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1.
In this paper we describe a technique for estimating chemical ozone loss in the Arctic vortex. Observed ozone and temperature profiles are combined with the model potential vorticity field to produce time series of vortex averaged ozone mixing ratios on chosen isentropic surfaces. Model-derived radiative heating rates and observed vertical gradients of ozone are then used to estimate the change in ozone that would occur due to diabatic descent. Discrepancies with the observed ozone are interpreted as being of chemical origin, assuming that there is negligible horizontal transport or mixing of air into the vortex. The technique is illustrated using ozone sonde measurements collected during the 1991/92 European Arctic Stratospheric Ozone Experiment (EASOE), meteorological analyses from the European Centre for Medium-range Weather Forecasts (ECMWF) and radiative heating rates extracted from the Global Atmospheric Modelling Programme (UGAMP) 3D General Circulation Model. Our results show that there was photochemical ozone destruction inside the Arctic vortex in early 1992 with a loss between 475 K and 550 K (around 20 km) of 0.32±0.15 ppmv in the first 20 days of January, equivalent to a rate of 0.51±0.24%/day (at the 95% confidence level).  相似文献   

2.
In the winter of 1994/95 the German Transall research aircraft performed 5 campaigns in the European Arctic with 22 flights altogether. An extensive dataset of HNO3, ClONO2 and O3 column amounts was obtained by MIPAS-FT (Michelson Interferometer for Passive Atmospheric Sounding - Flugzeug Transall) onboard the aircraft. In this paper we present the variability of the ClONO2 reservoir gas in the course of the winter. We include groundbased FTIR measurements of HF, HCl and ClONO2 to discuss the airborne observations with regard to the partitioning of inorganic chlorine.From mid-December until the end of January, MIPAS measured a stable ClONO2 collar with constantly low column amounts inside the polar vortex and maxima at the edge. This observation reflected widespread conversion of ClONO2 to reactive chlorine inside the vortex for at least six weeks. In good accordance, the ground stations measured low in-vortex HCl and ClONO2 column amounts and conversion of HCl into ClONO2 in the region of the ClONO2 maxima. In the first week of February the ClONO2 amounts started to increase in the edge region as well as inside the vortex. Between March 21 and 27, just one week after the last cold period, MIPAS observed exclusively high ClONO2 column amounts inside the vortex, indicating fast deactivation of active chlorine. In the same period the ground stations measured an excess of ClONO2 over HCl. Further, the high ClONO2 implies that the polar vortex was renoxified in March. Lower ClONO2 values, observed inside the vortex on the flights of April 5 and 8, and an increased HCl/ClONO2 ratio, measured from ground, marked the starting redistribution within the chlorine reservoir species to the photochemically more stable HCl.In February, March and April, MIPAS observed mixing of ClONO2-rich air masses with midlatitude air at the vortex edge. A very clear event happened on March 27. On this flight a distinct ClONO2 minimum was measured at the vortex edge, which was closely correlated with a filament of midlatitude air observed by OLEX (Ozone Lidar EXperiment) onboard the Transall.  相似文献   

3.
Infrared absorption features due to ClO in the lower stratosphere have been identified from groundbased solar absorption spectra taken from Aberdeen, U.K. (57° N, 2° W) on 20 January 1995. A vertical column abundance of 3.42 (±0.47)×1015 molec cm-2 has been derived from 13 independent absorption features in the P and R branches of the (0–1) vibration-rotation band of 35ClO, spanning the spectral region 817–855 cm-1. The observed absorption features are consistent with very high levels of ClO (approximately 2.6 parts per billion by volume (ppbv)) in the altitude range 16–22 km. A comparison of this profile with a 3D chemical transport model profile indicates the observation was made inside the polar vortex and shows good qualitative agreement but the model underestimates the concentrations of ClO. Simultaneous measurements of other species were made including HCl, HF and ClONO2. These columns yield a value for HCl+ClONO2+ClO of 7.02±0.65×1015 molec cm-2. This is lower than the total inorganic chlorine (ClO y ) column of 10.7±1.6×1015 molec cm-2 estimated from mean measured (HCl+ClONO2)/HF ratios together with in-vortex HF measurements. The discrepancy is probably due to significant amounts of the ClO dimer (Cl2O2) in the lower part of the stratosphere. The measurements of highly elevated levels of ClO are used to estimate O3 loss rates at the 400, 475 and 550 K levels making assumptions about the probable distribution of ClO and Cl2O2. These are compared with loss rates derived from ozone sonde data.  相似文献   

