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Impact of prescribed SSTs on climatologies and long-term trends in CCM simulations

Chemistry-Climate Model (CCM) simulations are commonly used to project the past and future development of the dynamics and chemistry of the stratosphere, and in particular the ozone layer. So far, CCMs are usually not interactively coupled to an ocean model, so that sea surface temperatures (SSTs) and sea ice coverage are prescribed in the simulations. While for future integrations SSTs have to be taken from precalculated climate model projections, for CCM experiments resembling the past either modelled or observed SSTs can be used. This study addresses the question to which extent atmospheric climatologies and long-term trends for the recent past simulated in the CCM E39C-A differ when choosing either observed or modelled SSTs. Furthermore, the processes of how the SST signal is communicated to the atmosphere, and in particular to the stratosphere are examined. Two simulations that differ only with respect to the prescribed SSTs and that span years 1960 to 1999 are used. Significant differences in temperature and ozone climatologies between the model simulations are found. The differences in ozone are attributed to differences in the meridional circulation, which are in turn driven by weaker wave forcing in the simulation with generally lower SSTs. The long-term trends over 40 years in annual mean temperature and ozone differ only in the troposphere, where temperatures are directly influenced by the local SST trends. Differences in temperature and ozone trends are only found on shorter time scales. The trends in tropical upwelling, as a measure of the strength of the Brewer-Dobson circulation (BDC), differ strongly between the simulations. A reverse from negative to positive trends is found in the late 1970s in the simulation using observed SSTs while trends are positive throughout the simulation when using modelled SSTs. The increase in the BDC is a robust feature of the simulations only after about 1980 and is evident mainly in the tropics in the lower stratosphere.
Classification of Northern Hemisphere stratospheric ozone and water vapor profiles by meteorological regime

The subtropical and polar upper troposphere fronts and the polar vortex serve as the boundaries to divide the Northern Hemisphere into four meteorological regimes. These regimes are defined as (1) the arctic regime – within the polar vortex, (2) the polar regime – between the polar front and the polar vortex, or when the latter is not present, the pole, (3) the midlatitude regime – between the subtropical and polar fronts, and (4) the tropical regime – between the equator and the subtropical front. Data from the Halogen Occultation Experiment (HALOE) and the Stratospheric Aerosol and Gas Experiment II (SAGE II) were used to show that within each meteorological regime, ozone and water profiles are characterized by unique ozonepause and hygropause heights. Daily measurements and seven-year (1997–2003) monthly climatologies showed that, within each meteorological regime, both constituents exhibited distinct profile shapes from the tropopause up to approximately 20 km. This distinction was most pronounced in the winter and spring months, and weak in the summer and fall. Despite differences in retrieval techniques and sampling between the SAGE and HALOE instruments, the seven-year monthly climatologies calculated for each regime agreed well for both species below ~22 km. Given that profiles of ozone and water vapor exhibit unique profiles shapes within each regime in the UTLS, trends in this region will therefore be the result of both changes within each meteorological regime, and changes in the relative contribution of each regime to a given zonal band over time.
Influence of entrainment of CCN on microphysical properties of warm cumulus

We use a 1-D cloud model with explicit microphysics and a binned representation of the aerosol size distribution to investigate the influence of entrainment of cloud condensation nuclei (CCN) on the microphysical development of warm cumulus clouds. For a more realistic representation of cloud drop spectral width, the model separates droplets that grow on aerosol that is initially present in the cloud from droplets growing on entrained aerosol. Model results are compared with observations of trade wind cumulus microphysics from the Rain in Cumulus over the Ocean experiment (RICO, 2004–2005). The results indicate that CCN are entrained throughout the entire cloud depth, and inside the cloud part of these may be activated. Compared to a simulation where entrainment of ambient CCN is neglected this leads to higher cloud droplet number concentrations (CDNC) and a continuous presence of droplets in the range smaller than ~5 μm that is consistent with the observations. Cloud dynamics are sensitive to the entrainment parameter as well as to the applied initial vertical velocity, as expressed by the liquid water content and cloud top height. However, simulated cloud drop spectra remain relatively unaffected for the specific conditions during RICO.
Evolution of stratospheric ozone and water vapour time series studied with satellite measurements

