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47 records · Page 3

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.↗

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↗

Computational Imaging for Intelligence in Highly Scattering Aerosols (Final Report)

Natural and man-made degraded visual environments pose major threats to national security. The random scattering and absorption of light by tiny particles suspended in the air reduces situational awareness and causes unacceptable down-time for critical systems and operations. To improve the situation, we have developed several approaches to interpret the information contained within scattered light to enhance sensing and imaging in scattering media. These approaches were tested at the Sandia National Laboratory Fog Chamber facility and with tabletop fog chambers. Computationally efficient light transport models were developed and leveraged for computational sensing. The models are based on a weak angular dependence approximation to the Boltzmann or radiative transfer equation that appears to be applicable in both the moderate and highly scattering regimes. After the new model was experimentally validated, statistical approaches for detection, localization, and imaging of objects hidden in fog were developed and demonstrated. A binary hypothesis test and the Neyman-Pearson lemma provided the highest theoretically possible probability of detection for a specified false alarm rate and signal-to-noise ratio. Maximum likelihood estimation allowed estimation of the fog optical properties as well as the position, size, and reflection coefficient of an object in fog. A computational dehazing approach was implemented to reduce the effects of scatter on images, making object features more readily discernible. We have developed, characterized, and deployed a new Tabletop Fog Chamber capable of repeatably generating multiple unique fog-analogues for optical testing in degraded visual environments. We characterized this chamber using both optical and microphysical techniques. In doing so we have explored the ability of droplet nucleation theory to describe the aerosols generated within the chamber, as well as Mie scattering theory to describe the attenuation of light by said aerosols, and correlated the aerosol microphysics to optical properties such as transmission and meteorological optical range (MOR). This chamber has proved highly valuable and has supported multiple efforts inclusive to and exclusive of this LDRD project to test optics in degraded visual environments. Circularly polarized light has been found to maintain its polarization state better than linearly polarized light when propagating through fog. This was demonstrated experimentally in both the visible and short-wave infrared (SWIR) by imaging targets made of different commercially available retroreflective films. It was found that active circularly polarized imaging can increase contrast and range compared to linearly polarized imaging. We have completed an initial investigation of the capability for machine learning methods to reduce the effects of light scattering when imaging through fog. Previously acquired experimental long-wave images were used to train an autoencoder denoising architecture. Overfitting was found to be a problem because of lack of variability in the object type in this data set. The lessons learned were used to collect a well labeled dataset with much more variability using the Tabletop Fog Chamber that will be available for future studies. We have developed several new sensing methods using speckle intensity correlations. First, the ability to image moving objects in fog was shown, establishing that our unique speckle imaging method can be implemented in dynamic scattering media. Second, the speckle decorrelation over time was found to be sensitive to fog composition, implying extensions to fog characterization. Third, the ability to distinguish macroscopically identical objects on a far-subwavelength scale was demonstrated, suggesting numerous applications ranging from nanoscale defect detection to security. Fourth, we have shown the capability to simultaneously image and localize hidden objects, allowing the speckle imaging method to be effective without prior object positional information. Finally, an interferometric effect was presented that illustrates a new approach for analyzing speckle intensity correlations that may lead to more effective ways to localize and image moving objects. All of these results represent significant developments that challenge the limits of the application of speckle imaging and open important application spaces. A theory was developed and simulations were performed to assess the potential transverse resolution benefit of relative motion in structured illumination for radar systems. Results for a simplified radar system model indicate that significant resolution benefits are possible using data from scanning a structured beam over the target, with the use of appropriate signal processing.

