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  1. Abstract

    To investigate how bedrock transforms to soil, we mapped the topography of the interface demarcating onset of weathering under an east‐west trending shale watershed in the Valley and Ridge province in the USA Using wave equation travel‐time tomography from a seismic array of >4,000 geophones, we obtained a 3D P‐wave velocity (Vp) model that resolves structures ∼20 m below land surface (mbls). The depth of mobile soil and the onset of dissolution of chlorite roughly match Vp = 600 m/s and Vp = 2,700 m/s, respectively. Chlorite dissolution initiates porosity growth in the shale matrix. Depth to the 2,700 m/s contour is greater under the N‐ as compared to S‐facing hillslopes and under sub‐planar as compared to concave‐up land surfaces. Broadly, the geometries of the ‘soil’ and ‘chlorite’ Vp contours are consistent with the calculated potential for shear fracture opening under weak regional compression. However, this calculated fracture potential does not consistently explain observations related to N‐ versus S‐facing aspect nor fracture density observed by borehole televiewer. Apparently, regional compression is only a secondary influence on Vp: the primary driver of P‐wave slowing in the upper layers of this catchment is topographic control of reactive water flowpaths and their integrated effects on weathering. The Vp result is best explained as the long‐term integrated effect of groundwater flow‐induced geochemical weathering of shale in response to climate‐driven patterns of micro‐ and macro‐topography.

     
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  2. Abstract

    Knowing little about how porosity and permeability are distributed at depth, we commonly develop models of groundwater by treating the subsurface as a homogeneous black box even though porosity and permeability vary with depth. One reason for this depth variation is that infiltrating meteoric water reacts with minerals to affect porosity in localized zones called reaction fronts. We are beginning to learn to map and model these fronts beneath headwater catchments and show how they are distributed. The subsurface landscapes defined by these fronts lie subparallel to the soil‐air interface but with lower relief. They can be situated above, below, or at the water table. These subsurface landscapes of reaction are important because porosity developed from weathering can control subsurface water storage. In addition, porosity often changes at the weathering fronts, and when this affects permeability significantly, the front can act like a valve that re‐orients water flowing through the subsurface. We explore controls on the positions of reaction fronts under headwater landscapes by accounting for the timescales of erosion, chemical equilibration, and solute transport. One strong control on the landscape of subsurface reaction is the land surface geometry, which is in turn a function of the erosion rate. In addition, the reaction fronts, like the water table, are strongly affected by the lithology and water infiltration rate. We hypothesize that relationships among the land surface, reaction fronts, and the water table are controlled by feedbacks that can push landscapes towards an ‘ideal hill’. In this steady state, reaction‐front valves partition water volumes into shallow and deep flowpaths. These flows dissolve low‐ and high‐solubility minerals, respectively, allowing their reaction fronts to advance at the erosion rate. This conceptualization could inform better models of subsurface porosity and permeability, replacing the black box.

     
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  3. Abstract

    Large‐scale models often use a single grid to represent an entire catchment assuming homogeneity; the impacts of such an assumption on simulating evapotranspiration (ET) and streamflow remain poorly understood. Here, we compare hydrological dynamics at Shale Hills (PA, USA) using a complex model (spatially explicit, >500 grids) and a simple model (spatially implicit, two grids using “effective” parameters). We asked two questions:What hydrological dynamics can a simple model reproduce at the catchment scale? What processes does it miss by ignoring spatial details?Results show the simple model can reproduce annual runoff ratios and ET, daily discharge peaks (e.g., storms, floods) but not discharge minima (e.g., droughts) under dry conditions. Neither can it reproduce different streamflow from the two sides of the catchment with distinct land surface characteristics. The similar annual runoff ratios between the two models indicate spatial details are not as important as climate in reproducing annual scale ET and discharge partitioning. Most of the calibrated parameters in the simple model are within the ranges in the complex model, except that effective porosity has to be reduced to 40% of the average porosity from the complex model. The form of the storage‐discharge relationship is similar. The effective porosity in the simple model however represents the dynamic and mobile water storage in the effective drainage area of the complex model that connects to the stream and contributes to high streamflow; it does not represent the passive, immobile water storage in the often disconnected uphill areas. This indicates that an additional uphill functioning unit is needed in the simple model to simulate the full spectrum of high‐low streamflow dynamics in natural catchments.

