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DOE OSTI2025

Chemical Imaging of Atmospheric Biomass Burning Particles from North American Wildfires

The effects of biomass burning aerosols (BBA) on radiative forcing and cloud formation depend on chemical composition and the internal structures of individual particles within smoke plumes. To improve our understanding of the chemical and physical properties of BBA emitted at different times of the day and their evolution during atmospheric aging, we conducted a study as a part of the Fire Influence on Regional to Global Environments and Air Quality field campaign. Particle samples were collected onboard a research aircraft from smoke plumes from a wildfire in eastern Oregon during late afternoon and nighttime flights on August 28, 2019. A time-resolved aerosol collector was used to collect samples on substrates for offline spectromicroscopic imaging to investigate the single-particle characteristics of BBA particles. Approximately 20,400 individual particles from 10 selected samples were analyzed using computer-controlled scanning electron microscopy coupled with energy-dispersive X-ray microanalysis, revealing their elemental composition, morphology, and viscosity. Elemental microanalysis indicated that aged potassium is likely found in the form of K 2 SO 4 , KNO 3 , and possible K-organic salts. Further chemical speciation and carbon bonding mapping within individual particles were conducted using synchrotron-based scanning transmission X-ray microscopy (STXM) coupled with near edge X-ray absorption fine structure (NEXAFS) spectroscopy. Real-time, water-soluble light absorption measurements were acquired using a particle-into-liquid sampler instrument coupled to a liquid waveguide capillary cell and total organic analyzer. In the late afternoon samples, 65% of the total particle number population consisted entirely of organic components, compared to 46% in the nighttime particles. These differences were attributed to discrepancies in composition at the time of emission and to the daytime condensation and accumulation of photochemically formed secondary organic material on existing BBA particles, a process that halts at night. Microscopy images indicated that particle viscosity was lower in the nighttime particles (<10 1 Pa·s), likely due to increased relative humidity and a higher contribution from hygroscopic inorganic components. The chemical heterogeneity of individual particles was quantified using STXM-derived mixing state parameters. The nature of carbon bonding within individual particles was inferred from the extent of carbon sp 2 hybridization derived from NEXAFS spectra. Average percentages of sp 2 hybridization range between 40% and 60%, with no noticeable differences between late afternoon and nighttime flights. These findings were compared with the online optical properties of both late afternoon and nighttime smoke plumes, providing valuable insights into the complex relationship between chemical composition and optical properties of BBA particles at different times of the day.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Efficient Nighttime Biogenic SOA Formation in a Polluted Residual Layer

Abstract Organic nitrates formed from nighttime reaction between anthropogenic nitrate radicals (NO3) and biogenic volatile organic compounds (BVOCs) are potentially an important but highly uncertain source of secondary organic aerosol (SOA). Here we report on the enhanced nighttime biogenic SOA formation observed in a polluted residual layer over Sacramento, California, the morning of 15 June 2010 during the Carbonaceous Aerosols and Radiative Effects Study (CARES). Trajectory analysis showed that the residual layer air, containing trace amounts of isoprene and monoterpenes left over after nighttime oxidation, was influenced by the San Francisco Bay Area emissions the previous evening. The residual layer aerosol was also enriched in nitrate, with about 64% of it estimated to be in the form of organic nitrates. The nitrate:organic mass ratio of the SOA was about 0.47±0.044, which corresponds to the range typically found in isoprene mononitrates. Assuming the SOA was composed of organic mononitrates, its nominal molecular weight was estimated at 186±11 g mol-1, consistent with the highly functionalized isoprene hydroxynitrates that have been observed in the particle phase in the southeast United States. Overall, our findings show that the efficiency of nighttime biogenic SOA formation, expressed as the change in organic aerosol mass relative to carbon monoxide (?OA/?CO), was about 100 µg m-3 ppmv, which falls in the range 77-157 µg m-3 ppmv previously estimated for enhanced daytime SOA formation from mixed anthropogenic and biogenic emissions during CARES.

