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All sourcesNASA NTRSDOE OSTI
NASA NTRS2012

Estimation and Bias Correction of Aerosol Abundance using Data-driven Machine Learning and Remote Sensing

Air quality information is increasingly becoming a public health concern, since some of the aerosol particles pose harmful effects to peoples health. One widely available metric of aerosol abundance is the aerosol optical depth (AOD). The AOD is the integrated light extinction coefficient over a vertical atmospheric column of unit cross section, which represents the extent to which the aerosols in that vertical profile prevent the transmission of light by absorption or scattering. The comparison between the AOD measured from the ground-based Aerosol Robotic Network (AERONET) system and the satellite MODIS instruments at 550 nm shows that there is a bias between the two data products. We performed a comprehensive analysis exploring possible factors which may be contributing to the inter-instrumental bias between MODIS and AERONET. The analysis used several measured variables, including the MODIS AOD, as input in order to train a neural network in regression mode to predict the AERONET AOD values. This not only allowed us to obtain an estimate, but also allowed us to infer the optimal sets of variables that played an important role in the prediction. In addition, we applied machine learning to infer the global abundance of ground level PM2.5 from the AOD data and other ancillary satellite and meteorology products. This research is part of our goal to provide air quality information, which can also be useful for global epidemiology studies.

Malakar, Nabin K.↗
DOE OSTI2025

Explosive Soot Challenge (Final Report)

This project assembled a broad ensemble of modeling and experimentation tools to study the morphological and optical properties of detonation soots in explosive fireballs. A gram-scale hemispherical high explosive was studied in a low-pressure controlled environment using in-situ experimentation with diffusely illuminated visible absorption spectroscopy, particle sizing through light scattering techniques, and post-test collections with subsequent morphological analysis. Hydrocode modeling was performed to replicate the detonation flow observations, and subsequent aerosol kinetics models provided particle size distributions and extinction coefficients from the hydrocode results. Experimentally observed soot morphologies agreed with expectation from the literature - a bimodal distribution was found, brought upon by the particles growing to a size where their inertia and fluid wakes are non-negligible. The aerosol kinetics model did not replicate the observed bimodal size distribution for lack of a coagulation kernel to represent the behavior. To recover particulate optical properties, a spectrally resolved absorption spectroscopy method termed Spectral diffuse back-illuminated extinction imaging (SBI-EI) was developed and implemented on two explosive types. Inverting the absorption spectra using a Kramers-Kronig consistent method yielded the complex index of refraction for the soots produced by the explosives. This method resulted in an unrealistic index of refraction for one of the two explosives, and this is suspected to be due to the model neglecting scattering brought upon by the large particle sizes observed. In addition to the core work, three additional studies were performed in parallel. These investigated the impact of scattering on diffuse absorption spectroscopy, studied how soots oxidate and sublimate in a well-controlled shock tube, and laid the theoretical groundwork for a new collision kernel to replicate the bimodal size distribution from the observations. Summaries of these efforts are included at the end of this report.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗
NASA NTRS2022

Simultaneous Retrievals of Biomass Burning Aerosols and Trace Gases From the Ultraviolet to Near-Infrared Over Northern Thailand During the 2019 Pre-Monsoon Season

