We describe a method of using the Aerosol Robotic Network (AERONET) size distributions and complex refractive indices to retrieve the relative proportion of carbonaceous aerosols and free iron ...minerals (hematite and goethite). We assume that soot carbon has a spectrally flat refractive index and enhanced imaginary indices at the 440 nm wavelength are caused by brown carbon or hematite. Carbonaceous aerosols can be separated from dust in imaginary refractive index space because 95 % of biomass burning aerosols have imaginary indices greater than 0.0042 at the 675–1020 nm wavelengths, and 95 % of dust has imaginary refractive indices of less than 0.0042 at those wavelengths. However, mixtures of these two types of particles can not be unambiguously partitioned on the basis of optical properties alone, so we also separate these particles by size. Regional and seasonal results are consistent with expectations. Monthly climatologies of fine mode soot carbon are less than 1.0 % by volume for West Africa and the Middle East, but the southern African and South American biomass burning sites have peak values of 3.0 and 1.7 %. Monthly averaged fine mode brown carbon volume fractions have a peak value of 5.8 % for West Africa, 2.1 % for the Middle East, 3.7 % for southern Africa, and 5.7 % for South America. Monthly climatologies of free iron volume fractions show little seasonal variability, and range from about 1.1 to 1.7 % for coarse mode aerosols in all four study regions. Finally, our sensitivity study indicates that the soot carbon retrieval is not sensitive to the component refractive indices or densities assumed for carbonaceous and free iron aerosols, and the retrieval differs by only 15.4 % when these parameters are altered from our chosen baseline values. The total uncertainty of retrieving soot carbon mass is ∼ 50 % (when uncertainty in the AERONET product and mixing state is included in the analysis).
Aerosol mixtures composed of coarse mode desert dust combined with fine mode combustion generated aerosols (from fossil fuel and biomass burning sources) were investigated at three locations that are ...in and/or downwind of major global aerosol emission source regions. Multiyear monitoring data at Aerosol Robotic Network sites in Beijing (central eastern China), Kanpur (Indo-Gangetic Plain, northern India), and Ilorin (Nigeria, Sudanian zone of West Africa) were utilized to study the climatological characteristics of aerosol optical properties. Multiyear climatological averages of spectral single scattering albedo (SSA) versus fine mode fraction (FMF) of aerosol optical depth at 675 nm at all three sites exhibited relatively linear trends up to 50% FMF. This suggests the possibility that external linear mixing of both fine and coarse mode components (weighted by FMF) dominates the SSA variation, where the SSA of each component remains relatively constant for this range of FMF only. However, it is likely that a combination of other factors is also involved in determining the dynamics of SSA as a function of FMF, such as fine mode particles adhering to coarse mode dust. The spectral variation of the climatological averaged aerosol absorption optical depth (AAOD) was nearly linear in logarithmic coordinates over the wavelength range of 440-870 nm for both the Kanpur and Ilorin sites. However, at two sites in China (Beijing and Xianghe), a distinct nonlinearity in spectral AAOD in logarithmic space was observed, suggesting the possibility of anomalously strong absorption in coarse mode aerosols increasing the 870 nm AAOD.
In January 2013, North China Plain experienced several serious haze events. Cimel sunphotometer measurements at seven sites over rural, suburban and urban regions of North China Plain from 1 to 30 ...January 2013 were used to further our understanding of spatial-temporal variation of aerosol optical parameters and aerosol radiative forcing (ARF). It was found that Aerosol Optical Depth at 500 nm (AOD500 nm) during non-pollution periods at all stations was lower than 0.30 and increased significantly to greater than 1.00 as pollution events developed. The Angstrom exponent (Alpha) was larger than 0.80 for all stations most of the time. AOD500 nm averages increased from north to south during both polluted and non-polluted periods on the three urban sites in Beijing. The fine mode AOD during pollution periods is about a factor of 2.5 times larger than that during the non-pollution period at urban sites but a factor of 5.0 at suburban and rural sites. The fine mode fraction of AOD675 nm was higher than 80% for all sites during January 2013. The absorption AOD675 nm at rural sites was only about 0.01 during pollution periods, while ~0.03–0.07 and 0.01–0.03 during pollution and non-pollution periods at other sites, respectively. Single scattering albedo varied between 0.87 and 0.95 during January 2013 over North China Plain. The size distribution showed an obvious tri-peak pattern during the most serious period. The fine mode effective radius in the pollution period was about 0.01–0.08 μm larger than during non-pollution periods, while the coarse mode radius in pollution periods was about 0.06–0.38 μm less than that during non-pollution periods. The total, fine and coarse mode particle volumes varied by about 0.06–0.34 μm3, 0.03–0.23 μm3, and 0.03–0.10 μm3, respectively, throughout January 2013. During the most intense period (1–16 January), ARF at the surface exceeded −50 W m−2, −180 W m−2, and −200 W m−2 at rural, suburban, and urban sites, respectively. The ARF readings at the top of the atmosphere were approximately −30 W m−2 in rural and −40–60 W m−2 in urban areas. Positive ARF at the top of the atmosphere at the Huimin suburban site was found to be different from others as a result of the high surface albedo due to snow cover.
