Interpreting methane variations in the past two decades using measurements of CH4 mixing ratio and isotopic composition

The availability 13C-CH4 measurements from atmospheric samples has significantly improved in recent years, which allows the construction of time series spanning up to about 2 decades. We have used these measurements to investigate the cause of the methane growth rate decline since 1980, with a special focus on the period 1998–2006 when the methane growth came to a halt. The constraints provided by the CH4 and 13C-CH4 measurements are used to construct hypothetical source and sink scenarios, which are translated into corresponding atmospheric concentrations using the atmospheric transport model TM3 for evaluation against the measurements. The base scenario, composed of anthropogenic emissions according to EDGAR 4.0, constant emissions from natural sources, and a constant atmospheric lifetime, overestimates the observed global growth rates of CH4 and 13C-CH4 by, respectively, 10 ppb yr−1 and 0.02‰yr−1 after the year 2000. It proves difficult to repair this inconsistency by modifying trends in emissions only, notably because a temporary reduction of isotopically light sources, such as natural wetlands, leads to a further increase of 13C-CH4. Furthermore, our results are difficult to reconcile with the estimated increase of 5 TgCH4 yr−1 in emissions from fossil fuel use in the period 2000–2005. On the other hand, we find that a moderate (less than 5% per decade) increase in the global OH concentration can bring the model in agreement with the measurements for plausible emission scenarios. This study demonstrates the value of global monitoring of methane isotopes, and calls for further investigation into the role OH and anthropogenic emissions to further improve our understanding of methane variations in recent years.JRC.H.2-Air and Climat

Atmospheric constraints on global emissions of methane from plants

We investigate whether a recently proposed large source of CH4 from vegetation can be reconciled with atmospheric measurements. Atmospheric transport model simulations with and without vegetation emissions are compared with background CH4, delta C-13-CH4 and satellite measurements. For present - day CH4 we derive an upper limit to the newly discovered source of 125 Tg CH4 yr(-1). Analysis of preindustrial CH4, however, points to 85 Tg CH4 yr(-1) as a more plausible limit. Model calculations with and without vegetation emissions show strikingly similar results at background surface monitoring sites, indicating that these measurements are rather insensitive to CH4 from plants. Simulations with 125 Tg CH4 yr(-1) vegetation emissions can explain up to 50% of the previously reported unexpectedly high CH4 column abundances over tropical forests observed by SCIAMACHY. Our results confirm the potential importance of vegetation emissions, and call for further research

Optimizing global CO emission estimates using a four-dimensional variational data assimilation system and surface network observations

We apply a four-dimensional variational (4D-VAR) data assimilation system to optimize carbon monoxide (CO) emissions for 2003 and 2004 and to reduce the uncertainty of emission estimates from individual sources using the chemistry transport model TM5. The system is designed to assimilate large (satellite) datasets, but in the current study only a limited amount of surface network observations from the National Oceanic and Atmospheric Administration Earth System Research Laboratory (NOAA/ESRL) Global Monitoring Division (GMD) is used to test the 4D-VAR system. By design, the system is capable to adjust the emissions in such a way that the posterior simulation reproduces background CO mixing ratios and large-scale pollution events at background stations. Uncertainty reduction up to 60 % in yearly emissions is observed over well-constrained regions and the inferred emissions compare well with recent studies for 2004. However, with the limited amount of data from the surface network, the system becomes data sparse resulting in a large solution space. Sensitivity studies have shown that model uncertainties (e.g., vertical distribution of biomass burning emissions and the OH field) and the prior inventories used, influence the inferred emission estimates. Also, since the observations only constrain total CO emissions, the 4D-VAR system has difficulties in separating anthropogenic and biogenic sources in particular. The inferred emissions are validated with NOAA aircraft data over North America and the agreement is significantly improved from the prior to posterior simulation. Validation with the Measurements Of Pollution In The Troposphere (MOPITT) instrument version 4 (V4) shows a slight improved agreement over the well-constrained Northern Hemisphere and in the tropics (except for the African continent). However, the model simulation with posterior emissions underestimates MOPITT CO total columns on the remote Southern Hemisphere (SH) by about 10 %. This is caused by a reduction in SH CO sources mainly due to surface stations on the high southern latitudes

Changes in the Isotopic Signature of Atmospheric Nitrous Oxide and Its Global Average Source During the Last Three Millennia

Nitrous oxide (N2O) is a strong greenhouse gas whose mole fraction in the atmosphere has increased over the industrial period. We present a new set of isotope measurements of N2O in air extracted from ice cores covering the last 3,000 years. For the preindustrial (PI) atmosphere, we find an average N2O mole fraction of (267 ± 1) nmol/mol and average tropospheric N2O isotopic values of δ15Nav PI = (9.5 ± 0.1)‰, δ18OPI = (47.1 ± 0.2)‰, δ15Nα PI = (17.8 ± 0.4)‰, and δ15Νβ PI = (1.2 ± 0.4)‰. From PI to modern times all isotope signatures decreased with a total change of δ15Nav = (−2.7 ± 0.2)‰, δ18O = (−2.5 ± 0.4)‰, δ15Nα = (−2.0 ± 0.7)‰, and δ15Νβ (−3.5 ± 0.7)‰. Interestingly, the temporal evolution is not the same for δ15Nav and δ18O. δ18O trends are relatively larger during the early part, and δ15Nav trends are larger during the late part of the industrial period, implying a decoupling of sources over the industrial period. Using a mass balance model, we determined the isotopic composition of the total average N2O source. Assuming that the total present source is the sum of a constant natural source and an increasing anthropogenic source, this anthropogenic source has an isotopic signature of δ15Nav source,anthrop = (−15.0 ± 2.6)‰, δ18Osource,anthrop = (30.0 ± 2.6)‰, δ15Nα source,anthrop = (−4.5 ± 1.7)‰, and δ15Nβ source,anthrop = (−24.0 ± 8.4)‰. The 15N site preference of the source has increased since PI times, which is indicative of a relative shift from denitrification to nitrification sources, consistent with agricultural emissions playing a major role in the N2O increase.SCOPUS: ar.jinfo:eu-repo/semantics/publishe

