Historical evolution of radiative forcing of climate

We have compiled the evolution of the radiative forcing for several mechanisms based on our radiative transfer models using a variety of information sources to establish time histories. The anthropogenic forcing mechanisms considered are well-mixed greenhouse gases, ozone, and tropospheric aerosols (direct and indirect effect). The natural forcing mechanisms taken into account are the radiative effects of solar irradiance variation and particles of volcanic origin. In general there has been an increase in the radiative forcing during the 20th century. The exception is a decline in the radiative forcing in the 1945–1970 period. We have found that the evolution of anthropogenic particle emissions in the same period may have been a major cause of this decline in the forcing. We have discussed uncertainties in the various forcings and their evolution. The uncertainties are large for many forcing mechanisms, especially the impact of anthropogenic aerosols. In particular the indirect effect of aerosols on clouds is difficult to quantify. Several evolutions of their effect may have been possible, strongly influencing the evolution of the total anthropogenic radiative forcing.     

Greenhouse effect of NOX

Through various processes the nitrogen oxides (NO_X) interact with trace gases in the troposphere and stratosphere which do absorb in the spectral range relevant to the greenhouse effect (infrared wavelengths). The net effect is an enhancement of the greenhouse effect. The catalytic role of NO_X in the production of tropospheric ozone provides the most prominent contribution. The global waming potential is estimated as GWP (NO_X = 30 – 33 and 7 – 10 for the respective time horizons of 20 and 100 years, and is thereby comparable to that of methane. NO_X emissions in rural areas of anthropogenically influenced regions, or those in the vicinity of the txopopause caused by air traffic, cause the greenhouse effectivity to be substantially more intense. We estimate an additional 5–23 % for Germany’s contribution to the anthropogenic greenhouse effect as a result of the indirect greenhouse effects stemming from NO_X. Furthermore, a small and still inaccurately defined amount of the deposited NO_X which has primarily been converted into nitrates is again released from the soil into the atmosphere in the form of the long-lived greenhouse gas nitrous oxide (N₂O). Thus, anthropogenically induced NO_X emissions contribute to enhanced greenhouse effect and to stratospheric ozone depletion in the time scale of more than a century.     

Cloud Albedo,Greenhouse Effects,Atmospheric Chemistry,and Climate Change

Changes in global atmospheric chemistry and climate are taking place as a result of observed trends in long-lived species such as CO₂, CH₄, N₂O, and the CFCs. The continuation of these trends is expected to eventually lead to a major atmospheric warming that might profoundly affect the society we live in. Trends in short-lived species such as NOx and SOx are also suspected. These trends are not as well established, because the shorter-lived species vary spatially and temporally. Trends in NOx would be expected to lead to increases in tropospheric ozone that would add to the warming created by the other greenhouse gases. Trends in NOx could also alter tropospheric OH concentrations that could lead to changes in CH₄ and some of the CFCs. On the other hand, increases in sulfur emissions may alter cloud optical properties. The changes in cloud optical properties could possibly offset the warming expected from increases in greenhouse gases, depending on the role of natural oceanic sulfur emissions. This paper summarizes recent research in these areas and the interactions of climate and atmospheric chemistry.     

