Extensive halogen-mediated ozone destruction over the tropical Atlantic Ocean

Increasing tropospheric ozone levels over the past 150 years have led to a significant climate perturbation; the prediction of future trends in tropospheric ozone will require a full understanding of both its precursor emissions and its destruction processes. A large proportion of tropospheric ozone loss occurs in the tropical marine boundary layer and is thought to be driven primarily by high ozone photolysis rates in the presence of high concentrations of water vapour. A further reduction in the tropospheric ozone burden through bromine and iodine emitted from open-ocean marine sources has been postulated by numerical models, but thus far has not been verified by observations. Here we report eight months of spectroscopic measurements at the Cape Verde Observatory indicative of the ubiquitous daytime presence of bromine monoxide and iodine monoxide in the tropical marine boundary layer. A year-round data set of co-located in situ surface trace gas measurements made in conjunction with low-level aircraft observations shows that the mean daily observed ozone loss is approximately 50 per cent greater than that simulated by a global chemistry model using a classical photochemistry scheme that excludes halogen chemistry. We perform box model calculations that indicate that the observed halogen concentrations induce the extra ozone loss required for the models to match observations. Our results show that halogen chemistry has a significant and extensive influence on photochemical ozone loss in the tropical Atlantic Ocean boundary layer. The omission of halogen sources and their chemistry in atmospheric models may lead to significant errors in calculations of global ozone budgets, tropospheric oxidizing capacity and methane oxidation rates, both historically and in the future.     

Reduction of soil carbon formation by tropospheric ozone under increased carbon dioxide levels

In the Northern Hemisphere, ozone levels in the troposphere have increased by 35 per cent over the past century, with detrimental impacts on forest and agricultural productivity, even when forest productivity has been stimulated by increased carbon dioxide levels. In addition to reducing productivity, increased tropospheric ozone levels could alter terrestrial carbon cycling by lowering the quantity and quality of carbon inputs to soils. However, the influence of elevated ozone levels on soil carbon formation and decomposition are unknown. Here we examine the effects of elevated ozone levels on the formation rates of total and decay-resistant acid-insoluble soil carbon under conditions of elevated carbon dioxide levels in experimental aspen (Populus tremuloides) stands and mixed aspen-birch (Betula papyrifera) stands. With ambient concentrations of ozone and carbon dioxide both raised by 50 per cent, we find that the formation rates of total and acid-insoluble soil carbon are reduced by 50 per cent relative to the amounts entering the soil when the forests were exposed to increased carbon dioxide alone. Our results suggest that, in a world with elevated atmospheric carbon dioxide concentrations, global-scale reductions in plant productivity due to elevated ozone levels will also lower soil carbon formation rates significantly.     

Northern Hemisphere forcing of climatic cycles in Antarctica over the past 360,000 years

The Milankovitch theory of climate change proposes that glacial-interglacial cycles are driven by changes in summer insolation at high northern latitudes. The timing of climate change in the Southern Hemisphere at glacial-interglacial transitions (which are known as terminations) relative to variations in summer insolation in the Northern Hemisphere is an important test of this hypothesis. So far, it has only been possible to apply this test to the most recent termination, because the dating uncertainty associated with older terminations is too large to allow phase relationships to be determined. Here we present a new chronology of Antarctic climate change over the past 360,000 years that is based on the ratio of oxygen to nitrogen molecules in air trapped in the Dome Fuji and Vostok ice cores. This ratio is a proxy for local summer insolation, and thus allows the chronology to be constructed by orbital tuning without the need to assume a lag between a climate record and an orbital parameter. The accuracy of the chronology allows us to examine the phase relationships between climate records from the ice cores and changes in insolation. Our results indicate that orbital-scale Antarctic climate change lags Northern Hemisphere insolation by a few millennia, and that the increases in Antarctic temperature and atmospheric carbon dioxide concentration during the last four terminations occurred within the rising phase of Northern Hemisphere summer insolation. These results support the Milankovitch theory that Northern Hemisphere summer insolation triggered the last four deglaciations.     

