A broadband cavity-enhanced spectrometer for atmospheric aerosol light extinction measurements
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Light extinction by aerosols during summer air pollution
In order to utilize satellite measurements of optical thickness over land for estimating aerosol properties during air pollution episodes, the optical thickness was measured from the surface and investigated. Aerosol optical thicknesses have been derived from solar transmission measurements in eight spectral bands within the band lambda 440-870 nm during the summers of 1980 and 1981 near Washington, DC. The optical thicknesses for the eight bands are strongly correlated. It was found that first eigenvalue of the covariance matrix of all observations accounts for 99 percent of the trace of the matrix. Since the measured aerosol optical thickness was closely proportional to the wavelength raised to a power, the aerosol size distribution derived from it is proportional to the diameter (d) raised to a power for the range of diameters between 0.1 to 1.0 micron. This power is insensitive to the total optical thickness. Changes in the aerosol optical thickness depend on several aerosol parameters, but it is difficult to identify the dominant one. The effects of relative humidity and accumulation mode concentration on the optical thickness are analyzed theoretically, and compared with the measurements.
Kaufman, Y. J.↗
A broadband cavity-enhanced spectrometer for atmospheric aerosol light extinction measurements
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54 ENVIRONMENTAL SCIENCES↗
Analysis of Antarctic stratospheric aerosol properties using SAGE II extinction measurements
Multispectra aerosol extinction data for the fall and spring of 1987 measured by the SAGE II sensor are employed to determine the physical characteristics of aerosols within the springtime Antarctic polar vortex. Attention is given to the physical processes that give rise to the apparent springtime 'cleansing' of the Antarctic stratosphere. The inferred vertical and radial structure compare favorably with in situ measurements but yield a previously unavailable 2D structure to the distribution of aerosols within the polar vortex. The springtime 'cleansing' of the Antarctic stratosphere is found to be a result of both large-scale subsidence and the preferential removal of large particles by the nucleation and subsequent sedimentation of polar stratospheric clouds.
Thomason, Larry W.↗
Airborne Sunphotometry of African Dust and Marine Boundary Layer Aerosols in PRIDE
The Puerto Rico Dust Experiment (PRIDE) was conducted during summer 2000 to study the radiative, microphysical and transport properties of Saharan dust in the Caribbean region. During PRIDE, NASA Ames Research Center's six-channel airborne autotracking sunphotometer (AATS-6) was operated aboard a Piper Navajo airplane based at Roosevelt Roads Naval Station on the northeast coast of Puerto Rico. AATS-6 measurements were taken during 21 science flights off the coast of Puerto Rico in the western Caribbean. Data were acquired within and above the Marine Boundary Layer (MBL) and the Saharan Aerosol Layer (SAL) up to 5.5 km altitude tinder a wide range of dust loadings. Aerosol optical depth (AOD) spectra and columnar water vapor (CWV) values have been calculated from the AATS-6 measurements by using sunphotometer calibration data obtained at Mauna Loa Observatory (3A kin ASL) before (May) and after (October) PRIDE. Mid-visible AOD values measured near the surface during PRIDE ranged from 0.07 on the cleanest day to 0.55 on the most turbid day. Values measured above the MBL were as high as 0.35; values above the SAL were as low as 0.01. The fraction of total column AOD due to Saharan dust cannot be determined precisely from AATS-6 AOD data alone due to the uncertainty in the extent of vertical mixing of the dust down through the MBL. However, analyses of ground-based and airborne in-situ aerosol sampling measurements and ground-based aerosol lidar backscatter data should yield accurate characterization of the vertical mixing that will enable calculation of the Saharan dust AOD component from the sunphotometer data. Examples will be presented showing measured AATS-6 AOD spectra, calculated aerosol extinction and water vapor density vertical profiles, and aerosol size distributions retrieved by inversion of the AOD spectra. Near sea-surface AOD spectra acquired by AATS-6 during horizontal flight legs at 30 m ASL are available for validation of AOD derived from coincident satellite sensor (TOMS, MODIS, MISR) measurements. AATS-6 AOD data acquired during numerous aircraft ascents and descents through the MBL and the SAL should permit atmospheric column closure analyses with respect to aerosol optical depth, extinction, and size distribution by comparison with coincident aircraft-based in-situ particle size distribution measurements and ground-based (Cabras Island, Puerto Rico) micropulse lidar aerosol backscatter measurements. The aerosol information derived from the column closure analyses can be used subsequently to calculate radiative flux changes, which can then be compared with coincident spectral flux measurements taken from aboard the aircraft with a solar spectral flux radiometer.
