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Global anthropogenic methane emissions 2005–2030: technical mitigation potentials and costs

This paper presents estimates of current and future global anthropogenic methane emissions, their technical mitigation potential and associated costs for the period 2005 to 2030. The analysis uses the GAINS model framework to estimate emissions, mitigation potentials and costs for all major sources of anthropogenic methane for 83 countries/regions, which are aggregated to produce global estimates. Global emissions are estimated at 323 Mt methane in 2005, with an expected increase to 414 Mt methane in 2030. The technical mitigation potential is estimated at 195 Mt methane in 2030, whereof about 80 percent is found attainable at a marginal cost less than 20 Euro t−1 CO2eq when using a social planner cost perspective. With a private investor cost perspective, the corresponding fraction is only 30 percent. Major uncertainty sources in emission estimates are identified and discussed.
Interpretation of FRESCO cloud retrievals in case of absorbing aerosol events

Cloud and aerosol information is needed in trace gas retrievals from satellite measurements. The Fast REtrieval Scheme for Clouds from the Oxygen A band (FRESCO) cloud algorithm employs reflectance spectra of the O2 A band around 760 nm to derive cloud pressure and effective cloud fraction. In general, clouds contribute more to the O2 A band reflectance than aerosols. Therefore, the FRESCO algorithm does not correct for aerosol effects in the retrievals and attributes the retrieved cloud information entirely to the presence of clouds, and not to aerosols. For events with high aerosol loading, aerosols may have a dominant effect, especially for almost cloud free scenes. We have analysed FRESCO cloud data and Absorbing Aerosol Index (AAI) data from the Global Ozone Monitoring Experiment (GOME-2) instrument on the Metop-A satellite for events with typical absorbing aerosol types, such as volcanic ash, desert dust and smoke. We find that the FRESCO effective cloud fractions are correlated with the AAI data for these absorbing aerosol events and that the FRESCO cloud pressure contains information on aerosol layer pressure. For cloud free scenes, the derived FRESCO cloud pressure is close to the aerosol layer pressure, especially for optically thick aerosol layers. For cloudy scenes, if the strongly absorbing aerosols are located above the clouds, then the retrieved FRESCO cloud pressure may represent the height of the aerosol layer rather than the height of the clouds. Combining FRESCO and AAI data, an estimate for the aerosol layer pressure can be given.
Tropospheric impact of methane emissions from clathrates in the Arctic Region

A highly potent greenhouse gas, methane, is locked in the solid phase as ice-like deposits containing a mixture of water and gas (mostly methane) called clathrates in both ocean sediments and underneath permafrost regions. Clathrates are stable under high pressures and low temperatures. In a warming climate, increases in ocean temperatures could lead to dissociation of the clathrates and release methane into the ocean and subsequently the atmosphere. This is of particular importance in the shallow parts of the Arctic Ocean, since clathrates are expected to start outgassing abruptly at depths of around 300 m. In this paper, we present a comparison of simulations from the Community Earth System Model (CESM1) for present-day conditions with and without additional methane emissions from a plausible clathrate release scenario based on a state-of-the-art ocean sediment model. The CESM model includes a fully interactive physical ocean and we added a fast atmospheric chemistry mechanism that represents methane as a fully interactive tracer (with emissions rather than concentration boundary conditions) along with the main chemical reactions for methane, ozone, and nitrous oxide. The results show that such Arctic clathrate emissions increase methane concentrations non-uniformly, and that increases in surface ozone concentrations are greatest in polluted regions. We also find that the interannual variability in surface methane and ozone increases.
On the formation of sulphuric acid – amine clusters in varying atmospheric conditions and its influence on atmospheric new particle formation

