Renewed growth of atmospheric methane Rigby, M.; Prinn, R. G.; Fraser, P. J. ...
Geophysical research letters,
November 2008, Letnik:
35, Številka:
22
Journal Article
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Following almost a decade with little change in global atmospheric methane mole fraction, we present measurements from the Advanced Global Atmospheric Gases Experiment (AGAGE) and the Australian ...Commonwealth Scientific and Industrial Research Organisation (CSIRO) networks that show renewed growth starting near the beginning of 2007. Remarkably, a similar growth rate is found at all monitoring locations from this time until the latest measurements. We use these data, along with an inverse method applied to a simple model of atmospheric chemistry and transport, to investigate the possible drivers of the rise. Specifically, the relative roles of an increase in emission rate or a decrease in concentration of the hydroxyl radical, the largest methane sink, are examined. We conclude that: 1) if the annual mean hydroxyl radical concentration did not change, a substantial increase in emissions was required simultaneously in both hemispheres between 2006 and 2007; 2) if a small drop in the hydroxyl radical concentration occurred, consistent with AGAGE methyl chloroform measurements, the emission increase is more strongly biased to the Northern Hemisphere.
This paper documents a global Bayesian variational inversion of CO2 surface fluxes during the period 1988–2008. Weekly fluxes are estimated on a 3.75° × 2.5° (longitude‐latitude) grid throughout the ...21 years. The assimilated observations include 128 station records from three large data sets of surface CO2 mixing ratio measurements. A Monte Carlo approach rigorously quantifies the theoretical uncertainty of the inverted fluxes at various space and time scales, which is particularly important for proper interpretation of the inverted fluxes. Fluxes are evaluated indirectly against two independent CO2 vertical profile data sets constructed from aircraft measurements in the boundary layer and in the free troposphere. The skill of the inversion is evaluated by the improvement brought over a simple benchmark flux estimation based on the observed atmospheric growth rate. Our error analysis indicates that the carbon budget from the inversion should be more accurate than the a priori carbon budget by 20% to 60% for terrestrial fluxes aggregated at the scale of subcontinental regions in the Northern Hemisphere and over a year, but the inversion cannot clearly distinguish between the regional carbon budgets within a continent. On the basis of the independent observations, the inversion is seen to improve the fluxes compared to the benchmark: the atmospheric simulation of CO2 with the Bayesian inversion method is better by about 1 ppm than the benchmark in the free troposphere, despite possible systematic transport errors. The inversion achieves this improvement by changing the regional fluxes over land at the seasonal and at the interannual time scales.
Methane is an important greenhouse gas, and its atmospheric concentration has nearly tripled since pre-industrial times. The growth rate of atmospheric methane is determined by the balance between ...surface emissions and photochemical destruction by the hydroxyl radical, the major atmospheric oxidant. Remarkably, this growth rate has decreased markedly since the early 1990s, and the level of methane has remained relatively constant since 1999, leading to a downward revision of its projected influence on global temperatures. Large fluctuations in the growth rate of atmospheric methane are also observed from one year to the next, but their causes remain uncertain. Here we quantify the processes that controlled variations in methane emissions between 1984 and 2003 using an inversion model of atmospheric transport and chemistry. Our results indicate that wetland emissions dominated the inter-annual variability of methane sources, whereas fire emissions played a smaller role, except during the 1997-1998 El Niño event. These top-down estimates of changes in wetland and fire emissions are in good agreement with independent estimates based on remote sensing information and biogeochemical models. On longer timescales, our results show that the decrease in atmospheric methane growth during the 1990s was caused by a decline in anthropogenic emissions. Since 1999, however, they indicate that anthropogenic emissions of methane have risen again. The effect of this increase on the growth rate of atmospheric methane has been masked by a coincident decrease in wetland emissions, but atmospheric methane levels may increase in the near future if wetland emissions return to their mean 1990s levels.