Indirect radiative forcing of climate change through ozone effects on the land-carbon sink

The evolution of the Earth's climate over the twenty-first century depends on the rate at which anthropogenic carbon dioxide emissions are removed from the atmosphere by the ocean and land carbon cycles. Coupled climate-carbon cycle models suggest that global warming will act to limit the land-carbon sink, but these first generation models neglected the impacts of changing atmospheric chemistry. Emissions associated with fossil fuel and biomass burning have acted to approximately double the global mean tropospheric ozone concentration, and further increases are expected over the twenty-first century. Tropospheric ozone is known to damage plants, reducing plant primary productivity and crop yields, yet increasing atmospheric carbon dioxide concentrations are thought to stimulate plant primary productivity. Increased carbon dioxide and ozone levels can both lead to stomatal closure, which reduces the uptake of either gas, and in turn limits the damaging effect of ozone and the carbon dioxide fertilization of photosynthesis. Here we estimate the impact of projected changes in ozone levels on the land-carbon sink, using a global land carbon cycle model modified to include the effect of ozone deposition on photosynthesis and to account for interactions between ozone and carbon dioxide through stomatal closure. For a range of sensitivity parameters based on manipulative field experiments, we find a significant suppression of the global land-carbon sink as increases in ozone concentrations affect plant productivity. In consequence, more carbon dioxide accumulates in the atmosphere. We suggest that the resulting indirect radiative forcing by ozone effects on plants could contribute more to global warming than the direct radiative forcing due to tropospheric ozone increases.     

Continuing emissions of methyl chloroform from Europe

The consumption of methyl chloroform (1,1,1-trichloroethane), an industrial solvent, has been banned by the 1987 Montreal Protocol because of its ozone-depleting potential. During the 1990s, global emissions have decreased substantially and, since 1999, near-zero emissions have been estimated for Europe and the United States. Here we present measurements of methyl chloroform that are inconsistent with the assumption of small emissions. Using a tracer transport model, we estimate that European emissions were greater than 20 Gg in 2000. Although these emissions are not significant for stratospheric ozone depletion, they have important implications for estimates of global tropospheric hydroxyl radical (OH) concentrations, deduced from measurements of methyl chloroform. Ongoing emissions therefore cast doubt upon recent reports of a strong and unexpected negative trend in OH during the 1990s and a previously calculated higher OH abundance in the Southern Hemisphere compared to the Northern Hemisphere.     

Insolation-driven changes in atmospheric circulation over the past 116,000 years in subtropical Brazil

During the last glacial period, large millennial-scale temperature oscillations--the 'Dansgaard/Oeschger' cycles--were the primary climate signal in Northern Hemisphere climate archives from the high latitudes to the tropics. But whether the influence of these abrupt climate changes extended to the tropical and subtropical Southern Hemisphere, where changes in insolation are thought to be the main direct forcing of climate, has remained unclear. Here we present a high-resolution oxygen isotope record of a U/Th-dated stalagmite from subtropical southern Brazil, covering the past 116,200 years. The oxygen isotope signature varies with shifts in the source region and amount of rainfall in the area, and hence records changes in atmospheric circulation and convective intensity over South America. We find that these variations in rainfall source and amount are primarily driven by summer solar radiation, which is controlled by the Earth's precessional cycle. The Dansgaard/Oeschger cycles can be detected in our record and therefore we confirm that they also affect the tropical hydrological cycle, but that in southern subtropical Brazil, millennial-scale climate changes are not as dominant as they are in the Northern Hemisphere.     

