General reversal of N-decomposition relationship during long-term decomposition in boreal and temperate forests.

Decomposition of dead organic matter is fundamental to carbon (C) and nutrient cycling in terrestrial ecosystems, influencing C fluxes from the biosphere to the atmosphere. Theory predicts and evidence strongly supports that the availability of nitrogen (N) limits litter decomposition. Positive relationships between substrate N concentrations and decomposition have been embedded into ecosystem models. This decomposition paradigm, however, relies on data mostly from short-term studies analyzing controls on early-stage decomposition. We present evidence from three independent long-term decomposition investigations demonstrating that the positive N-decomposition relationship is reversed and becomes negative during later stages of decomposition. First, in a 10-y decomposition experiment across 62 woody species in a temperate forest, leaf litter with higher N concentrations exhibited faster initial decomposition rates but ended up a larger recalcitrant fraction decomposing at a near-zero rate. Second, in a 5-y N-enrichment experiment of two tree species, leaves with experimentally enriched N concentrations had faster decomposition initial rates but ultimately accumulated large slowly decomposing fractions. Measures of amino sugars on harvested litter in two experiments indicated that greater accumulation of microbial residues in N-rich substrates likely contributed to larger slowly decomposing fractions. Finally, a database of 437 measurements from 120 species in 45 boreal and temperate forest sites confirmed that higher N concentrations were associated with a larger slowly decomposing fraction. These results challenge the current treatment of interactions between N and decomposition in many ecosystems and Earth system models and suggest that even the best-supported short-term controls of biogeochemical processes might not predict long-term controls.

Mineral composition controls the stabilization of microbially derived carbon and nitrogen in soils: Insights from an isotope tracing model.

Evidence is emerging that microbial products and residues (necromass) contribute greatly to stable soil organic matter (SOM), which calls for the necessity of separating the microbial necromass from other SOM pools in models. However, the understanding on how microbial necromass stabilizes in soil, especially the mineral protection mechanisms, is still lacking. Here, we incubated 13 C- and 15 N-labelled microbial necromass in a series of artificial soils varying in clay minerals and metal oxides. We found the mineralization, adsorption and desorption rate constants of necromass nitrogen were higher than those of necromass carbon. The accumulation rates of necromass carbon and nitrogen in mineral-associated SOM were positively correlated with the specific surface area of clay minerals. Our results provide direct evidence for the protection role of mineral in microbial necromass stabilization and provide a platform for simulating microbial necromass separately in SOM models.

Enhanced rock weathering increased soil phosphorus availability and altered root phosphorus-acquisition strategies.

Enhanced rock weathering (ERW) has been proposed as a measure to enhance the carbon (C)-sequestration potential and fertility of soils. The effects of this practice on the soil phosphorus (P) pools and the general mechanisms affecting microbial P cycling, as well as plant P uptake are not well understood. Here, the impact of ERW on soil P availability and microbial P cycling functional groups and root P-acquisition traits were explored through a 2-year wollastonite field addition experiment in a tropical rubber plantation. The results show that ERW significantly increased soil microbial carbon-use efficiency and total P concentrations and indirectly increased soil P availability by enhancing organic P mobilization and mineralization of rhizosheath carboxylates and phosphatase, respectively. Also, ERW stimulated the activities of P-solubilizing (gcd, ppa and ppx) and mineralizing enzymes (phoADN and phnAPHLFXIM), thus contributing to the inorganic P solubilization and organic P mineralization. Accompanying the increase in soil P availability, the P-acquisition strategy of the rubber fine roots changed from do-it-yourself acquisition by roots to dependence on mycorrhizal collaboration and the release of root exudates. In addition, the direct effects of ERW on root P-acquisition traits (such as root diameter, specific root length, and mycorrhizal colonization rate) may also be related to changes in the pattern of belowground carbon investments in plants. Our study provides a new insight that ERW increases carbon-sequestration potential and P availability in tropical forests and profoundly affects belowground plant resource-use strategies.

Large Seasonal Variation in Nitrogen Isotopic Abundances of Ammonia Volatilized from a Cropland Ecosystem and Implications for Regional NH3 Source Partitioning.

