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Chemical sediments from the Early Eocene Green River Formation can be used for assessing hydroclimate and basin evolution during their deposition. The Wilkins Peak Member (WPM) of the Green River Formation contains a relatively continuous record of perennial closed-basin saline lake deposition in the Bridger Basin, southwest Wyoming, from approximately 51.6 to 49.8 Ma. The volumes and paragenesis of authigenic chemical sediments in the WPM are intrinsically related to the chemical evolution of basin brines. The geographic distribution of those chemical sediments across the Bridger Basin relates to the syn- and post-depositional tectonic history of the basin. In this study, we integrated thermodynamic modeling of chemical evolution of lake brines with chemostratigraphic and lithostratigraphic interpretations of the basin-center Solvay S-34-1 core to evaluate physical and chemical changes to and within ancient Lake Gosiute during the Early Eocene. Fine-scale X-ray fluorescence (XRF) scanning along the length of the core provides a high-resolution chemical stratigraphy of the WPM. Thermodynamic modeling of the evaporation of hypothetical inflow waters and lake brines yield predicted sequences of evaporite minerals, allowing estimation of the salinities and evaporated volumes of water required to reach saturation with respect to observed mineral deposits from the basin. The spatial distributions of bedded evaporites allow us to investigate tectonic changes to the basin during and after the deposition of the WPM. Here, we integrate these data to interpret changes in lake-level, salinity, and hydroclimate of ancient Lake Gosiute during the Early Eocene.