Sulphuric acid is a key component in atmospheric new particle formation. However, sulphuric acid alone does not form stable enough clusters to initiate particle formation in atmospheric conditions. Strong bases, such as amines, have been suggested to stabilize sulphuric acid clusters and thus participate in particle formation. We modelled the formation rate of clusters with two sulphuric acid and two amine molecules (JA2B2) at varying atmospherically relevant conditions with respect to concentrations of sulphuric acid ([H2SO4]), dimethylamine ([DMA]) and trimethylamine ([TMA]), temperature and relative humidity (RH). We also tested how the model results change if we assume that the clusters with two sulphuric acid and two amine molecules would act as seeds for heterogeneous nucleation of organic vapours (other than amines) with higher atmospheric concentrations than sulphuric acid. The modelled formation rates JA2B2 were functions of sulphuric acid concentration with close to quadratic dependence, which is in good agreement with atmospheric observations of the connection between the particle formation rate and sulphuric acid concentration. The coefficients KA2B2 connecting the cluster formation rate and sulphuric acid concentrations as JA2B2=KA2B2[H2SO4]2 turned out to depend also on amine concentrations, temperature and relative humidity. We compared the modelled coefficients KA2B2 with the corresponding coefficients calculated from the atmospheric observations (Kobs) from environments with varying temperatures and levels of anthropogenic influence. By taking into account the modelled behaviour of JA2B2 as a function of [H2SO4], temperature and RH, the atmospheric particle formation rate was reproduced more closely than with the traditional semi-empirical formulae based on sulphuric acid concentration only. The formation rates of clusters with two sulphuric acid and two amine molecules with different amine compositions (DMA or TMA or one of both) had different responses to varying meteorological conditions and concentrations of vapours participating in particle formation. The observed inverse proportionality of the coefficient Kobs with RH and temperature agreed best with the modelled coefficient KA2B2 related to formation of a cluster with two H2SO4 and one or two TMA molecules, assuming that these clusters can grow in collisions with abundant organic vapour molecules. In case this assumption is valid, our results suggest that the formation rate of clusters with at least two of both sulphuric acid and amine molecules might be the rate-limiting step for atmospheric particle formation. More generally, our analysis elucidates the sensitivity of the atmospheric particle formation rate to meteorological variables and concentrations of vapours participating in particle formation (also other than H2SO4).
Retrieval of aerosol optical depth over land based on a time series technique using MSG/SEVIRI data

A novel approach for the joint retrieval of aerosol optical depth (AOD) and aerosol type, using Meteosat Second Generation – Spinning Enhanced Visible and Infrared Imagers (MSG/SEVIRI) observations in two solar channels, is presented. The retrieval is based on a Time Series (TS) technique, which makes use of the two visible bands at 0.6 μm and 0.8 μm in three orderly scan times (15 min interval between two scans) to retrieve the AOD over land. Using the radiative transfer equation for plane-parallel atmosphere, two coupled differential equations for the upward and downward fluxes are derived. The boundary conditions for the upward and downward fluxes at the top and at the bottom of the atmosphere are used in these equations to provide an analytic solution for the AOD. To derive these fluxes, the aerosol single scattering albedo (SSA) and asymmetry factor are required to provide a solution. These are provided from a set of six pre-defined aerosol types with the SSA and asymmetry factor. We assume one aerosol type for a grid of 1°×1° and the surface reflectance changes little between two subsequent observations. A k-ratio approach is used in the inversion to find the best solution of atmospheric properties and surface reflectance. The k-ratio approach assumes that the surface reflectance is little influenced by aerosol scattering at 1.6 μm and therefore the ratio of surface reflectances in the solar band for two subsequent observations can be well-approximated by the ratio of the reflectances at 1.6 μm. A further assumption is that the surface reflectance varies only slightly over a period of 30 min. The algorithm makes use of numerical minimisation routines to obtain the optimal solution of atmospheric properties and surface reflectance by selection of the most suitable aerosol type from pre-defined sets. A detailed analysis of the retrieval results shows that it is suitable for AOD retrieval over land from SEVIRI data. Six AErosol RObotic NETwork (AERONET) sites with different surface types are used for detailed analysis and 42 other AERONET sites are used for validation. From 445 collocations representing stable and homogeneous aerosol type, we find that >75% of the MSG-retrieved AOD at 0.6 and 0.8 μm values compare favourably with AERONET observed AOD values, within an error envelope of ± 0.05 ± 0.15 τ and a high correlation coefficient (R>0.86). The AOD datasets derived using the TS method with SEVIRI data is also compared with collocated AOD products derived from NASA TERRA and AQUA MODIS (The Moderate-resolution Imaging Spectroradiometer) data using the Dark Dense Vegetation (DDV) method and the Deep Blue algorithms. Using the TS method, the AOD could be retrieved for more pixels than with the NASA Deep Blue algorithm. This method is potentially also useful for surface reflectance retrieval using SEVIRI observations. The current paper focuses on AOD retrieval and analysis, and the analysis and validation of reflectance will be given in a following paper.
Extreme ozone depletion in the 2010–2011 Arctic winter stratosphere as observed by MIPAS/ENVISAT using a 2-D tomographic approach