4.
Vertical columns of HF, HCl, HNO3, ClONO2, N2O, ClO and COF2 were measured at Harestua, Norway (60.22° N, 10.75° E, Elevation 600 a.s.l.) beginning on 24 November 1994 and concluding on 1 May 1995 during Phase-III of the SESAME (Second European Stratospheric Arctic and Mid-latitude Experiment) measurement campaign. The vertical columns of HCl, HNO3 and ClONO2 measured on 81 days were compared with columns calculated by the 3-D Cambridge model SLIMCAT. In addition the results were also interpreted by comparison with a photochemical trajectory model. Good agreement was seen for HCl while the nitrogen compounds showed larger discrepancies, especially for ClONO2. Evidence for chlorine activation was seen with 65% reduction of the chlorine reservoirs (HCl + ClONO2) while the levels of ClO were greatly enhanced. Interpretation of the loss with the trajectory model indicated condensation of chlorine on PSCs. The vertical column ratio of COF2 and HF was measured to 0.21 outside the vortex and a factor of two lower inside. The recovery of ClONO2 was seen to be much faster than that of HCl in the early spring.  相似文献   

5.
Vertical Profile of Night-Time Stratospheric OClO   总被引：1，自引：0，他引：1  
The first night-time observation of the vertical profile of OClO wasperformed by the AMON balloon-borne spectrometer during the SESAME arcticcampaign, launched from Kiruna in northern Scandinavia. The flight, which tookplace inside the polar vortex on February 10, 1995, reveals mixing ratios of45±10 pptv at 20 km. These results are in excellent agreement with theREPROBUS 3D model simulations, which indicate that the observed OClOcorresponds to daytime ClO and BrO mixing ratios of 1.2 ppbv and 10 pptv,respectively.  相似文献   

6.
A new lightweight in situ instrument designed to measure ClO was flown on a balloon launched into the arctic vortex at dawn on February 3, 1995 at Kiruna, Sweden during the Second European Stratospheric Arctic and Mid-latitude Experiment (SESAME), together with instruments to measure ozone and long-lived tracers. Observations on ascent and descent at different solar zenith angles are compared to results from Lagrangian and box model calculations that assume the airmasses at similar potential temperatures had comparable photochemical histories. Between 20 and 22 km, in a region where ClO was significantly enhanced, a model constrained by currently recommended rate parameters significantly underestimates the abundances of ClO that were observed on ascent at high solar zenith angles, whereas the agreement is much better if a smaller ClO-Cl2O2 equilibrium constant, one inferred from previous ER-2 aircraft observations of ClO in the Arctic during nighttime, is assumed. On ascent, ClO is additionally enhanced in a narrow region between 20 and 21 km. We believe the most plausible explanation for this feature is rapid photolysis of OClO produced by the slow bimolecular reaction ClO + ClO over the 48 hours prior to the observations when the airmass was warmed to 225 K by adiabatic compression while in polar darkness. These results suggest that under special circumstances, OClO can be produced by a reaction other than one involving BrO, and, hence, OClO is not necessarily a universal proxy for BrO abundances in the perturbed polar vortex.  相似文献   