     
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  4. Abstract

    Soils derived from different lithologies and their controls on preferential flow remain underexplored in forested landscapes. In the same lithology, the propensity for preferential flow occurrence at different hillslope positions also remains largely elusive. By utilizing a soil moisture response time method, we compared preferential flow occurrence between a shale site (Shale Hills, silt loam soils) and a sandstone site (Garner Run, sandy loam soils) at four hillslope positions: ridge‐top, North‐ and South‐facing mid‐slopes and toe slope, for over 2 years. The catchments are neighbouring and covered by temperate forest. For the four hillslope positions, Shale Hills had higher preferential flow frequencies compared to Garner Run. Between these two catchments, the South‐facing mid‐slope sites showed the highest contrasts in preferential flow frequency (33.5% of events at Shale Hills vs. 8.8% at Garner Run) while the ridge‐top sites showed the lowest contrasts (18.7 vs. 13.2%). Additionally, over the unfrozen period, for seven out of eight monitoring sites, drier antecedent conditions tended to be more favourable for preferential flows to occur, with significant (p < .01) relationships at two sites. Except for the South‐facing mid‐slope sites, both Shale Hills and Garner Run had two preferential flow pathways. The characteristic preferential flow pathways at Shale Hills were the Bwand C horizons, and for Garner Run, preferential flow moved from the E/AE horizon to the Bwhorizon. This study shows that shale‐derived soils tended to have higher preferential flow occurrence than sandstone soils, but hillslope positions exhibit different levels of contrasts. More effort should be paid to study the impact of lithology on preferential flows in the context of land surface modelling and biogeochemical reactions to improve ecosystem services of headwater catchments.

     
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  5. Abstract

    Headwater catchments are the fundamental units that connect the land to the ocean. Hydrological flow and biogeochemical processes are intricately coupled, yet their respective sciences have progressed without much integration. Reaction kinetic theories that prescribe rate dependence on environmental variables (e.g., temperature and water content) have advanced substantially, mostly in well‐mixed reactors, columns, and warming experiments without considering the characteristics of hydrological flow at the catchment scale. These theories have shown significant divergence from observations in natural systems. On the other hand, hydrological theories, including transit time theory, have progressed substantially yet have not been incorporated into understanding reactions at the catchment scale. Here we advocate for the development of integrated hydro‐biogeochemical theories across gradients of climate, vegetation, and geology conditions. The lack of such theories presents barriers for understanding mechanisms and forecasting the future of the Critical Zone under human‐ and climate‐induced perturbations. Although integration has started and co‐located measurements are well under way, tremendous challenges remain. In particular, even in this era of “big data,” we are still limited by data and will need to (1) intensify measurements beyond river channels and characterize the vertical connectivity and broadly the shallow and deep subsurface; (2) expand to older water dating beyond the time scales reflected in stable water isotopes; (3) combine the use of reactive solutes, nonreactive tracers, and isotopes; and (4) augment measurements in environments that are undergoing rapid changes. To develop integrated theories, it is essential to (1) engage models at all stages to develop model‐informed data collection strategies and to maximize data usage; (2) adopt a “simple but not simplistic,” or fit‐for‐purpose approach to include essential processes in process‐based models; (3) blend the use of process‐based and data‐driven models in the framework of “theory‐guided data science.” Within the framework of hypothesis testing, model‐data fusion can advance integrated theories that mechanistically link catchments' internal structures and external drivers to their functioning. It can not only advance the field of hydro‐biogeochemistry, but also enable hind‐ and fore‐casting and serve the society at large. Broadly, future education will need to cultivate thinkers at the intersections of traditional disciplines with hollistic approaches for understanding interacting processes in complex earth systems.

    This article is categorized under:

    Engineering Water > Methods

     
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  6. Abstract

    Projections of future conditions within the critical zone—earthcasts—can be used to understand the potential effects of changes in climate on processes affecting landscapes. We are developing an approach to earthcast how weathering will change in the future using scenarios of climate change. As a first step here, we use the earthcasting approach to model aspect‐related effects on soil water chemistry and weathering on hillsides in a well‐studied east‐west trending watershed (Shale Hills, Pennsylvania, USA). We completed model simulations of solute chemistry in soil water with and without the effect of aspect for comparison to catchment observations. With aspect included, aqueous weathering fluxes were higher on the sunny side of the catchment. But the effect of aspect on temperature (0.8 °C warmer soil on sunny side) and recharge (100 mm/year larger on shaded side) alone did not explain the magnitude of the observed higher weathering fluxes on the sunny side. Modeled aspect‐related differences in weathering fluxes only approach field observations when we incorporated the measured differences in clay content observed in augered soils on the two hillslopes. We also had to include a biolifting module to accurately describe cation concentrations in soil water versus depth. Biolifting lowered some mineral dissolution rates while accelerating kaolinite precipitation. These short‐duration simulations also highlighted that the inherited differences in particle size on the two sides of the catchment might in themselves be explained by weathering under different microclimates caused by aspect—over longer durations than simulated with our models.

