Low European methyl chloroform emissions inferred from long-term atmospheric measurements

Methyl chloroform (CH3CCl3, 1,1,1,-trichloroethane) was used widely as a solvent before it was recognized to be an ozone-depleting substance and its phase-out was introduced under the Montreal Protocol. Subsequently, its atmospheric concentration has declined steadily and recent European methyl chloroform consumption and emissions were estimated to be less than 0.1 gigagrams per year. However, data from a short-term tropospheric measurement campaign (EXPORT) indicated that European methyl chloroform emissions could have been over 20 gigagrams in 2000 (ref. 6), almost doubling previously estimated global emissions. Such enhanced emissions would significantly affect results from the CH3CC13 method of deriving global abundances of hydroxyl radicals (OH) (refs 7-12)-the dominant reactive atmospheric chemical for removing trace gases related to air pollution, ozone depletion and the greenhouse effect. Here we use long-term, high-frequency data from Mace Head, Ireland and Jungfraujoch, Switzerland, to infer European methyl chloroform emissions. We find that European emission estimates declined from about 60 gigagrams per year in the mid-1990s to 0.3-1.4 and 1.9-3.4 gigagrams per year in 2000-03, based on Mace Head and Jungfraujoch data, respectively. Our European methyl chloroform emission estimates are therefore higher than calculated from consumption data, but are considerably lower than those derived from the EXPORT campaign in 2000 (ref. 6).     

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.     

Vertical structure of recent Arctic warming

Near-surface warming in the Arctic has been almost twice as large as the global average over recent decades-a phenomenon that is known as the 'Arctic amplification'. The underlying causes of this temperature amplification remain uncertain. The reduction in snow and ice cover that has occurred over recent decades may have played a role. Climate model experiments indicate that when global temperature rises, Arctic snow and ice cover retreats, causing excessive polar warming. Reduction of the snow and ice cover causes albedo changes, and increased refreezing of sea ice during the cold season and decreases in sea-ice thickness both increase heat flux from the ocean to the atmosphere. Changes in oceanic and atmospheric circulation, as well as cloud cover, have also been proposed to cause Arctic temperature amplification. Here we examine the vertical structure of temperature change in the Arctic during the late twentieth century using reanalysis data. We find evidence for temperature amplification well above the surface. Snow and ice feedbacks cannot be the main cause of the warming aloft during the greater part of the year, because these feedbacks are expected to primarily affect temperatures in the lowermost part of the atmosphere, resulting in a pattern of warming that we only observe in spring. A significant proportion of the observed temperature amplification must therefore be explained by mechanisms that induce warming above the lowermost part of the atmosphere. We regress the Arctic temperature field on the atmospheric energy transport into the Arctic and find that, in the summer half-year, a significant proportion of the vertical structure of warming can be explained by changes in this variable. We conclude that changes in atmospheric heat transport may be an important cause of the recent Arctic temperature amplification.     

Atmospheric science: early peak in Antarctic oscillation index

The principal extratropical atmospheric circulation mode in the Southern Hemisphere, the Antarctic oscillation (or Southern Hemisphere annular mode), represents fluctuations in the strength of the circumpolar vortex and has shown a trend towards a positive index in austral summer in recent decades, which has been linked to stratospheric ozone depletion and to increased atmospheric greenhouse-gas concentrations. Here we reconstruct the austral summer (December-January) Antarctic oscillation index from sea-level pressure measurements over the twentieth century and find that large positive values, and positive trends of a similar magnitude to those of past decades, also occurred around 1960, and that strong negative trends occurred afterwards. This positive Antarctic oscillation index and large positive trend during a period before ozone-depleting chemicals were released into the atmosphere and before marked anthropogenic warming, together with the later negative trend, indicate that natural forcing factors or internal mechanisms in the climate system must also strongly influence the state of the Antarctic oscillation.     

Long-term decline of global atmospheric ethane concentrations and implications for methane

After methane, ethane is the most abundant hydrocarbon in the remote atmosphere. It is a precursor to tropospheric ozone and it influences the atmosphere's oxidative capacity through its reaction with the hydroxyl radical, ethane's primary atmospheric sink. Here we present the longest continuous record of global atmospheric ethane levels. We show that global ethane emission rates decreased from 14.3 to 11.3 teragrams per year, or by 21 per cent, from 1984 to 2010. We attribute this to decreasing fugitive emissions from ethane's fossil fuel source--most probably decreased venting and flaring of natural gas in oil fields--rather than a decline in its other major sources, biofuel use and biomass burning. Ethane's major emission sources are shared with methane, and recent studies have disagreed on whether reduced fossil fuel or microbial emissions have caused methane's atmospheric growth rate to slow. Our findings suggest that reduced fugitive fossil fuel emissions account for at least 10-21 teragrams per year (30-70 per cent) of the decrease in methane's global emissions, significantly contributing to methane's slowing atmospheric growth rate since the mid-1980s.     

