scholarly journals Simultaneous measurement of the relative humidity dependent aerosol light extinction, scattering, absorption and single-scattering albedo with a humidified cavity-enhanced albedometer

Author(s):  
Jiacheng Zhou ◽  
Xuezhe Xu ◽  
Weixiong Zhao ◽  
Bo Fang ◽  
Qianqian Liu ◽  
...  

Abstract. Hygroscopic aerosols take up water and grow with increasing relative humidity (RH), giving rise to large changes in light extinction (bext), scattering (bscat), absorption (babs), and single scattering albedo (SSA, ω). The optical hygroscopic growth factors for each parameter (f(RH)ext,scat,abs,ω) are thus important for assessing aerosol effects on regional air quality, atmospheric visibility, and radiative forcing. The RH dependence of aerosol scattering and extinction has been studied in many laboratory and field studies. However, owing partly to the absence of suitable instrumentation, there are few reports of the RH dependence of aerosol absorption and ω. In this work, we report the development of a humidified cavity-enhanced albedometer (H-CEA) for simultaneous measurements of f(RH)ext,scat,abs,ω at λ = 532 nm from 10 % to 90 % RH. The instrument’s performance was evaluated with laboratory-generated ammonium sulphate, sodium chloride and nigrosin aerosols. Measured hygroscopic growth factors for different parameters were in good agreement with model calculations and literature reported values, demonstrating the accuracy of the H-CEA for measuring RH-dependent optical properties.

2020 ◽  
Vol 13 (5) ◽  
pp. 2623-2634
Author(s):  
Jiacheng Zhou ◽  
Xuezhe Xu ◽  
Weixiong Zhao ◽  
Bo Fang ◽  
Qianqian Liu ◽  
...  

Abstract. Hygroscopic aerosols take up water and grow with increasing relative humidity (RH), giving rise to large changes in light extinction (bext), scattering (bscat), absorption (babs), and single scattering albedo (SSA, ω). The optical hygroscopic growth factors for each parameter (f(RH)ext,scat,abs,ω) are thus important for assessing aerosol effects on regional air quality, atmospheric visibility, and radiative forcing. The RH dependence of aerosol scattering and extinction has been studied in many laboratory and field studies. However, owing partly to the absence of suitable instrumentation, there are few reports of the RH dependence of aerosol absorption and ω. In this work, we report the development of a humidified cavity-enhanced albedometer (H-CEA) for simultaneous measurements of f(RH)ext,scat,abs,ω at λ=532 nm from 10 % to 88 % RH. The instrument's performance was evaluated with laboratory-generated ammonium sulfate, sodium chloride, and nigrosin aerosols. Measured hygroscopic growth factors for different parameters were in good agreement with model calculations and literature-reported values, demonstrating the accuracy of the H-CEA for measuring RH-dependent optical properties.


2014 ◽  
Vol 14 (7) ◽  
pp. 9041-9065
Author(s):  
J. P. Putaud ◽  
F. Cavalli ◽  
S. Martins dos Santos ◽  
A. Dell'Acqua

Abstract. Aerosols properties have been monitored by ground-based in situ and remote sensing measurements at the station for atmospheric research located in Ispra on the edge of the Po Valley for almost one decade. In-situ measurements are performed according to Global Atmosphere Watch recommendations, and quality is assured through the participation in regular inter-laboratory comparisons. Sunphotometer data are produced by AERONET. Data show significant decreasing trends over 2004–2010 for a number of variables including particulate matter (PM) mass concentration, aerosol scattering, backscattering and absorption coefficients, and aerosol optical thickness (AOT). In-situ measurement data show no significant trend in the aerosol backscatter ratio, but a significant decreasing trend of about −0.7 ± 0.3% in the aerosol single scattering albedo in the visible light range. Similar trends are observed in the aerosol single scattering albedo retrieved from sunphotometer measurements. Correlations appear between in situ PM mass concentration and aerosol scattering coefficient on the one hand, and elemental carbon (EC) and aerosol absorption coefficient on the other hand, however, no increase in the EC / PM ratio was observed, which could have explained the decrease in SSA. The application of a simple approximation to calculate the direct radiative forcing by aerosols suggests a significant diminution in their cooling effect, mainly due to the decrease in AOT. Applying the methodology we present to those sites where the necessary suite of measurements is available would provide important information to inform future policies for air quality enhancement and fast climate change mitigation.