With the advent of spaceborne spectroradiometers in a geostationary constellation, measuring high spectral resolution ultraviolet–visible (UV-VIS) and selected near-/shortwave-infrared (NIR/SWIR) radiances can enable the probing of the life cycle of key atmospheric trace gases and aerosols at higher temporal resolutions over the globe. The UV-VIS measurements are important for retrieving several key trace gases (e.g., O 3 , SO 2 , NO 2 , and HCHO) and particularly for deriving aerosol characteristics (e.g., aerosol absorption and vertical profile). This study examines the merit of simultaneous retrievals of trace gases and aerosols using a ground-based spectroradiometer covering the UV-NIR to monitor their physicochemical processes and to obtain reliable aerosol information for various applications. During the 2019 pre-monsoon season over northern Thailand, we deployed a ground-based SMART–s (Spectral Measurements for Atmospheric Radiative Transfer–spectroradiometer) instrument, which is an extended-range Pandora with reliable radiometric calibration in the 330–820 nm range, to retrieve remotely sensed chemical and aerosol properties for the first time near biomass burning sources. The high spectral resolution (∼ 1.0 nm full width half maximum with ∼ 3.7 × oversampling) of sun and sky measurements from SMART–s provides several key trace gases (e.g., O 3 , NO 2 , and H 2 O) and aerosol properties covering the UV where significant light absorption occurs by the carbonaceous particles. During the measurement period, highly correlated total column amounts of NO 2 and aerosol optical thickness (т aer ) retrieved from SMART–s (correlation coefficient, R=0.74) indicated their common emissions from biomass burning events. The SMART–s retrievals of the spectral single scattering albedo (ω 0 ) of smoke aerosols showed an abrupt decrease in the UV, which is an important parameter dictating photochemical processes in the atmosphere. The values of ω 0 and column precipitable water vapor (H 2 O) gradually increase with the mixing of biomass burning smoke particles and higher water vapor concentrations when approaching the monsoon season. The retrieved ω 0 and weighted mean radius of fine-mode aerosols from SMART–s showed positive correlations with the H 2 O (R=0.81 for ω 0 at 330 nm and 0.56 for the volume-weighted mean radius), whereas the real part of the refractive index of fine-mode aerosol (n f ) showed negative correlations (R = -0.61 at 330 nm), which suggest that aerosol aging processes including hygroscopic growth (e.g., humidification and cloud processing) can be a major factor affecting the temporal trends of aerosol optical properties. Retrieved n f and ω 0 were closer to those of the water droplet (i.e., n f of about 1.33 and ω 0 of about 1.0) under lower amounts of NO 2 during the measurement period; considering that the NO 2 amounts in the smoke may indicate the aging of the plume after emission due to its short lifetime, the tendency is also consistent with active hygroscopic processes of the aerosols over this area. Retrieved UV aerosol properties from SMART–s generally support the assumed smoke aerosol models (i.e., the spectral shape of aerosol absorption) used in NASA's current satellite algorithms, and their spectral ω 0 retrievals from ground and satellites showed good agreements (R = 0.73–0.79). However, temporal and spectral variabilities in the aerosol absorption properties in the UV emphasize the importance of a realistic optical model of aerosols for further improvements in satellite retrievals.

biomass burning↗
NASA NTRS1983

Stratospheric aerosol light absorption before and after El Chichon

Direct in-situ measurements of aerosol light absorption before, during, and after the eruption of Mt. St. Helens and El Chichon reveal the presence of light absorbing species at all times. Large enhancements which appear to drop rapidly with time are found at certain locations immediately following volcanic events. Although a general patchiness is present in the aerosol and its associated absorption coefficient, post eruption values appear to remain elevated in the mean when compared to early 1979 data prior to the El Chichon eruption. From the data collected for this period, lower bounds for the single scatter albedo are presented along with implications for associated radiative effects.

Clarke, A. D.↗
DOE OSTI2023

Assessing the link between aerosol mixing state, structure and composition and their optical properties: Ascension Island as a testbed for the South‐East Atlantic aerosol regimes

