Atmospheric Radiation Measurement Research Articles

Aerosol Vertical Turbulent Mass Flux Retrievals Through Novel Remote Sensing Algorithm

AbstractIntegrated measurements of aerosol, radiation, cloud, and turbulent transport in the planetary boundary layer (PBL) are essential for understanding and modeling climate and air quality. Here, we developed a new technique for the identification of convective turbulent regions and deriving the vertical distribution of aerosol turbulent mass fluxes within PBL. The algorithm uses retrievals from coherent Doppler lidars and a high spectral resolution lidar. The technique was applied to study particle mass fluxes over 2 months (November–December 2020) during the campaign conducted at the DOE Atmospheric Radiation Measurement Southern Great Plains (SGP) site in Lamont, Oklahoma. The algorithm developed here is capable of continuously deriving vertically resolved (curtains) aerosol mass fluxes. Our data analysis shows that at the site, the 30‐min averaged fluxes at 135 m above the surface were mainly positive (upward) at ∼1 μg m−2 s−1, suggesting that the surface is the primary source of the particle mass supplied to the boundary layer at the SGP site. Analyses of the individual case studies have revealed that not all the derived fluxes can be linked to surface emissions. Both positive and negative values in a range of ±5 μg m−2 s−1 can be caused by convective thermals interacting between the residual layer and the mixed layer and by rotation of the horizontal wind with the height. Large erroneous negative fluxes can also be caused by drizzling/precipitating clouds. We anticipate that the application of the current technique will lead to a more realistic representation of aerosol mass budgets and bidirectional mixing rates.

Principles of stereo reconstruction of aerial objects using stationary cameras

ABSTRACT An overview is given here of the principles and mathematics of stereo reconstruction of objects in the sky using stationary cameras with an emphasis on meteorological applications. Through its Atmospheric Radiation Measurement program, the Department of Energy has operated stereo-photogrammetric cameras since 2017 as part of an effort to measure the life-cycle properties of clouds. At the core of that technology is stereo reconstruction, which calculates the real-world position of an object from the location of the object’s image in two cameras’ photographs. Here, stereo reconstruction is stripped down to its basic elements and presented using conventions tailored to applications in atmospheric science. In addition, the resulting equations are used to illustrate the high sensitivity of reconstructed cloud positions to errors in the cameras’ Euler angles. The interested reader will find here a self-contained guide to performing stereo reconstructions using distortion-corrected images from a pair of calibrated, stationary cameras, as well as a demonstration of the need for high accuracy in the measurement of camera properties and orientations.

Simulating Mixed‐Phase Open Cellular Clouds Observed During COMBLE: Evaluation of Parameterized Turbulence Closure

AbstractMarine cold‐air outbreaks, or CAOs, are airmass transformations whereby relatively cold boundary layer (BL) air is transported over relatively warm water. To more deeply understand BL and mixed‐phase cloud properties during CAO conditions, the Cold‐Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) took place from late 2019 into early 2020. During COMBLE, the U.S. Department of Energy's first Atmospheric Radiation Measurement Mobile Facility (AMF1) was deployed to Andenes, Norway, far downstream (∼1,000 km) from the Arctic pack ice. This study examines the two most intense CAOs sampled at the AMF1 site. The observed BL structures are open cellular with high (∼3–5 km) and cold (−30 to −50 C) cloud tops, and they often have pockets of high liquid water paths (LWPs; up to ∼1,000 g ) associated with strong updrafts and enhanced turbulence. We use a high‐resolution mesoscale model to explore how well four turbulence closure methods represent open cellular clouds. After applying a radar simulator to model outputs for direct evaluation, cloud top properties agree well with AMF1 observations (within ∼10%), but radar reflectivity and LWP agreement is more variable. Results suggest that the turbulent Prandtl number may play an important role for the simulated BL and cloud properties. All simulations produce enhanced precipitation rates that are well‐correlated with a cloud transition. Finally, the eddy‐diffusivity/mass‐flux approach produces the deepest cloud layer and therefore the largest and most coherent cellular structures. We recommend the use of a non‐local turbulence closure approach to better capture turbulent processes in intense CAOs.

