The indirect global warming potential and global temperature change potential due to methane oxidation

Methane is the second most important anthropogenic greenhouse gas in the atmosphere next to carbon dioxide. Its global warming potential (GWP) for a time horizon of 100 years is 25, which makes it an attractive target for climate mitigation policies. Although the methane GWP traditionally includes the methane indirect effects on the concentrations of ozone and stratospheric water vapour, it does not take into account the production of carbon dioxide from methane oxidation. We argue here that this CO2-induced effect should be included for fossil sources of methane, which results in slightly larger GWP values for all time horizons. If the global temperature change potential is used as an alternative climate metric, then the impact of the CO2-induced effect is proportionally much larger. We also discuss what the correction term should be for methane from anthropogenic biogenic sources.

Dietary prebiotics: current status and new definition

In November 2008, a group of scientists met at the 6th Meeting of the International Scientific Association of Probiotics and Prebiotics (ISAPP) in London, Ontario, Canada, to discuss the functionality of prebiotics. As a result of this, it was concluded that the prebiotic field is currently dominated by gastrointestinal events. However, in the future, it may be the case that other mixed microbial ecosystems may be modulated by a prebiotic approach, such as the oral cavity, skin and the urogenital tract. Therefore, a decision was taken to build upon the current prebiotic status and define a niche for ‘dietary prebiotics’. This review is co-authored by the working group of ISAPP scientists and sets the background for defining a dietary prebiotic as ‘‘a selectively fermented ingredient that results in specific changes in the composition and/or activity of the gastrointestinal microbiota, thus conferring benefit(s) upon host health’’.

Infrared absorption spectra, radiative efficiencies, and global warming potentials of perfluorocarbons: Comparison between experiment and theory

Experimentally and theoretically determined infrared spectra are reported for a series of straight-chain perfluorocarbons: C2F6, C3F8, C4F10, C5F12, C6F14, and C8F18. Theoretical spectra were determined using both density functional (DFT) and ab initio methods. Radiative efficiencies (REs) were determined using the method of Pinnock et al. (1995) and combined with atmospheric lifetimes from the literature to determine global warming potentials (GWPs). Theoretically determined absorption cross sections were within 10% of experimentally determined values. Despite being much less computationally expensive, DFT calculations were generally found to perform better than ab initio methods. There is a strong wavenumber dependence of radiative forcing in the region of the fundamental C-F vibration, and small differences in wavelength between band positions determined by theory and experiment have a significant impact on the REs. We apply an empirical correction to the theoretical spectra and then test this correction on a number of branched chain and cyclic perfluoroalkanes. We then compute absorption cross sections, REs, and GWPs for an additional set of perfluoroalkenes.

The effect of dietary nitrate on salivary, plasma, and urinary nitrate metabolism in humans

Dietary nitrate is metabolized to nitrite by bacterial flora on the posterior surface of the tongue leading to increased salivary nitrite concentrations. In the acidic environment of the stomach, nitrite forms nitrous acid, a potent nitrating/nitrosating agent. The aim of this study was to examine the pharmacokinetics of dietary nitrate in relation to the formation of salivary, plasma, and urinary nitrite and nitrate in healthy subjects. A secondary aim was to determine whether dietary nitrate increases the formation of protein-bound 3-nitrotyrosine in plasma, and if dietary nitrate improves platelet function. The pharmacokinetic profile of urinary nitrate excretion indicates total clearance of consumed nitrate in a 24 h period. While urinary, salivary, and plasma nitrate concentrations increased between 4- and 7-fold, a significant increase in nitrite was only detected in saliva (7-fold). High dietary nitrate consumption does not cause a significant acute change in plasma concentrations of 3-nitrotyrosine or in platelet function.

The dependence of clear-sky outgoing longwave radiation on surface temperature and relative humidity

A simulation of the earth's clear-sky long-wave radiation budget is used to examine the dependence of clear-sky outgoing long-wave radiation (OLR) on surface temperature and relative humidity. the simulation uses the European Centre for Medium-Range Weather Forecasts global reanalysed fields to calculate clear-sky OLR over the period from January 1979 to December 1993, thus allowing the seasonal and interannual time-scales to be resolved. the clear-sky OLR is shown to be primarily dependent on temperature changes at high latitudes and on changes in relative humidity at lower latitudes. Regions exhibiting a ‘super-greenhouse’ effect are identified and are explained by considering the changes in the convective regime associated with the Hadley circulation over the seasonal cycle, and with the Walker circulation over the interannual time-scale. the sensitivity of clear-sky OLR to changes in relative humidity diminishes with increasing relative humidity. This is explained by the increasing saturation of the water-vapour absorption bands with increased moisture. By allowing the relative humidity to vary in specified vertical slabs of the troposphere over an interannual time-scale it is shown that changes in humidity in the mid troposphere (400 to 700 hPa) are of most importance in explaining clear-sky OLR variations. Relative humidity variations do not appear to affect the positive thermodynamic water-vapour feedback significantly in response to surface temperature changes.

