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DOE OSTI2023

Airborne flux measurements of ammonia over the southern Great Plains using chemical ionization mass spectrometry

Abstract. Ammonia (NH3) is an abundant trace gas in the atmosphere and an important player in atmospheric chemistry, aerosol formation and the atmosphere–surface exchange of nitrogen. The accurate determination of NH3 emission rates remains a challenge, partly due to the propensity of NH3 to interact with instrument surfaces, leading to high detection limits and slow response times. In this paper, we present a new method for quantifying ambient NH3, using chemical ionization mass spectrometry (CIMS) with deuterated benzene cations as reagents. The setup aimed at limiting sample–surface interactions and achieved a 1σ precision of 10–20 pptv and an immediate 1/e response rate of < 0.4 s, which compares favorably to the existing state of the art. The sensitivity exhibited an inverse humidity dependence, in particular in relatively dry conditions. Background of up to 10 % of the total signal required consideration as well, as it responded on the order of a few minutes. To showcase the method's capabilities, we quantified NH3 mixing ratios from measurements obtained during deployment on a Gulfstream I aircraft during the HI-SCALE (Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems) field campaign in rural Oklahoma during May 2016. Typical mixing ratios were 1–10 parts per billion by volume (ppbv) for the boundary layer and 0.1–1 ppbv in the lower free troposphere. Sharp plumes of up to tens of ppbv of NH3 were encountered as well. We identified two of their sources as a large fertilizer plant and a cattle farm, and our mixing ratio measurements yielded upper bounds of 350 ± 50 and 0.6 kg NH3 h−1 for their respective momentary source rates. The fast response of the CIMS also allowed us to derive vertical NH3 fluxes within the turbulent boundary layer via eddy covariance, for which we chiefly used the continuous wavelet transform technique. As expected for a region dominated by agriculture, we observed predominantly upward fluxes, implying net NH3 emissions from the surface. The corresponding analysis focused on the most suitable flight, which contained two straight-and-level legs at ∼ 300 m above ground. We derived NH3 fluxes between 1 and 11 mol km−2 h−1 for these legs, at an effective spatial resolution of 1–2 km. The analysis demonstrated how flux measurements benefit from suitably arranged flight tracks with sufficiently long straight-and-level legs, and it explores the detrimental effect of measurement discontinuities. Following flux footprint estimations, comparison to the NH3 area emissions inventory provided by the U.S. Environmental Protection Agency indicated overall agreement but also the absence of some sources, for instance the identified cattle farm. Our study concludes that high-precision CIMS measurements are a powerful tool for in situ measurements of ambient NH3 mixing ratios, and even allow for the airborne mapping of the air–surface exchange of NH3.

58 GEOSCIENCES↗

DOE OSTI2023

Multi-scale Analysis of Surface Heterogeneity Induced Convection on Isentropic Coordinates

This research uses semi-idealized simulations to investigate multi-scale processes induced by the heterogeneity of soil moisture observed during the 2016 Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) field campaign. The semi-idealized simulations have realistic land heterogeneity, but large-scale winds are removed. Analysis on isentropic coordinates enables the tracking of circulation that transports energy vertically and facilitates the identification of the primary convective processes induced by realistic land heterogeneity. The isentropes associated with upward motion are found to connect the ground characterized by high latent heat flux to cloud bases directly over the ground with high sensible heat flux, while isentropes associated with downward motion connect precipitation to the ground characterized by high sensible heat fluxes. The mixing of dry, warm parcels ascending from the ground with high sensible heat fluxes and moist parcels from high latent heat regions leads to cloud formation. This new mechanism explains how soil moisture heterogeneity provides the key ingredients such as buoyancy and moisture for shallow cloud formation. We also found that the sub-mesoscale dominates upward energy transport in the boundary layer, while mesoscale circulations contribute to vertical energy transport above the boundary layer. Our novel method better illustrates and elucidates the nature of land atmospheric interactions under irregular and realistic soil moisture patterns.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

