Global air quality and pollution

The impact of global air pollution on climate and the environment is a new focus in atmospheric science. Intercontinental transport and hemispheric air pollution by ozone jeopardize agricultural and natural ecosystems worldwide and have a strong effect on climate. Aerosols, which are spread globally but have a strong regional imbalance, change global climate through their direct and indirect effects on radiative forcing. In the 1990s, nitrogen oxide emissions from Asia surpassed those from North America and Europe and should continue to exceed them for decades. International initiatives to mitigate global air pollution require participation from both developed and developing countries.     

Growth of continental-scale metro-agro-plexes, regional ozone pollution, and world food production

Three regions of the northern mid-latitudes, the continental-scale metro-agro-plexes, presently dominate global industrial and agricultural productivity. Although these regions cover only 23 percent of the Earth's continents, they account for most of the world's commercial energy consumption, fertilizer use, food-crop production, and food exports. They also account for more than half of the world's atmospheric nitrogen oxide (NOx,) emissions and, as a result, are prone to ground-level ozone (O(3)) pollution during the summer months. On the basis of a global simulation of atmospheric reactive nitrogen compounds, it is estimated that about 10 to 35 percent of the world's grain production may occur in parts of these regions where ozone pollution may reduce crop yields. Exposure to yield-reducing ozone pollution may triple by 2025 if rising anthropogenic NOx emissions are not abated.     

Instrumental requirements for global atmospheric chemistry

The field of atmospheric chemistry is data-limited, primarily because of the challenge of measuring the key chemical constituents in the global environment. Several recent advances, however, in rugged, portable, remotesensing, ground-based instrumentation and accurate, fast-response airborne instrumentation have provided powerful tools for the understanding of stratospheric ozone, particularly in polar regions. Current discoveries of the role of heterogeneous chemical processes point to the need for better techniques for characterization of stratospheric aerosols. In the troposphere, advances in in situ, sensitive methods for detecting reactive nitrogen compounds have demonstrated the role that these compounds have in controlling global oxidation processes, but better measurements of the reservoir species by which the long-ranged transport of pollutant-reactive nitrogen compounds is thought to occur are urgently needed. The role of hydrocarbons, particularly those of natural origin, in ozone formation in rural areas has focused attention on the requirement for better speciation of these ubiquitous compounds. Lastly, rigorous instrument intercomparison experiments have provided unbiased estimates of measurement capabilities.     

The global atmospheric circulation on moist isentropes

The global atmospheric circulation transports energy from the equatorial regions to higher latitudes through a poleward flow of high-energy and -entropy parcels and an equatorward flow of air with lower energy and entropy content. Because of its turbulent nature, this circulation can only be described in some averaged sense. Here, we show that the total mass transport by the circulation is twice as large when averaged on moist isentropes than when averaged on dry isentropes. The additional mass transport on moist isentropes corresponds to a poleward flow of warm moist air near Earth's surface that rises into the upper troposphere within mid-latitudes and accounts for up to half of the air in the upper troposphere in polar regions.     

Quantifying stratospheric ozone in the upper troposphere with in situ measurements of HCl

We have developed a chemical ionization mass spectrometry technique for precise in situ measurements of hydrochloric acid (HCl) from a high-altitude aircraft. In measurements at subtropical latitudes, minimum HCl values found in the upper troposphere (UT) were often near or below the detection limit of the measurements (0.005 parts per billion by volume), indicating that background HCl values are much lower than a global mean estimate. However, significant abundances of HCl were observed in many UT air parcels, as a result of stratosphere-to-troposphere transport events. We developed a method for diagnosing the amount of stratospheric ozone in these UT parcels using the compact linear correlation of HCl with ozone found throughout the lower stratosphere (LS). Expanded use of this method will lead to improved quantification of cross-tropopause transport events and validation of global chemical transport models.     

Role of deep cloud convection in the ozone budget of the troposphere

Convective updrafts in thunderstorms prolong the lifetime of ozone (O(3)) and its anthropogenic precursor NOx [nitric oxide (NO) + nitrogen dioxide (NO(2))] by carrying these gases rapidly upward from the boundary layer into a regime where the O(3) production efficiency is higher, chemical destruction is slower, and surface deposition is absent. On the other hand, the upper troposphere is relatively rich in O(3) and NOx from natural sources such as downward transport from the stratosphere and lightning; convective overturning conveys the O(3) and NOx toward the Earth's surface where these components are more efficiently removed from the atmosphere. Simulations with a three-dimensional global model suggest that the net result of these counteractive processes is a 20 percent overall reduction in total tropospheric O(3). However, the net atmospheric oxidation efficiency is enhanced by 10 to 20 percent.     

The ascent of atmospheric sciences

In this month's essay, Paul J. Crutzen and Veerabhadran Ramanathan chart some of the courses by which atmospheric sciences evolved from their beginnings, with curious scientists teasing apart the complexity of the air they breathe, into an ever more multidisciplinary enterprise that routinely generates globally consequential knowledge. The authors chronicle developments in chemistry and meteorology up to the early 1970s, before the possibility of human influence beyond the local scale became actualized. To illustrate how humanity's hand has grown to have global effects, they zero in on two contemporary issues: atmospheric ozone and global warming.     