7.
During SESAME phase I ground-based FTIR measurements were performed atEsrange near Kiruna, Sweden, from 28 January to 26 March 1994. Zenith columnamounts of ClONO2, HCl, HF, HNO3,O3, N2O, CH4, and CFC-12 werederived from solar absorption spectra. Time series of ClONO2and HCl indicate a chlorine activation at the end of January and around 1March. On 1 March a very low amount of HCl of 2.09times; 1015molec. cm-2 was detected, probably caused by a second chlorineactivation phase starting from an already decreased amount of HCl. The ratioof column amounts of HCl to ClONO2 decreased inside the vortexfrom about 1 in January to 0.4 in late March compared to values of about 2outside the vortex. Although the Arctic stratosphere was rather warm in winter1993/94 and PSCs occurred seldom, chlorine partitioning into its reservoirspecies HCl and ClONO2 changed during that winter andClONO2 is the major chlorine reservoir at the end of thewinter as in cold winters like 1991/92 and 1994/95.  相似文献   

8.
Vertical column abundances of HCl, ClONO2, HF and HNO3 have been obtained from infrared solar absorption measurements made at Aberdeen, UK (57°N, 2°W) during the periods January 13 1994 - May 8 1994 and November 23 1994 - April 19 1995. The measurements reveal the partitioning of inorganic chlorine (Cly) inside and outside the polar vortex during these two winter and spring periods. Stratospheric temperatures within the northern polar vortex during 1993/94 were not cold throughout January and most of February. The measurements reported here suggest that following a brief period of chlorine activation in late February and early March, the active chlorine within the vortex recovered rapidly to form ClONO2 resulting in in-vortex ClONO2 columns of 7 × 1015 molecules cm-2. In contrast, measurements during January 1995 suggest extensive invortex activation with in-vortex HCl + ClONO2 as low as 3.6×1015 molecules cm-2. High day-to-day variability in the ClONO2 columns observed during February is evidence for the transport of ClONO2 rich air from high to mid latitudes during the late winter. The implications for mid latitude O3 loss are discussed. A preliminary comparison of the HCl, ClONO2, and HNO3 column data from winter 94/95 with a three-dimensional chemical transport model shows that the model generally reproduces well the day-to-day variability and absolute magnitude of the observed columns, especially for HNO3 outside of the vortex.  相似文献   

9.
The set of high-resolution infrared solar observations made with the Atmospheric Trace Molecule Spectroscopy (ATMOS)-Fourier transform spectrometer from onboard Spacelab 3 (30 April-1 May 1985) has been used to evaluate the total budgets of the odd chlorine and fluorine chemical families in the stratosphere. These budgets are based on volume mixing ratio profiles measured for HCl, HF, CH3Cl, ClONO2, CCl4, CCl2F2, CCl3F, CHClF2, CF4, COF2, and SF6 near 30° north latitude. When including realistic concentrations for species not measured by ATMOS, i.e., the source gases CH3CCl3 and C2F3Cl3 below 25 km, and the reservoirs ClO, HOCl and COFCl between 15 and 40 km (five gases actually measured by other techniques), the 30° N zonal 1985 mean total mixing ratio of chlorine, Cl, was found to be equal to (2.58±0.10) ppbv (parts per billion by volume) throughout the stratosphere, with no significant decrease near the stratopause. The results for total fluorine indicate a slight, but steady, decrease of its volume mixing ratio with increasing altitude, around a mean stratospheric value of (1.15±0.12) ppbv. Both uncertainties correspond to one standard deviation. These mean springtime 1985 stratospheric budgets are commensurate with values reported for the tropospheric Cl and F concentrations in the early 1980s, when allowance is made for the growth rates of their source gases at the ground and the time required for tropospheric air to be transported into the stratosphere. The results are discussed with emphasis on conservation of fluorine and chlorine and the partitioning among source, sink, and reservoir gases throughout the stratosphere.  相似文献   