Celotno besedilo
Dostopno za:
DOBA, IJS, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
Atmospheric methane (CH4) increased from similar to 900 ppb (parts per billion, or nanomoles per mole of dry air) in 1900 to similar to 1800 ppb in 2010 at a rate unprecedented in any observational ...records. However, the contributions of the various methane sources and sinks to the CH4 increase are poorly understood. Here we use initial emissions from bottom-up inventories for anthropogenic sources, emissions from wetlands and rice paddies simulated by a terrestrial biogeochemical model, and an atmospheric general circulation model (AGCM)-based chemistry-transport model (i.e. ACTM) to simulate atmospheric CH4 concentrations for 1910-2010. The ACTM simulations are compared with the CH4 concentration records reconstructed from Antarctic and Arctic ice cores and firn air samples, and from direct measurements since the 1980s at multiple sites around the globe. The differences between ACTM simulations and observed CH4 concentrations are minimized to optimize the global total emissions using a mass balance calculation. During 1910-2010, the global total CH4 emission doubled from similar to 290 to similar to 580 Tg yr-1. Compared to optimized emission, the bottom-up emission data set underestimates the rate of change of global total CH4 emissions by similar to 30% during the high growth period of 1940-1990, while it overestimates by similar to 380% during the low growth period of 1990-2010. Further, using the CH4 stable carbon isotopic data ( delta 13C), we attribute the emission increase during 1940-1990 primarily to enhancement of biomass burning. The total lifetime of CH4 shortened from 9.4 yr during 1910-1919 to 9 yr during 2000-2009 by the combined effect of the increasing abundance of atomic chlorine radicals (Cl) and increases in average air temperature. We show that changes of CH4 loss rate due to increased tropospheric air temperature and CH4 loss due to Cl in the stratosphere are important sources of uncertainty to more accurately estimate the global CH4 budget from delta 13C observations.
Nanoscale resonators that oscillate at high frequencies are useful in many measurement applications. We studied a high-quality mechanical resonator made from a suspended carbon nanotube driven into ...motion by applying a periodic radio frequency potential using a nearby antenna. Single-electron charge fluctuations created periodic modulations of the mechanical resonance frequency. A quality factor exceeding 10⁵ allows the detection of a shift in resonance frequency caused by the addition of a single-electron charge on the nanotube. Additional evidence for the strong coupling of mechanical motion and electron tunneling is provided by an energy transfer to the electrons causing mechanical damping and unusual nonlinear behavior. We also discovered that a direct current through the nanotube spontaneously drives the mechanical resonator, exerting a force that is coherent with the high-frequency resonant mechanical motion.
Satellite retrievals of methane weighted atmospheric columns are assimilated within a Bayesian inversion system to infer the global and regional methane emissions and sinks for the period August 2009 ...to July 2010. Inversions are independently computed from three different space-borne observing systems and one surface observing system under several hypotheses for prior-flux and observation errors. Posterior methane emissions are compared and evaluated against surface mole fraction observations via a chemistry-transport model. Apart from SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CartograpHY), the simulations agree fairly well with the surface mole fractions. The most consistent configurations of this study using TANSO-FTS (Thermal And Near infrared Sensor for carbon Observation – Fourier Transform Spectrometer), IASI (Infrared Atmospheric Sounding Interferometer) or surface measurements induce posterior methane global emissions of, respectively, 565 ± 21 Tg yr−1, 549 ± 36 Tg yr−1 and 538 ± 15 Tg yr−1 over the one-year period August 2009–July 2010. This consistency between the satellite retrievals (apart from SCIAMACHY) and independent surface measurements is promising for future improvement of CH4 emission estimates by atmospheric inversions.
Computational anatomy studies typically use T1-weighted magnetic resonance imaging contrast to look at local differences in cortical thickness or grey matter volume across time or subjects. This type ...of analysis is a powerful and non-invasive tool to probe anatomical changes associated with neurodevelopment, aging, disease or experience-induced plasticity. However, these comparisons could suffer from biases arising from vascular and metabolic subject- or time-dependent differences. Differences in blood flow and volume could be caused by vasodilation or differences in vascular density, and result in a larger signal contribution of the blood compartment within grey matter voxels. Metabolic changes could lead to differences in dissolved oxygen in brain tissue, leading to T1 shortening. Here, we analyze T1 maps and T1-weighted images acquired during different breathing conditions (ambient air, hypercapnia (increased CO2) and hyperoxia (increased O2)) to evaluate the effect size that can be expected from changes in blood flow, volume and dissolved O2 concentration in computational anatomy studies. Results show that increased blood volume from vasodilation during hypercapnia is associated with an overestimation of cortical thickness (1.85%) and grey matter volume (3.32%), and that both changes in O2 concentration and blood volume lead to changes in the T1 value of tissue. These results should be taken into consideration when interpreting existing morphometry studies and in future study design. Furthermore, this study highlights the overlap in structural and physiological MRI, which are conventionally interpreted as two independent modalities.