Zaveri, Rahul A.↗

DOE OSTI2022

Particle phase-state variability in the North Atlantic free troposphere during summertime is determined by atmospheric transport patterns and sources

Abstract. Free tropospheric aerosol particles have important but poorly constrained climate effects due to transformations of their physicochemical properties during long-range transport. In this study, we investigate the chemical composition and provide an overview of the phase states of individual particles that have undergone long-range transport over the North Atlantic Ocean in June and July 2014, 2015, and 2017 to the Observatory of Mount Pico (OMP) in the Azores. The OMP is an ideal site for studying long-range-transported free tropospheric particles because local emissions have a negligible influence and contributions from the boundary layer are rare. We used the FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) to determine the origins and transport trajectories of sampled air masses and found that most of them originated from North America and recirculated over the North Atlantic Ocean. The FLEXPART analysis showed that the sampled air masses were highly aged (average plume age >10 d). Size-resolved chemical compositions of individual particles were probed using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). CCSEM-EDX results showed that the most abundant particle types were carbonaceous (∼ 29.9 % to 82.0 %), sea salt (∼ 0.3 % to 31.6 %), and sea salt with sulfate (∼ 2.4 % to 31.5 %). We used a tilted stage interfaced within an environmental scanning electron microscope (ESEM) to determine the phase states of individual submicron particles. We found that most particles (∼ 47 % to 99 %) were in the liquid state at the time of collection due to inorganic inclusions. Moreover, we also observed substantial fractions of solid and semisolid particles (∼ 0 % to 30 % and ∼ 1 % to 42 %, respectively) during different transport patterns and events, reflecting the particles' phase-state variability for different atmospheric transport events and sources. Combining phase state measurements with FLEXPART CO tracer analysis, we found that wildfire-influenced plumes can result in particles with a wide range of viscosities after long-range transport in the free troposphere. We also used temperature and RH values extracted from the Global Forecast System (GFS) along the FLEXPART-simulated path to predict the phase state of the particles during transport and found that neglecting internal mixing with inorganics would lead to an overestimation of the viscosity of free tropospheric particles. Our findings warrant future investigation aiming at the quantitative assessment of the influence of internal mixing on the phase states of the individual particles. This study also provides insights into the chemical composition and phase state of free tropospheric particles, which can help models to reduce uncertainties about the effects of ambient aerosol particles on climate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

The Role of the Toroidal Vortex in Cumulus Clouds' Entrainment and Mixing

Abstract Shallow convective clouds play a crucial role in Earth's energy budget, as they modulate the radiative transfer in the atmosphere and participate in the vertical transport of aerosols, energy, and humidity. The parameterizations representing these complex, vital players in weather and climate models are mostly based on a description of steady‐state plumes and are a source of major uncertainty. Recently, several studies have shown that buoyant thermals are inherent in atmospheric convection and contain a toroidal (ring) vortex. This work studies those vortices in growing shallow cumulus (Cu) clouds using high‐resolution (10 m) Large Eddy Simulations that resolve these vortices in much detail. Recent analysis of such data showed that small‐scale turbulent diffusion is unable to explain the large diluted portion of the cloud. Here we advocate for the important role of the Cu toroidal vortex (TV) in cloud dilution and present the complex dynamics and structure of a Cu TV. Nevertheless, since the vortex dominates the cloud's dilution, simplicity emerges when considering the cloud's lateral mass flux profile. The cloud mixing is quantified using direct flux calculations and Eulerian tracers. In addition, Lagrangian tracers are used to identify the origin of the entrained air and its thermodynamic properties. It shows that most of the air entrained by the vortex is not recycled by the vortex, yet is significantly more humid than the environment. We suggest that the development of new models describing thermals, together with their toroidal vortices, might improve cloud parameterizations in weather and climate models.