The long term evolution of stratospheric ozone and water vapour has been investigated by extending satellite time series to April 2008. For ozone, we examine monthly average ozone values from various satellite data sets for nine latitude and altitude bins covering 60° S to 60° N and 20–45 km and covering the time period of 1979–2008. Data are from the Stratospheric Aerosol and Gas Experiment (SAGE I+II), the HALogen Occultation Experiment (HALOE), the Solar BackscatterUltraViolet-2 (SBUV/2) instrument, the Sub-Millimetre Radiometer (SMR), the Optical Spectrograph InfraRed Imager System (OSIRIS), and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartograpY (SCIAMACHY). Monthly ozone anomalies are calculated by utilising a linear regression model, which also models the solar, quasi-biennial oscillation (QBO), and seasonal cycle contributions. Individual instrument ozone anomalies are combined producing an all instrument average. Assuming a turning point of 1997 and that the all instrument average is represented by good instrumental long term stability, the largest statistically significant ozone declines (at two sigma) from 1979–1997 are seen at the mid-latitudes between 35 and 45 km, namely −7.2%±0.9%/decade in the Northern Hemisphere and −7.1%±0.9%/in the Southern Hemisphere. Furthermore, for the period 1997 to 2008 we find that the same locations show the largest ozone recovery (+1.4% and +0.8%/decade respectively) compared to other global regions, although the estimated trend model errors indicate that the trend estimates are not significantly different from a zero trend at the 2 sigma level. An all instrument average is also constructed from water vapour anomalies during 1991–2008, using the SAGE II, HALOE, SMR, and the Microwave Limb Sounder (Aura/MLS) measurements. We report that the decrease in water vapour values after 2001 slows down around 2004–2005 in the lower tropical stratosphere (20–25 km) and has even shown signs of increasing until present. We show that a similar correlation is also seen with the temperature measured at 100 hPa during this same period.
Effect of regional precursor emission controls on long-range ozone transport – Part 1: Short-term changes in ozone air quality

Observations and models demonstrate that ozone and its precursors can be transported between continents and across oceans. We model the influences of 10% reductions in anthropogenic nitrogen oxide (NOx) emissions from each of nine world regions on surface ozone air quality in that region and all other regions. In doing so, we quantify the relative importance of long-range transport between all source-receptor pairs, for direct short-term ozone changes. We find that for population-weighted concentrations during the three-month "ozone-season", the strongest inter-regional influences are from Europe to the Former Soviet Union, East Asia to Southeast Asia, and Europe to Africa. The largest influences per unit of NOx reduced, however, are seen for source regions in the tropics and Southern Hemisphere, which we attribute mainly to greater sensitivity to changes in NOx in the lower troposphere, and secondarily to increased vertical convection to the free troposphere in tropical regions, allowing pollutants to be transported further. Results show, for example, that NOx reductions in North America are ~20% as effective per unit NOx in reducing ozone in Europe during summer, as NOx reductions from Europe itself. Reducing anthropogenic emissions of non-methane volatile organic compounds (NMVOCs) and carbon monoxide (CO) by 10% in selected regions, can have as large an impact on long-range ozone transport as NOx reductions, depending on the source region. We find that for many source-receptor pairs, the season of greatest long-range influence does not coincide with the season when ozone is highest in the receptor region. Reducing NOx emissions in most source regions causes a larger decrease in export of ozone from the source region than in ozone production outside of the source region.
Effect of regional precursor emission controls on long-range ozone transport – Part 2: Steady-state changes in ozone air quality and impacts on human mortality

Large-scale changes in ozone precursor emissions affect ozone directly in the short term, and also affect methane, which in turn causes long-term changes in ozone that affect surface ozone air quality. Here we assess the effects of changes in ozone precursor emissions on the long-term change in surface ozone via methane, as a function of the emission region, by modeling 10% reductions in anthropogenic nitrogen oxide (NOx) emissions from each of nine world regions. Reductions in NOx emissions from all world regions increase methane and long-term surface ozone. While this long-term increase is small compared to the intra-regional short-term ozone decrease, it is comparable to or larger than the short-term inter-continental ozone decrease for some source-receptor pairs. The increase in methane and long-term surface ozone per ton of NOx reduced is greatest in tropical and Southern Hemisphere regions, exceeding that from temperate Northern Hemisphere regions by roughly a factor of ten. We also assess changes in premature ozone-related human mortality associated with regional precursor reductions and long-range transport, showing that for 10% regional NOx reductions, the strongest inter-regional influence is for emissions from Europe affecting mortalities in Africa. Reductions of NOx in North America, Europe, the Former Soviet Union, and Australia are shown to reduce more mortalities outside of the source regions than within. Among world regions, NOx reductions in India cause the greatest number of avoided mortalities per ton, mainly in India itself. Finally, by increasing global methane, NOx reductions in one hemisphere tend to cause long-term increases in ozone concentration and mortalities in the opposite hemisphere. Reducing emissions of methane, and to a lesser extent carbon monoxide and non-methane volatile organic compounds, alongside NOx reductions would avoid this disbenefit.
The climatic effects of the direct injection of water vapour into the stratosphere by large volcanic eruptions

We describe a novel mechanism that can significantly lower the amplitude of the climatic response to certain large volcanic eruptions and examine its impact with a coupled ocean-atmosphere climate model. If sufficiently large amounts of water vapour enter the stratosphere, a climatically significant amount of water vapour can be left over in the lower stratosphere after the eruption, even after sulphate aerosol formation. This excess stratospheric humidity warms the tropospheric climate, and acts to balance the climatic cooling induced by the volcanic aerosol, especially because the humidity anomaly lasts for a period that is longer than the residence time of aerosol in the stratosphere. In particular, northern hemisphere high latitude cooling is reduced in magnitude. We discuss this mechanism in the context of the discrepancy between the observed and modelled cooling following the Krakatau eruption in 1883. We hypothesize that moist coignimbrite plumes caused by pyroclastic flows travelling over ocean rather than land, resulting from an eruption close enough to the ocean, might provide the additional source of stratospheric water vapour.
Factors controlling the distribution of ozone in the West African lower troposphere during the AMMA (African Monsoon Multidisciplinary Analysis) wet season campaign

