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1.
The nature of the Arctic polar stratosphere is observed to be similar in many respects to that of the Antarctic polar stratosphere, where an ozone hole has been identified. Most of the available chlorine (HCl and ClONO(2)) was converted by reactions on polar stratospheric clouds to reactive ClO and Cl(2)O(2) throughout the Arctic polar vortex before midwinter. Reactive nitrogen was converted to HNO(3), and some, with spatial inhomogeneity, fell out of the stratosphere. These chemical changes ensured characteristic ozone losses of 10 to 15% at altitudes inside the polar vortex where polar stratospheric clouds had occurred. These local losses can translate into 5 to 8% losses in the vertical column abundance of ozone. As the amount of stratospheric chlorine inevitably increases by 50% over the next two decades, ozone losses recognizable as an ozone hole may well appear.  相似文献   

2.
Simultaneous global measurements of nitric acid (HNO(3)), water (H(2)O), chlorine monoxide (CIO), and ozone (O(3)) in the stratosphere have been obtained over complete annual cycles in both hemispheres by the Microwave Limb Sounder on the Upper Atmosphere Research Satellite. A sizeable decrease in gas-phase HNO(3) was evident in the lower stratospheric vortex over Antarctica by early June 1992, followed by a significant reduction in gas-phase H(2)O after mid-July. By mid-August, near the time of peak CIO, abundances of gas-phase HNO(3) and H(2)O were extremely low. The concentrations of HNO(3) and H(2)O over Antarctica remained depressed into November, well after temperatures in the lower stratosphere had risen above the evaporation threshold for polar stratospheric clouds, implying that denitrification and dehydration had occurred. No large decreases in either gas-phase HNO(3) or H(2)O were observed in the 1992-1993 Arctic winter vortex. Although CIO was enhanced over the Arctic as it was over the Antarctic, Arctic O(3) depletion was substantially smaller than that over Antarctica. A major factor currently limiting the formation of an Arctic ozone "hole" is the lack of denitrification in the northern polar vortex, but future cooling of the lower stratosphere could lead to more intense denitrification and consequently larger losses of Arctic ozone.  相似文献   

3.
The reactions of dinitrogen pentoxide (N(2)O(5)) with H(2)O and hydrochloric acid (HCl) were studied on ice surfaces in a Knudsen cell flow reactor. The N(2)O(5) reacted on ice at 185 K to form condensed-phase nitric acid (HNO(3)). This reaction may provide a sink for odd nitrogen (NO(x)) during the polar winter, a requirement in nearly all models of Antarctic ozone depletion. A lower limit to the sticking coefficient, gamma, for N(2)O(5) on ice is 1 x 10(-3). Moreover, N(2)O(5) reacted on HCl-ice surfaces at 185 K, with gamma greater than 3 x 10(-3). This reaction, which produced gaseous nitryl chloride (ClNO(2)) and condensed-phase HNO(3), proceeded until all of the HCl within the ice was depleted. The ClNO(2), which did not react or condense on ice at 185 K, can be readily photolyzed in the Antarctic spring to form atomic chlorine for catalytic ozone destruction cycles. The other photolysis product, gaseous nitrogen dioxide (NO(2)), may be important in the partitioning of NO(x) between gaseous and condensed phases in the Antarctic winter.  相似文献   

4.
In order to test photochemical theories linking chlorofluorocarbon derivatives to ozone(O(3)) depletion at high latitudes in the springtime, several related atmospheric species, including O(3), chlorine monoxide(ClO), and bromine monoxide (BrO) were measured in the lower stratosphere with instruments mounted on the NASA ER-2 aircraft on 13 February 1988. The flight path from Moffett Field, California (37 degrees N, 121 degrees W), to Great Slave Lake, Canada (61 degrees N, 115 degrees W), extended to the center of the polar jet associated with but outside of the Arctic vortex, in which the abundance of O(3) was twice its mid-latitude value, whereas BrO levels were 5 parts per trillion by volume (pptv) between 18 and 21 kilometers, and 2.4 pptv below that altitude. The ClO mixing ratio was as much as 65 pptv at 60 degrees N latitude at an altitude of 20 kilometers, and was enhanced over mid-latitude values by a factor of 3 to 5 at altitudes above 18 kilometers and by as much as a factor of 40 at altitudes below 17 kilometers. Levels of ClO and O(3) were highly correlated on all measured distance scales, and both showed an abrupt change in character at 54 degrees N latitude. The enhancement of ClO abundance north of 54 degrees N was most likely caused by low nitrogen dioxide levels in the flight path.  相似文献   

