Agricultural soils encompass one of the major sources of anthropogenic nitrous oxide (N2O), a potent greenhouse gas and stratospheric ozone depleting substance. Therefore, accurate prediction of N2O emissions from soils and development of effective mitigation strategies are pertinent. However, the scientific understanding of mechanisms underlying N2O emissions is limited, in part, by the lack of suitable methods to assess sources of N2O, especially under field conditions and in undisturbed soil cores. In this dissertation, two ecological applications of source-partitioning N2O were considered: (1) the feedback of N2O emissions to elevated atmospheric CO2 and tropospheric O3 and (2) mechanisms underlying N2O emissions during a simulated rainfall event in a tomato cropping system in California. Furthermore, four methods were evaluated for their utility in source-partitioning N2O with minimal disturbance of the system: (1) tracing of added 15N enriched NH4 and/or NO3− to N2O, (2) use of natural abundance 15N of N2O and its precursors, (3) measuring the intramolecular distribution of 15N in N2O, expressed as site preference (SP), and (4) determining relationships between natural abundance 18O and 15N. Method comparisons elucidated that the use of isotope models that include all natural abundance isotopes of N2O and its precursors and uncertainty deductions for isotope fractionation factors to estimate N transformation rates and sources of N2O during peak N2O emissions is the most promising approach to improve our understanding of mechanisms underlying N2O emissions with minimal sampling-associated disturbance of the system. Various approaches to study sources of N2O and N-cycling suggested that elevated CO2 and O3 will unlikely cause a feedback on global climate change through altered N2O emissions in soybean agroecosystems in the Midwestern USA. Furthermore, elevated CO2 decelerated, whereas elevated O3 accelerated N-cycling if integrated over longer time scales. In a California tomato cropping system, N2O reduction to N2 decreased progressively as soil dried out following wetting up. Overall, this dissertation illustrates the added benefit of studying mechanisms underlying N2O emissions in addition to field N2O fluxes per se and encourages further research to source-partition N2O emissions and its needed methodology to understand N2O responses of agroecosystems in a changing global environment.

Emissions of nitrous oxide (N2O) in the Netherlands are reported to the UNFCCC on the basis of a country specific methodology. In this study we have identified and analysed the values for emission factors in measurement from in the Netherlands in the period 1993 – 2003. The overall averaged emission factor extracted from over 86 series of one year measurements on nitrous oxide emission from agricultural fields in the Netherlands is 1.1% and a weighed average for soil types is 1.01%. The average for mineral soils is 0.88%. The calculated emission factors are lower than the value suggested by the IPCC for EF1 for fertilizer and animal manure of 1.25%. We recommend to use a value of 1.0% for EF1 and to use corrections of EF1 in reporting the use of fertilizers without nitrate (0.5%), for subsurface application of manure (1.5%) and for fertilizer, manure and urine on organic soils (2.0%)

Atmospheric nitrous oxide (N2O) significantly impacts Earth's climate due to its dual role as an inert potent greenhouse gas in the troposphere and as a reactive source of ozone-destroying nitrogen oxides in the stratosphere. Global atmospheric concentrations of N2O, produced by natural and anthropogenic processes, continue to rise due to increases in emissions linked to human activity. The understanding of the impact of this gas is incomplete as there remain significant uncertainties in its global budget. The experiment described in this thesis, in which a global chemical transport model (MOZART-4), a fine-scale regional Lagrangian model (NAME), and new high-frequency atmospheric observations are combined, shows that uncertainty in N2O emissions estimates can be reduced in areas with continuous monitoring of N2O mole fraction and site-specific isotopic ratios. Due to unique heavy-atom (15N and 18O) isotopic substitutions made by different N2O sources, the measurement of N2O isotopic ratios in ambient air can help identify the distribution and magnitude of distinct sources. The new Stheno-TILDAS continuous wave laser spectroscopy instrument developed at MIT, recently installed at the Mace Head Atmospheric Research Station in western Ireland, can produce high-frequency timelines of atmospheric N2O isotopic ratios that can be compared to contemporaneous trends in correlative trace gas mole fractions and NAME-based statistical distributions of the origin of air sampled at the station. This combination leads to apportionment of the relative contribution from five major N2O sectors in the European region (agriculture, oceans, natural soils, industry, and biomass burning) plus well-mixed air transported from long distances to the atmospheric N2O measured at Mace Head. Bayesian inverse modeling methods that compare N2O mole fraction and isotopic ratio observations at Mace Head and at Diibendorf, Switzerland to simulated conditions produced using NAME and MOZART-4 lead to an optimized set of source-specific N2O emissions estimates in the NAME Europe domain. Notably, this inverse modeling experiment leads to a significant decrease in uncertainty in summertime emissions for the four largest sectors in Europe, and shows that industrial and agricultural N2O emissions in Europe are underestimated in inventories such as EDGAR v4.3.2. This experiment sets up future work that will be able to help constrain global estimates of N2O emissions once additional isotopic observations are made in other global locations and integrated into the NAME-MOZART inverse modeling framework described in this thesis.