Feedback mechanisms between precipitation and dissolution reactions across randomly heterogeneous conductivity fields

Our study investigates interplays between dissolution, precipitation, and transport processes taking place across randomly heterogeneous conductivity domains and the ensuing spatial distribution of preferential pathways. We do so by relying on a collection of computational analyses of reactive transport performed in two-dimensional systems where the (natural) logarithm of conductivity is characterized by various degrees of spatial heterogeneity. Our results document that precipitation and dissolution jointly take place in the system, the latter mainly occurring along preferential flowpaths associated with the conductivity field, the former being observed at locations close to and clearly separated from these. High conductivity values associated with the preferential flowpaths tend to further increase in time, giving rise to a self-sustained feedback between transport and reaction processes. The clear separation between regions where dissolution or precipitation takes place is imprinted onto the sample distributions of conductivity which tend to become visibly left skewed with time (with the appearance of a bimodal behavior at some times). The link between conductivity changes and reaction-driven processes promotes the emergence of non-Fickian effective transport features. The latter can be captured through a continuous time random walk model where solute travel times are approximated with a truncated power law probability distribution. The parameters of such a model shift towards values associated with increasingly high non-Fickian effective transport behavior as time progresses.

Which role do preferential flowpaths and fractures play in the subsurface reactivity in heterogeneous aquifers?

<p>The underground fracture pattern, which results from tectonic, climatic and biological stresses, drives water storage dynamic and nutrient cycling in the deep critical zone. Despite a gradual decrease of fracture density with depth, the fracture network is strongly heterogeneous and anisotropic, resulting in a complex pathway distribution with variable hydraulic conductivities. High celerities occurring in preferential flowpaths govern the dynamic response of discharge flows to extreme recharge events. However, the role of preferential flowpaths in transporting fresh meteoritic water and biota remains poorly studied, while the delivery of meteoritic reactants is crucial to initiate underground chemical reactions.</p><p>Here, we study a fractured aquifer in a crystalline catchment located in Brittany (Guidel, France) to investigate the link between depth, water transit time and subsurface reactivity in fractures. Oxygen is used as a tracer of fresh water inputs because its availability has a tremendous impact on oxidation-driven reactions such as weathering processes and microbial activity. We performed vertically sampling of fracture fluid with an inflatable packer capable of isolating fractures in an artesian well located in the discharge chemically-reduced zone of the aquifer. Major ions, dissolved reactive gases, dissolved anthropogenic gases, stable isotopes (O, Sr and Si) and microbial diversity were analysed on five fracture waters sampled at depth between 20 and 55 m. Significant differences have been observed between fractures and younger and more oxygenated waters were found intermittently in fractures at 47 and 54m, with dissolved oxygen concentrations ranging between 0.1 and 0.5 mg/L. The penetration of oxygen in deep fractures reveals either a rapid transport of oxygen or a low consumption of oxygen in preferential flowpaths. These hypotheses are tested with a Discrete Fracture Network model, where first-order reaction rates have been implemented, and the temporal dynamic of oxygen is assessed and linked to water transit time in fractures. We investigate the concept of transit time and water-rock contact time and discuss the relevance of mean transit time to evaluate subsurface reactivity.</p><p>Preferential flowpaths thus not only make fractured aquifers more dynamic but can also, under extreme recharge conditions, efficiently transport fresh water at high depth. The advective-dominant transport of oxygen through artery-like fractures could have a significant impact on short term microbial activity and the associated nutrient cycling but also on long term weathering front propagation.</p>

Hydrologic Flowpath Development Varies by Aspect during Spring Snowmelt in Complex Subalpine Terrain