TAMU TRACER: Targeted Mobile Measurements to Isolate the Impacts of Aerosols and Meteorology on Deep Convection

Abstract Difficulty in using observations to isolate the impacts of aerosols from meteorology on deep convection often stems from the inability to resolve the spatiotemporal variations in the environment serving as the storm’s inflow region. During the U.S. Department of Energy (DOE) Tracking Aerosol Convection interactions Experiment (TRACER) in June–September 2022, a Texas A&M University (TAMU) team conducted a mobile field campaign to characterize the meteorological and aerosol variability in air masses that serve as inflow to convection across the ubiquitous mesoscale boundaries associated with the sea and bay breezes in the Houston, Texas, region. These boundaries propagate inland over the fixed DOE Atmospheric Radiation Measurement (ARM) sites. However, convection occurs on either or both the continental or maritime sides or along the boundary. The maritime and continental air masses serving as convection inflow may be quite distinct, with different meteorological and aerosol characteristics that fixed-site measurements cannot simultaneously sample. Thus, a primary objective of TAMU TRACER was to provide mobile measurements similar to those at the fixed sites, but in the opposite air mass across these moving mesoscale boundaries. TAMU TRACER collected radiosonde, lidar, aerosol, cloud condensation nuclei (CCN), and ice nucleating particle (INP) measurements on 29 enhanced operations days covering a variety of maritime, continental, outflow, and prefrontal air masses. This paper summarizes the TAMU TRACER deployment and measurement strategy, instruments, and available datasets and provides sample cases highlighting differences between these mobile measurements and those made at the ARM sites. We also highlight the exceptional TAMU TRACER undergraduate student participation in high-impact learning activities through forecasting and field deployment opportunities.

Overview of preparation for the American WAKE ExperimeNt (AWAKEN)

The American WAKE ExperimeNt (AWAKEN) is a multi-institutional field campaign focused on gathering critical observations of wind farm–atmosphere interactions. These interactions are responsible for a large portion of the uncertainty in wind plant modeling tools that are used to represent wind plant performance both prior to construction and during operation and can negatively impact wind energy profitability. The AWAKEN field campaign will provide data for validation, ultimately improving modeling and lowering these uncertainties. The field campaign is designed to address seven testable hypotheses through the analysis of the observations collected by numerous instruments at 13 ground-based locations and on five wind turbines. The location of the field campaign in Northern Oklahoma was chosen to leverage existing observational facilities operated by the U.S. Department of Energy Atmospheric Radiation Measurement program in close proximity to five operating wind plants. The vast majority of the observations from the experiment are publicly available to researchers and industry members worldwide, which the authors hope will advance the state of the science for wind plants and lead to lower cost and increased reliability of wind energy systems.

Deep-learning-driven simulations of boundary layer clouds over the Southern Great Plains

Abstract. Based on long-term observations at the Southern Great Plains site by the Atmospheric Radiation Measurement (ARM) program for training and validation, a deep-learning model is developed to simulate the daytime evolution of boundary layer clouds (BLCs) from the perspective of land–atmosphere coupling. The model takes ARM measurements (including early-morning soundings and diurnally varying surface meteorological conditions and heat fluxes) as inputs and predicts hourly estimates (including cloud occurrence, the positions of cloud boundaries, and the vertical profile of the cloud fraction) as outputs. The deep-learning model offers good agreement with the observed cloud fields, especially in the accuracy with which cloud occurrence and base height are reproduced. When the inputs are substituted by reanalysis data from ERA5 and MERRA-2, the outputs of the deep-learning model provide a better agreement with observation than the cloud fields extracted from ERA5 and MERRA-2 themselves. Thus, the deep-learning model shows great potential to serve as a diagnostic tool for the performance of physics-based models in simulating stratiform and cumulus clouds. By quantifying biases in clouds and attributing them to the simulated atmospheric state variables versus the model-parameterized cloud processes, this observation-based deep-learning model may offer insights into the directions needed to improve the simulation of BLCs in physics-based models for weather forecasting and climate prediction.

How Well Does the DOE Global Storm Resolving Model Simulate Clouds and Precipitation Over the Amazon?

