Long-lived Greenhouse Gases Research Articles

Black carbon cookstove emissions: A field assessment of 19 stove/fuel combinations

Black carbon (BC) emissions from household cookstoves consuming solid fuel produce approximately 25 percent of total anthropogenic BC emissions. The short atmospheric lifetime of BC means that reducing BC emissions would result in a faster climate response than mitigating CO2 and other long-lived greenhouse gases. This study presents the results of optical BC measurements of two new cookstove emissions field assessments and 17 archived cookstove datasets. BC was determined from attenuation of 880 nm light, which is strongly absorbed by BC, and linearly related between 1 and 125 attenuation units. A relationship was experimentally determined correlating BC mass deposition on quartz filters determined via thermal optical analysis (TOA) and on PTFE and quartz filters using transmissometry, yielding an attenuation cross-section (σATN) for both filter media types. σATN relates TOA measurements to optical measurements on PTFE and quartz (σATN(PTFE) = 13.7 cm−2 μg, R2 = 0.87, σATN(Quartz) = 15.6 cm−2 μg, R2 = 0.87). These filter-specific σATN, optical measurements of archived filters were used to determine BC emission factors and the fraction of particulate matter (PM) in the form of black carbon (BC/PM). The 19 stoves measured fell into five stove classes; simple wood, rocket, advanced biomass, simple charcoal, and advanced charcoal. Advanced biomass stoves include forced- and natural-draft gasifiers which use wood or biomass pellets as fuel. Of these classes, the simple wood and rocket stoves demonstrated the highest median BC emission factors, ranging from 0.051 to 0.14 g MJ−1. The lowest BC emission factors were seen in charcoal stoves, which corresponds to the generally low PM emission factors observed during charcoal combustion, ranging from 0.0084 to 0.014 g MJ−1. The advanced biomass stoves generally showed an improvement in BC emissions factors compared to simple wood and rocket stoves, ranging from 0.0031 to 0.071 g MJ−1. BC/PM ratios were highest for the advanced and rocket stoves. Potential relative climate impacts were estimated by converting aerosol emissions to CO2-equivalent, and suggest that some advanced stove/fuel combinations could provide substantial climate benefits.

Diagnostic methods for atmospheric inversions of long-lived greenhouse gases

Abstract. The ability to predict the trajectory of climate change requires a clear understanding of the emissions and uptake (i.e., surface fluxes) of long-lived greenhouse gases (GHGs). Furthermore, the development of climate policies is driving a need to constrain the budgets of anthropogenic GHG emissions. Inverse problems that couple atmospheric observations of GHG concentrations with an atmospheric chemistry and transport model have increasingly been used to gain insights into surface fluxes. Given the inherent technical challenges associated with their solution, it is imperative that objective approaches exist for the evaluation of such inverse problems. Because direct observation of fluxes at compatible spatiotemporal scales is rarely possible, diagnostics tools must rely on indirect measures. Here we review diagnostics that have been implemented in recent studies and discuss their use in informing adjustments to model setup. We group the diagnostics along a continuum starting with those that are most closely related to the scientific question being targeted, and ending with those most closely tied to the statistical and computational setup of the inversion. We thus begin with diagnostics based on assessments against independent information (e.g., unused atmospheric observations, large-scale scientific constraints), followed by statistical diagnostics of inversion results, diagnostics based on sensitivity tests, and analyses of robustness (e.g., tests focusing on the chemistry and transport model, the atmospheric observations, or the statistical and computational framework), and close with the use of synthetic data experiments (i.e., observing system simulation experiments, OSSEs). We find that existing diagnostics provide a crucial toolbox for evaluating and improving flux estimates but, not surprisingly, cannot overcome the fundamental challenges associated with limited atmospheric observations or the lack of direct flux measurements at compatible scales. As atmospheric inversions are increasingly expected to contribute to national reporting of GHG emissions, the need for developing and implementing robust and transparent evaluation approaches will only grow.

