an inadvertent geoengineering termination shock produces substantial radiative warming

Abstract Human activities affect the Earth’s climate through modifying the composition of the atmosphere, which then creates radiative forcing that drives climate change. The warming effect of anthropogenic greenhouse gases has been partially balanced by the cooling effect of anthropogenic aerosols. In 2020, fuel regulations abruptly reduced the emission of sulfur dioxide from international shipping by about 80% and created an inadvertent geoengineering termination shock with global impact. Here we estimate the regulation leads to a radiative forcing of $$+0.2\pm 0.11$$ + 0.2 ± 0.11 Wm −2 averaged over the global ocean. The amount of radiative forcing could lead to a doubling (or more) of the warming rate in the 2020 s compared with the rate since 1980 with strong spatiotemporal heterogeneity. The warming effect is consistent with the recent observed strong warming in 2023 and expected to make the 2020 s anomalously warm. The forcing is equivalent in magnitude to 80% of the measured increase in planetary heat uptake since 2020. The radiative forcing also has strong hemispheric contrast, which has important implications for precipitation pattern changes. Our result suggests marine cloud brightening may be a viable geoengineering method in temporarily cooling the climate that has its unique challenges due to inherent spatiotemporal heterogeneity.

54 ENVIRONMENTAL SCIENCES↗

Biomass-burning smoke's properties and its interactions with marine stratocumulus clouds in WRF-CAM5 and southeastern Atlantic field campaigns

Abstract. A large part of the uncertainty in climate projections comes from uncertain aerosol properties and aerosol–cloud interactions as well as the difficulty in remotely sensing them. The southeastern Atlantic functions as a natural laboratory to study biomass-burning smoke and to constrain this uncertainty. We address these gaps by comparing the Weather Research and Forecasting with Chemistry Community Atmosphere Model (WRF-CAM5) to the multi-campaign observations ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS), CLARIFY (CLoud–Aerosol–Radiation Interaction and Forcing), and LASIC (Layered Atlantic Smoke Interactions with Clouds) in the southeastern Atlantic in August 2017 to evaluate a large range of the model's aerosol chemical properties, size distributions, processes, and transport, as well as aerosol–cloud interactions. Overall, while WRF-CAM5 is able to represent smoke properties and transport, some key discrepancies highlight the need for further analysis. Observations of smoke composition show an overall decrease in aerosol mean diameter as smoke ages over 4–12 d, while the model lacks this trend. A decrease in the mass ratio of organic aerosol (OA) to black carbon (BC), OA:BC, and the OA mass to carbon monoxide (CO) mixing ratio, OA:CO, suggests that the model is missing processes that selectively remove OA from the particle phase, such as photolysis and heterogeneous aerosol chemistry. A large (factor of ∼2.5) enhancement in sulfate from the free troposphere (FT) to the boundary layer (BL) in observations is not present in the model, pointing to the importance of properly representing secondary sulfate aerosol formation from marine dimethyl sulfide and gaseous SO2 smoke emissions. The model shows a persistent overprediction of aerosols in the marine boundary layer (MBL), especially for clean conditions, which multiple pieces of evidence link to weaker aerosol removal in the modeled MBL than reality. This evidence includes several model features, such as not representing observed shifts towards smaller aerosol diameters, inaccurate concentration ratios of carbon monoxide and black carbon, underprediction of heavy rain events, and little evidence of persistent biases in modeled entrainment. The average below-cloud aerosol activation fraction (NCLD/NAER) remains relatively constant in WRF-CAM5 between field campaigns (∼0.65), while it decreases substantially in observations from ORACLES (∼0.78) to CLARIFY (∼0.5), which could be due to the model misrepresentation of clean aerosol conditions. WRF-CAM5 also overshoots an observed upper limit on liquid cloud droplet concentration around NCLD= 400–500 cm−3 and overpredicts the spread in NCLD. This could be related to the model often drastically overestimating the strength of boundary layer vertical turbulence by up to a factor of 10. We expect these results to motivate similar evaluations of other modeling systems and promote model development to reduce critical uncertainties in climate simulations.