EPCAPE-Dalhousie Field Campaign Report

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

EPCAPE-Dalhousie Field Campaign Report

This project supported the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), which aimed to characterize the extent, radiative properties, aerosol interactions, and precipitation of stratocumulus clouds in the Eastern Pacific coastal region of La Jolla, California. Given the frequent anthropogenic aerosols emitted into this region, characterization of this important coastal cloud region and the aerosol impact on the cloud characteristics will improve the understanding of aerosol indirect effects and its representation in global climate models. This specific project deployed the fog droplet monitor (FM-120, Droplet Measurement Technologies) at the Scripps Institution of Oceanography’s Mt. Soledad site from 16 February 2023 to 15 February 2024. This instrument measured droplet number size spectra between 2 and 50 microns, from which droplet number concentration, liquid water content, and effective diameter were calculated. These measurements will be used to characterize the seasonal variability of clouds at Mt. Soledad and investigate differences in cloud properties under regional polluted and clean marine conditions. The collected data will soon be posted as part of the digital collection for EPCAPE data hosted by the University of California, San Diego (Russell et al. 2023).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Fine-Scale Variability of Observed and Simulated Surface Albedo Over the Southern Great Plains

Surface albedo can be highly variable in both space and time. The Department of Energy’s Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) field study provides a unique opportunity to characterize the variability over the Southern Great Plains of the United States using integrated tower, aircraft, and satellite observations of the surface albedo and Normalized Difference Vegetation Index (NDVI). The primary advantage of the aircraft and satellite observations is the ability to examine the spatial distribution of surface albedo and NDVI over a large area, while the tower measurements have the ability to examine both diurnal and day-to-day variability at a single location. In general, consistency was found between both the broadband (BB) albedo and NDVI measured from the surface, air and space. There was a small increase from 0.186 to 0.194 in the aircraft BB surface albedo between May and September (about 4% change), while the MODIS black-sky BB surface albedo increased from 0.151 to 0.166 over the same period (about 10% change) while the standard deviations in the aircraft and MODIS BB albedo were similar. The largest seasonal differences in both the aircraft BB albedo and NDVI were found for areas with winter wheat or forest, while areas with pasture or grasses showed a smaller seasonal diversity. The Weather Research and Forecasting (WRF) model was used to simulate the BB surface albedo. In comparison with the aircraft and satellite observations, the WRF-simulated BB surface albedo had no seasonal change and a much narrower distribution.

Berg, Larry K.↗

DOE OSTI2020

Simulation of Continental Shallow Cumulus Populations Using an Observation-Constrained Cloud-System Resolving Model

Continental shallow cumulus (ShCu) clouds observed on 30 August 2016 during the Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) field campaign are simulated by using an observation-constrained cloud-system resolving model. On this day, ShCu forms over Oklahoma and southern Kansas and some of these clouds transition to deeper, precipitating convection during the afternoon. We apply a four-dimensional ensemble-variational (4DEnVar) hybrid technique in the Community Gridpoint Statistical Interpolation (GSI) system to assimilate operational data sets and unique boundary layer measurements including a Raman lidar, radar wind profilers, radiosondes, and surface stations collected by the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) atmospheric observatory into the Weather Research and Forecasting (WRF) model to ascertain how improved environmental conditions can influence forecasts of ShCu populations and the transition to deeper convection. Independent observations from aircraft, satellite, as well as ARM's remote sensors are used to evaluate model performance in different aspects. Several model experiments are conducted to identify the impact of data assimilation (DA) on the prediction of clouds evolution. The analyses indicate that ShCu populations are more accurately reproduced after DA in terms of cloud initiation time and cloud base height, which can be attributed to an improved representation of the ambient meteorological conditions and the convective boundary layer. Extending the assimilation to 18 UTC (local noon) also improved the simulation of shallow-to-deep transitions of convective clouds.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Assessing CLUBB PDF Closure Assumptions for a Continental Shallow-to-Deep Convective Transition Case Over Multiple Spatial Scales