Sensitivity of the carbon footprint of New Zealand milk to greenhouse gas metrics

Milk production is responsible for emitting a range of greenhouse gases (GHGs), mainly carbon dioxide (CO2), nitrous oxide (N2O) and methane (CH4). In Life Cycle Assessments (LCA), the Global Warming Potential with a time horizon of 100 years (GWP100) is used almost universally to aggregate emissions of individual gases into so-called CO2-equivalent emissions that are used to calculate the overall carbon footprint of milk production. However, there is growing awareness that, depending on the purpose of the LCA, metrics other than GWP100 could be justified and some would give a very different weighting for the short-lived gas CH4 relative to the long-lived gases CO2 and N2O when calculating the carbon footprint. Pastoral dairy production systems at different levels of intensification differ in the balance of short- and long-lived GHGs associated with on- and off-farm emissions. Differences in the carbon footprint of different production systems could therefore be highly sensitive to the choice of GHG metric. Here we explore the extent to which alternative GHG metric choices would alter the carbon footprint of New Zealand milk production at different levels of intensification at national, regional and individual farm scales and compared to the carbon footprint of milk of selected European countries. We find that the ranking of different production systems and individual farms in terms of their carbon footprint is relatively robust against the choice of GHG metric, despite significant differences in their utilisation of pastures versus supplementary off-farm feed, fertiliser use and energy consumption at various stages of farm operations. However, there are instances where alternative GHG metric choices would fundamentally change the conclusions of LCA of different production systems, including whether a move towards higher or lower input systems would increase or decrease the average carbon footprint of milk production in New Zealand. Greater transparency about the implications of alternative GHG metrics for LCA, and the often inadvertent and implicit value judgements embedded in these metrics, would help ensure that policy decisions and consumer choices based on LCA indeed deliver the climate outcomes intended by end-users.

Transient climate and ambient health impacts due to national solid fuel cookstove emissions.

Residential solid fuel use contributes to degraded indoor and ambient air quality and may affect global surface temperature. However, the potential for national-scale cookstove intervention programs to mitigate the latter issues is not yet well known, owing to the spatial heterogeneity of aerosol emissions and impacts, along with coemitted species. Here we use a combination of atmospheric modeling, remote sensing, and adjoint sensitivity analysis to individually evaluate consequences of a 20-y linear phase-out of cookstove emissions in each country with greater than 5% of the population using solid fuel for cooking. Emissions reductions in China, India, and Ethiopia contribute to the largest global surface temperature change in 2050 [combined impact of -37 mK (11 mK to -85 mK)], whereas interventions in countries less commonly targeted for cookstove mitigation such as Azerbaijan, Ukraine, and Kazakhstan have the largest per cookstove climate benefits. Abatement in China, India, and Bangladesh contributes to the largest reduction of premature deaths from ambient air pollution, preventing 198,000 (102,000-204,000) of the 260,000 (137,000-268,000) global annual avoided deaths in 2050, whereas again emissions in Ukraine and Azerbaijan have the largest per cookstove impacts, along with Romania. Global cookstove emissions abatement results in an average surface temperature cooling of -77 mK (20 mK to -278 mK) in 2050, which increases to -118 mK (-11 mK to -335 mK) by 2100 due to delayed CO2 response. Health impacts owing to changes in ambient particulate matter with an aerodynamic diameter of 2.5 μm or less (PM2.5) amount to ∼22.5 million premature deaths prevented between 2000 and 2100.

Improving the inter-hemispheric gradient of total column atmospheric CO<sub>2</sub> and CH<sub>4</sub> in simulations with the ECMWF semi-Lagrangian atmospheric global model

Abstract. It is a widely established fact that standard semi-Lagrangian advection schemes are highly efficient numerical techniques for simulating the transport of atmospheric tracers. However, as they are not formally mass conserving, it is essential to use some method for restoring mass conservation in long time range forecasts. A common approach is to use global mass fixers. This is the case of the semi-Lagrangian advection scheme in the Integrated Forecasting System (IFS) model used by the Copernicus Atmosphere Monitoring Service (CAMS) at the European Centre for Medium-Range Weather Forecasts (ECMWF).Mass fixers are algorithms with substantial differences in complexity and sophistication but in general of low computational cost. This paper shows the positive impact mass fixers have on the inter-hemispheric gradient of total atmospheric column-averaged CO2 and CH4, a crucial feature of their spatial distribution. Two algorithms are compared: the simple "proportional" and the more complex Bermejo–Conde schemes. The former is widely used by several Earth system climate models as well the CAMS global forecasts and analysis of atmospheric composition, while the latter has been recently implemented in IFS. Comparisons against total column observations demonstrate that the proportional mass fixer is shown to be suitable for the low-resolution simulations, but for the high-resolution simulations the Bermejo–Conde scheme clearly gives better results. These results have potential repercussions for climate Earth system models using proportional mass fixers as their resolution increases. It also emphasises the importance of benchmarking the tracer mass fixers with the inter-hemispheric gradient of long-lived greenhouse gases using observations.