Atmospheric composition change: Climate–Chemistry interactions

Chemically active climate compounds are either primary compounds like methane (CH₄), removed by oxidation in the atmosphere, or secondary compounds like ozone (O₃), sulfate and organic aerosols, both formed and removed in the atmosphere. Man-induced climate–chemistry interaction is a two-way process: Emissions of pollutants change the atmospheric composition contributing to climate change through the aforementioned climate components, and climate change, through changes in temperature, dynamics, the hydrological cycle, atmospheric stability, and biosphere-atmosphere interactions, affects the atmospheric composition and oxidation processes in the troposphere. Here we present progress in our understanding of processes of importance for climate–chemistry interactions, and their contributions to changes in atmospheric composition and climate forcing. A key factor is the oxidation potential involving compounds like O₃ and the hydroxyl radical (OH). Reported studies represent both current and future changes. Reported results include new estimates of radiative forcing based on extensive model studies of chemically active climate compounds like O₃, and of particles inducing both direct and indirect effects. Through EU projects like ACCENT, QUANTIFY, and the AeroCom project, extensive studies on regional and sector-wise differences in the impact on atmospheric distribution are performed. Studies have shown that land-based emissions have a different effect on climate than ship and aircraft emissions, and different measures are needed to reduce the climate impact. Several areas where climate change can affect the tropospheric oxidation process and the chemical composition are identified. This can take place through enhanced stratospheric–tropospheric exchange of ozone, more frequent periods with stable conditions favoring pollution build up over industrial areas, enhanced temperature induced biogenic emissions, methane releases from permafrost thawing, and enhanced concentration through reduced biospheric uptake. During the last 5–10 years, new observational data have been made available and used for model validation and the study of atmospheric processes. Although there are significant uncertainties in the modeling of composition changes, access to new observational data has improved modeling capability. Emission scenarios for the coming decades have a large uncertainty range, in particular with respect to regional trends, leading to a significant uncertainty range in estimated regional composition changes and climate impact.     

A lagrangian approach to analyse the tropospheric ozone climatology in the tropics: Climatology of stratosphere–troposphere exchange at Reunion Island

Sixteen years of ozone measurements (1992–2006) at Reunion Island (21°S, 55.5°E) have been processed to detect stratospheric signatures on each single ozone profile.The characterisation method consists in the advection of the potential vorticity (PV) over two to ten days of backtrajectory with the lagrangian trajectory code LACYTRAJ. LACYTRAJ is a Trajectory-Reverse Domain Filling code using the ERA40 ECMWF database and allowing the reconstruction of high resolution advected PV profiles. Correlation between high values of ozone mixing ratio and high PV is interpreted as a stratospheric signature.A climatology of STE events at Reunion has been derived and reveals that STE events occur more frequently during spring (SON) and summer (DJF). The method is tested for a set of PV threshold values (i.e. 1 PVU, 1.5 PVU and 2 PVU) and for a set of duration of backtrajectories (i.e. 2 days, 5 days and 10 days). The number of detected STE is sensitive to PV threshold values and duration criterions. For instance, the number of stratospheric intrusions detected in October with a 1.5 PVU criterion ranges between 25% (2 days of backtrajectories) and 56% (10 days of backtrajectories). The vertical distributions of STE show intrusions covering the whole free troposphere (between 7 and 15 km) and mainly located in the upper troposphere.Finally, results show that an important number of stratospheric intrusions are detected during spring and in the upper troposphere what points at the contribution of the stratospheric source to the tropospheric ozone spring maximum which is strongly influenced by the biomass burning emissions from South Africa and Madagascar.     

Simulations of stratospheric to tropospheric transport during the tropical cyclone Marlene event

Enhanced ozone values observed in the upper troposphere near intense tropical cyclones have raised the question of the role of stratospheric–tropospheric exchange. The dynamical mechanisms involved in the enhanced ozone values of 6 April 1995 observed at Reunion and associated with the tropical cyclone Marlene could not be explained by ECMWF meteorological analysis with 1.125° horizontal resolution. A previous study based on the ECHAM model has demonstrated the impact of biomass burning, but of limited amplitude (<60–80 ppbv max). In this paper, the upper tropospheric ozone enhancement on the periphery of Marlene has been studied with a mesoscale model (MESO-NH). This model is able to reproduce a stratospheric PV filament into the troposphere, crossing the isentropes to the 350 K level. The ageostrophic circulation associated with divergence zones that have induced vertical movements has been shown. Further, the influence of vertical wind shear, evident in both the mesoscale analysis and in the idealized HURRICANE tropical cyclone model, also contributes to our understanding of this downward transport process.     