黑碳气溶胶研究新进展

黑碳气溶胶是气溶胶的重要组成部分,在大气物理、大气化学、大气光学、大气光化学等过程中具有重要作用。近年来研究表明,黑碳气溶胶对于全球变暖、区域气候变化有重要贡献,黑碳气溶胶可能是影响全球变暖的第二大重要因子,其作用仅次于CO2。因此,应控制黑碳的排放。考虑到黑碳气溶胶在全球变暖、区域气候、环境与健康等方面的作用,研究和评价黑碳气溶胶的作用已十分必要和迫切。     

Towards robust regional estimates of CO2 sources and sinks using atmospheric transport models

Information about regional carbon sources and sinks can be derived from variations in observed atmospheric CO2 concentrations via inverse modelling with atmospheric tracer transport models. A consensus has not yet been reached regarding the size and distribution of regional carbon fluxes obtained using this approach, partly owing to the use of several different atmospheric transport models. Here we report estimates of surface-atmosphere CO2 fluxes from an intercomparison of atmospheric CO2 inversion models (the TransCom 3 project), which includes 16 transport models and model variants. We find an uptake of CO2 in the southern extratropical ocean less than that estimated from ocean measurements, a result that is not sensitive to transport models or methodological approaches. We also find a northern land carbon sink that is distributed relatively evenly among the continents of the Northern Hemisphere, but these results show some sensitivity to transport differences among models, especially in how they respond to seasonal terrestrial exchange of CO2. Overall, carbon fluxes integrated over latitudinal zones are strongly constrained by observations in the middle to high latitudes. Further significant constraints to our understanding of regional carbon fluxes will therefore require improvements in transport models and expansion of the CO2 observation network within the tropics.     

Climate modelling: Northern Hemisphere circulation

Air pressure at sea level during winter has decreased over the Arctic and increased in the Northern Hemisphere subtropics in recent decades, a change that has been associated with 50% of the Eurasian winter warming observed over the past 30 years, with 60% of the rainfall increase in Scotland and with 60% of the rainfall decrease in Spain. This trend is inconsistent with the simulated response to greenhouse-gas and sulphate-aerosol changes, but it has been proposed that other climate influences--such as ozone depletion--could account for the discrepancy. Here I compare observed Northern Hemisphere sea-level pressure trends with those simulated in response to all the major human and natural climate influences in nine state-of-the-art coupled climate models over the past 50 years. I find that these models all underestimate the circulation trend. This inconsistency suggests that we cannot yet simulate changes in this important property of the climate system or accurately predict regional climate changes.     

Human contribution to more-intense precipitation extremes

Extremes of weather and climate can have devastating effects on human society and the environment. Understanding past changes in the characteristics of such events, including recent increases in the intensity of heavy precipitation events over a large part of the Northern Hemisphere land area, is critical for reliable projections of future changes. Given that atmospheric water-holding capacity is expected to increase roughly exponentially with temperature--and that atmospheric water content is increasing in accord with this theoretical expectation--it has been suggested that human-influenced global warming may be partly responsible for increases in heavy precipitation. Because of the limited availability of daily observations, however, most previous studies have examined only the potential detectability of changes in extreme precipitation through model-model comparisons. Here we show that human-induced increases in greenhouse gases have contributed to the observed intensification of heavy precipitation events found over approximately two-thirds of data-covered parts of Northern Hemisphere land areas. These results are based on a comparison of observed and multi-model simulated changes in extreme precipitation over the latter half of the twentieth century analysed with an optimal fingerprinting technique. Changes in extreme precipitation projected by models, and thus the impacts of future changes in extreme precipitation, may be underestimated because models seem to underestimate the observed increase in heavy precipitation with warming.     

