Methane Mixing Ratio Research Articles

Analytical constraints on layered gas trapping and smoothing of atmospheric variability in ice under low-accumulation conditions

Abstract. We investigate for the first time the loss and alteration of past atmospheric information from air trapping mechanisms under low-accumulation conditions through continuous CH4 (and CO) measurements. Methane concentration changes were measured over the Dansgaard–Oeschger event 17 (DO-17, ∼ 60 000 yr BP) in the Antarctic Vostok 4G-2 ice core. Measurements were performed using continuous-flow analysis combined with laser spectroscopy. The results highlight many anomalous layers at the centimeter scale that are unevenly distributed along the ice core. The anomalous methane mixing ratios differ from those in the immediate surrounding layers by up to 50 ppbv. This phenomenon can be theoretically reproduced by a simple layered trapping model, creating very localized gas age scale inversions. We propose a method for cleaning the record of anomalous values that aims at minimizing the bias in the overall signal. Once the layered-trapping-induced anomalies are removed from the record, DO-17 appears to be smoother than its equivalent record from the high-accumulation WAIS Divide ice core. This is expected due to the slower sinking and densification speeds of firn layers at lower accumulation. However, the degree of smoothing appears surprisingly similar between modern and DO-17 conditions at Vostok. This suggests that glacial records of trace gases from low-accumulation sites in the East Antarctic plateau can provide a better time resolution of past atmospheric composition changes than previously expected. We also developed a numerical method to extract the gas age distributions in ice layers after the removal of the anomalous layers based on comparison with a weakly smoothed record. It is particularly adapted for the conditions of the East Antarctic plateau, as it helps to characterize smoothing for a large range of very low-temperature and low-accumulation conditions.

Global height-resolved methane retrievals from the Infrared Atmospheric Sounding Interferometer (IASI) on MetOp

Abstract. This paper describes the global height-resolved methane (CH4) retrieval scheme for the Infrared Atmospheric Sounding Interferometer (IASI) on MetOp, developed at the Rutherford Appleton Laboratory (RAL). The scheme precisely fits measured spectra in the 7.9 micron region to allow information to be retrieved on two independent layers centred in the upper and lower troposphere. It also uses nitrous oxide (N2O) spectral features in the same spectral interval to directly retrieve effective cloud parameters to mitigate errors in retrieved methane due to residual cloud and other geophysical variables. The scheme has been applied to analyse IASI measurements between 2007 and 2015. Results are compared to model fields from the MACC greenhouse gas inversion and independent measurements from satellite (GOSAT), airborne (HIPPO) and ground (TCCON) sensors. The estimated error on methane mixing ratio in the lower- and upper-tropospheric layers ranges from 20 to 100 and from 30 to 40 ppbv, respectively, and error on the derived column-average ranges from 20 to 40 ppbv. Vertical sensitivity extends through the lower troposphere, though it decreases near to the surface. Systematic differences with the other datasets are typically < 10 ppbv regionally and < 5 ppbv globally. In the Southern Hemisphere, a bias of around 20 ppbv is found with respect to MACC, which is not explained by vertical sensitivity or found in comparison of IASI to TCCON. Comparisons to HIPPO and MACC support the assertion that two layers can be independently retrieved and provide confirmation that the estimated random errors on the column- and layer-averaged amounts are realistic. The data have been made publically available via the Centre for Environmental Data Analysis (CEDA) data archive (Siddans, 2016).

Atmospheric methane control mechanisms during the early Holocene

Abstract. Understanding processes controlling the atmospheric methane (CH4) mixing ratio is crucial to predict and mitigate future climate changes in this gas. Despite recent detailed studies of the last ∼ 1000 to 2000 years, the mechanisms that control atmospheric CH4 still remain unclear, partly because the late Holocene CH4 budget may be comprised of both natural and anthropogenic emissions. In contrast, the early Holocene was a period when human influence was substantially smaller, allowing us to elucidate more clearly the natural controls under interglacial conditions more clearly. Here we present new high-resolution CH4 records from Siple Dome, Antarctica, covering from 11.6 to 7.7 thousands of years before 1950 AD (ka). We observe four local CH4 minima on a roughly 1000-year spacing, which correspond to cool periods in Greenland. We hypothesize that the cooling in Greenland forced the Intertropical Convergence Zone (ITCZ) to migrate southward, reducing rainfall in northern tropical wetlands. The inter-polar difference (IPD) of CH4 shows a gradual increase from the onset of the Holocene to ∼ 9.5 ka, which implies growth of boreal source strength following the climate warming in the northern extratropics during that period.

