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All sourcesNASA NTRSDOE OSTI
NASA NTRSDate not supplied

Springtime SEA Air Is Consistently Both Smoky and Humid, but This Relationship (and Its Radiative Effects) Varies Spatially and Seasonally

The atmosphere over the southeast Atlantic Ocean (SEA) sees a consistent springtime biomass burning (BB) smoke from widespread agricultural fires on the African continent. This smoke layer is initially lofted high in a continental mixed layer (~5-6km) and is then transported westward in the free troposphere, where it overlies and ultimately mixes into the SEA stratocumulus-topped oceanic boundary layer. Coincident with this smoke is an elevated humidity signal which is present from the time a given airmass is over the continental source region. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) was a NASA Earth Venture Suborbital mission with the goal of measuring aerosol, cloud, and atmospheric properties over this region during three deployments in September 2016, August 2017, and October 2018. A previous study discussed the spatial characteristics of the water vapor-BB plume observations in the September 2016 flight data and their degree of agreement with several atmospheric reanalyses and models. In the present work, we first discuss atmospheric chemistry, structure, and aerosol results from all three ORACLES deployments to place these results in a broader seasonal context. Despite the differing locations and season of each deployment, we show that there continues to be good agreement between the airborne ORACLES dataset and large-scale reanalyses, specifically the ECMWF ERA5 and CAMS reanalyses. Other reanalyses (specifically NASA's MERRA-2) preserved the observed correlation between meteorology and biomass burning conditions, but, as was seen for 2016, was frequently displaced spatially relative to the observations. The CAMS reanalysis performs better with water vapor than with CO. Results comparing CAMS column AOD to the field measurements show slight overestimates, consistent with previous analysis, but the good relationship observed between AOD and inlet-based aerosol extinction demonstrates this metric's utility to broader studies. The good ERA5/CAMS/ORACLES agreement allows us to next examine the multi-year seasonal patterns and trends beyond the three ORACLES deployment periods. Looking at seven years of reanalysis data for the BB season, we find distinct variations between each month/deployment in terms of vertical smoke distribution and correlation to atmospheric specific humidity, due to changing conditions through the BB season. Using k-means clustering of these climatological reanalysis, we identify six canonical atmospheric profile types of varying total atmospheric humidity and vertical structure and describe their changing incidence spatially and throughout the season, and six analogous profile types for carbon monoxide, allowing us to characterize the atmospheric structure of both vapor and BB over time throughout the SEA region. This classification will allow for a more complete analysis of the broader radiative and dynamical effects of humid aerosols overlying stratocumulus clouds.

Kristina Marie Myers Pistone↗
DOE OSTI2021

Mass accommodation and gas–particle partitioning in secondary organic aerosols: dependence on diffusivity, volatility, particle-phase reactions, and penetration depth

