Nitrate trend reversal in Dutch dual-permeability chalk springs, evaluated by tritium-based groundwater travel time distributions

Historical use of fertilizer and manure on farmlands is known to have a lasting impact on ecosystems and water resources, but few studies assess the legacy of nitrate pollution on groundwater and surface water after farming applications were reduced. We studied the response of nitrate in spring water to a reduction of nitrogen fertilizer applications in agriculture realized since the mid-1980s. We assessed the travel time distribution of groundwater based on a time series of tritium measurements for 90 springs and small brooks that drain a dual porosity chalk aquifer. The travel time distributions were constrained using the tritium data in combination with time series of nitrate concentrations, applying a shape-free travel time distribution model. A clear trend reversal of nitrate concentrations was observed and simulated for springs with a large fraction of young water (< 30 years old) whereas the nitrate response in springs with relatively older water was attenuated and delayed. We conclude that obtaining a time series of tritium data helps to constrain age distributions of water that is discharged from dual permeability aquifers. The fraction of water aged 0.6) show higher peak concentrations, shorter lag-time between leaching and outflow peaks and steeper declines after trend reversal, relative to trends in springs which are dominantly fed by older groundwater. The study thus shows that the nitrate legacy of groundwater systems is strongly determined by the range of their travel time distributions, and trend reversal in receiving springs and surface waters may appear within 10 to 15 years after measures to reduce nitrate losses from farming. [Display omitted] •90 Springs show diverging, sometimes multi-modal, travel time distributions (TTDs).•Nitrate responses of springs following N-input reductions depend on their TTDs.•Models and measurements of 90 springs point to clear nitrate trend reversals.•TTDs influence peak concentrations, lag times and steepness of declines.•Large young water fractions favor high nitrate peaks and steep post-reversal declines.