Recent results from diverse air, ground, and laboratory studies using both radiometric and in situ techniques show that the fractions of black carbon, organic matter, and mineral dust in atmospheric ...aerosols determine the wavelength dependence of absorption (often expressed as Absorption Angstrom Exponent, or AAE). Taken together, these results hold promise of improving information on aerosol composition from remote measurements. The main purpose of this paper is to show that AAE values for an Aerosol Robotic Network (AERONET) set of retrievals from Sun-sky measurements describing full aerosol vertical columns are also strongly correlated with aerosol composition or type. In particular, we find AAE values near 1 (the theoretical value for black carbon) for AERONET-measured aerosol columns dominated by urban-industrial aerosol, larger AAE values for biomass burning aerosols, and the largest AAE values for Sahara dust aerosols. These AERONET results are consistent with results from other, very different, techniques, including solar flux-aerosol optical depth (AOD) analyses and airborne in situ analyses examined in this paper, as well as many other previous results. Ambiguities in aerosol composition or mixtures thereof, resulting from intermediate AAE values, can be reduced via cluster analyses that supplement AAE with other variables, for example Extinction Angstrom Exponent (EAE), which is an indicator of particle size. Together with previous results, these results strengthen prospects for determining aerosol composition from space, for example using the Glory Aerosol Polarimetry Sensor (APS), which seeks to provide retrievals of multiwavelength single-scattering albedo (SSA) and aerosol optical depth (and therefore aerosol absorption optical depth (AAOD) and AAE), as well as shape and other aerosol properties. Multidimensional cluster analyses promise additional information content, for example by using the Ozone Monitoring Instrument (OMI) to add AAOD in the near ultraviolet and CALIPSO aerosol layer heights to reduce height-absorption ambiguity.
We compared CALIPSO column aerosol optical depths at 0.532 μm to measurements at 147 AERONET sites, synchronized to within 30 min of satellite overpass times during a 3-yr period. We found 677 ...suitable overpasses, and a CALIPSO bias of −13% relative to AERONET for the entire data set; the corresponding absolute bias is −0.029, and the standard deviation of the mean (SDOM) is 0.014. Consequently, the null hypothesis is rejected at the 97% confidence level, indicating a statistically significant difference between the datasets. However, if we omit CALIPSO columns that contain dust from our analysis, the relative and absolute biases are reduced to −3% and −0.005 with a standard error of 0.016 for 449 overpasses, and the statistical confidence level for the null hypothesis rejection is reduced to 27%. We also analyzed the results according to the six CALIPSO aerosol subtypes and found relative and absolute biases of −29% and −0.1 for atmospheric columns that contain the dust subtype exclusively, but with a relatively high correlation coefficient of R = 0.58; this indicates the possibility that the assumed lidar ratio (40 sr) for the CALIPSO dust retrievals is too low. Hence, we used the AERONET size distributions, refractive indices, percent spheres, and forward optics code for spheres and spheroids to compute a lidar ratio climatology for AERONET sites located in the dust belt. The highest lidar ratios of our analysis occur in the non-Sahel regions of Northern Africa, where the median lidar ratio at 0.532 μm is 55.4 sr for 229 retrievals. Lidar ratios are somewhat lower in the African Sahel (49.7 sr for 929 retrievals), the Middle East (42.6 sr for 489 retrievals), and Kanpur, India (43.8 sr for 67 retrievals). We attribute this regional variability in the lidar ratio to the regional variability of the real refractive index of dust, as these two parameters are highly anti-correlated (correlation coefficients range from −0.51 to −0.85 for the various regions). The AERONET refractive index variability is consistent with the variability of illite concentration in dust across the dust belt.