We present observations of the 2010–2011 Arctic winter stratosphere from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) onboard ENVISAT. Limb sounding infrared measurements were taken by MIPAS during the Northern polar winter and into the subsequent spring, giving a continuous vertically resolved view of the Arctic dynamics, chemistry and polar stratospheric clouds (PSCs). We adopted a 2-D tomographic retrieval approach to account for the strong horizontal inhomogeneity of the atmosphere present under vortex conditions, self-consistently comparing 2011 to the 2-D analysis of 2003–2010. Unlike most Arctic winters, 2011 was characterized by a strong stratospheric vortex lasting until early April. Lower stratospheric temperatures persistently remained below the threshold for PSC formation, extending the PSC season up to mid-March, resulting in significant chlorine activation leading to ozone destruction. On 3 January 2011, PSCs were detected up to 30.5 ± 0.9 km altitude, representing the highest PSCs ever reported in the Arctic. Through inspection of MIPAS spectra, 83% of PSCs were identified as supercooled ternary solution (STS) or STS mixed with nitric acid trihydrate (NAT), 17% formed mostly by NAT particles, and only two cases by ice. In the lower stratosphere at potential temperature 450 K, vortex average ozone showed a daily depletion rate reaching 100 ppbv day−1. In early April at 18 km altitude, 10% of vortex measurements displayed total depletion of ozone, and vortex average values dropped to 0.6 ppmv. This corresponds to a chemical loss from early winter greater than 80%. Ozone loss was accompanied by activation of ClO, associated depletion of its reservoir ClONO2, and significant denitrification, which further delayed the recovery of ozone in spring. Once the PSC season halted, ClO was reconverted primarily into ClONO2. Compared to MIPAS observed 2003–2010 Arctic average values, the 2010–2011 vortex in late winter had 15 K lower temperatures, 40% lower HNO3 and 50% lower ozone, reaching the largest ozone depletion ever observed in the Arctic. The overall picture of this Arctic winter was remarkably closer to conditions typically found in the Antarctic vortex than ever observed before.
Commentary on using equivalent latitude in the upper troposphere and lower stratosphere

We discuss the use of potential vorticity (PV) based equivalent latitude (EqLat) and potential temperature (θ) coordinates in the upper troposphere and lower stratosphere (UTLS) for chemical transport studies. The main objective is to provide a cautionary note on using EqLat-θ coordinates for aggregating chemical tracers in the UTLS. Several examples are used to show 3-D distributions of EqLat together with chemical constituents for a range of θ. We show that the use of PV-θ coordinates may not be suitable for several reasons when tropospheric processes are an important part of a study. Due to the different static stability structures between the stratosphere and troposphere, the use of θ as a vertical coordinate does not provide equal representations of the UT and LS. Since the θ surfaces in the troposphere often intersect the surface of the Earth, the θ variable does not work well distinguishing the UT from the boundary layer when used globally as a vertical coordinate. We further discuss the duality of PV/EqLat as a tracer versus as a coordinate variable. Using an example, we show that while PV/EqLat serves well as a transport tracer in the UTLS region, it may conceal the chemical structure associated with wave breaking when used as a coordinate to average chemical tracers. Overall, when choosing these coordinates, considerations need to be made not only based on the time scale of PV being a conservative tracer, but also the specific research questions to be addressed.
Investigating sources of gaseous oxidized mercury in dry deposition at three sites across Florida, USA

