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[1] To investigate the timescales of regolith formation on hillslopes with contrasting topographic aspect, we measured U-series isotopes in regolith profiles from two hillslopes (north facing versus south facing) within the east-west trending Shale Hills catchment in Pennsylvania. This catchment is developed entirely on the Fe-rich, Silurian Rose Hill gray shale. Hillslopes exhibit a topographic asymmetry: The north-facing hillslope has an average slope gradient of~20, slightly steeper than the south-facing hillslope (~15 ). The regolith samples display significant U-series disequilibrium resulting from shale weathering. Based on the U-series data, the rates of regolith production on the two ridgetops are indistinguishable (40 AE 22 versus 45 AE 12 m/Ma). However, when downslope positions are compared, the regolith profiles on the south-facing hillslope are characterized by faster regolith production rates (50 AE 15 to 52 AE 15 m/Ma) and shorter durations of chemical weathering (12 AE 3 to 16 AE 5 ka) than those on the north-facing hillslope (17 AE 14 to 18 AE 13 m/Ma and 39 AE 20 to 43 AE 20 ka). The south-facing hillslope is also characterized by faster chemical weathering rates inferred from major element chemistry, despite lower extents of chemical depletion. These results are consistent with the influence of aspect on regolith formation at Shale Hills; we hypothesize that aspect affects such variables as temperature, moisture content, and evapotranspiration in the regolith zone, causing faster chemical weathering and regolith formation rates on the south-facing side of the catchment. The difference in microclimate between these two hillslopes is inferred to have been especially significant during the periglacial period that occurred at Shale Hills at least~15 ka before present. At that time, the erosion rates may also have been different from those observed today, perhaps denuding the south-facing hillslope of regolith but not quite stripping the north-facing hillslope. An analysis of hillslope evolution and response timescales with a linear mass transport model shows that the current landscape at Shale Hills is not in geomorphologic steady state (i.e., so-called dynamic equilibrium) but rather is likely still responding to the climate shift from the Holocene periglacial to the modern, temperate conditions.

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Research activity associated with various observations at the Strengbach catchment in the Vosges Massif (880-1150 m) addresses many questions in the domains of hydrology and geochemistry. The catchment is the observation and experimental site of the Observatoire Hydro-Géochimique de l'Environnement appointed by the Centre National de la Recherche Scientifique. It also belongs to the research facilities that form the French Network of Critical Zone Observatories (OZCAR), which supports a network of critical zone observatories. The catchment is small (0.8 km 2 ) with steep slopes (20-30%) on granitic bedrock that mainly allow for forestry (spruce and beech stands) as the main land cover. Meteorological, hydrological, and geochemical data have been monitored since 1986. The first studies conducted were dedicated to the elucidation of acid rain effects on forest ecosystems and particularly on forest decline. Multidisciplinary research studies conducted on the Strengbach catchment enable exploration of the following issues: (i) hydrological functioning at the scale of a small catchment and questions regarding the evolution and preservation of the water resources in mountainous environments (stock, recharge, infiltration, and water pathways), (ii) exchange processes observed at the soil-plant-atmosphere continuum and in particular weathering processes and the evolution of soil mineral fertility (Ca, Mg, K, P), (iii) processes responsible for the export of water and for associated fluxes (dissolved chemicals, suspended materials, bed loads) and their dynamic at the outlet, and (iv) responses of the ecosystems to environmental disturbances (acid rain, forest management, and climate change) and their current and future modeling. University of Strasbourg), is well suited for addressing such issues owing to (i) a long-term dataset available for the area (from 1985;Probst et al., 1987), (ii) the availability of field equipment and monitoring devices, and (iii) numerous scientific studies that have been performed on the area. Research performed at this catchment, which is located in the Vosges Mountains in northeastern France, has focused on the evaluation of water and soil resources in relation to climatic changes (i.e., rainfall regimes and atmospheric chemistry trends) and anthropogenic patterns (e.g., forest management and acid precipitation) occurring in this moderate-altitude mountainous region.Usually, in this type of ecosystem, water is scarce and not evenly distributed, and stocks may rapidly vary over time. In addition, although wood production is an economically important activity in these regions, soil degradation (e.g., from acidification and nutrient depletion) modifies soil fertility features and thus affects the development of forests.The scientific objective of the OHGE is to develop a detailed understanding of water transport processes and of related chemical fluxes (including nutrients and contaminants) through the critical zone extending from the near atmosphere to the near subsurface. The main purposes of...

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.

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A 2 m-thick spheroidal weathering profile, developed on a quartz diorite in the Rio Icacos watershed (Luquillo Mountains, eastern Puerto Rico), was analyzed for major and trace element concentrations, Sr and Nd isotopic ratios and U-series nuclides (238U-234U-230Th-226Ra). In this profile a 40 cm thick soil horizon is overlying a 150 cm thick saprolite which is separated from the basal corestone by a ∼40 cm thick rindlet zone. The Sr and Nd isotopic variations along the whole profile imply that, in addition to geochemical fractionations associated to water-rock interactions, the geochemical budget of the profile is influenced by a significant accretion of atmospheric dusts. The mineralogical and geochemical variations along the profile also confirm that the weathering front does not progress continuously from the top to the base of the profile. The upper part of the profile is probably associated with a different weathering system (lateral weathering of upper corestones) than the lower part, which consists of the basal corestone, the associated rindlet system and the saprolite in contact with these rindlets. Consequently, the determination of weathering rates from 238U-234U-230Th-226Ra disequilibrium in a series of samples collected along a vertical depth profile can only be attempted for samples collected in the lower part of the profile, i.e. the rindlet zone and the lower saprolite. Similar propagation rates were derived for the rindlet system and the saprolite by using classical models involving loss and gain processes for all nuclides to interpret the variation of U-series nuclides in the rindlet-saprolite subsystem. The consistency of these weathering rates with average weathering and erosion rates derived via other methods for the whole watershed provides a new and independent argument that, in the Rio Icacos watershed, the weathering system has reached a geomorphologic steady-state. Our study also indicates that even in environments with differential weathering, such as observed for the Puerto Rico site, the radioactive disequilibrium between the nuclides of a single radioactive series (here 238U-234U-230Th-226Ra) can still be interpreted in terms of a simplified scenario of congruent weathering. Incidentally, the U-Th-Ra disequilibrium in the corestone samples confirms that the outermost part of the corestone is already weathered.