2012 ◽  
Vol 12 (23) ◽  
pp. 11695-11721 ◽  
Author(s):  
P. J. Sheridan ◽  
E. Andrews ◽  
J. A. Ogren ◽  
J. L. Tackett ◽  
D. M. Winker

Abstract. Between June 2006 and September 2009, an instrumented light aircraft measured over 400 vertical profiles of aerosol and trace gas properties over eastern and central Illinois. The primary objectives of this program were to (1) measure the in situ aerosol properties and determine their vertical and temporal variability and (2) relate these aircraft measurements to concurrent surface and satellite measurements. The primary profile location was within 15 km of the NOAA/ESRL surface aerosol monitoring station near Bondville, Illinois. Identical instruments at the surface and on the aircraft ensured that the data from both platforms would be directly comparable and permitted a determination of how representative surface aerosol properties were of the lower column. Aircraft profiles were also conducted occasionally at two other nearby locations to increase the frequency of A-Train satellite underflights for the purpose of comparing in situ and satellite-retrieved aerosol data. Measurements of aerosol properties conducted at low relative humidity over the Bondville site compare well with the analogous surface aerosol data and do not indicate any major sampling issues or that the aerosol is radically different at the surface compared with the lowest flyby altitude of ~ 240 m above ground level. Statistical analyses of the in situ vertical profile data indicate that aerosol light scattering and absorption (related to aerosol amount) decreases substantially with increasing altitude. Parameters related to the nature of the aerosol (e.g., single-scattering albedo, Ångström exponent, etc.), however, are relatively constant throughout the mixed layer, and do not vary as much as the aerosol amount throughout the profile. While individual profiles often showed more variability, the median in situ single-scattering albedo was 0.93–0.95 for all sampled altitudes. Several parameters (e.g., submicrometer scattering fraction, hemispheric backscattering fraction, and scattering Ångström exponent) suggest that the fraction of smaller particles in the aerosol is larger near the surface than at high altitudes. The observed dependence of scattering on size, wavelength, angular integration range, and relative humidity, together with the spectral dependence of absorption, show that the aerosol at higher altitudes is larger, less hygroscopic, and more strongly absorbing at shorter wavelengths, suggesting an increased contribution from dust or organic aerosols. The aerosol profiles show significant differences among seasons. The largest amounts of aerosol (as determined by median light extinction profile measurements) throughout most of the sampled column were observed during summer, with the lowest amounts in the winter and intermediate values in the spring and fall. The highest three profile levels (3.1, 3.7, 4.6 km), however, showed larger median extinction values in the spring, which could reflect long-range transport of dust or smoke aerosols. The aerosols in the mixed layer were darkest (i.e., lowest single-scattering albedo) in the fall, in agreement with surface measurements at Bondville and other continental sites in the US. In situ profiles of aerosol radiative forcing efficiency showed little seasonal or vertical variability. Underflights of the CALIPSO satellite show reasonable agreement in a majority of retrieved profiles between aircraft-measured extinction at 532 nm (adjusted to ambient relative humidity) and CALIPSO-retrieved extinction, and suggest that routine aircraft profiling programs can be used to better understand and validate satellite retrieval algorithms. CALIPSO tended to overestimate the aerosol extinction at this location in some boundary layer flight segments when scattered or broken clouds were present, which could be related to problems with CALIPSO cloud screening methods. The in situ aircraft-collected aerosol data suggest extinction thresholds for the likelihood of aerosol layers being detected by the CALIOP lidar. In this study, aerosol layers with light extinction (532 nm) values > 50 Mm−1 were detected by CALIPSO ~ 95% of the time, while aerosol layers with extinction values lower than 10 Mm−1 had a detection efficiency of < 2%. For all collocated comparison cases, a 50% probability of detection falls at an in situ extinction level of 20–25 Mm−1. These statistical data offer guidance as to the likelihood of CALIPSO's ability to retrieve aerosol extinction at various locations around the globe.


2017 ◽  
Author(s):  
Duseong S. Jo ◽  
Rokjin J. Park ◽  
Jaein I. Jeong ◽  
Gabriele Curci ◽  
Hyung-Min Lee ◽  
...  

Abstract. Single Scattering Albedo (SSA), the ratio of scattering efficiency to total extinction efficiency, is an essential parameter used to estimate the Direct Radiative Forcing (DRF) of aerosols. However, SSA is one of the large contributors to the uncertainty of DRF estimations. In this study, we examined the sensitivity of SSA calculations to the physical properties of absorbing aerosols, in particular, Black Carbon (BC), Brown Carbon (BrC), and dust. We used GEOS-Chem 3-D global chemical transport model (CTM) simulations and a post-processing tool for the aerosol optical properties (FlexAOD). The model and input parameters were evaluated by comparison against the observed aerosol mass concentrations and the Aerosol Optical Depth (AOD) values obtained from global surface observation networks such as the global Aerosol Mass Spectrometer (AMS) dataset, the Surface Particulate Matter Network (SPARTAN), and the Aerosol Robotic Network (AERONET). The model was generally successful in reproducing the observed variability of both the Particulate Matter 2.5 μm (PM2.5) and AOD (R ~ 0.76) values, although it underestimated the magnitudes by approximately 20 %. Our sensitivity tests of the SSA calculation revealed that the aerosol physical parameters, which have generally received less attention than the aerosol mass loadings, can cause large uncertainties in the resulting DRF estimation. For example, large variations in the calculated BC absorption may result from slight changes of the geometric mean radius, geometric standard deviation, real and imaginary refractive indices, and density. The inclusion of BrC and observationally-constrained dust size distributions also significantly affected the SSA, and resulted in a remarkable improvement for the simulated SSA at 440 nm (bias was reduced by 44–49 %) compared with the AERONET observations. Based on the simulations performed during this study, we found that the global aerosol direct radiative effect was increased by 10 % after the SSA bias was reduced.


