scholarly journals Detailed characterization of the CAPS single scattering albedo monitor (CAPS PMssa) as a field-deployable instrument for measuring aerosol light absorption with the extinction-minus-scattering method

2020 ◽  
Author(s):  
Rob L. Modini ◽  
Joel C. Corbin ◽  
Benjamin T. Brem ◽  
Martin Irwin ◽  
Michele Bertò ◽  
...  

Abstract. The CAPS PMssa monitor is a recently commercialized instrument designed to measure aerosol single scattering albedo (SSA) with high accuracy (Onasch et al., 2015). The underlying extinction and scattering coefficient measurements made by the instrument also allow calculation of aerosol absorption coefficients via the extinction-minus-scattering (EMS) method. Care must be taken with EMS measurements due to the occurrence of large subtractive error amplification, especially for the predominantly scattering aerosols that are typically found in the ambient atmosphere. Practically this means that although the CAPS PMssa can measure scattering and extinction coefficients with high accuracy (errors on the order of 1–10 %), the corresponding errors in EMS-derived absorption range from ~ 10 % to greater than 100 %. Therefore, we examine the individual error sources in detail with the goal of constraining these as tightly as possible. Our main focus is on the correction of the scattered light truncation effect (i.e., accounting for the near-forward and -backward scattered light that is undetectable by the instrument), which we show to be the main source of underlying error in atmospheric applications. We introduce a new, modular framework for performing the truncation correction calculation that enables the consideration of additional physical processes such as reflection from the instrument’s glass sampling tube, which was neglected in an earlier truncation model. We validate the truncation calculations against comprehensive laboratory measurements. It is demonstrated that the process of glass tube reflection must be considered in the truncation calculation, but that uncertainty still remains regarding the effective length of the optical cavity. Another important source of uncertainty is the cross calibration constant that quantitatively links the scattering coefficient measured by the instrument to its extinction coefficient. We present measurements of this constant over a period of ~ 5 months that demonstrate that the uncertainty in this parameter is very well constrained for some instrument units (2–3 %), but higher for others. We then use two example field datasets to demonstrate and summarize the potential and the limitations of using the CAPS PMssa for measuring absorption. The first example uses mobile measurements on a highway road to highlight the excellent responsiveness and sensitivity of the instrument, which enables much higher time resolution measurements of relative absorption than is possible with filter-based instruments. The second example from a stationary field site (Cabauw, the Netherlands) demonstrates how truncation-related uncertainties can lead to large biases in EMS-derived absolute absorption coefficients. Nevertheless, we use a subset of fine-mode dominated aerosols from the dataset to show that under certain conditions and despite the remaining truncation uncertainties, the CAPS PMssa can still provide consistent EMS-derived absorption measurements, even for atmospheric aerosols with high SSA. Finally, we present a detailed list of recommendations for future studies that use the CAPS PMssa to measure absorption with the EMS method. These recommendations could also be followed to obtain accurate measurements (i.e., errors less than 5–10 %) of SSA, and scattering and extinction coefficients with the instrument.

2021 ◽  
Vol 14 (2) ◽  
pp. 819-851
Author(s):  
Rob L. Modini ◽  
Joel C. Corbin ◽  
Benjamin T. Brem ◽  
Martin Irwin ◽  
Michele Bertò ◽  
...  