Evidence from U-Th dating against Northern Hemisphere forcing of the penultimate deglaciation

Milankovitch proposed that summer insolation at mid-latitudes in the Northern Hemisphere directly causes the ice-age climate cycles. This would imply that times of ice-sheet collapse should correspond to peaks in Northern Hemisphere June insolation. But the penultimate deglaciation has proved controversial because June insolation peaks 127 kyr ago whereas several records of past climate suggest that change may have occurred up to 15 kyr earlier. There is a clear signature of the penultimate deglaciation in marine oxygen-isotope records. But dating this event, which is significantly before the 14C age range, has not been possible. Here we date the penultimate deglaciation in a record from the Bahamas using a new U-Th isochron technique. After the necessary corrections for alpha-recoil mobility of 234U and 230Th and a small age correction for sediment mixing, the midpoint age for the penultimate deglaciation is determined to be 135 +/- 2.5 kyr ago. This age is consistent with some coral-based sea-level estimates, but it is difficult to reconcile with June Northern Hemisphere insolation as the trigger for the ice-age cycles. Potential alternative driving mechanisms for the ice-age cycles that are consistent with such an early date for the penultimate deglaciation are either the variability of the tropical ocean-atmosphere system or changes in atmospheric CO2 concentration controlled by a process in the Southern Hemisphere.     

Changing boreal methane sources and constant biomass burning during the last termination

Past atmospheric methane concentrations show strong fluctuations in parallel to rapid glacial climate changes in the Northern Hemisphere superimposed on a glacial-interglacial doubling of methane concentrations. The processes driving the observed fluctuations remain uncertain but can be constrained using methane isotopic information from ice cores. Here we present an ice core record of carbon isotopic ratios in methane over the entire last glacial-interglacial transition. Our data show that the carbon in atmospheric methane was isotopically much heavier in cold climate periods. With the help of a box model constrained by the present data and previously published results, we are able to estimate the magnitude of past individual methane emission sources and the atmospheric lifetime of methane. We find that methane emissions due to biomass burning were about 45 Tg methane per year, and that these remained roughly constant throughout the glacial termination. The atmospheric lifetime of methane is reduced during cold climate periods. We also show that boreal wetlands are an important source of methane during warm events, but their methane emissions are essentially shut down during cold climate conditions.     

Detection of human influence on twentieth-century precipitation trends

Human influence on climate has been detected in surface air temperature, sea level pressure, free atmospheric temperature, tropopause height and ocean heat content. Human-induced changes have not, however, previously been detected in precipitation at the global scale, partly because changes in precipitation in different regions cancel each other out and thereby reduce the strength of the global average signal. Models suggest that anthropogenic forcing should have caused a small increase in global mean precipitation and a latitudinal redistribution of precipitation, increasing precipitation at high latitudes, decreasing precipitation at sub-tropical latitudes, and possibly changing the distribution of precipitation within the tropics by shifting the position of the Intertropical Convergence Zone. Here we compare observed changes in land precipitation during the twentieth century averaged over latitudinal bands with changes simulated by fourteen climate models. We show that anthropogenic forcing has had a detectable influence on observed changes in average precipitation within latitudinal bands, and that these changes cannot be explained by internal climate variability or natural forcing. We estimate that anthropogenic forcing contributed significantly to observed increases in precipitation in the Northern Hemisphere mid-latitudes, drying in the Northern Hemisphere subtropics and tropics, and moistening in the Southern Hemisphere subtropics and deep tropics. The observed changes, which are larger than estimated from model simulations, may have already had significant effects on ecosystems, agriculture and human health in regions that are sensitive to changes in precipitation, such as the Sahel.     