During 2009–2010, the State of Florida established a series of air quality monitoring stations to collect data for development of a statewide total maximum daily load (TMDL) for mercury (Hg). At three of these sites, located near Ft. Lauderdale (DVE), Pensacola (OLF), and Tampa Bay (TPA), passive samplers for the measurement of air Hg concentrations and surrogate surfaces for measurement of Hg dry deposition were deployed. While it is known that Hg in wet deposition in Florida is high compared to the rest of the United States, there is little information on Hg dry deposition. The objectives of the work were to: (1) investigate the utility of passive sampling systems for Hg in an area with low and consistent air concentrations as measured by the Tekran® mercury measurement system, (2) estimate dry deposition of gaseous oxidized Hg, and (3) investigate potential sources. This paper focuses on Objective 3. All sites were situated within 15 km of 1000 MW electricity generating plants (EGPs) and major highways. Bi-weekly dry deposition and passive sampler Hg uptake were not directly correlated with the automated Tekran® system measurements, and there was limited agreement between these systems for periods of high deposition. Using diel, biweekly, and seasonal Hg observations, and ancillary data collected at each site, the potential sources of Hg deposited to surrogate surfaces were investigated. With this information, we conclude that there are three major processes/sources contributing to Hg dry deposition in Florida, with these varying as a function of location and time of year. These include: (1) in situ oxidation of locally and regionally derived Hg facilitated by mobile source emissions, (2) indirect and direct inputs of Hg from local EGPs, and (3) direct input of Hg associated with long range transport of air from the northeastern United States. Based on data collected with the surrogate surface sampling system, natural background dry deposition for Florida is estimated to be 0.03 ng m−2 h−1. Deposition associated with mobile sources is 0.10 ng m−2 h−1 at TPA and DVE, and 0.03 ng m−2 h−1 at OLF. Long range transport contributes 0.8 ng m−2 h−1 in the spring. At DVE ~0.10 ng m−2 h−1 is contributed directly or indirectly from local point sources. We also suggest based on the data collected with the Tekran® and passive sampling systems that different chemical forms of GOM are associated with each of these sources.
Parameterization of homogeneous ice nucleation for cloud and climate models based on classical nucleation theory

A new analytical parameterization of homogeneous ice nucleation is developed based on extended classical nucleation theory including new equations for the critical radii of the ice germs, free energies and nucleation rates as simultaneous functions of temperature and water saturation ratio. By representing these quantities as separable products of the analytical functions of temperature and supersaturation, analytical solutions are found for the integral-differential supersaturation equation and concentration of nucleated crystals. Parcel model simulations are used to illustrate the general behavior of various nucleation properties under various conditions, for justifications of the further key analytical simplifications, and for verification of the resulting parameterization. The final parameterization is based upon the values of the supersaturation that determines the current or maximum concentrations of the nucleated ice crystals. The crystal concentration is analytically expressed as a function of time and can be used for parameterization of homogeneous ice nucleation both in the models with small time steps and for substep parameterization in the models with large time steps. The crystal concentration is expressed analytically via the error functions or elementary functions and depends only on the fundamental atmospheric parameters and parameters of classical nucleation theory. The diffusion and kinetic limits of the new parameterization agree with previous semi-empirical parameterizations.
The effects of mineral dust particles, aerosol regeneration and ice nucleation parameterizations on clouds and precipitation

This study focuses on the effects of aerosol particles on the formation of convective clouds and precipitation in the Eastern Mediterranean Sea, with a special emphasis on the role of mineral dust particles in these processes. We used a new detailed numerical cloud microphysics scheme that has been implemented in the Weather Research and Forecast (WRF) model in order to study aerosol–cloud interaction in 3-D configuration based on 1° × 1° resolution reanalysis meteorological data. Using a number of sensitivity studies, we tested the contribution of mineral dust particles and different ice nucleation parameterizations to precipitation development. In this study we also investigated the importance of recycled (regenerated) aerosols that had been released to the atmosphere following the evaporation of cloud droplets. The results showed that increased aerosol concentration due to the presence of mineral dust enhanced the formation of ice crystals. The dynamic evolution of the cloud system sets the time periods and regions in which heavy or light precipitation occurred in the domain. The precipitation rate, the time and duration of precipitation were affected by the aerosol properties only at small spatial scales (with areas of about 20 km2). Changes of the ice nucleation scheme from ice supersaturation-dependent parameterization to a recent approach of aerosol concentration and temperature-dependent parameterization modified the ice crystals concentrations but did not affect the total precipitation in the domain. Aerosol regeneration modified the concentration of cloud droplets at cloud base by dynamic recirculation of the aerosols but also had only a minor effect on precipitation. The major conclusion from this study is that the effect of mineral dust particles on clouds and total precipitation is limited by the properties of the atmospheric dynamics and the only effect of aerosol on precipitation may come from significant increase in the concentration of accumulation mode aerosols. In addition, the presence of mineral dust had a much smaller effect on the total precipitation than on its spatial distribution.