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At least 505 records · Page 28

Micro-spectroscopic and freezing characterization of ice-nucleating particles collected in the marine boundary layer in the eastern North Atlantic

Abstract. Formation of atmospheric ice plays a crucial role in the microphysical evolution of mixed-phase and cirrus clouds and thus climate. How aerosol particles impact ice crystal formation by acting as ice-nucleating particles (INPs) is a subject of intense research activities. To improve understanding of atmospheric INPs, we examined daytime and nighttime particles collected during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign conducted in summer 2017. Collected particles, representative of a remote marine environment, were investigated for their propensity to serve as INPs in the immersion freezing (IMF) and deposition ice nucleation (DIN) modes. The particle population was characterized by chemical imaging techniques such as computer-controlled scanning electron microscopy with energy-dispersive X-ray analysis (CCSEM/EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine-structure spectroscopy (STXM/NEXAFS). Four major particle-type classes were identified where internally mixed inorganic–organic particles make up the majority of the analyzed particles. Following ice nucleation experiments, individual INPs were identified and characterized by SEM/EDX. The identified INP types belong to the major particle-type classes consisting of fresh sea salt with organics or processed sea salt containing dust and sulfur with organics. Ice nucleation experiments show IMF events at temperatures as low as 231 K, including the subsaturated regime. DIN events were observed at lower temperatures of 210 to 231 K. IMF and DIN observations were analyzed with regard to activated INP fraction, ice-nucleation active site (INAS) densities, and a water activity-based immersion freezing model (ABIFM) yielding heterogeneous ice nucleation rate coefficients. Observed IMF and DIN events of ice formation and corresponding derived freezing rates demonstrate that the marine boundary layer aerosol particles can serve as INPs under typical mixed-phase and cirrus cloud conditions. The derived IMF and DIN parameterizations allow for implementation in cloud and climate models to evaluate predictive effects of atmospheric ice crystal formation.

54 ENVIRONMENTAL SCIENCES↗

Light Absorption by Brown Carbon over the South-East Atlantic Ocean

Biomass burning emissions often contain brown carbon (BrC), which represents a large family of light-absorbing organics that is chemically complex and therefore difficult to estimate their absorption of incoming solar radiation, resulting in large uncertainties in the estimation of the global direct radiative effect of aerosols. Here we investigate the contribution of BrC to the total light absorption of biomass burning aerosols over the South-East Atlantic Ocean with different optical models utilizing a suite of airborne measurements from the ORACLES 2018 campaign by introducing an effective refractive index of black carbon (BC), m eBC = n eBC +ik eBC , that accounts for all possible absorbing components at 660 nm wavelength to facilitate the attribution of absorption at shorter wavelengths. Most values of the imaginary part of the refractive index, k eBC , were larger than those commonly used for BC from biomass burning emissions, suggesting contributions from absorbers beyond BC at 660 nm. The TEM-EDX single particle analysis further suggests that these long-wavelength absorbers might include iron oxides, as iron is found to be present only when large values of k eBC are derived. Using this effective BC refractive index, we find that the contribution of BrC to the total absorption at 470 nm (R BrC,470 ) ranges from ~5–15 %, with the organic aerosol mass absorption coefficient (MAC OA,470 ) at this wavelength ranging from 0.25 ± 0.34 m 2 g -1 to 0.43 ± 0.12 m 2 g -1 . The core-shell model yielded much higher estimates of MAC OA,470 and R BrC,470 than homogeneous mixing models, underscoring the importance of model treatment. Another key finding was that estimates of the BrC contribution at 470 nm from the commonly used AAE (absorption Ångström exponent) attribution method (< 5 %) are much lower than the BrC contribution estimates (R BrC,470 ) using our new methodology that accounts for contributions from both BrC and non-carbonaceous, long-wavelength absorbers, such as magnetite. Thus, it is recommended that application of any optical properties-based attribution method use absorption coefficients at the longest possible wavelength to minimize the influence of BrC at the long wavelength and to account for potential contributions from other absorbing materials.

