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. We present a method to simulate fluid flow with reactivesolute transport in structured, partially saturated soils using a Lagrangianperspective. In this context, we extend the scope of the Lagrangian SoilWater and Solute Transport Model (LAST) (Sternagel et al., 2019) byimplementing vertically variable, non-linear sorption and first-orderdegradation processes during transport of reactive substances through apartially saturated soil matrix and macropores. For sorption, we develop anexplicit mass transfer approach based on Freundlich isotherms because thecommon method of using a retardation factor is not applicable in theparticle-based approach of LAST. The reactive transport method is testedagainst data of plot- and field-scale irrigation experiments with theherbicides isoproturon and flufenacet at different flow conditions overvarious periods. Simulations with HYDRUS 1-D serve as an additionalbenchmark. At the plot scale, both models show equal performance at a matrix-flow-dominated site, but LAST better matches indicators of preferential flowat a macropore-flow-dominated site. Furthermore, LAST successfully simulatesthe effects of adsorption and degradation on the breakthrough behaviour offlufenacet with preferential leaching and remobilization. The resultsdemonstrate the feasibility of the method to simulate reactive solutetransport in a Lagrangian framework and highlight the advantage of theparticle-based approach and the structural macropore domain to simulatesolute transport as well as to cope with preferential bypassing of topsoiland subsequent re-infiltration into the subsoil matrix.

Simulation of reactive solute transport in the critical zone: a Lagrangian model for transient flow and preferential transport