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DOE OSTI2024

Optical constants measurements of liquids for modeling aerosolized threats

Spectroscopic identification of aerosolized chemical threats is challenging due to the complex nature of the photon/particle interaction, as well as the diversity of possible particle sizes, morphologies, and compositions. Constructing a database of laboratory - measured transmittance spectra that covers each permutation is not practical. However, calculation of the spectra using the measured optical constants as a function of wavenumber, n(?) and k(?), for each of the liquids and/or solids composing the aerosol particles provides a viable alternative. These synthetic spectra (vis-à-vis laboratory-measured spectra) can be used to identify chemicals of interest and subtract out background interferents in field measurements. Using a well-established multiple pathlength approach, we measure the optical constants n/k for liquids that may be found as chemical species of interest or common background interferents aerosolized in plumes. These measurements are also used to generate several test case aerosol synthetic spectra.

Lockwood, Schuyler↗

NASA NTRS2006

Temporal Variation of Aerosol Properties at a Rural Continental Site and Study of Aerosol Evolution through Growth Law Analysis

Aerosol size distributions were measured by a Scanning Mobility Particle Sizer (SMPS) onboard the CIRPAS Twin Otter aircraft during 16 flights at the Southern Great Plains (SGP) site in northern central Oklahoma as part of the Aerosol Intensive Operation period in May, 2003. During the same period a second SMPS was deployed at a surface station and provided continuous measurements. Combined with trace gas measurements at the SGP site and back-trajectory analysis, the aerosol size distributions provided insights into the sources of aerosols observed at the SGP site. High particle concentrations, observed mostly during daytime, were well correlated with the sulfur dioxide (SO2) mixing ratios, suggesting nucleation involving sulfuric acid is likely the main source of newly formed particles at the SGP. Aerosols within plumes originating from wildfires in Central America were measured at the surface site. Vertically compact aerosol layers, which can be traced back to forest fires in East Asia, were intercepted at altitudes over 3000 meters. Analyses of size dependent particle growth rates for four periods during which high cloud coverage was observed indicate growth dominated by volume controlled reactions. Sulfate accounts for 50% to 72% of the increase in aerosol volume concentration; the rest of the volume concentration increase was likely due to secondary organic species. The growth law analyses and meteorological conditions indicate that the sulfate was produced mainly through aqueous oxidation of SO2 in clouds droplets and hydrated aerosol particles.

Wang, Jian↗

NASA NTRS2016

Aerosol Complexity and Implications for Predictability and Short-Term Forecasting

There are clear NWP and climate impacts from including aerosol radiative and cloud interactions. Changes in dynamics and cloud fields affect aerosol lifecycle, plume height, long-range transport, overall forcing of the climate system, etc. Inclusion of aerosols in NWP systems has benefit to surface field biases (e.g., T2m, U10m). Including aerosol affects has impact on analysis increments and can have statistically significant impacts on, e.g., tropical cyclogenesis. Above points are made especially with respect to aerosol radiative interactions, but aerosol-cloud interaction is a bigger signal on the global system. Many of these impacts are realized even in models with relatively simple (bulk) aerosol schemes (approx.10 -20 tracers). Simple schemes though imply simple representation of aerosol absorption and importantly for aerosol-cloud interaction particle-size distribution. Even so, more complex schemes exhibit a lot of diversity between different models, with issues such as size selection both for emitted particles and for modes. Prospects for complex sectional schemes to tune modal (and even bulk) schemes toward better selection of size representation. I think this is a ripe topic for more research -Systematic documentation of benefits of no vs. climatological vs. interactive (direct and then direct+indirect) aerosols. Document aerosol impact on analysis increments, inclusion in NWP data assimilation operator -Further refinement of baseline assumptions in model design (e.g., absorption, particle size distribution). Did not get into model resolution and interplay of other physical processes with aerosols (e.g., moist physics, obviously important), chemistry

Predictability↗

DOE OSTI2023

Long-range transported continental aerosol in the eastern North Atlantic: three multiday event regimes influence cloud condensation nuclei