54 ENVIRONMENTAL SCIENCES↗

Evaluation of liquid cloud albedo susceptibility in E3SM using coupled eastern North Atlantic surface and satellite retrievals

The impact of aerosol number concentration on cloud albedo is a persistent source of spread in global climate predictions due to multi-scale, interactive atmospheric processes that remain difficult to quantify. We use 5 years of geostationary satellite and surface retrievals at the US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) eastern North Atlantic (ENA) site in the Azores to evaluate the representation of liquid cloud albedo susceptibility for overcast cloud scenes in the DOE Energy Exascale Earth System Model version 1 (E3SMv1) and provide possible reasons for model–observation discrepancies. The overall distribution of surface 0.2 % CCN concentration values is reasonably simulated, but simulated liquid water path (LWP) is lower than observed and layer mean droplet concentration (N d ) comparisons are highly variable depending on the N d retrieval technique. E3SMv1's cloud albedo is greater than observed for given LWP and N d values due to a lower cloud effective radius than observed. However, the simulated albedo response to N d is suppressed due to a correlation between the solar zenith angle (SZA) and N d created by the seasonal cycle that is not observed. Controlling for this effect by examining the cloud optical depth (COD) shows that E3SMv1's COD response to CCN concentration is greater than observed. For surface-based retrievals, this is only true after controlling for cloud adiabaticity because E3SMv1's adiabaticities are much lower than observed. Assuming a constant adiabaticity in surface retrievals as done in top-of-atmosphere (TOA) retrievals narrows the retrieved ln N d distribution, which increases the cloud albedo sensitivity to ln N d to match the TOA sensitivity. The greater sensitivity of COD to CCN is caused by a greater Twomey effect in which the sensitivity of N d to CCN is greater than observed for TOA-retrieved N d , and once model–observation cloud adiabaticity differences are removed, this is also true for surface-retrieved N d . The LWP response to N d in E3SMv1 is overall negative as observed. Despite reproducing the observed LWP–N d relationship, observed clouds become much more adiabatic as N d increases, while E3SMv1 clouds do not, associated with more heavily precipitating clouds that are partially but not completely caused by deeper clouds and weaker inversions in E3SMv1. These cloud property differences indicate that the negative LWP–N d relationship is likely not caused by the same mechanisms in E3SMv1 and observations. The negative simulated LWP response also fails to mute the excessively strong Twomey effect, highlighting potentially important confounding factor effects that likely render the LWP–N d relationship non-causal. N d retrieval scales and assumptions, particularly related to cloud adiabaticity, contribute to substantial spreads in the model–observation comparisons, though enough consistency exists to suggest that aerosol activation, drizzle, and entrainment processes are critical areas to focus E3SMv1 development for improving the fidelity of aerosol–cloud interactions in E3SM.

54 ENVIRONMENTAL SCIENCES↗

Boundary layer moisture variability at the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic observatory during marine conditions

Abstract. Boundary layer moisture variability at the Eastern North Atlantic (ENA) site during marine conditions is examined at monthly and daily timescales using 5 years of ground-based observations and output from the European Center for Medium range Weather Forecast (ECMWF) reanalysis model. The annual cycle of the mixed-layer total water budgets is presented to estimate the relative contribution of large-scale advection, local moisture tendency, entrainment, and precipitation to balance the moistening due to surface latent heat flux on monthly timescales. When marine conditions prevail, advection of colder and dry air from the north acts as an important moisture sink (∼ 50 % of the overall budget) during fall and winter driving the seasonality of the budget. Entrainment and precipitation contribute to the drying of the boundary layer (∼ 25 % and ∼ 15 % respectively), and the local change in moisture contributes to a small residual part. On a daily temporal scale, moist and dry mesoscale columns of vapor (∼ 10 km) are analyzed during 10 selected days of precipitating stratocumulus clouds. Adjacent moist and dry columns present distinct mesoscale features that are strongly correlated with clouds and precipitation. Dry columns adjacent to moist columns have more frequent and stronger downdrafts immediately below the cloud base. Moist columns have more frequent updrafts, stronger cloud-top cooling, and higher liquid water path and precipitation compared to the dry columns. This study highlights the complex interaction between large-scale and local processes controlling the boundary layer moisture and the importance of spatial distribution of vapor to support convection and precipitation.