Assumed-PDF (probability density function) higher-order turbulence closures (APHOCs) are now widely used for parameterizing boundary layer turbulence and shallow convection in Earth system models (ESMs). A better understanding of the resolution-dependent behavior of APHOCs is essential for improving the performance of next-generation ESMs with intended horizontal resolutions finer than 10 km. In this study, we evaluate the PDF family of Analytic double-Gaussian 1 implemented in Cloud Layers Unified By Binormals (CLUBB) over a range of spatial scales (Dx) from 2 to 100 km. A 120-km-wide large eddy simulation (LES) for a continental convection case during 2016 Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) field campaign serves as benchmark to evaluate the PDF closure using an off-line approach. We find during the shallow convection period, the CLUBB PDF closure tends to produce positive biases of cloud properties and liquid water flux near cloud base for all scales of analysis. It produces negative biases for these variables near cloud top that are more severe for Dx larger than 25 km. Results show that replacing the CLUBB-parameterized moisture and temperature skewnesses with LES-derived ones can fix most of the biases if clipping of input moments is allowed to prevent the occurrence of unrealizable solutions. Overall, the performance of the PDF closure is better for smaller Dx = 2–5 km than for larger Dx = 50–100 km; for a given grid spacing, it is better when the convective clouds become deeper in the late afternoon. Likely causes for the resolution dependence and implications for improving the PDF closure are discussed.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Determining Spatial Scales of Soil Moisture—Cloud Coupling Pathways Using Semi-Idealized Simulations

The spatial scales of land-atmosphere interactions over heterogeneous, realistic soil moisture patterns are critical to improve our understanding of land-atmosphere interactions. However, these scales are poorly quantified. We use high-resolution numerical experiments to quantify the spatial scales for a selected day during the Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) campaign in Oklahoma. A semi-idealized approach (removing background winds and surface topography while retaining the real-world data for other boundary conditions) enables examination of the local influence from the surface. Simulations that apply uniform surface, variable land cover with uniform soil moisture, and variable land cover with variable soil moisture are then compared. Land cover variations, especially water and urban surfaces, create two variance peaks in the surface sensible heat flux in the scales >10 km (meso-β) and <6 km (meso-γ). Both peaks are enhanced by the observation-based soil moisture distribution that has most of its variance in the meso-β scale. Atmospheric response in the meso-β scale is hydrostatic with weak vertical motion. The land cover variations induce secondary circulations in the scales of 2.5–6 km. The additional soil moisture variability intensifies extreme circulations over dry soil patches and sharp sensible heat flux gradients, slightly extending the characteristic scales to 2.5–9 km. While their areal coverage is small, soil moisture variations on such “hotspots” lead to substantially larger convective cloud structure and domain-mean rainfall, calling for a consideration of their non-linear effect in large-scale models.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

pinacles

Predicting Interactions of Aerosol and Clouds in Large Eddy Simulation (PINACLES) is a high-performance, massively parallel, anelastic atmospheric model written in Python

Pressel, Kyle↗

DOE OSTI2023

Chemical identification of new particle formation and growth precursors through positive matrix factorization of ambient ion measurements

Abstract. In the lower troposphere, rapid collisions between ions and trace gases result in the transfer of positive charge to the highest proton affinity species and negative charge to the lowest proton affinity species. Measurements of the chemical composition of ambient ions thus provide direct insight into the most acidic and basic trace gases and their ion–molecule clusters – compounds thought to be important for new particle formation and growth. We deployed an atmospheric pressure interface time-of-flight mass spectrometer (APi-ToF) to measure ambient ion chemical composition during the 2016 Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) campaign at the United States Department of Energy Atmospheric Radiation Measurement facility in the Southern Great Plains (SGP), an agricultural region. Cations and anions were measured for alternating periods of ∼ 24 h over 1 month. We use binned positive matrix factorization (binPMF) and generalized Kendrick analysis (GKA) to obtain information about the chemical formulas and temporal variation in ionic composition without the need for averaging over a long timescale or a priori high-resolution peak fitting. Negative ions consist of strong acids including sulfuric and nitric acid, organosulfates, and clusters of NO3- with highly oxygenated organic molecules (HOMs) derived from monoterpene (MT) and sesquiterpene (SQT) oxidation. Organonitrates derived from SQTs account for most of the HOM signal. Combined with the diel profiles and back trajectory analysis, these results suggest that NO3 radical chemistry is active at this site. SQT oxidation products likely contribute to particle growth at the SGP site. The positive ions consist of bases including alkyl pyridines and amines and a series of high-mass species. Nearly all the positive ions contained only one nitrogen atom and in general support ammonia and amines as being the dominant bases that could participate in new particle formation. Overall, this work demonstrates how APi-ToF measurements combined with binPMF analysis can provide insight into the temporal evolution of compounds important for new particle formation and growth.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Re-evaluating cloud chamber constraints on depositional ice growth in cirrus clouds – Part 1: Model description and sensitivity tests

