scholarly journals Global scale variability of the mineral dust long-wave refractive index: a new dataset of in situ measurements for climate modeling and remote sensing

2017 ◽  
Vol 17 (3) ◽  
pp. 1901-1929 ◽  
Author(s):  
Claudia Di Biagio ◽  
Paola Formenti ◽  
Yves Balkanski ◽  
Lorenzo Caponi ◽  
Mathieu Cazaunau ◽  
...  

Abstract. Modeling the interaction of dust with long-wave (LW) radiation is still a challenge because of the scarcity of information on the complex refractive index of dust from different source regions. In particular, little is known about the variability of the refractive index as a function of the dust mineralogical composition, which depends on the specific emission source, and its size distribution, which is modified during transport. As a consequence, to date, climate models and remote sensing retrievals generally use a spatially invariant and time-constant value for the dust LW refractive index. In this paper, the variability of the mineral dust LW refractive index as a function of its mineralogical composition and size distribution is explored by in situ measurements in a large smog chamber. Mineral dust aerosols were generated from 19 natural soils from 8 regions: northern Africa, the Sahel, eastern Africa and the Middle East, eastern Asia, North and South America, southern Africa, and Australia. Soil samples were selected from a total of 137 available samples in order to represent the diversity of sources from arid and semi-arid areas worldwide and to account for the heterogeneity of the soil composition at the global scale. Aerosol samples generated from soils were re-suspended in the chamber, where their LW extinction spectra (3–15 µm), size distribution, and mineralogical composition were measured. The generated aerosol exhibits a realistic size distribution and mineralogy, including both the sub- and super-micron fractions, and represents in typical atmospheric proportions the main LW-active minerals, such as clays, quartz, and calcite. The complex refractive index of the aerosol is obtained by an optical inversion based upon the measured extinction spectrum and size distribution. Results from the present study show that the imaginary LW refractive index (k) of dust varies greatly both in magnitude and spectral shape from sample to sample, reflecting the differences in particle composition. In the 3–15 µm spectral range, k is between ∼ 0.001 and 0.92. The strength of the dust absorption at ∼ 7 and 11.4 µm depends on the amount of calcite within the samples, while the absorption between 8 and 14 µm is determined by the relative abundance of quartz and clays. The imaginary part (k) is observed to vary both from region to region and for varying sources within the same region. Conversely, for the real part (n), which is in the range 0.84–1.94, values are observed to agree for all dust samples across most of the spectrum within the error bars. This implies that while a constant n can be probably assumed for dust from different sources, a varying k should be used both at the global and the regional scale. A linear relationship between the magnitude of the imaginary refractive index at 7.0, 9.2, and 11.4 µm and the mass concentration of calcite and quartz absorbing at these wavelengths was found. We suggest that this may lead to predictive rules to estimate the LW refractive index of dust in specific bands based on an assumed or predicted mineralogical composition, or conversely, to estimate the dust composition from measurements of the LW extinction at specific wavebands. Based on the results of the present study, we recommend that climate models and remote sensing instruments operating at infrared wavelengths, such as IASI (infrared atmospheric sounder interferometer), use regionally dependent refractive indices rather than generic values. Our observations also suggest that the refractive index of dust in the LW does not change as a result of the loss of coarse particles by gravitational settling, so that constant values of n and k could be assumed close to sources and following transport. The whole dataset of the dust complex refractive indices presented in this paper is made available to the scientific community in the Supplement.

2016 ◽  
Author(s):  
Claudia Di Biagio ◽  
Paola Formenti ◽  
Yves Balkanski ◽  
Lorenzo Caponi ◽  
Mathieu Cazaunau ◽  
...  

