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The effects of soil properties and cropland age on atmospheric nitrous oxide (N2O) emissions following the conversion of grassland to cropland in temperate grassland ecosystems are uncertain. In this study, N2O emissions were compared among grassland and cropland soils in the agro-pastoral ecotone of Inner Mongolia over three growing seasons. Four adjacent sites with different land-use histories were selected, including grassland and croplands cultivated for 5, 10, and 50 years after conversion. N2O flux measurements were obtained using a closed-chamber method and were performed continuously during vegetation periods. After the conversion of grassland to cropland, N2O emission initially decreased and thereafter increased in the study sites. The cumulative N2O emissions of the cropland soils 5 and 10 years in age were 10–50% less than those of the grassland, and the N2O emissions from the cropland soil 50 years in age were 10–30% greater than the grassland. When the seasonal emissions were correlated against single soil parameter, the key soil parameter that affected N2O emissions over the entire growing season was the soil moisture content. When the interactions among soil parameters were considered, the amount of N2O emissions could be quantitatively described by a linear combination of two soil variables, the soil ammonium nitrogen (NH4+-N) and moisture concentrations. This study demonstrates how the time of land use conversion from grassland to cropland can positively or negatively affect N2O emission. [ABSTRACT FROM AUTHOR]