Transport impacts on atmosphere and climate: Shipping

Emissions of exhaust gases and particles from oceangoing ships are a significant and growing contributor to the total emissions from the transportation sector. We present an assessment of the contribution of gaseous and particulate emissions from oceangoing shipping to anthropogenic emissions and air quality. We also assess the degradation in human health and climate change created by these emissions. Regulating ship emissions requires comprehensive knowledge of current fuel consumption and emissions, understanding of their impact on atmospheric composition and climate, and projections of potential future evolutions and mitigation options. Nearly 70% of ship emissions occur within 400 km of coastlines, causing air quality problems through the formation of ground-level ozone, sulphur emissions and particulate matter in coastal areas and harbours with heavy traffic. Furthermore, ozone and aerosol precursor emissions as well as their derivative species from ships may be transported in the atmosphere over several hundreds of kilometres, and thus contribute to air quality problems further inland, even though they are emitted at sea. In addition, ship emissions impact climate. Recent studies indicate that the cooling due to altered clouds far outweighs the warming effects from greenhouse gases such as carbon dioxide (CO₂) or ozone from shipping, overall causing a negative present-day radiative forcing (RF). Current efforts to reduce sulphur and other pollutants from shipping may modify this. However, given the short residence time of sulphate compared to CO₂, the climate response from sulphate is of the order decades while that of CO₂ is centuries. The climatic trade-off between positive and negative radiative forcing is still a topic of scientific research, but from what is currently known, a simple cancellation of global mean forcing components is potentially inappropriate and a more comprehensive assessment metric is required. The CO₂ equivalent emissions using the global temperature change potential (GTP) metric indicate that after 50 years the net global mean effect of current emissions is close to zero through cancellation of warming by CO₂ and cooling by sulphate and nitrogen oxides.     

Climatic effect of observed changes in atmospheric trace gases at Antarctica

The seasonal decline in ozone in the Antarctic atmosphere has been termed the ‘Antarctic ozone hole’. Possibly this hole is caused by upper atmospheric wind, due to resumption of high solar activity after the polar night which produces large amounts of ozone-destroying nitric oxide or due to unusual chlorine chemistry at extreme cold temperatures and associated polar stratospheric clouds. Of particular concern is that the observed changes in ozone could be linked to the observed increases in the gases that affect ozone such as methane, nitrous oxide, etc. All these gases affect the climate of the Earth through their so-called ‘greenhouse’ action. We have examined the nature of the greenhouse effect on polar climate due to observed changes in atmospheric trace gases in Antarctica which are reported here.     

The ratio between nitrogen oxides and carbon monoxide total emissions as precursors of tropospheric hydroxyl content evolution

The Main Geophysical Observatory 2D channel photochemical model is used to study the behavior of tropospheric OH within the 30–60°N zonal belt in relation to changing NO_X and CO emissions. The changes of tropospheric OH as a function of the contributions by NO_X and CO emissions during the period 1850–2050 are calculated. Our estimations show that the largest annual increment of total tropospheric OH within the belt considered occurs in the 1985–1995 period, about 0.27% yr⁻¹. Based on scenarios of tropospheric pollution emissions in the first half of 21st century, the total tropospheric OH content will increase more slowly, by 0.12–0.15% yr⁻¹. The maximum growth of OH concentration occurs close to air pollution locations—in the lower troposphere during 1850–1995 but in the upper troposphere in the 21st century when the NO_X source from subsonic aircraft increases faster than the surface source.     

Estimation of the Natural Background of Ozone Present at Surface Rural Locations

The natural background in the ozone concentration at rural locations in the United States and western Europe has been estimated by use of several approaches. The approaches utilized include the following: (1) historical trends in ozone concentration measurements, (2) recent ozone measurements at remote sites, (3) use of tracers of air originating in the stratosphere or upper troposphere and (4) results from applications of tropospheric photochemical models. While each of these approaches has its own limitations it appears that the natural background of ozone during the warmer months of the year is in the range of 10 to 20 ppb. Most of the ozone originating in the lower stratosphere or upper troposphere is lost by chemical or physical removal processes as well as undergoing dilution by air in the lower troposphere before reaching ground level rural locations. Lower tropospheric photochemical processes, those below 5 km, are likely to account for most of the ozone measured at rural locations during the warmer months of the year.

A key aspect to improved quantitation of the contributions from lower tropospheric photochemical processes to ozone concentrations continues to be more extensive atmospheric measurements of the distribution of reactive species of nitrogen. The emission densities of anthropogenic sources of NO_x are known to be highly variable over populated areas of continents as well as between continental areas and the oceans. The emission densities of biogenic sources of NO_x are small, likely to be highly variable, but poorly quantitated. These wide variations indicate the need for use of three dimensional tropospheric photochemical models over large continental regions.