Ammonia (NH3) volatilization from agricultural lands is a main source of atmospheric reduced nitrogen species (NHx). Accurately quantifying its contribution to regional atmospheric NHx deposition is critical for controlling regional air nitrogen pollution. The stable nitrogen isotope composition (expressed by δ15N) is a promising indicator to trace atmospheric NHx sources, presupposing a reliable nitrogen isotopic signature of NH3 emission sources. To obtain more specific seasonal δ15N values of soil NH3 volatilization for reliable regional seasonal NH3 source partitioning, we utilized an active dynamic sampling technique to measure the δ15N-NH3 values volatilized from maize cropping land in northeast China. These values varied from -38.0 to -0.2‰, with a significantly lower rate-weighted value observed in the early period (May-June, -30.5 ± 6.7‰) as compared with the late period (July-October, -8.5 ± 4.3‰). Seasonal δ15N-NH3 variations were related to the main NH3 production pathway, degree of soil ammonium consumption, and soil environment. Bayesian isotope mixing model analysis revealed that without considering the seasonal δ15N variation in soil-volatilized NH3 could result in an overestimate by up to absolute 38% for agricultural volatile NH3 to regional atmospheric bulk ammonium deposition during July-October, further demonstrating that it is essential to distinguish seasonal δ15N profile of agricultural volatile NH3 in regional source apportionment.

NO2 Sensor Based on Faraday Rotation Spectroscopy Using Ring Array Permanent Magnets.

Faraday rotation spectroscopy (FRS) exploits the magneto-optical effect to achieve highly selective and sensitive detection of paramagnetic molecules. Usually, a solenoid coil is used to provide a longitudinal magnetic field to produce the magneto-optical effect. However, such a method has the disadvantages of excessive power consumption and susceptibility to electromagnetic interference. In the present work, a novel FRS approach based on a combination of a neodymium iron boron permanent magnet ring array and a Herriott multipass absorption cell is proposed. A longitudinal magnetic field was generated by using 14 identical neodymium iron boron permanent magnet rings combined in a non-equidistant form according to their magnetic field's spatial distribution characteristics. The average magnetic field strength within a length of 380 mm was 346 gauss. A quantum cascade laser was used to target the optimum 441 ← 440 Q-branch nitrogen dioxide transition at 1613.25 cm-1 (6.2 µm) with an optical power of 40 mW. Coupling to a Herriott multipass absorption cell, a minimum detection limit of 0.4 ppb was achieved with an integration time of 70 s. The low-power FRS nitrogen dioxide sensor proposed in this work is expected to be developed into a robust field-deployable environment monitoring system.

Source Apportionment of Atmospheric Ammonia at 16 Sites in China Using a Bayesian Isotope Mixing Model Based on δ15N-NHx Signatures.

Reducing atmospheric ammonia (NH3) emissions is critical to mitigating poor air quality. However, the contributions of major agricultural and non-agricultural source emissions to NH3 at receptor sites remain uncertain in many regions, hindering the assessment and implementation of effective NH3 reduction strategies. This study conducted simultaneous measurements of the monthly concentrations and stable nitrogen isotopes of NHx (gaseous NH3 plus particulate NH4+) at 16 sites across China. Ambient NHx concentrations averaged 21.7 ± 19.6 µg m-3 at rural sites, slightly higher than those at urban (19.2 ± 6.0 µg m-3) and three times of those at background (7.0 ± 6.9 µg m-3) sites. Based on revised δ15N values of the initial NH3, source apportionment results indicated that non-agricultural sources (traffic and waste) and agricultural sources (fertilizer and livestock) contributed 54 and 46% to NH3 at urban sites, 51 and 49% at rural sites, and 61 and 39% at background sites, respectively. Non-agricultural sources contributed more to NH3 at rural and background sites in cold than warm seasons, arising from traffic and waste, but were similar across seasons at urban sites. We concluded that non-agricultural sources need to be addressed when reducing ambient NH3 across China, even in rural regions.

Quantifying the Nitrogen Sources and Secondary Formation of Ambient HONO with a Stable Isotopic Method.

Nitrous acid (HONO) is a reactive gas that plays an important role in atmospheric chemistry. However, accurately quantifying its direct emissions and secondary formation in the atmosphere as well as attributing it to specific nitrogen sources remains a significant challenge. In this study, we developed a novel method using stable nitrogen and oxygen isotopes (δ15N; δ18O) for apportioning ambient HONO in an urban area in North China. The results show that secondary formation was the dominant HONO formation processes during both day and night, with the NO2 heterogeneous reaction contributing 59.0 ± 14.6% in daytime and 64.4 ± 10.8% at nighttime. A Bayesian simulation demonstrated that the average contributions of coal combustion, biomass burning, vehicle exhaust, and soil emissions to HONO were 22.2 ± 13.1, 26.0 ± 5.7, 28.6 ± 6.7, and 23.2 ± 8.1%, respectively. We propose that the isotopic method presents a promising approach for identifying nitrogen sources and the secondary formation of HONO, which could contribute to mitigating HONO and its adverse effects on air quality.

