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Atmospheric methane (CH 4 ) is a potent greenhouse gas, and its mole fraction has more than doubled since the preindustrial era 1 . Fossil fuel extraction and use are among the largest anthropogenic sources of CH 4 emissions, but the precise magnitude of these contributions is a subject of debate 2,3 . Carbon-14 in CH 4 ( 14 CH 4 ) can be used to distinguish between fossil ( 14 C-free) CH 4 emissions and contemporaneous biogenic sources; however, poorly constrained direct 14 CH 4 emissions from nuclear reactors have complicated this approach since the middle of the 20th century 4,5 . Moreover, the partitioning of total fossil CH 4 emissions (presently 172 to 195 teragrams CH 4 per year) 2,3 between anthropogenic and natural geological sources (such as seeps and mud volcanoes) is under debate; emission inventories suggest that the latter account for about 40 to 60 teragrams CH 4 per year 6,7 . Geological emissions were less than 15.4 teragrams CH 4 per year at the end of the Pleistocene, about 11,600 years ago 8 , but that period is an imperfect analogue for present-day emissions owing to the large terrestrial ice sheet cover, lower sea level and extensive permafrost. Here we use preindustrial-era ice core 14 CH 4 measurements to show that natural geological CH 4 emissions to the atmosphere were about 1.6 teragrams CH 4 per year, with a maximum of 5.4 teragrams CH 4 per year (95 per cent confidence limit)-an order of magnitude lower than the currently used estimates. This result indicates that anthropogenic fossil CH 4 emissions are underestimated by about 38 to 58 teragrams CH 4 per year, or about 25 to 40 per cent of recent estimates. Our record highlights the human impact on the atmosphere and climate, provides a firm target for inventories of the global CH 4 budget, and will help to inform strategies for targeted emission reductions 9,10 .

Atmospheric methane (CH4) is a potent greenhouse gas, and its mole fraction has more than doubled since the preindustrial era1. Fossil fuel extraction and use are among the largest anthropogenic sources of CH4 emissions, but the precise magnitude of these contributions is a subject of debate2,3. Carbon-14 in CH4 (14CH4) can be used to distinguish between fossil (14C-free) CH4 emissions and contemporaneous biogenic sources; however, poorly constrained direct 14CH4 emissions from nuclear reactors have complicated this approach since the middle of the 20th century4,5. Moreover, the partitioning of total fossil CH4 emissions (presently 172 to 195 teragrams CH4 per year)2,3 between anthropogenic and natural geological sources (such as seeps and mud volcanoes) is under debate; emission inventories suggest that the latter account for about 40 to 60 teragrams CH4 per year6,7. Geological emissions were less than 15.4 teragrams CH4 per year at the end of the Pleistocene, about 11,600 years ago8, but that period is an imperfect analogue for present-day emissions owing to the large terrestrial ice sheet cover, lower sea level and extensive permafrost. Here we use preindustrial-era ice core 14CH4 measurements to show that natural geological CH4 emissions to the atmosphere were about 1.6 teragrams CH4 per year, with a maximum of 5.4 teragrams CH4 per year (95 per cent confidence limit)-an order of magnitude lower than the currently used estimates. This result indicates that anthropogenic fossil CH4 emissions are underestimated by about 38 to 58 teragrams CH4 per year, or about 25 to 40 per cent of recent estimates. Our record highlights the human impact on the atmosphere and climate, provides a firm target for inventories of the global CH4 budget, and will help to inform strategies for targeted emission reductions9,10.

Measurements of carbon-14-containing carbon monoxide (14 CO) in glacial ice are useful for studies of the past oxidative capacity of the atmosphere as well as for reconstructing the past cosmic ray flux. The 14 CO abundance in glacial ice represents the combination of trapped atmospheric 14 CO and in situ cosmogenic 14 CO. The systematics of in situ cosmogenic 14 CO production and retention in ice are not fully quantified, posing an obstacle to interpretation of ice core 14 CO measurements. Here we provide the first comprehensive characterization of 14 CO at an ice accumulation site (Summit, Greenland), including measurements in the ice grains of the firn matrix, firn air and bubbly ice below the firn zone. The results are interpreted with the aid of a firn gas transport model into which we implemented in situ cosmogenic 14 C. We find that almost all (≈ 99.5 %) of in situ 14 CO that is produced in the ice grains in firn is very rapidly (in <1 year) lost to the open porosity and from there mostly vented to the atmosphere. The timescale of this rapid loss is consistent with what is expected from gas diffusion through ice. The small fraction of in situ 14 CO that initially stays in the ice grains continues to slowly leak out to the open porosity at a rate of ≈ 0.6 % yr -1. Below the firn zone we observe an increase in 14 CO content with depth that is due to in situ 14 CO production by deep-penetrating muons, confirming recent estimates of 14 CO production rates in ice via the muon mechanisms and allowing for narrowing constraints on these production rates. [ABSTRACT FROM AUTHOR]