1 2 3 Supporting Information Table S1. SOCs measured in fish by two modes of ionization. Electron Impact Ionization Negative Chemical Ionization Pesticides and degradation products: o,p’-DDT, p,p’-DDT, o,p’-DDD, p,p’-DDD, o,p’-DDE, p,p’-DDE, Methoxychlor, Acetochlor Pesticides and degradation products: Hexachlorocyclohexanes (HCH) (α, β, γ, δ) 2 Chlordanes (cis, trans, oxy), Nonachlor (cis, trans), Heptachlor, Heptachlor Epoxide, 3 Endosulfans (I, II, and sulfate), Dieldrin, Aldrin, Endrin, Endrin Aldehyde, Hexachlorobenzene (HCB), Dacthal, Chlorpyrifos, Chlorpyrifos oxon, Trifluralin, Metribuzin, Triallate, Mirex 1 PAHs : Acenaphthylene, Acenaphthene, Fluorene, Phenanthrene, Anthracene, Fluoranthene, Pyrene, Retene, Benz[a]anthracene, Chrysene, Triphenylene, Benzo[b]fluoranthene, Benzo[k]fluoranthene, Benzo[e]pyrene, Benzo[a]pyrene, Indeno[1,2,3-cd]pyrene, Dibenz[a,h]anthracene, Benzo[ghi]perylene Surrogates: d10-Fluorene, d10-Phenanthrene, d10-Pyrene, d12-Triphenylene, d12Benzo[a]pyrene, d12-Benzo[ghi]perylene, d8p,p’-DDE, d8-p,p’-DDT, d6-Methyl Parathion, Internal Standards: d10-Acenaphthene, d10Fluoranthene, d12-Benzo[k]fluoranthene 4 PCBs : PCB 74, PCB 101, PCB 118, PCB 138, PCB 153, PCB 183, and PCB 187 13 Surrogates: C12 PCB 101 (2,2’,4,5,5’13 Pentachlorobiphenyl), C12 PCB 180 (2,2’, 3,4,4’,5,5’-Heptachlorobiphenyl), d10 13 Chlorpyrifos, C6-HCB, d6-γ-HCH, d4Endosulfan I, d4-Endosulfan II Internal Standards: d14-Trifluralin 4 5 ΣPAHs= Chrysene+ Triphenylene+ Fluorene+ Phenanthrene+ Anthracene+ Fluoranthene+ Pyrene+ Retene+ Benz[a]anthracene+ Benzo[b]fluoranthene+ Benzo[k]fluoranthene+ Benzo[e]pyrene+ Benzo[a]pyrene+ Indeno[1,2,3cd]pyrene+ Dibenz[a,h]anthracene+ Benzo[ghi]perylene 2 Σchlordanes= oxy-chlordane+ trans-chlordane+ cis-chlordane+ cis-nonachlor+ trans-nonachlor 3 Σendosulfans= endosulfan I+ endosulfan II+ endosulfan sulfate 4 ΣPCBs= PCBs 101+ 118+ 138+ 153+ 183+ 187 1 1 1 2 3 4 5 6 7 Table S2: Number of fish exceeding subsistence fish consumption threshold established for human health. Numerator indicates number of fish exceeding consumption limit and denominator indicates number of fish analyzed. Shaded cells depict an exceedance. No fish exceeded the recreational fish consumption threshold. DCPA, dacthal; CLPRY, chlorpyrifos; γ-HCH, gamma-hexachlorohexane; ENDO, endosulfans; DLDRN, dieldrin; CLDN, chlordanes; HCB, hexachlorobenzene; ppDDE, p,p’-dichlorodiphenylethene SOC Park Water Body DCPA CLPYR γ-HCH ENDO DLDRN CLDN HCB ppDDE Tanada 0/6 0/6 0/6 0/6 6/6 0/6 0/6 0/6 Copper 0/6 0/6 0/6 0/6 6/6 0/6 0/6 0/6 Kijik 0 / 10 0 / 10 0 / 10 0 / 10 4 / 10 2 / 10 0 / 10 10 / 10 Kontrashibuna 0 / 10 0 / 10 0 / 10 0 / 10 6 / 10 1 / 10 0 / 10 0 / 10 Idavain 0 / 10 0 / 10 0 / 10 0 / 10 1 / 10 0 / 10 0 / 10 0 / 10 Brooks 0 / 10 0 / 10 0 / 10 0 / 10 7 / 10 0 / 10 0 / 10 4 / 10 Lassen Volcanic Summit 0/8 0/8 0/8 0/8 1/8 0/8 0/8 0/8 Yosemite Mildred 0 / 10 0 / 10 0 / 10 0 / 10 3 / 10 0 / 10 0 / 10 5 / 10 Bench 0 / 18 0 / 18 0 / 18 0 / 18 1 / 17 0 / 18 0 / 18 0 / 18 Kern Point 0 / 18 0 / 18 0 / 18 0 / 18 18 / 18 0 / 18 0 / 18 1 / 18 Dream 0/2 0/2 0/2 0/2 0/2 0/2 0/2 0/2 Haynach 0/3 0/3 0/3 0/3 3/3 0/3 0/3 0/3 Haiyaha 0/2 0/2 0/2 0/2 2/2 0/2 0/2 0/2 Lone Pine 0/2 0/2 0/2 0/2 0/2 0/2 0/2 0/2 Nanita 0/2 0/2 0/2 0/2 2/2 0/2 0/2 0/2 Spirit 0/2 0/2 