Recent and future trends in synthetic greenhouse gas radiative forcing

Atmospheric measurements show that emissions of hydrofluorocarbons (HFCs) and hydrochlorofluorocarbons are now the primary drivers of the positive growth in synthetic greenhouse gas (SGHG) radiative forcing. We infer recent SGHG emissions and examine the impact of future emissions scenarios, with a particular focus on proposals to reduce HFC use under the Montreal Protocol. If these proposals are implemented, overall SGHG radiative forcing could peak at around 355 mW m[superscript −2] in 2020, before declining by approximately 26% by 2050, despite continued growth of fully fluorinated greenhouse gas emissions. Compared to “no HFC policy” projections, this amounts to a reduction in radiative forcing of between 50 and 240 mW m[superscript −2] by 2050 or a cumulative emissions saving equivalent to 0.5 to 2.8 years of CO2 emissions at current levels. However, more complete reporting of global HFC emissions is required, as less than half of global emissions are currently accounted for.Natural Environment Research Council (Great Britain) (Advanced Research Fellowship NE/I021365/1)United States. National Aeronautics and Space Administration (Upper Atmospheric Research Program Grant NNX11AF17G)United States. National Oceanic and Atmospheric Administratio

Characterization of uncertainties in atmospheric trace gas inversions using hierarchical Bayesian methods

We present a hierarchical Bayesian method for atmospheric trace gas inversions. This method is used to estimate emissions of trace gases as well as "hyper-parameters" that characterize the probability density functions (PDFs) of the a priori emissions and model-measurement covariances. By exploring the space of "uncertainties in uncertainties", we show that the hierarchical method results in a more complete estimation of emissions and their uncertainties than traditional Bayesian inversions, which rely heavily on expert judgment. We present an analysis that shows the effect of including hyper-parameters, which are themselves informed by the data, and show that this method can serve to reduce the effect of errors in assumptions made about the a priori emissions and model-measurement uncertainties. We then apply this method to the estimation of sulfur hexafluoride (SF6) emissions over 2012 for the regions surrounding four Advanced Global Atmospheric Gases Experiment (AGAGE) stations. We find that improper accounting of model representation uncertainties, in particular, can lead to the derivation of emissions and associated uncertainties that are unrealistic and show that those derived using the hierarchical method are likely to be more representative of the true uncertainties in the system. We demonstrate through this SF6 case study that this method is less sensitive to outliers in the data and to subjective assumptions about a priori emissions and model-measurement uncertainties than traditional methods

TransCom N2O model inter-comparison - Part 2:Atmospheric inversion estimates of N2O emissions

This study examines N2O emission estimates from five different atmospheric inversion frameworks based on chemistry transport models (CTMs). The five frameworks differ in the choice of CTM, meteorological data, prior uncertainties and inversion method but use the same prior emissions and observation data set. The posterior modelled atmospheric N2O mole fractions are compared to observations to assess the performance of the inversions and to help diagnose problems in the modelled transport. Additionally, the mean emissions for 2006 to 2008 are compared in terms of the spatial distribution and seasonality. Overall, there is a good agreement among the inversions for the mean global total emission, which ranges from 16.1 to 18.7 TgN yr(-1) and is consistent with previous estimates. Ocean emissions represent between 31 and 38% of the global total compared to widely varying previous estimates of 24 to 38%. Emissions from the northern mid- to high latitudes are likely to be more important, with a consistent shift in emissions from the tropics and subtropics to the mid- to high latitudes in the Northern Hemisphere; the emission ratio for 0-30A degrees N to 30-90A degrees N ranges from 1.5 to 1.9 compared with 2.9 to 3.0 in previous estimates. The largest discrepancies across inversions are seen for the regions of South and East Asia and for tropical and South America owing to the poor observational constraint for these areas and to considerable differences in the modelled transport, especially inter-hemispheric exchange rates and tropical convective mixing. Estimates of the seasonal cycle in N2O emissions are also sensitive to errors in modelled stratosphere-to-troposphere transport in the tropics and southern extratropics. Overall, the results show a convergence in the global and regional emissions compared to previous independent studies

Trace gases and CO2 isotope records from cabo de rama, India

Concentrations of carbon dioxide (CO2), methane (CH4), carbon monoxide (CO), nitrous oxide (N2O) and hydrogen (H2), and the stable carbon (δ 13C-CO2) and oxygen (δ 18O-CO2) isotopic composition of CO2 have been measured in air samples collected from Cabo de Rama (CRI), India, for the period 1993-2002. The observations show clear signatures of Northern and Southern Hemispheric (NH and SH) air masses, mixed with their regional fluxes and chemical loss mechanisms, resulting in complex seasonal variation of these gases. The CRI measurements are compared with remote marine sites at Seychelles and Mauna Loa. Simulations of two major anthropogenic greenhouse gases (CO2 and CH4) concentrations using a chemistry-transport model for the CRI site suggest that globally optimized fluxes can produce results comparable to the observations. We discuss that CRI observations have provided critical guidance in optimizing the fluxes to constrain the regional source/sinks balance