Detectability of Arctic methane sources at six sites performing continuous atmospheric measurements

Abstract. Understanding the recent evolution of methane emissions in the Arctic is necessary to interpret the global methane cycle. Emissions are affected by significant uncertainties and are sensitive to climate change, leading to potential feedbacks. A polar version of the CHIMERE chemistry-transport model is used to simulate the evolution of tropospheric methane in the Arctic during 2012, including all known regional anthropogenic and natural sources, in particular freshwater emissions which are often overlooked in methane modelling. CHIMERE simulations are compared to atmospheric continuous observations at six measurement sites in the Arctic region. In winter, the Arctic is dominated by anthropogenic emissions; emissions from continental seepages and oceans, including from the East Siberian Arctic Shelf, can contribute significantly in more limited areas. In summer, emissions from wetland and freshwater sources dominate across the whole region. The model is able to reproduce the seasonality and synoptic variations of methane measured at the different sites. We find that all methane sources significantly affect the measurements at all stations at least at the synoptic scale, except for biomass burning. In particular, freshwater systems play a decisive part in summer, representing on average between 11 and 26 % of the simulated Arctic methane signal at the sites. This indicates the relevance of continuous observations to gain a mechanistic understanding of Arctic methane sources. Sensitivity tests reveal that the choice of the land-surface model used to prescribe wetland emissions can be critical in correctly representing methane mixing ratios. The closest agreement with the observations is reached when using the two wetland models which have emissions peaking in August–September, while all others reach their maximum in June–July. Such phasing provides an interesting constraint on wetland models which still have large uncertainties at present. Also testing different freshwater emission inventories leads to large differences in modelled methane. Attempts to include methane sinks (OH oxidation and soil uptake) reduced the model bias relative to observed atmospheric methane. The study illustrates how multiple sources, having different spatiotemporal dynamics and magnitudes, jointly influence the overall Arctic methane budget, and highlights ways towards further improved assessments.

Estimating the size of a methane emission point source at different scales: from local to landscape

Abstract. High methane (CH4) mixing ratios (up to 4 ppm) have occurred sporadically at our measurement site in Haddenham, Cambridgeshire, since July 2012. Isotopic measurements and back trajectories show that the source is the Waterbeach Waste Management Park 7 km SE of Haddenham. To investigate this further, measurements were made on 30 June and 1 July 2015 at other locations nearer to the source. Landfill emissions have been estimated using three different approaches at different scales; near source using the WindTrax inversion dispersion model, middle distance using a Gaussian plume (GP) model and at the landscape scale using the Numerical Atmospheric Modelling Environment (NAME) Inversion Technique for Emission Modelling (InTEM) inversion. The emission estimates derived using the WindTrax and Gaussian plume (GP) approaches agree well for the period of intense observations. Applying the Gaussian plume approach to all periods of elevated measurements seen at Haddenham produces year-round and monthly landfill emission estimates with an estimated annual emission of 11.6 Gg CH4 yr−1. The monthly emission estimates are highest in winter (2160 kg h−1 in February) and lowest in summer (620 kg h−1 in July). These data identify the effects of environmental conditions on landfill CH4 production and highlight the importance of year-round measurements to capture seasonal variability in CH4 emission.