Impact of Stratospheric Volcanic Aerosols on Age-of-Air and Transport of Long-Lived Species

The radiative perturbation associated to stratospheric aerosols from major explosive volcanic eruptions may induce significant changes in stratospheric dynamics. The aerosol heating rates warm up the lower stratosphere and cause a westerly wind anomaly, with additional tropical upwelling. Large scale transport of stratospheric trace species may be perturbed as a consequence of this intensified Brewer–Dobson circulation. The radiatively forced changes of the stratospheric circulation during the first two years after the eruption of Mt. Pinatubo (June 1991) may help explain the observed trend decline of long-lived greenhouse gases at surface stations (approximately −8 and −0.4 ppbv/year for CH4 and N2O, respectively). This decline is partly driven by the increased mid- to high-latitude downward flux at the tropopause and also by an increased isolation of the tropical pipe in the vertical layer near the tropopause, with reduced horizontal eddy mixing. Results from a climate-chemistry coupled model are shown for both long-lived trace species and the stratospheric age-of-air. The latter results to be younger by approximately 0.5 year at 30 hPa for 3–4 years after the June 1991 Pinatubo eruption, as a result of the volcanic aerosols radiative perturbation and is consistent with independent estimates based on long time series of in situ profile measurements of SF6 and CO2. Younger age of air is also calculated after Agung, El Chichón and Ruiz eruptions, as well as negative anomalies of the N2O growth rate at the extratropical tropopause layer. This type of analysis is made comparing the results of two ensembles of model simulations (1960–2005), one including stratospheric volcanic aerosols and their radiative interactions and a reference case where the volcanic aerosols do not interact with solar and planetary radiation.

Atmospheric abundance and global emissions of perfluorocarbons CF<sub>4</sub>, C<sub>2</sub>F<sub>6</sub> and C<sub>3</sub>F<sub>8</sub> since 1800 inferred from ice core, firn, air archive and in situ measurements

Abstract. Perfluorocarbons (PFCs) are very potent and long-lived greenhouse gases in the atmosphere, released predominantly during aluminium production and semiconductor manufacture. They have been targeted for emission controls under the United Nations Framework Convention on Climate Change. Here we present the first continuous records of the atmospheric abundance of CF4 (PFC-14), C2F6 (PFC-116) and C3F8 (PFC-218) from 1800 to 2014. The records are derived from high-precision measurements of PFCs in air extracted from polar firn or ice at six sites (DE08, DE08-2, DSSW20K, EDML, NEEM and South Pole) and air archive tanks and atmospheric air sampled from both hemispheres. We take account of the age characteristics of the firn and ice core air samples and demonstrate excellent consistency between the ice core, firn and atmospheric measurements. We present an inversion for global emissions from 1900 to 2014. We also formulate the inversion to directly infer emission factors for PFC emissions due to aluminium production prior to the 1980s. We show that 19th century atmospheric levels, before significant anthropogenic influence, were stable at 34.1 ± 0.3 ppt for CF4 and below detection limits of 0.002 and 0.01 ppt for C2F6 and C3F8, respectively. We find a significant peak in CF4 and C2F6 emissions around 1940, most likely due to the high demand for aluminium during World War II, for example for construction of aircraft, but these emissions were nevertheless much lower than in recent years. The PFC emission factors for aluminium production in the early 20th century were significantly higher than today but have decreased since then due to improvements and better control of the smelting process. Mitigation efforts have led to decreases in emissions from peaks in 1980 (CF4) or early-to-mid-2000s (C2F6 and C3F8) despite the continued increase in global aluminium production; however, these decreases in emissions appear to have recently halted. We see a temporary reduction of around 15 % in CF4 emissions in 2009, presumably associated with the impact of the global financial crisis on aluminium and semiconductor production.