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↗

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↗

Insights of warm-cloud biases in Community Atmospheric Model 5 and 6 from the single-column modeling framework and Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) observations

There has been a growing concern that most climate models predict precipitation that is too frequent, likely due to lack of reliable subgrid variability and vertical variations in microphysical processes in low-level warm clouds. In this study, the warm-cloud physics parameterizations in the singe-column configurations of NCAR Community Atmospheric Model version 6 and 5 (SCAM6 and SCAM5, respectively) are evaluated using ground-based and airborne observations from the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign near the Azores islands during 2017–2018. The 8-month single-column model (SCM) simulations show that both SCAM6 and SCAM5 can generally reproduce marine boundary layer cloud structure, major macrophysical properties, and their transition. The improvement in warm-cloud properties from the Community Atmospheric Model 5 and 6 (CAM5 to CAM6) physics can be found through comparison with the observations. Meanwhile, both physical schemes underestimate cloud liquid water content, cloud droplet size, and rain liquid water content but overestimate surface rainfall. Modeled cloud condensation nuclei (CCN) concentrations are comparable with aircraft-observed ones in the summer but are overestimated by a factor of 2 in winter, largely due to the biases in the long-range transport of anthropogenic aerosols like sulfate. We also test the newly recalibrated autoconversion and accretion parameterizations that account for vertical variations in droplet size. Compared to the observations, more significant improvement is found in SCAM5 than in SCAM6. This result is likely explained by the introduction of subgrid variations in cloud properties in CAM6 cloud microphysics, which further suppresses the scheme's sensitivity to individual warm-rain microphysical parameters. The predicted cloud susceptibilities to CCN perturbations in CAM6 are within a reasonable range, indicating significant progress since CAM5 which produces an aerosol indirect effect that is too strong. The present study emphasizes the importance of understanding biases in cloud physics parameterizations by combining SCM with in situ observations.

54 ENVIRONMENTAL SCIENCES↗

Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic

Abstract. Atmospheric ice nucleation impacts the hydrological cycle and climate by modifying the radiative properties of clouds. To improve our predictive understanding of ice formation, ambient ice-nucleating particles (INPs) need to be collected and characterized. Measurements of INPs at lower latitudes in a remote marine region are scarce. The Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign, in the region of the Azores islands, provided the opportunity to collect particles in the marine boundary layer (MBL) and free troposphere (FT) by aircraft during the campaign's summer and winter intensive operation period. The particle population in samples collected was examined by scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy. The identified INPs were analyzed by scanning electron microscopy with energy-dispersive X-ray analysis. We observed differences in the particle population characteristics in terms of particle diversity, mixing state, and organic volume fraction between seasons, mostly due to dry intrusion events during winter, as well as between the sampling locations of the MBL and FT. These differences are also reflected in the temperature and humidity conditions under which water uptake, immersion freezing (IMF), and deposition ice nucleation (DIN) proceed. Identified INPs reflect typical particle types within the particle population on the samples and include sea salt, sea salt with sulfates, and mineral dust, all associated with organic matter, as well as carbonaceous particles. IMF and DIN kinetics are analyzed with respect to heterogeneous ice nucleation rate coefficients, Jhet, and ice nucleation active site density, ns, as a function of the water criterion Δaw. DIN is also analyzed in terms of contact angles following classical nucleation theory. Derived MBL IMF kinetics agree with previous ACE-ENA ground-site INP measurements. FT particle samples show greater ice nucleation propensity compared to MBL particle samples. This study emphasizes that the types of INPs can vary seasonally and with altitude depending on sampling location, thereby showing different ice nucleation propensities, which is crucial information when representing mixed-phase cloud and cirrus cloud microphysics in models.