Abstract. Mass accommodation is an essential process for gas–particle partitioning of organic compounds in secondary organic aerosols (SOA). The mass accommodation coefficient is commonly described as the probability of a gas molecule colliding with the surface to enter the particle phase. It is often applied, however, without specifying if and how deep a molecule has to penetrate beneath the surface to be regarded as being incorporated into the condensed phase (adsorption vs. absorption). While this aspect is usually not critical for liquid particles with rapid surface–bulk exchange, it can be important for viscous semi-solid or glassy solid particles to distinguish and resolve the kinetics of accommodation at the surface, transfer across the gas–particle interface, and further transport into the particle bulk. For this purpose, we introduce a novel parameter: an effective mass accommodation coefficient αeff that depends on penetration depth and is a function of surface accommodation coefficient, volatility, bulk diffusivity, and particle-phase reaction rate coefficient. Application of αeff in the traditional Fuchs–Sutugin approximation of mass-transport kinetics at the gas–particle interface yields SOA partitioning results that are consistent with a detailed kinetic multilayer model (kinetic multilayer model of gas–particle interactions in aerosols and clouds, KM-GAP; Shiraiwa et al., 2012) and two-film model solutions (Model for Simulating Aerosol Interactions and Chemistry, MOSAIC; Zaveri et al., 2014) but deviate substantially from earlier modeling approaches not considering the influence of penetration depth and related parameters. For highly viscous or semi-solid particles, we show that the effective mass accommodation coefficient remains similar to the surface accommodation coefficient in the case of low-volatility compounds, whereas it can decrease by several orders of magnitude in the case of semi-volatile compounds. Such effects can explain apparent inconsistencies between earlier studies deriving mass accommodation coefficients from experimental data or from molecular dynamics simulations. Our findings challenge the approach of traditional SOA models using the Fuchs–Sutugin approximation of mass transfer kinetics with a fixed mass accommodation coefficient, regardless of particle phase state and penetration depth. The effective mass accommodation coefficient introduced in this study provides an efficient new way of accounting for the influence of volatility, diffusivity, and particle-phase reactions on SOA partitioning in process models as well as in regional and global air quality models. While kinetic limitations may not be critical for partitioning into liquid SOA particles in the planetary boundary layer (PBL), the effects are likely important for amorphous semi-solid or glassy SOA in the free and upper troposphere (FT–UT) as well as in the PBL at low relative humidity and low temperature.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2004

3D Cloud Radiative Effects on Aerosol Optical Thickness Retrievals in Cumulus Cloud Fields in the Biomass Burning Region in Brazil

Aerosol amount in clear regions of a cloudy atmosphere is a critical parameter in studying the interaction between aerosols and clouds. Since the global cloud cover is about 50%, cloudy scenes are often encountered in any satellite images. Aerosols are more or less transparent, while clouds are extremely reflective in the visible spectrum of solar radiation. The radiative transfer in clear-cloudy condition is highly three- dimensional (3D). This paper focuses on estimating the 3D effects on aerosol optical thickness retrievals using Monte Carlo simulations. An ASTER image of cumulus cloud fields in the biomass burning region in Brazil is simulated in this study. The MODIS products (i-e., cloud optical thickness, particle effective radius, cloud top pressure, surface reflectance, etc.) are used to construct the cloud property and surface reflectance fields. To estimate the cloud 3-D effects, we assume a plane-parallel stratification of aerosol properties in the 60 km x 60 km ASTER image. The simulated solar radiation at the top of the atmosphere is compared with plane-parallel calculations. Furthermore, the 3D cloud radiative effects on aerosol optical thickness retrieval are estimated.

Wen, Guo-Yong↗
DOE OSTI2018

Collaborative Project: Contributions of organic compounds to the growth of freshly nucleated atmospheric nanoparticles. Final Report

New-particle formation (NPF) is a significant source of aerosol particles into the atmosphere. However, these particles are initially too small to have climatic importance and must grow, primarily through net uptake of low-volatility species and more volatile gases that react in particles to form stable compounds, from diameters of ~1 nm to 30–100 nm in order to potentially impact climate. At the present time there are uncertainties in the physical and chemical processes associated with the growth of these freshly formed particles that lead to uncertainties in model predictions of aerosol-climate interactions. In this project, we used a combination of field, laboratory, and modelling studies to understand the processes leading to nanoparticle growth and evaluated and improved growth in global aerosol models. During this period this research team has either participated in, or analyzed observations from, four DOE-funded campaigns: the 2013 New Particle Formation Study (NPFS) at the ARM Southern Great Plains (SGP) site; the 2013 Biogenic Aerosols – Effects on Clouds and Climate campaign (BAECC) in Hyytiala, Finland; Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) in central Amazonia, Brazil; and, most recently, the 2016 Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) campaign at the SGP site. In addition, the research team explored nanoparticle growth mechanisms in laboratory experiments at the National Center for Atmospheric Research, University of California, Irvine, and the CLOUD chamber in Geneva, Switzerland. Modeling efforts resulted in a process-level model that incorporated both salt formation and the uptake of low-volatility organic compounds, which was able to connect measurements of gas and nanoparticle phase compounds observed during NPFS. In total, the results of this work have been described in 32 peer-reviewed publications and 34 invited or conference presentations.

