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The atmospheric history of molecular hydrogen (H 2 ) from 1852 to 2003 was reconstructed from measurements of firn air collected at Megadunes, Antarctica. The reconstruction shows that H 2 levels in the southern hemisphere were roughly constant near 330 parts per billion (ppb; nmol H 2 mol −1 air) during the mid to late 1800s. Over the twentieth century, H 2 levels rose by about 70% to 550 ppb. The reconstruction shows good agreement with the H 2 atmospheric history based on firn air measurements from the South Pole. The broad trends in atmospheric H 2 over the twentieth century can be explained by increased methane oxidation and anthropogenic emissions. The H 2 rise shows no evidence of deceleration during the last quarter of the twentieth century despite an expected reduction in automotive emissions following more stringent regulations. During the late twentieth century, atmospheric CO levels decreased due to a reduction in automotive emissions. It is surprising that atmospheric H 2 did not respond similarly as automotive exhaust is thought to be the dominant source of anthropogenic H 2. The monotonic late twentieth century rise in H 2 levels is consistent with late twentieth-century flask air measurements from high southern latitudes. An additional unknown source of H 2 is needed to explain twentieth-century trends in atmospheric H 2 and to resolve the discrepancy between bottom-up and top-down estimates of the anthropogenic source term. The firn air–based atmospheric history of H 2 provides a baseline from which to assess human impact on the H 2 cycle over the last 150 y and validate models that will be used to project future trends in atmospheric composition as H 2 becomes a more common energy source.
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Anthropogenic Impacts on Atmospheric Carbonyl Sulfide Since the 19th Century Inferred From Polar Firn Air and Ice Core Measurements
Abstract Carbonyl sulfide (COS) was measured in firn air collected during seven different field campaigns carried out at four different sites in Greenland and Antarctica between 2001 and 2015. A Bayesian probabilistic statistical model is used to conduct multisite inversions and to reconstruct separate atmospheric histories for Greenland and Antarctica. The firn air inversions cover most of the 20th century over Greenland and extend back to the 19th century over Antarctica. The derived atmospheric histories are consistent with independent surface air time series data from the corresponding sites and the Antarctic ice core COS records during periods of overlap. Atmospheric COS levels began to increase over preindustrial levels starting in the 19th century, and the increase continued for much of the 20th century. Atmospheric COS peaked at higher than present‐day levels around 1975 CE over Greenland and around 1987 CE over Antarctica. An atmosphere/surface ocean box model is used to investigate the possible causes of observed variability. The results suggest that changes in the magnitude and location of anthropogenic sources have had a strong influence on the observed atmospheric COS variability.
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- Award ID(s):
- 1839506
- PAR ID:
- 10450675
- Publisher / Repository:
- DOI PREFIX: 10.1029
- Date Published:
- Journal Name:
- Journal of Geophysical Research: Atmospheres
- Volume:
- 125
- Issue:
- 16
- ISSN:
- 2169-897X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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