58 GEOSCIENCES↗

TRACER-CAT-LANL Aerosol Optics and Chemical Speciation - CAPS-SSA

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↗

Intensive aerosol properties of boreal and regional biomass burning aerosol at Mt. Bachelor Observatory: larger and black carbon (BC)-dominant particles transported from Siberian wildfires

We characterize the aerosol physical and optical properties of 13 transported biomass burning (BB) events. BB events included long-range influence from fires in Alaskan and Siberian boreal forests transported to Mt. Bachelor Observatory (MBO) in the free troposphere (FT) over 8–14+ d and regional wildfires in northern California and southwestern Oregon transported to MBO in the boundary layer (BL) over 10 h to 3 d. Intensive aerosol optical properties and normalized enhancement ratios for BB events were derived from measured aerosol light scattering coefficients (σ scat ), aerosol light-absorbing coefficients (σ abs ), fine particulate matter (PM 1 ), and carbon monoxide (CO) measurements made from July to September 2019, with particle size distribution collected from August to September. The observations showed that the Siberian BB events had a lower scattering Ångström exponent (SAE), a higher mass scattering efficiency (MSE; Δσ scat /ΔPM 1 ), and a bimodal aerosol size distribution with a higher geometric mean diameter (D g ). We hypothesize that the larger particles and associated scattering properties were due to the transport of fine dust alongside smoke in addition to contributions from condensation of secondary aerosol, coagulation of smaller particles, and aqueous-phase processing during transport. Alaskan and Siberian boreal forest BB plumes were transported long distances in the FT and characterized by lower absorption Ångström exponent (AAE) values indicative of black carbon (BC) dominance in the radiative budget. Significantly elevated AAE values were only observed for BB events with <1 d transport, which suggests strong production of brown carbon (BrC) in these plumes but limited radiative forcing impacts outside of the immediate region.

54 ENVIRONMENTAL SCIENCES↗

Light Absorption by Brown Carbon over the South-East Atlantic Ocean

Biomass burning emissions often contain brown carbon (BrC), which represents a large family of light-absorbing organics that is chemically complex and therefore difficult to estimate their absorption of incoming solar radiation, resulting in large uncertainties in the estimation of the global direct radiative effect of aerosols. Here we investigate the contribution of BrC to the total light absorption of biomass burning aerosols over the South-East Atlantic Ocean with different optical models utilizing a suite of airborne measurements from the ORACLES 2018 campaign by introducing an effective refractive index of black carbon (BC), m eBC = n eBC +ik eBC , that accounts for all possible absorbing components at 660 nm wavelength to facilitate the attribution of absorption at shorter wavelengths. Most values of the imaginary part of the refractive index, k eBC , were larger than those commonly used for BC from biomass burning emissions, suggesting contributions from absorbers beyond BC at 660 nm. The TEM-EDX single particle analysis further suggests that these long-wavelength absorbers might include iron oxides, as iron is found to be present only when large values of k eBC are derived. Using this effective BC refractive index, we find that the contribution of BrC to the total absorption at 470 nm (R BrC,470 ) ranges from ~5–15 %, with the organic aerosol mass absorption coefficient (MAC OA,470 ) at this wavelength ranging from 0.25 ± 0.34 m 2 g -1 to 0.43 ± 0.12 m 2 g -1 . The core-shell model yielded much higher estimates of MAC OA,470 and R BrC,470 than homogeneous mixing models, underscoring the importance of model treatment. Another key finding was that estimates of the BrC contribution at 470 nm from the commonly used AAE (absorption Ångström exponent) attribution method (< 5 %) are much lower than the BrC contribution estimates (R BrC,470 ) using our new methodology that accounts for contributions from both BrC and non-carbonaceous, long-wavelength absorbers, such as magnetite. Thus, it is recommended that application of any optical properties-based attribution method use absorption coefficients at the longest possible wavelength to minimize the influence of BrC at the long wavelength and to account for potential contributions from other absorbing materials.