58 GEOSCIENCES↗
DOE OSTI2018

Final Report: Collaborative Project: Contributions of organic compounds to the growth of freshly nucleated atmospheric nanoparticles

New-particle formation (NPF) is a significant source of aerosol particles into the atmosphere. However, these particles are initially too small to have climatic importance and must grow, primarily through net uptake of low-volatility species and more volatile gases that react in particles to form stable compounds, from diameters of ~1 nm to 30–100 nm in order to potentially impact climate. At the present time there are uncertainties in the physical and chemical processes associated with the growth of these freshly formed particles that lead to uncertainties in model predictions of aerosol-climate interactions. In this project, we used a combination of field, laboratory, and modelling studies to understand the processes leading to nanoparticle growth and evaluated and improved growth in global aerosol models. During this period this research team has either participated in, or analyzed observations from, four DOE-funded campaigns: the 2013 New Particle Formation Study (NPFS) at the ARM Southern Great Plains (SGP) site; the 2013 Biogenic Aerosols – Effects on Clouds and Climate campaign (BAECC) in Hyytiala, Finland; Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) in central Amazonia, Brazil; and, most recently, the 2016 Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) campaign at the SGP site. In addition, the research team explored nanoparticle growth mechanisms in laboratory experiments at the National Center for Atmospheric Research, University of California, Irvine, and the CLOUD chamber in Geneva, Switzerland. Modeling efforts resulted in a process-level model that incorporated both salt formation and the uptake of low-volatility organic compounds, which was able to connect measurements of gas and nanoparticle phase compounds observed during NPFS. In total, the results of this work have been described in 32 peer-reviewed publications and 34 invited or conference presentations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German–Brazilian cooperative aircraft campaign ACRIDICON–CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (global precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September–October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90 nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5–72 h. We also found elevated concentrations of larger (> 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a conceptual model, where production of new aerosol particles takes place in the continental UT from biogenic volatile organic material brought up by deep convection and converted to condensable species in the UT. Subsequently, downward mixing and transport of upper tropospheric aerosol can be a source of particles to the PBL, where they increase in size by the condensation of biogenic volatile organic compound (BVOC) oxidation products. This may be an important source of aerosol particles for the Amazonian PBL, where aerosol nucleation and new particle formation have not been observed. We propose that this may have been the dominant process supplying secondary aerosol particles in the pristine atmosphere, making clouds the dominant control of both removal and production of atmospheric particles.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRSDate not supplied

Impacts of Aerosol and Cloud Variability on Satellite-Derived All-skies Direct Aerosol Radiative Effects (DARE) over the North and Southeast Atlantic

