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NASA NTRSDate not supplied

On Improving the Dust Lidar Ratios for Version 5 of CALIOP by Using Measurements with Source-tagged Model Results

Vertically resolved retrievals of aerosol backscatter and extinction have been available since 2006 from global measurements acquired by the space borne lidar CALIOP onboard the CALIPSO satellite. These retrievals depend crucially upon the ratio of extinction to backscatter (i.e., lidar ratio) which typically has to be assumed for the various aerosol species for an elastic backscatter lidar like CALIOP. For all CALIPSO data releases up until now (version 4.2), these lidar ratios have been taken as constant both spatially and temporally. However, it is well established that the aerosol lidar ratios can vary significantly regionally, seasonally, and also as a function of age and relative humidity. In particular, the dust lidar ratios show significant variation depending upon their source regions, which is related to the mineral composition of dust in that region. In this paper, we shall present a scheme to obtain the regionally and seasonally dependent lidar ratios of dust. In this scheme, which may be implemented in a forthcoming version of CALIOP aerosol extinction retrievals, we first derive lidar ratios of aerosol layers globally, classified as dust by CALIOP, by using the backscatter measurements constrained by collocated MODIS aerosol optical depths. Since this dust will frequently be a mixture of dust from various source regions, we obtain the corresponding regional contributions from the dust simulations using the GEOS model tagged to nine source regions. Finally, combining information from both measurements and models, we obtain the lidar ratios of dust corresponding to the nine source regions. The lidar ratio of the mixed dust anywhere can now be obtained from the tagged model fractions and the corresponding regional lidar ratio. We shall show the application of this scheme for various regions and seasons.

CALIPSO↗

NASA NTRS2022

Ultraviolet Spectropolarimetry with Polstar: Interstellar Medium Science

Continuum polarization over the UV-to-microwave range is due to dichroic extinction (or emission) by asymmetric, aligned dust grains. Scattering can also be an important source of polarization, especially at short wavelengths. Because of both grain alignment and scattering physics, the wavelength dependence of the polarization, generally, traces the size of the aligned grains. Similarly because of the differing wavelength dependencies of dichroic extinction and scattering polarization, the two can generally be reliably separated. Ultraviolet (UV) polarimetry therefore provides a unique probe of the smallest dust grains (diameter<0.09 μm ), their mineralogy and interaction with the environment. However, the current observational status of interstellar UV polarization is very poor with less than 30 lines of sight probed. With the modern, quantitative and well-tested, theory of interstellar grain alignment now available, we have the opportunity to advance the understanding of the interstellar medium (ISM) by executing a systematic study of the UV polarization in the ISM of the Milky Way and near-by galaxies. The Polstar mission will provide the sensitivity and observing time needed to carry out such a program (probing hundreds of stars in the Milky Way and dozens of stars in the LMC/SMC), addressing questions of dust composition as a function of size and location, radiation- and magnetic-field characteristics as well as unveiling the carrier of the 2175 Å extinction feature. In addition, using high-resolution UV line spectroscopy Polstar will search for and probe the alignment of, and polarization from, aligned atoms and ions - so called “Ground State Alignment”, a potentially powerful new probe of magnetic fields in the diffuse ISM.

B-G Andersson↗

NASA NTRSDate not supplied

Linear Polarizer Design for Application in the Far-Ultraviolet Spectral Range

New mission concepts that are under consideration by NASA call for the design and implementation of Far Ultraviolet (FUV) polarizer technologies that have not been developed yet. A team that includes members from the NASA Goddard Space Flight Center (GSFC), Arizona State University (ASU), and Woodruff Consulting, worked on the design and development of a polarizer design that produce very high extinction ratios in the FUV spectral range (100-200 nm). This polarizer consists of reflecting light through a series of mirrors from a combination of two silicon carbide (SiC) and two lithium fluoride (LiF) crystals positioned at angles of incidence (relative to surface normal) close to the average LiF Brewster’s angle in the FUV. The output is a highly linearly polarized beam. This polarizer concept was fabricated and tested in the existing McPherson 225 Vacuum Ultraviolet (VUV) spectrometer located in the Optics Branch at NASA-GSFC. Initial testing using a MgF2 crystal at the Brewster’s angle as an analyzer has shown that this design can produce state-of-the-art extinction ratios at the Hydrogen Lyman-Alpha (Ly-α) wavelength of 121.6 nm, and that the measured extinction ratio of the two crossed polarizers, ≈114, is mostly limited by the MgF2 analyzer. A polarizer with such a performance at this wavelength has never been reported and it signifies a breakthrough in FUV polarization technology. The levels of effectiveness paired with the polarizer’s compact design allows for a new polarizer capability that would one day be implemented in a future FUV spectropolarimetry space mission.

