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DOE OSTI2023

TAP Absorption Coefficients

The data set of aerosol light absorption coefficients were collected by two tricolor absorption photometers (TAP; Brechtel Model 2901) in July and August, 2022 during the TRACER field campaign at the AMF1 site in La Porte, Texas. One of the TAPs at the La Porte site was an RGB model measuring aerosol light absorption at 652, 528, 467 nm, and the other was an UV model measuring absorption at the same red and green wavelengths but at an additional UV wavelength at 365 nm. Since TAP is a filter-based optical instrument using 47-mm glass fiber filters, the output absorption coefficients are corrected for filter loading and scattering effects based on a correction scheme developed in "Comment on ‘Calibration and Intercomparison of Filter-Based Measurements of Visible Light Absorption by Aerosols’" by John A. Ogren 2010. This uploaded dataset contains both the Ogren corrected absorption coefficients (column header with “ Ogren”) and the raw absorption coefficients without the correction scheme (column header with “_ Raw”). During the field campaign, the two TAPs operated side by side with a shared inlet at a flow rate of 2 lpm. In July, no inlet impactors/cyclones were installed; however, beginning in August, a PM2.5 cyclone inlet was installed.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

IPN Absorption Coefficients

The dataset contains aerosol light absorption and scattering coefficients measured by three single-wavelength Integrated Photoacoustic Nephelometers (IPN). The absorption coefficients were measured at 405, 721, and 1047 nm, while the scattering coefficients were measured at 405 and 721 nm. The single scattering albedo (SSA) at 405 and 721 nm were also calculated from the IPN measurements. The three IPNs shared a common inlet without impactor/cyclone in July; in August, a PM2.5 cyclone inlet was installed to reduce measurement noise and improve data quality. The 721-nm IPN experienced laser shutdown issues, causing missing of a large fraction of the 721-nm measurements, especially in July. As described before, the 721-nm laser issue was less frequent in August after the cyclone installation, improving the data completeness and quality. The IPN raw data were noisy, making identifying patterns and trends difficult; therefore, the hourly average data are recommended over the raw data. The hourly average data were cross-checked with the filter-based TAP and PSAP measurements, which showed that their patterns, trends, and peaks matched. However, due to the differences in working mechanisms and principles of the filter-based and photoacoustic particle-phase instruments, the IPN measurements are lower than the filter-based measurements despite that they have consistent patterns, trends, and peaks.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Continuous Light Absorption Photometer (CLAP) Instrument Handbook

Reliable measurements of aerosol light absorption are crucial for quantifying the radiative forcing of climate. As a consequence, light absorption measurements are recommended for all stations in the Global Atmosphere Watch network, which is coordinated by the World Meteorological Organization. Aerosol light absorption is often dominated by soot-like particles produced by the incomplete combustion of carbonaceous fuels, commonly termed "black carbon", and optical methods are the primary way that equivalent black carbon concentrations are derived. Two basic approaches are used for determining the aerosol light absorption coefficient: in situ methods where the absorption is measured while the particles are suspended in air, and filter-based methods where the particles are deposited on a filter for real-time optical analysis. In situ methods are inherently more accurate because the physical state of the particles can be changed by the act of filtration. Unfortunately, currently available instruments for in situ measurements are more expensive and difficult to operate than filter-based methods, making them better suited for use in intensive field campaigns or as laboratory reference instruments. Filter-based instruments, because of their lower cost and simpler operation, have been the preferred choice for long-term measurements of aerosol light absorption in monitoring networks.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Establishing robust correction schemes for improved and reliable ARM-AOS aerosol optical data products