Abstract. Modelling the interaction of dust with longwave (LW) radiation is still a challenge due to the scarcity of information on the complex refractive index of dust from different source regions. In particular, little is known on the variability of the refractive index as a function of the dust mineralogical composition, depending on the source region of emission, and the dust size distribution, which is modified during transport. As a consequence, to date, climate models and remote sensing retrievals generally use a spatially-invariant and time-constant value for the dust LW refractive index. In this paper the variability of the mineral dust LW refractive index as a function of its mineralogical composition and size distribution is explored by in situ measurements in a large smog chamber. Mineral dust aerosols were generated from nineteen natural soils from Northern Africa, Sahel, Middle East, Eastern Asia, North and South America, Southern Africa, and Australia. Soil samples were selected from a total of 137 samples available in order to represent the diversity of sources from arid and semi-arid areas worldwide and to account for the heterogeneity of the soil composition at the global scale. Aerosol samples generated from soils were re-suspended in the chamber, where their LW extinction spectra (2–16 µm), size distribution, and mineralogical composition were measured. The generated aerosol exhibits a realistic size distribution and mineralogy, including both the sub- and super-micron fractions, and represents in typical atmospheric proportions the main LW-active minerals, such as clays, quartz, and calcite. The complex refractive index of the aerosol is obtained by an optical inversion based upon the measured extinction spectrum and size distribution. Results from the present study show that the LW refractive index of dust varies greatly both in magnitude and spectral shape from sample to sample, following the changes in the measured particle composition. The real part (n) of the refractive index is between 0.84 and 1.94, while the imaginary part (k) is ~ 0.001 and 0.92. For instance, the strength of the absorption at ~ 7 and 11.4 µm depends on the amount of calcite within the samples, while the absorption between 8 and 14 µm is determined by the relative abundance of quartz and clays. A linear relationship between the magnitude of the refractive index at 7.0, 9.2, and 11.4 µm and the mass concentration of calcite and quartz absorbing at these wavelengths was found. We suggest that this may lead to predictive rules to estimate the LW refractive index of dust in specific bands based on an assumed or predicted mineralogical composition, or conversely, to estimate the dust composition from measurements of the LW extinction at specific wavebands. Based on the results of the present study, we recommend using refractive indices specific for the different source regions, rather than generic values, in climate models and remote sensing applications. Our observations also suggest that the refractive index of dust in the LW does not change due to the loss of coarse particles by gravitational settling, so that a constant value could be assumed close to sources and during transport. The results of the present study also clearly suggest that the LW refractive index of dust varies at the regional scale. This regional variability has to be characterized further in order to better assess the influence of dust on regional climate, as well as to increase the accuracy of satellite retrievals over regions affected by dust. We make the whole dataset of the dust complex refractive indices obtained here available to the scientific community by publishing it in the supplementary material to this paper.


