Shift of nitrate sources in groundwater due to intensive livestock farming on Jeju Island, South Korea: With emphasis on legacy effects on water management.

• N isotopic compositions of nitrate indicate a shift of nitrate sources in groundwater. • Intensive livestock farming is currently a major N source via manure discharge. • Manure accounts for 33.5~81.8% of the nitrate contamination as of 2015–2018. • Based on the legacy effect, the contribution of manure will increase in the future. • Groundwater ages suggest the need of long-term (> 25yrs) management practices. Time lags between anthropogenic nitrogen inputs and their impacts to nitrate levels cause a misunderstanding for sources and subsequently misguide the groundwater management.We investigated the hydrochemical data of groundwater samples (n = 172 from 49 wells) with chlorofluorocarbons (CFCs)-based groundwater age dating and stable N (δ15N) and O isotopes (δ18O) of nitrate to assess the legacy effect of livestock farming to groundwater in an agricultural area where intensive livestock farming started in the 1970s and illegal dumping of manure wastewater in a lava cave was revealed in 2015. Approximately 90% of the groundwater samples had nitrate concentrations exceeding the natural threshold (5.5 mg/L NO 3 −) for nitrate contamination and 34% exceeded the World Health Organization's guideline for drinking water quality (44.3 mg/L), indicating severe nitrate contamination. The δ15N NO3 values (5.5 to 24.3‰) in groundwater exceeding the threshold of nitrate showed that livestock manure was a major nitrate source, while ammonium fertilizer also seemed influential given the δ15N NO3 values in the overlapping fields of N sources. Factor analysis of hydrochemical data also supported nitrate contamination by manure as well as by plant farming in the study area. Based on the spatial distribution of nitrate levels and δ15N NO3 , livestock farming affected nitrate contamination by illegal manure dumping in the leakage cave. According to a Bayesian mixing model, the contribution of manure wastewater was 33.5 to 81.8% as of 2015–2018, with the rest from fertilizers. Meanwhile, the groundwater ages showed negative correlations with both nitrate levels (r = –0.90) and δ15N NO3 values (r = –0.74) on a log scale, consistent with the increasing N release from livestock farming since the 1960s. In particular, the median value of δ15N NO3 rapidly increased to 9.2‰ in groundwater recharged between the late 1970s and early 1990s when N production exponentially increased, implying a significant effect of livestock farming after the 1980s. Groundwater quality is expected to deteriorate over the next several decades based on the groundwater ages (> 23.5 years), the increased N production from livestock farming, and the legacy effect of N. Long-term groundwater management plans (> 25 years) are required to decrease N loads in the study area, because it takes time for management practices to take effect. The study results are a good reference for groundwater management in regions with a source shift to livestock farming under intensive livestock production systems. Moreover, the chronological study using historical N production, groundwater age data, and dual nitrate isotopes can be applied to other regions with multiple N sources and their shifting for identifying sources and estimating time lags. Image, graphical abstract [ABSTRACT FROM AUTHOR]