Far Ultraviolet (FUV)↗

NASA NTRSDate not supplied

Exploring Environmental and Aerosol Impacts on Maritime Tropical Convection using Airborne Radiometer, Radar, Lidar, and Dropsondes

The field deployment phase of NASA’s Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex) took place around the Philippines during August–October 2019, with the primary goal of jointly investigating aerosols and tropical meteorology at the micro-β to meso-β scales. A suite of instruments was deployed on NASA’s P-3B Orion aircraft to accomplish this mission, including: the Advanced Microwave Precipitation Radiometer (AMPR), Airborne Precipitation and cloud Radar 3rd Generation (APR-3), High Spectral Resolution Lidar 2 (HSRL2), and Advanced Vertical Atmospheric Profiling System (AVAPS) dropsondes. To examine potential aerosol influences on maritime tropical convection, P-3 flight segments throughout CAMP2Ex were binned into similar environmental groups using “low,” “medium,” and “high” values of nine AVAPS-derived parameters with known physical connections to convective frequency and/or intensity. Aerosol concentrations in each flight segment were evaluated using three HSRL2 variables at 355 and 532 nm: aerosol backscatter, aerosol extinction, and aerosol optical thickness. A set of radiometer- and radar-derived variables directly related to convective frequency and/or intensity was used to characterize convection, which included: AMPR-derived integrated cloud liquid water; polarization-corrected temperatures at 10.7, 19.35, 37.1, and 85.5 GHz; peak equivalent radar reflectivity factor (ZH); peak height of 30-dBZ ZH; and the number of radar data columns with composite ZH > 30 dBZ. The ZH analyses were performed using both Ku- and Ka-band APR-3 data. For each flight segment, correlation coefficients were calculated between each convective parameter and aerosol concentrations within the “low,” “medium,” and “high” groups for each environmental variable. The environmental stratification thresholds were then varied in a series of sensitivity tests. Several noteworthy correlations were observed between the convective and aerosol parameters within the environmental groups, especially when stratifying the environments based on their 850–500-hPa temperature lapse rate, 700–500-hPa temperature lapse rate, and K-Index. The convective parameters were often correlated most strongly with 355-nm extinction, 532-nm extinction, and 532-nm backscatter, while the presence of precipitation-sized liquid and ice hydrometeors contributed to some unexpected negative correlations. In general, as environmental conditions became more favorable for convection, a stronger correlation was observed between the convective parameters and aerosol concentrations. However, a “Goldilocks” zone of medium aerosol concentration was correlated most strongly with the convective parameters in many cases. These results stress the importance of considering environmental and aerosol conditions together when evaluating their impacts on convection. This presentation will provide a detailed discussion of these results and their implications, a summary of the limitations associated with such an analysis, and suggestions for future work.

Corey G. Amiot↗

NASA NTRSDate not supplied

Satellite-Assisted Particulate Matter (SAPM) for the Models, In situ, and Remote Sensing of Aerosols (MIRA) Working Group