Abstract. The CAPS PMssa monitor is a recently commercialized instrument designed to measure aerosol single-scattering albedo (SSA) with high accuracy (Onasch et al., 2015). The underlying extinction and scattering coefficient measurements made by the instrument also allow calculation of aerosol absorption coefficients via the extinction-minus-scattering (EMS) method. Care must be taken with EMS measurements due to the occurrence of large subtractive error amplification, especially for the predominantly scattering aerosols that are typically found in the ambient atmosphere. Practically this means that although the CAPS PMssa can measure scattering and extinction coefficients with high accuracy (errors on the order of 1 %–10 %), the corresponding errors in EMS-derived absorption range from ∼10 % to greater than 100 %. Therefore, we examine the individual error sources in detail with the goal of constraining these as tightly as possible. Our main focus is on the correction of the scattered light truncation effect (i.e., accounting for the near-forward and near-backward scattered light that is undetectable by the instrument), which we show to be the main source of underlying error in atmospheric applications. We introduce a new, modular framework for performing the truncation correction calculation that enables the consideration of additional physical processes such as reflection from the instrument's glass sampling tube, which was neglected in an earlier truncation model. We validate the truncation calculations against comprehensive laboratory measurements. It is demonstrated that the process of glass tube reflection must be considered in the truncation calculation, but that uncertainty still remains regarding the effective length of the optical cavity. Another important source of uncertainty is the cross-calibration constant that quantitatively links the scattering coefficient measured by the instrument to its extinction coefficient. We present measurements of this constant over a period of ∼5 months that demonstrate that the uncertainty in this parameter is very well constrained for some instrument units (2 %–3 %) but higher for others. We then use two example field datasets to demonstrate and summarize the potential and the limitations of using the CAPS PMssa for measuring absorption. The first example uses mobile measurements on a highway road to highlight the excellent responsiveness and sensitivity of the instrument, which enables much higher time resolution measurements of relative absorption than is possible with filter-based instruments. The second example from a stationary field site (Cabauw, the Netherlands) demonstrates how truncation-related uncertainties can lead to large biases in EMS-derived absolute absorption coefficients. Nevertheless, we use a subset of fine-mode-dominated aerosols from the dataset to show that under certain conditions and despite the remaining truncation uncertainties, the CAPS PMssa can still provide consistent EMS-derived absorption measurements, even for atmospheric aerosols with high SSA. Finally, we present a detailed list of recommendations for future studies that use the CAPS PMssa to measure absorption with the EMS method. These recommendations could also be followed to obtain accurate measurements (i.e., errors less than 5 %–10 %) of SSA and scattering and extinction coefficients with the instrument.


2012 ◽  
Vol 12 (12) ◽  
pp. 5647-5659 ◽  
Author(s):  
A. Leskinen ◽  
A. Arola ◽  
M. Komppula ◽  
H. Portin ◽  
P. Tiitta ◽  
...  

Abstract. We introduce a four-year (in 2006–2010) continuous data set of aerosol optical properties at Puijo in Kuopio, Finland. We study the annual and diurnal variation of the aerosol scattering and absorption coefficients, hemispheric backscattering fraction, scattering Ångström exponent, and single scattering albedo, whose median values over this period were 7.2 Mm−1 (at 550 nm), 1.0 Mm−1 (at 637 nm), 0.15, 1.93 (between 450 and 550 nm), and 0.85, respectively. The scattering coefficient peaked in the spring and autumn, being 2–4 times those in the summer and winter. An exception was the summer of 2010, when the scattering coefficient was elevated to ~300 Mm−1 by plumes from forest fires in Russia. The absorption coefficient peaked in the winter when soot-containing particles derived from biomass burning were present. The higher relative absorption coefficients resulted in lower single scattering albedo in winter. The optical properties varied also with wind direction and time of the day, indicating the effect of the local pollutant sources and the age of the particles. Peak values in the single scattering albedo were observed when the wind blew from a paper mill and from the sector without local pollutant sources. These observations were linked, respectively, to the sulphate-rich aerosol from the paper mill and the oxygenated organics in the aged aerosol, which both are known to increase the scattering characteristics of aerosols. Decreases in the single scattering albedo in the morning and afternoon, distinct in the summertime, were linked to the increased traffic density at these hours. The scattering and absorption coefficients of residential and long-range transported aerosol (two separate cloud events) were found to be decreased by clouds. The effect was stronger for the scattering than absorption, indicating preferential activation of the more hygroscopic aerosol with higher scattering characteristics.