An influence of solar spectral variations on radiative forcing of climate

The thermal structure and composition of the atmosphere is determined fundamentally by the incoming solar irradiance. Radiation at ultraviolet wavelengths dissociates atmospheric molecules, initiating chains of chemical reactions-specifically those producing stratospheric ozone-and providing the major source of heating for the middle atmosphere, while radiation at visible and near-infrared wavelengths mainly reaches and warms the lower atmosphere and the Earth's surface. Thus the spectral composition of solar radiation is crucial in determining atmospheric structure, as well as surface temperature, and it follows that the response of the atmosphere to variations in solar irradiance depends on the spectrum. Daily measurements of the solar spectrum between 0.2?μm and 2.4?μm, made by the Spectral Irradiance Monitor (SIM) instrument on the Solar Radiation and Climate Experiment (SORCE) satellite since April 2004, have revealed that over this declining phase of the solar cycle there was a four to six times larger decline in ultraviolet than would have been predicted on the basis of our previous understanding. This reduction was partially compensated in the total solar output by an increase in radiation at visible wavelengths. Here we show that these spectral changes appear to have led to a significant decline from 2004 to 2007 in stratospheric ozone below an altitude of 45?km, with an increase above this altitude. Our results, simulated with a radiative-photochemical model, are consistent with contemporaneous measurements of ozone from the Aura-MLS satellite, although the short time period makes precise attribution to solar effects difficult. We also show, using the SIM data, that solar radiative forcing of surface climate is out of phase with solar activity. Currently there is insufficient observational evidence to validate the spectral variations observed by SIM, or to fully characterize other solar cycles, but our findings raise the possibility that the effects of solar variability on temperature throughout the atmosphere may be contrary to current expectations.     

紫外辐射时空变化规律研究进展

紫外辐射(ultraviolet radiation, UVR)会对人体健康,陆生及水生有机体产生伤害作用。因此,了解紫外辐射在全球及中国的分布及变化状况十分重要。综述了UVR在全球和中国地表分布状况,及影响因素。从全球而言,赤道附近南北纬23°之间UVR最强,亚马孙热带雨林地区低于周边地区,一些高海拔地区也是UVR高值区。中国UVR分布从南向北逐渐减小,从东向西增加,青藏高原一直是高值区;从时间分布来看,北半球和中国紫外辐射强度基本一致,1—7月紫外线逐渐增强,7月达到最大值,后逐渐减弱,12月达最小值。南半球时间变化与之相反,最高值出现在1月份。且因人类活动排放的消耗臭氧层物质作用,臭氧层仍持续减少,因此到达地表UVR强度最大将增加。从影响地表UVR分布因素而言,天文因素、臭氧、云、气溶胶及大气污染物、海拔高度、地表反照率等因素均对地表UVR产生重要影响。因此,加强UVR监测与预报,以及加强UVR对陆生与水生生态系统研究对生产、生活及科学研究等领域均十分重要。     

中国冰箱行业淘汰CFCs 的环境效益分析

以无《蒙特利尔议定书》的情景为基线情景, 从消耗臭氧层物质排放、温室气体排放及冰箱耗电量角度分析中国冰箱行业履约淘汰 CFCs 产生的环境效益。结果表明,截至2008年底,中国冰箱行业淘汰 CFCs已实现减排 273.5 MtCO₂-eq 和 4.7×10⁴t ODP; 2008 年后还将减排 619.8 MtCO₂-eq 和 1.0×10⁵t ODP;通过采用更加节能的制冷剂,截至 2008 年底累计节电 2.8×10¹⁰ kWh, 折合减排 24.2MtCO₂-eq,对中国节约资源和节能减排具有十分重要的现实意义。     

大气臭氧耗损的修复

评述了修复大气臭氧耗损的化学法和物理法，某些化学法如在南极旋涡中注入烃类可能由于生成另外的活性氯原子而不能有效地抑制大气臭氧耗损，某些物理法如利用大气电子电荷修复大气臭氧耗损，这是令人感兴趣的方法，它没有其他的化合物生成，但是会遇到技术和光电子材料的难题。在此，提出了另一类修复大气臭氧耗损的新方法，观测到卤代烃在细颗粒物渗溶冰晶表面的低温粘着系数比在冰晶上的粘着系数大2个数量级。因此有可能利用细颗粒物特性和低温非均相反应消除平流层的卤代烃及氯氟烃等达到阻断大气臭氧耗损的链反应。     

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.     