54 ENVIRONMENTAL SCIENCES↗

Aerosol hygroscopicity over the southeast Atlantic Ocean during the biomass burning season – Part 1: From the perspective of scattering enhancement​​​​​​​

Aerosol hygroscopicity plays a vital role in aerosol radiative forcing. One key parameter describing hygroscopicity is the scattering enhancement factor, f(RH), defined as the ratio of the scattering coefficient at humidified relative humidity (RH) to its dry value. Here, we utilize the f(80 %) from ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) 2016 and 2018 airborne measurements to investigate the hygroscopicity of aerosols, its vertical distribution, its relationship with chemical composition, and its sensitivity to organic aerosol (OA) hygroscopicity over the southeast Atlantic (SEA) Ocean during the biomass burning (BB) season. We found that aerosol hygroscopicity remains steady above 2 km, with a mean f(80 %) of 1.40 ± 0.17. Below 2 km, aerosol hygroscopicity increases with decreasing altitude, with a mean f(80 %) of 1.51 ± 0.22, consistent with higher values of BB aerosol hygroscopicity found in the literature. The hygroscopicity parameter of OA (κ OA ) is retrieved from the Mie model with a mean value of 0.11 ± 0.08, which is in the middle to upper range compared to the literature. Higher OA hygroscopicity is related to aerosols that are more aged, oxidized, and present at lower altitudes. The enhanced biomass burning aerosol (BBA) hygroscopicity at lower altitudes is mainly due to a lower OA fraction, increased sulfate fraction, and greater κ OA at lower altitudes. We propose a parameterization that quantifies f(RH) with chemical composition and κOA based on Mie simulation of internally mixed OA–(NH 4 ) 2 SO 4 –BC mixtures. The good agreement between the predictions and the ORACLES measurements implies that the aerosols in the SEA during the BB season can be largely represented by the OA–(NH 4 ) 2 SO 4 –BC internal mixture with respect to the f(RH) prediction. The sensitivity of f(RH) to κ OA indicates that applying a constant κ OA is only suitable when the OA fraction is low and κ OA shows limited variation. However, in situations deviating these two criteria, κ OA can notably impact scattering coefficients and aerosol radiative effect; therefore, accounting for κ OA variability is recommended.

54 ENVIRONMENTAL SCIENCES↗

Daytime variation in the aerosol indirect effect for warm marine boundary layer clouds in the eastern North Atlantic

Abstract. Warm boundary layer clouds in the eastern North Atlantic region exhibit significant diurnal variations in cloud properties. However, the diurnal cycle of the aerosol indirect effect (AIE) for these clouds remains poorly understood. This study takes advantage of recent advancements in the spatial resolution of geostationary satellites to explore the daytime variation in the AIE by estimating the cloud susceptibilities to changes in cloud droplet number concentration (Nd). Cloud retrievals for the month of July over 4 years (2018–2021) from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) on Meteosat-11 over this region are analyzed. Our results reveal a significant “U-shaped” daytime cycle in susceptibilities of the cloud liquid water path (LWP), cloud albedo, and cloud fraction. Clouds are found to be more susceptible to Nd perturbations at noon and less susceptible in the morning and evening. The magnitude and sign of cloud susceptibilities depend heavily on the cloud state defined by cloud LWP and precipitation conditions. Non-precipitating thin clouds account for 44 % of all warm boundary layer clouds in July, and they contribute the most to the observed daytime variation. Non-precipitating thick clouds are the least frequent cloud state (10 %), and they exhibit more negative LWP and albedo susceptibilities compared to thin clouds. Precipitating clouds are the dominant cloud state (46 %), but their cloud susceptibilities show minimal variation throughout the day. We find evidence that the daytime variation in LWP and albedo susceptibilities for non-precipitating clouds is influenced by a combination of the diurnal transition between non-precipitating thick and thin clouds and the “lagged” cloud responses to Nd perturbations. The daytime variation in cloud fraction susceptibility for non-precipitating thick clouds can be attributed to the daytime variation in cloud morphology (e.g., overcast or broken). The dissipation and development of clouds do not adequately explain the observed variation in cloud susceptibilities. Additionally, daytime variation in cloud susceptibility is primarily driven by variation in the intensity of cloud response rather than the frequency of occurrence of cloud states. Our results imply that polar-orbiting satellites with an overpass time at 13:30 LT underestimate daytime mean values of cloud susceptibility, as they observe susceptibility daily minima in the study region.