54 ENVIRONMENTAL SCIENCES↗

An attribution of the low single-scattering albedo of biomass burning aerosol over the southeastern Atlantic

Abstract. Aerosol over the remote southeastern Atlantic is some of the most sunlight-absorbing aerosol on the planet: the in situ free-tropospheric single-scattering albedo at the 530 nm wavelength (SSA530 nm) ranges from 0.83 to 0.89 within ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) aircraft flights from late August–September. Here we seek to explain the low SSA. The SSA depends strongly on the black carbon (BC) number fraction, which ranges from 0.15 to 0.4. Low organic aerosol (OA)-to-BC mass ratios of 8–14 and modified combustion efficiency values >0.975 point indirectly to the dry, flame-efficient combustion of primarily grass fuels, with back trajectories ending in the miombo woodlands of Angola. The youngest aerosol, aged 4–5 d since emission, occupied the top half of a 5 km thick plume sampled directly west of Angola with a vertically consistent BC:ΔCO (carbon monoxide) ratio, indicating a homogenization of the source emissions. The younger aerosol, transported more quickly off of the continent by stronger winds, overlaid older, slower-moving aerosol with a larger mean particle size and fraction of BC-containing particles. This is consistent with ongoing gas condensation and the coagulation of smaller non-BC particles upon the BC-containing particles. The particle volumes and OA:BC mass ratios of the older aerosol were smaller, attributed primarily to evaporation following fragmentation, instead of dilution or thermodynamics. The CLARIFY (CLoud–Aerosol–Radiation Interaction and Forcing: Year 2017) aircraft campaign sampled aerosols that had traveled further to reach the more remote Ascension Island. CLARIFY reported higher BC number fractions, lower OA:BC mass ratios, and lower SSA yet larger mass absorption coefficients compared to this study's. Values from one ORACLES 2017 flight, held midway to Ascension Island, are intermediate, confirming the long-range changes. Overall the data are most consistent with continuing oxidation through fragmentation releasing aerosols that subsequently enter the gas phase, reducing the OA mass, rather than evaporation through dilution or thermodynamics. The data support the following best fit: SSA530nm=0.801+0055⋅(OA:BC) (r=0.84). The fires of southern Africa emit approximately one-third of the world's carbon; the emitted aerosols are distinct from other regional smoke emissions, and their composition needs to be represented appropriately to realistically depict regional aerosol radiative effects.

54 ENVIRONMENTAL SCIENCES↗

On the differences in the vertical distribution of modeled aerosol optical depth over the southeastern Atlantic

Abstract. The southeastern Atlantic is home to an expansive smoke aerosol plume overlying a large cloud deck for approximately a third of the year. The aerosol plume is mainly attributed to the extensive biomass burning activities that occur in southern Africa. Current Earth system models (ESMs) reveal significant differences in their estimates of regional aerosol radiative effects over this region. Such large differences partially stem from uncertainties in the vertical distribution of aerosols in the troposphere. These uncertainties translate into different aerosol optical depths (AODs) in the planetary boundary layer (PBL) and the free troposphere (FT). This study examines differences of AOD fraction in the FT and AOD differences among ESMs (WRF-CAM5, WRF-FINN, GEOS-Chem, EAM-E3SM, ALADIN, GEOS-FP, and MERRA-2) and aircraft-based measurements from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign. Models frequently define the PBL as the well-mixed surface-based layer, but this definition misses the upper parts of decoupled PBLs, in which most low-level clouds occur. To account for the presence of decoupled boundary layers in the models, the height of maximum vertical gradient of specific humidity profiles from each model is used to define PBL heights. Results indicate that the monthly mean contribution of AOD in the FT to the total-column AOD ranges from 44 % to 74 % in September 2016 and from 54 % to 71 % in August 2017 within the region bounded by 25∘ S–0∘ N–S and 15∘ W–15∘ E (excluding land) among the ESMs. ALADIN and GEOS-Chem show similar aerosol plume patterns to a derived above-cloud aerosol product from the Moderate Resolution Imaging Spectroradiometer (MODIS) during September 2016, but none of the models show a similar above-cloud plume pattern to MODIS in August 2017. Using the second-generation High Spectral Resolution Lidar (HSRL-2) to derive an aircraft-based constraint on the AOD and the fractional AOD, we found that WRF-CAM5 produces 40 % less AOD than those from the HSRL-2 measurements, but it performs well at separating AOD fraction between the FT and the PBL. AOD fractions in the FT for GEOS-Chem and EAM-E3SM are, respectively, 10 % and 15 % lower than the AOD fractions from the HSRL-2. Their similar mean AODs reflect a cancellation of high and low AOD biases. Compared with aircraft-based observations, GEOS-FP, MERRA-2, and ALADIN produce 24 %–36 % less AOD and tend to misplace more aerosols in the PBL. The models generally underestimate AODs for measured AODs that are above 0.8, indicating their limitations at reproducing high AODs. The differences in the absolute AOD, FT AOD, and the vertical apportioning of AOD in different models highlight the need to continue improving the accuracy of modeled AOD distributions. These differences affect the sign and magnitude of the net aerosol radiative forcing, especially when aerosols are in contact with clouds.