The Top-of-Atmosphere (TOA) Shortwave (SW) Direct Aerosol Radiative Effect (DARE) in all-sky conditions (i.e., aerosols in clear skies and aerosols above and below all types of clouds) is the global change in upwelling radiative flux due to aerosols. It is one of the strongest indicators of global climate change due to aerosols. SW DARE at TOA depends on the Earth’s surface albedo, cloud fraction, cloud optical properties, and aerosol optical properties, which are all challenging to accurately characterize from space. The overarching goals of our project are to provide state-of-the-art observational all-sky TOA SW DARE, along with guidance on which aerosol and/or cloud properties are the most important to measure, and at which spatio-temporal scales, for accurate DARE observations. We compute all-sky DARE based on state-of-the-art cloud and aerosol retrieval algorithms from CALIOP (Cloud–Aerosol Lidar with Orthogonal Polarization) and MODIS (Moderate Resolution Imaging spectroradiometer) satellite sensors, as well as aerosol intensive properties from MERRA-2 (Modern-Era Retrospective Analysis for Research and Applications, version 2) simulations over three specific regions of the Atlantic Ocean from 2012 to 2016. In this symposium, we present a characterization of the cloud and aerosol optical and physical properties and the observational TOA SW DARE along three individual satellite tracks in the Southeast Atlantic region -- on September 18 and 20, 2016 and August 13, 2017. We then quantify the impact of assuming homogeneous cloud or aerosol fields in space-based TOA SW DARE calculations. And, finally, the resulting space-based all-skies aerosol vertical distribution and DARE calculations are evaluated using remote sensing observations from coincident suborbital flights from the NASA ORACLES (the ObseRvations of Aerosols above CLouds and their intEractionS, ORACLES field campaign) field campaign. The NASA Atmospheric Observing System (AOS) mission addresses the NASA Aerosol, Cloud, Convection and Precipitation (ACCP) designated observables and proposes, as one of its aerosol objectives, to reduce uncertainties in estimates of global mean all-sky SW DARE at TOA. Well characterizing clouds, aerosol vertical distributions, aerosol types and associated all-skies DARE over the Atlantic Ocean will inform the AOS community on where, when, how, and how often the satellite retrievals should be performed to estimate DARE and reduce all-skies DARE uncertainties most accurately. These comprehensive characterizations will also identify the key regions and times when the AOS (or other ACCP-related) suborbital missions should be conducted to evaluate and improve the AOS space-based observations and retrievals.

aerosol↗
NASA NTRS2012

The Effects of an Absorbing Smoke Layer on MODIS Marine Boundary Layer Cloud Optical Property Retrievals and Radiative Forcing

Clouds, aerosols, and their interactions are widely considered to be key uncertainty components in our current understanding of the Earth's atmosphere and radiation budget. The work presented here is focused on the quasi-permanent marine boundary layer . (MBL) clouds off the southern Atlantic coast of Africa and the effects on MODIS cloud optical property retrievals (MOD06) of an overlying absorbing smoke layer. During much of August and September, a persistent smoke layer resides over this region, produced from extensive biomass burning throughout the southern African savanna. The resulting absorption, which increases with decreasing wavelength, potentially introduces biases into the MODIS cloud optical property retrievals of the underlying MBL clouds. This effect is more pronounced in the cloud optical thickness retrievals, which over ocean are derived from the wavelength channel centered near 0.86 micron (effective particle size retrievals are derived from the longer-wavelength near-IR channels at 1.6, 2.1, and 3.7 microns). Here, the spatial distributions of the scalar statistics of both the cloud and aerosol layers are first determined from the CALIOP 5 km layer products. Next, the MOD06 look-up tables (LUTs) are adjusted by inserting an absorbing smoke layer of varying optical thickness over the cloud. Retrievals are subsequently performed for a subset of MODIS pixels collocated with the CALIOP ground track, using smoke optical thickness from the CALIOP 5km aerosol layer product to select the appropriate LUT. The resulting differences in cloud optical property retrievals due to the inclusion of the smoke layer in the LUTs will be examined. In addition, the direct radiative forcing of this smoke layer will be investigated from the perspective of the cloud optical property retrieval differences.

Meyer, Kerry↗
DOE OSTI2022

Indications of a Decrease in the Depth of Deep Convective Cores with Increasing Aerosol Concentration during the CACTI Campaign