Abstract. The eastern North Atlantic (ENA) is a region dominated by pristine marine environment and subtropical marine boundary layer clouds. Under unperturbed atmospheric conditions, the regional aerosol regime in the ENA varies seasonally due to different seasonal surface-ocean biogenic emissions, removal processes, and meteorological regimes. However, during periods when the marine boundary layer aerosol in the ENA is impacted by particles transported from continental sources, aerosol properties within the marine boundary layer change significantly, affecting the concentration of cloud condensation nuclei (CCN). Here, we investigate the impact of long-range transported continental aerosol on the regional aerosol regime in the ENA using data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility on Graciosa Island in 2017 during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. We develop an algorithm that integrates number concentrations of particles with optical particle dry diameter (Dp) between 100 and 1000 nm, single scattering albedo, and black carbon concentration to identify multiday events (with duration >24 consecutive hours) of long-range continental aerosol transport in the ENA. In 2017, we detected nine multiday events of long-range transported particles that correspond to ∼ 7.5 % of the year. For each event, we perform HYSPLIT 10 d backward trajectories analysis, and we evaluate CALIPSO aerosol products to assess, respectively, the origins and compositions of aerosol particles arriving at the ENA site. Subsequently, we group the events into three categories, (1) mixture of dust and marine aerosols, (2) mixture of marine and polluted continental aerosols from industrialized areas, and (3) biomass burning aerosol from North America and Canada, and we evaluate their influence on aerosol population and cloud condensation nuclei in terms of potential activation fraction and concentrations at supersaturation of 0.1 % and 0.2 %. The arrival of plumes dominated by the mixture of dust and marine aerosol in the ENA in the winter caused significant increases in baseline Ntot. Simultaneously, the baseline particle size modes and CCN potential activation fraction remained almost unvaried, while cloud condensation nuclei concentrations increased proportionally to Ntot. Events dominated by a mixture of marine and polluted continental aerosols in spring, fall, and winter led to a statistically significant increase in baseline Ntot, a shift towards larger particular sizes, a higher CCN potential activation fractions, and cloud condensation nuclei concentrations of >170 % and up to 240 % higher than during baseline regime. Finally, the transported aerosol plumes characterized by elevated concentration of biomass burning aerosol from continental wildfires detected in the summertime did not statistically contribute to increase baseline aerosol particle concentrations in the ENA. However, particle diameters were larger than under baseline conditions, and CCN potential activation fractions were >75 % higher. Consequentially, cloud concentration nuclei concentrations increased by ∼ 115 % during the period affected by the biomass burning events. Our results suggest that, through the year, multiday events of long-range continental aerosol transport periodically affect the ENA and represent a significant source of CCN in the marine boundary layer. Based on our analysis, in 2017, the multiday aerosol plume transport dominated by a mixture of dust and marine aerosol, a mixture of marine and polluted continental aerosols, and biomass burning aerosols caused increases in the NCCN baseline regime of, respectively, 6.6 %, 8 %, and 7.4 % at SS 0.1 % (and, respectively, 6.5 %, 8.2 %, and 7.3 % at SS 0.2 %) in the ENA.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

An Infrared Database of n/k Optical Constants for Calculating Aerosol Spectra for the PICARD Program

The objective of the PICARD Program is to develop fieldable sensing platforms for the rapid chemical identification of aerosol particles in plumes. Standoff detection involves interrogating the aerosol cloud from a distance using optical methods and probing the signal returned from direct backscattering from the aerosol particles or transmitted through the plume after reflection from a retroreflector or surface of opportunity (SOO). The identification of chemical species, however, in aerosols is complicated by their complex compositions and morphologies, chemical interferants, and non-uniform particle sizes. To advance standoff detection of aerosols, modelling the infrared transmittance, reflectance and scattering spectra of aerosolized liquid and solid chemical compounds is required, and then testing that model experimentally via laboratory and field experiments. To perform accurate modeling, the infrared optical constants (n/k), i.e., the complex refractive index, of the compounds of interest are required. Thus, PNNL was tasked to provide the optical constants for a set of analytes relevant to the PICARD program. This report describes the experimental techniques used to derive the optical constants of both liquid and solid compounds using established “gold-standard” protocols, how the experimental data are processed to produce the wavenumber dependent optical constant vectors, and how the data are used in the aerosol absorption spectra modeling.