     
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  7. Abstract

    Earth System Models (ESMs) are essential tools for understanding and predicting global change, but they cannot explicitly resolve hillslope‐scale terrain structures that fundamentally organize water, energy, and biogeochemical stores and fluxes at subgrid scales. Here we bring together hydrologists, Critical Zone scientists, and ESM developers, to explore how hillslope structures may modulate ESM grid‐level water, energy, and biogeochemical fluxes. In contrast to the one‐dimensional (1‐D), 2‐ to 3‐m deep, and free‐draining soil hydrology in most ESM land models, we hypothesize that 3‐D, lateral ridge‐to‐valley flow through shallow and deep paths and insolation contrasts between sunny and shady slopes are the top two globally quantifiable organizers of water and energy (and vegetation) within an ESM grid cell. We hypothesize that these two processes are likely to impact ESM predictions where (and when) water and/or energy are limiting. We further hypothesize that, if implemented in ESM land models, these processes will increase simulated continental water storage and residence time, buffering terrestrial ecosystems against seasonal and interannual droughts. We explore efficient ways to capture these mechanisms in ESMs and identify critical knowledge gaps preventing us from scaling up hillslope to global processes. One such gap is our extremely limited knowledge of the subsurface, where water is stored (supporting vegetation) and released to stream baseflow (supporting aquatic ecosystems). We conclude with a set of organizing hypotheses and a call for global syntheses activities and model experiments to assess the impact of hillslope hydrology on global change predictions.

     
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  8. Oxidative weathering of pyrite plays an important role in the biogeochemical cycling of Fe and S in terrestrial environments. While the mechanism and occurrence of biologically accelerated pyrite oxidation under acidic conditions are well established, much less is known about microbially mediated pyrite oxidation at circumneutral pH. Recent work (Percak-Dennett et al., 2017, Geobiology, 15, 690) has demonstrated the ability of aerobic chemolithotrophic microorganisms to accelerate pyrite oxidation at circumneutral pH and proposed two mechanistic models by which this phenomenon might occur. Here, we assess the potential relevance of aerobic microbially catalyzed circumneutral pH pyrite oxidation in relation to subsurface shale weathering at Susquehanna Shale Hills Critical Zone Observatory (SSHCZO) in Pennsylvania, USA. Specimen pyrite mixed with native shale was incubated in groundwater for 3 months at the inferred depth of in situ pyrite oxidation. The colonized materials were used as an inoculum for pyrite-oxidizing enrichment cultures. Microbial activity accelerated the release of sulfate across all conditions. 16S rRNA gene sequencing and metagenomic analysis revealed the dominance of a putative chemolithoautotrophic sulfur-oxidizing bacterium from the genus Thiobacillus in the enrichment cultures. Previously proposed models for aerobic microbial pyrite oxidation were assessed in terms of physical constraints, enrichment culture geochemistry, and metagenomic analysis. Although we conclude that subsurface pyrite oxidation at SSCHZO is largely abiotic, this work nonetheless yields new insight into the potential pathways by which aerobic microorganisms may accelerate pyrite oxidation at circumneutral pH. We propose a new “direct sulfur oxidation” pathway, whereby sulfhydryl-bearing outer membrane proteins mediate oxidation of pyrite surfaces through a persulfide intermediate, analogous to previously proposed mechanisms for direct microbial oxidation of elemental sulfur. The action of this and other direct microbial pyrite oxidation pathways have major implications for controls on pyrite weathering rates in circumneutral pH sedimentary environments where pore throat sizes permit widespread access of microorganisms to pyrite surfaces. 
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  9. Zang, RunGuo (Ed.)
    Root lifespan, often is estimated in landscape- and ecosystem-level carbon models using linear approximations. In water manipulation experiments, fine root lifespan can vary with soil water content. Soil water content is generally structured by complex topography, which is largely unaccounted for in landscape- and ecosystem-scale carbon models. Topography governs the range of soil water content experienced by roots which may impact their lifespan. We hypothesized that root lifespan varied nonlinearly across a temperate, mesic, forested catchment due to differences in soil water content associated with topographic position. We expected regions of the landscape that were too wet or too dry would have soils that were not optimal for roots and thus result in shorter root lifespans. Specifically, we hypothesized that root lifespan would be longest in areas that consistently had soil water content in the middle of the soil water content spectrum, while in soils at either very low or very high soil water content, root lifespan would be relatively short. We tested this hypothesis by collecting and analyzing two years of minirhizotron and soil moisture data in plots widely distributed in the Shale Hills catchment of the Susquehanna-Shale Hills Critical Zone Observatory in Pennsylvania. We found that fine root lifespans were longer in traditionally wetter topographic regions, but detected no short term (biweekly) effect of soil moisture on root lifespan. Additionally, depth in soil, soil series, slope face orientation, and season of birth strongly affected root lifespans across the catchment. In contrast, lifespan was unaffected by root diameter or mycorrhizal association. Failure to account for these variables could result in erroneous estimates of fine root lifespan and, consequentially, carbon flux in temperate forested regions. 
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