Abstract. Ice growth from vapor deposition is an important process for the evolution of cirrus clouds, but the physics of depositional ice growth at the low temperatures (<235 K) characteristic of the upper troposphere and lower stratosphere is not well understood. Surface attachment kinetics, generally parameterized as a deposition coefficient αD, control ice crystal habit and also may limit growth rates in certain cases, but significant discrepancies between experimental measurements have not been satisfactorily explained. Experiments on single ice crystals have previously indicated the deposition coefficient is a function of temperature and supersaturation, consistent with growth mechanisms controlled by the crystal's surface characteristics. Here we use observations from cloud chamber experiments in the Aerosol Interactions and Dynamics in the Atmosphere (AIDA) aerosol and cloud chamber to evaluate surface kinetic models in realistic cirrus conditions. These experiments have rapidly changing temperature, pressure, and ice supersaturation such that depositional ice growth may evolve from diffusion limited to surface kinetics limited over the course of a single experiment. In Part 1, we describe the adaptation of a Lagrangian parcel model with the Diffusion Surface Kinetics Ice Crystal Evolution (DiSKICE) model (Zhang and Harrington, 2014) to the AIDA chamber experiments. We compare the observed ice water content and saturation ratios to that derived under varying assumptions for ice surface growth mechanisms for experiments simulating ice clouds between 180 and 235 K and pressures between 150 and 300 hPa. We found that both heterogeneous and homogeneous nucleation experiments at higher temperatures (>205 K) could generally be modeled consistently with either a constant deposition coefficient or the DiSKICE model assuming growth on isometric crystals via abundant surface dislocations. Lower-temperature experiments showed more significant deviations from any depositional growth model, with different ice growth rates for heterogeneous and homogeneous nucleation experiments.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Substantial Diel Changes of Cloud Adjustments to Aerosols in Ship‐Tracks

Clouds adjust their albedo, amount and liquid water path to anthropogenic aerosols, and produce a climate forcing. Such cloud adjustments are complex functions of both environmental conditions and interaction time. However, direct observations of temporal changes in cloud adjustments are limited. Here, we develop a method to show observational evidence of substantial diel changes in cloud adjustments within ship-tracks. Polluted clouds experiencing extended nighttime exposure exhibit higher increases in cloud fraction while liquid-water path adjustments follow a non-monotonic evolution. The higher cloud fraction increase persists through daytime. Such diel variations likely stem from diel changes in solar heating and background cloud precipitation, and are important because nighttime changes persist and affect solar radiation during the day. Accounting for diel variations produces a stronger aerosol forcing, by −0.1 ∼−0.4 W⁢m −2 . Our approach reveals how the temporal evolution of cloud adjustments can have important implications for aerosol-cloud interactions.

Yuan, Tianle [NASA Goddard Space Flight Center (GS↗

DOE OSTI2023

TRACER Carbonaceous Aerosols Thrust – University of California, Davis Field Campaign Report