complex refractive index↗

DOE OSTI2023

Pyrocumulonimbus Events Over British Columbia in 2017: An Ensemble Model Study of Parameter Sensitivities and Climate Impacts of Wildfire Smoke in the Stratosphere

Abstract The Pyrocumulonimbus (pyroCb) events over British Columbia in 2017 were observed in the lower stratosphere for about 8–10 months after the smoke injections. Several previous studies used global climate models to investigate the physical parameters for the 2017 pyroCb events, but the conclusions show strong model dependency. In this study, we use the Energy Exascale Earth System Model (E3SM) and complete an ensemble of runs exploring three injection parameters: smoke aerosol mass, the percentage of black carbon within the smoke aerosols, and plume injection height. Additionally, we consider the heterogeneous reaction of ozone and primary organic matter. According to the satellite daily observed aerosol optical depth (AOD), we find that the best ensemble member is the simulation with 0.4 Tg of smoke, 3% of which is black carbon, a 13.5 km smoke injection height, and a 10 −5 probability factor of the heterogeneous reaction. Besides AOD, we examine the ensemble score based on the metrics used in previous studies: the metrics of the extinction coefficient at 18 km altitude and the maximum plume height. The conclusion of the best estimate of the injection parameters for 2017 pyroCb events shows strong not only model but also evaluation metric dependency. We use the Random Forest machine learning technique to quantify the relative importance of each parameter in accurately simulating the 2017 pyroCb events and find that the injection height is the most critical feature, no matter which metric is used to score the ensemble members.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRSDate not supplied

Challenges in Observing, Modeling, and Forecasting the June 2023 Smoke Event Over the Northeast United States

In the first week of May 2023, boreal Canada began an early start to the biomass burning season when fires erupted across Alberta and western Saskatchewan. Smoke entered the troposphere and spread across the United States as biomass burning emissions in Canada quadrupled the prior maximum since the onset of the MODIS satellite record. Adding to the already existing smoke, wildfires ignited in Quebec on June 2, 2023, producing a heavy plume of aerosol over the northeastern part of the continent. Meteorological factors, including an area of low pressure situated, nearly stationary, over Maine, transported the smoke into a densely populated corridor containing the cities of Washington, DC, Baltimore, Philadelphia, and New York City. Air quality alerts became widespread as near-surface levels of fine particulate matter (PM2.5) exceeded harmful levels due the low altitude of the smoke plume. Forecasting the smoke transport and impacts of such events requires a complex combination of observed initial conditions for meteorology and aerosols, knowledge of the emissions from wildfires, and a state-of-the-art Earth System model that couples these components together. Using a case-study perspective with the Goddard Earth Observing System (GEOS), challenges associated with near real time forecasting of the smoke plume are presented. Analyzed and forecasted aerosol optical depth will be evaluated using available satellite and AERONET observations, while surface aerosol will be assessed relative to observations of PM2.5. Lacking real time estimates of biomass burning emissions for inputs to our forecast model, particular attention is given to the use of day-old biomass burning emissions throughout the forecast period covering the first ten days in June 2023, and the resulting reduction in forecast skill will be quantified.

Allison Collow↗

NASA NTRSDate not supplied

Challenges in Observing, Modeling, and Forecasting the June 2023 Smoke Event over the Northeast United States

In the first week of May 2023, boreal Canada began an early start to the biomass burning season when fires erupted across Alberta and western Saskatchewan. Smoke entered the troposphere and spread across the United States as biomass burning emissions in Canada quadrupled the prior maximum since the onset of the MODIS satellite record. Adding to the already existing smoke, wildfires ignited in Quebec on June 2, 2023, producing a heavy plume of aerosol over the northeastern part of the continent. Meteorological factors, including an area of low pressure situated, nearly stationary, over Maine, transported the smoke into a densely populated corridor containing the cities of Washington, DC, Baltimore, Philadelphia, and New York City. Air quality alerts became widespread as near-surface levels of fine particulate matter (PM2.5) exceeded harmful levels due the low altitude of the smoke plume. Forecasting the smoke transport and impacts of such events requires a complex combination of observed initial conditions for meteorology and aerosols, knowledge of the emissions from wildfires, and a state-of-the-art Earth System model that couples these components together. Using a case-study perspective with the Goddard Earth Observing System (GEOS ), challenges associated with near real time forecasting of the smoke plume are presented. Analyzed and forecasted aerosol optical depth will be evaluated using available satellite and AERONET observations, while surface aerosol will be assessed relative to observations of PM2.5. Lacking real time estimates of biomass burning emissions for inputs to our forecast model, particular attention is given to the use of day-old biomass burning emissions throughout the forecast period covering the first ten days in June 2023, and the resulting reduction in forecast skill will be quantified.

