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Opis: Abstract. Constraining dust models to understand and quantify the effect of dust upon climate and ecosystems requires comprehensive analyses of the physiochemical properties of dust-emitting sediments in arid regions. Building upon previous studies in the Moroccan Sahara and Iceland, we analyse a diverse set of crusts and aeolian ripples (n=55) from various potential dust-emitting basins within the Mojave Desert, California, USA. Our focus is on characterizing the particle size distribution (PSD), mineralogy, aggregation/cohesion state, and Fe mode of occurrence. Our results show differences in fully and minimally dispersed PSDs, with crusts exhibiting average median diameters of 92 and 37 µm, respectively, compared to aeolian ripples with 226 and 213 µm, respectively. Mineralogical analyses unveiled strong variations between crusts and ripples, with crusts being enriched in phyllosilicates (24 % vs. 7.8 %), carbonates (6.6 % vs. 1.1 %), Na salts (7.3 % vs. 1.1 %), and zeolites (1.2 % and 0.12 %) and ripples being enriched in feldspars (48 % vs. 37 %), quartz (32 % vs. 16 %), and gypsum (4.7 % vs. 3.1 %). The size fractions from crust sediments display a homogeneous mineralogy, whereas those of aeolian ripples display more heterogeneity, mostly due to different particle aggregation. Bulk Fe content analyses indicate higher concentrations in crusts (3.0 ± 1.3 wt %) compared to ripples (1.9 ± 1.1 wt %), with similar proportions in their Fe mode of occurrence: nano-sized Fe oxides and readily exchangeable Fe represent ∼1.6 %, hematite and goethite ∼15 %, magnetite/maghemite ∼2.0 %, and structural Fe in silicates ∼80 % of the total Fe. We identified segregation patterns in the PSD and mineralogy differences in Na salt content within the Mojave basins, which can be explained by sediment transportation dynamics and precipitates due to groundwater table fluctuations described in previous studies in the region. Mojave Desert crusts show similarities with previously sampled crusts in the Moroccan Sahara in terms of the PSD and readily exchangeable Fe yet exhibit substantial differences in mineralogical composition, which should significantly influence the characteristic of the emitted dust particles.
Ključne besede: mineral dust, iron oxides
Objavljeno v RUNG: 29.11.2024; Ogledov: 186; Prenosov: 0
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Opis: Abstract. The chemical and morphological properties of mineral dust aerosols emitted by wind erosion from arid and semi-arid regions influence climate, ocean, and land ecosystems; air quality; and multiple socio-economic sectors. However, there is an incomplete understanding of the emitted dust particle size distribution (PSD) in terms of its constituent minerals that typically result from the fragmentation of soil aggregates during wind erosion. The emitted dust PSD affects the duration of particle transport and thus each mineral's global distribution, along with its specific effect upon climate. This lack of understanding is largely due to the scarcity of relevant in situ measurements in dust sources. To advance our understanding of the physicochemical properties of the emitted dust PSD, we present insights into the elemental composition and morphology of individual dust particles collected during the FRontiers in dust minerAloGical coMposition and its Effects upoN climaTe (FRAGMENT) field campaign in the Moroccan Sahara in September 2019. We analyzed more than 300 000 freshly emitted individual particles by performing offline analysis in the laboratory using scanning electron microscopy (SEM) coupled with energy-dispersive X-ray spectrometry (EDX). Eight major particle-type classes were identified with clay minerals making up the majority of the analyzed particles both by number and mass, followed by quartz, whereas carbonates and feldspar contributed to a lesser extent. We provide an exhaustive analysis of the PSD and potential mixing state of different particle types, focusing largely on iron-rich (Fe oxide-hydroxides) and feldspar particles, which are key to the effects of dust upon radiation and clouds, respectively. Nearly pure or externally mixed Fe oxide-hydroxides are present mostly in diameters smaller than 2 µm, with the highest fraction below 1 µm at about 3.75 % abundance by mass. Fe oxide-hydroxides tend to be increasingly internally mixed with other minerals, especially clays, as particle size increases; i.e., the volume fraction of Fe oxide-hydroxides in aggregates decreases with particle size. Pure (externally mixed) feldspar represented 3.2 % of all the particles by mass, of which we estimated about a 10th to be K-feldspar. The externally mixed total feldspar and K-feldspar abundances are relatively invariant with particle size, in contrast to the increasing abundance of feldspar-like (internally mixed) aggregates with particle size with mass fractions ranging from 5 % to 18 %. We also found that overall the median aspect ratio is rather constant across particle size and mineral groups, although we obtain slightly higher aspect ratios for internally mixed particles. The detailed information on the composition of freshly emitted individual dust particles and quantitative analysis of their mixing state presented here can be used to constrain climate models including mineral species in their representation of the dust cycle.
