Four-dimensional variational data assimilation for inverse modeling of atmospheric methane emissions: Analysis of SCIAMACHY observations

Recent observations from the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) instrument aboard ENVISAT have brought new insights in the global distribution of atmospheric methane. In particular, the observations showed higher methane concentrations in the tropics than previously assumed. Here, we analyze the SCIAMACHY observations and their implications for emission estimates in detail using a four-dimensional variational (4D-Var) data assimilation system. We focus on the period September to November 2003 and on the South American continent, for which the satellite observations showed the largest deviations from model simulations. In this set-up the advantages of the 4D-Var approach and the zooming capability of the underlying TM5 atmospheric transport model are fully exploited. After application of a latitude-dependent bias correction to the SCIAMACHY observations, the assimilation system is able to accurately fit those observations, while retaining consistency with a network of surface methane measurements. The main emission increments resulting from the inversion are an increase in the tropics, a decrease in South Asia, and a decrease at northern hemispheric high latitudes. The SCIAMACHY observations yield considerable additional emission uncertainty reduction, particularly in the (sub-)tropical regions, which are poorly constrained by the surface network. For tropical South America, the inversion suggests more than a doubling of emissions compared to the a priori during the 3 months considered. Extensive sensitivity experiments, in which key assumptions of the inversion set-up are varied, show that this finding is robust. Independent airborne observations in the Amazon basin support the presence of considerable local methane sources. However, these observations also indicate that emissions from eastern South America may be smaller than estimated from SCIAMACHY observations. In this respect it must be realized that the bias correction applied to the satellite observations does not take into account potential regional systematic errors, which - if identified in the future - will lead to shifts in the overall distribution of emission estimates

Four-dimensional variational data assimilation for inverse modelling of atmospheric methane emissions: method and comparison with synthesis inversion

A four-dimensional variational (4D-Var) data assimilation system for inverse modelling of atmospheric methane emissions is presented. The system is based on the TM5 atmospheric transport model. It can be used for assimilating large volumes of measurements, in particular satellite observations and quasi-continuous in-situ observations, and at the same time it enables the optimization of a large number of model parameters, specifically grid-scale emission rates. Furthermore, the variational method allows to estimate uncertainties in posterior emissions. Here, the system is applied to optimize monthly methane emissions over a 1-year time window on the basis of surface observations from the NOAA-ESRL network. The results are rigorously compared with an analogous inversion by Bergamaschi et al. (2007), which was based on the traditional synthesis approach. The posterior emissions as well as their uncertainties obtained in both inversions show a high degree of consistency. At the same time we illustrate the advantage of 4D-Var in reducing aggregation errors by optimizing emissions at the grid scale of the transport model. The full potential of the assimilation system is exploited in Meirink et al. (2008), who use satellite observations of column-averaged methane mixing ratios to optimize emissions at high spatial resolution, taking advantage of the zooming capability of the TM5 model

Inverse modeling of European CH4 emissions: sensitivity to the observational network

Inverse modeling is widely employed to provide “top-down” emission estimates using atmospheric measurements. Here, we analyze the dependence of derived CH4 emissions on the sampling frequency and density of the observational surface network, using the TM5-4DVAR inverse modeling system and synthetic observations. This sensitivity study focuses on Europe. The synthetic observations are created by TM5 forward model simulations. The inversions of these synthetic observations are performed using virtually no knowledge on the a priori spatial and temporal distribution of emissions, i.e. the emissions are derived mainly from the atmospheric signal detected by the measurement network. Using the European network of stations for which continuous or weekly flask measurements are available for 2001, the synthetic experiments can retrieve the “true” annual total emissions for single countries such as France within 20%, and for all North West European countries together within ~5%. However, larger deviations are obtained for South and East European countries due to the scarcity of stations in the measurement network. Upgrading flask sites to stations with continuous measurements leads to an improvement for central Europe in emission estimates. For realistic emission estimates over the whole European domain, however, a major extension of the number of stations in the existing network is required. We demonstrate the potential of an extended network of a total of ~60 European stations to provide realistic emission estimates over the whole European domain

What can 14 CO measurements tell us about OH?