54 ENVIRONMENTAL SCIENCES↗

Mid-Atlantic US observations of radiocarbon in CO 2 : fossil and biogenic source partitioning and model evaluation

Accurately quantifying regional anthropogenic CO 2 fluxes is fundamental to improving our understanding of the carbon cycle and for creating effective carbon mitigation policies, and the radiocarbon to total carbon ratio in atmospheric CO 2 (Δ 14 CO 2 ) is a robust tracer of fossil fuel CO 2 that can discriminate between biogenic and fossil fuel CO 2 sources. NASA's Atmospheric Carbon and Transport-America (ACT-America) airborne mission between 2016 and 2019 aimed to improve the accuracy of regional greenhouse gas flux estimates, through refining our understanding and characterization of fluxes and flux uncertainties in models. Δ 14 CO 2 observations from 26 flights are presented for examining seasonal CO 2 source partitioning in the Mid-Atlantic USA. Observed variability in boundary layer CO 2 at timescales ranging from intra-day to seasonal was largely driven by biogenic CO 2 (CO 2bio ) variability that ranged from −19.7 ppm in summer to 16.2 ppm in fall, while fossil fuel CO 2 (CO 2ff ) variability remained at 3.3±2.0 ppm. Carbonyl sulfide uptake was well-correlated with CO 2bio uptake, and examining this relationship, as well as that between CO 2 and CO 2bio variability reinforces the seasonal extent of gross primary productivity response throughout ACT-America. We use airborne Δ 14 CO 2 flask sampling alongside in situ carbon monoxide measurements to calculate high-frequency CO 2ff and evaluate the magnitude and diurnal variability of modeled CO 2ff , deducing likely transport errors in an example flight. Although ACT-America CO 2ff signals were attenuated due to the broad source regions sampled, results illustrate the value of Δ 14 CO 2 sampling and observation-based methodologies for regional CO 2 flux attribution, evaluation and improvement of modeled CO 2 .

Baier, Bianca C. [National Oceanic and Atmospheric↗

Biomass burning aerosol radiative effects in the Southeast Atlantic depend strongly on meteorological forcing method

Biomass burning aerosols (BBAs) from African fires may strongly impact Earth’s radiation budget in the southeast Atlantic (SEA), but the sign and magnitude of the overall radiative effect (RE) remain uncertain. Aerosol–climate models are needed to separately quantify direct, indirect, and semi-direct REs. Here, we evaluate improved simulations with the UK Met Office's Unified Model and explore REs resulting from various methods used to match observed meteorology (nudging or running forecasts reinitialized at different frequencies). REs are calculated as differences in radiative fluxes between simulations with and without smoke emissions and with and without aerosol absorption. All model setups agree on net warming for the SEA dominated by the direct effect. Simulated smoke, clouds, and the direct effect agree better with observations than previous studies using the same model, though biases in aerosol extinction and liquid water path remain. Changes in cloud droplet number concentration due to BBA self-lofting influence how cleanly we can separate cloud effects into semi-direct and indirect effects. Total RE, which remains unaffected, ranges from +3.0 to +7.9 W m −2 . The 4.9 W m −2 spread arises mainly from simulated semi-direct effects. Forecasts three days long or less probably do not allow time for plausible differences in boundary layer properties due to semi-direct effects to accumulate. Free running simulations with and without smoke accumulate differences in meteorology that are likely spurious “butterfly effects”. We recommend future research quantifying BBA REs over weeks to months to use meteorological forcing techniques that allow aerosol absorption to affect the boundary layer.