Drivers of foliar 15 N trends in southern China over the last century.

Foliar stable nitrogen (N) isotopes (δ15 N) generally reflect N availability to plants and have been used to infer about changes thereof. However, previous studies of temporal trends in foliar δ15 N have ignored the influence of confounding factors, leading to uncertainties on its indication to N availability. In this study, we measured foliar δ15 N of 1811 herbarium specimens from 12 plant species collected in southern China forests from 1920 to 2010. We explored how changes in atmospheric CO2 , N deposition and global warming have affected foliar δ15 N and N concentrations ([N]) and identified whether N availability decreased in southern China. Across all species, foliar δ15 N significantly decreased by 0.82‰ over the study period. However, foliar [N] did not decrease significantly, implying N homeostasis in forest trees in the region. The spatiotemporal patterns of foliar δ15 N were explained by mean annual temperature (MAT), atmospheric CO2 ( P CO 2 ), atmospheric N deposition, and foliar [N]. The spatiotemporal trends of foliar [N] were explained by MAT, temperature seasonality, P CO 2 , and N deposition. N deposition within the rates from 5.3 to 12.6 kg N ha-1  year-1 substantially contributed to the temporal decline in foliar δ15 N. The decline in foliar δ15 N was not accompanied by changes in foliar [N] and therefore does not necessarily reflect a decline in N availability. This is important to understand changes in N availability, which is essential to validate and parameterize biogeochemical cycles of N.

Vehicular Emissions Enhanced Ammonia Concentrations in Winter Mornings: Insights from Diurnal Nitrogen Isotopic Signatures.

A general feature in the diurnal cycle of atmospheric ammonia (NH3) concentrations is a morning spike that typically occurs around 07:00 to 10:00 (LST). Current hypotheses to explain this morning's NH3 increase remain elusive, and there is still no consensus whether traffic emissions are among the major sources of urban NH3. Here, we confirmed that the NH3 morning pulse in urban Beijing is a universal feature, with an annual occurrence frequency of 73.0% and a rapid growth rate (>20%) in winter. The stable nitrogen isotopic composition of NH3 (δ15N-NH3) in winter also exhibited a significant diurnal variation with an obvious morning peak at 07:00 to 10:00 (-18.6‰, mass-weighted mean), higher than other times of the day (-26.3‰). This diurnal pattern suggests that a large fraction of NH3 in the morning originated from nonagricultural sources, for example, power plants, vehicles, and coal combustion that tend to have higher δ15N-NH3 emission signatures relative to agricultural emissions. In particular, the contribution from vehicular emissions increased from 18% (00:00 to 07:00) to 40% (07:00 to 10:00), while the contribution of fertilizer sources to NH3 was reduced from 15.8% at 00:00 to 07:00 to 5.2% at 07:00 to 10:00. We concluded that NH3 concentrations in winter mornings in urban Beijing were indeed enhanced by vehicle emissions, which should be considered in air pollution regulations.

Mature conifers assimilate nitrate as efficiently as ammonium from soils in four forest plantations.

Conifers are considered to prefer to take up ammonium (NH4+ ) over nitrate (NO3- ). However, this conclusion is mainly based on hydroponic experiments that separate roots from soils. It remains unclear to what extent mature conifers can use nitrate compared to ammonium under field conditions where both roots and soil microbes compete for nitrogen (N). We conducted an in situ whole mature tree nitrogen-15 (15 N) labeling experiment (15 NH4+ vs 15 NO3- ) over 15 d to quantify ammonium and nitrate uptake and assimilation rates in four 40-yr-old monoculture coniferous plantations (Pinus koraiensis, Pinus sylvestris, Picea koraiensis and Larix olgensis, respectively). For the whole tree, 15 NO3- contributed 39% to 90% to total 15 N tracer uptake among four plantations during the study period. At day 3, the 15 NO3- accounted for 77%, 64%, 62% and 59% by Larix olgensis, Pinus koraiensis, Pinus sylvestris and Picea koraiensis, respectively. Our study indicates that mature coniferous trees assimilated nitrate as efficiently as ammonium from soils even at low soil nitrate concentration, in contrast to the results from hydroponic experiments showing that ammonium uptake dominated over nitrate. This implies that mature conifers can adapt to increasing availability of nitrate in soil, for example, under the context of globalization of N deposition and global warming.