5.
In situ measurements of chlorine monoxide (ClO) at mid- and high northern latitudes are reported for the period October 1991 to February 1992. As early as mid-December and throughout the winter, significant enhancements of this ozone-destroying radical were observed within the polar vortex shortly after temperatures dropped below 195 k. Decreases in ClO observed in February were consistent with the rapid formation of chlorine nitrate (ClONO(2)) by recombination of ClO with nitrogen dioxide (NO(2)) released photochemically from nitric acid (HNO(3)). Outside the vortex, ClO abundances were higher than in previous years as a result of NOx suppression by heterogeneous reactions on sulfate aerosols enhanced by the eruption of Mount Pinatubo.  相似文献   

6.
Observations at Thule, Greenland, that made use of direct light from the moon on 2,3, 4,5, and 7 February 1988 revealed nighttime chlorine dioxide (OClO) abundances that were less than those obtained in Antarctica by about a factor of 5, but that exceeded model predictions based on homogeneous (gas-phase) photochemistry by about a factor of 10. The observed time scale for the formation of OClO after sunset strongly supports the current understanding of the diurnal chemistry of OClO. These data suggest that heterogeneous (surface) reactions due to polar stratospheric clouds can occur in the Arctic, providing a mechanism for possible Arctic ozone depletion.  相似文献   

7.
Dramatic springtime depletions of ozone in polar regions require that polar stratospheric air has a high degree of dynamical isolation and extremely cold temperatures necessary for the formation of polar stratospheric clouds. Both of these conditions are produced within the stratospheric winter polar vortex. Recent aircraft missions have provided new information about the structure of polar vortices during winter and their relation to polar ozone depletions. The aircraft data show that gradients of potential vorticity and the concentration of conservative trace species are large at the transition from mid-latitude to polar air. The presence of such sharp gradients at the boundary of polar air implies that the inward mixing of heat and constituents is strongly inhibited and that the perturbed polar stratospheric chemistry associated with the ozone hole is isolated from the rest of the stratosphere until the vortex breaks up in late spring. The overall size of the polar vortex thus limits the maximum areal coverage of the annual polar ozone depletions. Because it appears that this limit has not been reached for the Antarctic depletions, the possibility of future increases in the size of the Antarctic ozone hole is left open. In the Northern Hemisphere, the smaller vortex and the more restricted region of cold temperatures suggest that this region has a smaller theoretical maximum for column ozone depletion, about 40 percent of the currently observed change in the Antarctic ozone column in spring.  相似文献   

8.
Stratospheric ozone and aerosol distributions were measured across the wintertime Arctic vortex from January to March 1992 with an airborne lidar system as part of the 1992 Airborne Arctic Stratospheric Expedition (AASE II). Aerosols from the Mount Pinatubo eruption were found outside and inside the vortex with distinctly different distributions that clearly identified the dynamics of the vortex. Changes in aerosols inside the vortex indicated advection of air from outside to inside the vortex below 16 kilometers. No polar stratospheric clouds were observed and no evidence was found for frozen volcanic aerosols inside the vortex. Between January and March, ozone depletion was observed inside the vortex from 14 to 20 kilometers with a maximum average loss of about 23 percent near 18 kilometers.  相似文献   

9.
In situ measurements of chlorine monoxide, bromine monoxide, and ozone are extrapolated globally, with the use of meteorological tracers, to infer the loss rates for ozone in the Arctic lower stratosphere during the Airborne Arctic Stratospheric Expedition II (AASE II) in the winter of 1991-1992. The analysis indicates removal of 15 to 20 percent of ambient ozone because of elevated concentrations of chlorine monoxide and bromine monoxide. Observations during AASE II define rates of removal of chlorine monoxide attributable to reaction with nitrogen dioxide (produced by photolysis of nitric acid) and to production of hydrochloric acid. Ozone loss ceased in March as concentrations of chlorine monoxide declined. Ozone losses could approach 50 percent if regeneration of nitrogen dioxide were inhibited by irreversible removal of nitrogen oxides (denitrification), as presently observed in the Antarctic, or without denitrification if inorganic chlorine concentrations were to double.  相似文献   