A progressively wetter climate in southern East Africa over the past 1.3 million years.

African climate is generally considered to have evolved towards progressively drier conditions over the past few million years, with increased variability as glacial-interglacial change intensified worldwide. Palaeoclimate records derived mainly from northern Africa exhibit a 100,000-year (eccentricity) cycle overprinted on a pronounced 20,000-year (precession) beat, driven by orbital forcing of summer insolation, global ice volume and long-lived atmospheric greenhouse gases. Here we present a 1.3-million-year-long climate history from the Lake Malawi basin (10°-14° S in eastern Africa), which displays strong 100,000-year (eccentricity) cycles of temperature and rainfall following the Mid-Pleistocene Transition around 900,000 years ago. Interglacial periods were relatively warm and moist, while ice ages were cool and dry. The Malawi record shows limited evidence for precessional variability, which we attribute to the opposing effects of austral summer insolation and the temporal/spatial pattern of sea surface temperature in the Indian Ocean. The temperature history of the Malawi basin, at least for the past 500,000 years, strongly resembles past changes in atmospheric carbon dioxide and terrigenous dust flux in the tropical Pacific Ocean, but not in global ice volume. Climate in this sector of eastern Africa (unlike northern Africa) evolved from a predominantly arid environment with high-frequency variability to generally wetter conditions with more prolonged wet and dry intervals.

The climate impact of Norwegians’ travel behavior

Transportation is the largest sector in Norway in terms of greenhouse gas emissions. The mitigation potential of this sector can be better understood by investigating the climate impact of disaggregated data on travel behavior. Here, we use travel behavior data for Norwegians travelling domestically and abroad in 2009 to explore mitigation potential in Norwegian transportation. The climate impact of this aggregated data is calculated by including the impact of all relevant long-lived greenhouse gases and short-lived climate forcers. The climate responses have been compared by using a range of emission metrics (both global temperature change and integrated radiative forcing, both pulse and sustained emissions for time horizons up to 100years). For most choices, the total climate impact is dominated about equally by air (55±20%) and car transport (36±19%), with air transport having a slightly stronger impact for a majority of the cases. The highest income quintile causes a climate impact that is 240% larger than the lowest income quintile. The few trips longer than 100km contribute to 68% of the impact. In addition, we analyze what the effect would be from several proposed mitigation policy targets in Norway and find that policies focused on technology have larger impacts than those on travel behavior.

Kinetic isotope effects of <sup>12</sup>CH<sub>3</sub>D + OH and <sup>13</sup>CH<sub>3</sub>D + OH from 278 to 313 K

Abstract. Methane is the second most important long-lived greenhouse gas and plays a central role in the chemistry of the Earth's atmosphere. Nonetheless there are significant uncertainties in its source budget. Analysis of the isotopic composition of atmospheric methane, including the doubly substituted species 13CH3D, offers new insight into the methane budget as the sources and sinks have distinct isotopic signatures. The most important sink of atmospheric methane is oxidation by OH in the troposphere, which accounts for around 84 % of all methane removal. Here we present experimentally derived methane + OH kinetic isotope effects and their temperature dependence over the range of 278 to 313 K for CH3D and 13CH3D; the latter is reported here for the first time. We find kCH4/kCH3D = 1.31 ± 0.01 and kCH4/k13CH3D = 1.34 ± 0.03 at room temperature, implying that the methane + OH kinetic isotope effect is multiplicative such that (kCH4/k13CH4)(kCH4/kCH3D) = kCH4/k13CH3D, within the experimental uncertainty, given the literature value of kCH4/k13CH4 = 1.0039 ± 0.0002. In addition, the kinetic isotope effects were characterized using transition state theory with tunneling corrections. Good agreement between the experimental, quantum chemical, and available literature values was obtained. Based on the results we conclude that the OH reaction (the main sink of methane) at steady state can produce an atmospheric clumped isotope signal (Δ(13CH3D) = ln([CH4][13CH3D]/[13CH4][CH3D])) of 0.02 ± 0.02. This implies that the bulk tropospheric Δ(13CH3D) reflects the source signal with relatively small adjustment due to the sink signal (i.e., mainly OH oxidation).