关于大气臭氧问题的主要研究进展

大气臭氧是非常重要的温室气体,其在全球的分布具有不均匀性,受到人类活动的显著影响,近几十年来由于对流层臭氧增加造成正的辐射强迫会增加大气温室效应,而平流臭氧减少会使其吸收的紫外线辐射减少,为负的辐射强迫,使得平流层大气降温。因此关于大气臭氧浓度变化及其对气候的影响是非常复杂的,一直是科学界研究的热点和难点问题。自从20世纪50年代末到70年代就发现臭氧浓度有减少的趋势。1985年英国南极考察队在南纬60°地区观测发现存在大气臭氧层空洞;自此开始,大气臭氧问题引起了世界各国的极大关注,并给予很多研究。目前,平流层和对流层臭氧浓度的观测仍然是研究的重点。鉴于对流层臭氧浓度持续升高和平流层臭氧浓度的不断下降,以及他们在对流层和平流层大气温度中所起的不同作用,本文将主要针对近五年来大气臭氧相关的研究进展进行简要的综述,包括对流层和平流层臭氧浓度及其观测研究,和人类活动的影响等方面进行分述。最后给出目前研究工作的不足和未来工作展望。     

Late Miocene decoupling of oceanic warmth and atmospheric carbon dioxide forcing

Deep-time palaeoclimate studies are vitally important for developing a complete understanding of climate responses to changes in the atmospheric carbon dioxide concentration (that is, the atmospheric partial pressure of CO(2), p(co(2))). Although past studies have explored these responses during portions of the Cenozoic era (the most recent 65.5 million years (Myr) of Earth history), comparatively little is known about the climate of the late Miocene (～12-5 Myr ago), an interval with p(co(2)) values of only 200-350?parts per million by volume but nearly ice-free conditions in the Northern Hemisphere and warmer-than-modern temperatures on the continents. Here we present quantitative geochemical sea surface temperature estimates from the Miocene mid-latitude North Pacific Ocean, and show that oceanic warmth persisted throughout the interval of low p(co(2)) ～12-5 Myr ago. We also present new stable isotope measurements from the western equatorial Pacific that, in conjunction with previously published data, reveal a long-term trend of thermocline shoaling in the equatorial Pacific since ～13?Myr ago. We propose that a relatively deep global thermocline, reductions in low-latitude gradients in sea surface temperature, and cloud and water vapour feedbacks may help to explain the warmth of the late Miocene. Additional shoaling of the thermocline after 5?Myr ago probably explains the stronger coupling between p(co(2)), sea surface temperatures and climate that is characteristic of the more recent Pliocene and Pleistocene epochs.     

Evidence from the Pacific troposphere for large global sources of oxygenated organic compounds

The presence of oxygenated organic compounds in the troposphere strongly influences key atmospheric processes. Such oxygenated species are, for example, carriers of reactive nitrogen and are easily photolysed, producing free radicals-and so influence the oxidizing capacity and the ozone-forming potential of the atmosphere-and may also contribute significantly to the organic component of aerosols. But knowledge of the distribution and sources of oxygenated organic compounds, especially in the Southern Hemisphere, is limited. Here we characterize the tropospheric composition of oxygenated organic species, using data from a recent airborne survey conducted over the tropical Pacific Ocean (30 degrees N to 30 degrees S). Measurements of a dozen oxygenated chemicals (carbonyls, alcohols, organic nitrates, organic pernitrates and peroxides), along with several C2-C8 hydrocarbons, reveal that abundances of oxygenated species are extremely high, and collectively, oxygenated species are nearly five times more abundant than non-methane hydrocarbons in the Southern Hemisphere. Current atmospheric models are unable to correctly simulate these findings, suggesting that large, diffuse, and hitherto-unknown sources of oxygenated organic compounds must therefore exist. Although the origin of these sources is still unclear, we suggest that oxygenated species could be formed via the oxidation of hydrocarbons in the atmosphere, the photochemical degradation of organic matter in the oceans, and direct emissions from terrestrial vegetation.     