Aerosol light absorption and scattering of solar radiation play an important role in the earth’s atmosphere in terms of direct and semi-direct radiative forcing. Optical parameters of importance to the US Department of Energy (DOE) climate models include absorption and scattering coefficients, single scattering albedo (SSA), absorption Angstrom exponents (AAE), and the asymmetry parameter (g). These parameters depend on aerosol size, shape and composition (refractive index), and are spectrally sensitive in the shortwave region. Additionally, these parameters have a complex dependency on the emission source, especially for carbonaceous aerosols. The DOE Atmospheric Radiation Measurement (ARM) user facility has deployed aerosol observing systems (AOS) containing several filter-based instruments to measure and constrain aerosol optical properties and related parameters at multiple sites worldwide. For measurement of aerosol light absorption, the AOS includes filter-based instruments (particle soot absorption photometer and tricolor absorption photometer) that infer particle-phase aerosol absorption coefficients at nominal red, green, and blue wavelength bands from the attenuation (ATN) of light passing through a particulate filter on which aerosols are deposited. Measurement of aerosol scattering is done in situ using nephelometers. By combining inferred absorption coefficients from filter-based ATN measurements and in situ scattering coefficients, value-added products (VAPs) such as SSA, AAE, and g are derived.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2018

Correcting for Trace Gas Absorption When Retrieving Aerosol Optical Depth from Satellite Observations of Reflected Shortwave Radiation

Retrieving aerosol optical depth (AOD) from top-of-atmosphere (TOA) satellite measured radiance requires separating the aerosol signal from the total observed signal. Total TOA radiance includes signal from underlying surface and from atmospheric constituents such as aerosols, clouds and gases. Multispectral retrieval algorithms, such as the dark-target (DT) algorithm that operates upon Moderate Resolution Imaging Spectroradiometer (MODIS, onboard Terra and Aqua satellites) and Visible Infrared Imaging Radiometer Suite (VIIRS, onboard Suomi-NPP) sensors, use wavelength bands in "window" regions. However, while small, the gas absorptions in these bands are non-negligible and require correction. In this paper we use High-resolution TRANsmission (HITRAN) database and Line-by-Line Radiative Transfer Model (LBLRTM) to derive consistent gas corrections for both MODIS and VIIRS wavelength bands. Absorptions from H2O, CO2 and O3 are considered, as well as other trace gases. Even though MODIS and VIIRS bands are "similar", they are different enough that applying MODIS specific gas corrections to VIIRS observations results in an underestimate of global mean AOD (by 0.01), but with much larger regional AOD biases up to 0.07. As recent studies are attempting to create a long-term data record by joining multiple satellite datasets, including MODIS and VIIRS, the consistency of gas correction becomes even more crucial.

Satellite Remote Sensing↗

NASA NTRS2019

Retrieving Aerosol Characteristics From the PACE Mission, Part 1: Ocean Color Instrument

NASA’s Plankton, Aerosol, Clouds, ocean Ecosystem (PACE) satellite mission is scheduled to launch in 2022, with the Ocean Color Instrument (OCI) on board. For the first time reflected sunlight from the Earth across a broad spectrum from the ultraviolet (UV: 350 nm) to the short wave infrared (SWIR: 2260 nm) will be measured from a single instrument at 1 km spatial resolution. While seven discrete bands will represent the SWIR, the spectrum from 350 to 890 nm will be continuously covered with a spectral resolution of 5 nm. OCI will thus combine in a single instrument (and at an enhanced spatial resolution for the UV) the heritage capabilities of the Moderate resolution Imaging Spectroradiometer (MODIS) and the Ozone Monitoring Instrument (OMI), while covering the oxygen A-band (O2A). Designed for ocean color and ocean biology retrievals, OCI also enables continuation of heritage satellite aerosol products and the development of new aerosol characterization from space. In particular the combination of MODIS and OMI characteristics allows deriving aerosol height, absorption and optical depth along with a measure of particle size distribution. This is achieved by using the traditional MODIS visible-to-SWIR wavelengths to constrain spectral aerosol optical depth and particle size. Extrapolating this information to the UV channels allows retrieval of aerosol absorption and layer height. A more direct method to derive aerosol layer height makes use of O2A absorption methods, despite the relative coarseness of the nominal 5 nm spectral resolution of OCI. Altogether the PACE mission with OCI will be an unprecedented opportunity for aerosol characterization that will continue climate data records from the past decades and propel aerosol science forward toward new opportunities.