Non-homogeneous vertical distribution of methane over Indian region using surface, aircraft and satellite based data

The upper tropospheric methane (UCH4) data from Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container (CARIBIC), the column average mixing ratio of methane (XCH4) from SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) and near-surface methane at two locations- Cape Rama, Goa, a Commonwealth Scientific Industrial Research Organization (CSIRO) network station and Ahmedabad (23.03°N; 72.45°E) were analysed to understand vertical inhomogenities in methane mixing ratio and the seasonal changes in the latitude sector 13°–24°N over India. XCH4 and UCH4 were found to follow more or less similar pattern over all the three latitude sectors, with the peak occurring in July–August, and minimum in late winter. The seasonal amplitude in XCH4 is less at low latitude sector (∼64 ppbv) compared to that of high latitudes (∼101 ppbv at 18°–22°N and 88 ppbv at 22°–24°N). On the other hand, the near surface methane shows opposite pattern peaking in winter attaining low in monsoon. During monsoon when methane sources are active at the surface, XCH4 > UCH4 and during other seasons UCH4 > XCH4 indicating presence of high altitude layers. This analysis revealed non-homogeneous distribution of methane in the troposphere indicative of stratified layers. The role of convective activity, boundary layer meteorology and long-range transport in controlling the seasonal changes in the vertical distribution of methane are examined in this study.

THE HUNT FOR PLANET NINE: ATMOSPHERE, SPECTRA, EVOLUTION, AND DETECTABILITY

ABSTRACT We investigate the physical characteristics of the solar system’s proposed Planet Nine using modeling tools with a heritage of studying Uranus and Neptune. For a range of plausible masses and interior structures, we find upper limits on the intrinsic T eff , from ∼35 to 50 K for masses of 5–20 M ⊕, and we also explore lower T eff values. Possible planetary radii could readily span from 2.7 to 6 R ⊕, depending on the mass fraction of any H/He envelope. Given its cold atmospheric temperatures, the planet encounters significant methane condensation, which dramatically alters the atmosphere away from simple Neptune-like expectations. We find that the atmosphere is strongly depleted in molecular absorption at visible wavelengths, suggesting a Rayleigh scattering atmosphere with a high geometric albedo approaching 0.75. We highlight two diagnostics for the atmosphere’s temperature structure: (1) the value of the methane mixing ratio above the methane cloud and (2) the wavelength at which cloud scattering can be seen, which yields the cloud-top pressure. Surface reflection may be seen if the atmosphere is thin. Due to collision-induced opacity of H2 in the infrared, the planet would be extremely blue instead of red in the shortest wavelength WISE colors if methane is depleted and would, in some cases, exist on the verge of detectability by WISE. For a range of models, thermal fluxes from ∼3 to 5 μm are ∼20 orders of magnitude larger than blackbody expectations. We report a search of the AllWISE Source Catalog for Planet Nine, but find no detection.

Validation of MIPAS IMK/IAA methane profiles

Abstract. The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) is an infrared (IR) limb emission spectrometer on the Envisat platform. It measures trace gas distributions during day and night, pole-to-pole, over an altitude range from 6 to 70 km in nominal mode and up to 170 km in special modes, depending on the measurement mode, producing more than 1000 profiles day−1. We present the results of a validation study of methane, version V5R_CH4_222, retrieved with the IMK/IAA (Institut für Meteorologie und Klimaforschung, Karlsruhe/Instituto de Astrofisica de Andalucia, Grenada) MIPAS scientific level 2 processor. The level 1 spectra are provided by the ESA (European Space Agency) and version 5 was used. The time period covered is 2005–2012, which corresponds to the period when MIPAS measured trace gas distributions at a reduced spectral resolution of 0.0625 cm−1. The comparison with satellite instruments includes the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), the HALogen Occultation Experiment (HALOE), the Solar Occultation For Ice Experiment (SOFIE) and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY). Furthermore, comparisons with MkIV balloon-borne solar occultation measurements and with air sampling measurements performed by the University of Frankfurt are presented. The validation activities include bias determination, assessment of stability, precision validation, analysis of histograms and comparison of corresponding climatologies. Above 50 km altitude, MIPAS methane mixing ratios agree within 3 % with ACE-FTS and SOFIE. Between 30 and 40 km an agreement within 3 % with SCIAMACHY has been found. In the middle stratosphere, there is no clear indication of a MIPAS bias since comparisons with various instruments contradict each other. In the lower stratosphere (below 25 km) MIPAS CH4 is biased high with respect to satellite instruments, and the most likely estimate of this bias is 14 %. However, in the comparison with CH4 data obtained from cryogenic whole-air sampler (cryosampler) measurements, there is no evidence of a high bias in MIPAS between 20 and 25 km altitude. Precision validation is performed on collocated MIPAS–MIPAS pairs and suggests a slight underestimation of its uncertainties by a factor of 1.2. No significant evidence of an instrumental drift has been found.