Models, In situ, and Remote sensing of Aerosols (MIRA) is an international working group that provides a forum for collaborations amongst these three atmospheric aerosol communities. MIRA consists of a collection of interdisciplinary and independently funded Topic/Project groups with clear goals and generally characterized by requests for additional scientific data. The Satellite-Assisted Particulate Matter (SAPM) Topic group focuses on the study of fine particulate matter (PM2.5), as it is a major contributor to air pollution and negatively impacts human health. Our group aims to provide intercomparisons of various methods and techniques for estimating surface PM2.5 assisted by satellite remote sensors (passive and active), global aerosol models, and in situ aerosol measurements. The overall motivation of our work is to enhance PM2.5 coverage beyond in situ ground stations, which can be limited. In this presentation, we provide an overview of various PM2.5 estimation approaches by current SAPM team members, as each approach has its own strengths and limitations. One approach uses near-surface aerosol extinction retrievals from the spaceborne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and an assumed value of mass extinction efficiency to derive PM2.5 concentrations (Toth et al 2019). A study using this method found a promising agreement (R=0.60; slope=0.89) with U.S. Environmental Protection Agency (EPA) in situ PM2.5 measurements over the contiguous United States (CONUS) for a 12-year (2007-2018) period (Toth et al 2022). In a different approach combining spaceborne lidar and a model, the Cloud Aerosol Transport System (CATS) lidar and Goddard Earth Observing System (GEOS) model are blended in an ensemble variational assimilation scheme to retrieve aerosol extinction and convert speciated mass concentrations to total PM2.5. A recent study (Matus et al in prep.) found agreement within 2 μg/m3 over the CONUS on the 2016 annual mean when compared to EPA ground-based measurements. Another study explored trends in city aerosol optical depth (AOD) from a spaceborne passive remote sensor, Moderate Resolution Imaging Spectroradiometer (MODIS), and found that these trends agree well with trends in city surface PM2.5, which provides confidence in the use of city AOD for city PM2.5 trend studies (Vohra et al 2021). In a follow-on study, steep and significant trends (~2.5 to 7.8% a-1) in AOD are found for several South Asian cities (e.g., Bangalore and Hyderabad), suggesting rapid growth in PM2.5 (Vohra et al 2022). Also in this presentation, we report results on our current collective SAPM study of India, a country that exhibits high levels of PM2.5 pollution. We show the temporal (i.e., seasonal) and spatial variability of PM2.5 over India using the CALIOP and CATS+model approaches, comparisons between the estimated PM2.5 from the retrieval schemes, and validation with in situ PM2.5 ground-based observations from the Central Pollution Control Board in India. This region provides us with an excellent case study to test our PM2.5 retrievals in heavily polluted scenes and over a complex and varying topography. The SAPM Topic group actively seeks international participants/collaborators in our group, including those working with in situ aerosol measurements (e.g., ACTRIS). We are interested in aerosol datasets in order to either improve our PM2.5 estimates from various approaches (e.g., using in situ mass scattering/absorption coefficient and aerosol hygroscopic properties for various aerosol species) and/or validate the PM2.5 estimates (e.g., using in situ ground-based PM2.5 concentrations).

Travis D Toth↗

NASA NTRSDate not supplied

Variable Lidar Ratios for Marine and Dusty Marine Using MODIS AOD Constrained Retrievals and GOCART Model Simulations and their Impact on Level 2 CALIPSO Data Products in Version 5

The Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) onboard CALIPSO provided global measurements of attenuated backscatter profiles of various tropospheric aerosol species from June 2006 through June 2023. Extinction profiles are retrieved from these backscatter measurements by assuming a value for the extinction-to-backscatter or lidar ratio (LR). Up until version V4.51 of the data products, only a constant global value for each of the species has been used, spatially and temporally. However, it has been well known from various ground-based measurements that LRs of each aerosol species can potentially vary spatially as well seasonally. For the forthcoming Version 5 of the CALIPSO products, the CALIPSO team will implement variable lidar ratios at 532 nm for the species classified as “marine” and “dusty marine”. Here we present the essential elements of this scheme, which involves estimating lidar ratios by constraining Fernald solutions for the CALIOP particulate backscatter profiles using aerosol optical depths (AOD) from collocated MODIS retrievals. To account for the lack of measurements in various regions and seasons (e.g., Arctic winters), we leverage collocated model sea-salt volume fractions (SSVF) simulated by the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model and use an empirical relationship between the SSVF and LR to build hybrid climatological maps for the entire globe, i.e., using the modelled values when reliable values of the constrained LRs are not available. Initial evaluation of the resulting extinction profiles and corresponding AODs, both globally and in specific regions are presented using a limited amount of data. The primary improvement in AOD occurs in the coastal areas, like the Arabian Sea and Bay of Bengal. The estimated marine LR values in these regions are significantly higher than the constant value of 23 sr used in previous data releases, likely due to mixing with offshore pollution which results in higher AODs. Initial validation results using the CALIPSO Ocean Derived Column Optical Depth (ODCOD) retrievals and ground-based AERONET AOD measurements are presented.