Exploring causes of interannual variability in the seasonal cycles of tropospheric nitrous oxide

Seasonal cycles in the mixing ratios of tropospheric nitrous oxide (N[subscript 2]O) are derived by detrending long-term measurements made at sites across four global surface monitoring networks. The detrended monthly data display large interannual variability, which at some sites challenges the concept of a "mean" seasonal cycle. In the Northern Hemisphere, correlations between polar winter lower stratospheric temperature and detrended N[subscript 2]O data, around the month of the seasonal minimum, provide empirical evidence for a stratospheric influence, which varies in strength from year to year and can explain much of the interannual variability in the surface seasonal cycle. Even at sites where a strong, competing, regional N[subscript 2]O source exists, such as from coastal upwelling at Trinidad Head, California, the stratospheric influence must be understood to interpret the biogeochemical signal in monthly mean data. In the Southern Hemisphere, detrended surface N[subscript 2]O monthly means are correlated with polar spring lower stratospheric temperature in months preceding the N[subscript 2]O minimum, providing empirical evidence for a coherent stratospheric influence in that hemisphere as well, in contrast to some recent atmospheric chemical transport model (ACTM) results. Correlations between the phasing of the surface N[subscript 2]O seasonal cycle in both hemispheres and both polar lower stratospheric temperature and polar vortex break-up date provide additional support for a stratospheric influence. The correlations discussed above are generally more evident in high-frequency in situ data than in data from weekly flask samples. Furthermore, the interannual variability in the N[subscript 2]O seasonal cycle is not always correlated among in situ and flask networks that share common sites, nor do the mean seasonal amplitudes always agree. The importance of abiotic influences such as the stratospheric influx and tropospheric transport on N[subscript 2]O seasonal cycles suggests that, at sites remote from local sources, surface N[subscript 2]O mixing ratio data by themselves are unlikely to provide information about seasonality in surface sources, e.g., for atmospheric inversions, unless the ACTMs employed in the inversions accurately account for these influences. An additional abioitc influence is the seasonal ingassing and outgassing of cooling and warming surface waters, which creates a thermal signal in tropospheric N[subscript 2]O that is of particular importance in the extratropical Southern Hemisphere, where it competes with the biological ocean source signal.United States. National Aeronautics and Space Administration (grant NNX08AB48G

Estimating regional methane surface fluxes: the relative importance of surface and GOSAT mole fraction measurements

We use an ensemble Kalman filter (EnKF), together with the GEOS-Chem chemistry transport model, to estimate regional monthly methane (CH₄) fluxes for the period June 2009–December 2010 using proxy dry-air column-averaged mole fractions of methane (XCH₄) from GOSAT (Greenhouse gases Observing SATellite) and/or NOAA ESRL (Earth System Research Laboratory) and CSIRO GASLAB (Global Atmospheric Sampling Laboratory) CH₄ surface mole fraction measurements. Global posterior estimates using GOSAT and/or surface measurements are between 510–516 Tg yr⁻¹, which is less than, though within the uncertainty of, the prior global flux of 529 ± 25 Tg yr⁻¹. We find larger differences between regional prior and posterior fluxes, with the largest changes in monthly emissions (75 Tg yr⁻¹) occurring in Temperate Eurasia. In non-boreal regions the error reductions for inversions using the GOSAT data are at least three times larger (up to 45%) than if only surface data are assimilated, a reflection of the greater spatial coverage of GOSAT, with the two exceptions of latitudes >60° associated with a data filter and over Europe where the surface network adequately describes fluxes on our model spatial and temporal grid. We use CarbonTracker and GEOS-Chem XCO₂ model output to investigate model error on quantifying proxy GOSAT XCH₄ (involving model XCO₂) and inferring methane flux estimates from surface mole fraction data and show similar resulting fluxes, with differences reflecting initial differences in the proxy value. Using a series of observing system simulation experiments (OSSEs) we characterize the posterior flux error introduced by non-uniform atmospheric sampling by GOSAT. We show that clear-sky measurements can theoretically reproduce fluxes within 10% of true values, with the exception of tropical regions where, due to a large seasonal cycle in the number of measurements because of clouds and aerosols, fluxes are within 15% of true fluxes. We evaluate our posterior methane fluxes by incorporating them into GEOS-Chem and sampling the model at the location and time of surface CH₄ measurements from the AGAGE (Advanced Global Atmospheric Gases Experiment) network and column XCH₄ measurements from TCCON (Total Carbon Column Observing Network). The posterior fluxes modestly improve the model agreement with AGAGE and TCCON data relative to prior fluxes, with the correlation coefficients (<i>r</i>²) increasing by a mean of 0.04 (range: −0.17 to 0.23) and the biases decreasing by a mean of 0.4 ppb (range: −8.9 to 8.4 ppb)