First observations of light non-methane hydrocarbons (C2–C5) over a high altitude site in the central Himalayas

Abstract This study presents observations of methane (CH 4 ) and light non-methane hydrocarbons (NMHCs) for the first time from a high altitude site Nainital (29.4°N, 79.5°E, 1958 m amsl) in the central Himalayas. The whole air samples collected with a frequency of 3 samples per week during April 2009–December 2011 are analyzed using a Gas Chromatograph equipped with Flame Ionization Detector (GC-FID). Additionally, samples were collected from two semi-urban sites (Haldwani and Pantnagar) in the adjoining Indo Gangetic plain region. CH 4 and NMHCs show a distinct seasonal cycle over this region with more frequent observations of higher levels during winter (DJF) and late autumn (SON) and lower levels during the summer–monsoon (JJA). Different NMHCs exhibit better correlations during autumn/winter as compared to the summer–monsoon season. The annual mean mixing ratios of methane, ethane, ethene, propane, propene, i-butane, n-butane, acetylene, and i-pentane at Nainital are measured to be 1.9 ± 0.1 ppmv, 1.8 ± 1.0, 0.7 ± 0.9, 0.6 ± 0.8, 0.6 ± 0.7, 0.6 ± 0.7, 0.5 ± 0.6, 1.0 ± 0.8, and 0.5 ± 0.6, respectively (all in ppbv). The seasonal cycle of CH 4 at Nainital is found to be similar to other global high altitude sites (Jungfraujoch and Mauna Loa) but somewhat different than a high altitude site Mt. Abu in India. NMHCs, other than ethane and propane, are found to be higher over this central Himalayan region than other sites. Additionally, composition of NMHCs is shown to be different over the study region when compared with other sites in the IGP region. A correlation study between ln((n-butane)/(ethane)) and ln((i-butane)/(ethane)) showed that oxidation by the OH radical is the main removal mechanism of these species over the central Himalaya and dilution maintains the ratios of these species. The lowest slope of propane and acetylene with CO during summer and spring are indicating absence of fresh air mass over this region. This study fills a major gap in observational data for light NMHCs in the Himalayas and has implications for better understanding of tropospheric chemistry over this region.

Natural and anthropogenic methane fluxes in Eurasia: a mesoscale quantification by generalized atmospheric inversion

Abstract. Eight surface observation sites providing quasi-continuous measurements of atmospheric methane mixing ratios have been operated since the mid-2000's in Siberia. For the first time in a single work, we assimilate 1 year of these in situ observations in an atmospheric inversion. Our objective is to quantify methane surface fluxes from anthropogenic and wetland sources at the mesoscale in the Siberian lowlands for the year 2010. To do so, we first inquire about the way the inversion uses the observations and the way the fluxes are constrained by the observation sites. As atmospheric inversions at the mesoscale suffer from mis-quantified sources of uncertainties, we follow recent innovations in inversion techniques and use a new inversion approach which quantifies the uncertainties more objectively than the previous inversion systems. We find that, due to errors in the representation of the atmospheric transport and redundant pieces of information, only one observation every few days is found valuable by the inversion. The remaining high-resolution quasi-continuous signal is representative of very local emission patterns difficult to analyse with a mesoscale system. An analysis of the use of information by the inversion also reveals that the observation sites constrain methane emissions within a radius of 500 km. More observation sites than the ones currently in operation are then necessary to constrain the whole Siberian lowlands. Still, the fluxes within the constrained areas are quantified with objectified uncertainties. Finally, the tolerance intervals for posterior methane fluxes are of roughly 20 % (resp. 50 %) of the fluxes for anthropogenic (resp. wetland) sources. About 50–70 % of Siberian lowlands emissions are constrained by the inversion on average on an annual basis. Extrapolating the figures on the constrained areas to the whole Siberian lowlands, we find a regional methane budget of 5–28 TgCH4 for the year 2010, i.e. 1–5 % of the global methane emissions. As very few in situ observations are available in the region of interest, observations of methane total columns from the Greenhouse Gas Observing SATellite (GOSAT) are tentatively used for the evaluation of the inversion results, but they exhibit only a marginal signal from the fluxes within the region of interest.

