Chemical and U–Sr isotopic variations in stream and source waters of the Strengbach watershed (Vosges mountains, France)

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Abstract. This is the first comprehensive study dealing with major and trace element data as well as 87Sr/86Sr isotope and (234U/238U) activity ratios (AR) determined on the totality of springs and brooks of the Strengbach catchment. It shows that the small and more or less monolithic catchment drains different sources and streamlets with very different isotopic and geochemical signatures. Different parameters control the diversity of the source characteristics. Of importance is especially the hydrothermal overprint of the granitic bedrock, which was stronger for the granite from the northern slope; also significant are the different meteoric alteration processes of the bedrock causing the formation of 0.5 to 9 m thick saprolite and above the formation of an up to 1m thick soil system. These processes mainly account for springs and brooks from the northern slope having higher Ca / Na, Mg / Na, and Sr / Na ratios, but lower 87Sr/86Sr isotopic ratios than those from the southern slope. The chemical compositions of the source waters in the Strengbach catchment are only to a small extent the result of alteration of primary bedrock minerals, and rather reflect dissolution/precipitation processes of secondary mineral phases like clay minerals. The (234U/238U) AR, however, are decoupled from the 87Sr/86Sr isotope system, and reflect to some extent the level of altitude of the source and, thus, the degree of alteration of the bedrock. The sources emerging at high altitudes have circulated through already weathered materials (saprolite and fractured bedrock depleted in 234U), implying (234U/238U) AR below 1, which is uncommon for surface waters. Preferential flow paths along constant fractures in the bedrocks might explain the – over time – homogeneous U AR of the different spring waters. However, the geochemical and isotopic variations of stream waters at the outlet of the catchment are controlled by variable contributions of different springs, depending on the hydrological conditions. It appears that the (234U/238U) AR are a very appropriate, important tracer for studying and deciphering the contribution of the different source fluxes at the catchment scale, because this unique geochemical parameter is different for each individual spring and at the same time remains unchanged for each of the springs with changing discharge and fluctuating hydrological conditions. This study further highlights the important impact of different and independent water pathways on fractured granite controlling the different geochemical and isotopic signatures of the waters. Despite the fact that soils and vegetation cover have a great influence on the water cycle balance (evapotranspiration, drainage, runoff), the chemical compositions of waters are strongly modified by processes occurring in deep saprolite and bedrock rather than in soils along the specific water pathways.