Abstract. The tundra plays a pivotal role in the Arctic mercury
(Hg) cycle by storing atmospheric Hg deposition and shuttling it to the
Arctic Ocean. A recent study revealed that 70 % of the atmospheric Hg
deposition to the tundra occurs through gaseous elemental mercury (GEM or Hg(0))
uptake by vegetation and soils. Processes controlling land–atmosphere
exchange of Hg(0) in the Arctic tundra are central, but remain
understudied. Here, we combine Hg stable isotope analysis of Hg(0) in the
atmosphere, interstitial snow air, and soil pore air, with Hg(0) flux
measurements in a tundra ecosystem at Toolik Field Station in northern
Alaska (USA). In the dark winter months, planetary boundary layer (PBL)
conditions and Hg(0) concentrations were generally stable throughout the day
and small Hg(0) net deposition occurred. In spring, halogen-induced
atmospheric mercury depletion events (AMDEs) occurred, with the fast
re-emission of Hg(0) after AMDEs resulting in net emission fluxes of Hg(0).
During the short snow-free growing season in summer, vegetation uptake of
atmospheric Hg(0) enhanced atmospheric Hg(0) net deposition to the Arctic
tundra. At night, when PBL conditions were stable, ecosystem uptake of
atmospheric Hg(0) led to a depletion of atmospheric Hg(0). The night-time
decline of atmospheric Hg(0) was concomitant with a depletion of lighter
Hg(0) isotopes in the atmospheric Hg pool. The enrichment factor,
ε202Hgvegetationuptake=-4.2 ‰ (±1.0 ‰) was consistent
with the preferential uptake of light Hg(0) isotopes by vegetation. Hg(0)
flux measurements indicated a partial re-emission of Hg(0) during daytime,
when solar radiation was strongest. Hg(0) concentrations in soil pore air
were depleted relative to atmospheric Hg(0) concentrations, concomitant with
an enrichment of lighter Hg(0) isotopes in the soil pore air, ε202Hgsoilair-atmosphere=-1.00 ‰
(±0.25 ‰) and E199Hgsoilair-atmosphere=0.07 ‰ (±0.04 ‰). These
first Hg stable isotope measurements of Hg(0) in soil pore air are
consistent with the fractionation previously observed during Hg(0) oxidation
by natural humic acids, suggesting abiotic oxidation as a cause for observed
soil Hg(0) uptake. The combination of Hg stable isotope fingerprints with
Hg(0) flux measurements and PBL stability assessment confirmed a dominant
role of Hg(0) uptake by vegetation in the terrestrial–atmosphere exchange of
Hg(0) in the Arctic tundra.