Co-utilization of two coal mine residues

In this study, the experiments were carried out in a circulating fluidized bed with different coal bed methane and coal gangue mixing ratios. The results show that bed temperature distribution becomes well-proportioned and the combustion efficiency increases when coal bed methane was introduced. The NO emission increases along with the excess air coefficient rise. The SO2 emission reduces first and then increases with the rising bed temperature and there is an optimum temperature corresponding to the lowest SO2 emission. At the same time, the effects of the bed temperature and excess air coefficient on pollutant emissions are more obvious when coal bed methane and coal gangue mixing ratio is less than 0.3. In the experiments, the best operation conditions have been found at coal bed methane and coal gangue mixing ratio of 0.2 and excess air coefficient of less than 1.3. The results show that the co-combustion of coal bed methane and coal gangue in circulating fluidized bed is feasible and provides some references for the combustion optimization.

Sensitivity of the recent methane budget to LMDz sub-grid-scale physical parameterizations

Abstract. With the densification of surface observing networks and the development of remote sensing of greenhouse gases from space, estimations of methane (CH4) sources and sinks by inverse modeling are gaining additional constraining data but facing new challenges. The chemical transport model (CTM) linking the flux space to methane mixing ratio space must be able to represent these different types of atmospheric constraints for providing consistent flux estimations. Here we quantify the impact of sub-grid-scale physical parameterization errors on the global methane budget inferred by inverse modeling. We use the same inversion setup but different physical parameterizations within one CTM. Two different schemes for vertical diffusion, two others for deep convection, and one additional for thermals in the planetary boundary layer (PBL) are tested. Different atmospheric methane data sets are used as constraints (surface observations or satellite retrievals). At the global scale, methane emissions differ, on average, from 4.1 Tg CH4 per year due to the use of different sub-grid-scale parameterizations. Inversions using satellite total-column mixing ratios retrieved by GOSAT are less impacted, at the global scale, by errors in physical parameterizations. Focusing on large-scale atmospheric transport, we show that inversions using the deep convection scheme of Emanuel (1991) derive smaller interhemispheric gradients in methane emissions, indicating a slower interhemispheric exchange. At regional scale, the use of different sub-grid-scale parameterizations induces uncertainties ranging from 1.2 % (2.7 %) to 9.4 % (14.2 %) of methane emissions when using only surface measurements from a background (or an extended) surface network. Moreover, spatial distribution of methane emissions at regional scale can be very different, depending on both the physical parameterizations used for the modeling of the atmospheric transport and the observation data sets used to constrain the inverse system. When using only satellite data from GOSAT, we show that the small biases found in inversions using a coarser version of the transport model are actually masking a poor representation of the stratosphere–troposphere methane gradient in the model. Improving the stratosphere–troposphere gradient reveals a larger bias in GOSAT CH4 satellite data, which largely amplifies inconsistencies between the surface and satellite inversions. A simple bias correction is proposed. The results of this work provide the level of confidence one can have for recent methane inversions relative to physical parameterizations included in CTMs.

High S/N Keck and Gemini AO imaging of Uranus during 2012–2014: New cloud patterns, increasing activity, and improved wind measurements