Livingston, John M.↗
Observations of aerosol by the HALOE experiment onboard UARS - A preliminary validation
The HALOE experiment measures vertical profiles of aerosol extinction at five infrared wavelengths. Four of these observations are obtained using a combination of gas filter and broadband radiometer measurements in bands of HF, HCl, CH4, and NO centered at wavelengths of 2.45, 3.40, 3.45, and 5.26 microns, respectively. The fifth is obtained using broadband radiometer measurements of CO2 transmission at 2.79 microns. Error analysis shows that the random extinction uncertainties are generally less than 10 percent in the aerosol layer, increasing to over 20 percent at the profile tops. HALOE spectral extinction measurements are shown to be consistent with predicted spectral extinction for stratospheric sulfate aerosol. Profile comparisons between HALOE and independent sources result in generally good agreement in the shape and magnitude of peak extinction and the altitude where the peak extinction occurs. In addition, global aerosol distributions obtained from the data are consistent with expected aerosol morphology. Although the validation is preliminary, the HALOE aerosol data appear to be of excellent quality and to accurately represent optical characteristics and distribution of the aerosols.
Hervig, Mark E.↗
Spectral signatures of polar stratospheric clouds and sulfate aerosol
Multiwavelength observations of Antarctic and midlatitude aerosol by the Cryogenic Limb Array Etalon Spectrometer (CLAES) experiment on the Upper Atmosphere Research Satellite (UARS) are used to demonstrate a technique that identifies the location of polar stratospheric clouds. The technique discussed uses the normalized area of the triangle formed by the aerosol extinctions at 925, 1257, and 1605/cm (10.8, 8.0, and 6.2 micrometers) to derive a spectral aerosol measure M of the aerosol spectrum. Mie calculations for spherical particles and T-matrix calculations for spheriodal particles are used to generate theoretical spectral extinction curves for sulfate and polar stratospheric cloud particles. The values of the spectral aerosol measure M for the sulfate and polar stratospheric cloud particles are shown to be different. Aerosol extinction data, corresponding to temperatures between 180 and 220 K at a pressure of 46 hPa (near 21-km altitude) for 18 August 1992, are used to demonstrate the technique. Thermodynamic calculations, based upon frost-point calculations and laboratory phase-equilibrium studies of nitric acid trihydrate, are used to predict the location of nitric acid trihydrate cloud particles.
Massie, S. T.↗
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.↗
Revisiting GloSSAC Using Space Based Measurements
We revisit Global Space-based stratospheric aerosol climatology (GloSSAC) and extend the dataset through 2021 in the latest version (version 2.2). Several space-based measurements have been used to construct GloSSAC. For version 2.2, important changes include implementation of a revised aerosol/cloud categorization for The Stratospheric Aerosol and Gas Experiment (SAGE III/ISS). SAGE III/ISS began its mission in June 2017. While SAGEIII/ISS makes reliable and robust solar occultation measurements in stratosphere—similar to its predecessors, interpreting aerosol extinction measurements in the vicinity of tropopause and in the troposphere have been a challenge for all SAGE measurements. Here, we study the challenges associated with the discrimination of aerosols and clouds from the extinction measurements. Here, we describe the methods implemented to categorize Clouds and aerosols using available SAGEIII/ISS aerosol measurements. We use version 5.2 of SAGE III/ISS extinction coefficients for the analysis. The current algorithm now classifies standard (background) and non-standard (enhanced) aerosols in the stratosphere and identify enhanced aerosols and aerosol/cloud mixture in the tropopause region. Extinction coefficient measurements from SAGE series of observations make an important contribution in the GloSSAC data base and therefore, the impact of cloud-filtered aerosol extinction coefficient measurements on the latest version of GloSSAC (version 2.2) is also discussed. Additionally, we discuss minor version changes occurred in other space-based measurements that include Optical Spectrograph and InfraRed Imaging System(OSIRIS) and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation(CALIPSO). We also plan on evaluating and using aerosol extinction profiles from other satellite data sets such as Ozone Mapping Profiler Suite (OMPS) in a future version.
