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Abstract Temporal patterns in chemistry of headwater streams reflect responses of water and elemental cycles to perturbations occurring at local to global scales. We evaluated multi-scale temporal patterns in up to 32 y of monthly observations of stream chemistry (ammonium, calcium, dissolved organic carbon, nitrate, total dissolved phosphorus, and sulfate) in 22 reference catchments within the northern temperate zone of North America. Multivariate autoregressive state-space (MARSS) models were applied to quantify patterns at multi-decadal, seasonal, and shorter intervals during a period that encompassed warming climate, seasonal changes in precipitation, and regional declines in atmospheric deposition. Significant long-term trends in solute concentrations within a subset of the catchments were consistent with recovery from atmospheric deposition (e.g., calcium, nitrate, sulfate) and increased precipitation (e.g., dissolved organic carbon). Lack of evidence for multi-decadal trends in most catchments suggests resilience of northern temperate ecosystems or that subtle net effects of simultaneous changes in climate and disturbance regimes do not result in directional trends. Synchronous seasonal oscillations of solute concentrations occurred across many catchments, reflecting shared climate and biotic drivers of seasonality within the northern temperate zone. Despite shared patterns among catchments at a seasonal scale, multi-scale temporal patterns were statistically distinct among even adjacent headwater catchments, implying that local attributes of headwater catchments modify the signals imparted by atmospheric phenomena and regional disturbances. To effectively characterize hydrologic and biogeochemical responses to changing climate and disturbance regimes, catchment monitoring programs could include multiple streams with contributing areas that encompass regional heterogeneity in vegetation, topography, and elevation. Overall, detection of long-term patterns and trends requires monitoring multiple catchments at a frequency that captures periodic variation (e.g., seasonality) and a duration encompassing the perturbations of interest. 

Abstract Tree-derived dissolved organic matter (DOM) comprises a significant carbon flux within forested watersheds. Few studies have assessed the optical properties of tree-derived DOM. To increase understanding of the factors controlling tree-derived DOM quality, we measured DOM optical properties, dissolved organic carbon (DOC) and calcium concentrations in throughfall and stemflow for 17 individual rain events during summer and fall in a temperate deciduous forest in Vermont, United States. DOC and calcium fluxes in throughfall and stemflow were enriched on average 4 to 70 times incident fluxes in rain. A multiway model was developed using absorbance and fluorescence spectroscopy to further characterize DOM optical properties. Throughfall contained a higher percentage of protein-like DOM fluorescence than stemflow while stemflow was characterized by a higher percentage of humic-like DOM fluorescence. DOM absorbance spectral slopes in yellow birch (Betula alleghaniensis) stemflow were significantly higher than in sugar maple (Acer saccharum) stemflow. DOM optical metrics were not influenced by rainfall volume, but percent protein-like fluorescence increased in throughfall during autumn when leaves senesced. Given the potential influence of tree-derived DOM fluxes on receiving soils and downstream ecosystems, future modeling of DOM transport and soil biogeochemistry should represent the influence of differing DOM quality in throughfall and stemflow across tree species and seasons. 

Abstract Atmospheric deposition of dissolved organic carbon (DOC) to terrestrial ecosystems is a small, but rarely studied component of the global carbon (C) cycle. Emissions of volatile organic compounds (VOC) and organic particulates are the sources of atmospheric C and deposition represents a major pathway for the removal of organic C from the atmosphere. Here, we evaluate the spatial and temporal patterns of DOC deposition using 70 data sets at least one year in length ranging from 40° south to 66° north latitude. Globally, the median DOC concentration in bulk deposition was 1.7 mg L⁻¹. The DOC concentrations were significantly higher in tropical (<25°) latitudes compared to temperate (>25°) latitudes. DOC deposition was significantly higher in the tropics because of both higher DOC concentrations and precipitation. Using the global median or latitudinal specific DOC concentrations leads to a calculated global deposition of 202 or 295 Tg C yr⁻¹respectively. Many sites exhibited seasonal variability in DOC concentration. At temperate sites, DOC concentrations were higher during the growing season; at tropical sites, DOC concentrations were higher during the dry season. Thirteen of the thirty‐four long‐term (>10 years) data sets showed significant declines in DOC concentration over time with the others showing no significant change. Based on the magnitude and timing of the various sources of organic C to the atmosphere, biogenic VOCs likely explain the latitudinal pattern and the seasonal pattern at temperate latitudes while decreases in anthropogenic emissions are the most likely explanation for the declines in DOC concentration. 

Abstract Arctic and boreal ecosystems are experiencing pronounced warming that is accelerating decomposition of soil organic matter and releasing greenhouse gases to the atmosphere. Future carbon storage in these ecosystems depends on the balance between microbial decomposition and primary production, both of which can be regulated by nutrients such as phosphorus. Phosphorus cycling in tundra and boreal regions is often assumed to occur through biological pathways with little interaction with soil minerals; that is, phosphate released from organic molecules is rapidly assimilated by plants or microorganisms. In contrast to this prevailing conceptual model, we use sequential extractions and spectroscopic techniques to demonstrate that iron (oxyhydr)oxides sequester approximately half of soil phosphate in organic soils from four arctic and boreal sites. Iron (III) (oxyhydr)oxides accumulated in shallow soils of low‐lying, saturated areas where circumneutral pH and the presence of a redox interface promoted iron oxidation and hydrolysis. Soils enriched in short‐range ordered iron oxyhydroxides, which are susceptible to dissolution under anoxic conditions, had high phosphate sorption capacities and maintained low concentrations of soluble phosphate relative to soils containing mostly organic‐bound iron or crystalline iron oxides. Thus, substantial quantities of phosphorus in these organic soils were associated with minerals that could reduce bioavailability but potentially also serve as phosphorus sources under anoxic conditions. The implication of this finding is that mineral surfaces effectively compete with biological processes for phosphate and must be considered as a nutrient regulator in these sensitive ecosystems.