Meteorology & Atmospheric Sciences↗

DOE OSTI2022

Molecular Characterization of Organosulfate-Dominated Aerosols over Agricultural Fields from the Southern Great Plains by High-Resolution Mass Spectrometry

The molecular composition of organic aerosols, especially for day/nighttime variations of organosulfates above agricultural fields, is not well understood despite profound impacts on regional climate, crop production, air quality, and human health. Here, nanospray desorption electrospray ionization with high-resolution mass spectrometry (nano-DESI-HRMS) is used to interrogate the molecular composition of organic aerosols collected at the Southern Great Plains, located in an agricultural region of Oklahoma. Identified molecular formulae featured carbon, hydrogen, oxygen (CHO), nitrogen (CHNO), and/or sulfur (CHOS, CHNOS), with higher organosulfate proportions during daytime (41%) compared to nighttime (30%). In this work, nighttime aerosols featured increases in CHO, CHNO, and extremely low volatility organic carbon (ELVOC) species. However, due to high relative humidity, the nighttime aerosols phase state was found to be more liquid-like than daytime aerosols using parametrized glass transition temperatures. Aerosol molecular composition from an anthropogenically influenced plume (southerly winds) showed significant increases in CHOS and ELVOC species. By comparison with chamber studies, CHOS species are suspected to be of mixed biogenic and anthropogenic origin, whereas CHNOS species (not identified in the southerly winds) are suggested to predominately be of biogenic origin. Overall, this study provides key insight into organosulfates above agricultural fields, demonstrating dependence upon day/night cycles and episodic anthropogenic emissions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2011

Integration of Dust Prediction Systems and Vegetation Phenology to Track Pollen for Asthma Alerts in Public Health

Pollen can be transported great distances. Van de Water et. al., 2003 reported Juniperus pollen, a significant aeroallergen was transported 200-600 km. Hence local observations of plant phenology may not be consistent with the timing and source of pollen collected by pollen sampling instruments. The DREAM (Dust REgional Atmospheric Model, Yin 2007) is a verified model for atmospheric dust transport modeling using MODIS data products to identify source regions and quantities of dust (Yin 2007). The use of satellite data products for studying phenology is well documented (White and Nemani 2006). We are modifying the DREAM model to incorporate pollen transport. The linkages already exist with DREAM through PHAiRS (Public Health Applications in remote Sensing) to the public health community. This linkage has the potential to fill this data gap so that health effects of pollen can better be tracked for linkage with health outcome data including asthma, respiratory effects, myocardial infarction, and lost work days. DREAM is based on the SKIRON/Eta modeling system and the Eta/NCEP regional atmospheric model. The dust modules of the entire system incorporate the state of the art parameterizations of all the major phases of the atmospheric dust life such as production, diffusion, advection, and removal. These modules also include effects of the particle size distribution on aerosol dispersion. The dust production mechanism is based on the viscous/turbulent mixing, shear-free convection diffusion, and soil moisture. In addition to these sophisticated mechanisms, very high resolution databases, including elevation, soil properties, and vegetation cover are utilized. The DREAM model was modified to use pollen sources instead of dust (PREAM). Pollen release will be estimated based on satellite-derived phenology of Juniperus spp. communities. The MODIS surface reflectance product (MOD09) will provide information on the start of the plant growing season, growth stage, peak greenness, dry-down and pollen release. Ground based observational records of pollen release timing and quantities will be used as verification. Techniques developed using MOD09 surface reflectance products will be directly applicable to the next generation sensors such as VIIRS. The resulting deterministic model for predicting and simulating pollen emission and downwind concentration to study details of phenology and meteorology and their dependencies. This information will be used to support the Centers for Disease Control and Prevention (CDC)'s National Environmental Public Health Tracking Program (EPHT) and the State of New Mexico environmental public health decision support for asthma and allergies alerts

Luvall, Jeffrey C.↗

DOE OSTI2025

The Energy Exascale Earth System Model Version 3: 1. Overview of the Atmospheric Component