PACE↗

NASA NTRS2004

In-Situ Measurements of Aerosol Optical Properties using New Cavity Ring-Down and Photoacoustics Instruments and Comparison with more Traditional Techniques

Carbonaceous species (BC and OC) are responsible for most of the absorption associated with aerosol particles. The amount of radiant energy an aerosol absorbs has profound effects on climate and air quality. It is ironic that aerosol absorption coefficient is one of the most difficult aerosol properties to measure. A new cavity ring-down (CRD) instrument, called Cadenza (NASA-ARC), measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. Absorption coefficient is obtained from the difference of measured extinction and scattering within the instrument. Aerosol absorption coefficient is also measured by a photoacoustic (PA) instrument (DRI) that was operated on an aircraft for the first time during the DOE Aerosol Intensive Operating Period (IOP). This paper will report on measurements made with this new instrument and other in-situ instruments during two field recent field studies. The first field study was an airborne cam;oaign, the DOE Aerosol Intensive Operating Period flown in May, 2003 over northern Oklahoma. One of the main purposes of the IOP was to assess our ability to measure extinction and absorption coefficient in situ. This paper compares measurements of these aerosol optical properties made by the CRD, PA, nephelometer, and Particle Soot Absorption Photometer (PSAP) aboard the CIRPAS Twin-Otter. During the IOP, several significant aerosol layers were sampled aloft. These layers are identified in the remote (AATS-14) as well as in situ measurements. Extinction profiles measured by Cadenza are compared to those derived from the Ames Airborne Tracking Sunphotometer (AATS-14, NASA-ARC). The regional radiative impact of these layers is assessed by using the measured aerosol optical properties in a radiative transfer model. The second study was conducted in the Caldecott Tunnel, a heavily-used tunnel located north of San Francisco, Ca. The aerosol sampled in this study was characterized by fresh automobile and diesel exhaust. Measurements from Cadenza and from an aethalometer are presented. The aethalometer is a filter-based photometer and the infrared channel is calibrated to produce a measure of BC mass loading.

Strawa, A. W.↗

DOE OSTI2020

An Exploratory Approach Using Regression and Machine Learning in the Analysis of Mass Absorption Cross Section of Black Carbon Aerosols: Model Development and Evaluation

Mass absorption cross-section of black carbon (MAC BC ) describes the absorptive cross-section per unit mass of black carbon, and is, thus, an essential parameter to estimate the radiative forcing of black carbon. Many studies have sought to estimate MAC BC from a theoretical perspective, but these studies require the knowledge of a set of aerosol properties, which are difficult and/or labor-intensive to measure. We therefore investigate the ability of seven data analytical approaches (including different multivariate regressions, support vector machine, and neural networks) in predicting MAC BC for both ambient and biomass burning measurements. Our model utilizes multi-wavelength light absorption and scattering as well as the aerosol size distributions as input variables to predict MAC BC across different wavelengths. We assessed the applicability of the proposed approaches in estimating MAC BC using different statistical metrics (such as coefficient of determination (R 2 ), mean square error (MSE), fractional error, and fractional bias). Overall, the approaches used in this study can estimate MAC BC appropriately, but the prediction performance varies across approaches and atmospheric environments. Based on an uncertainty evaluation of our models and the empirical and theoretical approaches to predict MAC BC , we preliminarily put forth support vector machine (SVM) as a recommended data analytical technique for use. We provide an operational tool built with the approaches presented in this paper to facilitate this procedure for future users.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2012

Photoacoustic Optical Properties at UV, VIS, and near IR Wavelengths for Laboratory Generated and Winter Time Ambient Urban Aerosols