AbstractThis study assesses a 40‐day 3.25‐km global simulation of the Simple Cloud‐Resolving E3SM Model (SCREAMv0) using high‐resolution ground‐based observations from the Atmospheric Radiation Measurement (ARM) Green Ocean Amazon (GoAmazon) field campaign. SCREAMv0 reasonably captures the diurnal timing of boundary layer clouds yet underestimates the boundary layer cloud fraction and mid‐level congestus. SCREAMv0 well replicates the precipitation diurnal cycle, however it exhibits biases in the precipitation cluster size distribution compared to scanning radar observations. Specifically, SCREAMv0 overproduces clusters smaller than 128 km, and does not form enough large clusters. Such biases suggest an inhibition of convective upscale growth, preventing isolated deep convective clusters from evolving into larger mesoscale systems. This model bias is partially attributed to the misrepresentation of land‐atmosphere coupling. This study highlights the potential use of high‐resolution ground‐based observations to diagnose convective processes in global storm resolving model simulations, identify key model deficiencies, and guide future process‐oriented model sensitivity tests and detailed analyses.

Iterative Error‐Driven Ensemble Labeling (IEDEL) Algorithm for Enhanced Data Quality Control for the Atmospheric Radiation Measurement (ARM) Program User Facility

AbstractFor over three decades, the Atmospheric Radiation Measurement (ARM) Program user facility has provided researchers with invaluable benchmark atmospheric data. Ensuring the accuracy and integrity of ARM data is vital, and to achieve this, the ARM Data Quality Office (DQO) has implemented customized quality control tests tailored to each variable, with guidance from instrument mentors. These tests are designed to pinpoint common issues, such as data exceeding valid ranges or persisting with little change over extended periods, and ARM offers tools for users to review and exclude contaminated data efficiently. However, certain quality issues, such as spikes in time series or data drift over time, sometimes evade detection by existing tests and require manual identification by data analysts and instrument mentors through visualization tools. To tackle these challenges more efficiently, the DQO has developed and implemented the Iterative Error‐Driven Ensemble Labeling (IEDEL) algorithm with unanimous voting and transfer learning techniques to efficiently generate labeled data at scale. This initiative has empowered the creation of high‐performing machine learning models, enabling real‐time monitoring of data quality issues within the ARM data and thereby enhancing data integrity and accessibility.

Mechanical and Thermal Forcing for Upslope Flows and Cumulus Convection over the Sierras de Córdoba

Abstract The upslope flow processes affecting the vertical extent of orographic cumulus convection are examined using observations from the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) Field Campaign. Specifically, clear-air returns from the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) C-band radar (CSAPR2) are used to characterize the structure and variability of the ridge-normal (i.e., up/downslope) flow components, which transport mass to the crest of Argentina’s Sierras de Córdoba and contribute to convective initiation. Data are compiled for the entire CACTI period (Oct-Apr), including days with clear skies, shallow cumuli, cumulus congestus, and deep convection. To examine shared variability amongst >70,000 radar scans we use (a) a principal component analysis (PCA) to isolate modes of variability in the upslope flow, and (b) composite analysis based on convective outcomes, determined from GOES16 satellite observations. These data are contextualized with observed surface sensible heat fluxes, thermodynamic profiles, and synoptic-scale analysis. Results indicate distinct thermally and mechanically forced upslope flow modes, modulated by diurnal heating and synoptic-scale variations, respectively. In some instances, there is a superposition of thermal and mechanical forcing, yielding either deeper or shallower upslope flow. The composite analyses based on satellite data show that successively deeper convective outcomes are associated with successively deeper upslope flow layers that more readily transport mass to the ridge crest in conjunction with lower lifting condensation levels, facilitating convective initiation. These results help to isolate the forcing mechanisms for orographic convection, and thus provide a foundation for parameterizing orographic convective processes in coarse resolution models.

Refining Planetary Boundary Layer Height Retrievals From Micropulse‐Lidar at Multiple ARM Sites Around the World