2012 ◽  
Vol 12 (2) ◽  
pp. 4719-4754
Author(s):  
A. Leskinen ◽  
A. Arola ◽  
M. Komppula ◽  
H. Portin ◽  
P. Tiitta ◽  
...  

Abstract. We introduce a four-year (2006–2010) continuous data set of aerosol optical properties at Puijo in Kuopio, Finland. We study the annual and diurnal variation of the aerosol scattering and absorption coefficients, hemispheric backscattering fraction, scattering Ångström exponent, and single scattering albedo, whose averages over this period were 11.1 Mm−1 (at 550 nm), 1.5 Mm−1 (at 670 nm), 0.13, 1.9, and 0.83, respectively. The scattering coefficient peaked in the spring and autumn, being 2–4 times those in the summer and winter. An exception was the summer of 2010, when the the scattering coefficient was elevated to ~300 Mm−1 by the plumes from forest fires in Russia. The absorption coefficient peaked in the winter with values of 2–3 times those in the summer. The single scattering albedo was lowest in the winter when more biomass burning derived, soot-containing aerosols were present. The optical properties varied also with wind direction and time of the day, indicating the effect of the local pollutant sources and the age of the particles. Peak values in the single scattering albedo were observed when the wind blew from a paper mill and from the sector without local pollutant sources. These observations were linked to the sulphate-rich aerosol from the paper mill and the oxygenated organics in the aged aerosol, which both are known to increase the scattering characteristics of aerosols. Changes in the single scattering albedo in the morning and afternoon in the summertime were linked to the increased traffic density at these hours. The scattering and absorption coefficients were found to be decreased by clouds. The effect was stronger for the scattering than absorption, indicating preferential activation of the more hygroscopic aerosol with higher scattering characteristics. What happens to the aerosol optical properties during a cloud event when the air masses come from different directions with different local sources, is under a more detailed inspection. Also, more aerosol mass spectrometry data will be analyzed in order to strengthen our knowledge about the role of the chemical composition of the aerosol particles in their activation into cloud droplets.


2015 ◽  
Vol 15 (22) ◽  
pp. 33675-33730
Author(s):  
X. Xu ◽  
W. Zhao ◽  
Q. Zhang ◽  
S. Wang ◽  
B. Fang ◽  
...  

Abstract. The optical properties and chemical composition of PM1.0 (particulate with an aerodynamic diameter of less than 1.0 μm) particles in a suburban environment (Huairou) near the mega-city Beijing were measured during the HOPE-J3A (Haze Observation Project Especially for Jing-Jin-Ji Area) field campaign. The campaign covered the period November 2014 to January 2015 during the winter coal heating season. The average and standard deviations for the extinction, scattering, absorption coefficients, and the aerosol single scattering albedo (SSA) at λ = 470 nm during the measurement period were 201 ± 240, 164 ± 202, 37 ± 43 Mm-1, and 0.80 ± 0.08, respectively. The mean mass scattering (MSE) and absorption (MAE) efficiencies were 4.77 ± 0.01 and 0.87 ± 0.03 m2g-1, respectively. Highly time-resolved air pollution episodes clearly show the dramatic evolution of the PM1.0 size distribution, extensive optical properties (extinction, scattering, and absorption coefficients) and intensive optical properties (single scattering albedo and complex refractive index) during haze formation, development and decline. Time periods were classified into three different pollution levels (clear, slightly polluted, and polluted) for further analysis. It was found that: (1) The diurnal patterns of the aerosol extinction, scattering, absorption coefficients, and SSA differed for the three pollution classes. (2) The real and imaginary part of complex refractive index (CRI) increased, while the SSA decreased from clear to polluted days. (3) The relative contributions of organic and inorganic species to observed aerosol composition changed significantly from clear to polluted days: the organic mass fraction decreased (50 to 43 %) while the proportion of sulfates, nitrates, and ammonium increased strongly (34 to 44 %). (4) The fractional contribution of chemical components to extinction coefficients was calculated by using the modified IMPROVE algorithm. Organic mass was the largest contributor (58 %) to the total extinction of PM1.0. When the air quality deteriorated, the change of the relative contribution of sulfate aerosol to the total extinction was small, but the contribution of nitrate aerosol increased significantly (from 17 % on clear days to 23 % on polluted days). (5) The observed mass scattering efficiencies increased consistently with the pollution extent, however, the observed mass absorption efficiencies increased consistently with increasing mass concentration in slightly pollution conditions, but decreased under polluted conditions.