We present the laboratory and ambient photoacoustic (PA) measurement of aerosol light absorption coefficients at ultraviolet wavelength (i.e., 355 nm) and compare with measurements at 405, 532, 870, and 1047 nm. Simultaneous measurements of aerosol light scattering coefficients were achieved by the integrating reciprocal nephelometer within the PA's acoustic resonator. Absorption and scattering measurements were carried out for various laboratory generated aerosols, including salt, incense, and kerosene soot to evaluate the instrument calibration and gain insight on the spectral dependence of aerosol light absorption and scattering. Ambient measurements were obtained in Reno, Nevada, between 18 December 2009 and 18 January 2010. The measurement period included days with and without strong ground level temperature inversions, corresponding to highly polluted (freshly emitted aerosols) and relatively clean (aged aerosols) conditions. Particulate matter (PM) concentrations were measured and analyzed with other tracers of traffic emissions. The temperature inversion episodes caused very high concentration of PM (sub 2.5) and PM( sub 10) (particulate matter with aerodynamic diameters less than 2.5 micrometers and 10 micrometers, respectively) and gaseous pollutants: carbon monoxide (CO), nitric oxide (NO), and nitrogen dioxide (NO2). The diurnal change of absorption and scattering coefficients during the polluted (inversion) days increased approximately by a factor of two for all wavelengths compared to the clean days. The spectral variation in aerosol absorption coefficients indicated a significant amount of absorbing aerosol from traffic emissions and residential wood burning. The analysis of single scattering albedo (SSA), Angstrom exponent of absorption (AEA), and Angstrom exponent of scattering (AES) for clean and polluted days provides evidences that the aerosol aging and coating process is suppressed by strong temperature inversion under cloudy conditions. In general, measured UV absorption coefficients were found to be much larger for biomass burning aerosol than for typical ambient aerosols.

absorptivity↗

NASA NTRS1984

Atmospheric Effects on Remote Sensing of the Earth's Surface

The main causes and magnitude of the atmospheric effects on remote sensing of the Earth's surface are determined. Theoretical study as well as measurements are included. The knowledge gained from this study will be used to develop atmospheric correction algorithms and to test them with satellite data. In a theoretical investigation of the relative effects of the aerosol optical thickness, absorption, and size distribution on remote sensing, it was found that aerosol absorption has a significant effect on satellite measurements of surface reflectivity. The absorption effect is stronger for high than for low surface reflectances. The aerosol optical thickness is dominant for small surface reflectances. The accuracy of clustering algorithms depends on both parameters. The vegetation index, however, is affected by the optical thickness but only weakly affected by the absorption. A laboratory simulation of the atmospheric effect on the radiance of sunlight scattered from the Earth's surface-atmosphere system was performed. This experiment verified the existence of the adjacency effect (the effect of a bright field on the radiance detected above a dark field) and was used to test 3-D radiative transfer models. In a theoretical study it was found that atmospheric scattering resulting from the adjacency effect reduces the separability between surface classes.

Fraser, R. E.↗

NASA NTRS2001

Shortwave Radiative Fluxes, Solar-Beam Transmissions, and Aerosol Properties: TARFOX and ACE-2 Find More Absorption from Flux Radiometry than from Other Measurements

The Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) and the Second Aerosol Characterization Experiment (ACE-2) made simultaneous measurements of shortwave radiative fluxes, solar-beam transmissions, and the aerosols affecting those fluxes and transmissions. Besides the measured fluxes and transmissions, other obtained properties include aerosol scattering and absorption measured in situ at the surface and aloft; aerosol single scattering albedo retrieved from skylight radiances; and aerosol complex refractive index derived by combining profiles of backscatter, extinction, and size distribution. These measurements of North Atlantic boundary layer aerosols impacted by anthropogenic pollution revealed the following characteristic results: (1) Better agreement among different types of remote measurements of aerosols (e.g., optical depth, extinction, and backscattering from sunphotometers, satellites, and lidars) than between remote and in situ measurements; 2) More extinction derived from transmission measurements than from in situ measurements; (3) Larger aerosol absorption inferred from flux radiometry than from other measurements. When the measured relationships between downwelling flux and optical depth (or beam transmission) are used to derive best-fit single scattering albedos for the polluted boundary layer aerosol, both TARFOX and ACE-2 yield midvisible values of 0.90 +/- 0.04. The other techniques give larger single scattering albedos (i.e. less absorption) for the polluted boundary layer, with a typical result of 0.95 +/- 0.04. Although the flux-based results have the virtue of describing the column aerosol unperturbed by sampling, they are subject to questions about representativeness and other uncertainties (e.g., unknown gas absorption). Current uncertainties in aerosol single scattering albedo are large in terms of climate effects. They also have an important influence on aerosol optical depths retrieved from satellite radiances. More tests are needed of the consistency among different methods and of the effects of changing humidity on aerosol.