Formation of molecular chlorine from the photolysis of ozone and aqueous sea-salt particles

Halogen atoms from the reactions of sea-salt particles may play a significant role in the marine boundary layer. Reactions of sodium chloride, the major component of sea-salt particles, with nitrogen oxides generate chlorine atom precursors. However, recent studies suggest there is an additional source of chlorine in the marine troposphere. This study shows that molecular chlorine is generated from the photolysis of ozone in the presence of sea-salt particles above their deliquescence point; this process may also occur in the ocean surface layer. Given the global distribution of ozone, this process may provide a global source of chlorine.     

Stratospheric wave spectra resembling turbulence

Pollution effects on ozone raise the question of the significance of turbulence in vertical transport in the stratosphere. The aircraft in situ measurements of velocity fluctuations previously employed to estimate turbulence transport were, it is hypothesized, due to atmospheric waves, despite their classical turbulence spectrum. This new hypothesis implies that previous turbulence estimates are invalid. Experimental tests are suggested.     

The sulfur cycle

Even granting our uncertainties about parts of our model of the sulfur cycle, we can draw some conclusions from it: 1) Man is now contributing about one half as much as nature to the total atmospheric burden of sulfur compounds, but by A.D. 2000 he will be contributing about as much, and in the Northern Hemisphere alone he will be more than matching nature. 2) In industrialized regions he is overwhelming natural processes, and the removal processes are slow enough (several days, at least) so that the increased concentration is marked for hundreds to thousands of kilometers downwind. 3) Our main areas of uncertainty, and ones that demand immediate attention because of their importance to the regional air pollution question, are: (i) the rates of conversion of H(2)S and SO(2) to sulfate particles in polluted as well as unpolluted atmospheres; (ii) the efficiency of removal of sulfur compounds by precipitation in polluted air. And for a better understanding of the global model we need to know: (i) the amount of biogenic H(2)S that enters the atmosphere over the continents and coastal areas; (ii) means of distinguishing man-made and biogenic contributions to excess sulfate in air and precipitation; (iii) the volcanic production of sulfur compounds, and their influence on the particle concentration in the stratosphere; (iv) the large-scale atmospheric circulation patterns that exchange air between stratosphere and troposphere (although absolute amounts of sulfate particles involved are small relative to the lower tropospheric burden); (v) the role of the oceans as sources or sinks for SO(2).     

福州大气污染日与气象条件关系

利用2008-2012年福州市大气污染逐日监测资料确定福州市大气污染日,并分析了其天气形势、地面气象资料及高空探测资料。结果表明,易产生大气污染日的气象特征包括:500 hPa高度场关键区被弱暖平流控制或冷空气势力较弱;850 hPa高度场关键区等高线稀疏,没有明显的天气系统;850 hPa以下大气一般存在逆温层、湿层与风向突变层,大气水平、垂直交流不畅,属静稳大气,易造成大气污染物堆积。大气污染日出现频率较高的海平面气压场类型有:大陆高压脊型、变性冷高压前部型、变性冷高压底部型或后部型、锋前暖区型、均压场型、地面倒槽暖区型。     

Quantifying Transport Between the Tropical and Mid-Latitude Lower Stratosphere

Airborne in situ observations of molecules with a wide range of lifetimes (methane, nitrous oxide, reactive nitrogen, ozone, chlorinated halocarbons, and halon-1211), used in a tropical tracer model, show that mid-latitude air is entrained into the tropical lower stratosphere within about 13.5 months; transport is faster in the reverse direction. Because exchange with the tropics is slower than global photochemical models generally assume, ozone at mid-latitudes appears to be more sensitive to elevated levels of industrial chlorine than is currently predicted. Nevertheless, about 45 percent of air in the tropical ascent region at 21 kilometers is of mid-latitude origin, implying that emissions from supersonic aircraft could reach the middle stratosphere.     

Hydrogen radicals, nitrogen radicals, and the production of O3 in the upper troposphere

The concentrations of the hydrogen radicals OH and HO2 in the middle and upper troposphere were measured simultaneously with those of NO, O3, CO, H2O, CH4, non-methane hydrocarbons, and with the ultraviolet and visible radiation field. The data allow a direct examination of the processes that produce O3 in this region of the atmosphere. Comparison of the measured concentrations of OH and HO2 with calculations based on their production from water vapor, ozone, and methane demonstrate that these sources are insufficient to explain the observed radical concentrations in the upper troposphere. The photolysis of carbonyl and peroxide compounds transported to this region from the lower troposphere may provide the source of HOx required to sustain the measured abundances of these radical species. The mechanism by which NO affects the production of O3 is also illustrated by the measurements. In the upper tropospheric air masses sampled, the production rate for ozone (determined from the measured concentrations of HO2 and NO) is calculated to be about 1 part per billion by volume each day. This production rate is faster than previously thought and implies that anthropogenic activities that add NO to the upper troposphere, such as biomass burning and aviation, will lead to production of more O3 than expected.     

