Between 1999 and 2006, a plateau interrupted the otherwise continuous increase of atmospheric methane concentration [CH4] since preindustrial times. Causes could be sink variability or a temporary reduction in industrial or climate-sensitive sources. We reconstructed the global history of [CH4] and its stable carbon isotopes from ice cores, archived air, and a global network of monitoring stations. A box-model analysis suggests that diminishing thermogenic emissions, probably from the fossil-fuel industry, and/or variations in the hydroxyl CH4 sink caused the [CH4] plateau. Thermogenic emissions did not resume to cause the renewed [CH4] rise after 2006, which contradicts emission inventories. Post-2006 source increases are predominantly biogenic, outside the Arctic, and arguably more consistent with agriculture than wetlands. If so, mitigating CH4 emissions must be balanced with the need for food production.
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. 14 CH 4 emissions from nuclear power plants 4,5. By contrast, palaeoatmospheric 14 CH 4 measurements from ice cores offer a direct constraint on natural geological CH 4 emissions without these complications. Whereas geological CH 4 emissions have the potential to change on tectonic-and glacial-cycle timescales 14 , they have very probably been constant over the past few centuries. The preindustrial-era emission estimates can therefore be applied to the modern CH 4 budget with confidence. Ice core 14 CH 4 analysis is challenging owing to both the very large sample requirement (~1,
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The atmospheric deposition of both macronutrients and micronutrients plays an important role in driving primary productivity, particularly in the low-latitude ocean. We report aerosol major ion measurements for five ship-based sampling campaigns in the western Pacific from~25°N to 20°S and compare the results with those from Atlantic meridional transects (~50°N to 50°S) with aerosols collected and analyzed in the same laboratory, allowing full incomparability. We discuss sources of the main nutrient species (nitrogen (N), phosphorus (P), and iron (Fe)) in the aerosols and their stoichiometry. Striking north-south gradients are evident over both basins with the Northern Hemisphere more impacted by terrestrial dust sources and anthropogenic emissions and the North Atlantic apparently more impacted than the North Pacific. We estimate the atmospheric supply rates of these nutrients and the potential impact of the atmospheric deposition on the tropical western Pacific. Our results suggest that the atmospheric deposition is P deficient relative to the needs of the resident phytoplankton. These findings suggest that atmospheric supply of N, Fe, and P increases primary productivity utilizing some of the residual excess phosphorus (P*) in the surface waters to compensate for aerosol P deficiency. Regional primary productivity is further enhanced via the stimulation of nitrogen fixation fuelled by the residual atmospheric iron and P*. Our stoichiometric calculations reveal that a P* of 0.1 μmol L À1 can offset the P deficiency in atmospheric supply for many months. This study suggests that atmospheric deposition may sustain~10% of primary production in both the western tropical Pacific.
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