Abstract
In order to assess the impact of mineral dust on climate and biogeochemistry, it is paramount to identify the sources of dust emission. In this regard, radiogenic isotopes have recently been used successfully for tracing North African dust provenance and its transport across the tropical Atlantic to the Caribbean. Here we present two time series of radiogenic isotopes (Pb, Sr and Nd) in dusts collected at the Cape Verde Islands and Barbados in order to determine the origin of the dust and examine the seasonality of westerly dust outflow from Northern Africa. Aerosol samples were collected daily during two campaigns - February 2012 (winter) and June-July 2013 (summer) - at the Cape Verde Atmospheric Observatory (CVAO) on the island of Sao Vicente (16.9 degrees N, 24.9 degrees W). A one-year-long time series of aerosols from Barbados (13.16 degrees N, 59.43 degrees W) - a receptor region in the Caribbean - was sampled at a lower, monthly resolution.Our results resolve a seasonal isotopic signal at Cape Verde shown by daily variations, with a larger radiogenic isotope variability in winter compared to that in summer. This summer signature is also observed over Barbados, indicating similar dust provenance at both locations, despite different sampling years. This constrains the isotope fingerprint of Saharan Air Layer (SAL) dust that is well-mixed during its transport. This result provides unequivocal evidence for a permanent, albeit of variable strength, long-range transport of African dust to the Caribbean and is in full agreement with atmospheric models of North African dust emission and transport across the tropical Atlantic in the SAL. The seasonal isotopic variability is related to changes in the dust source areas - mainly the Sahara and Sahel regions - that are active all-year-round, albeit with variable contributions in summer versus the winter months. Our results provide little support for much dust contributed from the Bodele Depression in Chad - the "dustiest" place on Earth - reaching Cape Verde and Barbados during the summer, while contributions during the winter months are likely patchy and minor at most.Importantly, a short-term isotopic excursion is resolved in the Cape Verde winter record during a dust outbreak on 06-08 February 2012. This features a highly radiogenic Pb and Sr and unradiogenic Nd signature, marking a clear shift in dust provenance relative to that of normal days. As the dust storm waned, continuous gradual changes are observed, reflecting mixing and progressive dilution with dust typical of normal days. These inferences from radiogenic isotope tracers are corroborated by both satellite images (CALIPSO and MODIS) and back-trajectory analyses. The radiogenic isotope fingerprinting of these presently-active North African dust sources, and especially the Saharan Air Layer, will prove invaluable in studies of past dust emission from Northern Africa, where imagery and back trajectory analysis are unavailable.