10.
Based upon airborne trace gas and isotope observations in the winter months 1991/1992 to1994/1995, transport pathways across the mid-latitude and Arctic tropopause areinvestigated. A powerful set of contrasting transport tracers are examined, such asdeuterated water vapor (HDO) which is shown to trace the passage of water vapor from thetroposphere into the lowermost stratosphere (LS), or the `SF6 age' defined as theresidence time of an air parcel within the stratosphere since its entry at thetropopause. Cross-tropopause transport in both directions was found near mid-latitudecyclones (at baroclinic flanks of troughs in the polar front), in which about 80% of thestratosphere-to-troposphere flux proceeded along potential temperature ()surfaces of 300 ± 10 K. As these isentropes are the lowest which reach into the LS(in winter), a mixing zone just above the Arctic tropopause (at least 1.5 km thick) isformed. Here, upwelling tropospheric air is mixed with downwelling LS air which isaffected by air from higher altitudes, the surf-zone and the polar vortex. The observedelevated D/H isotope ratio of water vapor within the mixing zone can be explained byinjection of subtropical water vapor that is transported to the tropopause by the warmconveyor belt associated with mid-latitude cyclones. Downward vertical transport ofArctic LS air, which may be influenced by ouflowing chemically disturbed polar vortexair, into the Arctic troposphere was found to be small.  相似文献   

11.
Simulations of polar ozone losses were performed using the three-dimensional high-resolution (1∘ × 1∘) chemical transport model MIMOSA-CHIM. Three Arctic winters 1999–2000, 2001–2002, 2002–2003 and three Antarctic winters 2001, 2002, and 2003 were considered for the study. The cumulative ozone loss in the Arctic winter 2002–2003 reached around 35% at 475 K inside the vortex, as compared to more than 60% in 1999–2000. During 1999–2000, denitrification induces a maximum of about 23% extra ozone loss at 475 K as compared to 17% in 2002–2003. Unlike these two colder Arctic winters, the 2001–2002 Arctic was warmer and did not experience much ozone loss. Sensitivity tests showed that the chosen resolution of 1∘ × 1∘ provides a better evaluation of ozone loss at the edge of the polar vortex in high solar zenith angle conditions. The simulation results for ozone, ClO, HNO3, N2O, and NO y for winters 1999–2000 and 2002–2003 were compared with measurements on board ER-2 and Geophysica aircraft respectively. Sensitivity tests showed that increasing heating rates calculated by the model by 50% and doubling the PSC (Polar Stratospheric Clouds) particle density (from 5 × 10−3 to 10−2 cm−3) refines the agreement with in situ ozone, N2O and NO y levels. In this configuration, simulated ClO levels are increased and are in better agreement with observations in January but are overestimated by about 20% in March. The use of the Burkholder et al. (1990) Cl2O2 absorption cross-sections slightly increases further ClO levels especially in high solar zenith angle conditions. Comparisons of the modelled ozone values with ozonesonde measurement in the Antarctic winter 2003 and with Polar Ozone and Aerosol Measurement III (POAM III) measurements in the Antarctic winters 2001 and 2002, shows that the simulations underestimate the ozone loss rate at the end of the ozone destruction period. A slightly better agreement is obtained with the use of Burkholder et al. (1990) Cl2O2 absorption cross-sections.  相似文献   

12.
Samples of interstitial air from within the snow pack on an ice floe on the Arctic Ocean were collected during the April 1994 Polar Sunrise Experiment. The concentrations of C2-C7 hydrocarbons are reported for the first time in the snow pack interstitial air. Alkane concentrations tended to be higher than concentrations in free air samples above the snow but very similar to winter measurements at various locations in the Arctic archipelago. However, ethyne concentrations in both interstitial and free air were highly correlated with ozone mixing ratios, consistent with previous demonstrations of the effects of Br atom chemistry. The analysis of total bromine within the snow pack indicate an enrichment in total Br at the interface layer between snow and free troposphere. The mixing ratios of some brominated compounds, such as CHBr3 and CHBr2Cl, are found to be higher in this top layer of snow relative to the boundary layer. Results were inconclusive due to the limited number of samples, but suggest the possible presence of active bromine in the snow pack and also that some differences exist between chemical reactions occurring in interstitial air compared to air in the boundary layer.  相似文献   