The undefined N source might be overestimated by 15 N tracer trials.

Based on data from previous 15 N-tracer trials, Yan et al. (Global Change Biology, 26, 191-199; 2020) accounted the sources of cereal crop nitrogen (N) from fertilizer inputs (from both current and previous seasons) and possible uptake of nonfertilizer N inputs, leaving a significant part of N source undefined. We argue that the undefined N source does not reflect the net change in soil N stock and might be overestimated for three reasons: (a) higher yield in 15 N tracer trials; (b) a low residue return rate is assumed; (c) underestimated contribution by fertilizer inputs from previous seasons due to the lack of long-term trials.

Large-scale importance of microbial carbon use efficiency and necromass to soil organic carbon.

Optimal methods for incorporating soil microbial mechanisms of carbon (C) cycling into Earth system models (ESMs) are still under debate. Specifically, whether soil microbial physiology parameters and residual materials are important to soil organic C (SOC) content is still unclear. Here, we explored the effects of biotic and abiotic factors on SOC content based on a survey of soils from 16 locations along a ~4000 km forest transect in eastern China, spanning a wide range of climate, soil conditions, and microbial communities. We found that SOC was highly correlated with soil microbial biomass C (MBC) and amino sugar (AS) concentration, an index of microbial necromass. Microbial C use efficiency (CUE) was significantly related to the variations in SOC along this national-scale transect. Furthermore, the effect of climatic and edaphic factors on SOC was mainly via their regulation on microbial physiological properties (CUE and MBC). We also found that regression models on explanation of SOC variations with microbial physiological parameters and AS performed better than the models without them. Our results provide the empirical linkages among climate, microbial characteristics, and SOC content at large scale and confirm the necessity of incorporating microbial biomass and necromass pools in ESMs under global change scenarios.

Dynamics and multi-annual fate of atmospherically deposited nitrogen in montane tropical forests.

The effects of nitrogen (N) deposition on forests largely depend on its fate after entering the ecosystem. While several studies have addressed the forest fate of N deposition using 15 N tracers, the long-term fate and redistribution of deposited N in tropical forests remains unknown. Here, we applied 15 N tracers to examine the fates of deposited ammonium ( NH 4 + ) and nitrate ( NO 3 - ) separately over 3 years in a primary and a secondary tropical montane forest in southern China. Three months after 15 N tracer addition, over 60% of 15 N was retained in the forests studied. Total ecosystem retention did not change over the study period, but between 3 months and 3 years following deposition 15 N recovery in plants increased from 10% to 19% and 13% to 22% in the primary and secondary forests, respectively, while 15 N recovery in the organic soil declined from 16% to 2% and 9% to 2%. Mineral soil retained 50% and 35% of 15 N in the primary and secondary forests, with retention being stable over time. The total ecosystem retention of the two N forms did not differ significantly, but plants retained more 15 NO 3 - than 15 NH 4 + and the organic soil more 15 NH 4 + than NO 3 - . Mineral soil did not differ in 15 NH 4 + and 15 NO 3 - retention. Compared to temperate forests, proportionally more 15 N was distributed to mineral soil and plants in these tropical forests. Overall, our results suggest that atmospherically deposited NH 4 + and NO 3 - is rapidly lost in the short term (months) but thereafter securely retained within the ecosystem, with retained N becoming redistributed to plants and mineral soil from the organic soil. This long-term N retention may benefit tropical montane forest growth and enhance ecosystem carbon sequestration.

Historical changes in the stomatal limitation of photosynthesis: empirical support for an optimality principle.

The ratio of leaf internal (ci ) to ambient (ca ) partial pressure of CO2 , defined here as χ, is an index of adjustments in both leaf stomatal conductance and photosynthetic rate to environmental conditions. Measurements and proxies of this ratio can be used to constrain vegetation model uncertainties for predicting terrestrial carbon uptake and water use. We test a theory based on the least-cost optimality hypothesis for modelling historical changes in χ over the 1951-2014 period, across different tree species and environmental conditions, as reconstructed from stable carbon isotopic measurements across a global network of 103 absolutely dated tree-ring chronologies. The theory predicts optimal χ as a function of air temperature, vapour pressure deficit, ca and atmospheric pressure. The theoretical model predicts 39% of the variance in χ values across sites and years, but underestimates the intersite variability in the reconstructed χ trends, resulting in only 8% of the variance in χ trends across years explained by the model. Overall, our results support theoretical predictions that variations in χ are tightly regulated by the four environmental drivers. They also suggest that explicitly accounting for the effects of plant-available soil water and other site-specific characteristics might improve the predictions.