Available results do indicate higher efficiencies for ozone formation at lower NO_x concentrations, especially below 1 ppb.     

Modeling of ozone reactions on aircraft-related soot in the upper troposphere and lower stratosphere

Several studies in modeling atmospheric processes have suggested that heterogeneous chemistry on soot emitted from high altitude aircraft could affect stratospheric ozone depletion. However, these modeling studies were limited because they did not adequately consider the decrease in reaction probability with time as the surface of the soot becomes “poisoned” by its interactions with various gases. Here we extend UIUC's two-dimensional chemical-transport model to investigate possible effects of heterogeneous reactions of ozone on aircraft-generated carbon particles, including a treatment of soot poisoning in the model. We generally follow literature recommendations for ozone uptake probabilities and determine the available active sites on soot given partial pressures of the reactants, temperature, and time since soot emission in order to investigate ozone decrease. The regeneration of soot active sites is also taken into account in this study. We find that, even if active sites on soot surfaces are regenerated, upper troposphere and lower stratosphere ozone losses on aircraft emitted soot occurring through heterogeneous reactions are insignificant once poisoning effects are considered.     

Impact of stratospheric volcanic aerosols on climate: Evidence for aerosol shortwave and longwave forcing in the Southeastern U.S.

Major volcanic eruptions inject massive amounts of dust and gases into the lower stratosphere and upper troposphere. Stratospheric volcanic aerosols can scatter incoming solar radiation to space, increasing planetary albedo, reducing the total amount of solar energy reaching the troposphere and the earth's surface, and decreasing the daytime maximum temperature (aerosol shortwave forcing). They can also absorb and scatter outgoing terrestrial longwave radiation, increasing the nighttime minimum surface temperature (longwave forcing). However, persuasive evidence of climate response to this forcing has thus far been lacking. Here we examine patterns of annual and seasonal variations in mean maximum and minimum temperature trend during the periods 1992–1994 and 1985–1987 relative to that during the period 1988–1990 at 47 stations in the southeastern U.S. for evidence of such climate responses. The stratospheric volcanic aerosol optical depths over the southeastern U.S. during the period 1985–1994 were inferred from the Stratospheric Aerosol and Gases Experiment (SAGE) 11 satellite extinction measurement. After the long-term trend signals are removed, it is shown that the dominant decreasing trend of mean maximum temperature and the dominant increasing trend of mean minimum temperature over periods 1992–1994 and 1985–1987 relative to that over the period 1988–1990 are consistent with the distribution of stratospheric volcanic aerosols and predictions from aerosol radiative forcing in the southeastern U.S.     

Estimation of direct radiative forcing due to non-methane hydrocarbons

The direct radiative forcing due to non-methane hydrocarbons (NMHCs) has not previously been quantified. We use new measurements of infrared absorption cross-sections and a narrow band radiative transfer model to estimate a forcing. An upper limit to the global mean anthropogenic forcing is likely to be in the region of 0.015 W m^-2, less than 1% of the forcing due to other greenhouse gases. However, taking account of the natural NMHC loading and the vertical profile of these gases the actual radiative forcing is likely to be somewhat less than this.     

The surface radiative forcing of nitric acid for northern mid-latitudes

Ground-based, high-resolution measurements of downward atmospheric thermal emission spectra are reported for a northern mid-latitude location for summer and winter conditions. These measurements clearly show the presence of the 11.3-μm thermal emission band of nitric acid situated between 850–920 cm⁻¹. By using the FASCOD3 line-by-line radiation code to simulate the background thermal emission, the measured seasonally averaged surface radiative forcing due to nitric acid is determined to be 0.055 W m⁻²±15%. The zenith column amounts of nitric acid are found to vary between 7.9×10¹⁵ and 1.1×10¹⁶ molecules cm⁻²±15%. An estimation is made of the contribution of nitric acid to the direct radiative forcing of the Earth's surface since pre-industrial times for northern mid-latitudes. This work suggests that nitric acid may play a role that is comparable to that of other greenhouse gases, such as CFC-11, in the forcing of the Earth's climate system. Under polluted conditions, nitric acid may contribute about half of the radiative forcing that is currently associated with tropospheric ozone.     

