Overview
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Key numbers
The worker extracted the full PDF text with layout preservation twice and compared extraction hashes before commit. The following lines are copied from numeric/table-bearing regions of the PDF and retain the source units and wording where legible:
- up to 80% of HgII deposition occurs over the ocean2,6. Once deposited, ders our understanding of the major reaction pathways of atmospheric
- the spring leg (April–June 2020, > 80° N) of the MOSAiC expedition dissociation (Table 1) when assuming near kinetic limit charging of
- to-charge ratios and natural abundance isotope patterns (Table S1). In compounds to form ions.
- of detection (LOD, Fig. S1). Other GOM species were either below the ionizes with NO3− mainly by proton transfer. This approach has been
- LOD or masked by local ship-emitted interferences (cf. “Methods”). In applied previously to quantify HIO329, chlorine oxyacids30 and highly
- BrHgINO -3 LOD
- nitrate ions. HgCl2·NO3−, BrHgCl·NO3− and HgBr2·NO3− spectra were measured on detection (LOD, 3σ + baseline signal; Table S2 and “Methods”), and grey shaded
- April but fell below the LOD by June (Fig. S5). Other halides, neutral or
- quartile range, IQR, 29–110 pg Hg m−3, full range: <LOD – 1177 pg Hg m−3)
- detection (LOD). CI-APi-TOF data in (a) and (b) are averaged over 180 min to lies well within the 5–705 pg Hg m−3 range reported across Antarctica by
- enthalpies (Table 1) and cluster lifetimes τdiss » τres (~300 ms). However, reactive mercury (GOM + particulate Hg) values from cation-exchange
- between 25 and 37 pg Hg m−3 for 60 min time resolution (Table S2 and oxidized mercury is dominated globally by HgCl2 (49%), followed by
- “Methods” for LOD determination). Note that the LOD is determined particulate Hg (22%), Hg(OH)2 (19%), and HOHgBr (9%)3, reflecting
- quartile range, IQR, min–max) of GOM in the central Arctic and Antarctica. MOSAiC Antarctic sites were reviewed in the literature by Dommergue et al.38 and spanning
- species, with a minor contribution ( < 0.1%) of HgBr2 globally42. Pho- transport models. The inclusion of these missing pathways will
- HgII species contributing minor amounts ( < 0.3%) (Fig. S6). Compared drive the polar mercury cycle.
- much broader range of HgII species contribute to the total observed based47, shipborne48, and airborne49 campaigns could further illumi-
- spring, HgBr2 was the only GOM species detected above the LOD, forward, targeted calibration of individual mercuric halide responses
- long-range transport of Hg. Refining the Hg chemistry schemes in effect on the measurements (Fig. 1). Data availability extends over the
- checked weekly. The two flows inside the CI-inlet are coaxial to elim- The mean mass accuracy was 5.3 ppm and always <15 ppm. MOSAiC
- induced nucleation occurring inside the inlet. Sample ionization in the (HNO3)2NO2(18O)–, C3F5O2–. The mean mass accuracy was 2.9 ppm and
- CI system occurs at ambient pressure for better sensitivity than low always <5 ppm.
- instrument is ~0.8 lpm through a 0.3 mm diameter pinhole. The always applied before further analysis. The limit of detection (LOD) of
- 26 and 27 Jan 2015, showed no detectable peaks at the m/z values of verted into the differential equations using the KPP 2.2.3 kinetic
- any mercury-halide species. The LOD was calculated by adding three preprocessor56. The photolysis rates were calculated using the
- term variability in temperature or counting statistics. The model is constrained with 1.5 ng m−3 of Hg0, 17 ppbv ozone, 90
- MOSAiC: At the MOSAiC site, the mercury-halide m/z values ppbv CO, 1.95 ppmv CH4, 8 pptv NO2 and 45 pptv DMS. Two scenarios
- cules and the XHgY.NO3− clusters are listed in Table S3. The geometries Proc. Natl. Acad. Sci. USA 117, 30949–30956 (2020).
- chemical scheme3,12,13,55 (Table S4). The model allows all the HgI,II 58, 12853–12864 (2024).
Methods (brief)
- ionization mass spectrometry. Our observations identify HgBr2 as the domi-
- TOF) mass spectrometry technique together with ambient anion neutral mercuric halide clustering with NO3− (cf. “Methods” for details).
- of detection (LOD, Fig. S1). Other GOM species were either below the ionizes with NO3− mainly by proton transfer. This approach has been
- LOD or masked by local ship-emitted interferences (cf. “Methods”). In applied previously to quantify HIO329, chlorine oxyacids30 and highly
- nitrate ions. HgCl2·NO3−, BrHgCl·NO3− and HgBr2·NO3− spectra were measured on detection (LOD, 3σ + baseline signal; Table S2 and “Methods”), and grey shaded
- the given LOD values should be taken as conservative values. In Ant-
- April but fell below the LOD by June (Fig. S5). Other halides, neutral or
- quartile range, IQR, 29–110 pg Hg m−3, full range: <LOD – 1177 pg Hg m−3)
- detection (LOD). CI-APi-TOF data in (a) and (b) are averaged over 180 min to lies well within the 5–705 pg Hg m−3 range reported across Antarctica by
- ClHgI. All compounds show values above the LOD, which is estimated chemistry. GEOS-Chem, a Hg chemical-transport model, predicts that
- “Methods” for LOD determination). Note that the LOD is determined particulate Hg (22%), Hg(OH)2 (19%), and HOHgBr (9%)3, reflecting
- spring, HgBr2 was the only GOM species detected above the LOD, forward, targeted calibration of individual mercuric halide responses
- understand the relevance of oxidants (ozone, bromine) to our obser- In Aboa and MOSAiC, most of the campaign was sampled using
- vations. The location of the ship during the spring leg 3 can be visua- negative polarity settings to sample anions. This is to target observa-
- exhaust can be pushed towards the sampling location with the wind. Aboa, we sampled two days of cations in positive polarity between 26
- flow is equal to the sample flow of approximately 10 lpm, which was HNO3NO3–, (HNO3)2NO3–, (HNO3)3NO3–, HgCl2NO3– and HgBr2NO3–.
- between the sample and charger ions is ~300 ms, which prevents ion- most favorable options from NO2−, NO2(18O)–, HNO3NO2(18O)–,
- induced nucleation occurring inside the inlet. Sample ionization in the (HNO3)2NO2(18O)–, C3F5O2–. The mean mass accuracy was 2.9 ppm and
Implications
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Update history
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