Retrievals of ethane from groundbased highresolution FTIR solar observations with updated line parameters: determination of the optimum strategy for the Jungfraujoch station.

Ethane (C2H6) is the most abundant Non-Methane HydroCarbon (NMHC) in the Earth’s atmosphere, with a lifetime of approximately 2 months. Its main sources are biomass burning, natural gas loss and biofuel consumption. Oxidation by the hydroxyl radical is the major C2H6 sink as it controls its strong modulation throug the year. C2H6 is involved in the formation of tropospheric O3 and in the destruction of atmospheric methane through changes in OH. C2H6 is an indirect greenhouse gas with a net-global warming potential of 5.5 (100-yr horizon). Updates of retrieval parameters such as the spectroscopic linelists have been recently published. We will therefore characterize three µ-windows encompassing the strongest C2H6 features after careful selection of these new parameters, accounting at best for all interfering species. The aim is to lessen the fitting residuals while maximizing the information content, the precision and the reliability of the retrieved product. We will present updated C2H6 total and tropospheric column time series, using the SFIT-2 algorithm (v3.91) and high-resolution Fourier Transform Infrared (FTIR) solar absorption spectra recorded with a Bruker 120HR instrument, at the high altitude research station of the Jungfraujoch (46.5°N, 8.0°E, 3580 m asl), within the framework of the Network for the Detection of Atmospheric Composition Change (NDACC, http://www.ndacc.org). Comparisons with synthetic data produced by chemical transport models will also be presented

Aircraft emission mitigation by changing route altitude: A multi-model estimate of aircraft NOx emission impact on O3 photochemistry

The atmospheric impact of aircraft NOx emissions are studied using updated aircraft inventories for the year 2006, in order to estimate the photochemistry-related mitigation potential of shifting cruise altitudes higher or lower by 2000 ft. Applying three chemistry-transport models (CTM) and two climatechemistry models (CCM) in CTM mode, all including detailed tropospheric and stratospheric chemistry, we estimate the short-lived radiative forcing (RF) from O3 to range between 16.4 and 23.5 mW m 2, with a mean value of 19.5 mW m 2. Including the long-lived RF caused by changes in CH4, the total NOxrelated RF is estimated to about 5 mW m 2, ranging 1e8 mW m 2. Cruising at 2000 ft higher altitude increases the total RF due to aircraft NOx emissions by 2 ± 1 mW m 2, while cruising at 2000 ft lower altitude reduces RF by 2 ± 1 mWm 2. This change is mainly controlled by short-lived O3 and show that chemical NOx impact of contrail avoiding measures is likely small

Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions

Significant reductions in stratospheric ozone occur inside the polar vortices each spring when chlorine radicals produced by heterogeneous reactions on cold particle surfaces in winter destroy ozone mainly in two catalytic cycles, the ClO dimer cycle and the ClO/BrO cycle. Chlorofluorocarbons (CFCs), which are responsible for most of the chlorine currently present in the stratosphere, have been banned by the Montreal Protocol and its amendments, and the ozone layer is predicted to recover to 1980 levels within the next few decades. During the same period, however, climate change is expected to alter the temperature, circulation patterns and chemical composition in the stratosphere, and possible geo-engineering ventures to mitigate climate change may lead to additional changes. To realistically predict the response of the ozone layer to such influences requires the correct representation of all relevant processes. The European project RECONCILE has comprehensively addressed remaining questions in the context of polar ozone depletion, with the objective to quantify the rates of some of the most relevant, yet still uncertain physical and chemical processes. To this end RECONCILE used a broad approach of laboratory experiments, two field missions in the Arctic winter 2009/10 employing the high altitude research aircraft M55-Geophysica and an extensive match ozone sonde campaign, as well as microphysical and chemical transport modelling and data assimilation. Some of the main outcomes of RECONCILE are as follows: (1) vortex meteorology: the 2009/10 Arctic winter was unusually cold at stratospheric levels during the six-week period from mid-December 2009 until the end of January 2010, with reduced transport and mixing across the polar vortex edge; polar vortex stability and how it is influenced by dynamic processes in the troposphere has led to unprecedented, synoptic-scale stratospheric regions with temperatures below the frost point; in these regions stratospheric ice clouds have been observed, extending over >106km2 during more than 3 weeks. (2) Particle microphysics: heterogeneous nucleation of nitric acid trihydrate (NAT) particles in the absence of ice has been unambiguously demonstrated; conversely, the synoptic scale ice clouds also appear to nucleate heterogeneously; a variety of possible heterogeneous nuclei has been characterised by chemical analysis of the non-volatile fraction of the background aerosol; substantial formation of solid particles and denitrification via their sedimentation has been observed and model parameterizations have been improved. (3) Chemistry: strong evidence has been found for significant chlorine activation not only on polar stratospheric clouds (PSCs) but also on cold binary aerosol; laboratory experiments and field data on the ClOOCl photolysis rate and other kinetic parameters have been shown to be consistent with an adequate degree of certainty; no evidence has been found that would support the existence of yet unknown chemical mechanisms making a significant contribution to polar ozone loss. (4) Global modelling: results from process studies have been implemented in a prognostic chemistry climate model (CCM); simulations with improved parameterisations of processes relevant for polar ozone depletion are evaluated against satellite data and other long term records using data assimilation and detrended fluctuation analysis. Finally, measurements and process studies within RECONCILE were also applied to the winter 2010/11, when special meteorological conditions led to the highest chemical ozone loss ever observed in the Arctic. In addition to quantifying the 2010/11 ozone loss and to understand its causes including possible connections to climate change, its impacts were addressed, such as changes in surface ultraviolet (UV) radiation in the densely populated northern mid-latitudes

Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions : (RECONCILE) ; activities and results

The international research project RECONCILE has addressed central questions regarding polar ozone depletion, with the objective to quantify some of the most relevant yet still uncertain physical and chemical processes and thereby improve prognostic modelling capabilities to realistically predict the response of the ozone layer to climate change. This overview paper outlines the scope and the general approach of RECONCILE, and it provides a summary of observations and modelling in 2010 and 2011 that have generated an in many respects unprecedented dataset to study processes in the Arctic winter stratosphere. Principally, it summarises important outcomes of RECONCILE including (i) better constraints and enhanced consistency on the set of parameters governing catalytic ozone destruction cycles, (ii) a better understanding of the role of cold binary aerosols in heterogeneous chlorine activation, (iii) an improved scheme of polar stratospheric cloud (PSC) processes that includes heterogeneous nucleation of nitric acid trihydrate (NAT) and ice on non-volatile background aerosol leading to better model parameterisations with respect to denitrification, and (iv) long transient simulations with a chemistry-climate model (CCM) updated based on the results of RECONCILE that better reproduce past ozone trends in Antarctica and are deemed to produce more reliable predictions of future ozone trends. The process studies and the global simulations conducted in RECONCILE show that in the Arctic, ozone depletion uncertainties in the chemical and microphysical processes are now clearly smaller than the sensitivity to dynamic variability

Update and evaluation of the ozone dry deposition in Oslo CTM3 v1.0

High concentrations of ozone in ambient air are hazardous not only to humans but to the ecosystem in general. The impact of ozone damage on vegetation and agricultural plants in combination with advancing climate change may affect food security in the future. While the future scenarios in themselves are uncertain, there are limiting factors constraining the accuracy of surface ozone modeling also at present: the distribution and amount of ozone precursors and ozone-depleting substances, the stratosphere–troposphere exchange, as well as scavenging processes. Removal of any substance through gravitational settling or by uptake by plants and soil is referred to as dry deposition. The process of dry deposition is important for predicting surface ozone concentrations and understanding the observed amount and increase of tropospheric background ozone. The conceptual dry deposition velocities are calculated following a resistance-analogous approach, wherein aerodynamic, quasi-laminar, and canopy resistance are key components, but these are hard to measure explicitly. We present an update of the dry deposition scheme implemented in Oslo CTM3. We change from a purely empirical dry deposition parameterization to a more process-based one which takes the state of the atmosphere and vegetation into account. We examine the sensitivity of the scheme to various parameters, e.g., the stomatal conductance-based description of the canopy resistance and the choice of ozone surface resistance, and evaluate the resulting modeled ozone dry deposition with respect to observations and multi-model studies. Individual dry deposition velocities are now available for each land surface type and agree generally well with observations. We also estimate the impact on the modeled ozone concentrations at the surface. We show that the global annual total ozone dry deposition decreases with respect to the previous model version (−37 %), leading to an increase in surface ozone of more than 100 % in some regions. While high sensitivity to changes in dry deposition to vegetation is found in the tropics and the Northern Hemisphere, the largest impact on global scales is associated with the choice of prescribed ozone surface resistance over the ocean and deserts