2019 ◽  
Author(s):  
Julia Perim de Faria ◽  
Ulrich Bundke ◽  
Andrew Freedman ◽  
Timothy B. Onasch ◽  
Andreas Petzold

Abstract. An evaluation of the performance and accuracy of a Cavity Attenuated Phase-Shift Single Scattering Albedo Monitor (CAPS PMssa, Aerodyne Res. Inc.) was conducted in an optical closure study with proven technologies: Cavity Attenuated Phase-Shift Particle Extinction Monitor (CAPS PMex, Aerodyne Res. Inc.); 3-wavelengh Integrating Nephelometer (TSI Model 3563); and 3-wavelength filter-based Particle Soot Absorption Photometer (PSAP, Radiance Research). The evaluation was conducted by connecting the instruments to a controlled aerosol generation system and comparing the measured scattering, extinction, and absorption coefficients measured by the CAPS PMssa with the independent measurements. Three different particle types were used to generate aerosol samples with single-scattering albedos (SSA) ranging from 0.4 to 1.0 at 630 nm wavelength. The CAPS PMssa measurements compared well with the proven technologies. Extinction measurement comparisons exhibited a slope of the linear regression line for the full data set of 0.96 (−0.02/&amp;plus;0.06), an intercept near zero, and a regression coefficient R2 > 0.99; whereas, scattering measurements had a slope of 1.01 (−0.07/&amp;plus;0.06), an intercept of less than &amp;plus;/−2 × 10−6 m−1 (Mm−1), and a coefficient R2 ∼ 1.0. The derived CAPS PMssa absorption compared well to the PSAP measurements at low levels (< 70 Mm−1) for the small particle sizes and modest (0.4 to 0.6) SSA values tested, with a linear regression slope of 1.0, an intercept of −4 Mm−1, and a coefficient R2 = 0.97. Comparisons at higher particle loadings were compromised by loading effects on the PSAP filters. For the SSA measurements, agreement was highest (regression slopes within 1% ) for SSA = 1.0 particles, though the difference between the measured values increased to 9 % for extinction coefficients lower than 55 Mm−1. SSA measurements for absorbing particles exhibited absolute differences up to 18 %, though it is not clear which measurement had the lowest accuracy. For a given particle type, the CAPS PMssa instrument exhibited the lowest scatter around the average. This study demonstrates that the CAPS PMssa is a robust and reliable instrument for the direct measurement of the scattering and extinction coefficients and thus SSA. This conclusion also holds as well for the indirect measurement of the absorption coefficient with the constraint that the accuracy of this particular measurement degrades as the SSA and particle size increases.


2020 ◽  
Author(s):  
Alessandro Bigi ◽  
Martine Collaud Coen ◽  
Elisabeth J. Andrews ◽  
Clémence Rose ◽  
Cathrine Lund Myhre ◽  
...  

