Atmospheric Lifetime Of Methane Research Articles

Atmospheric methane since the last glacial maximum was driven by wetland sources

Abstract. Atmospheric methane (CH4) has changed considerably in the time between the last glacial maximum (LGM) and the preindustrial (PI) periods. We investigate these changes in transient experiments with an Earth system model capable of simulating the global methane cycle interactively, focusing on the rapid changes during the deglaciation, especially pronounced in the Bølling–Allerød (BA) and Younger Dryas (YD) periods. We consider all relevant natural sources and sinks of methane and examine the drivers of changes in methane emissions as well as in the atmospheric lifetime of methane. We find that the evolution of atmospheric methane is largely driven by emissions from tropical wetlands, while variations in the methane atmospheric lifetime are small but not negligible. Our model reproduces most changes in atmospheric methane very well, with the exception of the mid-Holocene decrease in methane, although the timing of ice-sheet meltwater fluxes needs to be adjusted slightly in order to exactly reproduce the variations in the BA and YD.

UV production of methane from surface and sedimenting IDPs on Mars in light of REMS data and with insights for TGO

This paper refines model predictions for the production of methane from UV-irradiated interplanetary dust particles (IDPs) now that the Rover Environmental Monitoring Station (REMS) instrument onboard the Mars Science Laboratory (MSL) Rover has made the first measurements of the UV environment on the surface of Mars, at Gale Crater. Once these measurements are included in a UV radiative transfer model, we find that modelled UV sol-integrated energies across the planet are lower than pre-measurement estimates by 35% on average, considering all latitudes and seasons. This reduction, in turn, reduces the predicted production of methane from individual accreting IDPs, extending their lifetimes and increasing the surface concentration of organics that must accumulate in order to emit sufficient methane to balance the accretion of organic compounds to Mars. Emission from reasonable accumulations of IDPs could range up to ∼7.9 × 10−4 ppbv sol−1. Richer deposits of organic carbon at the surface may emit methane at no more than 3.9 ppbv sol−1. An examination of IDP-derived methane production during atmospheric settling indicates that no more than 0.32% of organic carbon from meteor streams may be deposited in the atmosphere. Thus, such a process cannot explain either the spikes observed in methane nor the low equilibrium values observed by MSL. Instead, this discrepancy may be explained if < 80 tons per year of organic carbon survives to the surface, the atmospheric lifetime of methane is < 110 years or the efficiency of the UV-CH4 process is <7%. Under the assumption of reduced carbon input cycling in the Martian system from these processes, both soil concentrations of organic carbon and atmospheric measurements of methane observed by MSL are consistent with the UV-CH4 process. This refinement of methane production from IDPs and its geographical and vertical distribution will be an important input for models attempting to understand the results to be derived from the Trace Gas Orbiter (TGO) mission that will map methane concentrations in the martian atmosphere in 2018 at 0.01 ppbv.

Modeling the observed tropospheric BrO background: Importance of multiphase chemistry and implications for ozone, OH, and mercury

AbstractAircraft and satellite observations indicate the presence of ppt (ppt ≡ pmol/mol) levels of BrO in the free troposphere with important implications for the tropospheric budgets of ozone, OH, and mercury. We can reproduce these observations with the GEOS‐Chem global tropospheric chemistry model by including a broader consideration of multiphase halogen (Br‐Cl) chemistry than has been done in the past. Important reactions for regenerating BrO from its nonradical reservoirs include HOBr + Br−/Cl− in both aerosols and clouds, and oxidation of Br− by ClNO3 and ozone. Most tropospheric BrO in the model is in the free troposphere, consistent with observations and originates mainly from the photolysis and oxidation of ocean‐emitted CHBr3. Stratospheric input is also important in the upper troposphere. Including production of gas phase inorganic bromine from debromination of acidified sea salt aerosol increases free tropospheric Bry by about 30%. We find HOBr to be the dominant gas‐phase reservoir of inorganic bromine. Halogen (Br‐Cl) radical chemistry as implemented here in GEOS‐Chem drives 14% and 11% decreases in the global burdens of tropospheric ozone and OH, respectively, a 16% increase in the atmospheric lifetime of methane, and an atmospheric lifetime of 6 months for elemental mercury. The dominant mechanism for the Br‐Cl driven tropospheric ozone decrease is oxidation of NOx by formation and hydrolysis of BrNO3 and ClNO3.

Aviation NOx-induced CH4 effect: Fixed mixing ratio boundary conditions versus flux boundary conditions

Atmospheric chemistry-climate models are often used to calculate the effect of aviation NOx emissions on atmospheric ozone (O3) and methane (CH4). Due to the long (∼10 yr) atmospheric lifetime of methane, model simulations must be run for long time periods, typically for more than 40 simulation years, to reach steady-state if using CH4 emission fluxes. Because of the computational expense of such long runs, studies have traditionally used specified CH4 mixing ratio lower boundary conditions (BCs) and then applied a simple parameterization based on the change in CH4 lifetime between the control and NOx-perturbed simulations to estimate the change in CH4 concentration induced by NOx emissions. In this parameterization a feedback factor (typically a value of 1.4) is used to account for the feedback of CH4 concentrations on its lifetime. Modeling studies comparing simulations using CH4 surface fluxes and fixed mixing ratio BCs are used to examine the validity of this parameterization. The latest version of the Community Earth System Model (CESM), with the CAM5 atmospheric model, was used for this study. Aviation NOx emissions for 2006 were obtained from the AEDT (Aviation Environmental Design Tool) global commercial aircraft emissions. Results show a 31.4 ppb change in CH4 concentration when estimated using the parameterization and a 1.4 feedback factor, and a 28.9 ppb change when the concentration was directly calculated in the CH4 flux simulations. The model calculated value for CH4 feedback on its own lifetime agrees well with the 1.4 feedback factor. Systematic comparisons between the separate runs indicated that the parameterization technique overestimates the CH4 concentration by 8.6%. Therefore, it is concluded that the estimation technique is good to within ∼10% and decreases the computational requirements in our simulations by nearly a factor of 8.