Abstract An aerosol indirect effect on deep convective cores (DCCs), by which increasing aerosol concentration increases cloud-top height via enhanced latent heating and updraft velocity, has been proposed in many studies. However, the magnitude of this effect remains uncertain due to aerosol measurement limitations, modulation of the effect by meteorological conditions, and difficulties untangling meteorological and aerosol effects on DCCs. The Cloud, Aerosol, and Complex Terrain Interactions (CACTI) campaign in 2018–19 produced concentrated aerosol and cloud observations in a location with frequent DCCs, providing an opportunity to examine the proposed aerosol indirect effect on DCC depth in a rigorous and robust manner. For periods throughout the campaign with well-mixed boundary layers, we analyze relationships that exist between aerosol variables (condensation nuclei concentration > 10 nm, 0.4% cloud condensation nuclei concentration, 55–1000-nm aerosol concentration, and aerosol optical depth) and meteorological variables [level of neutral buoyancy (LNB), convective available potential energy, midlevel relative humidity, and deep-layer vertical wind shear] with the maximum radar-echo-top height and cloud-top temperature (CTT) of DCCs. Meteorological variables such as LNB and deep-layer shear are strongly correlated with DCC depth. LNB is also highly correlated with three of the aerosol variables. After accounting for meteorological correlations, increasing values of the aerosol variables [with the exception of one formulation of aerosol optical depth (AOD)] are generally correlated at a statistically significant level with a warmer CTT of DCCs. Therefore, for the study region and period considered, increasing aerosol concentration is mostly associated with a decrease in DCC depth.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2016

An A-Train Climatology of Extratropical Cyclone Clouds

Extratropical cyclones (ETCs) are the main purveyors of precipitation in the mid-latitudes, especially in winter, and have a significant radiative impact through the clouds they generate. However, general circulation models (GCMs) have trouble representing precipitation and clouds in ETCs, and this might partly explain why current GCMs disagree on to the evolution of these systems in a warming climate. Collectively, the A-train observations of MODIS, CloudSat, CALIPSO, AIRS and AMSR-E have given us a unique perspective on ETCs: over the past 10 years these observations have allowed us to construct a climatology of clouds and precipitation associated with these storms. This has proved very useful for model evaluation as well in studies aimed at improving understanding of moist processes in these dynamically active conditions. Using the A-train observational suite and an objective cyclone and front identification algorithm we have constructed cyclone centric datasets that consist of an observation-based characterization of clouds and precipitation in ETCs and their sensitivity to large scale environments. In this presentation, we will summarize the advances in our knowledge of the climatological properties of cloud and precipitation in ETCs acquired with this unique dataset. In particular, we will present what we have learned about southern ocean ETCs, for which the A-train observations have filled a gap in this data sparse region. In addition, CloudSat and CALIPSO have for the first time provided information on the vertical distribution of clouds in ETCs and across warm and cold fronts. We will also discuss how these observations have helped identify key areas for improvement in moist processes in recent GCMs. Recently, we have begun to explore the interaction between aerosol and cloud cover in ETCs using MODIS, CloudSat and CALIPSO. We will show how aerosols are climatologically distributed within northern hemisphere ETCs, and how this relates to cloud cover.

clouds↗
NASA NTRS2018

Observations of the Interaction and Transport of Fine Mode Aerosols With Cloud and/or Fog in Northeast Asia From Aerosol Robotic Network and Satellite Remote Sensing

Analysis of Sun photometer measured and satellite retrieved aerosol optical depth (AOD) datahas shown that major aerosol pollution events with very highfine mode AOD (>1.0 in midvisible) in theChina/Korea/Japan region are often observed to be associated with significant cloud cover. This makesremote sensing of these events difficult even for high temporal resolution Sun photometer measurements.Possible physical mechanisms for these events that have high AOD include a combination of aerosolhumidification, cloud processing, and meteorological covariation with atmospheric stability andconvergence. The new development of Aerosol Robotic Network Version 3 Level 2 AOD with improved cloudscreening algorithms now allow for unprecedented ability to monitor these extremefine mode pollutionevents. Further, the spectral deconvolution algorithm (SDA) applied to Level 1 data (L1; no cloud screening)provides an even more comprehensive assessment offine mode AOD than L2 in current and previous dataversions. Studying the 2012 winter-summer period, comparisons of Aerosol Robotic Network L1 SDA dailyaveragefine mode AOD data showed that Moderate Resolution Imaging Spectroradiometer satellite remotesensing of AOD often did not retrieve and/or identify some of the highestfine mode AOD events in thisregion. Also, compared to models that include data assimilation of satellite retrieved AOD, the L1 SDAfinemode AOD was significantly higher in magnitude, particularly for the highest AOD events that were oftenassociated with significant cloudiness.