The proposed development is an attempt to enhance aerosol retrieval by emphasizing statistical optimization in inversion of advanced satellite observations. This optimization concept improves ...retrieval accuracy relying on the knowledge of measurement error distribution. Efficient application of such optimization requires pronounced data redundancy (excess of the measurements number over number of unknowns) that is not common in satellite observations. The POLDER imager on board the PARASOL micro-satellite registers spectral polarimetric characteristics of the reflected atmospheric radiation at up to 16 viewing directions over each observed pixel. The completeness of such observations is notably higher than for most currently operating passive satellite aerosol sensors. This provides an opportunity for profound utilization of statistical optimization principles in satellite data inversion. The proposed retrieval scheme is designed as statistically optimized multi-variable fitting of all available angular observations obtained by the POLDER sensor in the window spectral channels where absorption by gas is minimal. The total number of such observations by PARASOL always exceeds a hundred over each pixel and the statistical optimization concept promises to be efficient even if the algorithm retrieves several tens of aerosol parameters. Based on this idea, the proposed algorithm uses a large number of unknowns and is aimed at retrieval of extended set of parameters affecting measured radiation. The algorithm is designed to retrieve complete aerosol properties globally. Over land, the algorithm retrieves the parameters of underlying surface simultaneously with aerosol. In all situations, the approach is anticipated to achieve a robust retrieval of complete aerosol properties including information about aerosol particle sizes, shape, absorption and composition (refractive index). In order to achieve reliable retrieval from PARASOL observations even over very reflective desert surfaces, the algorithm was designed as simultaneous inversion of a large group of pixels within one or several images. Such multi-pixel retrieval regime takes advantage of known limitations on spatial and temporal variability in both aerosol and surface properties. Specifically the variations of the retrieved parameters horizontally from pixel-to-pixel and/or temporary from day-to-day are enforced to be smooth by additional a priori constraints. This concept is expected to provide satellite retrieval of higher consistency, because the retrieval over each single pixel will be benefiting from coincident aerosol information from neighboring pixels, as well, from the information about surface reflectance (over land) obtained in preceding and consequent observations over the same pixel. The paper provides in depth description of the proposed inversion concept, illustrates the algorithm performance by a series of numerical tests and presents the examples of preliminary retrieval results obtained from actual PARASOL observations. It should be noted that many aspects of the described algorithm design considerably benefited from experience accumulated in the preceding effort on developments of currently operating AERONET and PARASOL retrievals, as well as several core software components were inherited from those earlier algorithms.
Multi-year observations of aerosol microphysical and optical properties, obtained through ground-based remote sensing at 50 China Aerosol Remote Sensing Network (CARSNET) sites, were used to ...characterize the aerosol climatology for representative remote, rural, and urban areas over China to assess effects on climate. The annual mean effective radii for total particles (ReffT) decreased from north to south and from rural to urban sites, and high total particle volumes were found at the urban sites. The aerosol optical depth at 440 nm (AOD440 nm) increased from remote and rural sites (0.12) to urban sites (0.79), and the extinction Ångström exponent (EAE440–870 nm) increased from 0.71 at the arid and semi-arid sites to 1.15 at the urban sites, presumably due to anthropogenic emissions. Single-scattering albedo (SSA440 nm) ranged from 0.88 to 0.92, indicating slightly to strongly absorbing aerosols. Absorption AOD440 nm values were 0.01 at the remote sites versus 0.07 at the urban sites. The average direct aerosol radiative effect (DARE) at the bottom of atmosphere increased from the sites in the remote areas (−24.40 W m−2) to the urban areas (−103.28 W m−2), indicating increased cooling at the latter. The DARE for the top of the atmosphere increased from −4.79 W m−2 at the remote sites to −30.05 W m−2 at the urban sites, indicating overall cooling effects for the Earth–atmosphere system. A classification method based on SSA440 nm, fine-mode fraction (FMF), and EAE440–870 nm showed that coarse-mode particles (mainly dust) were dominant at the rural sites near the northwestern deserts, while light-absorbing, fine-mode particles were important at most urban sites. This study will be important for understanding aerosol climate effects and regional environmental pollution, and the results will provide useful information for satellite validation and the improvement of climate modelling.