Ključne besede: mineral dust, Moroccan Sahara, electron microscopy
Objavljeno v RUNG: 13.05.2024; Ogledov: 1052; Prenosov: 8
Celotno besedilo (7,13 MB)
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Ključne besede: PM2.5, aerosol, source apportionment
Objavljeno v RUNG: 10.05.2024; Ogledov: 992; Prenosov: 3
Celotno besedilo (3,62 MB)

Opis: Abstract. Black carbon (BC) is recognized as the most important warming agent among atmospheric aerosol particles. The absorption efficiency of pure BC is rather well-known, nevertheless the mixing of BC with other aerosol particles can enhance the BC light absorption efficiency, thus directly affecting Earth's radiative balance. The effects on climate of the BC absorption enhancement due to the mixing with these aerosols are not yet well constrained because these effects depend on the availability of material for mixing with BC, thus creating regional variations. Here we present the mass absorption cross-section (MAC) and absorption enhancement of BC particles (Eabs), at different wavelengths (from 370 to 880 nm for online measurements and at 637 nm for offline measurements) measured at two sites in the western Mediterranean, namely Barcelona (BCN; urban background) and Montseny (MSY; regional background). The Eabs values ranged between 1.24 and 1.51 at the urban station, depending on the season and wavelength used as well as on the pure BC MAC used as a reference. The largest contribution to Eabs was due to the internal mixing of BC particles with other aerosol compounds, on average between a 91 % and a 100 % at 370 and 880 nm, respectively. Additionally, 14.5 % and 4.6 % of the total enhancement at the short ultraviolet (UV) wavelength (370 nm) was due to externally mixed brown carbon (BrC) particles during the cold and the warm period, respectively. On average, at the MSY station, a higher Eabs value was observed (1.83 at 637 nm) compared to BCN (1.37 at 637 nm), which was associated with the higher fraction of organic aerosols (OA) available for BC coating at the regional station, as denoted by the higher organic carbon to elemental carbon (OC:EC) ratio observed at MSY compared to BCN. At both BCN and MSY, Eabs showed an exponential increase with the amount of non-refractory (NR) material available for coating (RNR-PM). The Eabs at 637 nm at the MSY regional station reached values up to 3 during episodes with high RNR-PM, whereas in BCN, Eabs kept values lower than 2 due to the lower relative amount of coating materials measured at BCN compared to MSY. The main sources of OA influencing Eabs throughout the year were hydrocarbon OA (HOA) and cooking-related OA (COA), i.e. primary OA (POA) from traffic and cooking emissions, respectively, at both 370 and 880 nm. At the short UV wavelength (370 nm), a strong contribution to Eabs from biomass burning OA (BBOA) and less oxidized oxygenated OA (LO-OOA) sources was observed in the colder period. Moreover, we found an increase of Eabs with the ageing state of the particles, especially during the colder period. This increase of Eabs with particle ageing was associated with a larger relative amount of secondary OA (SOA) compared to POA. The availability of a long dataset at both stations from offline measurements enabled a decade-long trend analysis of Eabs at 637 nm, that showed statistically significant (s.s.) positive trends of Eabs during the warmer months at the MSY station. This s.s. positive trend in MSY mirrored the observed increase of the OC:EC ratio over time. Moreover, in BCN during the COVID-19 lockdown period in spring 2020 we observed a sharp increase of Eabs due to the observed sharp increase of the OC:EC ratio. Our results show similar values of Eabs to those found in the literature for similar background stations.
Ključne besede: black carbomn, coating, organic aerosol, light absorption
Objavljeno v RUNG: 10.05.2024; Ogledov: 1016; Prenosov: 5
Celotno besedilo (2,74 MB)
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Opis: The effects of desert dust upon climate and ecosystems depend strongly on its particle size and size-resolved mineralogical composition. However, there is very limited quantitative knowledge on the particle size and composition of the parent sediments along with their variability within dust-source regions, particularly in dust emission hotspots. The lower Drâa Valley, an inland drainage basin and dust hotspot region located in the Moroccan Sahara, was chosen for a comprehensive analysis of sediment particle size and mineralogy. Different sediment type samples (n= 42) were collected, including paleo-sediments, paved surfaces, crusts, and dunes, and analysed for particle-size distribution (minimally and fully dispersed samples) and mineralogy. Furthermore, Fe sequential wet extraction was carried out to characterise the modes of occurrence of Fe, including Fe in Fe (oxyhydr)oxides, mainly from goethite and hematite, which are key to dust radiative effects; the poorly crystalline pool of Fe (readily exchangeable ionic Fe and Fe in nano-Fe oxides), relevant to dust impacts upon ocean biogeochemistry; and structural Fe. Results yield a conceptual model where both particle size and mineralogy are segregated by transport and deposition of sediments during runoff of water across the basin and by the precipitation of salts, which causes a sedimentary fractionation. The proportion of coarser particles enriched in quartz is higher in the highlands, while that of finer particles rich in clay, carbonates, and Fe oxides is higher in the lowland dust emission hotspots. There, when water ponds and evaporates, secondary carbonates and salts precipitate, and the clays are enriched in readily exchangeable ionic Fe, due to sorption of dissolved Fe by illite. The results differ from currently available mineralogical atlases and highlight the need for observationally constrained global high-resolution mineralogical data for mineral-speciated dust modelling. The dataset obtained represents an important resource for future evaluation of surface mineralogy retrievals from spaceborne spectroscopy.
Ključne besede: mineral dust, aerosols, geology
Objavljeno v RUNG: 12.01.2024; Ogledov: 1918; Prenosov: 5
Celotno besedilo (7,63 MB)
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