2021 ◽  
Author(s):  
Alain Miffre ◽  
Danaël Cholleton ◽  
Patrick Rairoux

<p>This abstract is dedicated to dual-wavelength polarization lidars (2β+2δ) and related particles backscattering Ångström exponents BAE<sub>p</sub>, as nowadays remotely evaluated by atmospheric multi-wavelength lidar instruments (Veselovskii et al., ACP, 2016). We here present two new lidar remote sensing developments applicable to every multi-wavelengths polarization lidars, as published in Miffre et al. (Rem. Sens. 2019, Opt. Lett. 2020).</p><p>As a first development, we investigate the size, shape and complex refractive index dependence of measured backscattering Ångström exponents (Miffre et al., Opt. Lett., 2020). If BAE<sub>p</sub> is generally considered as a particles size indicator, it actually depends on the particles size, shape (Mehri et al., Atm. Res., 2018) and complex refractive index as β<sub>p</sub> does. From a precise analysis of the polarization state of the backscattered radiation and of its wavelength dependence, in two components particle mixtures (p) = {s, ns} involving spherical (s) and nonspherical (ns)-particles, we could establish the relationship between BAE<sub>p</sub>, BAE<sub>s</sub> and BAE<sub>ns</sub>. Then, by numerically simulating the two latter, we could discuss on the range of involved particle sizes and complex refractive indices.</p><p>The second development is related to the remote sensing observation of a new particle formation event with a dual-wavelength polarization lidar (Miffre et al. Rem. Sens. 2019). Where previous thoughts were that it is not feasible due to the small size of involved particles, we identified the requirements ensuring a (UV, VIS) polarization lidar to be sensitive to the subsequent particles growth following nucleation events promoted by nonspherical mineral dust particles. The presentation will explicit these optical requirements in terms of polarization and spectroscopy, as recently published in (Miffre et al., Rem. Sens., 2019).</p><p>The oral presentation will first present our dual-wavelength polarization lidar remote sensing instrument (2β+2δ), based on an unique laboratory Pi-polarimeter (Miffre et al., JQSRT, 2016). Special focus will be made on the (UV, VIS) calibration of the polarization lidar, as a decisive point for precise observations and interpretations. As an application case study, the oral presentation will then consider the lidar remote sensing observation of a nucleation event promoted by mineral dust. There, the involved particles sizes of freshly nucleated sulfuric acid particles and mineral dust will be retrieved by considering the above backscattering Ångström exponents analysis. As expected, the retrieved involved particles sizes reveal the underlying physical-chemistry of the nucleation process promoted by mineral dust (Dupart et al., PNAS, 2012). We believe this work may then interest a wide community of scientists.</p><p>Veselovskii, I., P. Goloub, D. N. Whiteman, A. Diallo, T. Ndiaye, A. Kolgotin, and O. Dubovik, ACP, <strong>16</strong>(11), (2016).<br>Dupart, Y., A. Wiedensohler, H. Hermann, A. Miffre, P. Rairoux, B. D’Anna and C. George, PNAS, 109, 51, (2012).<br>Miffre, A., T. Mehri, M. Francis and P. Rairoux, JQSRT, 169, 79-90, (2016).<br>Mehri, T., P. Rairoux, T. Nousiainen, A. Miffre, Atm. Res. <strong>203</strong>, 44-61 (2018).<br>Miffre A, D Cholleton, T. Mehri and P Rairoux, Rem. Sens., 11(15), 1761, (2019).<br>Miffre, A., D. Cholleton, P. Rairoux, Opt. Lett.<strong> 45</strong>, 5, 1084-1087, (2020).</p>


2013 ◽  
Vol 6 (6) ◽  
pp. 10955-11010
Author(s):  
M. Taylor ◽  
S. Kazadzis ◽  
A. Tsekeri ◽  
A. Gkikas ◽  
V. Amiridis

Abstract. In order to exploit the full-Earth viewing potential of satellite instruments to globally characterise aerosols, new algorithms are required to deduce key microphysical parameters like the particle size distribution and optical parameters associated with scattering and absorption from space remote sensing data. Here, a methodology based on neural networks is developed to retrieve such parameters from satellite inputs and to validate them with ground-based remote sensing data. For key combinations of input variables available from MODIS and OMI Level 3 datasets, a grid of 100 feed-forward neural network architectures is produced, each having a different number of neurons and training proportion. The networks are trained with principal components accounting for 98% of the variance of the inputs together with principal components formed from 38 AERONET Level 2.0 (Version 2) retrieved parameters as outputs. Daily-averaged, co-located and synchronous data drawn from a cluster of AERONET sites centred on the peak of dust extinction in Northern Africa is used for network training and validation, and the optimal network architecture for each input parameter combination is identified with reference to the lowest mean squared error. The trained networks are then fed with unseen data at the coastal dust site Dakar to test their simulation performance. A NN, trained with co-located and synchronous satellite inputs comprising three aerosol optical depth measurements at 470, 500 and 660 nm, plus the columnar water vapour (from MODIS) and the modelled absorption aerosol optical depth at 500 nm (from OMI), was able to simultaneously retrieve the daily-averaged size distribution, the coarse mode volume, the imaginary part of the complex refractive index, and the spectral single scattering albedo – with moderate precision: correlation coefficients in the range 0.368 ≤ R ≤ 0.514. The network failed to recover the spectral behaviour of the real part of the complex refractive index with only 39–45% of the data falling within the acceptable level of uncertainty relative to ground-truth data at the daily timescale. In the context of Saharan desert dust, this new methodological approach appears to offer some potential for moderately accurate daily retrieval of previously inaccessible aerosol parameters from space.


