Ralf Toumi

An influence of solar spectral variations on radiative forcing of climate

The thermal structure and composition of the atmosphere is determined fundamentally by the incoming solar irradiance. Radiation at ultraviolet wavelengths dissociates atmospheric molecules, initiating chains of chemical reactions—specifically those producing stratospheric ozone—and providing the major source of heating for the middle atmosphere, while radiation at visible and near-infrared wavelengths mainly reaches and warms the lower atmosphere and the Earth’s surface. Thus the spectral composition of solar radiation is crucial in determining atmospheric structure, as well as surface temperature, and it follows that the response of the atmosphere to variations in solar irradiance depends on the spectrum. Daily measurements of the solar spectrum between 0.2 µm and 2.4 µm, made by the Spectral Irradiance Monitor (SIM) instrument on the Solar Radiation and Climate Experiment (SORCE) satellite since April 2004, have revealed that over this declining phase of the solar cycle there was a four to six times larger decline in ultraviolet than would have been predicted on the basis of our previous understanding. This reduction was partially compensated in the total solar output by an increase in radiation at visible wavelengths. Here we show that these spectral changes appear to have led to a significant decline from 2004 to 2007 in stratospheric ozone below an altitude of 45 km, with an increase above this altitude. Our results, simulated with a radiative-photochemical model, are consistent with contemporaneous measurements of ozone from the Aura-MLS satellite, although the short time period makes precise attribution to solar effects difficult. We also show, using the SIM data, that solar radiative forcing of surface climate is out of phase with solar activity. Currently there is insufficient observational evidence to validate the spectral variations observed by SIM, or to fully characterize other solar cycles, but our findings raise the possibility that the effects of solar variability on temperature throughout the atmosphere may be contrary to current expectations.

Carbon aerosols and atmospheric photochemistry

Carbon aerosols are produced by all combustion processes. This paper investigates some possible effects of heterogeneous reduction of atmospheric constituents on carbon aerosols. Reduction of HNO 3 , NO 2 , and O 3 on carbon aerosols may be an important effect of increased air traffic that has not been considered to date. It is shown that if HNO 3 , NO 2 and O 3 are heterogeneously reduced on atmospheric amorphous carbon aerosols, then a significant, lower stratospheric ozone loss mechanism could exist. This ozone loss mechanism is almost independent of temperature and does not require the presence of sunlight. The mechanism can operate at all latitudes where amorphous carbon aerosols are present. The relative importance of the mechanism increases with nightlength. The reduction of HNO 3 on carbon aerosols could also be a significant renoxification process wherever carbon aerosols are present. Owing to the very different soot levels in the two hemispheres, this implies that there should be a hemispheric assymetry in the role of these mechanisms. The renoxification leads to simulated tropospheric HNO 3 /NO x ratios that are close to those observed. In contrast to the stratospheric response, the tropospheric production of NO x due to the reduction of HNO 3 would lead to tropospheric ozone production.

Ice nucleation on soot particles

Abstract The ice-forming activity of soot particles of various sizes has been studied in a cloud chamber under temperatures ranging from −5 to −20°C. It was found that the fraction of aerosol particles forming ice crystals was influenced by the temperature, the mean radius of aerosol particles and the degree of oxidising of the soot particle surface. It was suggested that oxidising affected the concentration of surface chemical groups that could form hydrogen bonds with water molecules. A decrease in the temperature and an increase in the radius of particles led to an increase in the number of ice crystals. Data obtained were parameterised and an expression was derived that enables the concentration of ice crystals to be calculated for conditions in a low cloud. Based on these experiments, this particular soot is a very potent source of ice nuclei. Data obtained were compared with Fletcher theory. It was shown that the theory contradicts experimental data and cannot be recommended for evaluation of the number of ice crystals in clouds. An application of the data obtained to aircraft condensation trail formation is discussed.

Heterogeneous atmospheric bromine chemistry

This paper considers the effect of heterogeneous bromine reactions on stratospheric photochemistry. We have considered reactions on both sulfate aerosols and on polar stratospheric clouds (PSCs). It is shown that the hydrolysis of BrONO2 on sulfate aerosols enhances the HOBr concentration, which in turn enhances the OH and HO2 concentrations, thereby reducing the HCl lifetime and concentration. The hydrolysis of BrONO2 leads to a nighttime production of HOBr, making HOBr a major nighttime bromine reservoir. The photolysis of HOBr gives a rapid increase in the OH and HO2 concentration at dawn, as was recently observed by Salawitch et al. [1994]. The increase in the OH and HO2 concentration, and the decrease in the HCl concentration, leads to additional ozone depletion at all latitudes and for all season. At temperatures below 210 K the bulk phase reaction of HOBr with HCl in sulfate aerosols becomes important. The most important heterogeneous bromine reactions on polar stratospheric clouds are the mixed halogen reactions of HCl with HOBr and BrONO2 and of HBr with HOCl and ClONO2.

