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In the first multiyear sampling effort for POPs in the eastern Antarctic atmosphere, 32 PCBs and 38 organochlorine pesticides were targeted in air collected with a high-flow-through passive sampler. Agricultural chemicals were found to dominate atmospheric profiles, in particular HCB and endosulfan-I, with average concentrations of 12 600 and 550 fg/m3, respectively. HCB showed higher concentrations in the austral summer, indicative of local, temperature-dependent volatilisation, while endosulfan-I appeared to show fresh, late-austral-summer input followed by temporally decreasing levels throughout the year. The current-use herbicide, trifluralin, and the legacy pesticides mirex and toxaphene, were detected in Antarctic air for the first time. Trifluralin was observed at low but increasing levels over the five-year period. Its detection in the Antarctic atmosphere provides evidence of its persistence and long-range environmental transport capability. While a time frame of five years exceeds the duration of most Antarctic air monitoring efforts, it is projected that continuous monitoring at the decadal scale is required to detect an annual 10% change in atmospheric concentrations of key analytes. This finding emphasizes the importance of continuous, long-term monitoring efforts in polar regions, that serve a special role as sentinel environments of hemispheric chemical usage trends.