2019 ◽  
Author(s):  
Xiaolin Zhang ◽  
Mao Mao

Abstract. Aerosol complex refractive index (ACRI) is an important microphysical parameter used for the studies of modeling their radiative effects. With considerable uncertainties related to retrieval based on observations, a numerical study is a powerful method, if not the only one, to provide a better and more accurate understanding on retrieved optically effective ACRI of aged BC particles. Numerical investigations on the optically effective ACRI of polydisperse coated BC aggregates retrieved from their accurate scattering and absorption properties, which are calculated by the multiple-sphere T-matrix method (MSTM), without overall particle shape variations during retrieval, are carried out. The aim of this study is to evaluate the effects of aerosol microphysics, including shell/core Dp / Dc ratio, BC geometry, BC position inside coating, and size distribution, on retrieved optically effective ACRI of coated BC particles. At odds with expectations, retrieved optically effective ACRIs of coated BC particles in coarse mode, are not merely impacted by their chemical compositions and shell/core ratio, being highly complicated functions of particle microphysics. However, in accumulation mode, the coated BC optically effective ACRI is dominantly influenced by particle chemical compositions and shell/core ratio, although it shows slightly sensitive to BC geometry, BC position inside coating and particle size distribution. The popular volume weighted average (VWA) method and effective medium theory (EMT) provide acceptable ACRI results for coated BC in accumulation mode, and the resulting uncertainties in particle scattering and absorption are both less than approximately 10 %. For coarse coated BC, the VWA and EMT, nevertheless, produce dramatically higher imaginary parts than those of optically effective ACRIs, significantly overestimating particle absorption by a factor of nearly 2 for heavily coated BC with a large BC fractal dimension or BC close to coating boundary. Using the VWA could introduce significant overestimation in aged BC absorption analysis studies, and this may be one of the reasons why modelled aerosol optical depth is 20 % larger than observed, since it is widely employed in the state-of-the-art aerosol-climate models. We propose a simple new ACRI parameterization for fully coated BC with Dp / Dc ≥ 2.0 in coarse mode, which can serve as a guide for the improvement of ACRI of heavily coated BC, and its scattering and absorption errors are reduced by a factor of nearly 2 compared to the VWA. Our study indicates that a reliable estimate of the radiative effects of aged BC particles in coarse mode would require accounting for the optically effective ACRI, rather than the ACRI given by the VWA, in aerosol-climate models.


2014 ◽  
Vol 7 (9) ◽  
pp. 3151-3175 ◽  
Author(s):  
M. Taylor ◽  
S. Kazadzis ◽  
A. Tsekeri ◽  
A. Gkikas ◽  
V. Amiridis

Abstract. In order to exploit the full-earth viewing potential of satellite instruments to globally characterise aerosols, new algorithms are required to deduce key microphysical parameters like the particle size distribution and optical parameters associated with scattering and absorption from space remote sensing data. Here, a methodology based on neural networks is developed to retrieve such parameters from satellite inputs and to validate them with ground-based remote sensing data. For key combinations of input variables available from the MODerate resolution Imaging Spectro-radiometer (MODIS) and the Ozone Measuring Instrument (OMI) Level 3 data sets, a grid of 100 feed-forward neural network architectures is produced, each having a different number of neurons and training proportion. The networks are trained with principal components accounting for 98% of the variance of the inputs together with principal components formed from 38 AErosol RObotic NETwork (AERONET) Level 2.0 (Version 2) retrieved parameters as outputs. Daily averaged, co-located and synchronous data drawn from a cluster of AERONET sites centred on the peak of dust extinction in Northern Africa is used for network training and validation, and the optimal network architecture for each input parameter combination is identified with reference to the lowest mean squared error. The trained networks are then fed with unseen data at the coastal dust site Dakar to test their simulation performance. A neural network (NN), trained with co-located and synchronous satellite inputs comprising three aerosol optical depth measurements at 470, 550 and 660 nm, plus the columnar water vapour (from MODIS) and the modelled absorption aerosol optical depth at 500 nm (from OMI), was able to simultaneously retrieve the daily averaged size distribution, the coarse mode volume, the imaginary part of the complex refractive index, and the spectral single scattering albedo – with moderate precision: correlation coefficients in the range 0.368 ≤ R ≤ 0.514. The network failed to recover the spectral behaviour of the real part of the complex refractive index. This new methodological approach appears to offer some potential for moderately accurate daily retrieval of the total volume concentration of the coarse mode of aerosol at the Saharan dust peak in the area of Northern Africa.


