Climate sensitivity of radiative impacts from transport systems

Comparing individual components of a total climate impact is traditionally done in terms of radiative forcing. However, the climate impact of transport systems includes contributions that are likely to imply climate sensitivity parameters distinctly different from the “reference value” for a homogeneous CO2 perturbation. We propose to introduce efficacy factors for each component into the assessment. The way of proceeding is illustrated using aviation as an example, and prospects for evaluating the other transport system in the EU project QUANTIFY are given

A study on the sensitivities of simulated aerosol optical properties to composition and size distribution using airborne measurements

We present a flexible framework to calculate the optical properties of atmospheric aerosols at a given relative humidity based on their composition and size distribution. The similarity of this framework to climate model parameterisations allows rapid and extensive sensitivity tests of the impact of uncertainties in data or of new measurements on climate relevant aerosol properties. The data collected by the FAAM BAe-146 aircraft during the EUCAARI-LONGREX and VOCALS-REx campaigns have been used in a closure study to analyse the agreement between calculated and measured aerosol optical properties for two very different aerosol types. The agreement achieved for the EUCAARI-LONGREX flights is within the measurement uncertainties for both scattering and absorption. However, there is poor agreement between the calculated and the measured scattering for the VOCALS-REx flights. The high concentration of sulphate, which is a scattering aerosol with no absorption in the visible spectrum, made the absorption measurements during VOCALS-REx unreliable, and thus no closure study was possible for the absorption. The calculated hygroscopic scattering growth factor overestimates the measured values during EUCAARI-LONGREX and VOCALS-REx by ∼30% and ∼20%, respectively. We have also tested the sensitivity of the calculated aerosol optical properties to the uncertainties in the refractive indices, the hygroscopic growth factors and the aerosol size distribution. The largest source of uncertainty in the calculated scattering is the aerosol size distribution (∼35%), followed by the assumed hygroscopic growth factor for organic aerosol (∼15%), while the predominant source of uncertainty in the calculated absorption is the refractive index of organic aerosol (28–60%), although we would expect the refractive index of black carbon to be important for aerosol with a higher black carbon fraction

Changes in stratospheric composition, chemistry, radiation and climate caused by volcanic eruptions.

The primary effect of a volcanic eruption is to alter the composition of the stratosphere by the direct injection of ash and gases. On average, there is a stratospherically significant volcanic eruption about every 5.5 years. The principal effect of such an eruption is the enhancement of stratospheric sulphuric acid aerosol through the oxidation and condensation of the oxidation product H2SO4. Following the formation of the enhanced aerosol layer, observations have shown a reduction in the amount of direct radiation reaching the ground and a concomitant increase in diffuse radiation. This is associated with an increase in stratospheric temperature and a decrease in global mean surface temperature (although the spatial pattern of temperature changes is complex). In addition, the enhanced aerosol layer increases heterogeneous processing, and this reduces the levels of active nitrogen in the lower stratosphere. This in turn gives rise to either a decrease or an increase in stratospheric ozone levels, depending on the level of chlorine loading

Atmospheric impact of the 1783-1784 Laki Eruption: Part II - Climatic effect of sulphate aerosol

The long 1783-1784 eruption of Laki in southern Iceland, was one of the first eruptions to have been linked to an observed climate anomaly, having been held responsible for cold temperatures over much of the Northern Hemisphere in the period 1783-1785. Results from the first climate model simulation of the impact of a similar eruption to that of 1783-1784 are presented. Using sulphate aerosol fields produced in a companion chemical transport model simulation by Stevenson et al. (2003), the radiative forcing and climate response due to the aerosol are calculated here using the Reading Intermediate General Circulation Model (IGCM). The peak Northern Hemisphere mean direct radiative forcing is -5.5 Wm-2 in August 1783. The radiative forcing dies away quickly as the emissions from the volcano decrease; however, a small forcing remains over the Mediterranean until March 1784. There is little forcing in the Southern Hemisphere. There is shown to be an uncertainty of at least 50% in the direct radiative forcing due to assumptions concerning relative humidity and the sophistication of the radiative transfer code used. The indirect effects of the Laki aerosol are potentially large but essentially unquantifiable at the present time. In the IGCM at least, the aerosol from the eruption produces a climate response that is spatially very variable. The Northern Hemisphere mean temperature anomaly averaged over the whole of the calendar year containing most of the eruption is -0.21 K, statistically significant at the 95% level and in reasonable agreement with the available observations of the temperature during 1783

Radiative forcing and global warming potentials of 11 halogenated compounds

Radiative forcing values have been calculated for 11 halogenated compounds which are in current use or which have been suggested as possible replacements for the chlorofluorocarbons. Absorption cross-sections measured over a range of atmospheric temperature and pressure conditions as part of a multi-laboratory programme have been used together with a narrow band radiative transfer model. We provide a “best estimate” radiative forcing taking into account the likely vertical profile of the gas in each case. The Global Warming Potential over a variety of time horizons has also been calculated where the lifetime is available. We present the first such information for 1,2-dichloroethane. For chloroform our radiative forcing is 5 times higher than the value used in previous assessments, possibly because these ignored the effect of absorption outside the 800–1200 cm−1 “window”. For several of the other compounds considered here, our forcing is between 10 and 30% lower than previous assessments. The perfluorocarbons have been found to have large global warming potentials, many times that of CFC-11, due to both strong absorption and long lifetimes. The importance of absorption features at wavenumbers below 800 cm−1 and the effect of temperature variations in absorption cross-section on the radiative forcing are also investigated