Giuffrida, Eric [Carnegie Mellon University, Pitts↗

Regime-based aerosol–cloud interactions from CALIPSO-MODIS and the Energy Exascale Earth System Model version 2 (E3SMv2) over the Eastern North Atlantic

This study investigates aerosol-cloud interactions in marine boundary layer (MBL) clouds using an advanced deep-learning-driven synoptic-regime-based framework, combining satellite data (CALIPSO vertically resolved aerosol extinction and MODIS cloud properties) with 1° nudged Energy Exascale Earth System Model version 2 (E3SMv2) simulation over the Eastern North Atlantic (ENA; ∼10°×10°, 2006–2014). The E3SMv2 captures observed seasonal variations in cloud droplet number concentrations (N d ) and liquid water path (LWP), though it systematically underestimates N d . We then partition ENA meteorology into four synoptic regimes (Pre-Trough, Post-Trough, Ridge, Trough) via a deep-learning clustering of ERA5 reanalysis fields, enabling regime-dependent aerosol-cloud interactions analyses. Both satellite and E3SMv2 exhibit an inverted-V LWP-N d relationship. In Post-Trough and Ridge regimes, the satellite shows stronger negative LWP-N d sensitivities than in Pre-Trough regime. The Trough regime displays a muted satellite LWP response. In comparison, the model predicts more exaggerated LWP responses across regimes, with LWP increasing too quickly at low N d and decreasing more sharply at high N d , especially in Pre-Trough and Trough regimes. These exaggerated model LWP sensitivities may stem from uncertainties in representing drizzle processes, entrainment, and turbulent mixing. As for N d susceptibility to aerosols, N d increases with MBL aerosol extinction in both datasets, but the simulated aerosol-cloud interactions appear oversensitive to meteorological conditions. Overall, E3SMv2 better captures aerosol effects under regimes that favor stratiform clouds (Post-Trough, Ridge), but performance deteriorates for regimes with deeper, dynamically complex clouds (Trough), highlighting the need for improved representations of those cloud processes in climate models.

Environmental sciences↗

Cloud processing of dimethyl sulfide (DMS) oxidation products limits sulfur dioxide (SO 2 ) and carbonyl sulfide (OCS) production in the eastern North Atlantic marine boundary layer

Dimethyl sulfide (DMS) is the major sulfur species emitted from the ocean. The gas-phase oxidation of DMS by hydroxyl radicals proceeds through the stable, soluble intermediate hydroperoxymethyl thioformate (HPMTF), eventually forming carbonyl sulfide (OCS) and sulfur dioxide (SO 2 ). Recent work has shown that HPMTF is efficiently lost to marine boundary layer (MBL) clouds, thus arresting OCS and SO 2 production and their contributions to new-particle formation and growth events. To date, no long-term field studies exist to assess the extent to which frequent cloud processing impacts the fate of HPMTF. Here, we present 6 weeks of measurements of the cloud fraction and the marine sulfur species methanethiol, DMS, and HPMTF made at the Atmospheric Radiation Measurement (ARM) research facility on Graciosa Island, Azores, Portugal. Using an observationally constrained chemical box model, we determine that cloud loss is the dominant sink of HPMTF in this region of the MBL during the study, accounting for 79 %–91 % of HPMTF loss on average. When accounting for HPMTF uptake to clouds, we calculate campaign average reductions in DMS-derived MBL SO 2 and OCS of 52 %–60 % and 80 %–92 % for the study period. Using yearly measurements of the site- and satellite-measured 3D cloud fraction and DMS climatology, we infer that HPMTF cloud loss is the dominant sink of HPMTF in the eastern North Atlantic during all seasons and occurs on timescales faster than what is prescribed in global chemical transport models. Accurately resolving this rapid loss of HPMTF to clouds has important implications for constraining drivers of MBL new-particle formation.