Changes in stratospheric ozone

The ozone layer in the upper atmosphere is a natural feature of the earth's environment. It performs several important functions, including shielding the earth from damaging solar ultraviolet radiation. Far from being static, ozone concentrations rise and fall under the forces of photochemical production, catalytic chemical destruction, and fluid dynamical transport. Human activities are projected to deplete substantially stratospheric ozone through anthropogenic increases in the global concentrations of key atmospheric chemicals. Human-induced perturbations may be occurring already.     

Air pollution and climate-forcing impacts of a global hydrogen economy

If today's surface traffic fleet were powered entirely by hydrogen fuel cell technology, anthropogenic emissions of the ozone precursors nitrogen oxide (NOx) and carbon monoxide could be reduced by up to 50%, leading to significant improvements in air quality throughout the Northern Hemisphere. Model simulations of such a scenario predict a decrease in global OH and an increased lifetime of methane, caused primarily by the reduction of the NOx emissions. The sign of the change in climate forcing caused by carbon dioxide and methane depends on the technology used to generate the molecular hydrogen. A possible rise in atmospheric hydrogen concentrations is unlikely to cause significant perturbations of the climate system.     

Kinetics of the OH Reaction with Methyl Chloroform and Its Atmospheric Implications

The rate coefficients for the reaction of hydroxyl (OH) radicals with methyl chloroform (CH(3)CCI(3)) were measured between 243 and 379 kelvin with the pulsed photolysis-laserinduced fluorescence method. The measured rate coefficients at 298 and 277 kelvin were approximately 20 and approximately 15%, respectively, lower than earlier values. These results will increase the tropospheric OH concentrations derived from the CH(3)CCI(3) budget analysis by approximately 15%. The predicted atmospheric lifetimes of species whose main loss process is the reaction with OH in the troposphere will be lowered by 15% with consequent changes in their budgets, global warming potentials, and ozone depletion potentials.     

Export of north american ozone pollution to the north atlantic ocean

Measurement of the levels of ozone and carbon monoxide (a tracer of anthropogenic pollution) at three surface sites on the Atlantic coast of Canada allow the estimation of the amount of ozone photochemically produced from anthropogenic precursors over North America and transported to the lower troposphere over the temperate North Atlantic Ocean. This amount is greater than that injected from the stratosphere, the primary natural source of ozone. This conclusion supports the contention that ozone derived from anthropogenic pollution has a hemisphere-wide effect at northern temperate latitudes.     

Role of commercial aircraft in global monitoring systems

The role of commercial aircraft in monitoring meteorological parameters and atmospheric constituents has been limited in the former case and virtually nonexistent in the latter. I have tried to point out that this situation can and should be changed now. The new family of wide-bodied jets such as the 747, DC-10, and L-1011 aircraft can be used to supply important global atmospheric and tropical meteorological data for which there is a pressing need. While scientists are not in total agreement on the magnitude of the effect of particulates and gases on the atmosphere, there is almost unanimous concurrence that we are severely limited in information, and that global baseline concentrations must be established for particulates and gases in the troposphere and lower stratosphere as soon as possible. Also, more synoptic meteorological information from the tropical troposphere is highly desirable. In the final analysis, commercial aircraft may offer the most inexpensive way to monitor our atmosphere in the near future. Much of the instrumentation technology is here and the rest is certainly within our grasp. The fact of the matter is that there are now over 220 Boeing 747's and Douglas DC-10's in service, flying an average of 10 hours a day. Long-range flights, such as those from Tokyo to Anchorage to London in the Northern Hemisphere and from Hawaii to Pago Pago to Sydney in the Southern Hemisphere, are commonplace. These aircraft are equipped with inertial navigation systems and central air data computers coupled to advanced data storage systems which can readily be interrogated by satellite. This means that there is now a large amount of snyoptic weather information which can be obtained with a minimum of effort and cost. Likewise, a start at obtaining measurements of atmospheric constituents on a global basis can be made now. All we need to do is make the effort.     

大气氮沉降的研究进展*

 大气氮沉降的增加作为全球变化的重要内容,反映了人类活动加剧导致的大气活性氮污染,已经并将继续对全球生态系统产生重大影响。本文简要介绍了大气氮素干湿沉降的研究方法,回顾了国内外大气氮沉降形态、数量等方面的研究进展及大气氮沉降对水体、森林、农田生态系统的影响,并探讨了该领域目前存在的问题及未来的研究重点和方向。     

Global air pollution crossroads over the Mediterranean

The Mediterranean Intensive Oxidant Study, performed in the summer of 2001, uncovered air pollution layers from the surface to an altitude of 15 kilometers. In the boundary layer, air pollution standards are exceeded throughout the region, caused by West and East European pollution from the north. Aerosol particles also reduce solar radiation penetration to the surface, which can suppress precipitation. In the middle troposphere, Asian and to a lesser extent North American pollution is transported from the west. Additional Asian pollution from the east, transported from the monsoon in the upper troposphere, crosses the Mediterranean tropopause, which pollutes the lower stratosphere at middle latitudes.