2018 ◽  
Vol 18 (6) ◽  
pp. 4377-4401 ◽  
Author(s):  
Daniela Meloni ◽  
Alcide di Sarra ◽  
Gérard Brogniez ◽  
Cyrielle Denjean ◽  
Lorenzo De Silvestri ◽  
...  

Abstract. Detailed measurements of radiation, atmospheric and aerosol properties were carried out in summer 2013 during the Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region (ADRIMED) campaign in the framework of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx) experiment. This study focusses on the characterization of infrared (IR) optical properties and direct radiative effects of mineral dust, based on three vertical profiles of atmospheric and aerosol properties and IR broadband and narrowband radiation from airborne measurements, made in conjunction with radiosonde and ground-based observations at Lampedusa, in the central Mediterranean. Satellite IR spectra from the Infrared Atmospheric Sounder Interferometer (IASI) are also included in the analysis. The atmospheric and aerosol properties are used as input to a radiative transfer model, and various IR radiation parameters (upward and downward irradiance, nadir and zenith brightness temperature at different altitudes) are calculated and compared with observations. The model calculations are made for different sets of dust particle size distribution (PSD) and refractive index (RI), derived from observations and from the literature. The main results of the analysis are that the IR dust radiative forcing is non-negligible and strongly depends on PSD and RI. When calculations are made using the in situ measured size distribution, it is possible to identify the refractive index that produces the best match with observed IR irradiances and brightness temperatures (BTs). The most appropriate refractive indices correspond to those determined from independent measurements of mineral dust aerosols from the source regions (Tunisia, Algeria, Morocco) of dust transported over Lampedusa, suggesting that differences in the source properties should be taken into account. With the in situ size distribution and the most appropriate refractive index the estimated dust IR radiative forcing efficiency is +23.7 W m−2 at the surface, −7.9 W m−2 within the atmosphere, and +15.8 W m−2 at the top of the atmosphere. The use of column-integrated dust PSD from AERONET may also produce a good agreement with measured irradiances and BTs, but with significantly different values of the RI. This implies large differences, up to a factor of 2.5 at surface, in the estimated dust radiative forcing, and in the IR heating rate. This study shows that spectrally resolved measurements of BTs are important to better constrain the dust IR optical properties, and to obtain a reliable estimate of its radiative effects. Efforts should be directed at obtaining an improved description of the dust size distribution and its vertical distribution, as well as at including regionally resolved optical properties.


2014 ◽  
Vol 14 (20) ◽  
pp. 11093-11116 ◽  
Author(s):  
C. Di Biagio ◽  
H. Boucher ◽  
S. Caquineau ◽  
S. Chevaillier ◽  
J. Cuesta ◽  
...  