AbstractKnowledge of the planetary boundary layer height (PBLH) is crucial for various applications in atmospheric and environmental sciences. Lidar measurements are frequently used to monitor the evolution of the PBLH, providing more frequent observations than traditional radiosonde‐based methods. However, lidar‐derived PBLH estimates have substantial uncertainties, contingent upon the retrieval algorithm used. In addressing this, we applied the Different Thermo‐Dynamic Stabilities (DTDS) algorithm to establish a PBLH data set at five separate Department of Energy's Atmospheric Radiation Measurement sites across the globe. Both the PBLH methodology and the products are subject to rigorous assessments in terms of their uncertainties and constraints, juxtaposing them with other products. The DTDS‐derived product consistently aligns with radiosonde PBLH estimates, with correlation coefficients exceeding 0.77 across all sites. This study delves into a detailed examination of the strengths and limitations of PBLH data sets with respect to both radiosonde‐derived and other lidar‐based estimates of the PBLH by exploring their respective errors and uncertainties. It is found that varying techniques and definitions can lead to diverse PBLH retrievals due to the inherent intricacy and variability of the boundary layer. Our DTDS‐derived PBLH data set outperforms existing products derived from ceilometer data, offering a more precise representation of the PBLH. This extensive data set paves the way for advanced studies and an improved understanding of boundary‐layer dynamics, with valuable applications in weather forecasting, climate modeling, and environmental studies.

Evaluation of the hyperspectral radiometer (HSR1) at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site

Abstract. The Peak Design Ltd hyperspectral radiometer (HSR1) was tested at the Atmospheric Radiation Measurement (ARM) user facility Southern Great Plains (SGP) site in Lamont, Oklahoma, for 2 months from May to July 2022. The HSR1 is a prototype instrument that measures total (Ftotal) and diffuse (Fdiffuse) spectral irradiance from 360 to 1100 nm with a spectral resolution of 3 nm. The HSR1 spectral irradiance measurements are compared to nearby collocated spectral radiometers, including two multifilter rotating shadowband radiometers (MFRSRs) and the Shortwave Array Spectroradiometer–Hemispheric (SASHe) radiometer. The Ftotal at 500 nm for the HSR1 compared to the MFRSRs has a mean (relative) difference of 0.01 W m−2 nm−1 (1 %–2 %). The HSR1 mean Fdiffuse at 500 nm is smaller than the MFRSRs' by 0.03–0.04 (10 %) W m−2 nm−1. The HSR1 clear-sky aerosol optical depth (AOD) is also retrieved by considering Langley regressions and compared to collocated instruments such as the Cimel sunphotometer (CSPHOT), MFRSRs, and SASHe. The mean HSR1 AOD at 500 nm is larger than the CSPHOT's by 0.010 (8 %) and larger than the MFRSRs' by 0.007–0.017 (6 %–18 %). In general, good agreement between the HSR1 and other instruments is found in terms of the Ftotal, Fdiffuse, and AODs at 500 nm. The HSR1 quantities are also compared at other wavelengths to the collocated instruments. The comparisons are within ∼ 10 % for the Ftotal and Fdiffuse, except for 940 nm, where there is relatively larger disagreement. The AOD comparisons are within ∼ 10 % at 415 and 440 nm; however, a relatively larger disagreement in the AOD comparison is found for higher wavelengths.

Broadband and filter radiometers at Ross Island, Antarctica: detection of cloud ice phase versus liquid water influences on shortwave and longwave radiation

Abstract. Surface radiometer data from Ross Island, Antarctica, collected during the austral summer 2015–2016 by the US Department of Energy Atmospheric Radiation Measurement (ARM) program West Antarctic Radiation Experiment (AWARE), are used to evaluate how shortwave and longwave irradiance respond to changing cloud properties as governed by contrasting meteorological regimes. Shortwave atmospheric transmittance is derived from pyranometer measurements, and cloud conservative-scattering optical depth is derived from filter radiometer measurements at 870 nm. With onshore flow associated with marine air masses, clouds contain mostly liquid water. With southerly flow over the Transantarctic Mountains, orographic forcing induces substantial cloud ice water content. These ice and mixed-phase clouds attenuate more surface shortwave irradiance than the maritime-influenced clouds and also emit less longwave irradiance due to colder cloud base temperature. These detected irradiance changes are in a range that can mean onset or inhibition of surface melt over ice shelves. This study demonstrates how basic and relatively low-cost broadband and filter radiometers can be used to detect subtle climatological influences of contrasting cloud microphysical properties at very remote locations.