CALIPSO↗

NASA NTRSDate not supplied

Spaceborne Lidar Retrievals of PM2.5 for Air Quality Studies and Applications

Fine particulate matter (PM2.5) substantially contributes to air pollution and negatively affects human health. While many studies have investigated the use of passive column-integrated aerosol optical depth to infer surface PM2.5, the use of lidar observations for air quality characterization is not nearly as extensive. Lidar measurements are critical, however, due to the vertical aerosol information they provide, including near the surface. In this presentation, we first provide an overview of various lidar-based approaches for estimating PM2.5 concentrations and then discuss how lidar measurements can assist other air quality applications. For example, estimates of PM2.5 have been obtained in a physics-based approach through CALIOP near-surface aerosol extinction retrievals, assumptions on the mass extinction efficiency, and incorporating other parameters (an aerosol hygroscopic growth factor and PM2.5/PM10 ratio). Application of this algorithm over the contiguous United States (CONUS) from 2006 to 2018 yielded larger PM2.5 values over the eastern and western CONUS (~10-15 μg/m³) and lower PM2.5 levels in the central CONUS (~5 μg/m³). These spatial patterns were similar to those from gridded PM2.5 concentrations obtained through in situ measurements at ground stations operated by the US Environmental Protection Agency. In another approach, the Cloud Aerosol Transport System (CATS) lidar was used with the Goddard Earth Observing System (GEOS) model in a 1D ensemble-based variational technique to obtain PM2.5 over the US and Europe, and the spatial patterns of the CATS/GEOS based PM2.5 concentrations generally captured those from surface stations (with corresponding hourly EPA PM2.5 vs CATS PM2.5 statistics of R=0.4 and bias=1.5 μg/m³). In our recent work, as part of the Models, In situ, and Remote sensing of Aerosols (MIRA) Working Group, we have applied both the CALIOP and CATS/GEOS based approaches over the highly polluted country of India during the post-monsoon season (September-October 2016). We derived elevated levels of two-month mean PM2.5 (~100 μg/m³) in northern India, especially near New Delhi. These high PM2.5 concentrations in the Indo-Gangetic plain are driven in large part from the seasonal burning of crop residue and meteorological conditions typical at this time of the year, such as low wind speeds and a shallow boundary layer. While the satellite-derived PM2.5 moderately replicates (R = ~0.7-0.9) the spatial variability in the two-month mean of surface in situ PM2.5 from monitoring sites operated by the Central and State Pollution Control Boards, we show results from specific scenes for which there are large deviations between the satellite-derived PM2.5 and in situ measurements. Other current work on this topic focuses on developing PM2.5 estimates using airborne high spectral resolution lidar measurements through machine learning regression algorithms and involves several parameters (e.g., aerosol extinction, color ratio, lidar ratio). Application of this method over major metropolitan areas in the US and Asia have resulted in high correlations (R = 0.93) with surface measurements. This airborne lidar approach can be adapted to spaceborne lidar measurements, and all three of these approaches can be applied to ESA’s EarthCARE Atmospheric Lidar instrument, setting the stage for the future Cloud Aerosol Lidar for Global Scale Observations of the Ocean-Land Atmosphere System (CALIGOLA) mission. Ultimately, beyond estimates of PM2.5, the aerosol vertical distribution from lidars can benefit studies involving passive sensor approaches for PM2.5 proxies (including from geostationary satellites), wildfire smoke plume injection heights, volcanic emissions (e.g., ash height retrievals), and aerosol/air quality model assimilation, evaluation, and forecasts.