Allison Collow↗

NASA NTRS1982

Airborne aerosol measurements in the quiescent plume of Mount Saint Helens September, 1980

A study of the emissions from the Mt. St. Helens volcano was conducted to obtain data for an assessment of the importance of volcanoes as a global source of volatile trace elements to the atmosphere and to the global biochemical cycles of these elements. Sampling was done on board an Orion P-3 turboprop aircraft modified for tropospheric aerosol and gas sampling. Two filter collection systems were used. Samples were collected on a single flight on September 22, 1980, at which time the volcano was emitting a stable plume to an altitude of between 2 and 3 km. The results regarding the concentrations of aerosols obtained for this mission are presented in a table. Attention is also given to data concerning particulate vs. gas phase sulfur in the Mt. Saint Helens plume, and the estimated volcanic particle flux of selected volatile elements.

Phelan, J. M.↗

NASA NTRSDate not supplied

Simulating Sulfate Aerosol Size in the Hunga Tonga Plume: Comparisons with Observations

Using the NASA GEOS Chemistry Climate Model (CCM) coupled to a detailed sectional aerosol microphysical model, we have simulated the January 2022 Hunga Tonga-Hunga Ha’apai (HTHH) plume. We have developed a version of the Global Modeling Initiative (GMI) chemistry mechanism to include the requisite sulfur chemistry and coupled it to the Community Aerosol and Radiation Model for Atmospheres (CARMA) sectional aerosol microphysics within the GEOS CCM. Our simulations focus on the lifecycle of stratospheric sulfur injected by the eruption–from the oxidation of the injected sulfur dioxide to the nucleation, growth, coagulation, hydration, and eventual settling of the volcanic sulfate aerosol particles. In order to constrain the simulated microphysics, we focus on comparing our model to observations with aerosol size information, namely in-situ particle counter observations and multi-wavelength satellite observations from OMPS-LP and SAGE-III. This eruption provides an interesting test case for our model; both the modeled gas-phase chemistry as well as the modeled aerosol microphysics are perturbed by the massive injection of water that accompanied the primary sulfur emissions from the eruption.

aerosols↗

NASA NTRS2021

Airborne and Ground-Based Measurements of Aerosol Optical Depth of Freshly Emitted Anthropogenic Plumes in the Athabasca Oil Sands Region

In this work we report the airborne aerosol optical depth (AOD) from measurements within freshly emitted anthropogenic plumes arising from mining and processing operations in the Athabasca Oil Sands Region (AOSR) in the context of ground-based AERONET climatological daily averaged AODs at Fort McMurray (Alberta, Canada). During two flights on 9 and 18 June 2018, the NASA airborne 4STAR (Spectrometers for Sky-Scanning, Sun-Tracking Atmospheric Research) Sun photometer registered high fine-mode (FM, <1 µm) in-plume AODs of up to 0.4 and 0.9, respectively, in the vicinity of the plume source (<20 km). Particle composition shows that the plumes were associated with elevated concentrations of sulfates and ammonium. These high AODs significantly exceed climatological averages for June and were not captured by the nearby AERONET instrument (mean daily AODs of 0.10±0.01 and 0.07±0.02, maximum AOD of 0.12) due possibly to horizontal inhomogeneity of the plumes, plume dilution and winds which in certain cases were carrying the plume away from the ground-based instrument. The average 4STAR out-of-plume (background) AODs deviated only marginally from AERONET daily averaged values. While 4STAR AOD peaks were generally well correlated in time with peaks in the in situ-measured particle concentrations, we show that differences in particle size are the dominant factor in determining the 4STAR-derived AOD. During the two flights of 24 June and 5 July 2018 when plumes likely travelled distances of 60 km or more, the average 4STAR FM AOD increased by 0.01–0.02 over ∼50 km of downwind particle evolution, which was supported by the increases in layer AODs calculated from the in situ extinction measurements. Based on these observations as well as the increases in organic mass, we attribute the observed AOD increase, at least in part, to secondary organic aerosol formation. The in-plume and out-of-plume AODs for this second pair of flights, in contrast to clear differences in in situ optical and other measurements, were practically indistinguishable and compared favourably to AERONET within 0.01–0.02 AOD. This means that AERONET was generally successful in capturing the background AODs, but missed some of the spatially constrained high-AOD plumes with sources as close as 30–50 km, which is important to note since the AERONET measurements are generally thought to be representative of the regional AOD loading. The fact that industrial plumes can be associated with significantly higher AODs in the vicinity of the emission sources than previously reported from AERONET can potentially have an effect on estimating the AOSR radiative impact.