Forest and savanna fires are a major source of pollution over the globe. Such fire events emit to the atmosphere a considerable amount of “fluffy” fractal black looking particles that are often referred to as black carbon (BC) or soot aerosols. In fact, BC particles (aerosols) emitted from savanna and agricultural fires over the African continent play an important role in the region’s and the global climate. These fires occur each year between July and October, which is referred to as the biomass burning (BB) season and are considered among the globe's largest man-made emission sources of BC particles. However, during these fire events, not only BC particles are emitted, but also other types of particles and gases that can interact with each other to create new particles, generating a slew of particles often generally referred to as BB aerosols. Although the majority of the fire emissions occur inland in the sub-Saharan part of Africa, their effect reaches far beyond the continent due to the prevailing easterly winds, which transport those aerosols over the South-East Atlantic (SEA) ocean, off the west-coast of Africa. The reason why these particles are so important to the regional and global climate is that they absorb sunlight radiation, which overall warms the climate. However, the magnitude of this warming effect is highly uncertain and depends upon a multitude of aspects. Our overarching goal for this project was to better understand the changes in the aerosol properties as they transport from fire sources downstream toward the ocean and how this can eventually affect the earth's radiative budget in terms of warming or cooling. Following the above, our work here was focused on the investigation of the African BB aerosol plumes mixing state (mixing of BB aerosols and other aerosol types), composition and size distribution as they transport from the African continent towards the SEA ocean, and their link with some of the commonly measurable bulk optical properties such as mass absorption coefficient (MAC) and single scattering albedo (SSA). We utilized three field missions that were conducted over the SEA ocean between 2016 and 2018. Specifically, we used (1) ground-based measurements from the DOE ARM Mobile Facility (AMF1), which was deployed at Ascension Island (ASI) for the LASIC (Layered Atlantic Smoke Interactions with Clouds) campaign between June 2016 and October 2017, (2) airborne measurements from the UK CLARIFY (Clouds and Aerosol Radiative impacts and Forcing) campaign during Aug-Sep-2017, and (3) airborne measurements from the ORACLES (Observations of Aerosols above Clouds and their interactions) campaign during Aug-2017, and Sep-Oct-2018. The three campaigns cover a relatively large region, from the western African coast on the east towards Ascension Island in the middle of the SEA to the west. We used the data gathered by these campaigns to find how BB properties and composition change from near emission sources (the ORACLES campaign flights) downstream (the CLARIFY flights and the ground based LASIC measurements). We used particle trajectory following methodologies to connect the measurements from the different campaigns, which allowed us to follow a certain aerosol plume (airmass) from near-source towards Ascension Island. We found out that atmospheric aging processes governed by the UV light from the sun (photochemistry) and cloud processes (aqueous chemistry) govern the changes seen in the particle composition during the transport were more dominant in dictating aerosol composition than specific emission composition or source types. We assessed how aerosol optical properties change during the BB season and what are the main drivers of this change. We found that the enhanced ratio of BC to CO is well correlated with single scattering albedo (SSA) and mass absorption coefficient (MACBC), providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic Ocean. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/CO from June to August is likely to be caused by burning becoming more flaming (hot fires), and the decrease in BC/CO in September and October may be caused by smoldering (colder) fires. We found that aerosol hygroscopicity increases with decreasing altitude below 2km, and that enhanced BB hygroscopicity at lower altitudes is mainly due to a lower organic aerosol (OA) fraction, increased sulfate fraction, and greater hygroscopicity parameter of OA at lower altitudes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Correcting for filter-based aerosol light absorption biases at the Atmospheric Radiation Measurement program's Southern Great Plains site using photoacoustic measurements and machine learning

Abstract. Measurement of light absorption of solar radiation by aerosols is vital for assessing direct aerosol radiative forcing, which affects local and global climate. Low-cost and easy-to-operate filter-based instruments, such as the Particle Soot Absorption Photometer (PSAP), that collect aerosols on a filter and measure light attenuation through the filter are widely used to infer aerosol light absorption. However, filter-based absorption measurements are subject to artifacts that are difficult to quantify. These artifacts are associated with the presence of the filter medium and the complex interactions between the filter fibers and accumulated aerosols. Various correction algorithms have been introduced to correct for the filter-based absorption coefficient measurements toward predicting the particle-phase absorption coefficient (Babs). However, the inability of these algorithms to incorporate into their formulations the complex matrix of influencing parameters such as particle asymmetry parameter, particle size, and particle penetration depth results in prediction of particle-phase absorption coefficients with relatively low accuracy. The analytical forms of corrections also suffer from a lack of universal applicability: different corrections are required for rural and urban sites across the world. In this study, we analyzed and compared 3 months of high-time-resolution ambient aerosol absorption data collected synchronously using a three-wavelength photoacoustic absorption spectrometer (PASS) and PSAP. Both instruments were operated on the same sampling inlet at the Department of Energy's Atmospheric Radiation Measurement program's Southern Great Plains (SGP) user facility in Oklahoma. We implemented the two most commonly used analytical correction algorithms, namely, Virkkula (2010) and the average of Virkkula (2010) and Ogren (2010)–Bond et al. (1999) as well as a random forest regression (RFR) machine learning algorithm to predict Babs values from the PSAP's filter-based measurements. The predicted Babs was compared against the reference Babs measured by the PASS. The RFR algorithm performed the best by yielding the lowest root mean square error of prediction. The algorithm was trained using input datasets from the PSAP (transmission and uncorrected absorption coefficient), a co-located nephelometer (scattering coefficients), and the Aerosol Chemical Speciation Monitor (mass concentration of non-refractory aerosol particles). A revised form of the Virkkula (2010) algorithm suitable for the SGP site has been proposed; however, its performance yields approximately 2-fold errors when compared to the RFR algorithm. To generalize the accuracy and applicability of our proposed RFR algorithm, we trained and tested it on a dataset of laboratory measurements of combustion aerosols. Input variables to the algorithm included the aerosol number size distribution from the Scanning Mobility Particle Sizer, absorption coefficients from the filter-based Tricolor Absorption Photometer, and scattering coefficients from a multiwavelength nephelometer. The RFR algorithm predicted Babs values within 5 % of the reference Babs measured by the multiwavelength PASS during the laboratory experiments. Thus, we show that machine learning approaches offer a promising path to correct for biases in long-term filter-based absorption datasets and accurately quantify their variability and trends needed for robust radiative forcing determination.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Atmospheric Brown Carbon on the Tibetan Plateau: Regional Differences in Chemical Composition and Light Absorption Properties