Water vapour self-continuum and water dimers: 1. Analysis of recent work

Recent laboratory observations and advances in theoretical quantum chemistry allow a reappraisal of the fundamental mechanisms that determine the water vapour self-continuum absorption throughout the infrared and millimetre wave spectral regions. By starting from a framework that partitions bimolecular interactions between water molecules into free-pair states, true bound and quasi-bound dimers, we present a critical review of recent observations, continuum models and theoretical predictions. In the near-infrared bands of the water monomer, we propose that spectral features in recent laboratory-derived self-continuum can be well explained as being due to a combination of true bound and quasi-bound dimers, when the spectrum of quasi-bound dimers is approximated as being double the broadened spectrum of the water monomer. Such a representation can explain both the wavenumber variation and the temperature dependence. Recent observations of the self-continuum absorption in the windows between these near-infrared bands indicate that widely used continuum models can underestimate the true strength by around an order of magnitude. An existing far-wing model does not appear able to explain the discrepancy, and although a dimer explanation is possible, currently available observations do not allow a compelling case to be made. In the 8–12 micron window, recent observations indicate that the modern continuum models either do not properly represent the temperature dependence, the wavelength variation, or both. The temperature dependence is suggestive of a transition from the dominance of true bound dimers at lower temperatures to quasibound dimers at higher temperatures. In the mid- and far-infrared spectral region, recent theoretical calculations indicate that true bound dimers may explain at least between 20% and 40% of the observed self-continuum. The possibility that quasi-bound dimers could cause an additional contribution of the same size is discussed. Most recent theoretical considerations agree that water dimers are likely to be the dominant contributor to the self-continuum in the mm-wave spectral range.

Climate model calculations of the impact of aerosols from road transport and shipping

Road transport and shipping are copious sources of aerosols, which exert a 9 significant radiative forcing, compared to, for example, the CO2 emitted by these sectors. An 10 advanced atmospheric general circulation model, coupled to a mixed-layer ocean, is used to 11 calculate the climate response to the direct radiative forcing from such aerosols. The cases 12 considered include imposed distributions of black carbon and sulphate aerosols from road 13 transport, and sulphate aerosols from shipping; these are compared to the climate response 14 due to CO2 increases. The difficulties in calculating the climate response due to small 15 forcings are discussed, as the actual forcings have to be scaled by large amounts to enable a 16 climate response to be easily detected. Despite the much greater geographical inhomogeneity 17 in the sulphate forcing, the patterns of zonal and annual-mean surface temperature response 18 (although opposite in sign) closely resembles that resulting from homogeneous changes in 19 CO2. The surface temperature response to black carbon aerosols from road transport is shown 20 to be notably non-linear in scaling applied, probably due to the semi-direct response of clouds 21 to these aerosols. For the aerosol forcings considered here, the most widespread method of 22 calculating radiative forcing significantly overestimates their effect, relative to CO2, 23 compared to surface temperature changes calculated using the climate model.

Stratospheric temperature trends: our evolving understanding

We review the scientific literature since the 1960s to examine the evolution of modeling tools and observations that have advanced understanding of global stratospheric temperature changes. Observations show overall cooling of the stratosphere during the period for which they are available (since the late 1950s and late 1970s from radiosondes and satellites, respectively), interrupted by episodes of warming associated with volcanic eruptions, and superimposed on variations associated with the solar cycle. There has been little global mean temperature change since about 1995. The temporal and vertical structure of these variations are reasonably well explained bymodels that include changes in greenhouse gases, ozone, volcanic aerosols, and solar output, although there are significant uncertainties in the temperature observations and regarding the nature and influence of past changes in stratospheric water vapor. As a companion to a recent WIREs review of tropospheric temperature trends, this article identifies areas of commonality and contrast between the tropospheric and stratospheric trend literature. For example, the increased attention over time to radiosonde and satellite data quality has contributed to better characterization of uncertainty in observed trends both in the troposphere and in the lower stratosphere, and has highlighted the relative deficiency of attention to observations in the middle and upper stratosphere. In contrast to the relatively unchanging expectations of surface and tropospheric warming primarily induced by greenhouse gas increases, stratospheric temperature change expectations have arisen from experiments with a wider variety of model types, showingmore complex trend patterns associated with a greater diversity of forcing agents.

