scholarly journals Variability of the infrared complex refractive index of African mineral dust: experimental estimation and implications for radiative transfer and satellite remote sensing

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.

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.


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.


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.


2017 ◽  
Author(s):  
Daniela Meloni ◽  
Alcide di Sarra ◽  
Gérard Brogniez ◽  
Cyrielle Denjean ◽  
Lorenzo De Silvestri ◽  
...  

Abstract. Detailed atmospheric and aerosol properties, and radiation measurements 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 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 size distribution and refractive indices, 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 size distribution (SD) and refractive index (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 SD 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 brightness temperatures 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, its vertical distribution, and at including regionally-resolved optical properties.


2021 ◽  
Author(s):  
Marilena Teri ◽  
Thomas Müller ◽  
Josef Gasteiger ◽  
Sara Valentini ◽  
Helmuth Horvath ◽  
...  

Abstract. Aerosol particles in the atmosphere interact with solar radiation through scattering and absorption. Accurate aerosol optical properties are needed to reduce the uncertainties of climate predictions. The aerosol optical properties can be obtained via optical modeling based on the measured particle size distribution. This approach requires knowledge or assumptions on the particle refractive index and shape. Meanwhile, integrating nephelometry provides information on the aerosol scattering properties directly. However, their measurements are affected by angular non-idealities, and their data need to be corrected for angular truncation and illumination to provide the particle scattering coefficient. We performed an extensive closure study, including a laboratory and a simulated experiment, aiming to compare different nephelometer angular truncation and illumination corrections (further referred to as "angular corrections"). We focused on coarse mode irregularly shaped aerosols, such as mineral dust, a worldwide abundant aerosol component. The angular correction of irregular particles is found to be only ~2 % higher than the angular correction of volume equivalent spheres. If the angular correction is calculated with Mie theory, the particle size distribution is needed. Our calculations show that if the particle size distribution is retrieved from optical particle spectrometer measurements and the irregular shape effect is not considered, the angular correction can be overestimated by about 5 % and up to 22 %. For mineral dust, the traditional angular correction based on the wavelength dependency of the scattering coefficient seems more accurate. We propose a guideline to establish the most appropriate angular correction depending on the aerosol type and the investigated size range.


2021 ◽  
Author(s):  
Yaowei Li ◽  
John Dykema ◽  
Frank Keutsch

<p>Model results suggest organic aerosol represents a significant fraction of total stratospheric aerosol radiative forcing, which in itself could represent as much as a quarter of global radiative forcing. Other model investigations suggest that the radiative influence of organic aerosols and dust must be included to obtain consistency with satellite measurements of stratospheric aerosols. <em>In situ</em> observations suggest that stratospheric aerosol composition is strongly vertically dependent and contains a significant organic component in the lower stratosphere. Laboratory studies suggest a range of possible values for the complex refractive index of organic aerosols in the stratosphere. The real part of the refractive index could vary over a range that brackets the value of the real refractive index for pure sulfuric acid/water aerosols. The imaginary part of the refractive index of the organic component is highly uncertain, suggesting aerosols that range from being purely refractive to significantly absorbing (eg, brown carbon). The mixing state of these mixed composition aerosols is also uncertain; depending on the complex refractive index of the organic component, morphological variation could have a significant influence on aerosol radiative properties. In this work we perform a sensitivity study of shortwave radiative forcing of stratospheric aerosols, examining the influence of different plausible values of complex refractive index and particle morphologies. <em>In situ</em> measurements of aerosol size and composition are used to represent the size distribution, vertical profile, and organic mass fraction for the computation of aerosol optical properties. These profiles of aerosol optical properties are used as inputs to a radiative transfer model to calculate profiles of shortwave fluxes and radiative heating rates for standard model atmospheres. The implications of the variations in aerosol optical depth and resulting radiative forcing are interpreted in terms of implications for satellite measurements of stratospheric radiative forcing. The various radiative forcing results and remote sensing implications for different scenarios of organic complex refractive index and morphology call for better understandings of the effects of chemical evolution and transport dynamics on the aerosol optical properties in the stratosphere.</p>


2011 ◽  
Vol 11 (13) ◽  
pp. 6387-6410 ◽  
Author(s):  
P. Formenti ◽  
J. L. Rajot ◽  
K. Desboeufs ◽  
F. Saïd ◽  
N. Grand ◽  
...  