Simulation of tropospheric chemistry and aerosols with the climate model EC-Earth

Abstract. We have integrated the atmospheric chemistry and transport model TM5 into the global climate model EC-Earth version 2.4. We present an overview of the TM5 model and the two-way data exchange between TM5 and the IFS model from the European Centre for Medium-Range Weather Forecasts (ECMWF), the atmospheric general circulation model of EC-Earth. In this paper we evaluate the simulation of tropospheric chemistry and aerosols in a one-way coupled configuration. We have carried out a decadal simulation for present-day conditions and calculated chemical budgets and climatologies of tracer concentrations and aerosol optical depth. For comparison we have also performed offline simulations driven by meteorological fields from ECMWF's ERA-Interim reanalysis and output from the EC-Earth model itself. Compared to the offline simulations, the online-coupled system produces more efficient vertical mixing in the troposphere, which reflects an improvement of the treatment of cumulus convection. The chemistry in the EC-Earth simulations is affected by the fact that the current version of EC-Earth produces a cold bias with too dry air in large parts of the troposphere. Compared to the ERA-Interim driven simulation, the oxidizing capacity in EC-Earth is lower in the tropics and higher in the extratropics. The atmospheric lifetime of methane in EC-Earth is 9.4 years, which is 7% longer than the lifetime obtained with ERA-Interim but remains well within the range reported in the literature. We further evaluate the model by comparing the simulated climatologies of surface radon-222 and carbon monoxide, tropospheric and surface ozone, and aerosol optical depth against observational data. The work presented in this study is the first step in the development of EC-Earth into an Earth system model with fully interactive atmospheric chemistry and aerosols.

Global terrestrial isoprene emission models: sensitivity to variability in climate and vegetation

Abstract. Due to its effects on the atmospheric lifetime of methane, the burdens of tropospheric ozone and growth of secondary organic aerosol, isoprene is central among the biogenic compounds that need to be taken into account for assessment of anthropogenic air pollution-climate change interactions. Lack of process-understanding regarding leaf isoprene production as well as of suitable observations to constrain and evaluate regional or global simulation results add large uncertainties to past, present and future emissions estimates. Focusing on contemporary climate conditions, we compare three global isoprene models that differ in their representation of vegetation and isoprene emission algorithm. We specifically aim to investigate the between- and within model variation that is introduced by varying some of the models' main features, and to determine which spatial and/or temporal features are robust between models and different experimental set-ups. In their individual standard configurations, the models broadly agree with respect to the chief isoprene sources and emission seasonality, with maximum monthly emission rates around 20–25 Tg C, when averaged by 30-degree latitudinal bands. They also indicate relatively small (approximately 5 to 10 % around the mean) interannual variability of total global emissions. The models are sensitive to changes in one or more of their main model components and drivers (e.g., underlying vegetation fields, climate input) which can yield increases or decreases in total annual emissions of cumulatively by more than 30 %. Varying drivers also strongly alters the seasonal emission pattern. The variable response needs to be interpreted in view of the vegetation emission capacities, as well as diverging absolute and regional distribution of light, radiation and temperature, but the direction of the simulated emission changes was not as uniform as anticipated. Our results highlight the need for modellers to evaluate their implementations of isoprene emission models carefully when performing simulations that use non-standard emission model configurations.

Large methane releases lead to strong aerosol forcing and reduced cloudiness

Abstract. The release of vast quantities of methane into the atmosphere as a result of clathrate destabilization is a potential mechanism for rapid amplification of global warming. Previous studies have calculated the enhanced warming based mainly on the radiative effect of the methane itself, with smaller contributions from the associated carbon dioxide or ozone increases. Here, we study the effect of strongly elevated methane (CH4) levels on oxidant and aerosol particle concentrations using a combination of chemistry-transport and general circulation models. A 10-fold increase in methane concentrations is predicted to significantly decrease hydroxyl radical (OH) concentrations, while moderately increasing ozone (O3). These changes lead to a 70 % increase in the atmospheric lifetime of methane, and an 18 % decrease in global mean cloud droplet number concentrations (CDNC). The CDNC change causes a radiative forcing that is comparable in magnitude to the longwave radiative forcing ("enhanced greenhouse effect") of the added methane. Together, the indirect CH4-O3 and CH4-OH-aerosol forcings could more than double the warming effect of large methane increases. Our findings may help explain the anomalously large temperature changes associated with historic methane releases.

Changing boreal methane sources and constant biomass burning during the last termination

Past atmospheric methane concentrations show strong fluctuations in parallel to rapid glacial climate changes in the Northern Hemisphere superimposed on a glacial-interglacial doubling of methane concentrations. The processes driving the observed fluctuations remain uncertain but can be constrained using methane isotopic information from ice cores. Here we present an ice core record of carbon isotopic ratios in methane over the entire last glacial-interglacial transition. Our data show that the carbon in atmospheric methane was isotopically much heavier in cold climate periods. With the help of a box model constrained by the present data and previously published results, we are able to estimate the magnitude of past individual methane emission sources and the atmospheric lifetime of methane. We find that methane emissions due to biomass burning were about 45 Tg methane per year, and that these remained roughly constant throughout the glacial termination. The atmospheric lifetime of methane is reduced during cold climate periods. We also show that boreal wetlands are an important source of methane during warm events, but their methane emissions are essentially shut down during cold climate conditions.