HFC-23 (CHF3) emission trend response to HCFC-22 (CHClF2) production and recent HFC-23 emission abatement measures

HFC-23 (also known as CHF3 [CHF subscript 3], fluoroform or trifluoromethane) is a potent greenhouse gas (GHG), with a global warming potential (GWP) of 14 800 for a 100-year time horizon. It is an unavoidable by-product of HCFC-22 (CHClF2 [CHCIF subscript 2], chlorodifluoromethane) production. HCFC-22, an ozone depleting substance (ODS), is used extensively in commercial refrigeration and air conditioning, in the extruded polystyrene (XPS) foam industries (dispersive applications) and also as a feedstock in fluoropolymer manufacture (a non-dispersive use). Aside from small markets in specialty uses, HFC-23 has historically been considered a waste gas that was, and often still is, simply vented to the atmosphere. Efforts have been made in the past two decades to reduce HFC-23 emissions, including destruction (incineration) in facilities in developing countries under the United Nations Framework Convention on Climate Change's (UNFCCC) Clean Development Mechanism (CDM), and by process optimization and/or voluntary incineration by most producers in developed countries. We present observations of lower-tropospheric mole fractions of HFC-23 measured by "Medusa" GC/MSD instruments from ambient air sampled in situ at the Advanced Global Atmospheric Gases Experiment (AGAGE) network of five remote sites (2007–2009) and in Cape Grim air archive (CGAA) samples (1978–2009) from Tasmania, Australia. These observations are used with the AGAGE 2-D atmospheric 12-box model and an inverse method to produce model mole fractions and a "top-down" HFC-23 emission history. The model 2009 annual mean global lower-tropospheric background abundance is 22.6 (±0.2) pmol mol−1 [mol superscript -1]. The derived HFC-23 emissions show a "plateau" during 1997–2003, followed by a rapid ~50% increase to a peak of 15.0 (+1.3/−1.2) Gg/yr in 2006. Following this peak, emissions of HFC-23 declined rapidly to 8.6 (+0.9/−1.0) Gg/yr in 2009, the lowest annual emission of the past 15 years. We derive a 1990–2008 "bottom-up" HFC-23 emission history using data from the United Nations Environment Programme and the UNFCCC. Comparison with the top-down HFC-23 emission history shows agreement within the stated uncertainties. In the 1990s, HFC-23 emissions from developed countries dominated all other sources, then began to decline and eventually became fairly constant during 2003–2008. By this point, with developed countries' emissions essentially at a plateau, the major factor controlling the annual dynamics of global HFC-23 emissions became the historical rise of developing countries' HCFC-22 dispersive use production, which peaked in 2007. Thereafter in 2007–2009, incineration through CDM projects became a larger factor, reducing global HFC-23 emissions despite rapidly rising HCFC-22 feedstock production in developing countries.NASA Upper Atmospheric Research Program (Grant NNX07AE89G)NASA Upper Atmospheric Research Program (Grant NNX07AF09G)NASA Upper Atmospheric Research Program (Grant NNX07AE87G

The Antarctic ozone hole during 2014

We review the 2014 Antarctic ozone hole, making use of a variety of ground-based and space-based measurements of ozone and ultra-violet radiation, supplemented by meteorological reanalyses. Although the polar vortex was relatively stable in 2014 and persisted some weeks longer into November than was the case in 2012 or 2013, the vortex temperature was close to the long-term mean in September and October with modest warming events occurring in both months, preventing severe depletion from taking place. Of the seven metrics reported here, all were close to their respective median values of the 1979–2014 record, being ranked between 16th and 21st of the 35 years for which adequate satellite observations exist

The Antarctic ozone hole during 2015 and 2016

We reviewed the 2015 and 2016 Antarctic ozone holes, making use of a variety of ground-based and spacebased measurements of ozone and ultraviolet radiation, supplemented by meteorological reanalyses. The ozone hole of 2015 was one of the most severe on record with respect to maximum area and integrated deficit and was notably longlasting, with many values above previous extremes in October, November and December. In contrast, all assessed metrics for the 2016 ozone hole were at or below their median values for the 37 ozone holes since 1979 for which adequate satellite observations exist. The 2015 ozone hole was influenced both by very cold conditions and enhanced ozone depletion caused by stratospheric aerosol resulting from the April 2015 volcanic eruption of Calbuco (Chile)