Quantifying the impacts of an exogenous dust input to the soil and stream chemistry of an upland Mediterranean watershed using a reactive transport modeling framework

In upland watersheds, depletion of essential nutrients due to physical erosion and chemical weathering can be compensated by exogenous inputs such as aeolian dust deposition. The presence and chemical composition of exogenous dust arriving in natural environments is commonly analyzed in soil profiles using a suite of geochemical and isotopic tracers. However, it remains an outstanding challenge to describe the impacts of dust on the reaction rates that produce these profiles and how this cascades into ecosystem function and water chemistry. As increasingly intense and episodic periods of drought and aridity are promoted by a warming climate, the role of dust production and deposition in Critical Zone structure and function requires improved modeling techniques to facilitate rigorous quantification and prediction. Here we present a newly developed process-based reactive transport framework by modifying the open source CrunchTope software in order to quantitatively interpret the impacts of dust deposition and solubilization in stream water chemistry, regolith weathering rates, and ecosystem nutrient availability. We describe two simulations: (1) a generic model demonstrating a simplified system in which bedrock uplift and soil erosion occur in tandem with solid phase dust deposition at the land surface; (2) a case study based on a small (0.54 km²) upland Mediterranean watershed located on Mont Lozère in the National Park of Les Cévennes, France. In the absence of an exogenous dust input, long-term field observations of calcium in stream water, rain, bedrock, soil, and plant samples cannot be produced from reactive transport simulations of the weathering profile. By adding a carbonate-rich depositional input consistent with the composition of Saharan dust, both stream water chemistry and elemental mass-transfer coefficients in the soil profile better align with field observations, suggesting that dust has become a significant input to this field site in the last ~10 ka. Over this period, the deposition of exogenous carbonates has introduced far more calcium into the system than what could be supplied by the Ca-poor granitic bedrock. This highly soluble carbonate also limits the reactive potential of infiltrating precipitation, ultimately inhibiting chemical weathering rates and hence the component of elemental export fluxes derived from local bedrock. This is the first demonstration of solid-phase dust deposition incorporated into a multi-component reactive transport framework. Our update to the CrunchTope source code allows us to show how dust incorporation affects geochemical cycling across upland watersheds beyond the prohibitive limitations of simplified steady-state assumptions, a feature that will allow further research of a variety of Critical Zone systems subject to the effects of environmental change scenarios.