On the scientific basis for global warming scenarios

The scientific basis for current projections of significant warming due to enhanced minor greenhouse gases in the atmosphere is reviewed. Care is taken to distinguish the issue of changes in radiative forcing at the earth's surface from the issue of the climatic response to this forcing. With respect to the former, it is noted that the predicted forcing is, in fact, small (2 W m(-2) at the surface for a doubling of CO(2), or less than 1% of the absorbed solar flux). With respect to the latter, it is noted that predictions of significant warming are dependent on the presence of large positive feedbacks serving to amplify the response. The largest of these feedbacks in current models involves water vapor at upper levels in the troposphere. This feedback appears to be largely a model artifact, and evidence is presented that models may even have the wrong sign for this feedback. The possibility is examined that the response of climate to major volcanic eruptions may provide a test of the climate system's amplification. The basis for this possibility is the fact that the response delay of the ocean-atmosphere system is proportional to the system gain.     

Stabilization of the Greenhouse Impact Caused by Anthropogenic Emissions from Nordic Countries

Abstract

The possibility of decreasing the Nordic countries’ contribution to global warming in the future is examined. Anthropogenic carbon dioxide (CO2), methane (CH4), and nitrous oxide (N2O) emissions are considered. Global average radiative forcing is used as a measure of the greenhouse impact caused by the emissions. Past emissions are included in the study because they have impact far into the future. The calculation method utilized in this study can be applied to any other country.

Two hypothetical future emission development cases are presented, and the radiative forcing caused by them is calculated. In the higher emission (case A) CO2 emissions remain above current level, while N2O and CH4 emissions decrease. In the lower emission (case B) the emissions decrease to about one–tenth of the current emissions by the year 2100.

Only if very strict emission reductions (case B) take place will the greenhouse impact of the Nordic countries return to current levels during next century. Likewise, the per capita radiative forcing of Nordic countries will remain above global average unless the emissions decrease drastically (case B) and the current population levels are used in per capita calculation.     

Monitoring of ozone in a marine environment in Tenerife (Canary Islands)

In the Aguere Valley (in the oceanic boundary layer at Tenerife, 28°N, 16°W, 580 m a.s.l.) the ozone levels were monitored for ambient air quality assessment. Although precursors are emitted in this area, the strong correlation between ozone levels and wind velocity indicates that ozone is transported into the valley from the ocean. The inland ozone supply along the valley is induced by an orographic channelling effect of the northern oceanic air masses. The highest ozone concentrations are mostly recorded during the nocturnal stage under the influence of fresh oceanic air masses, and during high wind speed events. The seasonal cycle is characterised by elevated ozone mixing ratios in the spring (nighttime levels >45 ppbv) and low mixing ratios in the summer (nighttime levels in the range 20–35 ppbv). Back-trajectory analysis shows that the ozone monitored in the Aguere Valley is associated with long-range transport processes. High ozone events in the spring are associated with transport from upper tropospheric levels, both over the North Atlantic-high latitudes (>45°N) and Europe. This downward transport was observed in the western edge of upper tropospheric cyclones, which suggests that the upper tropospheric/low stratospheric ozone sources play a significant role. In summer, ozone is mainly transported from the North Atlantic-high latitudes (>45°N) and from mid- to low-tropospheric levels. In autumn and winter, the high ozone concentrations are transported from sources located a few km above the North Atlantic-high latitudes (>45°N) and over Europe. The Central-North Atlantic (<45°N) and North Africa are not significant sources of ozone. The high spring and lower summer ozone events in the Aguere Valley agree with other North Atlantic ozone observation in the oceanic boundary layer. However, this behaviour contrasts with the high ozone events frequently recorded at Izaña BAPMoN station (located in the free troposphere in Tenerife) during the summer, which have been attributed in the literature to downward transport from upper levels. An intensification of the inversion layer that separates the oceanic boundary layer of the free troposphere during the summer in Canary Islands is interpreted as the cause of this different behaviour between ozone in the Aguere Valley and Izaña BAPMoN station.     