Abstract. We performed airborne measurements of aerosol particle concentration, composition, size distribution and optical properties over Western Africa in the corridor 2–17° N and 3–5° E. Data were collected on board the French ATR-42 research aircraft in June–July 2006 as part of the African Monsoon Multidisciplinary Analysis (AMMA) intensive field phases in June–July 2006 using the AVIRAD airborne aerosol sampling system. The aerosol vertical distribution was documented on an almost daily basis. In particular, the vertical distribution of mineral dust emitted locally by Mesoscale Convective Systems (MSC) was distinguished from that of mineral dust that was transported from the Saharan by the African Easterly Jet (AEJ). Mineral dust emitted in the Sahel by convection-driven erosion was mostly confined in the boundary layer. One episode of injection of Sahelian mineral dust in the AEJ was observed. The elemental composition was found to be an element of difference between episodes, whereas the volume size distribution was more uniform. For non-mixed dust, the single scattering albedo ranged between 0.88–0.93 at 370 nm and between 0.91–0.99 at 950 nm, lower values being observed for Sahelian dust. In correspondence, the imaginary part of the complex refractive index varied between 0.002–0.004 at 370 nm and between 0.001–0.002 at 950 nm.


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.


2016 ◽  
Vol 63 (237) ◽  
pp. 133-147 ◽  
Author(s):  
S. McKENZIE SKILES ◽  
THOMAS PAINTER ◽  
GREGORY S. OKIN

ABSTRACTDust deposition to snow can have regionally important climatic and hydrologic impacts resulting from direct reduction of surface albedo and indirectly from the initiation of snow albedo feedbacks. Modeling the radiative impacts of dust deposited in snow requires knowledge of the optical properties of both components. Here we present an inversion technique to retrieve the effective optical properties of dust deposited in mountain snow cover from measurements of hemispherical dust reflectance and particle size distributions using radiative transfer modeling. First, modeled reflectance is produced from single scattering properties modeled with Mie theory for a specified grain size distribution over a range of values for the imaginary part of the complex refractive index (k = 0.00001–0.1). Then, a multi-step look-up table process is employed to retrieve kλ and single scattering optical properties by matching measured to modeled reflectance across the shortwave and near infrared. The real part of the complex refractive index, n, for dust aerosols ranges between 1.5 and 1.6 and a sensitivity analysis shows the method is relatively insensitive to the choice of n within this range, 1.525 was used here. Using the values retrieved by this method to update dust optical properties in a snow + aerosol radiative transfer model reduces errors in springtime albedo modeling by 50–70%.


2015 ◽  
Vol 15 (9) ◽  
pp. 13347-13393
Author(s):  
A. Pietrodangelo ◽  
R. Salzano ◽  
C. Bassani ◽  
S. Pareti ◽  
C. Perrino

Abstract. New information on the PM10 mineral dust from site-specific (Rome area, Latium) outcropped rocks, and on the microphysics, optical properties and radiative effects of mineral dust at local level were gained in this work. A multi-disciplinary approach was used, based on individual-particle scanning electron microscopy with X-ray energy-dispersive microanalysis (SEM XEDS), X-ray diffraction (XRD) analysis of dust, size distribution of mineral particles, and radiative transfer modelling (RTM).The mineral composition of Rome lithogenic PM10 varies between an end-member dominated by silicate minerals and one exclusively composed of calcite. The first is obtained from volcanic lithotypes, the second from travertine or limestones; lithogenic PM10 with intermediate composition derives mainly from siliciclastic rocks or marlstones of Rome area. Size and mineral species of PM10 particles of silicate-dominated dust types are tuned mainly by weathering and, to lesser extent, by debris formation or crystallization; chemical precipitation of CaCO3 plays a major role in calcite-dominated types. These differences are evidenced by the diversity of volume distributions, within either dust types, or mineral species. Further differences are observed between volume distributions of calcite from travertine (natural source) and from road dust (anthropic source), specifically on the width, shape and enrichment of the fine fraction (unimodal at 5 μm a.d. for travertine, bimodal at 3.8 and 1.8 μm a.d. for road dust). Log-normal probability density functions of volcanics and travertine dusts affect differently the single scattering albedo (SSA) and the asymmetry parameter (g) in the VISible and Near Infrared (NIR) regions, depending also on the absorbing/non-absorbing character of volcanics and travertine, respectively. The downward component of the BOA solar irradiance simulated by RTM for a volcanics-rich or travertine-rich atmosphere shows that volcanics contribution to the solar irradiance differs significantly from that of travertine in the NIR region, while similar contributions are modelled in the VIS.


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