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Many previous studies on lacustrine basins in the East African Rift System have directed their attention to climatic controls on contemporary sedimentation or climate change as part of palaeoenvironmental reconstruction. In contrast, this research focuses on the impact of tectonism and volcanism on rift deposition and develops models that help to explain their roles and relative importance. The study focuses on the spatial and temporal variability in bulk sediment geochemistry from a diverse range of modern and ancient rift sediments through an analysis of 519 samples and 50 major and trace elements. The basins examined variously include, or have contained, wetlands and/or shallow to deep, fresh to hypersaline lakes. Substantial spatial variability is documented for Holocene to modern deposits in lakes Turkana, Baringo, Bogoria, Magadi and Malawi. Mio‐Pleistocene sediments in the Central Kenya Rift and Quaternary deposits of the southern Kenya Rift illustrate temporal variability. Tectonic and volcanic controls on geochemical variability are explained in terms of: (i) primary controlling factors (faulting, subsidence, uplift, volcanism, magma evolution and antecedent lithologies and landscapes); (ii) secondary controls (bedrock types, rift shoulder and axis elevations, accommodation space, meteoric and hydrothermal fluids and mantleCO₂); and (iii) response factors (catchment area size, orographic rains, rain shadows, vegetation densities, erosion and weathering rates, and spring/runoff ratios). The models developed have, in turn, important implications for palaeoenvironmental interpretation in other depositional basins.

Modern and ancient lacustrine carbonate build‐ups provide uniquely sensitive sedimentary and geochemical records for understanding the interaction between tectonics, past climates, and local and regional scale basin hydrology. Large (metre to decametre), well‐developed carbonate mounds in the Green River Formation have long been recognized along the margins of an Eocene lake, known as Lake Gosiute. However, their mode of origin and significance with respect to palaeohydrology remain controversial. Here, new sedimentological, Sr isotope data and structural evidence show that significant spring discharge led to the formation of a decametre size complex of shoreline carbonate mounds in the upper Wilkins Peak Member of the Green River Formation at Little Mesa and adjacent areas in the Bridger Basin, Wyoming, USA. Sedimentological evidence indicates that spring discharge was predominantly subaqueous but was, at times, also subaerial, which produced tufa cascades and micro‐rimstone dam structures. The⁸⁷Sr/⁸⁶Sr ratios measured from these subaerial spring deposits are less radiogenic (⁸⁷Sr/⁸⁶Sr = 0.71040 to 0.71101) than contemporaneous palaeolake carbonates (⁸⁷Sr/⁸⁶Sr = 0.71195 to 0.71561) because their parent groundwaters likely interacted with less‐radiogenic Palaeozoic carbonate. Calcite‐cemented sandstone cones and spires (⁸⁷Sr/⁸⁶Sr = 0.71037 to 0.71057) in the Wasatch Formation directly below the spring deposits suggest that groundwaters derived from Palaeozoic carbonates preferentially flowed along thrust faults. These results imply that high spring discharge coincided with lake high stands of the upper Wilkins Peak Member, suggesting that recharge at the north‐west margin of the Bridger Basin contributed to Lake Gosiute’s water budget and lowered the salinity of an underfilled, evaporative lake basin. The findings of this study provide criteria for the recognition of groundwater discharge in palaeolake systems which may lead to the discovery of palaeospring systems in other ancient lake deposits.