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Polycyclic aromatic compounds (PACs) in Canadian air and deposition were examined at the national scale for the first time in over twenty-five years. Air concentrations spanned four orders of magnitude, and were highest near industrial emitters and lowest in the Arctic. Declines in unsubstituted PAHs were observed at locations close to industrial facilities that had reduced emissions, but trends elsewhere were modest or negligible. Retene concentrations are increasing at several locations. Ambient concentrations of benzo[a]pyrene exceeded Ontario's health-based guideline in many urban/industrial areas. The estimated toxicity of the ambient PAC mixture increased by up to a factor of six when including compounds beyond the US EPA PAHs. Knowledge of PAC deposition is limited to the Laurentian Great Lakes and Athabasca Oil Sands regions. The atmosphere remained a net source of PAHs to the Great Lakes, though atmospheric inputs were decreasing with halving times of 26-30 years. Chemical transport modelling substantially overestimated wet deposition, but model performance is unknown for dry deposition. Sources from Asia, Europe and North America contributed to Arctic and Sub-Arctic concentrations, whereas transboundary or long-range transport have not been assessed outside Canada's north. Climate-related impacts from re-emission and forest fires were implicated in maintaining air concentrations in the high Arctic that were not consistent with global emissions reductions. Industrial emission decreases were substantial at the national scale, but their influence on the environment was limited to areas near relevant facilities. When examined through the lens of ambient levels at the local scale, evidence suggested that contributions from residential wood combustion and motor vehicles were smaller and larger, respectively, than those reported in national inventories. Future work aimed at characterizing PACs beyond the EPA PAHs, improving measurement coverage, elucidating deposition phenomena, and refining estimates of source contributions would assist in reducing remaining knowledge gaps about PACs in Canada., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Crown Copyright © 2020. Published by Elsevier Ltd. All rights reserved.)

Use of elemental mercury (Hg 0 ) to enhance placer gold recovery is an effective method dating back centuries, but is associated with significant atmospheric Hg 0 losses. This method was widely used in the Canadian Klondike region during most of the 20th century when the mining industry experienced rapid growth. While the health risks associated with Hg 0 pollution are now well understood, few studies have assessed the environmental legacy of Hg 0 use in the Klondike. We used an annually resolved Picea glauca tree-ring Hg record (1864-2015) to reconstruct and evaluate changes in local atmospheric Hg 0 concentrations associated with gold production at the Bear Creek mining camp. Major temporal trends in the record are consistent with the scale of Bear Creek operations and are distinct from background trends at an unimpacted control site. Tree-ring Hg concentration increased most rapidly from 1923 to 1930, a period when several major mining operations were consolidated at Bear Creek. The highest Hg concentrations, ∼2.5× greater than pre-mining era, occurred in the 1930s, coinciding with maximum gold production at this site. Post-World War II economic factors adversely affected the industry, causing declining tree-ring Hg concentrations from 1939 to 1966. Closure of the Bear Creek camp in 1966 coincided with the strongest tree-ring Hg decline, although a return to background levels did not occur until the 1990s, likely due to re-emission of legacy Hg 0 from contaminated soils. Finally, a robust increase was observed over the last decade, similar to other tree-ring Hg records in N.W. Canada, which is linked to rising Hg 0 emissions in Asia. The Bear Creek tree-ring Hg record provides a unique opportunity to study the impact of Klondike gold mining on the local environment at annual resolution and demonstrates great potential to use Picea tree rings to study past changes in atmospheric Hg 0 from local and global emissions. MAIN FINDINGS: A 151-year long, annually resolved tree-ring Hg record was developed at a historic Klondike gold-mining site to investigate the influence of mining-related Hg 0 emissions on the local atmosphere and environment. Compared to a control site, the tree-ring Hg record documents highly elevated atmospheric Hg 0 concentrations during the period mining activities were ongoing at this site., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)