From 2007 to 2013, the globally averaged mole fraction of methane in the atmosphere increased by 5.7 ± 1.2 ppb yr À1. Simultaneously, δ 13 C CH4 (a measure of the 13 C/ 12 C isotope ratio in methane) has shifted to significantly more negative values since 2007. Growth was extreme in 2014, at 12.5 ± 0.4 ppb, with a further shift to more negative values being observed at most latitudes. The isotopic evidence presented here suggests that the methane rise was dominated by significant increases in biogenic methane emissions, particularly in the tropics, for example, from expansion of tropical wetlands in years with strongly positive rainfall anomalies or emissions from increased agricultural sources such as ruminants and rice paddies. Changes in the removal rate of methane by the OH radical have not been seen in other tracers of atmospheric chemistry and do not appear to explain short-term variations in methane. Fossil fuel emissions may also have grown, but the sustained shift to more 13 C-depleted values and its significant interannual variability, and the tropical and Southern Hemisphere loci of post-2007 growth, both indicate that fossil fuel emissions have not been the dominant factor driving the increase. A major cause of increased tropical wetland and tropical agricultural methane emissions, the likely major contributors to growth, may be their responses to meteorological change.

Atmospheric methane grew very rapidly in 2014 (12.7 ± 0.5 ppb/year), 2015 (10.1 ± 0.7 ppb/year), 2016 (7.0 ± 0.7 ppb/year), and 2017 (7.7 ± 0.7 ppb/year), at rates not observed since the 1980s. The increase in the methane burden began in 2007, with the mean global mole fraction in remote surface background air rising from about 1,775 ppb in 2006 to 1,850 ppb in 2017. Simultaneously the 13C/12C isotopic ratio (expressed as δ13CCH4) has shifted, now trending negative for more than a decade. The causes of methane's recent mole fraction increase are therefore either a change in the relative proportions (and totals) of emissions from biogenic and thermogenic and pyrogenic sources, especially in the tropics and subtropics, or a decline in the atmospheric sink of methane, or both. Unfortunately, with limited measurement data sets, it is not currently possible to be more definitive. The climate warming impact of the observed methane increase over the past decade, if continued at >5 ppb/year in the coming decades, is sufficient to challenge the Paris Agreement, which requires sharp cuts in the atmospheric methane burden. However, anthropogenic methane emissions are relatively very large and thus offer attractive targets for rapid reduction, which are essential if the Paris Agreement aims are to be attained.

Isotopic data provide powerful constraints on regional and global methane emissions and their source profiles. However, inverse modeling of spatially resolved methane flux is currently constrained by a lack of information on the variability of source isotopic signatures. In this study, isotopic signatures of emissions in the Fennoscandian Arctic have been determined in chambers over wetland, in the air 0.3 to 3 m above the wetland surface and by aircraft sampling from 100 m above wetlands up to the stratosphere. Overall, the methane flux to atmosphere has a coherent δ 13 C isotopic signature of À71 ± 1‰, measured in situ on the ground in wetlands. This is in close agreement with δ 13 C isotopic signatures of local and regional methane increments measured by aircraft campaigns flying through air masses containing elevated methane mole fractions. In contrast, results from wetlands in Canadian boreal forest farther south gave isotopic signatures of À67 ± 1‰. Wetland emissions dominate the local methane source measured over the European Arctic in summer. Chamber measurements demonstrate a highly variable methane flux and isotopic signature, but the results from air sampling within wetland areas show that emissions mix rapidly immediately above the wetland surface and methane emissions reaching the wider atmosphere do indeed have strongly coherent C isotope signatures. The study suggests that for boreal wetlands (>60°N) global and regional modeling can use an isotopic signature of À71‰ to apportion sources more accurately, but there is much need for further measurements over other wetlands regions to verify this.

Tropical methane sources are an important part of the global methane budget and include natural wetlands, rice agriculture, biomass burning, ruminants, fossil fuels, and waste. δ13CCH4 can provide strong constraints on methane source apportionment. For example, tropical wetlands in this study give δ13CCH4 values between −61.5 ± 2.9‰ and −53.0 ± 0.4‰ and in general are more enriched in 13C than temperate and boreal wetlands. However, thus far, relatively few measurements of δ13CCH4 in methane‐enriched air have been made in the tropics. In this study samples have been collected from tropical wetland, rice, ruminant, and biomass burning emissions to the atmosphere. Regional isotopic signatures vary greatly as different processes and source material affect methane signatures. Measurements were made to determine bulk source inputs to the atmosphere, rather than to study individual processes. These measurements provide inputs for regional methane budget models, to constrain emissions with better source apportionment.

As part of an NERC-funded project investigating the southern methane anomaly, a team drawn from the Universities of Bristol, Birmingham and Royal Holloway flew small unmanned multirotors from Ascension Island for the purposes of atmospheric sampling. The objective of these flights was to collect air samples from below, within and above a persistent atmospheric feature, the Trade Wind Inversion, in order to characterise methane concentrations and their isotopic composition. These parameters allow the methane in the different air masses to be tied to different source locations, which can be further analysed using back trajectory atmospheric computer modelling. This paper describes the campaigns as a whole including the design of the bespoke eight rotor aircraft and the operational requirements that were needed in order to collect targeted multiple air samples up to 2.5 km above the ground level in under 20 min of flight time. Key features of the system described include real-time feedback of temperature and humidity, as well as system health data. This enabled detailed targeting of the air sampling design to be realised and planned during the flight mission on the downward leg, a capability that is invaluable in the presence of uncertainty in the pre-flight meteorological data. Environmental considerations are also outlined together with the flight plans that were created in order to rapidly fly vertical transects of the atmosphere whilst encountering changing wind conditions. Two sampling campaigns were carried out in September 2014 and July 2015 with over one hundred high altitude sampling missions. Lessons learned are given throughout, including those associated with operating in the testing environment encountered on Ascension Island.