A Sensitivity Study on the Effects of Particle Chemistry, Asphericity and Size on the Mass Extinction Efficiency of Mineral Dust in the Earth's Atmosphere: From the Near to Thermal IR

Abstract. To determine a plausible range of mass extinction efficiencies (MEE) of terrestrial atmospheric dust from the near to thermal IR, sensitivity analyses are performed over an extended range of dust microphysical and chemistry perturbations. The IR values are subsequently compared to those in the near-IR, to evaluate spectral relationships in their optical properties. Synthesized size distributions consistent with measurements, model particle size, while composition is defined by the refractive indices of minerals routinely observed in dust, including the widely used OPAC/Hess parameterization. Single-scattering properties of representative dust particle shapes are calculated using the T-matrix, Discrete Dipole Approximation and Lorenz-Mie light-scattering codes. For the parameterizations examined, MEE ranges from nearly zero to 1.2 m2 g−1, with the higher values associated with non-spheres composed of quartz and gypsum. At near-IR wavelengths, MEE for non-spheres generally exceeds those for spheres, while in the thermal IR, shape-induced changes in MEE strongly depend on volume median diameter (VMD) and wavelength, particularly for MEE evaluated at the mineral resonant frequencies. MEE spectral distributions appear to follow particle geometry and are evidence for shape dependency in the optical properties. It is also shown that non-spheres best reproduce the positions of prominent absorption peaks found in silicates. Generally, angular particles exhibit wider and more symmetric MEE spectral distribution patterns from 8–10 μm than those with smooth surfaces, likely due to their edge-effects. Lastly, MEE ratios allow for inferring dust optical properties across the visible-IR spectrum. We conclude the MEE of dust aerosol are significant for the parameter space investigated, and are a key component for remote sensing applications and the study of direct aerosol radiative effects.

[1]  D. T. Griffen Silicate Crystal Chemistry , 1992 .

[2]  M. Schnaiter,et al.  Optical properties and mineralogical composition of different Saharan mineral dust samples: a laboratory study , 2006 .

[3]  D. A. Kleinman,et al.  Infrared Lattice Bands of Quartz , 1961 .

[4]  G. Rossman,et al.  Estimated optical constants of gypsum in the regions of weak absorptions: Application of scattering theories and comparisons to independent measurements , 2007 .

[5]  J. Seinfeld,et al.  Atmospheric Chemistry and Physics: From Air Pollution to Climate Change , 1997 .

[6]  E. Purcell,et al.  Scattering and Absorption of Light by Nonspherical Dielectric Grains , 1973 .

[7]  J. Reid,et al.  Remote sensing of mineral dust aerosol using AERI during the UAE 2 : A modeling and sensiti , 2008 .

[8]  E. Palik Handbook of Optical Constants of Solids , 1997 .

[9]  B. Draine,et al.  User Guide for the Discrete Dipole Approximation Code DDSCAT (Version 5a10) , 2000, astro-ph/0008151.

[10]  T. Müller,et al.  In situ measurements of optical properties at Tinfou (Morocco) during the Saharan Mineral Dust Experiment SAMUM 2006 , 2009 .

[11]  Eric P. Shettle,et al.  A Wind Dependent Desert Aerosol Model: Radiative Properties , 1988 .

[12]  Bin Chen,et al.  Morphological and chemical modification of mineral dust: Observational insight into the heterogeneous uptake of acidic gases , 2005 .

[13]  J. Pollack,et al.  Derivation of midinfrared (5-25 μm) optical constants of some silicates and palagonite , 1991 .

[14]  V. Grassian,et al.  Coupled infrared extinction and size distribution measurements for several clay components of mineral dust aerosol , 2008 .

[15]  K. Liou,et al.  Light scattering by hexagonal ice crystals: comparison of finite-difference time domain and geometric optics models , 1995 .

[16]  Howard DeVoe,et al.  Optical Properties of Molecular Aggregates. I. Classical Model of Electronic Absorption and Refraction , 1964 .

[17]  Bruce T. Draine,et al.  The Discrete Dipole Approximation for Light Scattering by Irregular Targets , 2000 .

[18]  M. Mishchenko,et al.  Light scattering by polydispersions of randomly oriented spheroids with sizes comparable to wavelengths of observation. , 1994, Applied optics.

[19]  P. Barber OPTICAL PROPERTIES OF AEROSOLS , 1982 .

[20]  W. Malm,et al.  Intercomparison and closure calculations using measurements of aerosol species and optical properties during the Yosemite Aerosol Characterization Study , 2005 .

[21]  C. Karr Infrared and Raman spectroscopy of lunar and terrestrial minerals , 1975 .

[22]  P. Quinn,et al.  Aerosol optical properties measured on board the Ronald H. Brown during ACE-Asia as a function of aerosol chemical composition and source region , 2004 .

[23]  Robbie Hood,et al.  The Saharan Air Layer and the Fate of African Easterly Waves—NASA's AMMA Field Study of Tropical Cyclogenesis , 2009 .

