D. V. Spracklen

Large contribution of natural aerosols to uncertainty in indirect forcing.

The effect of anthropogenic aerosols on cloud droplet concentrations and radiative properties is the source of one of the largest uncertainties in the radiative forcing of climate over the industrial period. This uncertainty affects our ability to estimate how sensitive the climate is to greenhouse gas emissions. Here we perform a sensitivity analysis on a global model to quantify the uncertainty in cloud radiative forcing over the industrial period caused by uncertainties in aerosol emissions and processes. Our results show that 45 per cent of the variance of aerosol forcing since about 1750 arises from uncertainties in natural emissions of volcanic sulphur dioxide, marine dimethylsulphide, biogenic volatile organic carbon, biomass burning and sea spray. Only 34 per cent of the variance is associated with anthropogenic emissions. The results point to the importance of understanding pristine pre-industrial-like environments, with natural aerosols only, and suggest that improved measurements and evaluation of simulated aerosols in polluted present-day conditions will not necessarily result in commensurate reductions in the uncertainty of forcing estimates.

Evidence for the role of organics in aerosol particle formation under atmospheric conditions

New particle formation in the atmosphere is an important parameter in governing the radiative forcing of atmospheric aerosols. However, detailed nucleation mechanisms remain ambiguous, as laboratory data have so far not been successful in explaining atmospheric nucleation. We investigated the formation of new particles in a smog chamber simulating the photochemical formation of H2SO4 and organic condensable species. Nucleation occurs at H2SO4 concentrations similar to those found in the ambient atmosphere during nucleation events. The measured particle formation rates are proportional to the product of the concentrations of H2SO4 and an organic molecule. This suggests that only one H2SO4 molecule and one organic molecule are involved in the rate-limiting step of the observed nucleation process. Parameterizing this process in a global aerosol model results in substantially better agreement with ambient observations compared to control runs.

Observations of increased tropical rainfall preceded by air passage over forests

Vegetation affects precipitation patterns by mediating moisture, energy and trace-gas fluxes between the surface and atmosphere. When forests are replaced by pasture or crops, evapotranspiration of moisture from soil and vegetation is often diminished, leading to reduced atmospheric humidity and potentially suppressing precipitation. Climate models predict that large-scale tropical deforestation causes reduced regional precipitation, although the magnitude of the effect is model and resolution dependent. In contrast, observational studies have linked deforestation to increased precipitation locally but have been unable to explore the impact of large-scale deforestation. Here we use satellite remote-sensing data of tropical precipitation and vegetation, combined with simulated atmospheric transport patterns, to assess the pan-tropical effect of forests on tropical rainfall. We find that for more than 60 per cent of the tropical land surface (latitudes 30 degrees south to 30 degrees north), air that has passed over extensive vegetation in the preceding few days produces at least twice as much rain as air that has passed over little vegetation. We demonstrate that this empirical correlation is consistent with evapotranspiration maintaining atmospheric moisture in air that passes over extensive vegetation. We combine these empirical relationships with current trends of Amazonian deforestation to estimate reductions of 12 and 21 per cent in wet-season and dry-season precipitation respectively across the Amazon basin by 2050, due to less-efficient moisture recycling. Our observation-based results complement similar estimates from climate models, in which the physical mechanisms and feedbacks at work could be explored in more detail.

Impacts of climate change from 2000 to 2050 on wildfire activity and carbonaceous aerosol concentrations in the western United States

[1] We investigate the impact of climate change on wildfire activity and carbonaceous aerosol concentrations in the western United States. We regress observed area burned onto observed meteorological fields and fire indices from the Canadian Fire Weather Index system and find that May–October mean temperature and fuel moisture explain 24–57% of the variance in annual area burned in this region. Applying meteorological fields calculated by a general circulation model (GCM) to our regression model, we show that increases in temperature cause annual mean area burned in the western United States to increase by 54% by the 2050s relative to the present day. Changes in area burned are ecosystem dependent, with the forests of the Pacific Northwest and Rocky Mountains experiencing the greatest increases of 78 and 175%, respectively. Increased area burned results in near doubling of wildfire carbonaceous aerosol emissions by midcentury. Using a chemical transport model driven by meteorology from the same GCM, we calculate that climate change will increase summertime organic carbon (OC) aerosol concentrations over the western United States by 40% and elemental carbon (EC) concentrations by 20% from 2000 to 2050. Most of this increase (75% for OC and 95% for EC) is caused by larger wildfire emissions with the rest caused by changes in meteorology and for OC by increased monoterpene emissions in a warmer climate. Such an increase in carbonaceous aerosol would have important consequences for western U.S. air quality and visibility.