Travis D Toth↗

DOE OSTI2023

n-Propylbenzene Droplet Combustion: Experiments and Numerical Modeling

n-Propylbenzene (PB, C9H12, 432K boiling point) is important as a constituent in surrogates for some transportation fuels but little is understood about its droplet burning characteristics. We present an experimental and numerical study of a fuel droplet burning under conditions where the sole means of gas transport is fuel evaporation at the droplet surface thereby creating a one-dimensional gas transport that is amenable to detailed numerical modeling. The one-dimensional gas transport that results is amenable to detailed numerical modeling. Initial droplet diameters (Do) ranged from 0.3 mm to about 5 mm to better understand the mechanisms that control burning over such a wide range of Do. For Do < 1 mm droplets were burned while anchored to 14 m SiC fibers within a sealed container in free-fall during which time the droplets were ignited by spark discharge and the burning process recorded by video cameras. Larger and free-floating droplets were studied in the spaced-based platform of the orbiting International Space Station for Do > 1.0 mm which provided unlimited times for experimental observation. Measurements of droplet, flame and soot shell diameters were made and are discussed in the presentation. The experimental results showed formation of optically thick soot clouds developing during burning that required a robust image analysis algorithm to enable measurement of droplet diameter. The measured droplet diameters were well predicted by a numerical model that included soot formation, a PB kinetic mechanism comprising 576 species and 27369 reactions, unsteady gas and liquid transport, variable properties and radiative transport. Flame diameters showed more variability compared to the simulations, depending on how the flame was defined (peak gas temperature and OH concentration). Droplets burned slower as Do was increased and the PB sooting propensity increased with Do. Flame extinction was observed for Do > 3.3 mm indicating a strong effect of radiation as Do was increased compared to the smaller droplet diameters examined where extinction was not experimentally observed. For the largest droplets examined the possibility that the observed extinction is indicative of a transition to cool flame burning is still under investigation.

Guo, Songtao↗

DOE OSTI2026

Demonstration of gold nanorod systems for enhanced total efficiency: Experimental and numerical analysis

This study investigates the photothermal performance of gold nanorods engineered to exhibit longitudinal plasmon resonances at 695 nm, 780 nm, and 970 nm. The work combines synthesis, structural characterization, extinction measurements, numerical modeling, and controlled temperature experiments to quantify how nanorod geometry, resonance tuning, concentration, and chamber shape jointly influence heat generation. Transmission electron microscopy confirms that increasing nanorod aspect ratio systematically shifts the longitudinal plasmon peak toward the near-infrared region. Extinction measurements show strong agreement with theoretical predictions, validating the numerical model across two independent datasets. Three chamber geometries were tested under laser excitation at 640 nm, 808 nm, and 980 nm: an ascending stepped base, a flat base, and a descending stepped base. Without nanorods, the ascending geometry produced the highest efficiency due to enhanced natural convection. After introducing gold nanorods, all geometries exhibited substantial thermal enhancement, with total efficiencies exceeding 20%. The strongest improvement was obtained for nanorods resonant at 780 nm with a mass concentration of 4.6 mg/mL implemented on the descending stepped-base geometry. This performance resulted from the combined effect of spectral overlapping with the 808 nm laser, the highest nanorod concentration, and localized heat accumulation that intensified buoyancy-driven flow. The findings demonstrate that total efficiency is governed by a synergistic interplay between optical resonance, nanoparticle concentration, and macroscopic chamber design, revealing the system-level coupling between nanoscale plasmonic absorption and macroscale heat-transfer phenomena. The results provide a validated framework for tuning nanoscale plasmonic absorbers and optimizing thermal systems for applications requiring efficient light-to-heat conversion.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2020

Turbulence/flame/wall interactions in non-premixed inclined slot-jet flames impinging at a wall using direct numerical simulation

In this paper, three-dimensional turbulent non-premixed oblique slot-jet flames impinging at a wall were investigated using direct numerical simulation (DNS). Two cases are considered with the Damköhler number (Da) of case A being twice that of case B. A 17 species and 73-step mechanism for methane combustion was employed in the simulations. It was found that flame extinction in case B is more prominent compared to case A. Reignition in the lower branch of combustion for case A occurs when the scalar dissipation rate relaxes, while no reignition occurs in the lower branch for case B due to excessive scalar dissipation rate. A method was proposed to identify the flame quenching edges of turbulent non-premixed flames in wall-bounded flows based on the intersections of mixture fraction and OH mass fraction iso-surfaces. The flame/wall interactions were examined in terms of the quenching distance and the wall heat flux along the quenching edges. There is essentially no flame/wall interaction in case B due to the extinction caused by excessive turbulent mixing. In contrast, significant interactions between flames and the wall are observed in case A. The quenching distance is found to be negatively correlated with wall heat flux as previously reported in turbulent premixed flames. The influence of chemical reactions and wall on flow topologies was identified. The FS/U and FC/U topologies are found near flame edges, and the NNN/U topology appears when reignition occurs. The vortex-dominant topologies, FC/U and FS/S, play an increasingly important role as the jet turbulence develops.