We imaged Uranus in the near infrared from 2012 into 2014, using the Keck/NIRC2 camera and Gemini/NIRI camera, both with adaptive optics. We obtained exceptional signal to noise ratios by averaging 8–16 individual exposures in a planet-fixed coordinate system. These noise-reduced images revealed many low-contrast discrete features and large scale cloud patterns not seen before, including scalloped waveforms just south of the equator, and an associated transverse ribbon wave near 6°S. In all three years numerous small (600–700km wide) and mainly bright discrete features were seen within the north polar region (north of about55°N). Two small dark spots with bright companions were seen at middle latitudes. Over 850 wind measurements were made, the vast majority of which were in the northern hemisphere. Winds at high latitudes were measured with great precision, revealing an extended region of solid body rotation between 62°N and at least 83°N, at a rate of 4.08±0.015°/h westward relative to the planet’s interior (radio) rotation of 20.88°/h westward. Near-equatorial speeds measured with high accuracy give different results for waves and small discrete features, with eastward drift rates of 0.4°/h and 0.1°/h respectively. The region of polar solid body rotation is a close match to the region of small-scale polar cloud features, suggesting a dynamical relationship. The winds from prior years and those from 2012–2014 are consistent with a mainly symmetric wind profile up to middle latitudes, with a small asymmetric component of ∼0.09°/h peaking near ±30°, and about 60% greater amplitude if only prior years are included, suggesting a declining mid-latitude asymmetry. While winds at high southern latitudes(50–90°S) are unconstrained by groundbased observations, a recent reanalysis of 1986 Voyager 2 observations by Karkoschka (Karkoschka [2015]. Icarus 250, 294–307) has revealed an extremely large north–south asymmetry in this region, which might be seasonal. Greatly increased activity was seen in 2014, including the brightest ever feature seen in K′ images (de Pater et al. [2015]. Icarus 252, 121–128), as well as other significant features, some of which had long lives. Over the 2012–2014 period we identified six persistent discrete features. Three were tracked for more than 2years, two more for more than 1year, and one for at least 5months and continuing. Several drifted in latitude towards the equator, and others appeared to exhibit latitudinal oscillations with long periods. We found two pairs of long-lived features that survived multiple passages within their own diameters of each other. Zonally averaged cloud patterns were found to persist over 2012–2014. When averaged over longitude, there is a brightness variation with latitude from 55°N to the pole that is similar to effective methane mixing ratio variations with latitude derived from 2012 STIS observations (Sromovsky et al. [2014]. Icarus 238, 137–155).

Evidence for a three-phase sequence during Heinrich Stadial 4 using a multiproxy approach based on Greenland ice core records

Abstract. Glacial climate was characterised by two types of abrupt events. Greenland ice cores record Dansgaard–Oeschger events, marked by abrupt warming in-between cold, stadial phases. Six of these stadials appear related to major Heinrich events (HEs), identified from ice-rafted debris (IRD) and large excursions in carbon- and oxygen-stable isotopic ratios in North Atlantic deep sea sediments, documenting major ice sheet collapse events. This finding has led to the paradigm that glacial cold events are induced by the response of the Atlantic Meridional Overturning Circulation to such massive freshwater inputs, supported by sensitivity studies conducted with climate models of various complexities. These models also simulate synchronous Greenland temperature and lower-latitude hydrological changes. To investigate the sequence of events between climate changes at low latitudes and in Greenland, we provide here the first 17O-excess record from a Greenland ice core during Dansgaard–Oeschger events 7 to 13, encompassing H4 and H5. Combined with other ice core proxy records, our new 17O-excess data set demonstrates that stadials are generally characterised by low 17O-excess levels compared to interstadials. This can be interpreted as synchronous change of high-latitude temperature and lower-latitude hydrological cycle (relative humidity at the oceanic source of evaporation or change in the water mass trajectory/recharge) and/or an influence of local temperature on 17O-excess through kinetic effect at snow formation. As an exception from this general pattern, stadial 9 consists of three phases, characterised first by Greenland cooling during 550 ± 60 years (as shown by markers of Greenland temperature δ18O and δ15N), followed by a specific lower-latitude fingerprint as identified from several proxy records (abrupt decrease in 17O-excess, increase in CO2 and methane mixing ratio, heavier δD-CH4 and δ18Oatm), lasting 740 ± 60 years, itself ending approximately 390 ± 50 years prior to abrupt Greenland warming. We hypothesise that this lower-latitude signal may be the fingerprint of Heinrich event 4 in Greenland ice cores. The proposed decoupling between stable cold Greenland temperature and low-latitude climate variability identified for stadial 9 provides new targets for benchmarking climate model simulations and testing mechanisms associated with millennial variability.

Analysis and demonstration of atmospheric methane monitoring by mid-infrared open-path chirped laser dispersion spectroscopy.

