Chemical sediments of the lacustrine Wilkins Peak Member of the Eocene Green River Formation potentially preserve detailed paleoclimate information relating to the conditions of their formation and preservation within the lake basin during the Early Eocene Climatic Optimum. The Green River Formation comprises the world's largest sodium-carbonate evaporite deposit in the form of trona (Na2CO3⋅NaHCO3⋅2H2O) in the Bridger Basin and nahcolite (NaHCO3) in the neighboring Piceance Creek Basin. Modern analogues suggest that these minerals necessitate the existence of an alkaline source water. Detrital provenance geochronometers suggest that the most likely source for volcanic waters to the Greater Green River Basin is the Colorado Mineral Belt, connected to the basin via the Aspen paleoriver.Here, we test the hypothesis that magmatic waters from the Colorado Mineral Belt could have supplied the Greater Green River Basin with the alkalinity needed to precipitate sodium-carbonate evaporites that are preserved in the Wilkins Peak Member by numerically simulating the evaporation of modern soda spring waters from northwestern Colorado at various temperature and atmospheric pCO2 conditions. The resulting simulated evaporite sequence is then compared to the mineralogy and textures preserved within the Wilkins Peak Member. Simulated evaporation of Steamboat Springs and Mineral Spring waters produce a close match to core observations and mineralogy. These simulations provide constraints on the salinities at which various minerals precipitated in the Wilkins Peak Member as well as insights into the regional temperature (>15 °C for gaylussite and trona; >27° for pirssonite and trona) and pCO2 conditions (<1200 ppm for gaylussite and trona) during the Early Eocene Climatic Optimum.