HESS opinions: a perspective on isotope versus non-isotope approaches to determine the contribution of transpiration to total evaporation

Current techniques to disentangle the evaporative fluxes from the continental surface into a contribution evaporated from soils and canopy, or transpired by plants, are under debate. Many isotope-based studies show that transpiration contributes generally more than 70% to the total evaporation, while other isotope-independent techniques lead to considerably smaller transpiration fractions. This paper provides a perspective on isotope-based versus non-isotope-based partitioning studies. Some partitioning results from isotope-based methods, hydrometric measurements, and modeling are presented for comparison. Moreover, the methodological aspects of the partitioning analysis are considered, including their limitations, and explanations of possible discrepancies between the methods are discussed. We suggest sources of systematic error that may lead to biases in the results, e.g., instruments inaccuracy, assumptions used in analyses, and calibration parameters. A number of comparison studies using isotope-based methods and hydrometric measurements in the same plants and climatic conditions are consistent within the errors; however, models tend to produce lower transpiration fractions. The relatively low transpiration fraction in current state-of-the-art land-surface models calls for a reassessment of the skill of the underlying model parameterizations. The scarcity of global evaporation data makes calibration and validation of global isotope-independent and isotope-based results difficult. However, isotope-enabled land-surface and global climate modeling studies allow for the evaluation of the parameterization of land-surface models by comparing the computed water isotopologue signals in the atmosphere with the available remote sensing and flux-based data sets. Future studies that allow for this evaluation could provide a better understanding of the hydrological cycle in vegetated regions

Analysis of global methane changes after the 1991 Pinatubo volcanic eruption

The global methane (CH4) growth rate showed large variations after the eruption of Mount Pinatubo in June 1991. Both sources and sinks of tropospheric CH4 were altered following the eruption, by feedback processes between climate and tropospheric photochemistry. Such processes include Ultra Violet (UV) radiative changes due to the presence of volcanic sulfur dioxide (SO2) and sulphate aerosols in the stratosphere, and due to stratospheric ozone depletion. Changes in temperature and water vapour in the following years caused changes in tropospheric chemistry, as well as in natural emissions. We present a sensitivity study that investigates the relative effects that these processes had on tropospheric CH4 concentrations, using a simple one-dimensional chemistry model representative for the global tropospheric column. To infer the changes in UV radiative fluxes, the chemistry model is coupled to a radiative transfer model. We find that the overall effect of natural processes after the eruption on the CH4 growth rate is dominated by the reduction in CH4 lifetime due to stratospheric ozone depletion. However, all the other processes are found to have non-negligible effects, and should therefore be taken into account in order to obtain a good estimate of CH4 concentrations after Pinatubo. We find that the overall effect was a small initial increase in the CH4 growth rate after the eruption, followed by a decrease of about 7 ppb yr(-1) by mid-1993. When changes in anthropogenic emissions are employed according to emission inventories, an additional decrease of about 5 ppb yr(-1) in the CH4 growth rate is obtained between the years 1991 and 1993. The results using the simplified single column model are in good qualitative agreement with observed changes in the CH4 growth rate. Further analysis, taking into account changes in the dynamics of the atmosphere, variations in emissions from biomass burning, and in biogenic emissions of non-methane volatile organic compounds (NMVOC), requires the use of a full three-dimensional model

Effect of UV radiation and temperature on the emission of methane from plant biomass and structural components

The recently reported finding that plant matter and living plants produce significant amounts of the important greenhouse gas methane under aerobic conditions has led to an intense scientific and public controversy. Whereas some studies question the up-scaling method that was used to estimate the global source strength, others have suggested that experimental artifacts could have caused the reported signals, and two studies, one based on isotope labeling, have recently reported the absence of CH<sub>4</sub> emissions from plants. Here we show – using several independent experimental analysis techniques – that dry and detached fresh plant matter, as well as several structural plant components, emit significant amounts of methane upon irradiation with UV light and/or heating. Emissions from UV irradiation are almost instantaneous, indicating a direct photochemical process. Long-time irradiation experiments demonstrate that the size of the CH<sub>4</sub> producing reservoir is large, exceeding potential interferences from degassing or desorption processes by several orders of magnitude. A dry leaf of a pure <sup>13</sup>C plant produces <sup>13</sup>CH<sub>4</sub> at a similar rate as dry leaves of non-labeled plants produce non-labeled methane

Результати ексгумації останків загиблих солдатів у центрі селища Цумань у 2010 р.

В статті висвітлюються результати археологічних досліджень Цуманської рятівної експедицією ДП « Волинські Старожитності» ДП НДЦ ОАСУ ІА НАН України, проведених у червні 2010 р. на місцезнаходженні останків солдатів Червоної армії часів Другої світової війни у центрі селища Цумань Ківерцівського району Волинської області