Atmospheric methane concentration levels were detected using a custom built laser dispersion spectrometer in a long open-path beam configuration. The instrument is driven by a chirped distributed feedback mid-infrared quantum cascade laser centered at ~1283.46 cm-1 and covers intense rotational-vibrational transitions from the fundamental ν4 band of methane. A full forward model simulating molecular absorption and dispersion profiles, as well as instrumental noise, is demonstrated. The instrument's analytical model is validated and used for quantitative instrumental optimization. The temporal evolution of atmospheric methane mixing ratios is retrieved using a fitting algorithm based on the model. Full error propagation analysis on precision gives a normalized sensitivity of ~3 ppm.m.Hz-0.5 for atmospheric methane.

Methane depletion in both polar regions of Uranus inferred from HST/STIS and Keck/NIRC2 observations

From Space Telescope Imaging Spectrograph (STIS) observations of Uranus in 2012, when good views of its north polar regions were available, we found that the methane volume mixing ratio declined from about 4% at low latitudes to about 2% at 60–80°N. This depletion in the north polar region of Uranus in 2012 is similar in magnitude and depth to that found in the south polar regions in 2002. This similarity is remarkable because of the strikingly different appearance of clouds in the two polar regions: we have never seen any obvious signs of convective activity in the south polar region, while the north has been peppered with numerous small clouds thought to be of convective origin. Keck and Hubble Space Telescope imaging observations close to equinox at wavelengths of 1080nm and 1290nm, with different sensitivities to methane and hydrogen absorption but similar vertical contribution functions, imply that the depletions were simultaneously present in 2007, and at least their gross character is probably a persistent feature of the Uranus atmosphere. The depletion appears to be mainly restricted to the upper troposphere, with the depth increasing poleward from about 30°N, reaching ∼4bars at 45°N and perhaps much deeper at 70°N, where it is not well constrained by our observations. The latitudinal variations in degree and depth of the depletions are important constraints on models of meridional circulation. Our observations are qualitatively consistent with previously suggested circulation cells in which rising methane-rich gas at low latitudes is dried out by condensation and sedimentation of methane ice particles as the gas ascends to altitudes above the methane condensation level, then is transported to high latitudes, where it descends and brings down methane depleted gas. Since this cell would seem to inhibit formation of condensation clouds in regions where clouds are actually inferred from spectral modeling, it suggests that sparse localized convective events may be important in cloud formation. A more complex meridional circulation pattern may be necessary to reproduce the observed cloud distribution, but microwave observations appear to be most compatible with a single deep circulation cell. The small-scale latitudinal variations we found in the effective methane mixing ratio between 55°N and 82°N have significant inverse correlations with zonal mean latitudinal variations in cloud reflectivity in near-IR Keck images taken before and after the HST observations. If the CH4/H2 absorption ratio variations are interpreted as local variations in para fraction instead of methane mixing ratio, we find that downwelling correlates with reduced cloud reflectivity. While there has been no significant secular change in the brightness of Uranus at continuum wavelengths between 2002 and 2012, there have been significant changes at wavelengths sensing methane and/or hydrogen absorption, with the southern hemisphere darkening considerably between 2002 and 2012, by ∼25% at mid latitudes near 827nm, for example, while the northern hemisphere has brightened by ∼25% at mid latitudes at the same wavelength.

Exploring the spatial, temporal, and vertical distribution of methane in Pluto’s atmosphere

High-resolution spectra of Pluto in the 1.66μm region, recorded with the VLT/CRIRES instrument in 2008 (2 spectra) and 2012 (5 spectra), are analyzed to constrain the spatial and vertical distribution of methane in Pluto’s atmosphere and to search for mid-term (4year) variability. A sensitivity study to model assumptions (temperature structure, surface pressure, Pluto’s radius) is performed. Results indicate that (i) no variation of the CH4 atmospheric content (column-density or mixing ratio) with Pluto rotational phase is present in excess of 20%, (ii) CH4 column densities show at most marginal variations between 2008 and 2012, with a best guess estimate of a ∼20% decrease over this time frame. As stellar occultations indicate that Pluto’s surface pressure has continued to increase over this period, this implies a concomitant decrease of the methane mixing ratio (iii) the data do not show evidence for an altitude-varying methane distribution; in particular, they imply a roughly uniform mixing ratio in at least the first 22–27km of the atmosphere, and high concentrations of low-temperature methane near the surface can be ruled out. Our results are also best consistent with a relatively large (>1180km) Pluto radius. Comparison with predictions from a recently developed global climate model indicates that these features are best explained if the source of methane occurs in regional-scale CH4 ice deposits, including both low latitudes and high Northern latitudes, evidence for which is present from the rotational and secular evolution of the near-IR features due to CH4 ice. Our “best guess” predictions for the New Horizons encounter in 2015 are: a 1184km radius, a 17μbar surface pressure, and a 0.44% CH4 mixing ratio with negligible longitudinal variations.