54 ENVIRONMENTAL SCIENCES↗

Long-range transported continental aerosol in the eastern North Atlantic: three multiday event regimes influence cloud condensation nuclei

Abstract. The eastern North Atlantic (ENA) is a region dominated by pristine marine environment and subtropical marine boundary layer clouds. Under unperturbed atmospheric conditions, the regional aerosol regime in the ENA varies seasonally due to different seasonal surface-ocean biogenic emissions, removal processes, and meteorological regimes. However, during periods when the marine boundary layer aerosol in the ENA is impacted by particles transported from continental sources, aerosol properties within the marine boundary layer change significantly, affecting the concentration of cloud condensation nuclei (CCN). Here, we investigate the impact of long-range transported continental aerosol on the regional aerosol regime in the ENA using data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility on Graciosa Island in 2017 during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. We develop an algorithm that integrates number concentrations of particles with optical particle dry diameter (Dp) between 100 and 1000 nm, single scattering albedo, and black carbon concentration to identify multiday events (with duration >24 consecutive hours) of long-range continental aerosol transport in the ENA. In 2017, we detected nine multiday events of long-range transported particles that correspond to ∼ 7.5 % of the year. For each event, we perform HYSPLIT 10 d backward trajectories analysis, and we evaluate CALIPSO aerosol products to assess, respectively, the origins and compositions of aerosol particles arriving at the ENA site. Subsequently, we group the events into three categories, (1) mixture of dust and marine aerosols, (2) mixture of marine and polluted continental aerosols from industrialized areas, and (3) biomass burning aerosol from North America and Canada, and we evaluate their influence on aerosol population and cloud condensation nuclei in terms of potential activation fraction and concentrations at supersaturation of 0.1 % and 0.2 %. The arrival of plumes dominated by the mixture of dust and marine aerosol in the ENA in the winter caused significant increases in baseline Ntot. Simultaneously, the baseline particle size modes and CCN potential activation fraction remained almost unvaried, while cloud condensation nuclei concentrations increased proportionally to Ntot. Events dominated by a mixture of marine and polluted continental aerosols in spring, fall, and winter led to a statistically significant increase in baseline Ntot, a shift towards larger particular sizes, a higher CCN potential activation fractions, and cloud condensation nuclei concentrations of >170 % and up to 240 % higher than during baseline regime. Finally, the transported aerosol plumes characterized by elevated concentration of biomass burning aerosol from continental wildfires detected in the summertime did not statistically contribute to increase baseline aerosol particle concentrations in the ENA. However, particle diameters were larger than under baseline conditions, and CCN potential activation fractions were >75 % higher. Consequentially, cloud concentration nuclei concentrations increased by ∼ 115 % during the period affected by the biomass burning events. Our results suggest that, through the year, multiday events of long-range continental aerosol transport periodically affect the ENA and represent a significant source of CCN in the marine boundary layer. Based on our analysis, in 2017, the multiday aerosol plume transport dominated by a mixture of dust and marine aerosol, a mixture of marine and polluted continental aerosols, and biomass burning aerosols caused increases in the NCCN baseline regime of, respectively, 6.6 %, 8 %, and 7.4 % at SS 0.1 % (and, respectively, 6.5 %, 8.2 %, and 7.3 % at SS 0.2 %) in the ENA.

54 ENVIRONMENTAL SCIENCES↗

Vertical profiles of trace gas and aerosol properties over the eastern North Atlantic: variations with season and synoptic condition