Persistent Nonagricultural and Periodic Agricultural Emissions Dominate Sources of Ammonia in Urban Beijing: Evidence from 15N Stable Isotope in Vertical Profiles.

Ammonia (NH3) emission reduction is key to limiting the deadly PM2.5 pollution globally. However, studies of long-term source apportionment of vertical NH3 are relatively limited. On the basis of the one-year measurements of weekly vertical profiles of δ15N-NH3 at 5 heights (2, 15, 102, 180, and 320 m) on a 325-m meteorological tower in urban Beijing, we found that vertical profiles of NH3 concentrations generally remained stable with height. δ15N-NH3 increased obviously as a function of height in cold seasons (with heating) and decreased in warm seasons (with fertilization), indicating a stronger human-induced seasonal variation via regional transport at higher altitudes. Relatively stable δ15N-NH3 near the ground surface suggested the strong local emission. The results of isotopic mixing model (SIAR) indicate that source apportionment using measured δ15N-NH3 only would overestimate the contribution of agricultural emissions to NH3. By using an estimation of initial δ15N-NH3, we found that nonagricultural sources contributed ∼72% of NH3 on average. Our study suggests that (i) both persistent nonagricultural and periodic agricultural emissions drive atmospheric NH3 concentration and its vertical distribution in urban Beijing; and (ii) source apportionment based on measured δ15N-NH3 only likely underestimates fossil fuel source contribution, if the combined NHx isotope effects are not considered.

Insight into the Variability of the Nitrogen Isotope Composition of Vehicular NOx in China.

Nitrogen isotope (δ15N) monitoring is a potentially powerful tool in tracing atmospheric nitrogen oxides (NOx); however, the isotopic fingerprint of vehicle exhaust remains poorly interpreted. This deficiency limits our understanding of the origin of atmospheric haze pollution, especially in China. In this study, we systemically explored the δ15N-NOx fingerprints of various vehicle exhausts (n = 137) in China. The δ15N-NOx values of vehicle exhausts ranged from -18.8‰ to +6.4‰, presenting a significant correlation with NOx concentrations (p < 0.01). The highest δ15N-NOx values were observed for liquefied petroleum gas vehicles (-0.1 ± 1.8‰), followed by gasoline vehicles (-7.0 ± 4.8‰) and diesel vehicles (-12.7 ± 3.4‰), all of which displayed a rising trend as emissions standards were continuously updated. The δ15N-NOx values under working conditions followed the trend warm start (-5.9 ± 5.0‰) > driving (-7.3 ± 5.9‰) > cold start (-9.2 ± 2.7‰). By establishing a suitable model for assessing representative δ15N-NOx values, the δ15N-NOx values of various vehicles, including different fuel types with different emission standards, were evaluated. A model of δ15N-NOx associated with motor vehicle data was developed, which estimated the national δ15N-NOx value of vehicle emissions to be -12.6 ± 2.2‰, but there was considerable variation among different target areas in China.

Isotopic Interpretation of Particulate Nitrate in the Metropolitan City of Karachi, Pakistan: Insight into the Oceanic Contribution to NOx.

Nitrogen oxide (NOx) abatement has become the focus of air quality management strategies. In this study, we examined NOx sources and the atmospheric conversion of NOx in Karachi, Pakistan, a megacity in South Asia with serious particulate pollution problems. Oceanic contributions to NOx were quantified for the first time based on a novel approach using nitrogen/oxygen isotopic analysis in nitrate (δ15N-NO3-; δ18O-NO3-) and a Bayesian model. Our results showed that δ15N-NO3- in Karachi varied between -10.2‰ and +12.4‰. As indicated by the δ18O-NO3- findings (+66.2 ± 7.8‰), the •OH pathway dominated NOx conversion throughout the nearly two-year observation, but high NO3- events were attributed to the O3 pathway. Coal combustion was the most significant source (32.0 ± 9.8%) of NOx in Karachi, with higher contributions in the autumn and winter; a similar situation occurred for biomass burning + lightning (30.3 ± 6.5%). However, mobile sources (25.2 ± 6.4%) and microbial processes (12.5 ± 7.5%) exhibited opposite seasonal trends. The oceanic contributions to NOx in Karachi were estimated to be 16.8%, of which lightning, shipping emissions, and microbial processes accounted for 20.3%, 46.3%, and 33.4%, respectively, emphasizing the dominance of shipping emissions as an oceanic NOx source.