The temperature response to stratospheric water vapour changes

This study uses an analytical model, based on the cooling-to-space approximation, and a fixed dynamical heating model to investigate the structure of the stratospheric cooling that occurs in response to a uniform increase in stratospheric water vapour (SWV). At all latitudes, the largest cooling occurs in the lower stratosphere and decreases in magnitude with height. The cooling is strongly enhanced in the Extratropics compared to the Tropics. This is markedly different to the case of an increase in CO2, which causes maximum cooling near the stratopause and a small warming in the tropical lower stratosphere. The qualitative differences in the structure of the cooling can be explained by the smaller opacity of water vapour bands in the stratosphere compared to CO2. The small opacity means that the magnitude of the initial heating rate perturbation only decreases by a factor of four between the upper and lower stratosphere for a SWV perturbation. Therefore, to balance the heating rate perturbation, the largest temperature change is required in the lower stratosphere. Increasing the background concentration of SWV causes the water vapour bands to become more opaque. For a SWV perturbation applied to a background SWV concentration ≥30 ppmv, the heating rate perturbation and temperature change structurally resemble those from an increase in CO2. In the Extratropics, the lower height of the tropopause is found to cause the enhancement in the cooling at those latitudes. By controlling the depth of atmosphere which adjusts to the SWV perturbation, the tropopause height affects the net exchange of radiation between the layers in the stratosphere as they cool. The latitudinal gradient in upwelling infrared radiation at the tropopause and variations in the background temperature are found to have only a minor effect on the structure of the stratospheric temperature response to a change in SWV.

Assessment of the consistency of H2O line intensities over the near-infrared using sun-pointing ground-based Fourier transform spectroscopy

We report on the consistency of water vapour line intensities in selected spectral regions between 800–12,000 cm−1 under atmospheric conditions using sun-pointing Fourier transform infrared spectroscopy. Measurements were made across a number of days at both a low and high altitude field site, sampling a relatively moist and relatively dry atmosphere. Our data suggests that across most of the 800–12,000 cm−1 spectral region water vapour line intensities in recent spectral line databases are generally consistent with what was observed. However, we find that HITRAN-2008 water vapour line intensities are systematically lower by up to 20% in the 8000–9200 cm−1 spectral interval relative to other spectral regions. This discrepancy is essentially removed when two new linelists (UCL08, a compilation of linelists and ab-initio calculations, and one based on recent laboratory measurements by Oudot et al. (2010) [10] in the 8000–9200 cm−1 spectral region) are used. This strongly suggests that the H2O line strengths in the HITRAN-2008 database are indeed underestimated in this spectral region and in need of revision. The calculated global-mean clear-sky absorption of solar radiation is increased by about 0.3 W m−2 when using either the UCL08 or Oudot line parameters in the 8000–9200 cm−1 region, instead of HITRAN-2008. We also found that the effect of isotopic fractionation of HDO is evident in the 2500–2900 cm−1 region in the observations.

Water vapour continuum absorption in near-infrared windows derived from laboratory measurements

In most near-infrared atmospheric windows, absorption of solar radiation is dominated by the water vapor self-continuum and yet there is a paucity of measurements in these windows. We report new laboratory measurements of the self-continuum absorption at temperatures between 293 and 472 K and pressures from 0.015 to 5 atm in four near-infrared windows between 1 and 4 m (10000-2500 cm-1); the measurements are made over a wider range of wavenumber, temperatures and pressures than any previous measurements. They show that the self-continuum in these windows is typically one order of magnitude stronger than given in representations of the continuum widely used in climate and weather prediction models. These results are also not consistent with current theories attributing the self continuum within windows to the far-wings of strong spectral lines in the nearby water vapor absorption bands; we suggest that they are more consistent with water dimers being the major contributor to the continuum. The calculated global-average clear-sky atmospheric absorption of solar radiation is increased by 0.75 W/m2 (which is about 1% of the total clear-sky absorption) by using these new measurements as compared to calculations with the MT_CKD-2.5 self-continuum model.

Characterising North Atlantic weather patterns for climate-optimal aircraft routing

Daily weather patterns over the North Atlantic are classified into relevant types: typical weather patterns that may characterize the range of climate impacts from aviation in this region, for both summer and winter. The motivation is to provide a set of weather types to facilitate an investigation of climate-optimal aircraft routing of trans-Atlantic flights (minimizing the climate impact on a flight-by-flight basis). Using the New York to London route as an example, the time-optimal route times are shown to vary by over 60 min, to take advantage of strong tailwinds or avoid headwinds, and for eastbound routes latitude correlates well with the latitude of the jet stream. The weather patterns are classified by their similarity to the North Atlantic Oscillation and East Atlantic teleconnection patterns. For winter, five types are defined; in summer, when there is less variation in jet latitude, only three types are defined. The types can be characterized by the jet strength and position, and therefore the location of the time-optimal routes varies by type. Simple proxies for the climate impact of carbon dioxide, ozone, water vapour and contrails are defined, which depend on parameters such as the route time, latitude and season, the time spent flying in the stratosphere, and the distance over which the air is supersaturated with respect to ice. These proxies are then shown to vary between weather types and between eastbound and westbound routes.