The possible use of 14CO measurements to constrain hydroxyl radical (OH) concentrations in the atmosphere is investigated. 14CO is mainly produced in the upper atmosphere from cosmic radiation. Measurements of 14CO at the surface show lower concentrations compared to the upper atmospheric source region, which is the result of oxidation by OH. In this paper, the sensitivity of 14CO mixing ratio surface measurements to the 3-D OH distribution is assessed with the TM5 model. Simulated 14CO mixing ratios agree within a few molecules 14CO cm¿3 (STP) with existing measurements at five locations worldwide. The simulated cosmogenic 14CO distribution appears mainly sensitive to the assumed upper atmospheric 14C source function, and to a lesser extend to model resolution. As a next step, the sensitivity of 14CO measurements to OH is calculated with the adjoint TM5 model. The results indicate that 14CO measurements taken in the tropics are sensitive to OH in a spatially confined region that varies strongly over time due to meteorological variability. Given measurements with an accuracy of 0.5 molecules 14CO cm¿3 STP, a good characterization of the cosmogenic 14CO fraction, and assuming perfect transport modeling, a single 14CO measurement may constrain OH to 0.2¿0.3×106 molecules OH cm¿3 on time scales of 6 months and spatial scales of 70×70 degrees (latitude×longitude) between the surface and 500 hPa. The sensitivity of 14CO measurements to high latitude OH is about a factor of five higher. This is in contrast with methyl chloroform (MCF) measurements, which show the highest sensitivity to tropical OH, mainly due to the temperature dependent rate constant of the MCF¿OH reaction. A logical next step will be the analysis of existing 14CO measurements in an inverse modeling framework. This paper presents the required mathematical framework for such an analysis

Three years of greenhouse gas column-averaged dry air mole fractions retrieved from satellite – Part 2: Methane

Carbon dioxide (CO2) and methane (CH4) are the two most important anthropogenic greenhouse gases. SCIAMACHY on ENVISAT is the first satellite instrument whose measurements are sensitive to concentration changes of the two gases at all altitude levels down to the Earth's surface where the source/sink signals are largest. We have processed three years (2003–2005) of SCIAMACHY near-infrared nadir measurements to simultaneously retrieve vertical columns of CO2 (from the 1.58 µm absorption band), CH4 (1.66 µm) and oxygen (O2 A-band at 0.76 µm) using the scientific retrieval algorithm WFM-DOAS. We show that the latest version of WFM-DOAS, version 1.0, which is used for this study, has been significantly improved with respect to its accuracy compared to the previous versions while essentially maintaining its high processing speed (~1 min per orbit, corresponding to ~6000 single measurements, and per gas on a standard PC). The greenhouse gas columns are converted to dry air column-averaged mole fractions, denoted XCO2 (in ppm) and XCH4 (in ppb), by dividing the greenhouse gas columns by simultaneously retrieved dry air columns. For XCO2 dry air columns are obtained from the retrieved O2 columns. For XCH4 dry air columns are obtained from the retrieved CO2 columns because of better cancellation of light path related errors compared to using O2 columns retrieved from the spectrally distant O2 A-band. Here we focus on a discussion of the XCH4 data set. The XCO2 data set is discussed in a separate paper (Part 1). For 2003 we present detailed comparisons with the TM5 model which has been optimally matched to highly accurate but sparse methane surface observations. After accounting for a systematic low bias of ~2% agreement with TM5 is typically within 1–2%. We investigated to what extent the SCIAMACHY XCH4 is influenced by the variability of atmospheric CO2 using global CO2 fields from NOAA's CO2 assimilation system CarbonTracker. We show that the CO2 corrected and uncorrected XCH4 spatio-temporal pattern are very similar but that agreement with TM5 is better for the CarbonTracker CO2 corrected XCH4. In line with previous studies (e.g., Frankenberg et al., 2005b) we find higher methane over the tropics compared to the model. We show that tropical methane is also higher when normalizing the CH4 columns with retrieved O2 columns instead of CO2. In consistency with recent results of Frankenberg et al. (2008b) it is shown that the magnitude of the retrieved tropical methane is sensitive to the choice of the spectroscopic line parameters of water vapour. Concerning inter-annual variability we find similar methane spatio-temporal pattern for 2003 and 2004. For 2005 the retrieved methane shows significantly higher variability compared to the two previous years, most likely due to somewhat larger noise of the spectral measurement

The impact of air pollutant and methane emission controls on tropospheric ozone and radiative forcing: CTM calculations for the period 1990-2030