54 ENVIRONMENTAL SCIENCES↗

Multi-Grid-Cell Validation of Satellite Aerosol Property Retrievals in INTEX/ITCT/ICARTT 2004

Aerosol transport off the US Northeast coast during the Summer 2004 International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) Intercontinental Chemical Transport Experiment (INTEX) and Intercontinental Transport and Chemical Transformation (ITCT) experiments produced a wide range of aerosol types and aerosol optical depth (AOD) values, often with strong horizontal AOD gradients. In these conditions we flew the 14-channel NASA Ames Airborne Tracking Sun photometer (AATS) on a Jetstream 31 (J31) aircraft. Legs flown at low altitude (usually less than 100 m ASL) provided comparisons of AATS AOD spectra to retrievals for 90 grid cells of the satellite radiometers MODIS-Terra, MODIS-Aqua, and MISR, all over the ocean. Characterization of the retrieval environment was aided by using vertical profiles by the J31 (showing aerosol vertical structure) and, on occasion, shipboard measurements of light scattering and absorption. AATS provides AOD at 13 wavelengths lambda from 354 to 2138 nm, spanning the range of aerosol retrieval wavelengths for MODIS over ocean (466-2119 nm) and MISR (446-866 nm). Midvisible AOD on low-altitude J31 legs in satellite grid cells ranged from 0.05 to 0.9, with horizontal gradients often in the range 0.05 to 0.13 per 10 km. When possible, we used ship measurements of humidified aerosol scattering and absorption to estimate AOD below the J31. In these cases, which had J31 altitudes 60-110 m ASL (typical of J31 low-altitude transects), estimated midvisible AOD below the J31 ranged from 0.003 to 0.013, with mean 0.009 and standard deviation 0.003. These values averaged 6 percent of AOD above the 53 1. MISR-AATS comparisons on 29 July 2004 in 8 grid cells (each -17.6 km x 17.6 km) show that MISR versions 15 and 16 captured the AATS-measured AOD gradient (correlation coefficient R2 = 0.87 to 0.92), but the MISR gradient was somewhat weaker than the AATS gradient. The large AOD (midvisible values up to -0.9) and differing gradients in this case produced root-mean-square (RMS) MISR-AATS AOD differences of 0.03 to 0.21 (9 to 31%). MISR V15 Angstrom exponent alpha (= -dlnAOD/dln lambda) was closer to AATS than was MISR V16. MODIS-AATS AOD comparisons on 8 overpasses using 61 grid cells (each nominally 10 km x 10 km) had R2 approximately 0.97, with RMS AOD difference approximately 0.03 (approximately 20%). About 87% of the MODIS AOD retrievals differed from AATS values by less than the predicted MODIS over-ocean uncertainty, Delta tau = plus/minus 0.03 plus/minus 0.05 tau. In contrast to the small MODIS-AATS differences in AOD, MODIS-AATS differences in Angstrom exponent alpha were large: RMS differences for alpha (553, 855 nm) were 0.28 for MODIS-Terra and 0.64 for MODIS-Aqua; RMS differences for alpha (855, 2119 nm) were larger still, 0.61 for MODIS-Terra and 1.14 for MODIS-Aqua. The largest MODIS-AATS Angstrom exponent differences were associated with small AOD values, for which MODIS AOD relative uncertainty is large. Excluding cases with AOD(855 nm) less than 0.1 reduced MODIS-AATS alpha differences substantially. In one grid cell on 21 July 2004, smoke over cloud appeared to impair the MODIS-Aqua cloud mask, resulting in retrieved AODs that significantly exceeded AATS values. Experiments with extending MODIS retrievals into the glint mask yielded MODIS AODs consistently less than AATS AODs, especially at long wavelength, indicating that the current MODIS glint mask limits should not be reduced to the extent tried here. The sign of the AOD differences within the glint mask (MODIS AOD less than AATS AOD) is consistent with ship-measured wind speeds there.

