The contribution of global aviation to anthropogenic climate forcing for 2000 to 2018.

Global aviation operations contribute to anthropogenic climate change via a complex set of processes that lead to a net surface warming. Of importance are aviation emissions of carbon dioxide (CO2), nitrogen oxides (NOx), water vapor, soot and sulfate aerosols, and increased cloudiness due to contrail formation. Aviation grew strongly over the past decades (1960-2018) in terms of activity, with revenue passenger kilometers increasing from 109 to 8269 billion km yr-1, and in terms of climate change impacts, with CO2 emissions increasing by a factor of 6.8 to 1034 Tg CO2 yr-1. Over the period 2013-2018, the growth rates in both terms show a marked increase. Here, we present a new comprehensive and quantitative approach for evaluating aviation climate forcing terms. Both radiative forcing (RF) and effective radiative forcing (ERF) terms and their sums are calculated for the years 2000-2018. Contrail cirrus, consisting of linear contrails and the cirrus cloudiness arising from them, yields the largest positive net (warming) ERF term followed by CO2 and NOx emissions. The formation and emission of sulfate aerosol yields a negative (cooling) term. The mean contrail cirrus ERF/RF ratio of 0.42 indicates that contrail cirrus is less effective in surface warming than other terms. For 2018 the net aviation ERF is +100.9 milliwatts (mW) m-2 (5-95% likelihood range of (55, 145)) with major contributions from contrail cirrus (57.4 mW m-2), CO2 (34.3 mW m-2), and NOx (17.5 mW m-2). Non-CO2 terms sum to yield a net positive (warming) ERF that accounts for more than half (66%) of the aviation net ERF in 2018. Using normalization to aviation fuel use, the contribution of global aviation in 2011 was calculated to be 3.5 (4.0, 3.4) % of the net anthropogenic ERF of 2290 (1130, 3330) mW m-2. Uncertainty distributions (5%, 95%) show that non-CO2 forcing terms contribute about 8 times more than CO2 to the uncertainty in the aviation net ERF in 2018. The best estimates of the ERFs from aviation aerosol-cloud interactions for soot and sulfate remain undetermined. CO2-warming-equivalent emissions based on global warming potentials (GWP* method) indicate that aviation emissions are currently warming the climate at approximately three times the rate of that associated with aviation CO2 emissions alone. CO2 and NOx aviation emissions and cloud effects remain a continued focus of anthropogenic climate change research and policy discussions.

Transport impacts on atmosphere and climate: Aviation.

Aviation alters the composition of the atmosphere globally and can thus drive climate change and ozone depletion. The last major international assessment of these impacts was made by the Intergovernmental Panel on Climate Change (IPCC) in 1999. Here, a comprehensive updated assessment of aviation is provided. Scientific advances since the 1999 assessment have reduced key uncertainties, sharpening the quantitative evaluation, yet the basic conclusions remain the same. The climate impact of aviation is driven by long-term impacts from CO2 emissions and shorter-term impacts from non-CO2 emissions and effects, which include the emissions of water vapour, particles and nitrogen oxides (NO x ). The present-day radiative forcing from aviation (2005) is estimated to be 55 mW m-2 (excluding cirrus cloud enhancement), which represents some 3.5% (range 1.3-10%, 90% likelihood range) of current anthropogenic forcing, or 78 mW m-2 including cirrus cloud enhancement, representing 4.9% of current forcing (range 2-14%, 90% likelihood range). According to two SRES-compatible scenarios, future forcings may increase by factors of 3-4 over 2000 levels, in 2050. The effects of aviation emissions of CO2 on global mean surface temperature last for many hundreds of years (in common with other sources), whilst its non-CO2 effects on temperature last for decades. Much progress has been made in the last ten years on characterizing emissions, although major uncertainties remain over the nature of particles. Emissions of NO x result in production of ozone, a climate warming gas, and the reduction of ambient methane (a cooling effect) although the overall balance is warming, based upon current understanding. These NO x emissions from current subsonic aviation do not appear to deplete stratospheric ozone. Despite the progress made on modelling aviation's impacts on tropospheric chemistry, there remains a significant spread in model results. The knowledge of aviation's impacts on cloudiness has also improved: a limited number of studies have demonstrated an increase in cirrus cloud attributable to aviation although the magnitude varies: however, these trend analyses may be impacted by satellite artefacts. The effect of aviation particles on clouds (with and without contrails) may give rise to either a positive forcing or a negative forcing: the modelling and the underlying processes are highly uncertain, although the overall effect of contrails and enhanced cloudiness is considered to be a positive forcing and could be substantial, compared with other effects. The debate over quantification of aviation impacts has also progressed towards studying potential mitigation and the technological and atmospheric tradeoffs. Current studies are still relatively immature and more work is required to determine optimal technological development paths, which is an aspect that atmospheric science has much to contribute. In terms of alternative fuels, liquid hydrogen represents a possibility and may reduce some of aviation's impacts on climate if the fuel is produced in a carbon-neutral way: such fuel is unlikely to be utilized until a 'hydrogen economy' develops. The introduction of biofuels as a means of reducing CO2 impacts represents a future possibility. However, even over and above land-use concerns and greenhouse gas budget issues, aviation fuels require strict adherence to safety standards and thus require extra processing compared with biofuels destined for other sectors, where the uptake of such fuel may be more beneficial in the first instance.