[24]  John W. Salisbury,et al.  Infrared (2.1-25 μm) spectra of minerals , 1991 .

[25]  Munrr H. MexculrANri,et al.  GLAUCONITES: CATION EXCHANGE CAPACITIES AND INFRARED SPECTRA PATI II. INFRARED ABSORPTION CHARACTERISTICS OF GLAUCONITES , 2007 .

[26]  T. Takemura,et al.  Aerosol optical depth, physical properties and radiative forcing over the Arabian Sea , 2006 .

[27]  Eric P. Shettle,et al.  Atmospheric Aerosols: Global Climatology and Radiative Characteristics , 1991 .

[28]  F. Lázaro,et al.  The speciation of iron in desert dust collected in Gran Canaria (Canary Islands): Combined chemical, magnetic and optical analysis , 2008 .

[29]  C. Zerefos,et al.  Dust specific extinction cross-sections over the Eastern Mediterranean using the BSC-DREAM model and sun photometer data: the case of urban environments , 2009 .

[30]  P. Koepke,et al.  Optical Properties of Aerosols and Clouds: The Software Package OPAC , 1998 .

[31]  Jeffrey S. Reid,et al.  An Assessment of the Surface Longwave Direct Radiative Effect of Airborne Saharan Dust During the NAMMA Field Campaign , 2010 .

[32]  T. Roush Near-infrared (0.67–4.7 μm) optical constants estimated for montmorillonite , 2005 .

[33]  Thomas Trautmann,et al.  Solar radiative effects of a Saharan dust plume observed during SAMUM assuming spheroidal model particles , 2009 .

[34]  A. Smirnov,et al.  AERONET-a federated instrument network and data archive for aerosol Characterization , 1998 .

[35]  R. Knacke,et al.  Optical constants of chlorite and serpentine between 2.5 and 50 μm , 1985 .

[36]  P. Formenti,et al.  Size distribution, shape, and composition of mineral dust aerosols collected during the African Monsoon Multidisciplinary Analysis Special Observation Period 0: Dust and Biomass-Burning , 2008 .

[37]  Patrick Minnis,et al.  Taklimakan dust aerosol radiative heating derived from CALIPSO observations using the Fu-Liou radiation model with CERES constraints , 2009 .

[38]  W. Malm,et al.  Aerosol size distributions and visibility estimates during the Big Bend regional aerosol and visibility observational (BRAVO) study , 2002 .

[39]  Pedro A. Hernandez-Leal,et al.  SeaWiFS data to detect AVHRR-derived SST affected by aerosols , 2005 .

[40]  Gunnar Myhre,et al.  Global sensitivity experiments of the radiative forcing due to mineral aerosols , 2001 .

[41]  S. Ross The Infrared Spectra of Minerals , 1974 .

[42]  B. T. Draine,et al.  Radiative Torques on Interstellar Grains: I. Superthermal Spinup , 1996 .

[43]  Irina N. Sokolik,et al.  Characterization of iron oxides in mineral dust aerosols: Implications for light absorption , 2006 .

[44]  David J. Diner,et al.  Aerosol source plume physical characteristics from space-based multiangle imaging , 2007 .

[45]  M. Chin,et al.  Characterization of Asian Dust during ACE-Asia , 2006 .

[46]  F. Volz,et al.  Infrared optical constants of ammonium sulfate, sahara dust, volcanic pumice, and flyash. , 1973, Applied optics.

[47]  Hugh Coe,et al.  Regional variability of the composition of mineral dust from western Africa: Results from the AMMA SOP0/DABEX and DODO field campaigns , 2008 .

[48]  Michael J. Garay,et al.  Satellite-derived aerosol optical depth over dark water from MISR and MODIS : Comparisons with AERONET and implications for climatological studies , 2007 .

[49]  L. Larrabee Strow,et al.  Infrared dust spectral signatures from AIRS , 2006 .

[50]  V. Freudenthaler,et al.  Mineral dust observed with AERONET Sun photometer, Raman lidar, and in situ instruments during SAMUM 2006: Shape‐independent particle properties , 2010 .

[51]  Barry J. Huebert,et al.  Size distributions and mixtures of dust and black carbon aerosol in Asian outflow: Physiochemistry and optical properties , 2004 .

[52]  O. V. Kalashnikovaa,et al.  Modeling the radiative properties of nonspherical soil-derived mineral aerosols , 2004 .

[53]  F. Mandl American Institute of Physics Handbook 3rd edn , 1973 .

[54]  M. Querry,et al.  Optical constants of minerals and other materials from the millimeter to the ultraviolet , 1987 .

[55]  R. J. Bell,et al.  Optical properties of calcite and gypsum in crystalline and powdered form in the infrared and far-infrared , 1993 .

[56]  Larry D. Travis,et al.  Capabilities and limitations of a current FORTRAN implementation of the T-matrix method for randomly oriented, rotationally symmetric scatterers , 1998 .