Russell, P. B.↗

Photoaging of phenolic secondary organic aerosol in the aqueous phase: evolution of chemical and optical properties and effects of oxidants

Abstract. While gas-phase reactions are well established to have significant impacts on the mass concentration, chemical composition, and optical properties of secondary organic aerosol (SOA), the aqueous-phase aging of SOA remains poorly understood. In this study, we performed a series of long-duration photochemical aging experiments to investigate the evolution of the composition and light absorption of the aqueous SOA (aqSOA) from guaiacyl acetone (GA), a semivolatile phenolic carbonyl that is common in biomass burning smoke. The aqSOA was produced from reactions of GA with hydroxyl radical (•OH-aqSOA) or a triplet excited state of organic carbon (3C∗-aqSOA) and was then photoaged in water under conditions that simulate sunlight exposure in northern California for up to 48 h. The effects of increasing aqueous-phase •OH or 3C∗ concentration on the photoaging of the aqSOA were also studied. High-resolution aerosol mass spectrometry (HR-AMS) and UV–Vis spectroscopy were utilized to characterize the composition and the light absorptivity of the aqSOA and to track their changes during aging. Compared to •OH-aqSOA, the 3C∗-aqSOA is produced more rapidly and shows less oxidation, a greater abundance of oligomers, and higher light absorption. Prolonged photoaging promotes fragmentation and the formation of more volatile and less light-absorbing products. More than half of the initial aqSOA mass is lost, and substantial photobleaching occurs after 10.5 h of prolonged aging under simulated sunlight illumination for 3C∗-aqSOA and 48 h for •OH-aqSOA. By performing positive matrix factorization (PMF) analysis of the combined HR-AMS and UV–Vis spectral data, we resolved three generations of aqSOA with distinctly different chemical and optical properties. The first-generation aqSOA shows significant oligomer formation and enhanced light absorption at 340–400 nm. The second-generation aqSOA is enriched in functionalized GA species and has the highest mass absorption coefficients in 300–500 nm, while the third-generation aqSOA contains more fragmented products and is the least light absorbing. These results suggest that intermediately aged phenolic aqSOA is more light absorbing than other generations, and that the light absorptivity of phenolic aqSOA results from a competition between brown carbon (BrC) formation and photobleaching, which is dependent on aging time. Although photoaging generally increases the oxidation of aqSOA, a slightly decreased O/C of the •OH-aqSOA is observed after 48 h of prolonged photoaging with additional •OH exposure. This is likely due to greater fragmentation and evaporation of highly oxidized compounds. Increased oxidant concentration accelerates the transformation of aqSOA and promotes the decay of BrC chromophores, leading to faster mass reduction and photobleaching. In addition, compared with •OH, photoaging by 3C∗ produces more low-volatility functionalized products, which counterbalances part of the aqSOA mass loss due to fragmentation and evaporation.

54 ENVIRONMENTAL SCIENCES↗

EPCAPE-PT-LANL Measurements: Photoacoustic Extinctometer

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: Photoacoustic Extinctiometer at 870 nm (Droplet Measurement Technology) Header: - AbsorptionNoise_870nm[1/Mm]: Noise level associated with the absorption measurement at 870 nm, expressed in inverse megameters (Mm⁻¹). - Absorption_870nm[1/Mm]: Absorption coefficient of aerosols measured at 870 nm, expressed in inverse megameters (Mm⁻¹). - Extinction_870nm[1/Mm]: Extinction coefficient of aerosols measured at 870 nm, expressing the sum of scattering and absorption by aerosols, in inverse megameters (Mm⁻¹). - Scattering_870nm[1/Mm]: Scattering coefficient of aerosols measured at 870 nm, expressed in inverse megameters (Mm⁻¹). - BackgroundAbsorption_870nm[1/Mm]: Background absorption measurement at 870 nm, used to correct the primary absorption data, expressed in inverse megameters (Mm⁻¹). - BackgroundScattering_870nm[1/Mm]: Background scattering measurement at 870 nm, used to correct the primary scattering data, expressed in inverse megameters (Mm⁻¹). - Temperature[C]: The ambient temperature at the time of the measurement, expressed in degrees Celsius. - RelativeHumidity[%]: The relative humidity at the time of the measurement, expressed as a percentage. - CVI_Flag[bool]: A boolean flag indicating whether the Counterflow Virtual Impactor (CVI) was active (true) or inactive (false) during the measurement