&lt;p&gt;Atmospheric aerosols are known to play a key role in Earth&amp;#8217;s radiative budget, although the quantification of their climate forcing is still highly uncertain. In order to improve the scientific understanding of their climatic effect, in-situ ground-based aerosol properties observations are needed by the research community. Such data would also allow the global assessment of the effect of environmental policies over both the short and the long term.&lt;/p&gt;&lt;p&gt;To develop a robust and consistent view over time of the worldwide variability of aerosol properties, data resulting from a fully-characterized value chain, including uncertainty estimation, is needed.&lt;/p&gt;&lt;p&gt;The present work is part of a wider project, having among its goals the investigation of the variability of climate-relevant aerosol properties observed at all sites connected to the Global Atmospheric Watch network, whose data are publicly available from the World Data Centre for Aerosols and follow the aforementioned specifications.&lt;/p&gt;&lt;p&gt;This work focuses on aerosol optical proprieties, i.e. the aerosol light scattering coefficient (&amp;#963;&lt;sub&gt;sp&lt;/sub&gt;), the aerosol light absorption coefficient (&amp;#963;&lt;sub&gt;ap&lt;/sub&gt;), single scattering albedo (&amp;#969;&lt;sub&gt;o&lt;/sub&gt;) and both scattering and absorption &amp;#197;ngstr&amp;#246;m exponents (&amp;#229;&lt;sub&gt;sp&lt;/sub&gt; and &amp;#229;&lt;sub&gt;ap&lt;/sub&gt;).&lt;/p&gt;&lt;p&gt;The analysis includes 108 yearly datasets collected either during 2016 or 2017 at different sites: 53 for absorption and 55 for scattering coefficient datasets, respectively. For 29 of these sites it was also possible to compute single scattering albedo.&lt;/p&gt;&lt;p&gt;The spatial variability in extensive and intensive optical properties was analysed in terms of each site&amp;#8217;s geographical location (either polar, continental, coastal or mountain) and its footprint (from pristine to urban, representing increasing levels of anthropogenic influence).&lt;/p&gt;&lt;p&gt;The results highlight the impact of anthropogenic emissions and biomass burning on absolute levels and annual variability. The effect of sea spray or long range transport of dust is also evident for several sites, along with the influence of regional emissions. The largest seasonality in aerosol loading was observed at mountain sites under mixed footprint conditions, while the lowest seasonality occurred at urban sites. Urban sites also exhibited the highest &amp;#963;sp and &amp;#963;ap values. The lowest levels in &amp;#963;&lt;sub&gt;sp&lt;/sub&gt; and &amp;#963;&lt;sub&gt;ap&lt;/sub&gt; were observed at some polar sites, along with few coastal and mountain sites, despite their typically mixed footprint.&lt;/p&gt;&lt;p&gt;&lt;strong&gt;Acknowledgements&lt;/strong&gt;&lt;/p&gt;&lt;p&gt;The authors acknowledge WMO-GAW World Data Centre on Aerosol for providing data available at http://ebas.nilu.no&lt;/p&gt;


2014 ◽  
Vol 7 (3) ◽  
pp. 2981-3019
Author(s):  
W. Zhao ◽  
X. Xu ◽  
M. Dong ◽  
W. Chen ◽  
X. Gu ◽  
...  

Abstract. We report on the development of a cavity enhanced aerosol single scattering albedometer incorporating incoherent broad-band cavity-enhanced spectroscopy (IBBCEAS) approach and an integrating sphere (IS) for simultaneous in situ measurements of aerosol scattering and extinction coefficients in the exact same sample volume. The cavity enhanced albedometer employed a blue light-emitting diode (LED) based IBBCEAS approach for the measurement of wavelength-resolved aerosol optical extinction over the spectral range of 445–480 nm. An integrating sphere nephelometer coupled to the IBBCEAS setup was used for the measurement of aerosol scattering. The scattering signal was measured with a single channel photomultiplier tube (PMT), providing an integrated value over a narrow bandwidth (FWHM ~ 9 nm) in the spectral region of 465–474 nm. A scattering coefficient at a wavelength of 470 nm was deduced as an averaged scattering value and used for data analysis and instrumental performance comparison. Performance evaluation of the albedometer was carried out using laboratory-generated particles and ambient aerosol. The scattering and extinction measurements of monodisperse polystyrene latex (PSL) spheres generated in laboratory proved excellent correlation between two channels of the albedometer. The retrieved refractive index (RI) from the measured scattering and extinction efficiencies agreed well with the values reported in previously published papers. Aerosol light scattering and extinction coefficients, single scattering albedo (SSA) and NO2 concentrations in an ambient sample were directly and simultaneously measured using the developed albedometer. The developed instrument was validated via an intercomparison of the measured aerosol scattering coefficient and NO2 trace concentration against a TSI 3563 integrating nephelometer and a chemiluminescence detector, respectively.