Aerosol-induced closure of marine cloud cells: enhanced effects in the presence of precipitation

Abstract. The Weather Research Forecasting (WRF) version 4.3 model is configured within a Lagrangian framework to quantify the impact of aerosols on evolving cloud fields. Kilometer-scale simulations utilizing meteorological boundary conditions are based on 10 case study days offering diverse meteorology during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA). Measurements from aircraft, the ground-based Atmosphere Radiation Measurement (ARM) site at Graciosa Island in the Azores, and A-Train and geostationary satellites are utilized for validation, demonstrating good agreement with the WRF-simulated cloud and aerosol properties. Higher aerosol concentration leads to suppressed drizzle and increased cloud water content in all case study days. These changes lead to larger radiative cooling rates at cloud top, enhanced vertical velocity variance, and increased vertical and horizontal wind speed near the base of the lower-tropospheric inversion. As a result, marine cloud cell area expands, narrowing the gap between shallow clouds and increasing cloud optical thickness, liquid water content, and the top-of-atmosphere outgoing shortwave flux. While similar aerosol effects are observed in lightly to non-raining clouds, they tend to be smaller by comparison. These simulations show a relationship between cloud cell area expansion and the radiative adjustments caused by liquid water path and cloud fraction changes. The adjustments are positive and scale as 74 % and 51 %, respectively, relative to the Twomey effect. While higher-resolution large-eddy simulations may provide improved representation of cloud-top mixing processes, these results emphasize the importance of addressing mesoscale cloud-state transitions in the quantification of aerosol radiative forcing that cannot be attained from traditional climate models.

Cloud micro- and macrophysical properties from ground-based remote sensing during the MOSAiC drift experiment.

In the framework of the Multidisciplinary drifting Observatory for the Study of Arctic Climate Polarstern expedition, the Leibniz Institute for Tropospheric Research, Leipzig, Germany, operated the shipborne OCEANET-Atmosphere facility for cloud and aerosol observations throughout the whole year. OCEANET-Atmosphere comprises, amongst others, a multiwavelength Raman lidar, a microwave radiometer, and an optical disdrometer. A cloud radar was operated aboard Polarstern by the US Atmospheric Radiation Measurement program. These measurements were processed by applying the so-called Cloudnet methodology to derive cloud properties. To gain a comprehensive view of the clouds, lidar and cloud radar capabilities for low- and high-altitude observations were combined. Cloudnet offers a variety of products with a spatiotemporal resolution of 30 s and 30 m, such as the target classification, and liquid and ice microphysical properties. Additionally, a lidar-based low-level stratus retrieval was applied for cloud detection below the lowest range gate of the cloud radar. Based on the presented dataset, e.g., studies on cloud formation processes and their radiative impact, and model evaluation studies can be conducted.

Ozone Monitoring Spectrometer-Limb observation (OMSL) on-orbit polarization correction for atmospheric radiation measurements

OMSL is a passive, space-based spectrometer designed to obtain the vertical profiles of trace gases such as ozone, by measuring atmospheric radiation in limb-viewing mode. Due to the presence of internal components such as gratings and dichroic mirror, OMSL is sensitive to polarization of incident light, which can lead to errors in the radiometric measurements, especially when the incident light is fully polarized. To eliminate the errors, an on-orbit polarization correction method is applied to OMSL. The key to this method is to calculate the polarization correction factor by combining the on-orbit polarization measurement and the pre-flight polarization calibration. In this paper, the on-orbit polarization correction method is introduced in detail. Furthermore, the first results of the on-orbit correction are analyzed and compared with simulation of the SCIATRAN.

62°S Witnesses the Transition of Boundary Layer Marine Aerosol Pattern Over the Southern Ocean (50°S–68°S, 63°E–150°E) During the Spring and Summer: Results From MARCUS (I)