42 ENGINEERING↗

DOE OSTI2023

Subnanometer Visualization of Spatially Varying Local Field Resonances that Drive Tip-Enhanced Optical Spectroscopy

Our knowledge of the electromagnetic fields that power modern nanoscale optical measurements, including (non)linear tip-enhanced Raman and photoluminescence, chiefly stems from numerical simulations. Aside from idealized in silico vs heterogeneous (nano)structures in the laboratory, challenges in quantitative descriptions of nanoscale light–matter interactions more generally stem from the very nature of the problem, which lies at the interface of classical and quantum theories. This is particularly the case in ultrahigh spatial resolution measurements that are sensitive to local optical field variations that take place on subnanometer length scales. Here this work approaches this challenge through extinction-based spectral nanoimaging experiments. We demonstrate <1 nm spatial resolution in hyperspectral extinction measurements that track spatially varying plasmon resonances. We describe the principles behind our experiments and highlight more general implications of our observations.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2020

Planck 2018 results XII. Galactic astrophysics using polarized dust emission

Observations of the submillimetre emission from Galactic dust, in both total intensity I and polarization, have received tremendous interest thanks to the Planck full-sky maps. In this paper we make use of such full-sky maps of dust polarized emission produced from the third public release of Planck data. As the basis for expanding on astrophysical studies of the polarized thermal emission from Galactic dust, we present full-sky maps of the dust polarization fraction p, polarization angle ψ, and dispersion function of polarization angles S . The joint distribution (one-point statistics) of p and NH confirms that the mean and maximum polarization fractions decrease with increasing NH. The uncertainty on the maximum observed polarization fraction, pmax = 22.0 -1.4 +3.5% at 353 GHz and 80' resolution, is dominated by the uncertainty on the Galactic emission zero level in total intensity, in particular towards diffuse lines of sight at high Galactic latitudes. Furthermore, the inverse behaviour between p and S found earlier is seen to be present at high latitudes. This follows the S ∝ p -1 relationship expected from models of the polarized sky (including numerical simulations of magnetohydrodynamical turbulence) that include effects from only the topology of the turbulent magnetic field, but otherwise have uniform alignment and dust properties. Thus, the statistical properties of p, ψ, and S for the most part reflect the structure of the Galactic magnetic field. Nevertheless, we search for potential signatures of varying grain alignment and dust properties. First, we analyse the product map S × p, looking for residual trends. While the polarization fraction p decreases by a factor of 3-4 between NH = 10 20 cm -2 and NH = 2 x 10 22 cm -2 , out of the Galactic plane, this product S × p only decreases by about 25%. Because S is independent of the grain alignment efficiency, this demonstrates that the systematic decrease in p with N H is determined mostly by the magnetic-field structure and not by a drop in grain alignment. This systematic trend is observed both in the diffuse interstellar medium (ISM) and in molecular clouds of the Gould Belt. Second, we look for a dependence of polarization properties on the dust temperature, as we would expect from the radiative alignment torque (RAT) theory. We find no systematic trend of S × p with the dust temperature T d , whether in the diffuse ISM or in the molecular clouds of the Gould Belt. In the diffuse ISM, lines of sight with high polarization fraction p and low polarization angle dispersion S tend, on the contrary, to have colder dust than lines of sight with low p and high S . We also compare the Planck thermal dust polarization with starlight polarization data in the visible at high Galactic latitudes. The agreement in polarization angles is remarkable, and is consistent with what we expect from the noise and the observed dispersion of polarization angles in the visible on the scale of the Planck beam. The two polarization emission-to-extinction ratios, R P/p and R S/V , which primarily characterize dust optical properties, have only a weak dependence on the column density, and converge towards the values previously determined for translucent lines of sight. We also determine an upper limit for the polarization fraction in extinction, p V /E(B - V), of 13% at high Galactic latitude, compatible with the polarization fraction p ≈ 20% observed at 353 GHz. Taken together, these results provide strong constraints for models of Galactic dust in diffuse gas.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2024

EPCAPE-PT-LANL Measurements: Humidified Cavity Attenuated Phase Shift Spectroscopy

