C. Di Biagio 1, P. Formenti 1, Y. Balkanski 2, M. Cazaunau 1, E. Pangui 1, E. Journet 1, S. Nowak 3, S. Caquineau 4, and J.F.

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Laboratory estimates of the mineral dust shortwave and longwave refractive index from global sources: a new dataset for climate modelling and remote sensing C. Di Biagio 1, P. Formenti 1, Y. Balkanski 2, M. Cazaunau 1, E. Pangui 1, E. Journet 1, S. Nowak 3, S. Caquineau 4, and J.F. Doussin 1 1 LISA, CNRS-IPSL UPD UPEC 2 LSCE, CEA CNRS UVSQ 3 Univ. Paris Diderot 4 Intitut de Recherche pour le Developpement 1

Aerosol direct radiative effect * Global annual mean at TOA, all-sky Anthropogenic aerosols Direct effect* (Wm -2 ) -0.95 +0.05 IPCC, 2013 Mineral dust IPCC, 2013 +0.1-0.3-2.2 Direct effect* (Wm -2 ) +0.76 Haywood et al., 1999; Woodward, 2001; Miller et al., 2004; Reddy et al., 2005; Balkanski et al., 2007; Zhao et al., 2011; Yue et al., 2010; Rap et al., 2013; Colarco et al. 2014, Kok et al. 2017 2

The absorption properties of mineral dust are a persisting major uncertainty Complex refractive index (CRI) = n-ik Natural variability (size, mineralogy..), sampling artefacts 3

The absorption properties of mineral dust are a persisting major uncertainty Complex refractive index (CRI) = n-ik Volz1972 (Germany) Volz 1973 (Barbados) Fouquart1987 (Niger) Carlson1980 Longtin 1988 OPAC Di Biagio 2014 (Niger, Algeria) Natural variability (size, mineralogy..), sampling artefacts 4

Climate models and remote sensing retrievals use a spatially invariant generic refractive index 5

In 2014 the LABEX-IPSL supported a new laboratory chamber activity to investigate the climate relevant spectral optical properties of mineral dust A laboratory-based project targeting the absorption optical properties of mineral dust according to wavelength (UV/visible/IR) soil mineralogy size distribution atmospheric ageing 6

Soil sample databank (>150 soils) 19 selected soils worldwide Di Biagio et al., 2014a, 2017; Caponi et al., 2017 7

Mineralogy of selected vs global soils Samples selected to represent the natural mineralogical variability of the global soils according to the soil database by Journet al al. (2014) 19 selected soils Hematite (%) Goethite (%) Goethite (%) Di Biagio et al., 2014a, 2017; Caponi et al., 2017 8

The CESAM simulation chamber Stainless-steel, 4.2 m 3 volume Generating aerosols under controlled conditions Long lifetime (> 24h for submicron aerosols) Simultaneous measurements of physico-chemical and optical properties www.cesam.cnrs.fr 9

Laboratory simulations - simultaneous measurements of physico-chemical and spectral optical properties In situ FTIR 2-16 µm, res 0.5 cm -1 Size distribution 4.2 m 3 Size distribution Nephelometer Aethalometer CAPS Pmex Mineralogical composition authentic mineral dust from natural soils 10

Experiments Mass concentration (µg m -3 ) Progressive loss of coarse particles D eff,c =3 4 µm D eff,c =2 µm Mineralogical composition integrated over the whole experiment Scattering coefficient (7-170 ) (Mm -1 ) Extinction coefficient (Mm -1 ) Morocco dust 11

Experiments Progressive loss of coarse particles (D eff,c =3 4 µm 2 µm) Mass concentration (µg m -3 ) CRI and SSA retrieved at 10-min temporal resolution Scattering coefficient (7-170 ) (Mm -1 ) Extinction coefficient (Mm -1 ) Same on LW extinction Morocco dust 12

Generated dust aerosols: variable and realistic mineralogy Iron oxides < 5.8% Total elemental iron 2.4 10.6% Di Biagio et al., 2017 13

Generated dust aerosols: realistic size distribution Injected in CESAM (mimic source dust) Seen by the instruments (mimic transported dust) Losses above 10 µm diameter Di Biagio et al., 2017

Dust SW refractive index: regional scale variability 15

Dust LW refractive index: regional scale variability 16

UV-VIS Comparison with previous results IR.how to translate this variability for models? 17

Relationship between CRI and iron and iron oxide content Average values for each experiment y=0.0011x y=0.0007x y=0.0003x y=0.0005x y=0.0003x y=0.0001x Consistent with previous work by Moosmüller et al. (2012) and Engelbrecht et al. (2016), PM2.5 dust 18

Imaginary part (k) Relationship between LW CRI and clays, calcite, and quartz content Average values for each experiment Calcite 1-23% by mass Clays 45-92% Quartz 2-42% 19 source regions Niger Patagonia Namibia clays calcite quartz Di Biagio et al., 2017 Wavelength (µm)

Relationship between LW CRI and clays, calcite, and quartz content CALCITE BANDS QUARTZ BANDS CLAYS BANDS 38

Summary Systematic laboratory measurements of the CRI at UV-VIS-IR wavelengths on natural dust aerosol samples representing the global mineralogy of particles smaller than 10 µm The real part of the refractive index don t change regionally, suggesting that a sourceinvariant spectral n can be used in models and remote sensing applications Conversely the imaginary part of CRI (absorption) shows a clear spectral dependence and a regional variability that mostly depends on mineralogy In the UV-VIS: linear with the iron oxide and the total iron content (even better when particles are smaller than 2.5 µm (not shown) At selected bands in the LW: linear with the content of calcite, quartz and clays (more tricky) Same for the UV-VIS single scattering albedo (not shown) 21