The Li-rich brine contained within the halite body of the Salar de Atacama is uncommon for two reasons: First, it has an exceptionally high Li concentration, even compared to other closed basins in the Li triangle of South America; and second, it is widespread within the halite nucleus and not restricted to a localized area. This study focusses on the southern half of the salar where Li production occurs and draws comparisons with its northern neighboring basin through which the Loa river flows. Concentration and isotope data for water inflowing to this part of the salar were obtained from surface inflow as well as wells located within the alluvial fans on its eastern margin. Lithium varies between 0.2 and 20 mg/L before reaching the salar where small amounts of the brine and or salts that precipitated from it can increase its concentration up to 400 mg/L or higher. The δ⁷Li of the inflow water varies between +4.9‰ and +11.2‰ and increases to +12.6‰ within the salar margin, consistent with salar brine based on reported measurements. Boron isotopes indicate that it is unlikely that solutes are derived from sedimentary evaporites or mineral cements, unlike the situation in the adjacent Loa basin. Water that flows through an aquifer laterally confined by a basement block and a line of volcanoes has a notably higher δ⁷Li than other inflow water, around +9‰, and increasing to +10.5‰. δ⁷Li values are overall higher than were measured in the adjacent Loa basin, indicating that here the water–rock reactions for Li are more evolved due to longer residence times. Lithium concentrations increased with sodium and chloride, but sedimentary evaporites are shown to be unimportant from δ¹¹B. This is accounted for two ways: evaporated saline inflow leaks from higher elevation basins and inflows are partly derived from or modified by active volcanic systems. Active and dormant volcanoes plus the massive Altiplano–Puna magmatic body are important as heat sources, which enhance water–rock reactions. The large topographic difference between the mean elevation of Altiplano on which these volcanoes sit and the salar surface allows hydrothermal fluids, which would otherwise stay deep below the surface under the modern arc, to uplift at the salar.

Prior to the 24-26 March 2015 extreme precipitation event that impacted northern Chile, the scenarios for Pleistocene and Holocene wetter paleoclimate intervals in the hyperarid core of the Atacama Desert had been attributed to eastern or southwestern moisture sources. The March 2015 precipitation event offered the first modern opportunity to evaluate a major regional precipitation event relative to those hypothetical paleoclimate scenarios. It was the first opportunity to determine the 18O and 2H composition of a major precipitation event that might eventually be preserved in geological materials. The driver for the March 2015 event was a synoptic-scale weather system, a cutoff cold upper-level low system that traversed the Pacific Ocean at a time of unusually warm temperatures of Pacific surface water. Ground-based precipitation data, stable isotopes in precipitation and river samples, NCEP/NCAR reanalysis atmospheric data and air mass tracking are utilized to connect the Earth surface processes to atmospheric conditions. The δ18O and δ2H of the precipitation and ephemeral rivers were significantly heavier than the rain, snow and ephemeral rivers fed by more frequent but less voluminous precipitation events registered prior to March 2015. Consistent with the atmospheric analyses, the rain isotopic compositions are typical of a water vapor whose source was at more equatorial latitudes of the Pacific and which moved southward. The late March 2015 system was an unforeseen scenario even for El Niño Pacific ocean conditions. Furthermore, the late summer season warmth led to greater potential for erosion and sediment transport than typical of more common moderate precipitation scenarios which usually include widely distributed snow. A comparison of the March 2015 scenario to the spatial distribution of wetter paleoclimate intervals leads to the hypothesis that the March 2015 scenario likely better fits some parts of the paleoclimate record of the continental interior hyperarid Atacama Desert than do the eastern or southwestern moisture source paleoclimate scenarios deduced previously.