Magnitude and timing of temperature change in the Indo-Pacific warm pool during deglaciation

Ocean-atmosphere interactions in the tropical Pacific region have a strong influence on global heat and water vapour transport and thus constitute an important component of the climate system. Changes in sea surface temperatures and convection in the tropical Indo-Pacific region are thought to be responsible for the interannual to decadal climate variability observed in extra-tropical regions, but the role of the tropics in climate changes on millennial and orbital timescales is less clear. Here we analyse oxygen isotopes and Mg/Ca ratios of foraminiferal shells from the Makassar strait in the heart of the Indo-Pacific warm pool, to obtain synchronous estimates of sea surface temperatures and ice volume. We find that sea surface temperatures increased by 3.5-4.0 degrees C during the last two glacial-interglacial transitions, synchronous with the global increase in atmospheric CO2 and Antarctic warming, but the temperature increase occurred 2,000-3,000 years before the Northern Hemisphere ice sheets melted. Our observations suggest that the tropical Pacific region plays an important role in driving glacial-interglacial cycles, possibly through a system similar to how El Ni?o/Southern Oscillation regulates the poleward flux of heat and water vapour.     

Holocene Southern Ocean surface temperature variability west of the Antarctic Peninsula

The disintegration of ice shelves, reduced sea-ice and glacier extent, and shifting ecological zones observed around Antarctica highlight the impact of recent atmospheric and oceanic warming on the cryosphere. Observations and models suggest that oceanic and atmospheric temperature variations at Antarctica's margins affect global cryosphere stability, ocean circulation, sea levels and carbon cycling. In particular, recent climate changes on the Antarctic Peninsula have been dramatic, yet the Holocene climate variability of this region is largely unknown, limiting our ability to evaluate ongoing changes within the context of historical variability and underlying forcing mechanisms. Here we show that surface ocean temperatures at the continental margin of the western Antarctic Peninsula cooled by 3-4 °C over the past 12,000 years, tracking the Holocene decline of local (65° S) spring insolation. Our results, based on TEX(86) sea surface temperature (SST) proxy evidence from a marine sediment core, indicate the importance of regional summer duration as a driver of Antarctic seasonal sea-ice fluctuations. On millennial timescales, abrupt SST fluctuations of 2-4 °C coincide with globally recognized climate variability. Similarities between our SSTs, Southern Hemisphere westerly wind reconstructions and El Ni?o/Southern Oscillation variability indicate that present climate teleconnections between the tropical Pacific Ocean and the western Antarctic Peninsula strengthened late in the Holocene epoch. We conclude that during the Holocene, Southern Ocean temperatures at the western Antarctic Peninsula margin were tied to changes in the position of the westerlies, which have a critical role in global carbon cycling.     

Increasing risk of Amazonian drought due to decreasing aerosol pollution

The Amazon rainforest plays a crucial role in the climate system, helping to drive atmospheric circulations in the tropics by absorbing energy and recycling about half of the rainfall that falls on it. This region (Amazonia) is also estimated to contain about one-tenth of the total carbon stored in land ecosystems, and to account for one-tenth of global, net primary productivity. The resilience of the forest to the combined pressures of deforestation and global warming is therefore of great concern, especially as some general circulation models (GCMs) predict a severe drying of Amazonia in the twenty-first century. Here we analyse these climate projections with reference to the 2005 drought in western Amazonia, which was associated with unusually warm North Atlantic sea surface temperatures (SSTs). We show that reduction of dry-season (July-October) rainfall in western Amazonia correlates well with an index of the north-south SST gradient across the equatorial Atlantic (the 'Atlantic N-S gradient'). Our climate model is unusual among current GCMs in that it is able to reproduce this relationship and also the observed twentieth-century multidecadal variability in the Atlantic N-S gradient, provided that the effects of aerosols are included in the model. Simulations for the twenty-first century using the same model show a strong tendency for the SST conditions associated with the 2005 drought to become much more common, owing to continuing reductions in reflective aerosol pollution in the Northern Hemisphere.     

南极臭氧洞对全球气候影响的数值试验

采用ＩＡＰ九层全球大气环流模式进行了南极臭氧洞气候效应的数值试验．试验和分析表明,南半球高纬和极地平流层臭氧含量的减少,不仅对南半球气候有明显影响,而且影响到北半球,使全球气候产生明显变化．