M. Cain

Rising atmospheric methane: 2007-2014 growth and isotopic shift

From 2007 to 2013, the globally averaged mole fraction of methane in the atmosphere increased by 5.7u2009±u20091.2u2009ppbu2009yr−1. Simultaneously, δ13CCH4 (a measure of the 13C/12C isotope ratio in methane) has shifted to significantly more negative values since 2007. Growth was extreme in 2014, at 12.5u2009±u20090.4u2009ppb, 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 13C-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.

Extensive release of methane from Arctic seabed west of Svalbard during summer 2014 does not influence the atmosphere

We find that summer methane (CH4) release from seabed sediments west of Svalbard substantially increases CH4 concentrations in the ocean but has limited influence on the atmospheric CH4 levels. Our conclusion stems from complementary measurements at the seafloor, in the ocean, and in the atmosphere from land-based, ship and aircraft platforms during a summer campaign in 2014. We detected high concentrations of dissolved CH4 in the ocean above the seafloor with a sharp decrease above the pycnocline. Model approaches taking potential CH4 emissions from both dissolved and bubble-released CH4 from a larger region into account reveal a maximum flux compatible with the observed atmospheric CH4 mixing ratios of 2.4–3.8u2009nmolu2009m−2u2009s−1. This is too low to have an impact on the atmospheric summer CH4 budget in the year 2014. Long-term ocean observatories may shed light on the complex variations of Arctic CH4 cycles throughout the year.

Measurement of the 13C isotopic signature of methane emissions from northern European wetlands

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 3u2009m above the wetland surface and by aircraft sampling from 100u2009m above wetlands up to the stratosphere. Overall, the methane flux to atmosphere has a coherent δ13C isotopic signature of −71u2009±u20091‰, measured in situ on the ground in wetlands. This is in close agreement with δ13C 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 −67u2009±u20091‰. 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 −71‰ to apportion sources more accurately, but there is much need for further measurements over other wetlands regions to verify this.

Implications of possible interpretations of ‘greenhouse gas balance’ in the Paris Agreement

The main goal of the Paris Agreement as stated in Article 2 is ‘holding the increase in the global average temperature to well below 2°C above pre-industrial levels and pursuing efforts to limit the temperature increase to 1.5°C’. Article 4 points to this long-term goal and the need to achieve ‘balance between anthropogenic emissions by sources and removals by sinks of greenhouse gases. This statement on ‘greenhouse gas balance’ is subject to interpretation, and clarifications are needed to make it operational for national and international climate policies. We study possible interpretations from a scientific perspective and analyse their climatic implications. We clarify how the implications for individual gases depend on the metrics used to relate them. We show that the way in which balance is interpreted, achieved and maintained influences temperature outcomes. Achieving and maintaining net-zero CO2-equivalent emissions conventionally calculated using GWP100 (100-year global warming potential) and including substantial positive contributions from short-lived climate-forcing agents such as methane would result in a sustained decline in global temperature. A modified approach to the use of GWP100 (that equates constant emissions of short-lived climate forcers with zero sustained emission of CO2) results in global temperatures remaining approximately constant once net-zero CO2-equivalent emissions are achieved and maintained. Our paper provides policymakers with an overview of issues and choices that are important to determine which approach is most appropriate in the context of the Paris Agreement. This article is part of the theme issue ‘The Paris Agreement: understanding the physical and social challenges for a warming world of 1.5°C above pre-industrial levels.

Measurements of δ13C in CH4 and using particle dispersion modeling to characterize sources of arctic methane within an air mass

Abstract A stratified air mass enriched in methane (CH4) was sampled at ~600u2009m to ~2000u2009m altitude, between the north coast of Norway and Svalbard as part of the Methane in the Arctic: Measurements and Modelling campaign on board the UKs BAe‐146‐301 Atmospheric Research Aircraft. The approach used here, which combines interpretation of multiple tracers with transport modeling, enables better understanding of the emission sources that contribute to the background mixing ratios of CH4 in the Arctic. Importantly, it allows constraints to be placed on the location and isotopic bulk signature of the emission source(s). Measurements of δ13C in CH4 in whole air samples taken while traversing the air mass identified that the source(s) had a strongly depleted bulk δ13C CH4 isotopic signature of −70 (±2.1)‰. Combined Numerical Atmospheric‐dispersion Modeling Environment and inventory analysis indicates that the air mass was recently in the planetary boundary layer over northwest Russia and the Barents Sea, with the likely dominant source of methane being from wetlands in that region.

Sensitivity of tropospheric ozone to chemical kinetic uncertainties in air masses influenced by anthropogenic and biomass burning emissions

We use a Lagrangian chemical transport model with a Monte Carlo approach to determine impacts of kinetic rate uncertainties on simulated concentrations of ozone, NOy and OH in a high-altitude biomass burning plume and a low-level industrial pollution plume undergoing long-range transport. Uncertainties in kinetic rate constants yield 10–12 ppbv (5th to 95th percentile) uncertainty in the ozone concentration, dominated by reactions that cycle NO and NO2, control NOx conversion to NOy reservoir species, and key reactions contributing to O3 loss (O(1D) + H2O, HO2 + O3). Our results imply that better understanding of the peroxyacetylnitrate (PAN) thermal decomposition constant is key to predicting large-scale O3 production from fire emissions and uncertainty in the reaction of NO + O3 at low temperatures is particularly important for both the anthropogenic and biomass burning plumes. The highlighted reactions serve as a useful template for targeting new laboratory experiments aimed at reducing uncertainties in our understanding of tropospheric O3 photochemistry.

