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Poly(lactic-co-glycolic acid) (PLGA) particle carriers of synthetic DNA have recently received increased attention for environmental applications due to their biodegradability, customizability, and nearly limitless number of uniquely identifiable "labels". In this paper, we present methodologies for the preparation of DNA-labeled particles, control of particle size, extraction of DNA-labels, and analysis via quantitative polymerase chain reaction (qPCR). Characterization and analysis of the DNA-labeled particles reveal spherical particles of diameters ranging from 60 to 1000 nm, with consistent zeta potentials around -45 mV, that are stable to aggregation, even in the presence of concentrated mono- and divalent cations. A highly correlated and consistent relationship between particle concentration and DNA-label count was observed, with a detection range spanning 7 orders of magnitude, from 0.01 to 10,000 mg/L (10-10 particles/μL). The results of two environmental applications of the DNA-labeled particles are also presented, highlighting their feasibility for use in environmental studies. Whether exploring size-dependent transport phenomena or identifying potential pathogen transport pathways, the DNA-labeled particle approach presented here provides a powerful tool for the identification of overlapping particle signals at a range of concentrations.

Colloid transport through complex and dynamic (i.e. non-steady-state) hydrologic systems is rarely studied, owing to the difficulty of constraining initial and boundary conditions and quantifying colloid-porous media and colloid-colloid interactions in transient flow systems. Here we present a particle tracer experiment conducted on a sloped lysimeter receiving periodic rainfall events for 10 days. Four unique, DNA-labelled particle tracers were injected both in sequence and in parallel, together with a conservative tracer (deuterium), over the course of the first day and allowed to move through the system. Discharge-particle tracer concentration curves and the spatial distribution of particle tracer mass retained in the soil at the end of the experiment were found to be highly dependent on the timing of the tracer injection and the precipitation input and subsequent dynamic response of the water table. Overall, neglecting the total DLT recovery rate, the DLT particle tracer breakthrough trend (DNA-labelled particle tracer 4) was similar to deuterium and decreased over time with the exception of a few peaks later in the experiment. The individual particle tracer breakthrough curves suggest a complex system with different fast transport mechanisms (e.g. capillary barrier and size exclusion effect) and slow retention-release mechanisms (e.g. straining, physical-chemical adsorption), which resulted in particle tracers transferring faster than deuterium in the first 10 h of the experiment but being exceeded by deuterium soon after deuterium started to break through. The experiment not only highlights the interaction of repeated colloidal pollution events in hydrologic systems with different pre-event saturation conditions, but also the benefits of using multiple synchronous or sequential tracer applications to dissect explicit formulations of water flow and colloid transport processes in complex and dynamic hydrological systems. Such explicit process formulations could help improve understanding hydrologically-controlled transport through catchments and the quantitative prediction of these processes with water quality models. 2003a; Smith et al., 2007; Vasiliadou and Chrysikopoulos, 2011; Wan and Wilson, 1994b; Wang et al., 2018). Colloids have a high sorptive capacity and have been shown to facilitate transport of many contaminants through the vadose zone to streams or groundwater including heavy metals, pesticides, herbicides and other pollutants that

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