AbstractThe Atmospheric Radiation Measurement Mobile Facility‐2 was installed onboard the research vessel Aurora Australis to measure aerosol properties during the 2017–2018 Measurement of Aerosols, Radiation, and CloUds over the pristine Southern ocean (MARCUS) Experiment, providing unique data on aerosols latitudinal and seasonal variation, including south of 60°S where previous observations are scarce. Data from a Cloud Condensation Nuclei (CCN) counter and Ultra‐High‐Sensitivity Aerosol Spectrometer show that both the number concentration (NCCN) and size distribution of CCN‐active aerosols, with diameters (D) between 60 nm < D < 1,000 nm are different over the North Southern Ocean (NSO) (50°S–60°S) and the South Southern Ocean (SSO) (62°S–68°S). The average NSO NCCN at 0.2% and 0.5% supersaturation were 28% and 49% less than that over the SSO. This increase of CCN over the SSO is caused by the increase of aerosols with 60 nm < D < 200 nm, consistent with calculations of Aerosol Scattering Angstrom Exponents derived from a nephelometer. Aerosol hygroscopicity growth factor measured by the Hygroscopic Tandem Differential Mobility Analyzer stayed close to 1.41 for aerosols with 50 nm < D < 250 nm over the SSO, but increased from 1.30 to 1.67 over the NSO, indicating different chemical compositions. Both CCN and Ice Nucleating Particles (INPs) showed a stronger variation with season than with latitude. The variation of heat‐labile and presumably proteinacous INPs suggests an increase of ice nucleating‐active microbes in summer.

Extending the wind profile beyond the surface layer by combining physical and machine learning approaches

Abstract. Accurate estimation of the wind profile, especially in the lowest few hundred meters of the atmosphere, is of great significance for the weather, climate, and renewable energy sector. Nevertheless, the Monin–Obukhov similarity theory fails above the surface layer over a heterogeneous underlying surface, causing an unreliable wind profile to be obtained from conventional extrapolation methods. To solve this problem, we propose a novel method called the PLM-RF method that combines the power-law method (PLM) with the random forest (RF) algorithm to extend wind profiles beyond the surface layer. The underlying principle is to treat the wind profile as a power-law distribution in the vertical direction, with the power-law exponent (α) determined by the PLM-RF model. First, the PLM-RF model is constructed based on the atmospheric sounding data from 119 radiosonde (RS) stations across China and in conjunction with other data such as surface wind speed, land cover type, surface roughness, friction velocity, geographical location, and meteorological parameters from June 2020 to May 2021. Afterwards, the performance of the PLM-RF, PLM, and RF methods over China is evaluated by comparing them with RS observations. Overall, the wind speed at 100 m from the PLM-RF model exhibits high consistency with RS measurements, with a determination coefficient (R2) of 0.87 and a root mean squared error (RMSE) of 0.92 m s−1. By contrast, the R2 and RMSE of wind speed results from the PLM (RF) method are 0.75 (0.83) and 1.37 (1.04) m s−1, respectively. This indicates that the estimates from the PLM-RF method are much closer to observations than those from the PLM and RF methods. Moreover, the RMSE of the wind profiles estimated by the PLM-RF model is relatively large for highlands, while it is small for plains. This result indicates that the performance of the PLM-RF model is affected by the terrain factor. Finally, the PLM-RF model is applied to three atmospheric radiation measurement sites for independent validation, and the wind profiles estimated by the PLM-RF model are found to be consistent with Doppler wind lidar observations. This confirms that the PLM-RF model has good applicability. These findings have great implications for the weather, climate, and renewable energy sector.

Chemical properties and single-particle mixing state of soot aerosol in Houston during the TRACER campaign

Abstract. A high-resolution soot particle aerosol mass spectrometer (SP-AMS) was used to selectively measure refractory black carbon (rBC) and its associated coating material using both the ensemble size-resolved mass spectral mode and the event trigger single particle (ETSP) mode in Houston, Texas, in summer 2022. This study was conducted as part of the Department of Energy Atmospheric Radiation Measurement (ARM) program's TRacking Aerosol Convection interactions ExpeRiment (TRACER) field campaign. The study revealed an average (±1σ) rBC concentration of 103 ± 176 ng m−3. Additionally, the coatings on the BC particles were primarily composed of organics (59 %; 219 ± 260 ng m−3) and sulfate (26 %; 94 ± 55 ng m−3). Positive matrix factorization (PMF) analysis of the ensemble mass spectra of BC-containing particles resolved four distinct types of soot aerosol, including an oxidized organic aerosol (OOABC,PMF) factor associated with processed primary organic aerosol, an inorganic sulfate factor (SO4,BC,PMF), an oxidized rBC factor (O-BCPMF), and a mixed mineral dust–biomass burning aerosol factor with significant contribution from potassium (K-BBBC,PMF). Additionally, K-means clustering analysis of the single-particle mass spectra identified eight different clusters, including soot particles enriched in hydrocarbon-like organic aerosol (HOABC,ETSP), sulfate (SO4,BC,ETSP), two types of rBC, OOA (OOABC,ETSP), chloride (ClBC,ETSP), and nitrate (NO3,BC,ETSP). The single-particle measurements demonstrate substantial variation in BC coating thickness with coating-to-rBC mass ratios ranging from 0.1 to 100. The mixing state index (χ), which denotes the degree of homogeneity of the soot aerosol, varied from 4 % to 94 % with a median of 40 %, indicating that the aerosol population lies in between internal and external mixing but has large temporal and source type variability. In addition, a significant fraction of BC-containing particles, a majority enriched with oxidized organics and sulfate, exhibit sufficiently high κ values and diameters conducive to activation as cloud nuclei under atmospherically relevant supersaturation conditions. This finding bears significance in comprehending the aging processes of rBC-containing particles and their activation into cloud droplets. Our analysis highlights the complex nature of soot aerosol and underscores the need to comprehend its variability across different environments for accurate assessment of climate change.