The many possible climates from the Paris Agreement’s aim of 1.5 °C warming

The United Nations’ Paris Agreement includes the aim of pursuing efforts to limit global warming to only 1.5u2009°C above pre-industrial levels. However, it is not clear what the resulting climate would look like across the globe and over time. Here we show that trajectories towards a ‘1.5u2009°C warmer world’ may result in vastly different outcomes at regional scales, owing to variations in the pace and location of climate change and their interactions with society’s mitigation, adaptation and vulnerabilities to climate change. Pursuing policies that are considered to be consistent with the 1.5u2009°C aim will not completely remove the risk of global temperatures being much higher or of some regional extremes reaching dangerous levels for ecosystems and societies over the coming decades.The results of efforts to limit global mean warming to below 1.5u2009°C may include many possible future world climates.

A cautionary tale: A study of a methane enhancement over the North Sea

Airborne measurements of a methane (CH4) plume over the North Sea from August 2013 are analyzed. The plume was only observed downwind of circumnavigated gas fields, and three methods are used to determine its source. First, a mass balance calculation assuming a gas field source gives a CH4 emission rate between 2.5±0.8x104 and 4.6±1.5x104 kg h−1. This would be greater than the industry target of a 0.5% leak rate if it were emitting for more than half the time. Second, annual average UK CH4 emissions are combined with an atmospheric dispersion model to create pseudo-observations. Clean air from the North Atlantic passed over mainland UK, picking up anthropogenic emissions. To best explain the observed plume using pseudo-observations, an additional North Sea source from the gas rigs area is added. Third, the δ13C-CH4 from the plume is shown to be -53%0, which is lighter than fossil gas but heavier than the UK average emission. We conclude that either an additional small-area mainland source is needed, combined with temporal variability in emission or transport in small-scale meteorological features. Alternatively, a combination of additional sources that are at least 75% from the mainland (-58%0) and up to 25% from the North Sea gas rigs area (-32%0) would explain the measurements. Had the isotopic analysis not been performed, the likely conclusion would have been of a gas field source of CH4. This demonstrates the limitation of analysing mole fractions alone, as the simplest explanation is rejected based on analysis of isotopic data.

Methane mole fraction and δ13C above and below the trade wind inversion at Ascension Island in air sampled by aerial robotics

Ascension Island is a remote South Atlantic equatorial site, ideal for monitoring tropical background CH4. In September 2014 and July 2015, octocopters were used to collect air samples in Tedlar bags from different heights above and below the well-defined Trade Wind Inversion (TWI), sampling a maximum altitude of 2700 meters above mean sea-level. Sampling captured both remote air in the marine boundary layer below the TWI, and also air masses above the TWI that had been lofted by convective systems in the African tropics. Air above the TWI was characterized by higher CH4 but no distinct shift in δ13C was observed compared to the air below. Back-trajectories indicate that lofted CH4 emissions from southern hemisphere Africa have bulk δ13CCH4 signatures similar to background, suggesting mixed emissions from wetlands, agriculture and biomass burning. The campaigns illustrate the usefulness of UAS sampling, and Ascensions value for atmospheric measurement in an understudied region.

A solution to the misrepresentations of CO 2 -equivalent emissions of short-lived climate pollutants under ambitious mitigation

While cumulative carbon dioxide (CO2) emissions dominate anthropogenic warming over centuries, temperatures over the coming decades are also strongly affected by short-lived climate pollutants (SLCPs), complicating the estimation of cumulative emission budgets for ambitious mitigation goals. Using conventional Global Warming Potentials (GWPs) to convert SLCPs to “CO2-equivalent” emissions misrepresents their impact on global temperature. Here we show that peak warming under a range of mitigation scenarios is determined by a linear combination of cumulative CO2 emissions to the time of peak warming and non-CO2 radiative forcing immediately prior to that time. This may be understood by expressing aggregate non-CO2 forcing as cumulative CO2 forcing-equivalent (CO2-fe) emissions. We show further that contributions to CO2-fe emissions are well approximated by a new usage of GWP, denoted GWP*, which relates cumulative CO2 emissions to date with the current rate of emission of SLCPs. GWP* accurately indicates the impact of emissions of both long-lived and short-lived pollutants on radiative forcing and temperatures over a wide range of timescales, including under ambitious mitigation when conventional GWPs fail. Measured by GWP*, implementing the Paris Agreement would reduce the expected rate of warming in 2030 by 28% relative to a No Policy scenario. Expressing mitigation efforts in terms of their impact on future cumulative emissions aggregated using GWP* would relate them directly to contributions to future warming, better informing both burden-sharing discussions and long-term policies and measures in pursuit of ambitious global temperature goals.Climate mitigation: An improved emission metricA new approach allows the temperature forcing of CO2 and short-lived climate pollutants (SLCPs) to be examined under a common cumulative framework. While anthropogenic warming is largely determined by cumulative emissions of CO2, SLCPs—including soot, other aerosols and methane—also play a role. Quantifying their impact on global temperature is, however, distorted by existing methodologies using conventional Global Warming Potentials (GWP) to convert SLCPs to CO2-equivalent emissions. A team of international scientists led by Myles Allen at the University of Oxford provide a solution. A modified form of GWP—GWP*, which relates cumulative CO2 emissions with contemporary SLCP emissions—is shown to better represent the future climate forcing of both long- and short-term pollutants. Use of GWP* could improve climate policy design, benefiting mitigation strategies to achieve the Paris Agreement targets.