2018 ◽  
Author(s):  
Krista Luoma ◽  
Aki Virkkula ◽  
Pasi Aalto ◽  
Tuukka Petäjä ◽  
Markku Kulmala

Abstract. The aerosol optical properties (AOPs) of particles smaller than 10 μm (PM10) and 1 μm (PM1) have been measured at SMEAR II since 2006 and 2010, respectively. For the PM10 particles the mean values of the scattering and absorption coefficients, single-scattering albedo, and backscatter fraction at δ = 550 nm, and scattering and absorption Ångström exponents at the wavelength ranges 450–700 nm and 370–950 nm were 15.2 Mm−1, 2.1 Mm−1, 0.86, 0.15, 1.80 and 0.94 respectively. The time series were used to examine the trends and variation in the AOPs. Statistically significant trends were found for example for the PM10 scattering and absorption coefficients, single-scattering albedo, and backscatter fraction, and the slopes of these trends were −0.342 Mm−1, −0.0952 Mm−1, 3.4 ‧ 10−3, and 1.3 ‧ 10−3 per year. The tendency for the extensive AOPs to decrease correlated well with the decrease in aerosol number and volume concentration. The tendency for the singlescattering albedo and backscattering fraction to increase affected to the effective aerosol forcing efficiency, indicating that the dry aerosols were scattering the radiation more effectively back into space. In addition to these trends, we also observed seasonal and diurnal variations and variations between the AOPs of the PM1 and PM10 particles.


2019 ◽  
Vol 19 (17) ◽  
pp. 11363-11382 ◽  
Author(s):  
Krista Luoma ◽  
Aki Virkkula ◽  
Pasi Aalto ◽  
Tuukka Petäjä ◽  
Markku Kulmala

Abstract. Aerosol optical properties (AOPs) describe the ability of aerosols to scatter and absorb radiation at different wavelengths. Since aerosol particles interact with the sun's radiation, they impact the climate. Our study focuses on the long-term trends and seasonal variations of different AOPs measured at a rural boreal forest site in northern Europe. To explain the observed variations in the AOPs, we also analyzed changes in the aerosol size distribution. AOPs of particles smaller than 10 µm (PM10) and 1 µm (PM1) have been measured at SMEAR II, in southern Finland, since 2006 and 2010, respectively. For PM10 particles, the median values of the scattering and absorption coefficients, single-scattering albedo, and backscatter fraction at λ=550 nm were 9.8 Mm−1, 1.3 Mm−1, 0.88, and 0.14. The median values of scattering and absorption Ångström exponents at the wavelength ranges 450–700 and 370–950 nm were 1.88 and 0.99, respectively. We found statistically significant trends for the PM10 scattering and absorption coefficients, single-scattering albedo, and backscatter fraction, and the slopes of these trends were −0.32 Mm−1, −0.086 Mm−1, 2.2×10-3, and 1.3×10-3 per year. The tendency for the extensive AOPs to decrease correlated well with the decrease in aerosol number and volume concentrations. The tendency for the backscattering fraction and single-scattering albedo to increase indicates that the aerosol size distribution consists of fewer larger particles and that aerosols absorb less light than at the beginning of the measurements. The trends of the single-scattering albedo and backscattering fraction influenced the aerosol radiative forcing efficiency, indicating that the aerosol particles are scattering the radiation more effectively back into space.


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