0/2 0/2 2/2 0/2 0/2 0/2 Ypsilon 0/2 0/2 0/2 0/2 0/2 0/2 0/2 1/2 Sand Creek 0/8 0/8 0/8 0/8 4/8 0/8 0/8 0/8 Wrangell-St. Elias Lake Clark Katmai Sequoia & Kings Canyon Rocky Mountain Great Sand Dunes 2 Table S3: Number of fish exceeding kingfisher health thresholds. Numerator indicates number of fish exceeding consumption limit and denominator indicates number of fish analyzed. Shaded cells depict an exceedance. No fish exceeded the mink or river otter health thresholds. Park codes identified in Table 1. DLDRN, dieldrin; CLDN, chlordanes; ppDDE, p,p’-dichlorodiphenylethene SOC Park Water Body DLDRN CLDN ppDDE Tanada 0/6 0/6 0/6 Copper 0/6 0/6 0/6 Kijik 0 / 10 8 / 10 10 / 10 Kontrashibuna 0 / 10 2 / 10 0 / 10 Idavain 0 / 10 0 / 10 0 / 10 Brooks 0 / 10 7 / 10 2 / 10 Lassen Volcanic Summit 0/8 0/8 0/8 Yosemite Mildred 0 / 10 0 / 10 4 / 10 Bench 0 / 18 0 / 17 0 / 18 Kern Point 0 / 18 0 / 18 1 / 18 Dream 0/2 0/2 0/2 Haynach 0/3 1/3 0/3 Haiyaha 0/2 0/2 0/2 Lone Pine 0/2 0/2 0/2 Nanita 0/2 1/2 0/2 Spirit 0/2 0/2 0/2 Ypsilon 0/2 0/2 0/2 Sand Creek 0/8 0/8 0/8 Wrangell-St. Elias Lake Clark Katmai Sequoia & Kings Canyon Rocky Mountain Great Sand Dunes 3 Table S4: Sub-cooled Vapor pressure (Pa), Log KOW, and Log KOA at 25oC (KOAWIN 1.10, EPI Suite v4.11EPA, 2012) for 12 pesticides frequently measured in fish. Vapor Pressure, o Pa, 25 C Log KOW, o 25 C Log KOA, o 25 C Dacthal 0.0064 4.24 8.29 Chlorpyrifos 0.004 4.66 8.43 γ-HCH 0.0244 4.26 9.02 Endosulfan I, II 0.0005 3.50 8.30 Endosulfan sulfate 0.0013 3.64 8.52 Dieldrin 0.0389 5.45 9.04 Chlordane 0.0084 6.26 7.97 Nonachlor 0.0022 6.44 9.44 HCB 0.226 5.86 7.57 p'p-DDE 0.0034 6.00 8.78 α-HCH 0.0244 4.26 9.02 Mirex 0.0018 7.01 8.37 Current-Use Pesticides Historic-Use Pesticides 4 Figure S1. Mean SOC concentrations in fish (ng/g lipid), by national park, in the current studyresearch (2006–2011). Those SOCs excluded from Figure 1 are displayed here. Bars represent standard error. The number of fish, n, for each park is listed on the graph. ND, no detect; *, ND > 50% of lake fish 5 6 Figure S2. Concentrations of SOCs in fish (ng/g lipid) from current research (2006–2011) and previous study (2003–2005). Top of bar indicates the mean concentration and the circles indicate concentrations of individual fish. Black bars depict data from the current, post-WACAP study; white bars depict previously published data from WACAP (Ackerman et al., 2008; Landers et al., 2010). ND, no detect; *, ND > 50% of lake fish. Parks ordered by mountain rangeregion on the x-axis (L to R: Alaskan, Cascades, Sierra Nevada, Rockies); park codes identified in Table 1. 7 Figure S2 (continued). 8 Figure S3. Concentrations of SOCs in fish (ng/g ww) compared to human health fish consumption thresholds. Dashed lines represent the subsistence threshold; solid lines represent the recreational threshold. Top of bar indicates the mean concentration and the circles indicate concentrations of individual fish. Black bars depict data from the current study (2006–2011); white bars depict previously published data (2003–2005) (Ackerman et al., 2008; Landers et al., 2010). ND, no detect; *, ND > 50% of lake fish. Parks ordered by mountain rangeregion on the x-axis (L to R: Alaskan, Cascades, Sierra Nevada, Rockies); park codes identified in Table 1. 9