In many mountainous regions around the world, snow and soil moisture are key components of the hydrologic cycle. Preferential flowpaths of snowmelt water through snow have been known to occur for years with few studies observing the effect on soil moisture. In this study, statistical analysis of the topographical and hydrological controls on the spatio-temporal variability of snow water equivalent and soil moisture during snowmelt was undertaken at a subalpine forested setting with north, south, and flat aspects as a seasonally persistent snowpack melts. We investigated if preferential flowpaths in snow can be observed and the effect on soil moisture through measurements of snow water equivalent and near surface soil moisture in addition to observing how SWE and near surface soil moisture vary on hillslopes relative to the toes of hillslopes and flat areas. We then compared snowmelt infiltration beyond the near surface soil between flat and sloping terrain during the entire snowmelt season using soil moisture sensor profiles. This study was conducted during varying snowmelt seasons representing above normal, relatively normal, and below normal snow seasons in northern Colorado. Evidence is presented of preferential meltwater flowpaths at the snow-soil interface on the north facing slope with the effects observed in changes in SWE and infiltration into the soil at 20 cm depth; less association is observed in the near surface soil moisture (top 7 cm). We present a conceptualization of the meltwater flowpaths that develop based on slope aspect and soil properties. The resulting flowpaths are shown to increase the snow water equivalent by as much as 170 % at the base of a north facing hillslope. Results from this study show that snow acts as an extension of the vadose zone during spring snowmelt and future hydrologic investigations will benefit from studying the snow and soil together.

Identification of runoff formation with two dyes in a mid-latitude mountain headwater

Subsurface flow in Peat Bog areas and its role in the hydrological cycle has garnered increased attention as water scarcity and floods have increased due to a changing climate. In order to further probe the mechanisms in Peat Bog areas and contextualize them at the catchment scale, this experimental study identifies runoff formation at two opposite hillslopes in a peaty mountain headwater; a slope with organic Peat soils and a shallow phreatic zone (0.5 m below surface) and a slope with mineral Podzol soils and no detectable groundwater (> 2 m below surface). Similarities and differences in infiltration, percolation, and preferential flowpaths between both hillslopes could be identified by sprinkling experiments with Brilliant Blue and Sodium-Fluorescein. To our knowledge, this is the first time these two dyes have been compared in their ability to stain preferential flowpaths in soils. Dye-stained soil profiles within and downstream of the sprinkling areas were excavated parallel (lateral profiles) and perpendicular (frontal profiles) to the slopes' gradients. That way preferential flow patterns in the soil could be clearly identified. The results show that biomat flow, shallow subsurface flow in the organic topsoil layer, occurred at both hillslopes, however at the Peat Bog hillslope it was significantly more prominent. The dye solutions infiltrated into the soil and continued either as lateral subsurface pipeflow in the case of the Peat Bog, or percolated vertically towards the bedrock in the case of the Podzol. This study provides evidence that subsurface pipeflow, lateral preferential flow along decomposed tree roots or logs in the unsaturated zone, is a major runoff formation process at the Peat Bog hillslope and in the adjacent riparian zone.

Numerical Simulation of Contaminant Dynamic Transfer in Dual-Domain Model

Preferential flowpaths (PFP) causes highly heterogeneity of soil. In this study a preferential flowpaths generalized model has been established, based on dual-domain model (DDM) which reflects contaminant transport and the dynamic transfer between mobile and immobile domains, quantitatively analyses the contaminant mass transfer in pore scale at three different conditions. Besides, define relative hydraulic conductivity reflect the impact of PFP physical parameters, results show that it can affect the contaminant transport form and the distribution of contaminant concentration.

Unstable Flow in Repellent and Sub-critically Repellent Soils: Theory and Management Implications

Water repellency causes unstable wetting fronts that result in water moving in preferential flowpaths through homogeneous soils as well in structured soils where macropores enhance the preferential flow pattern. Water repellency is typically associated with extended water ponding on the soil surface, but we have found that repellency is important even before the water ponds. Preferential flow fingers can form under conditions where the contact angle is less than 90o, but greater than 0o. This means that even when the soil is considered wettable (i.e., immediate penetration of water), water distribution in the soil profile can be significantly non-uniform. Our work concentrated on various aspects of this subject, with an emphasis on visualizing water and colloid flow in soil, characterizing mathematically the important processes that affect water distribution, and defining the chemical components that are important for determining contact angle. Five papers have been published to date from this research, and there are a number of papers in various stages of preparation.