Trends in stratospheric humidity and the sensitivity of ozone to these trends

Measurements of stratospheric water vapor and methane from the Halogen Occultation Experiment (HALOE) mounted on the Upper Atmosphere Research Satellite (UARS) are used to investigate changes in stratospheric water vapor over the period 1992–1996 inclusive. An increase in water vapor mixing ratio is found at levels between 30 km and 65 km across the globe which fit, to first order, a linear trend varying with altitude from 40 parts per billion by volume per year (ppbv yr−1) to a maximum of 90 ppbv yr−1 at 45 km. These trends appear to be greater than that expected due to the growth in tropospheric methane over the past several decades, and possible mechanisms accounting for this are discussed. The trend of the combined budget of 2 × CH4 + H2O is approximately constant with altitude with a global mean value of 61±4 ppbv yr−1. On the basis of these estimates, sensitivity studies have been performed using a two-dimensional (2-D) radiative-chemical-dynamical model to assess the impact on concentrations of stratospheric ozone of this degree of change in stratospheric water vapor over timescales consistent with doubling CO2 scenarios. We find that the impact of increased stratospheric water vapor is to enhance the ozone increase in the midstratosphere by ∼1–2% compared to the response due to a doubling of CO2 itself of ∼5–10%. In the upper stratosphere the destruction of ozone is enhanced and the changeover from production to loss is lowered to ∼50 km (from ∼70 km). A chemical mechanism for these processes involving enhanced OH and NO2 is identified.

REDUCING THE CLIMATE CHANGE IMPACTS OF AVIATION BY RESTRICTING CRUISE ALTITUDES

Two of the ways in which air travel affects climate are the emission of carbon dioxide and the creation of high-altitude contrails. One possible impact reduction strategy is to significantly reduce the formation of contrails. This could be achieved by limiting the cruise altitude of aircraft. If implemented, this could severely constrain air space capacity, especially in parts of Europe. In addition, carbon emissions would likely be higher due to less efficient aircraft operation at lower cruise altitudes. This paper describes an analysis of these trade-offs using an air space simulation model as applied to European airspace. The model simulates the flight paths and altitudes of each aircraft and is here used to calculate emissions of carbon dioxide and changes in the journey time. For a one-day Western European traffic sample, calculations suggest annual mean CO2 emissions would increase by only 4% if cruise altitudes were restricted to prevent contrail formation. The change in journey time depended on aircraft type and route, but average changes were less than 1 min. Our analysis demonstrates that altitude restrictions on commercial aircraft could be an effective means of reducing climate change impacts, though it will be necessary to mitigate the increased controller workload conflicts that this will generate.

The role of microphysical and chemical processes in prolonging the climate forcing of the Toba Eruption

The mega-eruption of Toba, Sumatra, occurred around 73 Ka ago, during the onset of a glaciation of the Late Quaternary. This coincidence combined with the unprecedented amount of sulphur released by this volcano has led to the hypothesis that Toba sulphate aerosols caused a transient surface cooling which may have contributed to a shift of the climate system. Because of the self limiting effect of gravitational sedimentation, the climatic impact of extremely large sulphur injections into the stratosphere are thought to be rather limited. Here we present model calculations combining microphysical and chemical feedbacks which show that the eruption could instead have led to the formation of a long-lasting volcanic aerosol layer. Although the concentrations of radiatively active species such as O3 or SO2 could also have been considerably perturbed, the resulting forcings should have only slightly moderated the aerosol cooling effect during the first few years following the eruption. According to our results, extremely high stratospheric sulphur loading could lead to a more prolonged effect on the climate than previously assumed.

Some doubts concerning a link between cosmic ray fluxes and global cloudiness

Svensmark and Friis-Christensen (1997, henceforth SFC) showed a strong correlation between cosmic ray flux and ISCCP total cloudiness between 1984 and 1990. They concluded that ionisation by cosmic rays, more prevalent at times of lower solar activity, might explain apparent correlations between solar activity and climate through changes in cloud radiative forcing. We have extended SFCs approach with a study of the different cloud types, restricting our analysis to the period 1985 to 1988 during which the ISCCP calibration is believed to be stable. We find no clear relationship between individual cloud types and cosmic ray flux. Inclusion of data at high latitudes decreases the amplitude of the apparent correlation although ionisation by cosmic rays is greatest at high latitudes. Thin high cloud shows an increase throughout the period such that the combined effect of the changes in cloud types suggests an almost monotonic increase in cloud radiative forcing between 1985 and 1988 which is not related to cosmic ray activity.

BrO as a sink for dimethylsulphide in the marine atmosphere

Dimethylsulphide (DMS) is the major biogenic sulphur source gas. It is known to be oxidised by OH and NO3 to ultimately yield sulphate particles which are important in acid deposition and are also involved in the atmospheric radiative balance. In the laboratory BrO has also been shown to oxidise DMS. Here I present atmospheric model calculations based on inorganic Bromine measurements and find that oxidation by BrO is a sink for DMS.

The relationship between leaf area index and microclimate in tropical forest and oil palm plantation: Forest disturbance drives changes in microclimate

Highlights • Microclimate was monitored in primary forest, logged forest and oil palm plantation.• There were strong relationships between leaf area index and diurnal climate.• Logged forest is up to 2.5 °C warmer on average than primary forest.• Oil palm plantations are up to 6.5 °C warmer on average than primary forest.• Forest disturbance led to desiccation of the air near the forest floor.