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Surface water samples were collected from 43 streams distributed throughout watersheds of mixed land use in southern Ontario, Canada. Absorbance and fluorescence spectroscopy with parallel factor analysis (PARAFAC) was used to characterize dissolved organic matter (DOM). DOM characteristics were related to environmental variables, microbial activity indicators (bacterial production and extracellular leucine aminopeptidase activity), and riparian land use to understand better how these factors influence DOM in streams. PARAFAC produced a six-component model (C1 to C6). Temperature correlated with each PARAFAC component, suggesting that water source, drainage area, and light penetration broadly affected DOM characteristics. C1 and C2 represented terrestrial, humic-like DOM fluorophore groups and comprised 41-65% of stream DOM fluorescence. C5, a tryptophan-like component, related negatively to a humification index but positively to leucine-aminopeptidase activity and recently produced DOM, suggesting that C5 consisted of autochthonous, microbially produced DOM. C3, C4, and C6 showed signs of quinone-like, humic-like, and microbial transformable fluorophores. The distribution of these potentially redox-active PARAFAC components indicated that DOM was in a more reduced state in streams with higher bacterial production and agricultural land use than in streams with increased wetlands area, which had greater relative abundance of the oxidized quinone-like component. Anthropogenic land use and microbial activity altered the quantity and quality of DOM exported from human-affected streams from that observed in forest-and wetland-dominated streams. DOM in agriculturally affected streams was likely more labile and accessible to the microbial community than DOM in wetland streams, which supported low rates of microbial activity.

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The flux of terrestrial C to rivers has increased relative to preindustrial levels, a fraction of which is aged dissolved organic C (DOC). In rivers, C is stored in sediments, exported to the ocean, or (bio)chemically processed and released as CO. Disturbance changes land cover and hydrology, shifting potential sources and processing of DOC. To investigate the likely sources of aged DOC, we analyzed radiocarbon ages, chemical, and spectral properties of DOC and major ions from 19 rivers draining the coterminous U.S. and Arctic. DOC optics indicated that the majority is exported as aromatic, high molecular weight, modern molecules while aged DOC tended to consist of smaller, microbial degradation products. Aged DOC exports, observed regularly in arid basins and during base flow in arctic rivers, are associated with higher proportion of mineral weathering products, suggesting deeper flows paths. These patterns also indicate potential for production of microbial byproducts as DOC ages in soil and water with longer periods of time between production and transport. Thus, changes in hydrology associated with landscape alteration (e.g., tilling or shifting climates) that can result in deeper flow paths or longer residence times will likely lead to a greater proportion of aged carbon in riverine exports.

The use of cover crops and crop residues is a common strategy to mitigate sediment and nutrient losses from land to water. In cold climates, elevated dissolved P losses can occur associated with freeze-thaw of plant materials. Here, we review the impacts of cover crops and crop residues on dissolved P and total P loss in cold climates across ?41 studies, exploring linkages between water-extractable P (WEP) in plant materials and P loss in surface runoff and subsurface drainage. Water-extractable P concentrations are influenced by plant type and freezing regimes. For example, WEP was greater in brassica cover crops than in non-brassicas, and increased with repeated freeze-thaw cycles. However, total P losses in surface runoff and subsurface drainage from cropped fields under cold climates were much lower than plant WEP, owing to retention of 45 to >99% of released P by soil. In cold climatic regions, cover crops and crop residues generally prevented soil erosion and loss of particle-bound P during nongrowing seasons in erodible landscapes but tended to elevate dissolved P loss in nonerodible soils. Their impact on total P loss was inconsistent across studies and complicated by soil, climate, and management factors. More research is needed to understand interactions between these factors and plant type that influence P loss, and to improve the assessment of crop contributions to P loss in field settings in cold climates. Further, tradeoffs between P loss and the control of sediment loss and N leaching by plants should be acknowledged.

In the Anthropocene 1 , watershed chemical transport is increasingly dominated by novel combinations elements, which are hydrologically linked together as 'chemical cocktails.' Chemical cocktails are novel because human activities greatly enhance elemental concentrations and their probability for biogeochemical interactions and shared transport along hydrologic flowpaths. A new chemical cocktail approach advances our ability to: trace contaminant mixtures in watersheds, develop chemical proxies with high-resolution sensor data, and manage multiple water quality problems. We explore the following questions: (1) Can we classify elemental transport in watersheds as chemical cocktails using a new approach? (2) What is the role of climate and land use in enhancing the formation and transport of chemical cocktails in watersheds? To address these questions, we first analyze trends in concentrations of carbon, nutrients, metals, and salts in fresh waters over 100 years. Next, we explore how climate and land use enhance the probability of formation of chemical cocktails of carbon, nutrients, metals, and salts. Ultimately, we classify transport of chemical cocktails based on solubility, mobility, reactivity, and dominant phases: (1) sieved chemical cocktails (e.g., particulate forms of nutrients, metals and organic matter); (2) filtered chemical cocktails (e.g., dissolved organic matter and associated metal complexes); (3) chromatographic chemical cocktails (e.g., ions eluted from soil exchange sites); and (4) reactive chemical cocktails (e.g., limiting nutrients and redox sensitive elements). Typically, contaminants are regulated and managed one element at a time, even though combinations of elements interact to influence many water-quality problems such as toxicity to life, eutrophication, infrastructure and water treatment. A chemical cocktail approach significantly expands evaluations of water-quality signatures and impacts beyond single elements to mixtures. High-frequency sensor data (pH, specific conductance, turbidity, etc.) can serve as proxies for chemical cocktails and improve real-time analyses of water-quality violations, identify regulatory needs, and track water quality recovery following and extreme climate events. Ultimately, a watershed chemical cocktail approach is necessary for effectively co-managing groups of contaminants and provides a more holistic approach for studying, monitoring, and managing water quality in the Anthropocene.