• Energy Research

Abstract. Nitrous oxide (N2O) is the primary atmospheric constituent involved in stratospheric ozone depletion and contributes strongly to changes in the climate system through a positive radiative forcing mechanism. The atmospheric abundance of N2O has increased from 270 ppb (parts per billion, 10−9 mole mole−1) during the pre-industrial era to approx. 330 ppb in 2018. Even though it is well known that microbial processes in agricultural and natural soils are the major N2O source, the contribution of specific soil processes is still uncertain. The relative abundance of N2O isotopocules (14N14N16N, 14N15N16O, 15N14N16O, and 14N14N18O) carries process-specific information and thus can be used to trace production and consumption pathways. While isotope ratio mass spectroscopy (IRMS) was traditionally used for high-precision measurement of the isotopic composition of N2O, quantum cascade laser absorption spectroscopy (QCLAS) has been put forward as a complementary technique with the potential for on-site analysis. In recent years, pre-concentration combined with QCLAS has been presented as a technique to resolve subtle changes in ambient N2O isotopic composition. From the end of May until the beginning of August 2016, we investigated N2O emissions from an intensively managed grassland at the study site Fendt in southern Germany. In total, 612 measurements of ambient N2O were taken by combining pre-concentration with QCLAS analyses, yielding δ15Nα, δ15Nβ, δ18O, and N2O concentration with a temporal resolution of approximately 1 h and precisions of 0.46 ‰, 0.36 ‰, 0.59 ‰, and 1.24 ppb, respectively. Soil δ15N-NO3- values and concentrations of NO3- and NH4+ were measured to further constrain possible N2O-emitting source processes. Furthermore, the concentration footprint area of measured N2O was determined with a Lagrangian particle dispersion model (FLEXPART-COSMO) using local wind and turbulence observations. These simulations indicated that night-time concentration observations were largely sensitive to local fluxes. While bacterial denitrification and nitrifier denitrification were identified as the primary N2O-emitting processes, N2O reduction to N2 largely dictated the isotopic composition of measured N2O. Fungal denitrification and nitrification-derived N2O accounted for 34 %–42 % of total N2O emissions and had a clear effect on the measured isotopic source signatures. This study presents the suitability of on-site N2O isotopocule analysis for disentangling source and sink processes in situ and found that at the Fendt site bacterial denitrification or nitrifier denitrification is the major source for N2O, while N2O reduction acted as a major sink for soil-produced N2O.

Abstract. Nitrous oxide (N2O) is the primary atmospheric constituent involved in stratospheric ozone depletion and contributes strongly to changes in the climate system through a positive radiative forcing mechanism. The atmospheric abundance of N2O has increased from 270 ppb (parts per billion, 10−9 mole mole−1) during the pre-industrial era to approx. 330 ppb in 2018. Even though it is well known that microbial processes in agricultural and natural soils are the major N2O source, the contribution of specific soil processes is still uncertain. The relative abundance of N2O isotopocules (14N14N16N, 14N15N16O, 15N14N16O, and 14N14N18O) carries process-specific information and thus can be used to trace production and consumption pathways. While isotope ratio mass spectroscopy (IRMS) was traditionally used for high-precision measurement of the isotopic composition of N2O, quantum cascade laser absorption spectroscopy (QCLAS) has been put forward as a complementary technique with the potential for on-site analysis. In recent years, pre-concentration combined with QCLAS has been presented as a technique to resolve subtle changes in ambient N2O isotopic composition. From the end of May until the beginning of August 2016, we investigated N2O emissions from an intensively managed grassland at the study site Fendt in southern Germany. In total, 612 measurements of ambient N2O were taken by combining pre-concentration with QCLAS analyses, yielding δ15Nα, δ15Nβ, δ18O, and N2O concentration with a temporal resolution of approximately 1 h and precisions of 0.46 ‰, 0.36 ‰, 0.59 ‰, and 1.24 ppb, respectively. Soil δ15N-NO3- values and concentrations of NO3- and NH4+ were measured to further constrain possible N2O-emitting source processes. Furthermore, the concentration footprint area of measured N2O was determined with a Lagrangian particle dispersion model (FLEXPART-COSMO) using local wind and turbulence observations. These simulations indicated that night-time concentration observations were largely sensitive to local fluxes. While bacterial denitrification and nitrifier denitrification were identified as the primary N2O-emitting processes, N2O reduction to N2 largely dictated the isotopic composition of measured N2O. Fungal denitrification and nitrification-derived N2O accounted for 34 %–42 % of total N2O emissions and had a clear effect on the measured isotopic source signatures. This study presents the suitability of on-site N2O isotopocule analysis for disentangling source and sink processes in situ and found that at the Fendt site bacterial denitrification or nitrifier denitrification is the major source for N2O, while N2O reduction acted as a major sink for soil-produced N2O.