In this work, fine particulate matter (PM 2.5 ) filter samples were collected from two high-altitude remote sites located in the southern (QOMS) and northern (WLG) regions of the Tibetan Plateau (TP) to explore the regional differences in brown carbon (BrC) properties. Chemical differences in BrC composition representative of these two areas were inferred from molecular-level analysis of the PM 2.5 samples using high-performance liquid chromatography coupled with photodiode array and high-resolution mass spectrometry detectors. The results show that more polar BrC chromophores were abundant in QOMS samples, while contributions from polar and less polar chromophores were comparable in WLG samples. A higher mass absorption coefficient of BrC was observed at QOMS than at WLG. Strong BrC chromophores in QOMS samples were identified as oxygenated aromatics and nitrophenol compounds, while organosulfate compounds were found in the WLG sample. The results of this study indicate regional differences in BrC chromophores and provide insights into their sources and chemical processes, which should be considered for predictive understanding and modeling of the radiative forcing of aerosol in the TP area.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1994

UV laser long-path absorption spectroscopy

Long path Differential Optical Absorption Spectroscopy (DOAS) using a picosecond UV laser as a light source was developed in our institute. Tropospheric OH radicals are measured by their rotational absorption lines around 308 nm. The spectra are obtained using a high resolution spectrograph. The detection system has been improved over the formerly used optomechanical scanning device by application of a photodiode array which increased the observed spectral range by a factor of 6 and which utilizes the light much more effectively leading to a considerable reduction of the measurement time. This technique provides direct measurements of OH because the signal is given by the product of the absorption coefficient and the OH concentration along the light path according to Lambert-Beers law. No calibration is needed. Since the integrated absorption coefficient is well known the accuracy of the measurement essentially depends on the extent to which the OH absorption pattern can be detected in the spectra. No interference by self generated OH radicals in the detection lightpath has been observed. The large bandwidth (greater than 0.15 nm) and the high spectral resolution (1.5 pm) allows absolute determination of interferences by other trace gas absorptions. The measurement error is directly accessible from the absorption-signal to baseline-noise ratio in the spectra. The applicability of the method strongly depends on visibility. Elevated concentrations of aerosols lead to considerable attenuation of the laser light which reduces the S/N-ratio. In the moderately polluted air of Julich, where we performed a number of OH measurement spectra. In addition absorption features of unidentified species were frequently detected. A quantitative deconvolution even of the known species is not easy to achieve and can leave residual structures in the spectra. Thus interferences usually increase the noise and deteriorate the OH detection sensitivity. Using diode arrays for sensitive absorption measurements some specific problems of those detectors have to be solved experimentally (i.e. fixed pattern noise, dark signal noise, nonuniform efficiency of individual elements, spatial sensitivity variations). In order to improve the low spatial resolution we performed laboratory studies using a multiple reflection cell to convert the long path technique to a real in situ point measurement. Under the conditions of field experiments in Julich residual absorbance signals at present are about 1.5x10(exp -4) corresponding to an OH detection sensitivity of 2x10(exp 6) OH/cm(exp 3) using a light path of 5.8 km. Total integration times for one measurement point vary between a few minutes and an hour.

Dorn, Hans-Peter↗
DOE OSTI2024

Utilizing highly scattered light for intelligence through aerosols

A method for modeling light transport through a scattering medium prior to being incident on a detector and a corresponding system is disclosed. The method determines the effects of scattering and absorption caused by particles as a function of the density, size, and refractive index of the particles, as well as the wavelength of the light source. Based on the determined scattering and absorption coefficients, the signal incident on the detector may be calculated. The calculation may also be inverted such that based upon the detected signal, an object may be detected, and its location in the scattering medium may be estimated.