Oxidation products of biogenic emissions contribute to nucleation of atmospheric particles.

Out of the Air New-particle formation from gaseous precursors in the atmosphere is a complex and poorly understood process with importance in atmospheric chemistry and climate. Laboratory studies have had trouble reproducing the particle formation rates that must occur in the natural world. Riccobono et al. (p. 717) used the CLOUD (Cosmics Leaving Outdoor Droplets) chamber at CERN to recreate a realistic atmospheric environment. Sulfuric acid and oxidized organic vapors in typical natural concentrations caused particle nucleation at similar rates to those observed in the lower atmosphere. Experiments in the CLOUD chamber at CERN reproduce particle nucleation rates observed in the lower atmosphere. Atmospheric new-particle formation affects climate and is one of the least understood atmospheric aerosol processes. The complexity and variability of the atmosphere has hindered elucidation of the fundamental mechanism of new-particle formation from gaseous precursors. We show, in experiments performed with the CLOUD (Cosmics Leaving Outdoor Droplets) chamber at CERN, that sulfuric acid and oxidized organic vapors at atmospheric concentrations reproduce particle nucleation rates observed in the lower atmosphere. The experiments reveal a nucleation mechanism involving the formation of clusters containing sulfuric acid and oxidized organic molecules from the very first step. Inclusion of this mechanism in a global aerosol model yields a photochemically and biologically driven seasonal cycle of particle concentrations in the continental boundary layer, in good agreement with observations.

Sources and properties of Amazonian aerosol particles

This review provides a comprehensive account of what is known presently about Amazonian aerosol particles and concludes by formulating outlook and priorities for further research. The review is organized to follow the life cycle of Amazonian aerosol particles. It begins with a discussion of the primary and secondary sources relevant to the Amazonian particle burden, followed by a presentation of the particle properties that characterize the mixed populations present over the Amazon Basin at different times and places. These properties include number and mass concentrations and distributions, chemical composition, hygroscopicity, and cloud nucleation ability. The review presents Amazonian aerosol particles in the context of natural compared to anthropogenic sources as well as variability with season and meteorology. This review is intended to facilitate an understanding of the current state of knowledge on Amazonian aerosol particles specifically and tropical continental aerosol particles in general and thereby to enhance future research in this area. Copyright

Boreal forests, aerosols and the impacts on clouds and climate

Previous studies have concluded that boreal forests warm the climate because the cooling from storage of carbon in vegetation and soils is cancelled out by the warming due to the absorption of the Suns heat by the dark forest canopy. However, these studies ignored the impacts of forests on atmospheric aerosol. We use a global atmospheric model to show that, through emission of organic vapours and the resulting condensational growth of newly formed particles, boreal forests double regional cloud condensation nuclei concentrations (from approx. 100 to approx. 200 cm−3). Using a simple radiative model, we estimate that the resulting change in cloud albedo causes a radiative forcing of between −1.8 and −6.7 W m−2 of forest. This forcing may be sufficiently large to result in boreal forests having an overall cooling impact on climate. We propose that the combination of climate forcings related to boreal forests may result in an important global homeostasis. In cold climatic conditions, the snow–vegetation albedo effect dominates and boreal forests warm the climate, whereas in warmer climates they may emit sufficiently large amounts of organic vapour modifying cloud albedo and acting to cool climate.