Update and evaluation of the ozone dry deposition in Oslo CTM3 v1.0

High concentrations of ozone in ambient air are hazardous not only to humans but to the ecosystem in general. The impact of ozone damage on vegetation and agricultural plants in combination with advancing climate change may affect food security in the future. While the future scenarios in themselves are uncertain, there are limiting factors constraining the accuracy of surface ozone modeling also at present: the distribution and amount of ozone precursors and ozone-depleting substances, the stratosphere–troposphere exchange, as well as scavenging processes. Removal of any substance through gravitational settling or by uptake by plants and soil is referred to as dry deposition. The process of dry deposition is important for predicting surface ozone concentrations and understanding the observed amount and increase of tropospheric background ozone. The conceptual dry deposition velocities are calculated following a resistance-analogous approach, wherein aerodynamic, quasi-laminar, and canopy resistance are key components, but these are hard to measure explicitly. We present an update of the dry deposition scheme implemented in Oslo CTM3. We change from a purely empirical dry deposition parameterization to a more process-based one which takes the state of the atmosphere and vegetation into account. We examine the sensitivity of the scheme to various parameters, e.g., the stomatal conductance-based description of the canopy resistance and the choice of ozone surface resistance, and evaluate the resulting modeled ozone dry deposition with respect to observations and multi-model studies. Individual dry deposition velocities are now available for each land surface type and agree generally well with observations. We also estimate the impact on the modeled ozone concentrations at the surface. We show that the global annual total ozone dry deposition decreases with respect to the previous model version (−37 %), leading to an increase in surface ozone of more than 100 % in some regions. While high sensitivity to changes in dry deposition to vegetation is found in the tropics and the Northern Hemisphere, the largest impact on global scales is associated with the choice of prescribed ozone surface resistance over the ocean and deserts

Land cover change in low-warming scenarios may enhance the climate role of secondary organic aerosols

Most socioeconomic pathways compatible with the aims of the Paris Agreement include large changes to land use and land cover. The associated vegetation changes can interact with the atmosphere and climate through numerous mechanisms. One of these is emissions of biogenic volatile organic compounds (BVOCs), which may lead to the formation of secondary organic aerosols (SOAs) and atmospheric chemistry changes. Here, we use a modeling framework to explore potential future global and regional changes in SOA and tropospheric ozone following idealized, large-scale vegetation perturbations, and their resulting radiative forcing (RF). Guided by projections in low-warming scenarios, we modify crop and forest cover, separately, and in concurrence with changes in anthropogenic emissions and CO2 level. We estimate that increasing global forest cover by 30% gives a 37% higher global SOA burden, with a resulting forcing of −0.13 W m−2. The effect on tropospheric ozone is relatively small. Large SOA burden changes of up to 48% are simulated for South America and Sub-Saharan Africa. Conversely, increasing crop cover at the expense of tropical forest, yields similar changes but of opposite sign. The magnitude of these changes is strongly affected by the concurrent evolution of anthropogenic emissions. Our land cover perturbations are representative of energy crop expansion and afforestation, two key mitigation measures in 1.5 °C compatible scenarios. Our results hence indicate that depending on the role of these two in the underlying mitigation strategies, scenarios with similar long-term global temperature levels could lead to opposite effects on SOA. Combined with the complexity of factors that control SOA, this highlights the importance of including BVOC effects in further studies and assessments of climate and air quality mitigation involving the land surface

Retrievals of ethane from ground-based high-resolution FTIR solar observations with updated line parameters: determination of the optimum strategy for the Jungfraujoch station.