2021 ◽  
Author(s):  
Archana Devi ◽  
Sreedharan Krishnakumari Satheesh

Abstract. Single Scattering Albedo (SSA) is a leading contributor to the uncertainty in aerosol radiative impact assessments. Therefore accurate information on aerosol absorption is required on a global scale. In this study, we have applied a multi-satellite algorithm to retrieve SSA using the concept of ‘critical optical depth.’ Global maps of SSA were generated following this approach using spatially and temporally collocated data from Clouds and the Earth’s Radiant Energy System (CERES) and Moderate Resolution Imaging Spectroradiometer (MODIS) sensors on board Terra and Aqua satellites. The method has been validated using the data from aircraft-based measurements of various field campaigns. The retrieval uncertainty is ±0.03 and depends on both the surface albedo and aerosol absorption. Global mean SSA estimated over land and ocean is 0.93 and 0.97, respectively. Seasonal and spatial distribution of SSA over various regions are also presented. The global maps of SSA, thus derived with improved accuracy, provide important input to climate models for assessing the climatic impact of aerosols on regional and global scales.


2019 ◽  
Author(s):  
Mohanan R. Manoj ◽  
Sreedharan K. Satheesh ◽  
Krishnaswamy K. Moorthy ◽  
Hugh Coe

Abstract. Vertical structures of aerosol single scattering albedo (SSA), from near the surface through the free troposphere, have been estimated for the first time at distinct geographical locations over the Indian mainland and adjoining oceans, using in-situ measurements of aerosol scattering and absorption coefficients aboard the FAAM BAe-146 aircraft during the South West Asian Aerosol Monsoon Interactions (SWAAMI) campaign from June to July 2016. These are used to examine the spatial variation of SSA profiles and also to characterize its transformation from just prior to the onset of Indian Summer Monsoon (June 2016) to its active phase (July 2016). Very strong aerosol absorption, with SSA values as low as 0.7, persisted in the lower altitudes (


2020 ◽  
Vol 20 (6) ◽  
pp. 4031-4046
Author(s):  
Mohanan R. Manoj ◽  
Sreedharan K. Satheesh ◽  
Krishnaswamy K. Moorthy ◽  
Hugh Coe

Abstract. Vertical structures of aerosol single scattering albedo (SSA), from near the surface through the free troposphere, have been estimated for the first time at distinct geographical locations over the Indian mainland and adjoining oceans, using in situ measurements of aerosol scattering and absorption coefficients aboard the Facility for Airborne Atmospheric Measurements (FAAM) BAe-146 aircraft during the South West Asian Aerosol Monsoon Interactions (SWAAMI) campaign from June to July 2016. These are used to examine the spatial variation of SSA profiles and also to characterize its transformation from just prior to the onset of Indian Summer Monsoon (June 2016) to its active phase (July 2016). Very strong aerosol absorption, with SSA values as low as 0.7, persisted in the lower altitudes (<3 km) over the Indo-Gangetic Plains (IGP), prior to the monsoon onset, with a west-to-east gradient; lower values occurred in the north-western arid regions, peaking in the central IGP and somewhat decreasing towards the eastern end. During the active phase of the monsoon, the SSA is found to increase remarkably, indicating far less absorption. Nevertheless, significant aerosol absorption persisted in the lower and middle troposphere over the IGP. Inputting these SSA and extinction profiles into a radiative transfer model, we examined the effects of using height-resolved information in estimating atmospheric heating rates due to aerosols, over similar estimates made using a single columnar value. It was noted that use of a single SSA value leads to an underestimation (overestimation) of the heating rates over regions with low (high) SSA, emphasizing the importance of height-resolved information. Further, the use of realistic profiles showed significant heating of the atmosphere by submicron aerosol absorption at the middle troposphere, which may have strong implications for clouds and climate.


2010 ◽  
Vol 23 (19) ◽  
pp. 5288-5293 ◽  
Author(s):  
Norman G. Loeb ◽  
Wenying Su

Abstract To provide a lower bound for the uncertainty in measurement-based clear- and all-sky direct aerosol radiative forcing (DARF), a radiative perturbation analysis is performed for the ideal case in which the perturbations in global mean aerosol properties are given by published values of systematic uncertainty in Aerosol Robotic Network (AERONET) aerosol measurements. DARF calculations for base-state climatological cloud and aerosol properties over ocean and land are performed, and then repeated after perturbing individual aerosol optical properties (aerosol optical depth, single-scattering albedo, asymmetry parameter, scale height, and anthropogenic fraction) from their base values, keeping all other parameters fixed. The total DARF uncertainty from all aerosol parameters combined is 0.5–1.0 W m−2, a factor of 2–4 greater than the value cited in the Intergovernmental Panel on Climate Change’s (IPCC’s) Fourth Assessment Report. Most of the total DARF uncertainty in this analysis is associated with single-scattering albedo uncertainty. Owing to the greater sensitivity to single-scattering albedo in cloudy columns, DARF uncertainty in all-sky conditions is greater than in clear-sky conditions, even though the global mean clear-sky DARF is more than twice as large as the all-sky DARF.


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