The magnitude and causes of uncertainty in global model simulations of cloud condensation nuclei

Abstract. Aerosol–cloud interaction effects are a major source of uncertainty in climate models so it is important to quantify the sources of uncertainty and thereby direct research efforts. However, the computational expense of global aerosol models has prevented a full statistical analysis of their outputs. Here we perform a variance-based analysis of a global 3-D aerosol microphysics model to quantify the magnitude and leading causes of parametric uncertainty in model-estimated present-day concentrations of cloud condensation nuclei (CCN). Twenty-eight model parameters covering essentially all important aerosol processes, emissions and representation of aerosol size distributions were defined based on expert elicitation. An uncertainty analysis was then performed based on a Monte Carlo-type sampling of an emulator built for each model grid cell. The standard deviation around the mean CCN varies globally between about ±30% over some marine regions to ±40–100% over most land areas and high latitudes, implying that aerosol processes and emissions are likely to be a significant source of uncertainty in model simulations of aerosol–cloud effects on climate. Among the most important contributors to CCN uncertainty are the sizes of emitted primary particles, including carbonaceous combustion particles from wildfires, biomass burning and fossil fuel use, as well as sulfate particles formed on sub-grid scales. Emissions of carbonaceous combustion particles affect CCN uncertainty more than sulfur emissions. Aerosol emission-related parameters dominate the uncertainty close to sources, while uncertainty in aerosol microphysical processes becomes increasingly important in remote regions, being dominated by deposition and aerosol sulfate formation during cloud-processing. The results lead to several recommendations for research that would result in improved modelling of cloud–active aerosol on a global scale.

Evidence for marine production of monoterpenes

Environmental context. Laboratory incubation experiments and shipboard measurements in the Southern Atlantic Ocean have provided the first evidence for marine production of monoterpenes. Nine marine phytoplankton monocultures were investigated using a GC-MS equipped with an enantiomerically-selective column and found to emit monoterpenes including (–)-/(+)-pinene, limonene and p-ocimene, all of which were previously thought to be exclusively of terrestrial origin. Maximum levels of 100–200 pptv total monoterpenes were encountered when the ship crossed an active phytoplankton bloom. Abstract. Laboratory incubation experiments and shipboard measurements on the Southern Atlantic Ocean have provided the first evidence for marine production of monoterpenes. Nine marine phytoplankton monocultures were investigated using a GC-MS equipped with an enantiomerically-selective column and found to emit at rates, expressed as nmol C10H16 (monoterpene) g [chlorophyll a]–1 day–1, from 0.3 nmol g [chlorophyll a]–1 day–1 for Skeletonema costatum and Emiliania huxleyi to 225.9 nmol g [chlorophyll a]–1 day–1 for Dunaliella tertiolecta. Nine monoterpenes were identified in the sample and not in the control, namely: (–)-/(+)-pinene, myrcene, (+)-camphene, (–)-sabinene, (+)-3-carene, (–)-pinene, (–)-limonene and p-ocimene. In addition, shipboard measurements of monoterpenes in air were made in January–March 2007, over the South Atlantic Ocean. Monoterpenes were detected in marine air sufficiently far from land as to exclude influence from terrestrial sources. Maximum levels of 100–200 pptv total monoterpenes were encountered when the ship crossed an active phytoplankton bloom, whereas in low chlorophyll regions monoterpenes were mostly below detection limit.

Lessons from community-based payment for ecosystem service schemes: from forests to rangelands

Climate finance investments and international policy are driving new community-based projects incorporating payments for ecosystem services (PES) to simultaneously store carbon and generate livelihood benefits. Most community-based PES (CB-PES) research focuses on forest areas. Rangelands, which store globally significant quantities of carbon and support many of the worlds poor, have seen little CB-PES research attention, despite benefitting from several decades of community-based natural resource management (CBNRM) projects. Lessons from CBNRM suggest institutional considerations are vital in underpinning the design and implementation of successful community projects. This study uses documentary analysis to explore the institutional characteristics of three African community-based forest projects that seek to deliver carbon-storage and poverty-reduction benefits. Strong existing local institutions, clear land tenure, community control over land management decision-making and up-front, flexible payment schemes are found to be vital. Additionally, we undertake a global review of rangeland CBNRM literature and identify that alongside the lessons learned from forest projects, rangeland CB-PES project design requires specific consideration of project boundaries, benefit distribution, capacity building for community monitoring of carbon storage together with awareness-raising using decision-support tools to display the benefits of carbon-friendly land management. We highlight that institutional analyses must be undertaken alongside improved scientific studies of the carbon cycle to enable links to payment schemes, and for them to contribute to poverty alleviation in rangelands.