Geochemical signatures of paleodepositional and diagenetic environments: A STEM/AEM study of authigenic clay minerals from an arid rift basin, Olduvai Gorge, Tanzania

Olduvai Gorge, Tanzania (East African Rift) exposes a 100 m thick Plio-Pleistocene sequence of dominantly volcaniclastic sediments deposited in a 50 km wide closed basin containing a playa lake. A scanning transmission electron and analytical electron microscopy (STEM/AEM) study of authigenic clay minerals in sediments from representative depositional environments in the basin (pyroclastic fan, fluvial plain, wetland, lake margin and lake basin) was undertaken to determine whether clay compositions and textures could provide unique geochemical fingerprints characteristic of source area (Plio-Pleistocene trachytic volcanics vs. Precambrian quartzose-feldspathic basement) or paleoenvironmental conditions. Our study shows that compositional signatures obtained by clay minerals during early pedogenesis are inherited from their parent source rocks. Sediments sourced from volcanics contain highly disordered, dioctahedral smectite. Those sourced from Precambrian basement are similar, but are more Al-rich. Subsequent neoformation in the pedogenic (soil) or diagenetic (lake-margin, lake) environments results in the modification of original clay mineralogy, compositions, and textures, and unique paleoenvironmental fingerprints are acquired. Soils developed on the distal pyroclastic fan contain smectite with more Fe(III) and Mg than smectite from the proximal pyroclastic fan sediments. A trend of decreasing Al and increasing Mg content occurs in smectite compositions in samples from the fluvial to lake-margin and lake environments as a result of partial replacement of original dioctahedral Al-rich smectite by neoformed trioctahedral Mg-rich smectite (stevensite). Neoformed celadonite replaces smectite in the most saline lake sediments. The STEM/AEM data collectively indicate that diagenesis in the saline-alkaline lake results in the replacement of Al-rich dioctahedral smectite by Mg-rich trioctahedral smectite (stevensite) and Mg- and Al-rich celadonite. Thus, determination of clay mineral compositions at a basin-wide scale provides a useful tool for interpreting the spatial distribution of depositional and diagenetic environments.