Abstract. Experimental estimations of the infrared refractive index of African mineral dust have been retrieved from laboratory measurements of particle transmission spectra in the wavelength range 2.5–25 μm. Five dust samples collected at Banizoumbou (Niger) and Tamanrasset (Algeria) during dust events originated from different Western Saharan and Sahelian areas have been investigated. The real (n) and imaginary (k) parts of the refractive index obtained for the different dust samples vary in the range 1.1–2.7 and 0.05–1.0, respectively, and are strongly sensitive to the mineralogical composition of the particles, especially in the 8–12 and 17–25 μm spectral intervals. Dust absorption is controlled mainly by clays (kaolinite, illite, smectite) and, to a lesser extent, by quartz and calcium-rich minerals (e.g. calcite, gypsum). Significant differences are obtained when comparing our results with existing experimental estimations available in the literature, and with the values of the OPAC (Optical Properties of Aerosols and Clouds) database. The different data sets appear comparable in magnitude, with our values of n and k falling within the range of variability of past studies. However, literature data fail in accurately reproducing the spectral signatures of the main minerals, in particular clays, and they significantly overestimate the contribution of quartz. Furthermore, the real and the imaginary parts of the refractive index from some literature studies are found not to verify the Kramers–Kronig relations, thus being theoretically incorrect. The comparison between our results, from western Africa, and literature data, from different locations in Europe, Africa, and the Caribbean, nonetheless, confirms the expected large variability of the dust infrared refractive index. This highlights the necessity for an extended systematic investigation of dust properties at infrared wavelengths. For the five analysed dust samples, aerosol intensive optical properties relevant to radiative transfer (mass extinction efficiency, kext, single scattering albedo, ω, and asymmetry factor, g) have been calculated, by using the Mie theory, based on the estimated refractive index and measured particle size distribution. The optical properties show a large sample-to-sample variability, with kext, ω, and g varying in the range 0.05–0.35, 0.25–1.0, and 0.05–0.75. This variability is expected to significantly impact satellite retrievals of atmospheric and surface parameters (e.g. from the Infrared Atmospheric Sounding Interferometer, IASI) and estimates of the dust radiative forcing.


2014 ◽  
Vol 14 (7) ◽  
pp. 10597-10657 ◽  
Author(s):  
C. Di Biagio ◽  
H. Boucher ◽  
S. Caquineau ◽  
S. Chevaillier ◽  
J. Cuesta ◽  
...  

Abstract. Experimental estimations of the infrared refractive index of African mineral dust have been retrieved from laboratory measurements of particle transmission spectra in the wavelength range 2.5–25 μm. Five dust samples collected at Banizoumbou (Niger) and Tamanrasset (Algeria) during dust events originated from different Western Saharan and Sahelian areas have been investigated. The obtained real (n) and imaginary (k) parts of the refractive index for the different dust cases vary in the range 1.1–2.7 and 0.05–1.0, respectively, and appear to be strongly sensitive to the mineralogical composition of the particles, especially in the 8–12 μm and 17–25 μm spectral intervals. Dust absorption is controlled mainly by clays, and, in minor fraction, by quartz and Ca-rich minerals. Size distribution, and the coarse fraction in particular, plays also a role in determining the refractive index. Significant differences are obtained when comparing our results with existing experimental estimations available in the literature, and with the values of the OPAC (Optical Properties of Aerosols and Clouds) database. The different datasets appear comparable in magnitude, with our values of n and k falling in the range of variability of past studies. However, literature data fail in accurately reproducing the spectral signatures of main minerals, in particular clays, and they significantly overestimate the contribution of quartz. We also found that the real and the imaginary parts of the refractive index from part of literature studies do not verify Kramers–Kronig relations, thus resulting theoretically incorrect. The comparison between our results, from Western Africa, and literature data, from different locations in Europe, Africa, and the Caribbean, nonetheless, confirms the expected large variability of the infrared refractive index of dust, thus highlighting the necessity for an extended systematic investigation. Aerosol intensive optical properties relevant to radiative transfer (mass extinction efficiency, kext, single scattering albedo, ω, and asymmetry factor, g), have been calculated, by using the Mie theory, for the five analysed dust samples, based on the estimated refractive index and measured particle size distribution. The optical properties show a large sample-to-sample variability. This variability is expected to significantly impact satellite retrievals of atmospheric and surface parameters and estimates of the dust radiative forcing.


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