Abstract. Because of their extensive coverage, marine low clouds greatly impact the global climate. Presently, the response of marine low clouds to the changes in atmospheric aerosols remains a major source of uncertainty in climate simulations. One key contribution to this large uncertainty derives from the poor understanding of the properties and processes of marine aerosols under natural conditions and the perturbation by anthropogenic emissions. The eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer (MBL) clouds, where cloud albedo and precipitation are highly susceptible to perturbations in aerosol properties. Here we examine the key processes that drive the cloud condensation nuclei (CCN) population in the MBL using comprehensive characterizations of aerosol and trace gas vertical profiles during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. During ACE-ENA, a total of 39 research flights were conducted in the Azores: 20 during summer 2017 and 19 during winter 2018. During summer, long-range-transported aerosol layers were periodically observed in the lower free troposphere (FT), leading to elevated FT CCN concentrations (NCCN). Both biomass burning and pollution from North America contribute to submicron aerosol mass in these layers, with pollution likely the dominant contributor. In contrast, long-range transported continental emissions have a much weaker influence on the aerosol properties in the ENA during the winter season. While the entrainment of FT air is a major source of particle number in the MBL for both seasons, on average it does not serve as a direct source of CCN in the MBL because the average FT NCCN is the same or even lower than that in the MBL. The particle number flux due to FT entrainment is dominated by pre-CCN (particles that are too small to form cloud droplets under typical conditions, i.e., particles with sizes below the Hoppel minimum) due to the elevated Npre-CCN in the lower FT. Once these pre-CCN are entrained into the MBL, they can grow and reach CCN size range through condensational growth, representing an indirect and major source of MBL CCN in the ENA. The impact of synoptic conditions on the aerosol properties is examined. Under pre-front and post-front conditions, shallow convective activity often leads to a deep and decoupled boundary layer. Coalescence scavenging and evaporation of drizzle below clouds lead to reduced NCCN and larger accumulation-mode particle sizes in the upper cloud-containing decoupled layer, indicating that surface measurements overestimate the NCCN relevant to the formation of MBL clouds under decoupled conditions.

54 ENVIRONMENTAL SCIENCES↗

Identifying a regional aerosol baseline in the eastern North Atlantic using collocated measurements and a mathematical algorithm to mask high-submicron-number-concentration aerosol events

Abstract. High-time-resolution measurements of in situ aerosol and cloud properties provide the ability to study regional atmospheric processes that occur on timescales of minutes to hours. However, one limitation to this approach is that continuous measurements often include periods when the data collected are not representative of the regional aerosol. Even at remote locations, submicron aerosols are pervasive in the ambient atmosphere with many sources. Therefore, periods dominated by local aerosol should be identified before conducting subsequent analyses to understand aerosol regional processes and aerosol–cloud interactions. Here, we present a novel method to validate the identification of regional baseline aerosol data by applying a mathematical algorithm to the data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility in the eastern North Atlantic (ENA). The ENA central facility (C1) includes an aerosol observing system (AOS) for the measurement of aerosol physical, optical, and chemical properties at time resolutions from seconds to minutes. A second temporary supplementary facility (S1), located ∼0.75 km from C1, was deployed for ∼1 year during the Aerosol and Cloud Experiments (ACE-ENA) campaign in 2017. First, we investigate the local aerosol at both locations. We associate periods of high submicron number concentration (Ntot) in the fine-mode condensation particle counter (CPC) and size distributions from the Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) as a function of wind direction using a meteorology sensor with local sources. Elevated concentrations of Aitken-mode (< 100 nm diameter) particles were observed in correspondence with the wind directions associated with airport operations. At ENA, the Graciosa Airport and its associated activities were found to be the main sources of high-concentration aerosol events at ENA, causing peaks in 1 min Ntot that exceeded 8000 and 10 000 cm−3 at C1, in summer and winter, respectively, and 5000 cm−3 at S1 in summer. Periods with high Ntot not associated with these wind directions were also observed. As a result, the diverse local sources at ENA yielded a poor relationship between Ntot measurements collected at C1 and S1 (R2=0.03 with a slope =0.05±0.001). As a first approach to mask these events, the time periods when the wind direction was associated with the airport operations (west to northwest and southeast to south at C1 and east to south at S1) were applied. The meteorological masks removed 38.9 % of the data at C1 and 43.4 % at S1, and they did not significantly improve the relationship between the two sites (R2=0.18 with a slope =0.06±0.001). Due to the complexity of high-Ntot events observed at ENA, we develop and validate a mathematical ENA Aerosol Mask (ENA-AM) to identify high-Ntot events using 1 min resolution data from the AOS CPC at C1 and S1. After its parameterization and application, ENA-AM generated a high correlation between Ntot in the summer at C1 and S1 (R2=0.87 with a slope =0.84±0.001). We identified the regional baseline at ENA to be 428±228 cm−3 in the summer and 346±223 cm−3 in the winter. Lastly, we compared masked measurements from the AOS with the ARM Aerial Facility (AAF) during flights over C1 in the summer to understand submicron aerosol vertical mixing over C1. The high correlation (R2=0.71 with a slope of 1.04±0.01) observed between C1 and the AAF Ntot collected within an area of 10 km surrounding ENA and at altitudes < 500 m indicated that the submicron aerosol at ENA was well mixed within the first 500 m of the marine boundary layer during the month of July during ACE-ENA. Our novel method for determining a regional aerosol baseline at ENA can be applied to other time periods and at other locations with validation by a secondary site or additional collocated measurements.

54 ENVIRONMENTAL SCIENCES↗