Ethane (C2H6) is the most abundant Non-Methane HydroCarbon (NMHC) in the Earth’s atmosphere, with a lifetime of approximately 2 months. C2H6 has both anthropogenic and natural emission sources such as biomass burning, natural gas loss and biofuel consumption. Oxidation by the hydroxyl radical is by far the major C2H6 sink as the seasonally changing OH concentration controls the strong modulation of the ethane abundance throughout the year. Ethane lowers Cl atom concentrations in the lower stratosphere and is a major source of peroxyacetyl nitrate (PAN) and carbon monoxide (by reaction with OH). Involved in the formation of tropospheric ozone and in the destruction of atmospheric methane through changes in OH, C2H6 is a non-direct greenhouse gas with a net-global warming potential (100-yr horizon) of 5.5. The retrieval of ethane from ground-based infrared (IR) spectra is challenging. Indeed, the fitting of the ethane features is complicated by numerous interferences by strong water vapor, ozone and methane absorptions. Moreover, ethane has a complicated spectrum with many interacting vibrational modes and the current state of ethane parameters in HITRAN (e.g. : Rothman et al., 2009, see http://www.hitran.com) was rather unsatisfactory in the 3 µm region. In fact, PQ branches outside the 2973–3001 cm-1 range are not included in HITRAN, and most P and R structures are missing. New ethane absorption cross sections recorded at the Molecular Spectroscopy Facility of the Rutherford Appleton Laboratory (Harrison et al., 2010) are used in our retrievals. They were calibrated in intensity by using reference low-resolution spectra from the Pacific Northwest National Laboratory (PNNL) IR database. Pseudoline parameters fitted to these ethane spectra have been combined with HITRAN 2004 line parameters (including all the 2006 updates) for all other species encompassed in the selected microwindows. Also, the improvement brought by the update of the line positions and intensities of methyl chloride (CH3Cl) in the 3.4 m region (Bray et al., 2011) will be quantified. The ethane a priori volume mixing ratio (VMR) profile and associated covariance are based on synthetic data from the chemical transport model (CTM) of the University of Oslo. In this contribution, we will present updated ethane total and tropospheric column retrievals, using the SFIT-2 algorithm (v3.91) and high-resolution Fourier Transform Infrared (FTIR) solar absorption observations recorded with a Bruker 120HR instrument, at the high altitude research station of the Jungfraujoch (46.5°N, 8°E, 3580 m asl), within the framework of the Network for the Detection of Atmospheric Composition Change (NDACC, visit http://www.ndacc.org). We will characterize three microwindows encompassing the strongest ethane features after careful selection of a priori VMR profiles, spectroscopic parameters, accounting at best for all interfering species. We will then present the retrieval strategy representative of the best combination of those three characterized micro-windows in order to minimize the fitting residuals while maximizing the information content, the precision and the reliability of the retrieved product. The long-term C2H6 column time series will be produced using the Jungfraujoch observational database. Comparisons with synthetic data produced by two chemical transport model (CHASER and the one of the University of Oslo) will also be presented and analyzed, aiming at the determination and interpretation of long-term trends and interannual variations of ethane at Northern mid-latitudes

Atmospheric Ozone and Methane in a Changing Climate

Ozone and methane are chemically active climate-forcing agents affected by climate–chemistry interactions in the atmosphere. Key chemical reactions and processes affecting ozone and methane are presented. It is shown that climate-chemistry interactions have a significant impact on the two compounds. Ozone, which is a secondary compound in the atmosphere, produced and broken down mainly in the troposphere and stratosphre through chemical reactions involving atomic oxygen (O), NOx compounds (NO, NO2), CO, hydrogen radicals (OH, HO2), volatile organic compounds (VOC) and chlorine (Cl, ClO) and bromine (Br, BrO). Ozone is broken down through changes in the atmospheric distribution of the afore mentioned compounds. Methane is a primary compound emitted from different sources (wetlands, rice production, livestock, mining, oil and gas production and landfills).Methane is broken down by the hydroxyl radical (OH). OH is significantly affected by methane emissions, defined by the feedback factor, currently estimated to be in the range 1.3 to 1.5, and increasing with increasing methane emission. Ozone and methane changes are affected by NOx emissions. While ozone in general increase with increases in NOx emission, methane is reduced, due to increases in OH. Several processes where current and future changes have implications for climate-chemistry interactions are identified. It is also shown that climatic changes through dynamic processes could have significant impact on the atmospheric chemical distribution of ozone and methane, as we can see through the impact of Quasi Biennial Oscillation (QBO). Modeling studies indicate that increases in ozone could be more pronounced toward the end of this century. Thawing permafrost could lead to important positive feedbacks in the climate system. Large amounts of organic material are stored in the upper layers of the permafrost in the yedoma deposits in Siberia, where 2 to 5% of the deposits could be organic material. During thawing of permafrost, parts of the organic material that is deposited could be converted to methane. Furthermore, methane stored in deposits under shallow waters in the Arctic have the potential to be released in a future warmer climate with enhanced climate impact on methane, ozone and stratospheric water vapor. Studies performed by several groups show that the transport sectors have the potential for significant impacts on climate-chemistry interactions. There are large uncertainties connected to ozone and methane changes from the transport sector, and to methane release and climate impact during permafrost thawing