Recently, some authors have suggested that the absorption Ångström exponent (AAE) can be used to deduce the component aerosol absorption optical depths (AAODs) of carbonaceous aerosols in the AERONET ...database. This AAE approach presumes that AAE ≪ 1 for soot carbon, which contrasts the traditional small particle limit of AAE = 1 for soot carbon. Thus, we provide an overview of the AERONET retrieval, and we investigate how the microphysics of carbonaceous aerosols can be interpreted in the AERONET AAE product. We find that AAE ≪ 1 in the AERONET database requires large coarse mode fractions and/or imaginary refractive indices that increase with wavelength. Neither of these characteristics are consistent with the current definition of soot carbon, so we explore other possibilities for the cause of AAE ≪ 1. AAE is related to particle size, and coarse mode particles have a smaller AAE than fine mode particles for a given aerosol mixture of species. We also note that the mineral goethite has an imaginary refractive index that increases with wavelength, is very common in dust regions, and can easily contribute to AAE ≪ 1. We find that AAE ≪ 1 can not be caused by soot carbon, unless soot carbon has an imaginary refractive index that increases with wavelength throughout the visible and near-infrared spectrums. Finally, AAE is not a robust parameter for separating carbonaceous absorption from dust aerosol absorption in the AERONET database.
Long-range-transported Canadian smoke layers in the stratosphere over
northern France were detected by three lidar systems in August 2017. The
peaked optical depth of the stratospheric smoke layer
...exceeds 0.20 at 532 nm, which is
comparable with the simultaneous tropospheric aerosol optical depth. The
measurements of satellite sensors revealed that the observed stratospheric
smoke plumes were transported from Canadian wildfires after being lofted by
strong pyro-cumulonimbus. Case studies at two observation sites, Lille (lat
50.612, long 3.142, 60 m a.s.l.) and Palaiseau (lat 48.712, long 2.215,
156 m a.s.l.), are presented in detail. Smoke particle depolarization
ratios are measured at three wavelengths: over 0.20 at 355 nm, 0.18–0.19 at
532 nm, and 0.04–0.05 at 1064 nm. The high depolarization ratios and their
spectral dependence are possibly caused by the irregular-shaped aged smoke
particles and/or the mixing with dust particles. Similar results are found by
several European lidar stations and an explanation that can fully resolve
this question has not yet been found. Aerosol inversion based on lidar
2α+3β data derived a smoke effective radius of about
0.33 µm for both cases. The retrieved single-scattering albedo is
in the range of 0.8 to 0.9, indicating that the smoke plumes are absorbing.
The absorption can cause perturbations to the temperature vertical profile,
as observed by ground-based radiosonde, and it is also related to the ascent
of the smoke plumes when exposed in sunlight. A direct radiative
forcing (DRF) calculation is performed using the obtained optical and
microphysical properties. The calculation revealed that the smoke plumes in
the stratosphere can significantly reduce the radiation arriving at the
surface, and the heating rate of the plumes is about 3.5 K day−1. The
study provides a valuable characterization for aged smoke in the
stratosphere, but efforts are still needed in reducing and quantifying the
errors in the retrieved microphysical properties as well as radiative forcing
estimates.
West Africa and the adjacent oceanic regions are very important locations for studying dust properties and their influence on weather and climate. The SHADOW (study of SaHAran Dust Over West Africa) ...campaign is performing a multiscale and multilaboratory study of aerosol properties and dynamics using a set of in situ and remote sensing instruments at an observation site located at the IRD (Institute for Research and Development) in Mbour, Senegal (14° N, 17° W). In this paper, we present the results of lidar measurements performed during the first phase of SHADOW (study of SaHAran Dust Over West Africa) which occurred in March–April 2015. The multiwavelength Mie–Raman lidar acquired 3β + 2α + 1δ measurements during this period. This set of measurements has permitted particle-intensive properties, such as extinction and backscattering Ångström exponents (BAE) for 355/532 nm wavelengths' corresponding lidar ratios and depolarization ratio at 532 nm, to be determined. The mean values of dust lidar ratios during the observation period were about 53 sr at both 532 and 355 nm, which agrees with the values observed during the SAMUM-1 and SAMUM-2 campaigns held in Morocco and Cabo Verde in 2006 and 2008. The mean value of the particle depolarization ratio at 532 nm was 30 ± 4.5 %; however, during strong dust episodes this ratio increased to 35 ± 5 %, which is also in agreement with the results of the SAMUM campaigns. The backscattering Ångström exponent during the dust episodes decreased to ∼ −0.7, while the extinction Ångström exponent, though negative, was greater than −0.2. Low values of BAE can likely be explained by an increase in the imaginary part of the dust refractive index at 355 nm compared to 532 nm. The dust extinction and backscattering coefficients at multiple wavelengths were inverted to the particle microphysics using the regularization algorithm and the model of randomly oriented spheroids. The analysis performed has demonstrated that the spectral dependence of the imaginary part of the dust refractive index may significantly influence the inversion results and should be taken into account.
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