In this study water balance components as well as nitrogen and dissolved organic carbon leaching were quantified by means of large weighable grassland lysimeters at three sites (860, 770 and 600 m a.s.l.) for both intensive and extensive management. Our results show that at E600, the site with highest air temperature (8.6 °C) and lowest precipitation (981.9 mm), evapotranspiration losses were 100.7 mm higher as at the site (E860) with lowest mean annual air temperature (6.5 °C) and highest precipitation (1359.3 mm). Seepage water formation was substantially lower at E600 (-440.9 mm) as compared to E860. Compared to climate, impacts of management on water balance components were negligible. However, intensive management significantly increased total nitrogen leaching rates across sites as compared to extensive management from 2.6 kg N ha-1 year-1 (range: 0.5-6.0 kg N ha-1 year-1) to 4.8 kg N ha-1 year-1 (range: 0.9-12.9 kg N ha-1 year-1). N leaching losses were dominated by nitrate (64.7%) and less by ammonium (14.6%) and DON (20.7%). The low rates of N leaching (0.8-6.9% of total applied N) suggest a highly efficient nitrogen uptake by plants as measured by plant total N content at harvest. Moreover, plant uptake was often exceeding slurry application rates, suggesting further supply of N due to soil organic matter decomposition. The low risk of nitrate losses via leaching and surface runoff of cut grassland on non-sandy soils with vigorous grass growth may call for a careful site and region specific re-evaluation of fixed limits of N fertilization rates as defined by e.g. the German Fertilizer Ordinance following requirements set by the European Water Framework and Nitrates Directive.

In this study water balance components as well as nitrogen and dissolved organic carbon leaching were quantified by means of large weighable grassland lysimeters at three sites (860, 770 and 600 m a.s.l.) for both intensive and extensive management. Our results show that at E600, the site with highest air temperature (8.6 °C) and lowest precipitation (981.9 mm), evapotranspiration losses were 100.7 mm higher as at the site (E860) with lowest mean annual air temperature (6.5 °C) and highest precipitation (1359.3 mm). Seepage water formation was substantially lower at E600 (-440.9 mm) as compared to E860. Compared to climate, impacts of management on water balance components were negligible. However, intensive management significantly increased total nitrogen leaching rates across sites as compared to extensive management from 2.6 kg N ha-1 year-1 (range: 0.5-6.0 kg N ha-1 year-1) to 4.8 kg N ha-1 year-1 (range: 0.9-12.9 kg N ha-1 year-1). N leaching losses were dominated by nitrate (64.7%) and less by ammonium (14.6%) and DON (20.7%). The low rates of N leaching (0.8-6.9% of total applied N) suggest a highly efficient nitrogen uptake by plants as measured by plant total N content at harvest. Moreover, plant uptake was often exceeding slurry application rates, suggesting further supply of N due to soil organic matter decomposition. The low risk of nitrate losses via leaching and surface runoff of cut grassland on non-sandy soils with vigorous grass growth may call for a careful site and region specific re-evaluation of fixed limits of N fertilization rates as defined by e.g. the German Fertilizer Ordinance following requirements set by the European Water Framework and Nitrates Directive.