Fire management business in Australia's tropical savannas: Lighting the way for a new ecosystem services model for the north?

Fire management business in Australia's tropical savannas: Lighting the way for a new ecosystem services model for the north?

Radiative forcing and climate response to projected 21st century aerosol decreases

Abstract. It is widely expected that global emissions of atmospheric aerosols and their precursors will decrease strongly throughout the remainder of the 21st century, due to emission reduction policies enacted to protect human health. For instance, global emissions of aerosols and their precursors are projected to decrease by as much as 80 % by the year 2100, according to the four Representative Concentration Pathway (RCP) scenarios. The removal of aerosols will cause unintended climate consequences, including an unmasking of global warming from long-lived greenhouse gases. We use the Geophysical Fluid Dynamics Laboratory Coupled Climate Model version 3 (GFDL CM3) to simulate future climate over the 21st century with and without the aerosol emission changes projected by each of the RCPs in order to isolate the radiative forcing and climate response resulting from the aerosol reductions. We find that the projected global radiative forcing and climate response due to aerosol decreases do not vary significantly across the four RCPs by 2100, although there is some mid-century variation, especially in cloud droplet effective radius, that closely follows the RCP emissions and energy consumption projections. Up to 1 W m−2 of radiative forcing may be unmasked globally from 2005 to 2100 due to reductions in aerosol and precursor emissions, leading to average global temperature increases up to 1 K and global precipitation rate increases up to 0.09 mm day−1. However, when using a version of CM3 with reduced present-day aerosol radiative forcing (−1.0 W m−2), the global temperature increase for RCP8.5 is about 0.5 K, with similar magnitude decreases in other climate response parameters as well. Regionally and locally, climate impacts can be much larger than the global mean, with a 2.1 K warming projected over China, Japan, and Korea due to the reduced aerosol emissions in RCP8.5, as well as nearly a 0.2 mm day−1 precipitation increase, a 7 g m−2 LWP decrease, and a 2 μm increase in cloud droplet effective radius. Future aerosol decreases could be responsible for 30–40 % of total climate warming (or 10–20 % with weaker aerosol forcing) by 2100 in East Asia, even under the high greenhouse gas emissions scenario (RCP8.5). The expected unmasking of global warming caused by aerosol reductions will require more aggressive greenhouse gas mitigation policies than anticipated in order to meet desired climate targets.

Three years of semicontinuous greenhouse gas measurements at the Puy de Dôme station (central France)

Abstract. Three years of greenhouse gas measurements, obtained using a gas chromatograph (GC) system located at the Puy de Dôme station at 1465 m a.s.l. in central France, are presented. The GC system was installed in 2010 at Puy de Dôme and was designed for automatic and accurate semicontinuous measurements of atmospheric carbon dioxide, methane, nitrous oxide and sulfur hexafluoride mole fractions. We present in detail the instrumental setup and the calibration strategy, which together allow the GC to reach repeatabilities of 0.1 μmol mol−1, 1.2 nmol mol−1, 0.3 nmol mol−1 and 0.06 pmol mol−1 for CO2, CH4, N2O and SF6, respectively. The analysis of the 3-year atmospheric time series revealed how the planetary boundary layer height drives the mole fractions observed at a mountain site such as Puy de Dôme where air masses alternate between the planetary boundary layer and the free troposphere. Accurate long-lived greenhouse gas measurements collocated with 222Rn measurements as an atmospheric tracer allowed us to determine the CO2, CH4 and N2O emissions in the catchment area of the station. The derived CO2 surface flux revealed a clear seasonal cycle, with net uptake by plant assimilation in the spring and net emission caused by the biosphere and burning of fossil fuel during the remainder of the year. We calculated a mean annual CO2 flux of 1310 ± 680 t CO2 km−2. The derived CH4 and N2O emissions in the station catchment area were 7.0 ± 4.0 t CH4 km−2 yr−1 and 1.8 ± 1.0 t N2O km−2 yr−1, respectively. Our derived annual CH4 flux is in agreement with the national French inventory, whereas our derived N2O flux is 5 times larger than the same inventory.