Quantification of chemical and physical processes influencing ozone during long-range transport using a trajectory ensemble

During long-range transport, many distinct processes – including photochemistry, deposition, emissions and mixing – contribute to the transformation of air mass composition. Partitioning the effects of different processes can be useful when considering the sensitivity of chemical transformation to, for example, a changing environment or anthropogenic influence. However, transformation is not observed directly, since mixing ratios are measured, and models must be used to relate changes to processes. Here, four cases from the ITCT-Lagrangian 2004 experiment are studied. In each case, aircraft intercepted a distinct air mass several times during transport over the North Atlantic, providing a unique dataset and quantifying the net changes in composition from all processes. A new framework is presented to deconstruct the change in O3 mixing ratio (Δ O3) into its component processes, which were not measured directly, taking into account the uncertainty in measurements, initial air mass variability and its time evolution. The results show that the net chemical processing (Δ O3chem) over the whole simulation is greater than net physical processing (Δ O3phys) in all cases. This is in part explained by cancellation effects associated with mixing. In contrast, each case is in a regime of either net photochemical destruction (lower tropospheric transport) or production (an upper tropospheric biomass burning case). However, physical processes influence O3 indirectly through addition or removal of precursor gases, so that changes to physical parameters in a model can have a larger effect on Δ O3chem than Δ O3phys. Despite its smaller magnitude, the physical processing distinguishes the lower tropospheric export cases, since the net photochemical O3 change is −5 ppbv per day in all three cases. Processing is quantified using a Lagrangian photochemical model with a novel method for simulating mixing through an ensemble of trajectories and a background profile that evolves with them. The model is able to simulate the magnitude and variability of the observations (of O3, CO, NOy and some hydrocarbons) and is consistent with the time-average OH following air-masses inferred from hydrocarbon measurements alone (by Arnold et al., 2007). Therefore, it is a useful new method to simulate air mass evolution and variability, and its sensitivity to process parameters

Indications of Distinctive Efficacies of Transport Related Ozone Perturbations

Two series of equilibrium climate change simulations forced by ozone change patterns from transport emissions have been performed with two climate models. It is investigated whether radiative forcings like this lead to climate sensitivity and efficacy parameters that are significantly different among each other and from a reference forcing caused by a homogeneous CO2 increase. Identification of such differences is complicated by an unexpectedly strong dependence of the climate sensitivity on the strength of certain forcing patterns. Efficacy parameters calculated for the radiative forcings due to ozone increases resulting from aviation, shipping, and land transport emissions vary from unity by no more than 10%. Our results confirm earlier studies that hinted at the necessity to weight radiative forcings from different mechanisms individually in assessment studies, according to their efficacy, but more work is necessary before reliable efficacy parameters can be attributed to such forcings

Stratospheric heating by potential geoengineering aerosols

A fixed dynamical heating model is used to investigate the pattern of zonal-mean stratospheric temperature change resulting from geoengineering with aerosols composed of sulfate, titania, limestone and soot. Aerosol always heats the tropical lower stratosphere, but at the poles the response can be either heating, cooling, or neutral. The sign of the change in stratospheric Pole-Equator temperature difference depends on aerosol type, size and season. This has implications for modelling geoengineering impacts and the response of the stratospheric circulation

Atmospheric impact of the 1783-1784 Laki eruption: Part I Chemistry modelling.

Results from the first chemistry-transport model study of the impact of the 1783–1784 Laki fissure eruption (Iceland: 64°N, 17°W) upon atmospheric composition are presented. The eruption released an estimated 61 Tg(S) as SO₂ into the troposphere and lower stratosphere. The model has a high resolution tropopause region, and detailed sulphur chemistry. The simulated SO₂ plume spreads over much of the Northern Hemisphere, polewards of ~40°N. About 70% of the SO₂ gas is directly deposited to the surface before it can be oxidised to sulphuric acid aerosol. The main SO₂ oxidants, OH and H₂O₂, are depleted by up to 40% zonally, and the lifetime of SO₂ consequently increases. Zonally averaged tropospheric SO₂ concentrations over the first three months of the eruption exceed 20 ppbv, and sulphuric acid aerosol reaches ~2 ppbv. These compare to modelled pre-industrial/present-day values of 0.1/0.5 ppbv SO₂ and 0.1/1.0 ppbv sulphate. A total sulphuric acid aerosol yield of 17–22 Tg(S) is produced. The mean aerosol lifetime is 6–10 days, and the peak aerosol loading of the atmosphere is 1.4–1.7 Tg(S) (equivalent to 5.9–7.1 Tg of hydrated sulphuric acid aerosol). These compare to modelled pre-industrial/present-day sulphate burdens of 0.28/0.81 Tg(S), and lifetimes of 6/5 days, respectively. Due to the relatively short atmospheric residence times of both SO₂ and sulphate, the aerosol loading approximately mirrors the temporal evolution of emissions associated with the eruption. The model produces a reason-able simulation of the acid deposition found in Greenland ice cores. These results appear to be relatively insensitive to the vertical profile of emissions assumed, although if more of the emissions reached higher levels (>12 km), this would give longer lifetimes and larger aerosol yields. Introducing the emissions in episodes generates similar results to using monthly mean emissions, because the atmospheric lifetimes are similar to the repose periods between episodes. Most previous estimates of the global aerosol loading associated with Laki did not use atmospheric models; this study suggests that these earlier estimates have been generally too large in magnitude, and too long-lived. Environmental effects following the Laki eruption may have been dominated by the widespread deposition of SO₂ gas rather than sulphuric acid aerosol