Dynamic-chemical coupling of the upper troposphere and lower stratosphere region

The importance of the interaction between chemistry and dynamics in the upper troposphere and lower stratosphere for chemical species like ozone is investigated using two chemistry-climate models and a Lagrangian trajectory model. Air parcels from the upper troposphere, i.e. regions of lightning and aircraft emissions, are able to be transported into the lowermost stratosphere (LMS). Trajectory calculations suggest that the main transport pathway runs via the inter tropical convergence zone, across the tropical tropopause and then to higher latitudes, i.e. into the LMS. NOx from aircraft emissions at mid-latitudes are unlikely to perturb the LMS since they are washed-out while still in the troposphere. In contrast, NOx from tropical lightning has the chance to accumulate in the LMS. Because of the longer residence times of NOx in the LMS, compared to the upper troposphere, this excess NOx from lightning has the potential to form ozone in the LMS, which then is transported back to the troposphere at mid-latitudes. In the models, around 10% of the ozone concentration and 50% of the NOx concentration in the northern hemisphere LMS is produced by lightning NOx At least 5% of the ozone concentration and 35% the NOx concentration at 150 hPa at mid-latitudes originates from tropical lightning in the climate-chemistry simulations.     

What is causing high ozone at Summit,Greenland?

Causes for the unusually high and seasonally anomalous ozone concentrations at Summit, Greenland were investigated. Surface data from continuous monitoring, ozone sonde data, tethered balloon vertical profiling data, correlation of ozone with the radionuclide tracers ⁷Be and ²¹⁰Pb, and synoptic transport analysis were used to identify processes that contribute to sources and sinks of ozone at Summit. Northern Hemisphere (NH) lower free troposphere ozone mixing ratios in the polar regions are ∼20 ppbv higher than in Antarctica. Ozone at Summit, which is at 3212 m above sea level, reflects its altitude location in the lower free troposphere. Transport events that bring high ozone and dry air, likely from lower stratospheric/higher tropospheric origin, were observed ∼40% of time during June 2000. Comparison of ozone enhancements with radionuclide tracer records shows a year-round correlation of ozone with the stratospheric tracer ⁷Be. Summit lacks the episodic, sunrise ozone depletion events, which were found to reduce the annual, median ozone at NH coastal sites by up to ∼3 ppbv. Synoptic trajectory analyses indicated that, under selected conditions, Summit encounters polluted continental air with increased ozone from central and western Europe. Low ozone surface deposition fluxes over long distances upwind of Summit reduce ozone deposition losses in comparison to other NH sites, particularly during the summer months. Surface-layer photochemical ozone production does not appear to have a noticeable influence on Summit's ozone levels.     

Impact of vertical transport processes on the tropospheric ozone layering above Europe.: Part II: Climatological analysis of the past 30 years

Using the set of multivariate criteria described in a companion paper, ozone-rich layers detected in tropospheric soundings are clustered according to their stratospheric or boundary layer origin. An additional class for aged tropospheric air masses is also considered. This analysis is exclusively based on the measured physical properties of the layers. The database includes 27,000 ozone profiles collected above 11 European stations—two of which provide measurements since 1970. The seasonal cycle of the tropospheric ozone stratification exhibits a clear summer maximum. This increase is due to aged tropospheric air masses that are more frequently detected, suggesting an enhanced lifetime of layers in summer. In terms of ozone content, the relative impact of stratospheric ozone compared to the other sources is highest in winter while export from the boundary layer presents a uniform seasonal cycle. Altitude and thickness distributions of the layers are consistent with the dynamical processes involved in the layering. Northernmost and southernmost stations are more exposed to stratospheric air intrusions into the free troposphere. Long-term trends show that transport from the tropopause region has increased since the mid 1980s. This trend being concomitant with lower ozone content of such layers, a moderate trend of the transport efficiency from the stratosphere on total tropospheric ozone is observed. The increase of ozone detected in tropospheric layers since the mid 1980s cannot be attributed to any recent export process from either the stratosphere or the boundary layer but rather to enhanced photochemical production in aged air masses or to an increase in the lifetime of the layers.