The broader U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s TRacking Aerosol Convection interactions ExpeRiment (TRACER) campaign aims to increase our understanding of convective cloud life cycles and aerosol-convection interactions. Our TRACER Carbonaceous Aerosols Thrust-University of California, Davis (TRACER-CAT-UCDavis) study complemented these broader aims by characterizing and quantifying the optical properties and composition of carbonaceous aerosols during part of the TRACER intensive sampling period (July 1- July 31, 2022) at the first ARM Mobile Facility (AMF1) main site (M1) in La Porte, Texas. Our measurements complemented the suite of instrumentation already provided by the AMF1, expanding the capabilities through deployment of unique, state-of-the-science instrumentation. The instrumentation included: (i) two cavity-attenuated phase shift spectroscopy single-scatter albedo (CAPS-SSA) instruments operating at 530 nm and 630 nm, and that were modified to characterize particle light absorption, extinction, and scattering at elevated humidities; (ii) the UC Davis dual-wavelength cavity ringdown-photoacoustic spectrometer (CRD-PAS), which characterizes dry particle extinction and absorption at 405 nm and 532 nm; (iii) a soot particle aerosol mass spectrometer (SP-AMS) that operated in “laser only” mode that characterized the size-dependent compositions of black carbon (BC)-containing particles; (v) a thermal denuder, to remove coatings on particles; and (vi) a scanning electrical mobility sizer (SEMS), to characterize particle mobility diameters from 10-1300 nm. Our measurements occurred alongside complementary observations made by Los Alamos National Laboratory (LANL) during the TRACER-CAT-LANL study, including a humidified CAPS-SSA instrument operating at 450 nm. Our primary scientific interest is in understanding the relationship between particle composition and light absorption, with a particular focus on the influence of water uptake. While it is known that coatings on BC can enhance absorption, the extent to which this occurs in the atmosphere and the specific role that water plays as a coating remain unclear. The TRACER-CAT-UCDavis measurements were made with near-complete coverage for the CRD-PAS, SP-AMS, and SEMS throughout the intensive period. The UC Davis humidified CAPS-SSA instruments had significant challenges with operation owing to the demanding conditions (large temperature fluctuations, high humidity), exacerbated by supply chain issues that delayed resolution of these challenges. However, the humidified CAPS-SSA instrument operated by LANL operated throughout the intensive period with near-complete coverage. The dry light extinction measurements from the CRD-PAS measurements and the LANL CAPS-SSA exhibited a good correlation, although the CAPS-SSA systematically measured greater extinction values than expected. While all instruments, with the exception of an aerodynamic particle sizer (APS), measured behind a common particulate matter (PM)2.5 μm cyclone, the greater extinction measured by the LANL CAPS-SSA compared to the CRD-PAS may have resulted from different losses of larger particles in the sampling lines from the cyclone to the instruments; the tubing length was shorter from the cyclone to the LANL CAPS-SSA, consistent with this idea. A summary of the TRACER-CAT-UCDavis measurements, along with some of the TRACER-CAT-LANL measurements, are shown in the figure below. Notably, there were periods when the contributions of presumed dust were substantial and even dominated the observed light extinction and absorption. Also, there was a clear shift in the behavior of submicron particles from before July 16, 2022 to after, with the prior period exhibiting regular episodes of new particle formation and the latter period exhibiting rapid variations in the concentrations of small particles.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Examining Aerosol Vertical Transport and Removal during Deep Convective Events

Atmospheric aerosols affect the global energy budget by scattering and absorbing sunlight (direct effects) and by changing the microphysical structure, lifetime, and coverage of clouds (indirect effects). Globally, the free troposphere is a major source of nucleation- and Aitken-mode aerosols due to the enhanced new particle formation rates at high altitudes. Recent studies have shown deep convective systems are capable of transporting these small aerosols from the free troposphere to the boundary layer by strong convective downdrafts and weaker downward motions in the stratiform regions. These vertically transported aerosols can grow into cloud condensation nuclei (CCN) and play a significant role in the global climate. During the deep convective processes, existing accumulation-mode aerosols that act as coagulation sinks of smaller particles are also removed by wet scavenging. Compared to the vertical transport of these particles by entrainment mixing, which is slower but more prevalent, the deep convective downdraft processes may be more rapid and efficient in the vertical transport of aerosols. However, most of the current climate models do not include this mechanism as a source of CCN, mainly because the frequency of deep convective events varies significantly with geographic location and thus their contributions to CCN are unpredictable. We target this critical gap in understanding the vertical transport and removal of aerosols by deep convections. We proposed to analyze a multi-year, multi-site measurement record available from the U.S. Department of Energy (DOE) ARM program, including the observations from the 2014/15 Observations and Modeling of the Green Ocean Amazon (GoAmazon) field campaign, the 2017/18 Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign, the 2018/19 Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign, the 2021/22 Tracking Aerosol Convection Interactions Experiment (TRACER) field campaign, and the long-term measurements collected at the Southern Great Plains (SGP) atmospheric observatory, where deep convective clouds were frequently observed. This project is aimed at the following three objectives: (1) Gaining a detailed and quantitative understanding of the aerosols transported by a convective downdraft and their evolution in the atmosphere; (2) Examining the wet scavenging mechanisms and efficiencies of aerosols at altitudes of deep convective systems based on ground and aircraft measurements; (3) Evaluating the contribution of deep convective systems to CCN as both a source and a sink of atmospheric aerosols and its seasonal variabilities.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Science Plan for the Deployment of the Third ARM Mobile Facility to the Southeastern United States at the Bankhead National Forest, Alabama (AMF3 BNF)