stratospheric aerosol↗
Advancing the quantification of aerosol-cloud interactions with the CALIPSO-CloudSat-Aqua/MODIS record
Aerosol-cloud-precipitation interactions are assessed over the non-polar ocean using more than 11 years of combined Aqua-MODIS, CALIPSO-CALIOP, and CloudSat products. The analysis first shows the benefit of incorporating vertically resolved aerosol extinction coefficient (σext) in aerosol-cloud interactions (ACI) assessments, demonstrating that: σext vertically collocated with the cloud layer () correlates best with cloud droplet number concentration (Nd), column-integrated aerosol optical depth (AOD) cannot explain the Nd variability in the extratropics, and the S-shape of the AOD-Nd relationship reported in previous studies is not replicated when using instead of AOD, with a Nd- linearity more consistent with in-situ studies over the ocean. ACI metric, estimated as the log-scale regression between CALIOP and MODIS Nd reveals that the eastern Pacific is the region with the strongest ACI, followed by the Southern Ocean. The susceptibility of clouds to changes in their liquid water path (LWP) and frequency of precipitation followed a 2-step calculation by combining the Nd- regression (ACI) with the regression between these macrophysical variables and Nd. LWP susceptibility is negative (LWP decreases with aerosol loading) and statistically significant over the eastern Pacific, eastern Atlantic, and extratropics. In contrast, vast areas of the tropical and subtropical ocean feature negligible changes in LWP with aerosol. Precipitation frequency susceptibility is negative, but the values are only significant over the coastal eastern Pacific and Atlantic. The findings suggest that previous modeling assessments relying on AOD may need to be revisited by taking advantage of the synergy between passive and active sensors.
Li, Zhujun↗
An Empirical Characterization of the Aerosol Angstrom Exponent Interpolation Bias using SAGE III/ISS Data
This work uses multispectral measurements of vertically resolved aerosol extinction coefficients from the Stratospheric Aerosol and Gas Experiment (SAGE) III on the International Space Station (ISS) to demonstrate how the use of the Ångström exponent for interpolation of aerosol data between two different wavelengths creates a bias. An empirical relationship is derived between the magnitude of this bias and the Ångström exponent at several different SAGE wavelengths. This relationship can thus be used as a correction factor for other studies, such as multi-instrument intercomparisons or merging, that wish to convert aerosol data from one wavelength to another using the Ångström exponent and is applicable to all stratospheric non-cloud aerosol except highly aged particles that are evaporating at altitudes above the Junge layer.
Aerosol↗
Application of the CALIOP Layer Product to Evaluate the Vertical Distribution of Aerosols Estimated by Global Models: AeroCom Phase I Results
The CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) layer product is used for a multimodel evaluation of the vertical distribution of aerosols. Annual and seasonal aerosol extinction profiles are analyzed over 13 sub-continental regions representative of industrial, dust, and biomass burning pollution, from CALIOP 2007-2009 observations and from AeroCom (Aerosol Comparisons between Observations and Models) 2000 simulations. An extinction mean height diagnostic (Z-alpha) is defined to quantitatively assess the models' performance. It is calculated over the 0-6 km and 0-10 km altitude ranges by weighting the altitude of each 100 m altitude layer by its aerosol extinction coefficient. The mean extinction profiles derived from CALIOP layer products provide consistent regional and seasonal specificities and a low inter-annual variability. While the outputs from most models are significantly correlated with the observed Z-alpha climatologies, some do better than others, and 2 of the 12 models perform particularly well in all seasons. Over industrial and maritime regions, most models show higher Z-alpha than observed by CALIOP, whereas over the African and Chinese dust source regions, Z-alpha is underestimated during Northern Hemisphere Spring and Summer. The positive model bias in Z-alpha is mainly due to an overestimate of the extinction above 6 km. Potential CALIOP and model limitations, and methodological factors that might contribute to the differences are discussed.