Bentz, Brian Z.↗
DOE OSTI2025

Extinction of Laser Light Due to Arctic Haze Final Campaign Report

Recent changes in emission patterns may have altered the historical stability of light attenuation strengths within the Arctic and, more specifically, the polar dome. While there have been decades of past and ongoing research on how atmospheric constituents, such as aerosols, affect light absorption, the bulk of this work is focused on the visible region. In recent years, there has been renewed interest in understanding laser light propagation at wavelengths such as 1 and 2 µm in this area. There is a need to evaluate how specific environmental parameters affect the propagation of light in this wavelength region, in particular: the extinction, scattering, and absorption coefficients, and how they relate to particle concentration; cn 2 and refractive index variations. Seasonally dependent variations in particle concentrations and compositions introduce different absorption and scattering characteristics that, in conjunction with varying temperatures, index-of-refraction variations, and wind, can result in laser beam focus and irradiance degradation. Understanding the fundamental influence of these parameters with respect to the propagation of light across a wide spectral band could lead to new insights about the minimal required datastreams required to provide accurate light propagation forecasting.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

pH dependence of brown-carbon optical properties in cloud water

Abstract. Light-absorbing organic species present in aerosols, collectively called brown carbon (BrC), have important but highly uncertain effects on climate. Clouds likely represent a significant medium for secondary BrC production and for bleaching reactions, though the relative importance of the formation and loss processes in clouds is unknown at present. The acidity (or pH) of atmospheric particles and clouds affects the optical properties of BrC and bleaching rates. Given the wide variability of pH in the atmosphere (pH in particles and clouds ranges from −1 to 8), the optical properties of BrC and its bleaching behavior are expected to vary significantly, and the link between pH and BrC is yet another uncertainty in attempts to constrain its climate forcing effects. In this work, we characterize the pH dependence of BrC optical properties – including light absorption at 365 nm (Abs365), the mass absorption coefficient (MAC365), and the absorption Ångström exponent (AAE) – in bulk cloud water sampled from the summit of Whiteface Mountain, NY. In all samples (n=17), Abs365 and MAC365 increased linearly with increasing pH, highlighting the importance of reporting pH in studies of BrC in aqueous media. There was strong variability in the sensitivity of Abs365 to pH, with normalized slopes that ranged from 5.1 % to 17.2 % per pH unit. The normalized slope decreased strongly with increasing cloud water [K+], suggesting that the non-biomass-burning BrC has optical properties that are more sensitive to pH than BrC associated with biomass burning. AAE also showed a distinct pH dependence as it was relatively flat between pH 1.5–5 and then decreased significantly above pH 5. The cloud water composition was used to inform thermodynamic predictions of aerosol pH upwind and/or downwind of Whiteface Mountain and the subsequent changes in BrC optical properties. Overall, these results show that, in addition to secondary BrC production, photobleaching, and the altitudinal distribution, the climate forcing of BrC is quite strongly affected by its pH-dependent absorption.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Realistic operation of two residential cordwood-fired outdoor hydronic heater appliances—Part 3: Optical properties of black and brown carbon emissions

Residential biomass combustion is a source of carbonaceous aerosol. Inefficient combustion, particularly of solid fuels produces large quantities of black and brown carbon (BC and BrC). These particle types are important as they have noted effects on climate forcing and human health. One method of measuring these quantities is by measurement of aerosol light-absorption and scattering, which can be performed using an aethalometer and nephelometer, respectively. These instruments are widely deployed in the study of ambient air and are frequently used in air quality modeling and source apportionment studies. In this study, we will describe (1) a method for measuring primary BC and BrC emissions from two residential log-fired wood hydronic heaters and (2) the BC and BrC emission from these devices over a wide range of operating conditions, such as cold-starts, warm-starts, four different levels of output ranging from 15% to 100% maximum rated output, and periods of repeated cycling. The range in flue-gas BC concentrations, measured using an aethalometer at the 880 nanometer (nm) wavelength, were between 5.09 × 10 2 and 2.24 × 10 4 micrograms per cubic meter (µg/m 3 ) while the scattering coefficient of the flue-gas, measured by a nephelometer at 880 nm, ranged between 2.20 × 10 3 and 8.56 × 10 5 inverse megameters (Mm –1 ). The BrC concentrations, measured using the 370 nm wavelength of an aethalometer, were between 9.10 × 10 1 and 3.56 × 10 4 µg/m 3 . The calculated Angstrom Absorption Exponent (AAE) of the flue-gas aerosol ranged between 1.54 and 3.63. Performing a comparison between the measured BC concentration and an external particulate matter (PM) concentration showed that overall BC makes up roughly a quarter of the PM emitted by either of the two appliances. Further for both appliances, the cold-start and the test phase immediately following it had the highest BC and BrC concentrations, the highest measured scattering coefficient, as well as a low AAE.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
NASA NTRS1981