In 2018, the U.S. Department of Energy (DOE) held a workshop for the Atmospheric Radiation Measurement (ARM) (Mather and Voyles 2013) user facility to discuss critical climate challenges and locations where key ARM Mobile Facility (AMF) observational assets could impact Earth system modeling (ESM). As an outcome, the southeast United States (SE U.S.) was identified as a high-priority region to target climate-process studies that promote a deeper understanding of the climate system and bolster ARM interactions with the community to drive ESM advancement. The DOE ARM user facility is a globally recognized leader in deploying and operating strategically located observation sites around the world for studying the properties of aerosols and clouds and their interaction with radiation, precipitation, and the Earth’s surface. In partnering with the DOE Atmospheric System Research (ASR) program, ARM solicited a multi-agency Site Science Team approach to provide input and close interaction with ARM management towards a successful SE U.S. deployment of the ARM third Mobile Facility (AMF3) (Miller et al. 2016). These efforts included identifying key locations, science drivers and instruments, and measurement strategies to address the wider climate-process needs and ESM improvement. Community input served a vital role in establishing, refining, and informing the relevant drivers and decisions regarding this AMF3 deployment. The team has identified Northern Alabama (N. AL) as regionally representative to unlock the key opportunities that will improve our understanding and model representation of aerosol, cloud, and land surface processes and their couplings in the SE U.S. A defining aspect of the AMF3 deployment is its commitment to long-term (anticipated five-year) observations to mitigate potential seasonal-to-annual variability that often limits appropriate attribution of phenomena to local or larger-scale processes. The proposed location may leverage nearby surface networks and multi-agency and partner assets to enrich this multi-year deployment. One motivation is to understand the role of spatiotemporal variability (thermodynamic, land-surface) across aspects of the climate system, with our AMF3 team anticipating future demands on characterizing the relationships between local-to-regional cloud development and surface processes across a diverse patchwork of natural, managed, and urban landscapes as found throughout the N. AL regions. The main site targets an intact, representative, forested region – the Bankhead National Forest (BNF) – underscoring further team commitment to regionally important land atmosphere two-way interactive studies “from the canopy to the clouds”, with enhanced tower instrumentation augmenting traditional ARM capabilities adjacent to this site. Multiple supplemental sites will also be distributed across this region, prioritizing added needs for biodiversity. Anticipated high-priority cloud science themes will target N. AL as a regional SE U.S. hotbed for high-impact weather, convective cloud onset, and shallow to-deep cloud transitioning. Anticipated aerosol drivers will focus on chemical processes that control the evolution of organic aerosol, the seasonality and spatial distribution of water vapor and particle-phase water, and its role on aerosol optical properties. Anticipated land atmosphere drivers consider the two-way feedbacks between surface influence on aerosols, clouds, and precipitation properties and the associated radiative impacts on plant physiology and canopy-scale fluxes. Emphasis will include the study of the impact of surface processes on aerosols via precursor emission, and on clouds via moisture flux and thermal development.

Doppler lidar, aerosols, convection↗

DOE OSTI2023

Science Plan for the Deployment of the Third ARM Mobile Facility to the Southeastern United States at the Bankhead National Forest, Alabama (AMF3 BNF)