Assessing Radiative Impacts of African Smoke Aerosols Over the Southeastern Atlantic Ocean

AbstractBiomass burning smoke aerosols are efficient at attenuating incoming solar radiation. The Layered Atlantic Smoke Interactions with Clouds campaign was conducted from June 2016 to October 2017. The U. S. Department of Energy mobile Atmospheric Radiation Measurement site located on Ascension Island (AMF‐ASI) identified several instances of smoke plume intrusions. Increases in surface and column measurements of aerosol loading were directly related to increases in fine mode fraction, number concentrations of aerosols (Na), and cloud condensation nuclei (NCCN). During periods of weak lower tropospheric stability, smoke particles were more likely to be advected downward either by boundary layer turbulence or cloud top entrainment under non‐overcast sky conditions. Backward trajectory analysis illustrated that smoke aerosols reaching the AMF‐ASI site were fine mode, less aged, strongly absorbing, and had shorter boundary layer trajectories while longer boundary layer trajectories denoted mixtures of weakly absorbing smoke and coarse mode marine aerosols. The most polluted smoke cases of August 2016 and 2017 revealed a notable contrast in radiative forcing per unit aerosol optical depth or radiative forcing efficiency (ΔFeff) at the top of the atmosphere (TOA) and near‐surface (BOA). The weakly (strongly) absorbing 2016 cases exhibited weaker (stronger) ΔFeff at the TOA and BOA suggesting a warming (cooling) effect within the boundary layer. The 2017 cases featured the strongest ΔFeff suggesting more of a cooling effect at the TOA and BOA due to mixing of fresh smoke with marine aerosols during transport.

The Physics behind Precipitation Onset Bias in CMIP6 Models: The Pseudo-Entrainment Diagnostic and Trade-Offs between Lapse Rate and Humidity

Abstract Conditional instability and the buoyancy of plumes drive moist convection but have a variety of representations in model convective schemes. Vertical thermodynamic structure information from Atmospheric Radiation Measurement (ARM) sites and reanalysis (ERA5), satellite-derived precipitation (TRMM3b42), and diagnostics relevant for plume buoyancy are used to assess climate models. Previous work has shown that CMIP6 models represent moist convective processes more accurately than their CMIP5 counterparts. However, certain biases in convective onset remain pervasive among generations of CMIP modeling efforts. We diagnose these biases in a cohort of nine CMIP6 models with subdaily output, assessing conditional instability in profiles of equivalent potential temperature, θe, and saturation equivalent potential temperature, θes, in comparison to a plume model with different mixing assumptions. Most models capture qualitative aspects of the θes vertical structure, including a substantial decrease with height in the lower free troposphere associated with the entrainment of subsaturated air. We define a “pseudo-entrainment” diagnostic that combines subsaturation and a θes measure of conditional instability similar to what entrainment would produce under the small-buoyancy approximation. This captures the trade-off between larger θes lapse rates (entrainment of dry air) and small subsaturation (permits positive buoyancy despite high entrainment). This pseudo-entrainment diagnostic is also a reasonable indicator of the critical value of integrated buoyancy for precipitation onset. Models with poor θe/θes structure (those using variants of the Tiedtke scheme) or low entrainment runs of CAM5, and models with low subsaturation, such as NASA-GISS, lie outside the observational range in this diagnostic.