54 ENVIRONMENTAL SCIENCES↗

Look-up Table for Lidar and Polarimeter Liquid Water Cloud Studies

- Combined lidar and polarimeter retrievals of aerosol, cloud and ocean microphysical properties involve single scattering cloud calculations that are time consuming. - We create a look-up table to speed up calculations for water droplets in the atmosphere. The gained increase in computational efficiency is up to 10^(4). - In our new Lorenz-Mie look-up table we tabulate the light scattering by an ensemble of homogeneous isotropic spheres at wavelengths starting from 0.35 µm. - The look-up table covers liquid water cloud particles with radii in the range of 0.001—500 µm. - The covered complex refractive indices range from 1.25 to 1.36 for the real part and from 0 to 0.001 for the imaginary part. - Using look-up table, we can precisely compute inherent optical properties for the particle size distributions ranging up to 100 µm for the effective radius and up to 0.6 for the effective variance. - We test wavelengths from 0.35 to 2.3 µm and find that the P12 element of the normalized scattering matrix is precise to within 1% for 96.7% of cases; the absorption and backscatter coefficients, and lidar ratio are precise to within 1% for 99% of cases; the P11 , P33 and P34 elements of the normalized scattering matrix, the asymmetry parameter, the extinction and scattering coefficients are precise to within 1% for all cases. - We provide an example of using the look-up table with in situ measurements to determine agreement with remote sensing. - The look-up table along with examples of its use soon will be freely available at https://science.larc.nasa.gov/polarimetry

Eduard Chemyakin↗

LASE validation experiment: preliminary processing of relative humidity from LASE derived water vapor in the middle to upper troposphere

Lidar Atmospheric Sensing Experiment (LASE) is the first fully engineered, autonomous airborne DIAL (Differentials Absorption Lidar) system to measure water vapor, aerosols, and clouds throughout the troposphere. This system uses a double-pulsed Ti:sapphire laser, which is pumped by a frequency-doubled flashlamp-pumped Nd: YAG laser, to transmit light in the 815 mn absorption band of water vapor. LASE operates by locking to a strong water vapor line and electronically tuning to any spectral position on the absorption line to choose the suitable absorption cross-section for optimum measurements over a range of concentrations in the atmosphere. During the LASE Validation Experiment, which was conducted over Wallops Island during September, 1995, LASE operated on either the strong water line for measurements in middle to upper troposphere, or on the weak water line for measurements made in the middle to lower troposphere including the boundary layer. Comparisons with water vapor measurements made by airborne dew point and frost point hygrometers, NASA/GSFC (Goddard Space Flight Center) Raman Lidar, and radiosondes showed the LASE water vapor mixing ratio measurements to have an accuracy of better than 6% or 0.01 g/kg, whichever is larger, throughout the troposphere. In addition to measuring water vapor mixing ratio profiles, LASE simultaneously measures aerosol backscattering profiles at the off-line wavelength near 815 nm from which atmospheric scattering ratio (ASR) profiles are calculated. ASR is defined as the ratio of total (aerosol + molecular) atmospheric scattering to molecular scattering. Assuming a region with very low aerosol loading can be identified, such as that typically found just below the tropopause, then the ASR can be determined. The ASR profiles are calculated by normalizing the scattering in the region containing enhanced aerosols to the expected scattering by the "clean" atmosphere at that altitude. Images of the total ASR clearly depict cloud regions, including multiple cloud layers, thin upper level cirrus, etc., throughout the troposphere. New data products that are being derived from the LASE aerosol and water measurements include: 1) aerosol extinction coefficient, 2) aerosol optical thickness, 3) precipitable water vapor, and 4) relative humidity (RH). These products can be compared with airborne in-situ, and ground and satellite remote sensing measurements,. This paper presents a preliminary examination of RH profiles in the middle to upper troposphere that are generated from LASE measured water vapor mixing ratio profiles coupled with rawinsonde profiles of temperature and pressure.

Brackett, Vincent G.↗