10.
How strong is the case linking global release of chlorofluorocarbons to episodic disappearance of ozone from the Antarctic stratosphere each austral spring? Three lines of evidence defining a link are (i) observed containment in the vortex of ClO concentrations two orders of magnitude greater than normal levels; (ii) in situ observations obtained during ten high-altitude aircraft flights into the vortex as the ozone hole was forming that show a decrease in ozone concentrations as ClO concentrations increased; and (iii) a comparison between observed ozone loss rates and those predicted with the use of absolute concentrations of ClO and BrO, the rate-limiting radicals in an array of proposed catalytic cycles. Recent advances in our understanding of the kinetics, photochemistry, and structural details of key intermediates in these catalytic cycles as well as an improved absolute calibration for ClO and BrO concentrations at the temperatures and pressures encountered in the lower antarctic stratosphere have been essential for defining the link.  相似文献   

11.
Earth's modern climate, characterized by polar ice sheets and large equator-to-pole temperature gradients, is rooted in environmental changes that promoted Antarctic glaciation ~33.7 million years ago. Onset of Antarctic glaciation reflects a critical tipping point for Earth's climate and provides a framework for investigating the role of atmospheric carbon dioxide (CO(2)) during major climatic change. Previously published records of alkenone-based CO(2) from high- and low-latitude ocean localities suggested that CO(2) increased during glaciation, in contradiction to theory. Here, we further investigate alkenone records and demonstrate that Antarctic and subantarctic data overestimate atmospheric CO(2) levels, biasing long-term trends. Our results show that CO(2) declined before and during Antarctic glaciation and support a substantial CO(2) decrease as the primary agent forcing Antarctic glaciation, consistent with model-derived CO(2) thresholds.  相似文献   

12.
Upper Atmosphere Research Satellite observations indicate that extensive denitrification without significant dehydration currently occurs only in the Antarctic during mid to late June. The fact that denitrification occurs in a relatively warm month in the Antarctic raises concern about the likelihood of its occurrence and associated effects on ozone recovery in a colder and possibly more humid future Arctic lower stratosphere. Polar stratospheric cloud lifetimes required for Arctic denitrification to occur in the future are presented and contrasted against the current Antarctic cloud lifetimes. Model calculations show that widespread severe denitrification could enhance future Arctic ozone loss by up to 30%.  相似文献   

13.
The reliability of Arctic climate predictions is currently hampered by insufficient knowledge of natural climate variability in the past. A sediment core from Lake El'gygytgyn in northeastern (NE) Russia provides a continuous, high-resolution record from the Arctic, spanning the past 2.8 million years. This core reveals numerous "super interglacials" during the Quaternary; for marine benthic isotope stages (MIS) 11c and 31, maximum summer temperatures and annual precipitation values are ~4° to 5°C and ~300 millimeters higher than those of MIS 1 and 5e. Climate simulations show that these extreme warm conditions are difficult to explain with greenhouse gas and astronomical forcing alone, implying the importance of amplifying feedbacks and far field influences. The timing of Arctic warming relative to West Antarctic Ice Sheet retreats implies strong interhemispheric climate connectivity.  相似文献   

14.
Brine rejection that accompanies ice formation in coastal polynyas is responsible for ventilating several globally important water masses in the Arctic and Antarctic. However, most previous studies of this process have been indirect, based on heat budget analyses or on warm-season water column inventories. Here, we present direct measurements of brine rejection and formation of North Pacific Intermediate Water in the Okhotsk Sea from moored winter observations. A steady, nearly linear salinity increase unambiguously caused by local ice formation was observed for more than a month.  相似文献   