54 ENVIRONMENTAL SCIENCES↗

Atmospheric processing and aerosol aging responsible for observed increase in absorptivity of long-range-transported smoke over the southeast Atlantic

Biomass burning aerosol (BBA) from agricultural fires in southern Africa contributes about one-third of the global carbonaceous aerosol load. These particles have strong radiative effects in the southeast Atlantic (SEA), which depend in part on the radiative contrast between the aerosol layer in the free troposphere (FT) and the underlying cloud layer. However, there is large disagreement in model estimates of aerosol-driven climate forcing due to uncertainties in the vertical distribution, optical properties, and life cycle of these particles. This study applies a novel method combining remote sensing observations with regional model outputs to investigate the aging of the BBA and its impact on the optical properties during transatlantic transport from emission sources in Africa to the SEA. Results show distinct variations in extinction Ångström exponent (EAE) and single-scattering albedo (SSA) as aerosols age. Near the source, fresh aerosols are characterized by low mean SSA (0.84) and high EAE (1.85), indicating smaller, highly absorbing particles. By isolating marine contributions from the total column during BBA transport across the SEA, our analysis reveals an initial decrease in BBA absorptivity, with mean FT SSA of 0.87 after 6–7 d, followed by increased absorptivity with mean FT SSA of 0.84 after 10 d, suggesting enhanced absorption due to chemical aging. These findings indicate that BBA becomes more absorbing during extended transport across the SEA, with implications for reducing model uncertainties. Our remote-sensing-based results agree well with previous in situ studies and offer new insights into aerosol–radiation interactions and the energy balance over the SEA.

54 ENVIRONMENTAL SCIENCES↗

Dust semi-direct effects: low-level cloud response to free-tropospheric dust-induced longwave radiation over the North Atlantic Ocean

Aerosol semi-direct effect is the adjustment of the radiative budget due to the cloud response to radiation absorption. Although dust accounts for about a third of aerosols' shortwave absorption, our understanding of its semi-direct effect often relies on traditional shortwave-focused mechanisms previously established for biomass-burning aerosols, and implications of dust longwave absorption on clouds have yet to be explored. Here, we assess the low-level cloud cover (LLCC) response to changes in properties and characteristics of the free-tropospheric dust layer over the North Atlantic Ocean (May–August, 2007–2017). We find that, consistent with previous studies, LLCC typically responds positively (increases in clouds) to an overlying dust layer. However, this response weakens with increasing dust optical depth (DOD), dust geometric thickness (DGT), and dust-layer base height (DBH). Specifically, we find that the LLCC response weakens by 4.3 ± 1.04 % and 1.6 ± 0.65 %, respectively, for a one-standard-deviation increase in DOD and DGT, and a smaller response to DBH (0.19 ± 0.45 %). We also find that the weakened LLCC response is primarily due to enhanced dust-induced longwave-dominated cloud-top warming, which counteracts the mean cloud-top cooling by as much as 19 % (mean of 9 %). Sensitivity analysis further indicates that the variability in dust properties, influenced by dust size distribution and refractive index, dominates the changes in dust-induced cloud-top warming, rather than variabilities in cloud properties or thermodynamic profiles. Our result adds to the traditional understanding of LLCC enhancement through shortwave-driven atmospheric stability, often associated with aerosol semi-direct effects, and highlights the role of dust-induced cloud-top longwave warming in dust semi-direct effects.

