The role of vegetation in setting strontium stable isotope ratios in the Critical Zone

At Earth's surface the stable isotope ratio of strontium (88Sr/86Sr) is predominantly set by biological uptake of Sr and its storage in plant litter. This conclusion was reached from a stable isotope mass balance that was independently validated by direct determination of elemental fluxes between the Critical Zone compartments (rock, soil, vegetation, and stream water) of three field sites located in the Swiss Alps, the US Sierra Nevada, and the tropical highlands of Sri Lanka. These sites cover a gradient in erosion rates, which is inversely related to the residence time of solids in the Critical Zone thereby constituting an “erodosequence”. For eroding landscapes, previous stable isotope models predicted that isotope ratios are set by the rate at which secondary solids form during the conversion of rock to regolith. Counter to this expectation we found that, after release from primary minerals, Sr is partitioned into one fraction taken up by plants and the remainder into dissolved Sr flux. The formation of secondary weathering products such as clays and oxides plays a subordinate role in determining the Sr budget. A Sr isotope fractionation factor for biological uptake was determined for each of the three ecosystems from the average Sr stable isotope composition in bulk plants and its dissolved counterpart in stream water. This fractionation factors range from ca. −0.3 ‰ for the Alps and Sierra Nevada to ∼0 ‰ for the tropical Sri Lanka site. That these isotope fingerprints caused by biologic uptake are preserved means that more Sr was physically removed in plant litter than recycled. Such Sr removal in plant litter appears to be strongest at the slowly-eroding site, whereas the dissolved Sr export by streams is highest at the site with the fastest erosion rate. There, all Sr taken up by plants is returned from litter back into solution. The site with short residence time of solids is the only one at which parent material and dissolved export differ in their Sr isotope composition. Our study shows that the behavior of Sr in the Critical Zone is in stark contrast to that of metals of which the isotope fractionation is not affected by biological uptake (for example lithium, mostly set by formation of secondary solids) or affected by both secondary solid formation and biological uptake (for example silicon). Strontium stable isotope signatures offer the new opportunity to quantify nutrient cycling in the Critical Zone as a function of environmental and ecological parameters.