Aerosols and particles↗
Respirable particulate monitoring with remote sensors. (Public health ecology: Air pollution)
The feasibility of monitoring atmospheric aerosols in the respirable range from air or space platforms was studied. Secondary reflectance targets were located in the industrial area and near Galveston Bay. Multichannel remote sensor data were utilized to calculate the aerosol extinction coefficient and thus determine the aerosol size distribution. Houston Texas air sampling network high volume data were utilized to generate computer isopleth maps of suspended particulates and to establish the mass loading of the atmosphere. In addition, a five channel nephelometer and a multistage particulate air sampler were used to collect data. The extinction coefficient determined from remote sensor data proved more representative of wide areal phenomena than that calculated from on site measurements. It was also demonstrated that a significant reduction in the standard deviation of the extinction coefficient could be achieved by reducing the bandwidths used in remote sensor.
Severs, R. K.↗
Development and validation of a humidified CAPS-PMSSA with an improved methodology to calculate the truncation correction factor
Absorbing aerosols play an important role in the Earth’s radiation budget, and current uncertainties associated with their radiative impacts remain substantial. An element of this uncertainty derives from insufficient understanding of the extent to which water, as a coating on absorbing particles, enhances the absorption. Here, we describe and characterize the performance of a cavity-attenuated phase shift single scatter albedo spectrometer (CAPS-PMSSA) system that has been modified to enable concurrent aerosol extinction and scattering measurements, from which aerosol absorption is derived, at relative humidities up to ~90%. The modified instrument is referred to as the humidified CAPS (HCAPS). Additionally, we develop and validate an update to a method to calculate the truncation correction factor, used to correct the scattering measurements, that can account for the effects of particle growth and compositional changes resulting from water uptake. The method can be applied to experiments that use either size-selected or polydisperse aerosol samples of either known or unknown composition. Overall, we show that measurements made with the HCAPS, when processed using the updated truncation correction method, enable accurate measurement of the influence of water uptake on light absorption.
Dal Porto, Rachael [University of California, Davi↗
Comparison of satellite-inferred (SAGE II) aerosol optical depths with corresponding airborne sunphotometer optical depths
Solar radiation measurements were made with an airborne multiwavelength autotracking sunphotometer detector off the northeastern coast of Brazil on April 6, 1985. These measurements are used to validate solar radiation measurements from the Stratospheric Aerosol and Gas Experiment (SAGE II). The SAGE II data below 17.5 km are dominated by attenuation due to thunderstorm-generated cirrus clouds. When integrated above 17.5 km, however, the aerosol extinction profiles from SAGE II yield aerosol optical depths that are consistent with the corresponding sunphotometer values above 10.1 km.
Livingston, John M.↗
Shipboard Sunphotometer Measurements of Aerosol Optical Depth Spectra and Columnar Water Vapor During ACE-2 and Comparison with Selected Land, Ship, Aircraft, and Satellite Measurements
Analyses of aerosol optical depth (AOD) and colurnmn water vapor (CWV) measurements acquired with NASA Ames Research Center's 6-channel Airborne Tracking Sunphotometer (AATS-6) operated aboard the R/V Professor Vodyanitskiy during the 2nd Aerosol Characterization Experiment (ACE-2) are discussed. Data are compared with various in situ and remote measurements for selected cases. The focus is on 10 July, when the Pelican airplane flew within 70 km of the ship near the time of a NOAA-14/AVHRR satellite overpass and AOD measurements with the 14-channel Ames Airborne Tracking Sunphotometer (AATS-14) above the marine boundary layer (MBL) permitted calculation of AOD within the MBL from the AATS-6 measurements. A detailed column closure test is performed for MBL AOD on 10 July by comparing the AATS-6 MBL AODs with corresponding values calculated by combining shipboard particle size distribution measurements with models of hygroscopic growth and radiosonde humidity profiles (plus assumptions on the vertical profile of the dry particle size distribution and composition). Large differences (30-80% in the mid-visible) between measured and reconstructed AODs are obtained, in large part because of the high sensitivity of the closure methodology to hygroscopic growth models, which vary considerably and have not been validated over the necessary range of particle size/composition distributions. The wavelength dependence of AATS-6 AODs is compared with the corresponding dependence of aerosol extinction calculated from shipboard measurements of aerosol size distribution and of total scattering mearured by a shipboard integrating nephelometer for several days. Results are highly variable, illustrating further the great difficulty of deriving column values from point measurements. AATS-6 CWV values are shown to agree well with corresponding values derived from radiosonde measurements during 8 soundings on 7 days and also with values calculated from measurements taken on 10 July with the AATS-14 and the University of Washington Passive Humidigraph aboard the Pelican.