This paper describes the atmospheric component of the US Department of Energy's Energy Exascale Earth System Model (E3SM) version 3. Significant updates have been made to the atmospheric physics compared to earlier versions. Specifically, interactive gas chemistry has been implemented, along with improved representations of aerosols and dust emissions. A new stratiform cloud microphysics scheme more physically treats ice processes and aerosol‐cloud interactions. The deep convection parameterization has been largely improved with sophisticated microphysics for convective clouds, making model convection sensitive to large‐scale dynamics, and incorporating the dynamical and physical effects of organized mesoscale convection. Improvements in aerosol wet removal processes and parameter re‐tuning of key aerosol and cloud processes have improved model aerosol radiative forcing. The model's vertical resolution has increased from 72 to 80 layers with the extra eight layers added in the lower stratosphere to better simulate the Quasi‐Biennial Oscillation. These improvements have enhanced E3SM's capability to couple aerosol, chemistry, and biogeochemistry and reduced some long‐standing biases in simulating tropical variability. Compared to its predecessors, the model shows a much stronger signal for the Madden‐Julian Oscillation, Kelvin waves, mixed Rossby‐gravity waves, and eastward inertia‐gravity waves. Aerosol radiative forcing has been considerably reduced and is now better aligned with community best estimates, leading to significantly improved skill in simulating historical temperature records. Its simulated mean‐state climate is largely comparable to E3SMv2, but with some notable degradation in shortwave cloud radiative effect, precipitable water, and surface wind stress, which will be addressed in future updates.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2007

Multi-Layer Arctic Mixed-Phase Clouds Simulated by a Cloud-Resolving Model: Comparison with ARM Observations and Sensitivity Experiments

A cloud-resolving model (CRM) is used to simulate the multiple-layer mixed-phase stratiform (MPS) clouds that occurred during a three-and-a-half day subperiod of the Department of Energy-Atmospheric Radiation Measurement Program s Mixed-Phase Arctic Cloud Experiment (M-PACE). The CRM is implemented with an advanced two-moment microphysics scheme, a state-of-the-art radiative transfer scheme, and a complicated third-order turbulence closure. Concurrent meteorological, aerosol, and ice nucleus measurements are used to initialize the CRM. The CRM is prescribed by time-varying large-scale advective tendencies of temperature and moisture and surface turbulent fluxes of sensible and latent heat. The CRM reproduces the occurrences of the single- and double-layer MPS clouds as revealed by the M-PACE observations. However, the simulated first cloud layer is lower and the second cloud layer thicker compared to observations. The magnitude of the simulated liquid water path agrees with that observed, but its temporal variation is more pronounced than that observed. As in an earlier study of single-layer cloud, the CRM also captures the major characteristics in the vertical distributions and temporal variations of liquid water content (LWC), total ice water content (IWC), droplet number concentration and ice crystal number concentration (nis) as suggested by the aircraft observations. However, the simulated mean values differ significantly from the observed. The magnitude of nis is especially underestimated by one order of magnitude. Sensitivity experiments suggest that the lower cloud layer is closely related to the surface fluxes of sensible and latent heat; the upper cloud layer is probably initialized by the large-scale advective cooling/moistening and maintained through the strong longwave (LW) radiative cooling near the cloud top which enhances the dynamical circulation; artificially turning off all ice-phase microphysical processes results in an increase in LWP by a factor of 3 due to interactions between the excessive LW radiative cooling and extra cloud water; heating caused by phase change of hydrometeors could affect the LWC and cloud top height by partially canceling out the LW radiative cooling. It is further shown that the resolved dynamical circulation appears to contribute more greatly to the evolution of the MPS cloud layers than the parameterized subgrid-scale circulation.

Luo, Yali↗

DOE OSTI2024

Lightning and Radar Measures of Mixed-Phase Updraft Variability in Tracked Storms during the TRACER Field Campaign in Houston, Texas