Recent Northern Hemisphere tropical expansion primarily driven by black carbon and tropospheric ozone

Observational analyses have shown the width of the tropical belt increasing in recent decades as the world has warmed. This expansion is important because it is associated with shifts in large-scale atmospheric circulation and major climate zones. Although recent studies have attributed tropical expansion in the Southern Hemisphere to ozone depletion, the drivers of Northern Hemisphere expansion are not well known and the expansion has not so far been reproduced by climate models. Here we use a climate model with detailed aerosol physics to show that increases in heterogeneous warming agents--including black carbon aerosols and tropospheric ozone--are noticeably better than greenhouse gases at driving expansion, and can account for the observed summertime maximum in tropical expansion. Mechanistically, atmospheric heating from black carbon and tropospheric ozone has occurred at the mid-latitudes, generating a poleward shift of the tropospheric jet, thereby relocating the main division between tropical and temperate air masses. Although we still underestimate tropical expansion, the true aerosol forcing is poorly known and could also be underestimated. Thus, although the insensitivity of models needs further investigation, black carbon and tropospheric ozone, both of which are strongly influenced by human activities, are the most likely causes of observed Northern Hemisphere tropical expansion.     

Arctic warming aloft is data set dependent

Arctic sea ice and snow on land have retreated polewards at an alarming pace in the past few decades. Such retreat locally amplifies surface warming through a positive feedback, which causes the Arctic surface to warm faster than the rest of the globe. In contrast, ice and snow retreat causes little warming in the atmosphere above when the stable winter atmosphere inhibits vertical heat exchange. We therefore find surprising the recent report by Graversen et al. in which they claim that recent Arctic atmospheric warming extends far deeper into the atmosphere than expected, and can even exceed the surface warming during the polar night. Using a different data set, we show that there is much less warming aloft in winter, consistent with the recent retreat of ice and snow, as well as recent changes in atmospheric heat transport.     

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.     

兰州城区臭氧浓度时空变化特征及其与气象条件的关系

依据兰州市环境监测站１９８５－１９９６年大气Ｏ３的监测资料,对兰州城区Ｏ３浓度的年际变化,年变化,日变化和空间分布等时空变化特征进行了分析研究,并分析了其浓度变化与气象条件的关系。结果表明：兰州城区大气Ｏ３浓度存在着较明显的年际变化,最近几年有准两年的变化周期,且其年平均浓度值有波动式升高的趋势;年变化与日变化为单周期,浓度最大值分别出现在７月和午后,空间分布以兰州西固区Ｏ３浓度最高;Ｏ３浓度分布     

特征向量数量对反演大气参数的影响

大气温湿信息是天气预报、研究和业务的主要参教。具有通道多、信息量大、光谱窄等优点的AIRS已逐渐成为大气垂直探测的主流和方向。如何从卫星观测到的辐射测值推算出大气参数显得尤为重要。本文运用特征向量法反演晴空大气温度、臭氧廓线,试验不同数量的特征向量对反演晴空大气温度等参数精度的影响。结果表明适当增加特征向量的数量,对改进反演大气温度、臭氧廓线的精度有明显改善。     

Rapid responses of British butterflies to opposing forces of climate and habitat change.

Habitat degradation and climate change are thought to be altering the distributions and abundances of animals and plants throughout the world, but their combined impacts have not been assessed for any species assemblage. Here we evaluated changes in the distribution sizes and abundances of 46 species of butterflies that approach their northern climatic range margins in Britain-where changes in climate and habitat are opposing forces. These insects might be expected to have responded positively to climate warming over the past 30 years, yet three-quarters of them declined: negative responses to habitat loss have outweighed positive responses to climate warming. Half of the species that were mobile and habitat generalists increased their distribution sites over this period (consistent with a climate explanation), whereas the other generalists and 89% of the habitat specialists declined in distribution size (consistent with habitat limitation). Changes in population abundances closely matched changes in distributions. The dual forces of habitat modification and climate change are likely to cause specialists to decline, leaving biological communities with reduced numbers of species and dominated by mobile and widespread habitat generalists.     