Ozone and its precursors were measured on board the Facility for Airborne Atmospheric Measurements (FAAM) BAe 146 Atmospheric Research Aircraft during the monsoon season 2006 as part of the African Monsoon Multidisciplinary Analysis (AMMA) campaign. One of the main features observed in the west African boundary layer is the increase of the ozone mixing ratios from 25 ppbv over the forested area (south of 12° N) up to 40 ppbv over the Sahelian area. We employ a two-dimensional (latitudinal versus vertical) meteorological model coupled with an O3-NOx-VOC chemistry scheme to simulate the distribution of trace gases over West Africa during the monsoon season and to analyse the processes involved in the establishment of such a gradient. Including an additional source of NO over the Sahelian region to account for NO emitted by soils we simulate a mean NOx concentration of 0.7 ppbv at 16° N versus 0.3 ppbv over the vegetated region further south in reasonable agreement with the observations. As a consequence, ozone is photochemically produced with a rate of 0.25 ppbv h−1 over the vegetated region whilst it reaches up to 0.75 ppbv h−1 at 16° N. We find that the modelled gradient is due to a combination of enhanced deposition to vegetation, which decreases the ozone levels by up to 11 pbbv, and the aforementioned enhanced photochemical production north of 12° N. The peroxy radicals required for this enhanced production in the north come from the oxidation of background CO and CH4 as well as from VOCs. Sensitivity studies reveal that both the background CH4 and partially oxidised VOCs, produced from the oxidation of isoprene emitted from the vegetation in the south, contribute around 5–6 ppbv to the ozone gradient. These results suggest that the northward transport of trace gases by the monsoon flux, especially during nighttime, can have a significant, though secondary, role in determining the ozone gradient in the boundary layer. Convection, anthropogenic emissions and NO produced from lightning do not contribute to the establishment of the discussed ozone gradient.
Satellite observations and model simulations of tropospheric NO2 columns over south-eastern Europe

Satellite observations of nitrogen dioxide (NO2) tropospheric columns over south-eastern Europe are analyzed to study the characteristics of the spatial and temporal variability of pollution in the area. The interannual variability of the tropospheric NO2 columns is presented over urban, rural and industrial locations based on measurements from four satellite instruments, GOME/ERS-2, SCIAMACHY/Envisat, OMI/Aura and GOME-2/MetOp spanning a period of over twelve years. The consistency between the different datasets over the area is investigated. Two operational algorithms for the retrieval of tropospheric NO2 are considered, the one developed jointly by the Royal Netherlands Meteorological Institute and Belgian Institute for Space Astronomy and the one developed by the University of Bremen. The tropospheric NO2 columns for the area under study have been simulated for the period 1996–2001 with the Comprehensive Air Quality Model (CAMx) and are compared with GOME measurements. Over urban and industrial locations the mean tropospheric NO2 columns range between 3 and 7.0×1015 molecules/cm2, showing a seasonal variability with a peak to peak amplitude of about 6.0×1015 molecules/cm2, while the background values over rural sites are close to 1.1×1015 molecules/cm2. Differences in the overpass time and spatial resolution of the different satellites, as well as differences in the algorithms, introduce significant differences in the estimated columns however the correlation between the different estimates is higher than 0.8. It is found that the model simulations reveal similar spatial patterns as the GOME observations, a result which is consistent with both algorithms. Although the model simulations show a mean bias of −0.1×1015 molecules/cm2 under clean conditions, the modeled temporal correlation of 0.5 is poor in absence of biogenic and biomass burning emissions.
An overview of two years of ozone radio soundings over Cotonou as part of AMMA

As part of the African Monsoon Multidisciplinary Analysis (AMMA) program, a total of 98 ozone vertical profiles over Cotonou, Benin, have been measured during a 26 month period (December 2004–January 2007). These regular measurements broadly document the seasonal and interannual variability of ozone in both the troposphere and the lower stratosphere over West Africa for the first time. This data set is complementary to the MOZAIC observations made from Lagos between 0 and 12 km during the period 1998–2004. Both data sets highlight the unique way in which West Africa is impacted by two biomass burning seasons: in December–February (dry season) due to burning in the Sahelian band and in June-August (wet season) due to burning in southern Africa. High interannual variabilities between Cotonou and Lagos data sets and within each data set are observed and are found to be a major characteristic of this region. In particular, the dry and wet seasons are discussed in order to set the data of the Special Observing Periods (SOPs) into a climatological context. Compared to other dry and wet seasons, the 2006 dry and wet season campaigns took place in rather high ozone environments. During the sampled wet seasons, southern intrusions of biomass burning were particularly frequent with concentrations up to 120 ppbv of ozone in the lower troposphere. An insight into the ozone distribution in the upper troposphere and the lower stratosphere (up to 26 km) is given. The first tropospheric columns of ozone based on in-situ data over West Africa are assessed. They compare well with satellite products on seasonal and interannual time-scales, provided that the layer below 850 hPa where the remote instrument is less sensitive to ozone, is removed.