Formation of C7F15COOH (PFOA) and other perfluorocarboxylic acids during the atmospheric oxidation of 8:2 fluorotelomer alcohol.

Calculations using a three-dimensional global atmospheric chemistry model (IMPACT) indicate that n-C8F17CH2CH2OH (widely used in industrial and consumer products) degrades in the atmosphere to give perfluorooctanoic acid (PFOA) and other perfluorocarboxylic acids (PFCAs). PFOA is persistent, bioaccumulative, and potentially toxic. Molar yields of PFOA depend on location and season, are in the range of 1-10%, and are of the correct order of magnitude to explain the observed levels in Arctic fauna. Fluorotelomer alcohols such as n-C8F17CH2CH2OH appear to be a significant global source of persistent bioaccumulative perfluorocarboxylic acid pollution. This is the first modeling study of the atmospheric chemistry of a fluorotelomer alcohol.

Effects of aerosol from biomass burning on the global radiation budget.

An analysis is made of the likely contribution of smoke particles from biomass burning to the global radiation balance. These particles act to reflect solar radiation directly; they also can act as cloud condensation nuclei, increasing the reflectivity of clouds. Together these effects, although uncertain, may add up globally to a cooling effect as large as 2 watts per square meter, comparable to the estimated contribution of sulfate aerosols. Anthropogenic increases of smoke emission thus may have helped weaken the net greenhouse warming from anthropogenic trace gases.

Empirical formula for optical absorption by fractal aerosol agglomerates.

An empirical formula for calculating the optical absorption of fractal aerosol agglomerates over a broad frequency range is derived based on extensive calculations made on five smoke agglomerates having a widely varying number of particles ranging from 12 to 372 and an almost constant fractal dimension in the 1.7-1.9 range. The expansion coefficients in the empirical formula were determined by least-squares curve fiting of numerical data obtained using the volume integral equation formulation (VIEF).(1) The formula satisfies the frequency dependence of the absorption at lower frequencies and up to the resonance frequency of the agglomerate. Expressions for the resonance frequency (f(0)), as well as the constant coefficients in the empiricial formula, are derived in terms of the structural dimensions, number and size of the primary particles, and the complex permittivity of the aerosol agglomerate. Numerical results obtained from the empirical formula are generally in good agreement with those calculated by the VIEF for soot particles with a magnitude of complex permittivity |epsilon*| in the 1-7 range. The average error in the absorption calculation is <5%. The formula thus provides a simple and inexpensive method for calculating the optical absorption of aerosol agglomerates, which otherwise require complicated and expensive methods of calculation. This formula also facilitates the implementation of the accurate VIEF results in large climate codes such as the general circulation model.

Optical scattering and absorption by branched chains of aerosols.

We utilize the Volume Integral Equation Formulation (VIEF) and the method of moments to calculate the electromagnetic scattering and absorption of aerosol particles with branched-chain structures. Two kinds of polarization of the incident electromagnetic wave were considered: the cross- and end-fire polarizations. The numerical results of internal electric field distribution, absorbed power, and extinction and scattering cross sections, obtained from the VIEF, show excellent agreement with the Mie theory for the special case of spherical particles. Comparison between the results of the VIEF and Iterative Extended Boundary Condition Method for very long oriented (elongated) chains of particles also showed good agreement. After validating the accuracy of the VIEF, the absorption characteristics of three branched-chain structuressimulated from microscopic pictures of coagulated smoke aerosol particles were calculated. Results showed that the ratio of absorption in the two polarization cases, P(cross-fire)/P(end-fire), for very long oriented chain structures is as high as a factor of 4 at lower frequencies (lambda =10microm). While in the higher frequency (lambda = 0.5-microm) case, the ratio Of P(cross-fire)/P(end-fire) is reduced to 2.0. For branched-chain structures, the ratio Of P(cross-fire)/P(end-fire) decreased with the increase in the number of the side branches. These observations show that the frequency, polarization, and structure factors play important roles in determining the optical characteristics of branched chains of aerosol particles.