Pandey, Satyendra K. [Univ. of California, Merced,↗

Offshore wind energy forecasting sensitivity to sea surface temperature input in the Mid-Atlantic

Abstract. As offshore wind farm development expands, accurate wind resource forecasting over the ocean is needed. One important yet relatively unexplored aspect of offshore wind resource assessment is the role of sea surface temperature (SST). Models are generally forced with reanalysis data sets, which employ daily SST products. Compared with observations, significant variations in SSTs that occur on finer timescales are often not captured. Consequently, shorter-lived events such as sea breezes and low-level jets (among others), which are influenced by SSTs, may not be correctly represented in model results. The use of hourly SST products may improve the forecasting of these events. In this study, we examine the sensitivity of model output from the Weather Research and Forecasting model (WRF) 4.2.1 to different SST products. We first evaluate three different data sets: the Multiscale Ultrahigh Resolution (MUR25) SST analysis, a daily, 0.25∘ × 0.25∘ resolution product; the Operational Sea Surface Temperature and Ice Analysis (OSTIA), a daily, 0.054∘ × 0.054∘ resolution product; and SSTs from the Geostationary Operational Environmental Satellite 16 (GOES-16), an hourly, 0.02∘ × 0.02∘ resolution product. GOES-16 is not processed at the same level as OSTIA and MUR25; therefore, the product requires gap-filling using an interpolation method to create a complete map with no missing data points. OSTIA and GOES-16 SSTs validate markedly better against buoy observations than MUR25, so these two products are selected for use with model simulations, while MUR25 is at this point removed from consideration. We run the model for June and July of 2020 and find that for this time period, in the Mid-Atlantic, although OSTIA SSTs overall validate better against in situ observations taken via a buoy array in the area, the two products result in comparable hub-height (140 m) wind characterization performance on monthly timescales. Additionally, during hours-long flagged events (< 30 h each) that show statistically significant wind speed deviations between the two simulations, both simulations once again demonstrate similar validation performance (differences in bias, earth mover's distance, correlation, and root mean square error on the order of 10−1 or less), with GOES-16 winds validating nominally better than OSTIA winds. With a more refined GOES-16 product, which has been not only gap-filled but also assimilated with in situ SST measurements in the region, it is likely that hub-height winds characterized by GOES-16-informed simulations would definitively validate better than those informed by OSTIA SSTs.

17 WIND ENERGY↗

Seasonal variability of wake impacts on US mid-Atlantic offshore wind plant power production

Abstract. The mid-Atlantic will experience rapid wind plant development due to its promising wind resource located near large population centers. Wind turbines and wind plants create wakes, or regions of reduced wind speed, that may negatively affect downwind turbines and plants. We evaluate wake variability and annual energy production with the first yearlong modeling assessment using the Weather Research and Forecasting model, deploying 12 MW turbines across the domain at a density of 3.14 MW km−2, matching the planned density of 3 MW km−2. Using a series of simulations with no wind plants, one wind plant, and complete build-out of lease areas, we calculate wake effects and distinguish the effect of wakes generated internally within one plant from those generated externally between plants. We also provide a first step towards uncertainty quantification by testing the amount of added turbulence kinetic energy (TKE) by 0 % and 100 %. We provide a sensitivity analysis by additionally comparing 25 % and 50 % for a short case study period. The strongest wakes, propagating 55 km, occur in summertime stable stratification, just when New England's grid demand peaks in summer. The seasonal variability of wakes in this offshore region is much stronger than the diurnal variability of wakes. Overall, yearlong simulated wake impacts reduce power output by a range between 38.2 % and 34.1 % (for 0 %–100 % added TKE). Internal wakes cause greater yearlong power losses, from 29.2 % to 25.7 %, compared to external wakes, from 14.7 % to 13.4 %. The overall impact is different from the linear sum of internal wakes and external wakes due to non-linear processes. Additional simulations quantify wake uncertainty by modifying the added amount of turbulent kinetic energy from wind turbines, introducing power output variability of 3.8 %. Finally, we compare annual energy production to New England grid demand and find that the lease areas can supply 58.8 % to 61.2 % of annual load. We note that the results of this assessment are not intended to make nor are they suitable to make commercial judgments about specific wind projects.

17 WIND ENERGY↗