Properties of 7488 thunderstorms are summarized for June–September 2022 during the Tracking Aerosol Convection Interactions Experiment (TRACER) field campaign Houston, Texas, using polarimetric weather radar and VHF 3D Lightning Mapping Array data. Automated tracking of storms linked each instrument’s measurements to a data-defined, time-evolving storm footprint. Within each storm, the depth and magnitude of episodic columns of radar differential reflectivity and specific differential phase quantified the prevalence of updrafts that activated mixed-phase precipitation pathways. Lightning measurements further distinguished the degree of rimed precipitation formation: the fraction of tracks with lightning varied from day to day and cells with lightning had stronger polarimetric columns. Track-level correlation of the lightning flash rate with radar polarimetric measures had substantial spread, showing that lightning provides an additional signal of mixed-phase precipitation processes that can complement future studies of thermodynamic and aerosol controls on cloud microphysics in the Houston region.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1990

Differential absorption lidar detection of ozone in the troposphere and lower stratosphere

The DIAL technique for deriving O3 profiles from lidar measurements is discussed. Examples of a variety of O3 and aerosol measurements are presented from studies of (1) photochemically produced O3 in the summertime over the eastern United States and in biomass burning plumes during the dry season over the Amazon Basin of Brazil; (2) vertical O3 transport from the mixed layer into the free troposphere via cloud dynamics and from the stratosphere into the troposphere via tropopause fold events; and (3) O3 depletion in the O3 hole over Antarctica. The NASA airborne DIAL system is considered to be an advanced field system.

Browell, E. V.↗

DOE OSTI2026

Understanding the causes of satellite–model discrepancies in aerosol–cloud interactions using near-LES simulations of marine boundary layer clouds

Aerosol–cloud interactions (ACI) remain the largest source of uncertainty in model estimates of anthropogenic radiative forcing, primarily because of deficiencies in representing aerosol–cloud microphysical processes that lead to inconsistent cloud liquid water path (LWP) responses to aerosol perturbations between observations and models. To investigate this discrepancy, we conducted a series of large-eddy-scale simulations driven by realistic meteorology over the eastern North Atlantic, and evaluated LWP susceptibility, precipitation processes, and boundary layer thermodynamics using satellite and ground-based observations. Simulated LWP responses show a strong dependence on cloud state. Non-precipitating thin clouds exhibit a modest LWP decrease with increasing cloud droplet number concentration (N d ), consistent in sign but weaker in magnitude than satellite estimates, reflecting enhanced turbulent mixing and evaporation. The largest model-observation discrepancy occurs in non-precipitating thick clouds, where simulated LWP susceptibilities are strongly positive (+0.32) while observations indicate large negative values (−0.69). This discrepancy stems from excessive precipitation driven by underestimated entrainment, overly active accretion, and overly broad drop-size distributions in polluted conditions. While our high-resolution setup mitigates the excessive drizzling common in coarser models and captures key regime transitions, these biases persist – highlighting that improved parameterizations of cloud-top processes, precipitation, and aerosol effects are needed beyond simply increasing model resolution. Additionally, misrepresented moisture inversions in reanalysis introduce a moist bias in cloud-top relative humidity, further amplifying positive LWP susceptibility. Our results also suggest that large negative N d –LWP relationships in observations may reflect internal cloud processes rather than true ACI effects.

Aerosol-cloud interaction↗

NASA NTRS1975

Studies on possible propagation of microbial contamination in planetary atmospheres

Maintained aerosols were studied to demonstrate the metabolism and propagation of microbes in clouds which could occur in the course of a probe of a planetary atmosphere. Bacteriophage was used as a tool to test whether the mechanisms for DNA production remain intact and functional within the airborne bacterial cell. In one test method, bacteria were mixed with coliphage in an atomizer to allow attachment before aerosolization; in another, two suspensions were atomized saperately into a common air stream prior to aerosolization. Results show that biochemical and physiological mechanisms to allow aerobic microbes to propagate in the airborne state do exist.