[57]  Howard DeVoe,et al.  Optical Properties of Molecular Aggregates. II. Classical Theory of the Refraction, Absorption, and Optical Activity of Solutions and Crystals , 1965 .

[58]  J. Aronson,et al.  Optical constants of minerals and rocks. , 1975, Applied optics.

[59]  Olga V. Kalashnikova,et al.  Ability of multiangle remote sensing observations to identify and distinguish mineral dust types : Optical models and retrievals of optically thick plumes : Quantifying the radiative and biogeochemical impacts of mineral dust , 2005 .

[60]  J. Veverka Optical properties of inhomogeneous materials—Applications to geology, astronomy, chemistry, and engineering: Walter G. Egan and Theodore W. Hilgeman. Academic Press, New York, 1979. 235 pp., $27.50 , 1980 .

[61]  Jost Heintzenberg,et al.  Shape of atmospheric mineral particles collected in three Chinese arid‐regions , 2001 .

[62]  Superthermal,et al.  Radiative Torques on Interstellar Grains : I . , 1996 .

[63]  P. Formenti,et al.  Chemical composition of mineral dust aerosol during the Saharan Dust Experiment (SHADE) airborne campaign in the Cape Verde region, September 2000 , 2003 .

[64]  Manfred Wendisch,et al.  Desert dust aerosol air mass mapping in the western Sahara, using particle properties derived from space-based multi-angle imaging , 2009 .

[65]  J. Reid,et al.  Characterization of African dust transported to Puerto Rico by individual particle and size segregated bulk analysis , 2003 .

[66]  Irina N. Sokolik,et al.  Incorporation of mineralogical composition into models of the radiative properties of mineral aerosol from UV to IR wavelengths , 1999 .

[67]  L. W. Mckeehan The Crystal Structure of Quartz , 1923 .

[68]  Olga V. Kalashnikova,et al.  Importance of shapes and compositions of wind‐blown dust particles for remote sensing at solar wavelengths , 2002 .

[69]  J. Niemi,et al.  Single‐scattering modeling of thin, birefringent mineral‐dust flakes using the discrete‐dipole approximation , 2009 .

[70]  D. Drummond The Infra-Red Absorption Spectra of Quartz and Fused Silica from 1 to 7$ \cdot $5 $ \mu $. II. Experimental Results , 1936 .

[71]  T. Müller,et al.  Spectral absorption coefficients and imaginary parts of refractive indices of Saharan dust during SAMUM-1 , 2009 .

[72]  Martin Wirth,et al.  Airborne measurements of dust layer properties, particle size distribution and mixing state of Saharan dust during SAMUM 2006 , 2009 .

[73]  H. Maring,et al.  Aerosol physical and optical properties and their relationship to aerosol composition in the free troposphere at Izaña, Tenerife, Canary Islands, during July 1995 , 2000 .

[74]  Oleg Dubovik,et al.  Global aerosol optical properties and application to Moderate Resolution Imaging Spectroradiometer aerosol retrieval over land , 2007 .

[75]  A. Wiedensohler,et al.  Size distribution, mass concentration, chemical and mineralogical composition and derived optical parameters of the boundary layer aerosol at Tinfou, Morocco, during SAMUM 2006 , 2009 .

[76]  Timothy D. Glotch,et al.  Mid-infrared (5–100 μm) reflectance spectra and optical constants of ten phyllosilicate minerals , 2007 .

[77]  C. Thorncroft,et al.  African Monsoon Multidisciplinary Analysis: An International Research Project and Field Campaign , 2006 .

[78]  Y. Balkanski,et al.  Reevaluation of Mineral aerosol radiative forcings suggests a better agreement with satellite and AERONET data , 2006 .

[79]  G. Jeong Bulk and single-particle mineralogy of Asian dust and a comparison with its source soils , 2008 .

[80]  Olga V. Kalashnikova,et al.  Modeling the radiative properties of nonspherical soil-derived mineral aerosols , 2004 .

[81]  Jeffrey S. Reid,et al.  Remote sensing of mineral dust aerosol using AERI during the UAE2: A modeling and sensitivity study , 2008 .

[82]  Jenny L. Hand,et al.  Review of aerosol mass scattering efficiencies from ground-based measurements since 1990 , 2007 .

[83]  Gerard Capes,et al.  Overview of the Dust and Biomass‐burning Experiment and African Monsoon Multidisciplinary Analysis Special Observing Period‐0 , 2008 .

[84]  Timo Nousiainen,et al.  Optical modeling of mineral dust particles: A review , 2009 .

[85]  Alexander Smirnov,et al.  Comparison of size and morphological measurements of coarse mode dust particles from Africa , 2003 .

[86]  K. Voss,et al.  Dominance of mineral dust in aerosol light-scattering in the North Atlantic trade winds , 1996, Nature.

[87]  E. Shettle,et al.  Models for the aerosols of the lower atmosphere and the effects of humidity variations on their optical properties , 1979 .

[88]  S. Piketh,et al.  Dynamics of southwest Asian dust particle size characteristics with implications for global dust research , 2008 .