In situ correlative measurements for the ultraviolet differential absorption lidar and the high spectral resolution lidar air quality remote sensors: 1980 PEPE/NEROS program

In situ correlative measurements were obtained with a NASA aircraft in support of two NASA airborne remote sensors participating in the Environmental Protection Agency's 1980persistent elevated pollution episode (PEPE) and Northeast regional oxidant study (NEROS) field program in order to provide data for evaluating the capability of two remote sensors for measuring mixing layer height, and ozone and aerosol concentrations in the troposphere during the 1980 PEPE/NEROS program. The in situ aircraft was instrumented to measure temperature, dewpoint temperature, ozone concentrations, and light scattering coefficient. In situ measurements for ten correlative missions are given and discussed. Each data set is presented in graphical and tabular format aircraft flight plans are included.

Gregory, G. L.↗
DOE OSTI2023

TRACER-CAT-UCDAVIS Aerosol Optical Properties and Sizing - crdps

Aerosol size distribution and optical properties collected in La Port TX, during TRACER-CAT-UCDavis, July 2022. Speciated particle composition measurements are reported separately. All sampling was conducted with an identical aerosol inlet as the standard ARM-AOS systems. The TRacking Aerosol Convection interactions ExpeRiment Carbonaceous Aerosols Thrust by UC Davis (TRACER-CAT-UCDavis, July 2022) was designed to complement the larger ARM TRACER science goals to understand convective cloud lifecycles and aerosol-convection interactions. TRACER-CAT-UCDavis is focused on understanding the relationship between particle composition and light absorption and the influence of water uptake on this relationship. This aerosol data can be used to understand the relationship between particle composition and light absorption and the influence of water uptake on this relationship. Instruments include: UC Davis two-wavelength cavity ringdown-photoacoustic spectrometer (CRD-PAS); Brechtel scanning electrical mobility sizer (SEMS); modified humidified cavity attenuated phase shift spectrometer with single scatter albedo (H-CAPS-SSA)

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Burning conditions and transportation pathways determine biomass-burning aerosol properties in the Ascension Island marine boundary layer

African biomass-burning aerosol (BBA) in the southeast Atlantic Ocean (SEA) marine boundary layer (MBL) is an important contributor to Earth’s radiation budget yet its representation remains poorly constrained in regional and global climate models. Data from the Layered Atlantic Smoke Interactions with Clouds (LASIC) field campaign on Ascension Island (-7.95° N, -14.36° E) detail how fire source regions (burning conditions and fuel type), transport pathways, and longer-term chemical processing affect the chemical, microphysical, and optical properties of the BBA in the remote MBL between June and September of 2017. Ten individual plume events characterize the seasonal evolution of BBA characteristics. Inefficient burning conditions, determined by the mass ratio of refractory black carbon to above-background carbon monoxide (rBC:ΔCO), enhance organic- and sulfate-rich aerosol concentrations in June–July. In contrast, the heart of the burning season exhibited higher rBC:ΔCO values indicative of efficient burning conditions, correlating with more rBC-enriched BBA. Toward the end of the burning season, a mix of burning conditions results in increased variation of the BBA properties. The BBA transit to Ascension Island was predominantly through slow-moving pathways in the MBL and lower free troposphere (FT), facilitating prolonged chemical transformations through heterogeneous and aqueous phase processes. Heterogeneous oxidation can persist for up to 10 days, resulting in a considerable decrease in organic aerosol (OA) mass. OA to rBC mass ratios (OA:rBC) in the MBL between 2 and 5 contrast to higher values of 5 to 15 observed in the nearby FT. Conversely, early-season aqueous-phase processes primarily contributed to aerosol oxidation and some aerosol production, but not appreciable aerosol removal. These two chemical processes yield more light-absorbing BBA in the MBL than in the FT and explain the notably low scattering albedo at 530 nm (SSA 530 ) values (< 0.80) at Ascension Island. This study establishes a robust correlation between SSA 530 and OA:rBC across both MBL and FT, underscoring the dependency of optical properties on chemical composition. These findings highlight how the interplay between chemical composition and atmospheric processing can be improved in global and regional climate models. Questions remain on the mixing of aerosols with different pathway histories, and on what accounts for the doubling of the mass absorption coefficient in the boundary layer.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2004