Multiyear Measurements on Δ17O of Stream Nitrate Indicate High Nitrate Production in a Temperate Forest.

Nitrification is a crucial step in ecosystem nitrogen (N) cycling, but scaling up from plot-based measurements of gross nitrification to catchments is difficult. Here, we employed a newly developed method in which the oxygen isotope anomaly (Δ17O) of nitrate (NO3-) is used as a natural tracer to quantify in situ catchment-scale gross nitrification rate (GNR) for a temperate forest from 2014 to 2017 in northeastern China. The annual GNR ranged from 71 to 120 kg N ha-1 yr-1 (average 94 ± 10 kg N ha-1 yr-1) over the 4 years in this forest. This result and high stream NO3- loss (4.2-8.9 kg N ha-1 yr-1) suggest that the forested catchment may have been N-saturated. At the catchment scale, the total N output of 10.7 kg N ha-1 yr-1, via leaching and gaseous losses, accounts for 56% of the N input from bulk precipitation (19.2 kg N ha-1 yr-1). This result indicates that the forested catchment is still retaining a large fraction of N from atmospheric deposition. Our study suggests that estimating in situ catchment-scale GNR over several years when combined with other conventional flux estimates can facilitate the understanding of N biogeochemical cycling and changes in the ecosystem N status.

Fate of atmospherically deposited NH4+ and NO3- in two temperate forests in China: temporal pattern and redistribution.

The impacts of anthropogenic nitrogen (N) deposition on forest ecosystems depend in large part on its fate. However, our understanding of the fates of different forms of deposited N as well as the redistribution over time within different ecosystems is limited. In this study, we used the 15 N-tracer method to investigate both the short-term (1 week to 3 months) and long-term (1-3 yr) fates of deposited NH4+ or NO3- by following the recovery of the 15 N in different ecosystem compartments in a larch plantation forest and a mixed forest located in northeastern China. The results showed similar total ecosystem retention for deposited NH4+ and NO3- , but their distribution within the ecosystems (plants vs. soil) differed distinctly particularly in the short-term, with higher 15 NO3- recoveries in plants (while lower recoveries in organic layer) than found for 15 NH4+ . The different short-term fate was likely related to the higher mobility of 15 NO3- than 15 NH4+ in soils instead of plant uptake preferences for NO3- over NH4+ . In the long-term, differences between N forms became less prevalent but higher recoveries in trees (particularly in the larch forest) of 15 NO3- than 15 NH4+ tracer persisted, suggesting that incoming NO3- may contribute more to plant biomass increment and forest carbon sequestration than incoming NH4+ . Differences between the two forests in recoveries were largely driven by a higher 15 N recovery in the organic layer (both N forms) and in trees (for 15 NO3- ) in the larch forest compared to the mixed forest. This was due to a more abundant organic layer and possibly higher tree N demand in the larch forest than in the mixed forest. Leachate 15 N loss was minor (<1% of the added 15 N) for both N forms and in both forests. Total 15 N recovery averaged 78% in the short-term and decreased to 55% in the long-term but with increasing amount of 15 N label (re)-redistributed into slow turn-over pools (e.g., trees and mineral soil). The different retention dynamics of deposited NH4+ and NO3- may have implications in environmental policy related to the anthropogenic emissions of the two N forms.

Microbial denitrification dominates nitrate losses from forest ecosystems.

Denitrification removes fixed nitrogen (N) from the biosphere, thereby restricting the availability of this key limiting nutrient for terrestrial plant productivity. This microbially driven process has been exceedingly difficult to measure, however, given the large background of nitrogen gas (N2) in the atmosphere and vexing scaling issues associated with heterogeneous soil systems. Here, we use natural abundance of N and oxygen isotopes in nitrate (NO3 (-)) to examine dentrification rates across six forest sites in southern China and central Japan, which span temperate to tropical climates, as well as various stand ages and N deposition regimes. Our multiple stable isotope approach across soil to watershed scales shows that traditional techniques underestimate terrestrial denitrification fluxes by up to 98%, with annual losses of 5.6-30.1 kg of N per hectare via this gaseous pathway. These N export fluxes are up to sixfold higher than NO3 (-) leaching, pointing to widespread dominance of denitrification in removing NO3 (-) from forest ecosystems across a range of conditions. Further, we report that the loss of NO3 (-) to denitrification decreased in comparison to leaching pathways in sites with the highest rates of anthropogenic N deposition.