•Increased blood volume leads to overestimation of grey matter thickness and volume.•Changes in O2 concentration and blood volume lead to changes in the T1 of tissue.•Changes in grey matter from blood volume cover most of cortex and are bilateral.•The impact of blood volume is on a similar scale as aging and diseases changes.
The recent increase of atmospheric methane is investigated by using two atmospheric inversions to quantify the distribution of sources and sinks for the 2006-2008 period, and a process-based model of ...methane emissions by natural wetland ecosystems. Methane emissions derived from the two inversions are consistent at a global scale: emissions are decreased in 2006 (-7 Tg) and increased in 2007 (+21 Tg) and 2008 (+18 Tg), as compared to the 1999-2006 period. The agreement on the latitudinal partition of the flux anomalies for the two inversions is fair in 2006, good in 2007, and not good in 2008. In 2007, a positive anomaly of tropical emissions is found to be the main contributor to the global emission anomalies (~60-80%) for both inversions, with a dominant share attributed to natural wetlands (~2/3), and a significant contribution from high latitudes (~25%). The wetland ecosystem model produces smaller and more balanced positive emission anomalies between the tropics and the high latitudes for 2006, 2007 and 2008, mainly due to precipitation changes during these years. At a global scale, the agreement between the ecosystem model and the inversions is good in 2008 but not satisfying in 2006 and 2007. Tropical South America and Boreal Eurasia appear to be major contributors to variations in methane emissions consistently in the inversions and the ecosystem model. Finally, changes in OH radicals during 2006-2008 are found to be less than 1% in inversions, with only a small impact on the inferred methane emissions.
Air was sampled from the porous firn layer at the NEEM site in Northern Greenland. We use an ensemble of ten reference tracers of known atmospheric history to characterise the transport properties of ...the site. By analysing uncertainties in both data and the reference gas atmospheric histories, we can objectively assign weights to each of the gases used for the depth-diffusivity reconstruction. We define an objective root mean square criterion that is minimised in the model tuning procedure. Each tracer constrains the firn profile differently through its unique atmospheric history and free air diffusivity, making our multiple-tracer characterisation method a clear improvement over the commonly used single-tracer tuning. Six firn air transport models are tuned to the NEEM site; all models successfully reproduce the data within a 1σ Gaussian distribution. A comparison between two replicate boreholes drilled 64 m apart shows differences in measured mixing ratio profiles that exceed the experimental error. We find evidence that diffusivity does not vanish completely in the lock-in zone, as is commonly assumed. The ice age- gas age difference (Δage) at the firn-ice transition is calculated to be 182+3−9 yr. We further present the first intercomparison study of firn air models, where we introduce diagnostic scenarios designed to probe specific aspects of the model physics. Our results show that there are major differences in the way the models handle advective transport. Furthermore, diffusive fractionation of isotopes in the firn is poorly constrained by the models, which has consequences for attempts to reconstruct the isotopic composition of trace gases back in time using firn air and ice core records.
It has recently been recognised that the strong spin-orbit interaction present in solids can lead to new phenomena, such as materials with non-trivial topological order. Although the atomic ...spin-orbit coupling in carbon is weak, the spin-orbit coupling in carbon nanotubes can be significant due to their curved surface. Previous works have reported spin-orbit couplings in reasonable agreement with theory, and this coupling strength has formed the basis of a large number of theoretical proposals. Here we report a spin-orbit coupling in three carbon nanotube devices that is an order of magnitude larger than previously measured. We find a zero-field spin splitting of up to 3.4 meV, corresponding to a built-in effective magnetic field of 29 T aligned along the nanotube axis. Although the origin of the large spin-orbit coupling is not explained by existing theories, its strength is promising for applications of the spin-orbit interaction in carbon nanotubes devices.