Russell, Philip B.↗

NASA NTRS2006

Impact of Nonabsorbing Anthropogenic Aerosols on Clear-Sky Atmospheric Absorption

Absorption of solar radiation by atmospheric aerosol has become recognized as important in regional and global climate. Nonabsorbing, hydrophilic aerosols, such as sulfate, potentially affect atmospheric absorption in opposing ways: first, decreasing absorption through aging initially hydrophobic black carbon (BC) to a hydrophilic state, enhancing its removal by wet scavenging, and consequently decreasing BC lifetime and abundance, and second, increasing absorption through enhancement of the BC absorption efficiency by internal mixing as well as through increasing the amount of diffuse solar radiation in the atmosphere. On the basis of General Circulation Model studies with an embedded microphysical aerosol module we systematically demonstrate the significance of these mechanisms both on the global and regional scales. In remote transport regions, the first mechanism prevails, reducing atmospheric absorption, whereas in the vicinity of source regions, despite enhanced wet scavenging, absorption is enhanced owing to the prevalence of the second mechanisms. Our findings imply that the sulfur to BC emission ratio plays a key role in aerosol absorption.

Stier, Philip↗

NASA NTRS1997

Light Absorption in the Stratosphere: Trend, Soot Aerosol Concentration and Contribution by...

The light absorption coefficient, Beta(a) of the stratospheric aerosol is an important quantity that determines its radiative effects. When combined with the aerosol scattering coefficient, Beta(a) it becomes possible to evaluate the aerosol single scatter albedo, omega = Beta(s)/(Beta(s) + Beta(a)) which is essential for modeling the overall radiative effects of the stratospheric aerosol. Pollack1 determined that omega = 0.98 is a critical value that separates stratospheric cooling from warming.

Pueschel, R. F.↗

DOE OSTI2021

Humidified single-scattering albedometer (H-CAPS-PM SSA ): Design, data analysis, and validation

In this work, we report the development and validation of a new humidified aerosol single-scattering albedometer to quantify the effects of water uptake on submicrometer particle optical properties. The instrument simultaneously measures in situ aerosol light extinction ( σ ep ) and scattering ( σ sp ) using a cavity-attenuated phase shift-single scattering albedo particulate matter (PM) monitor (CAPS-PM SSA , Aerodyne Research, Inc., Billerica, MA, USA). It retrieves by difference aerosol light absorption ( σ ap ) and directly quantifies aerosol single-scattering albedo (SSA), the aerosol “brightness.” We custom built a relative humidity (RH) control system using a water vapor-permeable membrane humidifier and coupled it to the CAPS-PM SSA to enable humidified aerosol observations. Our humidified instrument (H-CAPS-PM SSA ) overcomes problems with noise caused by mirror purge-flow humidification, heating, and characterizing cell RH. Careful angular truncation corrections in scattering, particularly for larger particles, were combined with empirical observations. Results show that the optimal operational size to be D p < 400 nm. The H-CAPS-PM SSA was evaluated with several pure single-component aerosols including ammonium sulfate ((NH 4 ) 2 SO 4 ), absorbing nigrosin, and levoglucosan, an organic biomass smoke tracer. The measured σ ep , σ sp , and the derived optical hygroscopicity parameter ( κ ) for size-selected ammonium sulfate are in good agreement with literature values. For dry size-selected nigrosin in the 100 < D p < 400 nm range, SSA values increased from ~0.3 to 0.65 with increasing D p . The enhancement in nigrosin σ ap at RH = 80% was a factor of 1.05–1.20 relative to dry conditions, with the larger particles showing greater enhancement. SSA increased with RH with the largest fractional enhancement measured for the smallest particles. For polydisperse levoglucosan, we measured an optical κ of 0.26 for both light extinction and scattering and negligible absorption. Our new instrument enables reliable observations of the effects of ambient humidity on mixed aerosol optical properties, particularly for light-absorbing aerosols whose climate forcing is uncertain due to measurement gaps.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1984