13.
Far-infrared emission spectroscopy has beendemonstrated to be a valuable method for remotesensing of trace species in the stratosphere, with theability to simultaneously detect a number of keychemical species. SAFIRE-A is a new far-infraredFourier Transform (FT) spectrometer which has beenspecifically designed to operate on board of a highaltitude aircraft in the lower stratosphere and uppertroposphere regions where relatively few remotesensing measurements have been made. Using newtechnology, the sensitivity of the FT spectrometermethod has been substantially improved for the longwavelength region. Results are reported formeasurements of O3, HNO3 and N2O at 17and 19 km using a detection window near 23 cm-1.Geographical and altitude variability of the volumemixing ratio of these constituents and their relativecorrelation are discussed. Ozone measurements agreewell with in situ measurements, except in regions ofstrong stirring and mixing associated with deformationof the northern vortex edge. Whilst SAFIREmeasurements of trace gases do not capture all of thelocal variability seen by rapid in-situ techniques,they can indicate horizontal variability close to, butnot intercepted by, the aircraft's flight path. Apossible detection of ClO at the low background levelsexpected outside the polar vortex is also reported.  相似文献   

14.
Airborne measurements of stratospheric ozone and N2O from the SCIAMACHY (Scanning Imaging Absorption Spectrometer) Validation and Utilization Experiment (SCIA-VALUE) are presented. The campaign was conducted in September 2002 and February–March 2003. The Airborne Submillimeter Radiometer (ASUR) observed stratospheric constituents like O3 and N2O, among others, spanning a latitude from 5°S to 80°N during the survey. The tropical ozone source regions show high ozone volume mixing ratios (VMRs) of around 11 ppmv at 33 km altitude, and the altitude of the maximum VMR increases from the tropics to the Arctic. The N2O VMRs show the largest value of 325 ppbv in the lower stratosphere, indicating their tropospheric origin, and they decrease with increasing altitude and latitude due to photolysis. The sub-tropical and polar mixing barriers are well represented in the N2O measurements. The most striking seasonal difference found in the measurements is the large polar descent in February–March. The observed features are interpreted with the help of SLIMCAT and Bremen Chemical Transport Model (CTMB) simulations. The SLIMCAT simulations are in good agreement with the measured O3 and N2O values, where the differences are within 1 ppmv for O3 and 15 ppbv for N2O. However, the CTMB simulations underestimate the tropical middle stratospheric O3 (1–1.5 ppmv) and the tropical lower stratospheric N2O (15–30 ppbv) measurements. A detailed analysis with various measurements and model simulations suggests that the biases in the CTMB simulations are related to its parameterised chemistry schemes.  相似文献   

15.
The inability to explain the observedoxygen suppression of chlorine photosensitized ozoneloss remains a gap in our understanding of thephotochemistry responsible for depletion of thestratospheric ozone layer. It has been suggested thatthe presence of a weakly bound ClO·O2complexcould explain this effect. The existence of thiscomplex would alter the chlorine budget of thestratosphere, perhaps reducing the chlorine availablefor catalytic ozone destruction. On the other hand,the chemistry of ClO·O2 provides two newpathwaysfor ClO dimer formation, which could increase the rateof catalytic ozone loss. In this paper, we constrainthe kinetic rate system of ClO·O2 tomatch themeasured Cly budget. It is shown thatClO·O2cannot be both fairly stable and rapidly form the ClOdimer, or the resulting partitioning of chlorinebecomes incompatible with observations of both ClO andtotal available chlorine. These constraints allow thateither: (1) the ClO·O2 is fairly stable,but doesnot significantly enhance ClO dimer formation andtherefore has a negligible effect on ozone loss rates,or (2) the ClO·O2 complex is only veryweaklystable, but does rapidly form the ClO dimer, andtherefore can influence stratospheric ozone depletion.Even at the ClO·O2 mixing ratios allowedunderthe assumption of weak stability, 0.1 to 0.2 ppbv,significant ozone loss rate enhancements werecalculated. Of course, the chlorine budget constraintalso allows for a thirdpossibility; that ClO·O2 is neither verystablenor forms Cl2O2 very rapidly. Measuredlimits on the reaction rates for ClO·O2to form the ClO dimer would greatly aid the resolution of thisissue. Since the uncertainties aboutClO·O2chemistry are so large, a potential role forClO·O2 in stratospheric ozone loss cannotbe ruled out at this time.  相似文献   