To explore the relationship between tropospheric ozone and radiative forcing with changing emissions, we compiled two sets of global scenarios for the emissions of the ozone precursors methane (CH₄), carbon monoxide (CO), non-methane volatile organic compounds (NMVOC) and nitrogen oxides (NO_x) up to the year 2030 and implemented them in two global Chemistry Transport Models. The 'Current Legislation' (CLE) scenario reflects the current perspectives of individual countries on future economic development and takes the anticipated effects of presently decided emission control legislation in the individual countries into account. In addition, we developed a 'Maximum technically Feasible Reduction' (MFR) scenario that outlines the scope for emission reductions offered by full implementation of the presently available emission control technologies, while maintaining the projected levels of anthropogenic activities. Whereas the resulting projections of methane emissions lie within the range suggested by other greenhouse gas projections, the recent pollution control legislation of many Asian countries, requiring introduction of catalytic converters for vehicles, leads to significantly lower growth in emissions of the air pollutants NO_x, NMVOC and CO than was suggested by the widely used and more pessimistic IPCC (Intergovernmental Panel on Climate Change) SRES (Special Report on Emission Scenarios) scenarios (Nakicenovic et al., 2000), which made Business-as-Usual assumptions regarding emission control technology. With the TM3 and STOCHEM models we performed several long-term integrations (1990-2030) to assess global, hemispheric and regional changes in CH₄, CO, hydroxyl radicals, ozone and the radiative climate forcings resulting from these two emission scenarios. Both models reproduce broadly the observed trends in CO, and CH₄ concentrations from 1990 to 2002. <P style='line-height: 20px;'> For the 'current legislation' case, both models indicate an increase of the annual average ozone levels in the Northern Hemisphere by 5ppbv, and up to 15ppbv over the Indian sub-continent, comparing the 2020s (2020-2030) with the 1990s (1990-2000). The corresponding higher ozone and methane burdens in the atmosphere increase radiative forcing by approximately 0.2 Wm^-2. Full application of today's emissions control technologies, however, would bring down ozone below the levels experienced in the 1990s and would reduce the radiative forcing of ozone and methane to approximately -0.1 Wm^-2. This can be compared to the 0.14-0.47 Wm^-2 increase of methane and ozone radiative forcings associated with the SRES scenarios. While methane reductions lead to lower ozone burdens and to less radiative forcing, further reductions of the air pollutants NO_x and NMVOC result in lower ozone, but at the same time increase the lifetime of methane. Control of methane emissions appears an efficient option to reduce tropospheric ozone as well as radiative forcing

Development of a tunable diode laser absorption spectrometer for measurement of the 13C/12C ratio in methane

A tunable diode laser absorption spectrometer (TDLAS) for measuring the ratio in methane has been developed. Using a triple path arrangement the spectra of the CH4 sample, a isotope standard and pure 13CH4 are recorded simultaneously and compared to evaluate the ratio of the sample, using a 13CH4---12CH4 absorption line pair near 3007 cm−1. Systematic effects due to variations in temperature, pressure, and optical density were measured for this rotational-vibrational transition pair. Optical interference effects are effectively suppressed by linearly polarizing the laser beam and using Brewster windows for gas cells and detectors. The overall δ13C accuracy vs. the PDB scale is about ± 1 ‰ for a CH4 concentration of 2.5 % (sample size: 5 μmoles = 0.11 STP cm3 CH4) using 36 cm long absorption cells. The future application of a multipass cell should allow measurement concentrations of CH4 down to about 50 ppm. The main advantages of the new method are the short measurement time of 10–15 min for one sample and the direct measurement on the CH4 molecule without the need to chemically convert it to CO2. With the present accuracy the new method should be useful for the measurement of CH4 sources, allowing a greater sample throughput compared to the conventional mass spectrometry technique

Melhoria da qualidade do leite em propriedade leiteira: uma abordagem inicial.

A sanidade animal deficiente é um dos fatores que afeta negativamente a qualidade do leite bovino. Dentre as doenças relacionadas com a qualidade do leite, a mastite é a mais importante por estar amplamente distribuída nos rebanhos e ser reconhecida como de erradicação impossível, dependendo da etiologia da doença. Este trabalho foi realizado para obter o diagnóstico de situação da doença em um rebanho bovino leiteiro, que é o passo inicial e fundamental para a adoção de medidas preventivas eficazes. Amostras de leite de 53 animais de um rebanho de 135 vacas em lactação foram investigadas quanto à presença de microrganismos. Houve a identificação de microrganismos causadores de mastite em 39 amostras (73,6%), enquanto que em 12 (22,6%) foram encontrados resultados negativos e em duas (3,8%) ocorreram contaminações. Staphylococcus aureus foram os microrganismos de maior ocorrência e apresentaram resistência in vitro a três princípios ativos. Todos os isolados foram resistentes à penicilina, enquanto 54% e 4% dos isolados foram resistentes à gentamicina e à ciprofloxacina, respectivamente. Os principais microrganismos identificados como causadores de mastite foram os de origem contagiosa. A partir destes resultados, medidas de controle contra a doença podem ser propostas para atuar sobre as fontes de infecção e a transmissibilidade dos patógenos, com a detecção de animais doentes e o tratamento adequado, quando conveniente.bitstream/CPPSE-2010/19013/1/PROCIBolPesDes23LFZ2009.00317.pd