Properties of the Upper Tropospheres of Uranus and Neptune Derived from Observations at Visible to Near-Infrared Wavelengths

Photons at wavelengths between 0.3 and 4.5 microns penetrate the atmospheres of Uranus and Neptune to pressures between about 0.01 bar and 10 bars. This pressure range brackets the radiative convective boundary in both atmospheres and is therefore designated upper troposphere. Physical processes which govern the transfer of radiation in Uranus's and Neptune's atmospheres at these wavelengths include Rayleigh/Raman scattering by hydrogen, scattering and broadband absorption by suspended aerosol particles and absorption in discrete bands and lines by methane and hydrogen. Consequently, tropospheric properties constrained by observations at these wavelengths include optical properties and distribution of aerosol particles, methane/hydrogen ratio, and ortho/para hydrogen ratio. Recent observations of Uranus and Neptune in this spectral range, are reviewed and compared with predictions based on models of the atmospheric structures. Significant results for Uranus include the presence of an opaque lower boundary to the visible atmosphere very near the level corresponding to 2 bars pressure, and consequently a methane/hydrogen ratio no less than 3 percent.

Bergstralh, J. T.↗

NASA NTRS1974

Scattering and absorption from poly-dispersed aerosols

Results from numerical computations of the diffuse sky radiances and degree of polarization are given. These results were obtained by solving the equation of radiative transfer in the formulation of Eschelbach. In these computations, multiple scattering and absorption by aerosol particles were considered. In addition, results from experimental measurements of the complex refractive index of aerosol samples at different relative humidities are presented. From the radiation flux divergences which were computed based on the determined properties of atmospheric aerosol particles, atmospheric heating rates were derived which were found to be comparable to the heating rates by water vapor.

Bullrich, K.↗

NASA NTRS2017

The HITRAN2016 Molecular Spectroscopic Database

This paper describes the contents of the 2016 edition of the HITRAN molecular spectroscopic compilation. The new edition replaces the previous HITRAN edition of 2012 and its updates during the intervening years. The HITRAN molecular absorption compilation is composed of five major components: the traditional line-by-line spectroscopic parameters required for high-resolution radiative-transfer codes, infrared absorption cross-sections for molecules not yet amenable to representation in a line-by-line form, collision-induced absorption data, aerosol indices of refraction, and general tables such as partition sums that apply globally to the data. The new HITRAN is greatly extended in terms of accuracy, spectral coverage, additional absorption phenomena, added line-shape formalisms, and validity. Moreover, molecules, isotopologues, and perturbing gases have been added that address the issues of atmospheres beyond the Earth. Of considerable note, experimental IR cross-sections for almost 300 additional molecules important in different areas of atmospheric science have been added to the database. The compilation can be accessed through www.hitran.org. Most of the HITRAN data have now been cast into an underlying relational database structure that offers many advantages over the long-standing sequential text-based structure. The new structure empowers the user in many ways. It enables the incorporation of an extended set of fundamental parameters per transition, sophisticated line-shape formalisms, easy user-defined output formats, and very convenient searching, filtering, and plotting of data. A powerful application programming interface making use of structured query language (SQL) features for higher-level applications of HITRAN is also provided.

HITRAN↗

NASA NTRS2021

Retrievals of Aerosol Optical Depth and Spectral Absorption from DSCOVR EPIC

A new algorithm is described for joint retrievals of the aerosol optical depth and spectral absorption from EPIC observations in the UV—Vis spectral range. The retrievals are illustrated on examples of the wildfire smoke events over North America, and dust storms over greater Sahara region in 2018. An initial evaluation of single scattering albedo (SSA) at 443 nm over these regions shows a good agreement with AERONET data, generally within the uncertainty of AERONET SSA of ± 0.03. A particularly good agreement is achieved for dust with R∼0.62, rmse∼0.02, negligible bias, and 85% points within the expected error. This new capability is part of version 2 MAIAC EPIC algorithm. The v2 algorithm has recently completed reprocessing of the EPIC record covering the period of 2015–2020.

EPIC↗