Sandrine Caquineau

Saharan dust: Clay ratio as a relevant tracer to assess the origin of soil-derived aerosols

The aim of this study is to find a tracer allowing retrieval of the regional origin of mineral dust for Saharan aerosols transported over the North Atlantic Ocean. Because of physical and chemical fractionation processes occurring at the soil-atmosphere interface and during the atmospheric transport of dust, clay mineral species seem to be the best candidate. This study shows that the ratio between relative abundance of illite and kaolinite (I/K ratio) is the parameter that is the most sensitive to the regional origin of Saharan dust collected on Sal Island (Cape Verde). By comparing the I/K ratio measured in dust emitted from the same Saharan source and collected along its transport both on Sal Island and Barbados (Caribbean Sea), we show that this ratio seems to remain unchanged after long-range transport.

CHARACTERISTICS OF CLAY MINERALS IN ASIAN DUST AND THEIR ENVIRONMENTAL SIGNIFICANCE

The objectives of this research were to characterise the clay minerals composition of soil-derived dust in Northern China and to set up a mineralogical signature to trace their origin. Mineral composition of aerosol particles was investigated at Aksu, Dunhuang, Yulin, Tongliao and Changwu during an intensive field campaign period of ACE-Asia. The results show that the kaolinite (K) to chlorite (C) ratio is sensitive to the regional origin of Asian dust. Western source areas (represented by Aksu) displayed the lowest K/C ratio of 0.3 (average), while it was found to increase up to 0.70 (average) upon moving towards northern source areas (represented by Yulin). By studying transported dust in a deposition area representative of the Chinese Loess Plateau, the usefulness of the K/C ratio, when associated with back air-mass trajectories, was found to lie in revealing the origin of the dust. Comparison of the mineralogical data between Asian dust and Sahara dust, shows that the K/C ratio is also an effective signature to identify the source areas on a hemisphere scale.

Dominance of goethite over hematite in iron oxides of mineral dust from Western Africa: Quantitative partitioning by X‐ray absorption spectroscopy

This paper reports on the X-ray absorption analysis of samples of mineral dust emitted from or transported to Western Africa. We found that iron oxides account, by mass, for 38% to 72% of the total elemental iron. They are composed of minerals in the Fe(III) oxidation state: goethite (FeO·OH) and hematite (Fe2O3). The apparent fraction of iron oxide attributed to goethite is higher than hematite regardless of the source region from which the dust originated. The goethite percent content of iron oxides is in the range 52–78% (by mass), the highest values being measured for dust originating in the Sahel. The limited number of samples analyzed and the sample-to-sample variability prevent us from concluding firmly on the regional variability of the goethite-to-hematite ratio. Based on the experimental data on mineralogical composition and on concurrent measurements of the number size distribution, the optical properties of mineral dust have been calculated in a Mie approximation for homogeneous spherical particles. At 550 nm, the single-scattering albedo ω0 ranges between 0.89 and 0.93, the asymmetry factor g ranges between 0.76 and 0.8 and the mass extinction efficiency kext varies between 0.5 and 1.1 m2 g−1; these values are all in the range of those from independent direct measurements. Neglecting the partitioning between hematite and goethite and the assimilation of iron oxides by hematite, as it is often done with models, lowers the single-scattering albedo and increases the asymmetry factor in the UV-visible spectral region below 550 nm. The mass extinction efficiency is insensitive to the nature of the iron oxides but rather responds to variations in the number size distribution. The mineralogy of iron oxides should therefore be taken into account when assessing the effect of mineral dust on climate and atmospheric chemistry, in particular via interactions involving photolysis.

Long‐range transport across the Atlantic in summertime does not enhance the hygroscopicity of African mineral dust

We present the first direct evidence that the hygroscopic properties of super micron (>1 µm) African dust particles did not change despite undergoing long-range transport across the Atlantic toward the Caribbean. Concurrent measurements of chemical composition show that most of mineral dust was chemically unprocessed and externally mixed. A minor portion of mineral dust was internally mixed with sulfate and chloride (~13–24% by number) or aggregated with sea-salt particles (~3–6%). Only dust particles aggregated with sea salt showed significant hygroscopic growth above 75% relative humidity (RH), resulting in a decrease in extinction mass efficiency by up to a factor 2.2. All other dust particles did not take up significant amounts of water when exposed to up to 94% RH. These results demonstrate that the direct radiative effect of African dust in this region remained independent of RH and an external mixing state could be considered for evaluating the climate effects of dust.

Palaeohydrological controls on sedimentary organic matter in an Amazon floodplain lake, Lake Maracá (Brazil) during the late Holocene

In order to understand the impact of hydrological changes of the Amazon River on sedimentary organic matter (OM) composition in Amazonian floodplain lakes, three sediment cores were collected from Lake Maracá (eastern Amazonia) along a transect from the Amazon River main channel to inland. The cores were dated with 14C accelerator mass spectrometry (AMS) and studied by x-ray, mineralogical composition, total organic carbon (TOC) and total nitrogen (TN) contents, stable isotopic composition of TOC and TN (δ13COC and δ15N) and glycerol dialkyl glycerol tetraether (GDGT) distributions. Two distinctive sedimentary depositional phases were identified based on the mineralogical composition and the geochemical characteristics of sedimentary OM. During the early–mid Holocene (~13,000–3200 cal. yr BP), low values of TOC followed by a break in sedimentation suggest a complete drying of the lake caused by drier climatic conditions. Between 3600 and 3200 cal. yr BP, this lake received a reduced influence of the Amazon River main stem. This induced a predominant deposition of C3-plant-derived OM supplied by surface erosion and runoff of acidic soil. A distinct connection of Lake Maracá to the Amazon River began after 3200 cal. yr BP and became permanently established, with its modern characteristics, at 1880 cal. yr BP. This change provoked an increased contribution of phytoplankton and semi-aquatic C4 macrophytes as well as C3 plant derived more alkaline soil OM to the sedimentary OM pool. Consequently, our study demonstrates that the source of sedimentary OM in the Amazon floodplain lakes was strongly linked to the Amazon River hydrodynamics during the late Holocene.

Quantitative study of the mineralogical composition of mineral dust aerosols by X-ray diffraction

Mineral dust aerosols, produced by wind erosion in arid regions and semi-arid surfaces, are important components of the atmosphere that affect the Earth radiative budget, atmospheric chemistry and biogeochemical cycles. Dust aerosol particles are composed of a complex mixture of various minerals, mainly clays, calcite, quartz, feldspars and iron oxides. The nature and the relative abundance of the minerals are key parameters to evaluate mineral dust environmental impacts. Strong limitations remain to quantify the mineralogical composition of dust particles, mainly due to the low mass of in-situ collected dust particle samples. In this study, an analytical method and X-Ray Diffraction (XRD) measurements are presented to quantify the mineralogical composition of low mass aerosol particle samples. The method is applied on reference minerals (illite, kaolinite and palygorskite) commonly present in desert dust aerosols, as well as on lab-generated dust aerosols from desert soils. XRD measurements of theses samples in rotation in a glass capillary are combined with the Rietveld refinement method. The results obtained are repeatable and confronted to theoretical values given in the literature for the reference minerals. This method allows us to quantify the mineralogical composition of low mass dust mineral samples with an unprecedented accuracy.