Eck, T. F.↗
DOE OSTI2023

Observational study of relationships between entrainment rate, homogeneity of mixing, and cloud droplet relative dispersion

The entrainment–mixing process is key to the cloud’s dynamical and microphysical processes. However, to the best of our knowledge, no study has quantitatively linked entrainment rate and homogeneity of mixing. Additionally, their combined effects on cloud droplet relative dispersion and physical mechanisms are even more unclear. This study analyzed the aircraft measurements of cumulus clouds collected in the Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems field campaign to identify these relationships. The relationship between the entrainment rate and homogeneous mixing degree was found to be moderately positive, and the underlying mechanisms related to mixing and evaporation time scales and environmental relative humidity were explored. The relationship between relative dispersion and entrainment rate changes from positive to negative with increasing entrainment rate, depending on the dominance of evaporation of large or small droplets. The relative dispersion first increases and then decreases with increasing homogeneous mixing degree, validating the results of previous model simulations. Further, the results shed new light on understanding the interactions between cloud microphysics and cloud dynamics through turbulent entrainment and mixing processes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA)

With their extensive coverage, marine low clouds greatly impact global climate. Presently, marine low clouds are poorly represented in global climate models, and the response of marine low clouds to changes in atmospheric greenhouse gases and aerosols remains the major source of uncertainty in climate simulations. The Eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer clouds, whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. In addition, the ENA is periodically impacted by continental aerosols, making it an excellent location to study the cloud condensation nuclei (CCN) budget in a remote marine region periodically perturbed by anthropogenic emissions, and to investigate the impacts of long-range transport of aerosols on remote marine clouds. The Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) campaign was motivated by the need of comprehensive in-situ measurements for improving the understanding of marine boundary layer CCN budget, cloud and drizzle microphysics, and the impact of aerosol on marine low cloud and precipitation. The airborne deployments took place from June 21 to July 20, 2017 and January 15 to February 18, 2018 in the Azores. The flights were designed to maximize the synergy between in-situ airborne measurements and ongoing long-term observations at a ground site. Here we present measurements, observation strategy, meteorological conditions during the campaign, and preliminary findings. Lastly, we discuss future analyses and modeling studies that improve the understanding and representation of marine boundary layer aerosols, clouds, precipitation, and the interactions among them.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Characterization of Surface Heterogeneity-Induced Convection Using Cluster Analysis

Land-atmosphere interactions and boundary layer processes often control the formation of shallow clouds and subsequently deep convective precipitation over the Southern Great Plains. In this study, we examine the impacts of large-scale advection on the cloud populations and land-atmospheric coupling observed during the Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) field campaign in 2016. In this work, we performed two Large Eddy Simulations (LES) using the Weather Research and Forecasting Model for a day in which the transition from clear-sky to shallow precipitating clouds and isolated deep convection was observed. The control simulation reproduced the overall distribution of cloud populations by using realistic soil conditions with an interactive land model. In the sensitivity simulation where large-scale advection is removed, a strong relationship between the land and boundary layer is found. To study the timing, location, and intensity of convective initiation and the relationship of clouds with land surface properties, a cluster analysis of equivalent potential temperature is performed for the simulation without large-scale advection. That analysis shows that convective clouds first form over regions with higher surface sensible heat flux. Precipitation from those convective clouds likely triggers new updrafts nearby about two hours later through the lifting associated with cold pools. Furthermore, the cluster analysis also shows that in addition to the spatial pattern of soil moisture, land use and soil texture in western Oklahoma also influence the location of convective initiation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