Environmental implications of perfluorotributylamine—a potent greenhouse gas

Perfluorotributylamine (PFTBA), a newly discovered greenhouse gas with the highest radiative efficiency, may have been released into the environment from a variety of industrial and medical uses in small amounts, leading to the potential contribution to the global warming addressed in the United Nations Framework Convention on Climate Change Kyoto Protocol. The aims of this article are to review the physicochemical properties and commercial/potential uses of PFTBA reported in the current available literature and also discuss its environmental implications based on its molecular structure. Results showed that PFTBA had extremely low solubility in water and relatively high vaporization from the water bodies, suggesting that this long-lived greenhouse gas will sink into the atmosphere. This paper also addressed the possible loss pathways through reactions with highly reactive ions in the upper atmosphere and toxic decomposition products (e.g., hydrogen fluoride, fluorine, and carbonyl fluoride) emitted when heated at high temperature. In this regard, there is a need for PFTBA emission reduction strategies due to its increasing usage in many professional applications and its potential contribution to anthropogenic climate forcing in the near future.

Embracing uncertainty in climate change policy

This Perspective explores whether policymakers can learn from adaptive management techniques to make climate policies 'anti-fragile', embracing and benefitting from scientific uncertainty, rather than simply being robust to it. The 'pledge and review' approach to reducing greenhouse-gas emissions presents an opportunity to link mitigation goals explicitly to the evolving climate response. This seems desirable because the progression from the Intergovernmental Panel on Climate Change's fourth to fifth assessment reports has seen little reduction in uncertainty. A common reaction to persistent uncertainties is to advocate mitigation policies that are robust even under worst-case scenarios, thereby focusing attention on upper extremes of both the climate response and the costs of impacts and mitigation, all of which are highly contestable. Here we ask whether those contributing to the formation of climate policies can learn from 'adaptive management' techniques. Recognizing that long-lived greenhouse gas emissions have to be net zero by the time temperatures reach a target stabilization level, such as 2 °C above pre-industrial levels, and anchoring commitments to an agreed index of attributable anthropogenic warming would provide a transparent approach to meeting such a temperature goal without prior consensus on the climate response.

Carbon dioxide, methane and nitrous oxide fluxes from podzols of a fire chronosequence in the boreal forests in Värriö, Finnish Lapland

In boreal forests, wild fire is an important factor influencing the greenhouse gas (GHG) fluxes and emission rates. As the frequency and severity of forest fires are predicted to increase with a changing climate, the knowledge on the influence of GHG fluxes from fires and burned areas on the atmospheric warming will be of high importance. We studied the effect of forest fire and the time since the last fire on fluxes of three important long-lived GHGs from soil: carbon dioxide (CO2), methane (CH4) and nitrous oxide (N2O) in northern boreal subarctic Scots pine forest stands with 5 to 155years since the last forest fire. There was a seasonal pattern in all measured GHG fluxes: emissions of CO2 and N2O, and uptake of CH4 were increasing towards the end of the growing season throughout all fire chronosequence classes. Emission of CO2 was lowest in June, in area where the fire was 5years ago (0.061mg CO2 s−1m−2) and highest in August in the area which burnt 155years ago (0.120mg CO2 s−1m−2). We also found that the soil was a CH4 sink throughout the post-fire chronosequence in all stand ages. The uptake of methane was compensating the increase in radiative forcing resulting from the carbon dioxide emissions at the recently burned sites, but the compensating effect was very small. The influence and duration of the impact of forest fire were strongest on the carbon dioxide fluxes, but on the methane and nitrous oxide fluxes the effects were less evident.

Assessment of N2O Emission Factor of Autumn Chinese Cabbage Fields at Three Different Geographical Location in South Korea

The level of nitrous oxide (N₂O), a long-lived greenhouse gas, in atmosphere has increased mainly due to anthropogenic sources, especially application of nitrogen fertilizers. Quantifying N₂O emission in the agricultural field is essential to develop national inventories of greenhouse gases (GHGs) emission. The objective of this study was to develop an emission factor to estimate the direct N₂O emission from an agricultural field cultivated with the Chinese cabbage during autumn season in 2010-2012. Emission factor of N₂O calculated over three years experiment using accumulated N₂O emission, nitrogen fertilization rate, and background N₂O emission was 0.0058±0.00254 kg N₂O-N kg -1 N. More extensive studies need to be conducted to develop N₂O emission factors for other upland crops in the various regions of Korea because N₂O emission is influenced by many factors including climate characteristics, soil properties, and agricultural practices as well as crop species.