Dimmick, R. L.↗

NASA NTRS2021

Preconditioning of overcast-to-broken cloud transitions by riming in marine cold air outbreaks

Marine cold air outbreaks (CAOs) commonly form overcast cloud decks that transition into broken cloud fields downwind, dramatically altering the local radiation budget. In this study, we investigate the impact of frozen hydrometeors on these transitions. We focus on a CAO case in the NW Atlantic, the location of the multi-year flight campaign ACTIVATE (Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment). We use MERRA-2 (Modern-Era Retrospective analysis for Research and Applications, version 2) reanalysis fields to drive large eddy simulations with mixed-phase two-moment microphysics in a Lagrangian framework. We find that transitions are triggered by substantial rain (rainwater paths >25 g m−2), and only simulations that allow for aerosol depletion result in sustained breakups, as observed. Using a range of diagnostic ice nucleating particle concentrations, Ninp, we find that increasing ice progressively accelerates transitions, thus abbreviating the overcast state. Ice particles affect the cloud-topped boundary layer evolution, primarily through riming-related processes prior to substantial rain, leading to (1) a reduction in cloud liquid water, (2) early consumption of cloud condensation nuclei, and (3) early and light precipitation cooling and moistening below cloud. We refer to these three effects collectively as “preconditioning by riming”. Greater boundary layer aerosol concentrations available as cloud condensation nuclei (CCN) delay the onset of substantial rain. However, cloud breakup and low CCN concentration final stages are found to be inevitable in this case, due, primarily, to liquid water path buildup. An ice-modulated cloud transition speed suggests the possibility of a negative cloud–climate feedback. To address prevailing uncertainties in the model representation of mixed-phase processes, the magnitude of ice formation and riming impacts and, thereby, the strength of an associated negative cloud–climate feedback process, requires further observational evaluation by targeting riming hot spots with in situ imaging probes that allow for both the characterization of ice particles and abundance of supercooled droplets.

Marine cold air outbreaks↗

DOE OSTI2021

Toward closure between predicted and observed particle viscosity over a wide range of temperatures and relative humidity

Abstract. Atmospheric aerosols can exist in amorphous semi-solid or glassy phase states whose viscosity varies with atmospheric temperature and relative humidity. The temperature and humidity dependence of viscosity has been hypothesized to be predictable from the combination of a water–organic binary mixing rule of the glass transition temperature, a glass-transition-temperature-scaled viscosity fragility parameterization, and a water uptake parameterization. This work presents a closure study between predicted and observed viscosity for sucrose and citric acid. Viscosity and glass transition temperature as a function of water content are compiled from literature data and used to constrain the fragility parameterization. New measurements characterizing viscosity of sub-100 nm particles using the dimer relaxation method are presented. These measurements extend the available data of temperature- and humidity-dependent viscosity to −28 ∘C. Predicted relationships agree well with observations at room temperature and with measured isopleths of constant viscosity at ∼107 Pa s at temperatures warmer than −28 ∘C. Discrepancies at colder temperatures are observed for sucrose particles. Simulations with the kinetic multi-layer model of gas–particle interactions suggest that the observed deviations at colder temperature for sucrose can be attributed to kinetic limitations associated with water uptake at the timescales of the dimer relaxation experiments. Using the available information, updated equilibrium phase-state diagrams (-80∘C

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Influence of Gel Formation on the Heterogeneous Oxidation of Organic Aerosol

Recent work has shown that divalent cations can perturb the viscosity and phase state of oxygenated organic particles in unexpected ways, sometimes leading to the formation of gel states. Despite the prevalence of divalent cations and oxygenated organic molecules in atmospheric aerosol, particularly in marine environments, the influence of gel states on the reaction rates is not well established. Here, in this work, we measure and compare the impact of viscosity and gel formation on the ozonolysis chemistry of aerosol particles containing the unsaturated, oxygenated organic species ascorbic acid (AA). AA serves as an excellent proxy compound for highly oxidized molecules in the atmosphere. We measured the hygroscopic growth, phase state, viscosity, and water diffusion rate in binary particles containing AA and water and in ternary particles with an additional co-solute of either ammonium sulfate or CaCl 2 . These measurements reveal gel formation in particles mixed with CaCl 2 , as particles become rigid but allow for relatively rapid diffusion rates of water, consistent with previous observations of gel behavior. We measured the rate of ozonolysis of these particles under a range of relative humidity (RH) conditions, showing a clear decrease in the rate with decreasing RH, consistent with the increase in viscosity and slowed diffusion. Notably, we measured the rate of ozonolysis of particles existing in a gel state, showing that following an initial period of decay, the rate of reaction arrests, indicating that the organic material in the solid state is protected from the reaction. This work shows that viscous particles and gel particles exhibit different reactivity toward heterogeneous oxidants, with significant implications for how we understand the chemical evolution of aerosol particles in the atmosphere.