AERONET↗

NASA NTRS1981

Photochemistry in planetary atmospheres

Widely varying paths of evolutionary history, atmospheric processes, solar fluxes, and temperatures have produced vastly different planetary atmospheres. The similarities and differences between the earth atmosphere and those of the terrestrial planets (Venus and Mars) and of the Jovian planets are discussed in detail; consideration is also given to the photochemistry of Saturn, Uranus, Pluto, Neptune, Titan, and Triton. Changes in the earth's ancient atmosphere are described, and problems of interest in the earth's present troposphere are discussed, including the down wind effect, plume interactions, aerosol nucleation and growth, acid rain, and the fate of terpenes. Temperature fluctuations in the four principal layers of the earth's atmosphere, predicted decreases in the ozone concentration as a function of time, and spectra of particles in the earth's upper atmosphere are also presented. Finally, the vertical structure of the Venus cloud system and the thermal structure of the Jovian planets are shown graphically.

Levine, J. S.↗

NASA NTRS1986

Generation of attenuation corrected images from lidar data

The interpretation of data generated by aerosol backscatter lidars is often facilitated by presentation of RHI and PPI images. These pictures are especially useful in studies of atmospheric boundary layer structure where convective elements, stratifications and aerosol laden plumes can be easily delineated. Procedures used at the University of Wisconsin to generate lidar images on a color enhanced raster scan display are described.

Eloranta, E. W.↗

NASA NTRS1992

A portable lidar using a diode-pumped YAG laser

A Mie lidar system is technically established and is used for monitoring air pollution, stratospheric and boundary layer aerosol distribution, plume dispersion, visibility, and the study of atmospheric structure and cloud physics. However, a lidar system is not widely used because of its cumbersome handling and unwieldy portability. Although the author developed a laser diode lidar system based on RM-CW technique, it has a limit of measurement distance. Here we report the development of an all solid Mie lidar system using a diode-pumped Nd:YAG laser and a Si-APD detector. This was constructed as a prototype of a handy lidar system.

Takeuchi, N.↗

NASA NTRS1991

Analysis of active volcanoes from the Earth Observing System

The Earth Observing System (EOS) scheduled for launch in 1997 and 1999 is briefly described, and the EOS volcanology investigation objectives are discussed. The volcanology investigation will include long- and short-term monitoring of selected volcanoes, the detection of precursor activity associated with unanticipated eruptions, and a detailed study of on-going eruptions. A variety of instruments on the EOS platforms will enable the study of local- and regional-scale thermal and deformational features of volcanoes, and the chemical and structural features of volcanic eruption plumes and aerosols.

Mouginis-Mark, Peter↗

NASA NTRS2021

Effect of volcanic emissions on clouds during the 2008 and 2018 Kilauea degassing events