Dust-climate couplings over the past 800,000 years from the EPICA Dome C ice core

Dust can affect the radiative balance of the atmosphere by absorbing or reflecting incoming solar radiation; it can also be a source of micronutrients, such as iron, to the ocean. It has been suggested that production, transport and deposition of dust is influenced by climatic changes on glacial-interglacial timescales. Here we present a high-resolution record of aeolian dust from the EPICA Dome C ice core in East Antarctica, which provides an undisturbed climate sequence over the past eight climatic cycles. We find that there is a significant correlation between dust flux and temperature records during glacial periods that is absent during interglacial periods. Our data suggest that dust flux is increasingly correlated with Antarctic temperature as the climate becomes colder. We interpret this as progressive coupling of the climates of Antarctic and lower latitudes. Limited changes in glacial-interglacial atmospheric transport time suggest that the sources and lifetime of dust are the main factors controlling the high glacial dust input. We propose that the observed approximately 25-fold increase in glacial dust flux over all eight glacial periods can be attributed to a strengthening of South American dust sources, together with a longer lifetime for atmospheric dust particles in the upper troposphere resulting from a reduced hydrological cycle during the ice ages.     

Detection of stratospheric ozone intrusions by windprofiler radars

Stratospheric ozone attenuates harmful ultraviolet radiation and protects the Earth's biosphere. Ozone is also of fundamental importance for the chemistry of the lowermost part of the atmosphere, the troposphere. At ground level, ozone is an important by-product of anthropogenic pollution, damaging forests and crops, and negatively affecting human health. Ozone is critical to the chemical and thermal balance of the troposphere because, via the formation of hydroxyl radicals, it controls the capacity of tropospheric air to oxidize and remove other pollutants. Moreover, ozone is an important greenhouse gas, particularly in the upper troposphere. Although photochemistry in the lower troposphere is the major source of tropospheric ozone, the stratosphere-troposphere transport of ozone is important to the overall climatology, budget and long-term trends of tropospheric ozone. Stratospheric intrusion events, however, are still poorly understood. Here we introduce the use of modern windprofiler radars to assist in such transport investigations. By hourly monitoring the radar-derived tropopause height in combination with a series of frequent ozonesonde balloon launches, we find numerous intrusions of ozone from the stratosphere into the troposphere in southeastern Canada. On some occasions, ozone is dispersed at altitudes of two to four kilometres, but on other occasions it reaches the ground, where it can dominate the ozone density variability. We observe rapid changes in radar tropopause height immediately preceding these intrusion events. Such changes therefore serve as a valuable diagnostic for the occurrence of ozone intrusion events. Our studies emphasize the impact that stratospheric ozone can have on tropospheric ozone, and show that windprofiler data can be used to infer the possibility of ozone intrusions, as well as better represent tropopause motions in association with stratosphere-troposphere transport.     

Changes in tropospheric ozone levels over the Three Representative Regions of China observed from space by the Tropospheric Emission Spectrometer (TES), 2005–2010

Tropospheric ozone observations over China from 2005 to 2010 at three pressure levels (484,681 and 825 hPa) from the Tropospheric Emission Spectrometer on board the NASA Aura satellite have been analyzed.Fourier Transform analysis revealed the trends and seasonality of regionally-averaged,monthly-mean ozone concentrations over western,northern and southern China.Significant increases in ozone levels are found over all three regions at 464 hPa and the rate of increase is fastest over northern China,reaching 0.89±0.059 nL/(La).At 681 hPa,ozone shows increases over northern and western China,at a rate of 0.57± 0.065 nL/(La) and 0.41±0.041 nL/(La) respectively,but is constant over southern China.At 825 hPa,ozone increases at a rate of 0.36±0.074 nL/(La) over northern China,while decreasing over southern China at a rate of 0.21±0.061 nL/(La).Over the three regions,ozone levels are generally higher in summer and lower in winter.Over southern China at all three pressure levels and northern China at the 825 hPa level,ozone shows double peaks occurring in spring and autumn as a result of the combined effects of atmospheric chemistry and global transport.This work provides a useful observational dataset and tools for future analysis of changes in tropospheric ozone over China.     

气象因子对近地面层臭氧浓度的影响

利用近几年来近地面层臭氧浓度和常规气象要素的观测资料。分析了温度、降水、蒸发、风向风速等气象要素对近地面层臭氧浓度的影响．结果表明，近地面层臭氧浓度随着气温的升高而升高，臭氧浓度的日变化和季节变化有同样趋势；而降水、湿度的影响刚好与气温相反；大风或有雾的天气条件也会成为近地面层臭氧浓度增高的因素。这可能与大风对引起近地面臭氧产生的前体物的搬运作用以及雾内湍流将高层臭氧向下的输送作用有关。