15.
Laboratory studies of heterogeneous reactions important for ozone depletion over Antarctica are reported. The reaction of chlorine nitrate (ClONO(2)) with H(2)0 and hydrogen chloride (HCl) on surfaces that simulate polar stratospheric clouds [ice and nitric acid (HNO(3))-ice and sulfuric acid] are studied at temperatures relevant to the Antarctic stratosphere. The reaction of ClONO(2) on ice and certain mixtures of HNO(3) and ice proceeded readily. The sticking coefficient of ClONO(2) on ice of 0.009 +/- 0.002 was observed. A reaction produced gas-phase hypochlorous acid (HOCl) and condensed-phase HNO(3); HOC1 underwent a secondary reaction on ice producing dichlorine monoxide (Cl(2)O). In addition to the reaction with H(2)0, ClONO(2) reacted with HCl on ice to form gas-phase chlorine (Cl(2)) and condensed-phase HNO(3.) Essentially all of the HCl in the bulk of the ice can react with ClONO(2) on the ice surface. The gaseous products of the above reactions, HOCl, Cl(2)0, and Cl(2), could readily photolyze in the Antarctic spring to produce active chlorine for ozone depletion. Furthermore, the formation of condensed-phase HNO(3) could serve as a sink for odd nitrogen species that would otherwise scavenge the active chlorine.  相似文献   

16.
Simultaneous in situ measurements of hydrochloric acid (HCl) and chlorine monoxide (ClO) in the Arctic winter vortex showed large HCl losses, of up to 1 part per billion by volume (ppbv), which were correlated with high ClO levels of up to 1.4 ppbv. Air parcel trajectory analysis identified that this conversion of inorganic chlorine occurred at air temperatures of less than 196 +/- 4 kelvin. High ClO was always accompanied by loss of HCI mixing ratios equal to (1/2)(ClO + 2Cl(2)O(2)). These data indicate that the heterogeneous reaction HCl + ClONO(2) --> Cl(2) + HNO(3) on particles of polar stratospheric clouds establishes the chlorine partitioning, which, contrary to earlier notions, begins with an excess of ClONO(2), not HCl.  相似文献   

17.
Nitric oxide reductase (NOR) is an iron-containing enzyme that catalyzes the reduction of nitric oxide (NO) to generate a major greenhouse gas, nitrous oxide (N(2)O). Here, we report the crystal structure of NOR from Pseudomonas aeruginosa at 2.7 angstrom resolution. The structure reveals details of the catalytic binuclear center. The non-heme iron (Fe(B)) is coordinated by three His and one Glu ligands, but a His-Tyr covalent linkage common in cytochrome oxidases (COX) is absent. This structural characteristic is crucial for NOR reaction. Although the overall structure of NOR is closely related to COX, neither the D- nor K-proton pathway, which connect the COX active center to the intracellular space, was observed. Protons required for the NOR reaction are probably provided from the extracellular side.  相似文献   

18.
Interpretation of recent Southern Hemisphere climate change   总被引：5，自引：0，他引：5  
Climate variability in the high-latitude Southern Hemisphere (SH) is dominated by the SH annular mode, a large-scale pattern of variability characterized by fluctuations in the strength of the circumpolar vortex. We present evidence that recent trends in the SH tropospheric circulation can be interpreted as a bias toward the high-index polarity of this pattern, with stronger westerly flow encircling the polar cap. It is argued that the largest and most significant tropospheric trends can be traced to recent trends in the lower stratospheric polar vortex, which are due largely to photochemical ozone losses. During the summer-fall season, the trend toward stronger circumpolar flow has contributed substantially to the observed warming over the Antarctic Peninsula and Patagonia and to the cooling over eastern Antarctica and the Antarctic plateau.  相似文献   

19.
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.  相似文献   

20.
The current understanding of stratospheric chemistry is reviewed with particular attention to the influence of human activity. Models are in good agreement with measurements for a variety of species in the mid-latitude stratosphere, with the possible exception of ozone (O(3)) at high altitude. Rates calculated for loss of O(3) exceed rates for production by about 40 percent at 40 kilometers, indicating a possible but as yet unidentified source of high-altitude O(3). The rapid loss of O(3) beginning in the mid-1970s at low altitudes over Antarctica in the spring is due primarily to catalytic cycles involving halogen radicals. Reactions on surfaces of polar stratospheric clouds play an important role in regulating the abundance of these radicals. Similar effects could occur in northern polar regions and in cold regions of the tropics. It is argued that the Antarctic phenomenon is likely to persist: prompt drastic reduction in the emission of industrial halocarbons is required if the damage to stratospheric O(3) is to be reversed.  相似文献   

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