Volcanic eruptions in otherwise clean environments are “natural experiments” wherein the effects of aerosol emissions on clouds and climate can be partitioned from meteorological variability and anthropogenic activities. In this work, we combined satellite retrievals, reanalysis products, and atmospheric modeling to analyze the mechanisms of aerosol–cloud interactions during two degassing events at the Kilauea volcano in 2008 and 2018. The eruptive nature of the 2008 and 2018 degassing events was distinct from long-term volcanic activity for Kilauea. Although previous studies assessed the modulation of cloud properties from the 2008 event, this is the first time such an analysis has been reported for the 2018 event and that multiple degassing events have been analyzed and compared at this location. Both events resulted in significant changes in cloud effective radius and cloud droplet number concentration that were decoupled from local meteorology and in line with an enhanced cloud albedo. However, it is likely that the effects of volcanic emissions on liquid water path and cloud fraction were largely offset by meteorological variability. Comparison of cloud anomalies between the two events suggested a threshold response of aerosol–cloud interactions to overcome meteorological effects, largely controlled by aerosol loading. In both events, the ingestion of aerosols within convective parcels enhanced the detrainment of condensate in the upper troposphere, resulting in deeper clouds than observed under pristine conditions. Accounting for ice nucleation on ash particles led to enhanced ice crystal concentrations at cirrus levels and a slight decrease in ice water content, improving the correlation of the model results with the satellite retrievals. Overall, aerosol loading, plume characteristics, and meteorology contributed to changes in cloud properties during the Kilauea degassing events.

Katherine H. Breen↗

DOE OSTI2021

The influence of fire aerosols on surface climate and gross primary production in the Energy Exascale Earth System Model (E3SM)

Fire-emitted aerosols play an important role in influencing Earth’s climate, directly by scattering and absorbing radiation and indirectly by influencing cloud microphysics. The quantification of fire-aerosol interactions, however, remains challenging and subject to uncertainties in emissions, plume parameterizations, and aerosol properties. Here we optimized fire-associated aerosol emissions in the Energy Exascale Earth System Model (E3SM) using the Global Fire Emissions Database (GFED) and AERONET aerosol optical depth (AOD) observations during 1997-2016. Furthermore, we distributed fire emissions vertically using smoke plume heights from Multi-angle Imaging SpectroRadiometer (MISR) satellite observations. From the optimization, we estimate that global fires emit 45.5 Tg y -1 of primary particulate organic matter and 3.9 Tg y -1 of black carbon. We then performed two climate simulations with and without the optimized fire emissions. We find that fire aerosols significantly increase global AOD by 14 ± 7% and contribute to a reduction in net shortwave radiation at the surface (-2.3 ± 0.5 W m -2 ). Together, fire-induced direct and indirect aerosol effects cause annual mean global land surface air temperature to decrease by 0.17 ± 0.15°C, relative humidity to increase by 0.4 ± 0.3%, and diffuse light fraction to increase by 0.5 ± 0.3%. In response, GPP declines by 2.8 Pg C y -1 , as a result of large positive drivers (decreases in temperature and increases in humidity and diffuse light) nearly cancelling out large negative drivers (decreases shortwave radiation and soil moisture). Our analysis highlights the importance of fire aerosols in modifying surface climate and photosynthesis across the tropics.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Aerosol size distribution changes in FIREX-AQ biomass burning plumes: the impact of plume concentration on coagulation and OA condensation/evaporation

Abstract. The evolution of organic aerosol (OA) and aerosol size distributions within smoke plumes is uncertain due to the variability in rates of coagulation and OA condensation/evaporation between different smoke plumes and at different locations within a single plume. We use aircraft data from the FIREX-AQ campaign to evaluate differences in evolving aerosol size distributions, OA, and oxygen to carbon ratios (O:C) between and within smoke plumes during the first several hours of aging as a function of smoke concentration. The observations show that the median particle diameter increases faster in smoke of a higher initial OA concentration (>1000 µg m−3), with diameter growth of over 100 nm in 8 h – despite generally having a net decrease in OA enhancement ratios – than smoke of a lower initial OA concentration (<100 µg m−3), which had net increases in OA. Observations of OA and O:C suggest that evaporation and/or secondary OA formation was greater in less concentrated smoke prior to the first measurement (5–57 min after emission). We simulate the size changes due to coagulation and dilution and adjust for OA condensation/evaporation based on the observed changes in OA. We found that coagulation explains the majority of the diameter growth, with OA evaporation/condensation having a relatively minor impact. We found that mixing between the core and edges of the plume generally occurred on timescales of hours, slow enough to maintain differences in aging between core and edge but too fast to ignore the role of mixing for most of our cases.

54 ENVIRONMENTAL SCIENCES↗