gels↗

NASA NTRS2010

Airborne and Ground-Based Measurements Using a High-Performance Raman Lidar

A high-performance Raman lidar operating in the UV portion of the spectrum has been used to acquire, for the first time using a single lidar, simultaneous airborne profiles of the water vapor mixing ratio, aerosol backscatter, aerosol extinction, aerosol depolarization and research mode measurements of cloud liquid water, cloud droplet radius, and number density. The Raman Airborne Spectroscopic Lidar (RASL) system was installed in a Beechcraft King Air B200 aircraft and was flown over the mid-Atlantic United States during July August 2007 at altitudes ranging between 5 and 8 km. During these flights, despite suboptimal laser performance and subaperture use of the telescope, all RASL measurement expectations were met, except that of aerosol extinction. Following the Water Vapor Validation Experiment Satellite/Sondes (WAVES_2007) field campaign in the summer of 2007, RASL was installed in a mobile trailer for groundbased use during the Measurements of Humidity and Validation Experiment (MOHAVE-II) field campaign held during October 2007 at the Jet Propulsion Laboratory s Table Mountain Facility in southern California. This ground-based configuration of the lidar hardware is called Atmospheric Lidar for Validation, Interagency Collaboration and Education (ALVICE). During theMOHAVE-II field campaign, during which only nighttime measurements were made, ALVICE demonstrated significant sensitivity to lower-stratospheric water vapor. Numerical simulation and comparisons with a cryogenic frost-point hygrometer are used to demonstrate that a system with the performance characteristics of RASL ALVICE should indeed be able to quantify water vapor well into the lower stratosphere with extended averaging from an elevated location like Table Mountain. The same design considerations that optimize Raman lidar for airborne use on a small research aircraft are, therefore, shown to yield significant dividends in the quantification of lower-stratospheric water vapor. The MOHAVE-II measurements, along with numerical simulation, were used to determine that the likely reason for the suboptimal airborne aerosol extinction performance during theWAVES_2007 campaign was amisaligned interference filter. With full laser power and a properly tuned interference filter,RASL is shown to be capable ofmeasuring themain water vapor and aerosol parameters with temporal resolutions of between 2 and 45 s and spatial resolutions ranging from 30 to 330 m from a flight altitude of 8 km with precision of generally less than 10%, providing performance that is competitive with some airborne Differential Absorption Lidar (DIAL) water vapor and High Spectral Resolution Lidar (HSRL) aerosol instruments. The use of diode-pumped laser technology would improve the performance of an airborne Raman lidar and permit additional instrumentation to be carried on board a small research aircraft. The combined airborne and ground-based measurements presented here demonstrate a level of versatility in Raman lidar that may be impossible to duplicate with any other single lidar technique.

Whiteman, David N.↗

NASA NTRS1990

The polar stratospheric cloud event of January 24. II - Photochemistry

During the 1988/89 Airborne Arctic Stratospheric Expedition (AASE), observations of the chemical composition, aerosol characteristics and atmospheric state were obtained from two aircraft, a NASA ER-2 and a DC-8. This paper presents a diagnosis of observations obtained using the ER-2 on January 24, 1989, using a Lagrangian coupled microphysical-photochemical model. The high chlorine monoxide mixing ratios observed from the ER-2 on the afternoon of January 24, 1989 are interpreted as a result of in situ heterogeneous release of reactive chlorine from the reservoirs HCl and CIONO2 on type-1 polar stratospheric cloud particles observed to be present at that time. This essential element in theories of polar ozone depletion has never before been observed directly in the stratosphere.

Jones, R. L.↗

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↗