In 2018, the U.S. Department of Energy (DOE) held a workshop for the Atmospheric Radiation Measurement (ARM) (Mather and Voyles 2013) user facility to discuss critical climate challenges and locations where key ARM Mobile Facility (AMF) observational assets could impact Earth system modeling (ESM). As an outcome, the southeast United States (SE U.S.) was identified as a high-priority region to target climate-process studies that promote a deeper understanding of the climate system and bolster ARM interactions with the community to drive ESM advancement. The DOE ARM user facility is a globally recognized leader in deploying and operating strategically located observation sites around the world for studying the properties of aerosols and clouds and their interaction with radiation, precipitation, and the Earth’s surface. In partnering with the DOE Atmospheric System Research (ASR) program, ARM solicited a multi-agency Site Science Team approach to provide input and close interaction with ARM management towards a successful SE U.S. deployment of the ARM third Mobile Facility (AMF3) (Miller et al. 2016). These efforts included identifying key locations, science drivers and instruments, and measurement strategies to address the wider climate-process needs and ESM improvement. Community input served a vital role in establishing, refining, and informing the relevant drivers and decisions regarding this AMF3 deployment. The team has identified Northern Alabama (N. AL) as regionally representative to unlock the key opportunities that will improve our understanding and model representation of aerosol, cloud, and land-surface processes and their couplings in the SE U.S. A defining aspect of the AMF3 deployment is its commitment to long-term (anticipated five-year) observations to mitigate potential seasonal-to-annual variability that often limits appropriate attribution of phenomena to local or larger-scale processes. The proposed location may leverage nearby surface networks and multi-agency and partner assets to enrich this multi-year deployment. One motivation is to understand the role of spatiotemporal variability (thermodynamic, land-surface) across aspects of the climate system, with our AMF3 team anticipating future demands on characterizing the relationships between local-to-regional cloud development and surface processes across a diverse patchwork of natural, managed, and urban landscapes as found throughout the N. AL regions. The main site targets an intact, representative, forested region – the Bankhead National Forest (BNF) – underscoring further team commitment to regionally important land-atmosphere two-way interactive studies “from the canopy to the clouds”, with enhanced tower instrumentation augmenting traditional ARM capabilities adjacent to this site. Multiple supplemental sites will also be distributed across this region, prioritizing added needs for biodiversity. Anticipated high-priority cloud science themes will target N. AL as a regional SE U.S. hotbed for high-impact weather, convective cloud onset, and shallow-to-deep cloud transitioning. Anticipated aerosol drivers will focus on chemical processes that control the evolution of organic aerosol, the seasonality and spatial distribution of water vapor and particle-phase water, and its role on aerosol optical properties. Anticipated land-atmosphere drivers consider the two-way feedbacks between surface influence on aerosols, clouds, and precipitation properties and the associated radiative impacts on plant physiology and canopy-scale fluxes. Emphasis will include the study of the impact of surface processes on aerosols via precursor emission, and on clouds via moisture flux and thermal development.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

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↗

DOE OSTI2025

Dependence of Convective Cloud Microphysical Properties on Environmental Conditions during the TRACER and ESCAPE Field Campaigns: A Synergistic Approach of Observations, Machine Learning and Parcel Models

The sensitivity of convective clouds to aerosols and their interactions with environment, combined with limited observational constraints in parameterizations, introduces significant uncertainties in atmospheric models. Here, this study investigates the dependence of convective cloud microphysical properties on environmental conditions using a synergistic approach that combines unique observations from the TRACER and ESCAPE field campaigns, machine learning techniques, and parcel model simulations with a super-droplet microphysics scheme. A random forest algorithm identifies in-situ vertical velocity (w), temperature (T), and surface fine-mode aerosol mass concentration as the three most important environmental conditions influencing cloud properties including liquid water content (LWC), number concentration for particles with D max < 50 μm (N c ,<50), 50 μm ≤ D max ≤ 3000 μm (N c,50–3000 ), and droplet effective diameter (D e ). Results show that LWC, N c,<50 , and N c,50–3000 significantly increase with w in updrafts. Across w bins, as T decreases, LWC, D e , and N c,50–3000 increase, while N c,<50 decreases, which are closely linked to the distance above cloud bases. Warmer cloud bases yield higher LWC, greater N c,50–3000 , and smaller N c,<50 , while polluted environments produce greater N c,<50 . Parcel model simulations successfully replicate these observed dependencies. The simulation results indicate that warmer cloud bases enhance condensation generating larger droplets, and differences in droplet sizes are then amplified through collision-coalescence, resulting in a greater N c,50–3000 . Polluted conditions result in a greater N c,<50 primarily due to enhanced cloud condensation nuclei activation despite increased collision-coalescence rates compared to pristine conditions. This study provides observed quantitative patterns characterizing cloud microphysical properties as a function of key environmental parameters, offering valuable constraints for improving physics parameterizations and numerical models.

54 ENVIRONMENTAL SCIENCES↗