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

Ammonia (NH 3 ) is an abundant trace gas in the atmosphere and an important player in atmospheric chemistry, aerosol formation and the atmosphere-surface exchange of nitrogen. It is recognized as a major source of aerosol pollution, and it may limit the formation of cloud nuclei in remote or cold parts of the atmosphere. For soil and plants, NH 3 -mediated nitrogen can act as a harmful pollutant or as a desirable nutrient, mostly in natural and agricultural settings, respectively. Agriculture is also the main source of atmospheric NH 3 via volatilization from fertilizers and manure processing in livestock farming. The accurate determination of NH 3 emission rates remains a challenge, partly due to the propensity of NH 3 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 NH 3 , using chemical ionization mass spectrometry (CIMS) with deuterated benzene cations as reagents. The setup aimed at limiting sample-surface interactions and achieved a 1-σ precision of 10–20 pptv and an immediate 1/e response rate < 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 10s 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 NH 3 h –1 for their respective momentary source rates. The fast response of the CIMS also allowed us to derive vertical NH 3 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 NH 3 emissions from surface. The corresponding analysis focused on the most suitable flight, which contained two straight-and-level legs at ~300 m above ground. We derived NH 3 fluxes between –4 and 18 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 explores the detrimental effect of measurement discontinuities. Following flux footprint estimations, comparison to the NH 3 area emissions inventory provided by the US 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 NH 3 mixing ratios, and even allow for the airborne mapping of the air-surface exchange of NH 3 .

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Tendencies of Soil Microbial NO Emissions During HI‐SCALE as Predicted by a Nitrification/Denitrification Scheme

Many atmospheric chemical processes, including the formation of secondary organic aerosol (SOA), are strongly modulated by the reactions of NO and NO 2 (NO x ). Though NO x is controlled by anthropogenic emissions near urban areas, in rural areas soil microbes can be a significant contribution to NO emission globally. The relative rates of emissions of different nitrogen-containing species (e.g., NO, N 2 O, HONO, and N 2 ) are strong functions of soil properties such as temperature, moisture content, pH, and soil carbon and nitrogen pools. However, typical large-scale biogeochemical models either express these emissions simplistically, or not at all. Here we investigate the potential impact of soil NO emissions on atmospheric chemistry and SOA formation over regional and monthly time scales, specifically the 2016 spring and summer Intensive Observational Periods (IOPs) of the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) field campaign. We implement the soil NO nitrification/denitrification parameterization of Rasool et al. (2019) into the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), supplemented by a 1-km soil moisture analysis. We then simulate both IOPs over the U.S. Great Plains, evaluating against ground stations and flight data. We show that soil NO emissions can account for a large fraction of total NO x and locally increase O 3 concentrations by up to 25%, while alleviating negative biases of gases and aerosols toward observations. Soil moisture and temperature changes between IOP1 and IOP2 lead to overall differences in emissions, but with large regional variability due to heterogeneous surface characteristics.

Atmoshpheric Chemistry↗
NASA NTRS2022

Global Reduction in Ship-tracks from Sulfur Regulations for Shipping Fuel

Ship-tracks are produced by ship-emitted aerosols interacting with low clouds. Here, we apply deep learning models on satellite data to produce the first global climatology map of ship-tracks. We show that ship-tracks are at the nexus of cloud physics, maritime shipping, and fuel regulation. Our map captures major shipping lanes while missing others because of background conditions. Ship-track frequency is more than 10 times higher than a previous survey, and its interannual fluctuations reflect variations in cross-ocean trade, shipping activity, and fuel regulations. Fuel regulation can alter both detected frequency and shipping routes due to cost. The 2020 fuel regulation, together with the coronavirus disease 2019 pandemic, reduced ship-track frequency to its lowest level in recent decades across the globe and may have ushered in an era of low frequency. The regulation reduces the aerosol indirect forcing from ship emissions by 46% or between 0.02 and 0.27 W m −2 given its current estimates.

ship tracks↗