Tunable diode laser in-situ CH<sub>4</sub> measurements aboard the CARIBIC passenger aircraft: instrument performance assessment

Abstract. A laser spectrometer for automated monthly measurements of methane (CH4) mixing ratios aboard the CARIBIC passenger aircraft is presented. The instrument is based on a commercial Fast Greenhouse Gas Analyser (FGGA, Los Gatos Res.), which was adapted to meet the requirements imposed by unattended airborne operation. It was characterised in the laboratory with respect to instrument stability, precision, cross sensitivity to H2O, and accuracy. For airborne operation, a calibration strategy is described that utilises CH4 measurements obtained from flask samples taken during the same flights. The precision of airborne measurements is 2 ppb for 10 s averages. The accuracy at aircraft cruising altitude is 3.85 ppb. During aircraft ascent and descent, where no flask samples were obtained, instrumental drifts can be less accurately determined and the uncertainty is estimated to be 12.4 ppb. A linear humidity bias correction was applied to the CH4 measurements, which was most important in the lower troposphere. On average, the correction bias was around 6.5 ppb at an altitude of 2 km, and negligible at cruising flight level. Observations from 103 long-distance flights are presented that span a large part of the northern hemispheric upper troposphere and lowermost stratosphere (UT/LMS), with occasional crossing of the tropics on flights to southern Africa. These accurate data mark the largest UT/LMS in-situ CH4 dataset worldwide. An example of a tracer-tracer correlation study with ozone is given, highlighting the possibility for accurate cross-tropopause transport analyses.

Atmospheric Methane Mixing Ratio in a South Indian Coastal City Interlaced by Wetlands

Industrialisation and urbanization leads to an increase in concentration of greenhouse gases, which eventually alters the radiation balance of the climate system. Urban regions are hotspots of greenhouse gas emissions which include CO2, CH4, N2O, etc. Methane emitting sources hosted by cities include fossil fuel combustion, municipal waste and sewage management, blocked drains and pools etc. Waste discharges from the residences, food wastes, market places etc., contribute to the methane production. Urban heat island causing warm nights in the city is also a suitable condition for the generation of methane.Ground level mixing ratio of methane in the tropical coastal city of Cochin in South India, during calm early morning periods was measured in this study. A mobile traverse method was employed from January 2011 to March 2013. Measurements were taken during both winter and summer seasons. It was observed that the ground level methane concentrations were significantly higher than the global average value. Intra-city variation in ground level mixing ratio was also significant. The maximum value of ground level methane in winter and summer were 3.85ppm and 3.21ppm respectively. The study reveals that the city acts as a source of atmospheric methane.

Atmospheric methane removal by methane-oxidizing bacteria immobilized on porous building materials

Biological treatment using methane-oxidizing bacteria (MOB) immobilized on six porous carrier materials have been used to mitigate methane emission. Experiments were performed with different MOB inoculated in building materials at high (~20 % (v/v)) and low (~100 ppmv) methane mixing ratios. Methylocystis parvus in autoclaved aerated concrete (AAC) exhibited the highest methane removal rate at high (28.5 ± 3.8 μg CH₄ g⁻¹ building material h⁻¹) and low (1.7 ± 0.4 μg CH₄ g⁻¹ building material h⁻¹) methane mixing ratio. Due to the higher volume of pores with diameter >5 μm compared to other materials tested, AAC was able to adsorb more bacteria which might explain for the higher methane removal observed. The total methane and carbon dioxide-carbon in the headspace was decreased for 65.2 ± 10.9 % when M. parvus in Ytong was incubated for 100 h. This study showed that immobilized MOB on building materials could be used to remove methane from the air and also act as carbon sink.