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: Humidified Cavity Attenuated Phase Shift Particulate Matter Single Scattering Albedo (H-CAPS-PMSSA, Aerodyne Inc) Data Notes: The scattering truncation correction was not applied to Bsca. The Bext needs no correction. Files: data_10sec_CAPS.csv, data_10min_CAPS.csv Header: - Bext_wet_CAPS_450nm[1/Mm]: Wet aerosol extinction coefficient measured at 450 nm by the CAPS, in inverse megameters (Mm⁻¹). - Bsca_wet_CAPS_450nm[1/Mm]: Wet aerosol scattering coefficient measured at 450 nm by the CAPS, in inverse megameters (Mm⁻¹). - Temp_wet_CAPS[K]: Temperature inside the wet CAPS measurement chamber, in Kelvin. - Bext_dry_CAPS_450nm[1/Mm]: Dry aerosol extinction coefficient measured at 450 nm by the CAPS, in inverse megameters (Mm⁻¹). - Bsca_dry_CAPS_450nm[1/Mm]: Dry aerosol scattering coefficient measured at 450 nm by the CAPS, in inverse megameters (Mm⁻¹). - Temp_dry_CAPS[K]: Temperature inside the dry CAPS measurement chamber, in Kelvin. - Wet_RH_preCAPS[%]: Relative humidity before entering the wet CAPS, in percent. - Wet_RH_postCAPS[%]: Relative humidity after exiting the wet CAPS, in percent. - Humidifier_RH_CAPS[%]: Relative humidity inside the humidifier used with the CAPS, in percent. - dualCAPS_inlet_RH[%]: Relative humidity at the inlet of the dual (wet/dry) CAPS setup, in percent. - Wet_Temp_preCAPS[C]: Temperature before entering the wet CAPS, in degrees Celsius. - Wet_Temp_postCAPS[C]: Temperature after exiting the wet CAPS, in degrees Celsius. - Humidifier_Temp[C]: Temperature inside the humidifier used with the CAPS, in degrees Celsius. - dualCAPS_inlet_Temp[C]: Temperature at the inlet of the dual (wet/dry) CAPS setup, in degrees Celsius. - Zero_dry_CAPS: 1 is a calibration check for the dry CAPS to ensure zero reading under filter air conditions. - Zero_wet_CAPS: 1 is a calibration check for the wet CAPS to ensure zero reading under filter air conditions. - 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↗

NASA NTRSDate not supplied

Particulate Emission and Optical Measurements in n-Heptane Low-Swirl Non-Premixed Flames at Elevated Pressures

A series of ground combustion tests conducted at elevated pressures demonstrates in-chamber optical measurements of soot emissions, combined with conventional gaseous and particle emissions sampling techniques. Utilizing a micro-radial-entry counter-swirl (MRX) burner, we successfully stabilized an n-heptane low-swirl, non-premixed spray flame across a wide range of equivalence ratios at pressures reaching 250 psia. Our optical diagnostics feature a temporally gated diffused-backlight illumination extinction imaging (DBI-EI) system, equipped with a 470-nm strobe high-intensity LED array as the illumination source, along with a line-of-sight telecentric camera. By accessing the flame tube, the pulsed DBI-EI provides illuminating optical extinction images, enabling experimental estimation of soot volume fractions within the reaction zone. This imaging technique will allow for real-time observation of soot formation dynamics occurring above the air-blast fuel injector. To further enhance our analysis, we employed simultaneous gaseous and particulate extractive diagnostics, interpreting in-flame particulate information through CO2 sampling, exhaust particle sizing, and particle counting. The processed dataset reveals a promising application of DBI-EI for propulsion emission analysis in high-pressure environments, where optical beam-steering effects can significantly impact results. This report is essential to bridging the divide between in-flame optical diagnostics and exhaust extractive measurements. By achieving an understanding of non-premixed combustion emission characteristics, we attempt to provide invaluable data for computer code validation, advancing the field of combustion research and supporting the development of cleaner, more efficient engines.

high-pressure flame↗

NASA NTRSDate not supplied

Particulate Emission and Optical Measurements in n-Heptane Low-Swirl Non-Premixed Flames at Elevated Pressures

high-pressure flame↗

DOE OSTI2021

Active Tuning of Optical Constants in the Visible–UV: Praseodymium-Doped Ceria—a Model Mixed Ionic–Electronic Conductor