Cavity Ring-Down Measurement of Aerosol Optical Properties During the Asian Dust Above Monterey Experiment and DOE Aerosol Intensive Operating Period

Large uncertainties in the effects of aerosols on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This paper describes preliminary results from Cadenza, a new continuous wave cavity ring-down (CW-CRD) instrument designed to address these uncertainties. Cadenza measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. In the past year Cadenza was deployed in the Asian Dust Above Monterey (ADAM) and DOE Aerosol Intensive Operating Period (IOP) field projects. During these flights Cadenza produced measurements of aerosol extinction in the range from 0.2 to 300/Mm with an estimated precision of 0.1/Mm for 1550 nm light and 0.2/Mm for 675 nm light. Cadenza data from the ADAM and Aerosol IOP missions compared favorably with data from the other instruments aboard the CIRPAS Twin Otter aircraft and participating in those projects. We present comparisons between the Cadenza measurements and those from a TSI nephelometer, Particle Soot Absorption Photometer (PSAP), and the AATS 14 sun-photometer. Measurements of the optical properties of smoke and dust plumes sampled during these campaigns are presented and estimates of heating rates due to these plumes are made.

Ricci, K.↗
NASA NTRS2003

Airborne Cavity Ring-Down Measurement of Aerosol Extinction and Scattering During the Aerosol IOP

Large uncertainties in the effects of aerosols on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This paper describes preliminary results from Cadenza, a new continuous wave cavity ring-down (CW-CRD) instrument designed to address these uncertainties. Cadenza measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. In the past year Cadenza was deployed in the Asian Dust Above Monterey (ADAM) and DOE Aerosol Intensive Operating Period (IOP) field projects. During these flights Cadenza produced measurements of aerosol extinction in the range from 0.2 to 300 Mm-1 with an estimated precision of 0.1 Min-1 for 1550 nm light and 0.2 Mm-1 for 675 nm light. Cadenza data from the ADAM and Aerosol IOP missions compared favorably with data from the other instruments aboard the CIRPAS Twin Otter aircraft and participating in those projects.= We present comparisons between the Cadenza measurements and those friom a TSI nephelometer, Particle Soot Absorption Photometer (PSAP), and the AATS 14 sun-photometer. Measurements of the optical properties of smoke and dust plumes sampled during these campaigns are presented and estimates of heating rates due to these plumes are made.

Strawa, A. W.↗
DOE OSTI2023

TRACER-CAT-LANL Aerosol Optics and Chemical Speciation - PASS

Aerosol size distribution, optical properties, and speciation data collected in La Port TX, during TRACER-CAT-LANL, July 2022, with basic trace gas measurements. All sampling was conducted with an identical aerosol inlet as the standard ARM-AOS systems. The TRacking Aerosol Convection interactions ExpeRiment Carbonaceous Aerosols Thrust by Los Alamos National Laboratory (TRACER-CAT-LANL, July 2022) was designed to complement the larger ARM TRACER science goals to understand convective cloud lifecycles and aerosol-convection interactions. TRACER-CAT-LANL is focused on understanding the relationship between particle composition and light absorption and the influence of water uptake on this relationship. This aerosol and trace gas data can be used to understand the relationship between particle composition and light absorption and the influence of water uptake on this relationship. Instruments Include: Picarro GHG Photoacoustic Soot Spectrometer (PASS-3) Humidified-cavity attenuated phase shift-single scattering albedo particulate matter monitor (H-CAPS-PMSSA) Soot Particle Aerosol Mass Spectrometer (SPAMS) Single-Particle Soot Photometer (SP2) Cloud Condensation Nuclei Counter (CCNc) Aerodynamic Particle Sizer (APS) Scanning Mobility Particle Sizer (SMPS)

54 ENVIRONMENTAL SCIENCES↗