Livingston, John M.↗
Shipboard Sunphotometer Measurements of Aerosol Optical Depth Spectra and Columnar Water Vapor During ACE-2, and Comparison with Selected Land, Ship, Aircraft, and Satellite Measurements
Analyses of aerosol optical depth (AOD) and columnar water vapor (CWV) measurements acquired with NASA Ames Research Center's six-channel Airborne Tracking Sunphotometer (AATS-6) operated aboard the R/V (research vehicle) Professor Vodyanitskiy during the second Aerosol Characterization Experiment (ACE-2) are discussed. Data are compared with various in situ and remote measurements for selected cases. The focus is on 10 July, when the Pelican airplane flew within 70 km of the ship near the time of a NOAA (National Oceanographic and Atmospheric Administration)-14/AVHRR (Advanced Very High Resolution Radiometer) satellite overpass and AOD measurements with the 14-channel Ames Airborne Tracking Sunphotometer (AATS-14) above the marine boundary layer (MBL) permitted calculation of AOD within the MBL from the AATS-6 measurements. A detailed column closure test is performed for MBL AOD on 10 July by comparing the AATS-6 MBL AODs with corresponding values calculated by combining shipboard particle size distribution measurements with models of hygroscopic growth and radiosonde humidity profiles (plus assumptions on the vertical profile of the dry particle size distribution and composition). Large differences (30-80% in the mid-visible) between measured and reconstructed AODs are obtained, in large part because of the high sensitivity of the closure methodology to hygroscopic growth models, which vary considerably and have not been validated over the necessary range of particle size/composition distributions. The wavelength dependence of AATS-6 AODs is compared with the corresponding dependence of aerosol extinction calculated from shipboard measurements of aerosol size distribution and of total scattering measured by a shipboard integrating nephelometer for several days. Results are highly variable, illustrating further the great difficulty of deriving column values from point measurements. AATS-6 CWV values are shown to agree well with corresponding values derived from radiosonde measurements during eight soundings on seven days and also with values calculated from measurements taken on 10 July with the AATS-14 and the University of Washington Passive Humidigraph aboard the Pelican.
Livingston, John M.↗
Major Optical Depth Perturbations to the Stratosphere from Volcanic Eruptions: Stellar-Extinction Period, 1961-1978
A revised chronology of stratospheric aerosol extinction due to volcanic eruptions has been assembled for the period 1961-1978, which immediately precedes the era of dedicated satellite measurements. On the whole, the most accurate data consist of published observations of stellar extinction, supplemented in part by other kinds of observational data. The period covered encompasses the important eruptions of Agung (1963) and Fuego (1974), whose dust veils are discussed with respect to their transport, decay, and total mass. The effective (area-weighted mean) radii of the aerosols for both eruptions are found to be 0.3-0.4 microns. It is confirmed that, among known tropical eruptions, Agung's dust was unique for a low-latitude eruption in remaining almost entirely confined to the hemisphere of its production. A new table of homogeneous visual optical depth perturbations, listed by year and by hemisphere, is provided for the whole period 1881-1978, including the pyrheliometric period before 1961 that was investigated previously.
Stothers, Richard B.↗