Air mass distribution and the heterogeneity of the climate change signal in the Hudson Bay/Foxe Basin region, Canada

The linkage between changes in air mass distribution and temperature trends from 1971 to 2010 is explored in the Hudson Bay/Foxe Basin region. Statistically significant temperature increases were found of varying spatial and temporal magnitude. Concurrent statistically significant changes in air mass frequency at the same locations were also detected, particularly in the declining frequency of dry polar (DP) air. These two sets of changes were found to be linked, and we thus conclude that the heterogeneity of the climatic warming signal in the region is at least partially the result of a fundamental shift in the concurrent air mass frequency in addition to global and regional changes in radiative forcing due to increases in long-lived greenhouse gases.

Nitrous oxide fluxes in estuarine environments: response to global change.

Nitrous oxide is a powerful, long-lived greenhouse gas, but we know little about the role of estuarine areas in the global N2 O budget. This review summarizes 56 studies of N2 O fluxes and associated biogeochemical controlling factors in estuarine open waters, salt marshes, mangroves, and intertidal sediments. The majority of in situ N2 O production occurs as a result of sediment denitrification, although the water column contributes N2 O through nitrification in suspended particles. The most important factors controlling N2 O fluxes seem to be dissolved inorganic nitrogen (DIN) and oxygen availability, which in turn are affected by tidal cycles, groundwater inputs, and macrophyte density. The heterogeneity of coastal environments leads to a high variability in observations, but on average estuarine open water, intertidal and vegetated environments are sites of a small positive N2 O flux to the atmosphere (range 0.15-0.91; median 0.31; Tg N2 O-N yr(-1) ). Global changes in macrophyte distribution and anthropogenic nitrogen loading are expected to increase N2 O emissions from estuaries. We estimate that a doubling of current median NO3 (-) concentrations would increase the global estuary water-air N2 O flux by about 0.45 Tg N2 O-N yr(-1) or about 190%. A loss of 50% of mangrove habitat, being converted to unvegetated intertidal area, would result in a net decrease in N2 O emissions of 0.002 Tg N2 O-N yr(-1) . In contrast, conversion of 50% of salt marsh to unvegetated area would result in a net increase of 0.001 Tg N2 O-N yr(-1) . Decreased oxygen concentrations may inhibit production of N2 O by nitrification; however, sediment denitrification and the associated ratio of N2 O:N2 is expected to increase.

Local sources of global climate forcing from different categories of land use activities

Abstract. Identifying and quantifying the sources of climate impacts from land use and land cover change (LULCC) is necessary to optimize policies regarding LULCC for climate change mitigation. These climate impacts are typically defined relative to emissions of CO2, or sometimes emissions of other long-lived greenhouse gases. Here we use previously published estimates of the radiative forcing (RF) of LULCC that include the short-lived forcing agents O3 and aerosols, in addition to long-lived greenhouse gases and land albedo change, for six projections of LULCC as a metric for quantifying climate impacts. The LULCC RF is attributed to three categories of LULCC activities: direct modifications to land cover, agriculture, and wildfire response, and sources of the forcing are ascribed to individual grid points for each sector. Results for the year 2010 show substantial positive forcings from the direct modifications and agriculture sectors, particularly from south and southeast Asia, and a smaller magnitude negative forcing response from wildfires. The spatial distribution of future sources of LULCC RF is highly scenario-dependent, but we show that future forest area change can be used as a predictor of the future RF from direct modification activities, especially in the tropics, suggesting that deforestation-prevention policies that value land based on its C-content may be particularly effective at mitigating climate forcing originating in the tropics from this sector. However, the response of wildfire RF to tropical land cover changes is not as easily scalable and yet imposes a non-trivial feedback onto the total LULCC RF.