Mixed ionic-electronic conductors offer chemical and electrical means for active tuning of their optical constants, e.g. with variations in oxygen non-stoichiometry in Pr 0.1 Ce 0.9 O 2-δ , enabling implementation of adaptive thin film optical devices. Here, we demonstrate in-situ chemo-tuning of the extinction coefficient in Pr 0.1 Ce 0.9 O 2-δ at elevated temperatures and provide a tuning model that treats the interdependence of mobile oxygen vacancies and small polarons coupled to variations in optically active praseodymium ions. Further, a new means for electro-tuning of the optical constants of mixed ionic-electronic conductors was demonstrated experimentally and modeled for Pr 0.1 Ce 0.9 O 2-δ thin films deposited on grid-like electrode structures. Modeling of non-steady state optical transmittance modulations in the latter allows for estimation of oxygen vacancy mobility that determines the switching speed of the device. Quenched-in values of nr and k to room temperature become nonvolatile, providing a modulation range in the extinction coefficient of Δk ~0.1 (change of ~800%) and in the refractive index of Δn r ~0.1 (relative to initial n r of ~2.35). Key figures of merit including, transmission optical modulation of ~0.04 per 1 mV nm -1 , switching energy per area of 670 pJ μm -2 and switching times of seconds, were demonstrated, with further improvements possible.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Enhancing and Extinguishing the Different Emission Features of 2D (EA(1-)(x)FA(x))(4)Pb3Br10 Perovskite Films

2D hybrid perovskites are attractive for optoelectronic devices. In thin films, the color of optical emission and the texture of crystalline domains are often difficult to control. Here, a method for extinguishing or enhancing different emission features is demonstrated for the family of 2D Ruddlesden-Popper perovskites (EA(1-)(x)FA(x))(4)Pb3Br10 (EA = ethylammonium, FA = formamidinium). When grown from aqueous hydrobromic acid, crystals of (EA(1-)(x)FA(x))(4)Pb3Br10 retain all the emission features of their parent compound, (EA)(4)Pb3Br10. Surprisingly, when grown from dimethylformamide (DMF), an emission feature, likely self-trapped exciton (STE), near 2.7 eV is missing. Extinction of this feature is correlated with DMF being incorporated between the 2D Pb-Br sheets, forming (EA(1-)(x)FA(x))(4)Pb3Br10 center dot(DMF)(y). Without FA, films grown from DMF form (EA)(4)Pb3Br10, retain little solvent, and have strong emission near 2.7 eV. Slowing the kinetics of film growth strengthens a different emission feature, likely a different type of STE, which is much broader and present in all compositions. Films of (EA(1-)(x)FA(x))(4)Pb3Br10 center dot(DMF)(y) have large, micron-sized domains and homogeneous orientation of the semiconducting sheets, resulting in low electronic disorder near the absorption edge. The ability to selectively strengthen or extinguish different emission features in films of (EA(1-)(x)FA(x))(4)Pb3Br10 center dot(DMF)(y) reveals a pathway to tune the emission color in these compounds.

2D halide perovskites↗

DOE OSTI2020

Development of limited-view tomography for measurement of Spray G plume direction and liquid volume fraction

Abstract The method for direct injection of fuel in the cylinder of an IC engines is important to high-efficiency and low-emission performance. Optical spray diagnostics plays an important role in understanding plume movement and interaction for multi-hole injectors, and providing baseline understanding used for computational optimization of fuel delivery. Traditional planar or line-of-sight diagnostics fail to capture the liquid distribution because of optical thickness concerns. This work proposes a high-speed (67 kHz) extinction imaging technique at various injector rotations coupled to computed tomography (CT) for time-resolved reconstruction of liquid volume fraction in three dimensions. The number of views selected and processing were based on synthetic (modeled) liquid volume fraction data where extinction and CT adequately reconstructed each plume. The exercise showed that for an 8-hole, symmetric-design injector (ECN Spray G), only three different views are enough to reproduce the direction of each plume, and particularly the mean plume direction. Therefore, the number of views was minimized for experiments to save expense. Measurements applying this limited-view technique confirm plume–plume variations also detected with mechanical patternation, while providing better spatial and temporal resolution than achieved previously. Uncertainties due to the limited view within pressurized spray chambers, the droplet size, and optically thick regions are discussed. Graphic abstract

42 ENGINEERING↗