16.
Near-total depletions of ozone have been observed in the Arctic spring since the mid 1980s. The autocatalytic reaction cycles involving reactive halogens are now recognized to be of main importance for ozone depletion events in the polar boundary layer. We present sensitivity studies using the model MISTRA in the box-model mode on the influence of chemical species on these ozone depletion processes. In order to test the sensitivity of the chemistry under polar conditions, we compared base runs undergoing fluxes of either Br2, BrCl, or Cl2 to induce ozone depletions, with similar runs including a modification of the chemical conditions. The role of HCHO, H2O2, DMS, Cl2, C2H6, HONO, NO2, and RONO2 was investigated. Cases with elevated mixing ratios of HCHO, H2O2, DMS, Cl2, and HONO induced a shift in bromine speciation from Br / BrO to HOBr/HBr, while high mixing ratios of C2H6 induced a shift from HOBr/HBr to Br/BrO. The shifts from Br/BrO to HOBr/HBr accelerated the aerosol debromination, but also increased the total amount of deposited bromine at the surface (mainly via increased deposition of HOBr). For all NOy species studied (HONO, NO2, RONO2) the chemistry is characterized by an increased bromine deposition on snow reducing the amount of reactive bromine in the air. Ozone is less depleted under conditions of high mixing ratios of NOx. The production of HNO3 led to the acid displacement of HCl, and the release of chlorine out of salt aerosol (Cl2 or BrCl) increased.  相似文献   

17.
We call attention to the likely importance of the potential reaction OH+ClOHCl+O2. It may only be a minor channel for the reaction of OH with ClO, which is often ignored in models, but if it occurs it considerably increases the rate of recovery of HCl after an air parcel has encountered a polar stratospheric cloud (PSC). The net effect of this reaction on the ozone concentration depends on the relative HCl concentration and whether the air parcel is in a PSC. When an air parcel is in a PSC and the HCl concentration is less than the sum of the HOCl and ClONO2 concentrations, heterogeneous ClO x production is rate limited by the production of HCl. Under these conditions the reaction allows HCl to be reprocessed more rapidly by the heterogeneous reactions of HCl with HOCl and ClONO2. This allows high ClO x concentration to be maintained for longer, and at a slightly higher level, than would otherwise be possible which in turn leads to more ozone depletion. When there are PSCs but HCl is in excess, or outside of the PSC regions (i.e. during the recovery phase), the reaction will always reduce the ClO/HCl ratio and hence slightly reduce the ozone loss.  相似文献   

18.
Measurements of NOx (NO +NO2) and the sum of reactive nitrogenconstituents, NOy, were made near the surface atAlert (82.5°N), Canada during March and April1998. In early March when solar insolation was absentor very low, NOx mixing ratios were frequentlynear zero. After polar sunrise when the sun was abovethe horizon for much or all of the day a diurnalvariation in NOx and NOy was observed withamplitudes as large as 30–40 pptv. The source ofactive nitrogen is attributed to release from the snowsurface by a process that is apparently sensitized bysunlight. If the source from the snowpack is a largescale feature of the Arctic then the diurnal trendsalso require a competing process for removal to thesurface. From the diurnal change in the NO/NO2ratio, mid-April mixing ratios for the sum of peroxyand halogen oxide radicals of 10 pptv werederived for periods when ozone mixing ratios were inthe normal range of 30–50 ppbv. Mid-day ozoneproduction and loss rates with the active nitrogensource were estimated to be 1–2 ppbv/day and in nearbalance. NOy mixing ratios which averaged only295±66 pptv do not support a large accumulation inthe high Arctic surface layer in the winter and springof 1998. The small abundance of NOy relative tothe elevated mixing ratios of other long-livedanthropogenic constituents requires that reactivenitrogen be removed to the surface during transport toor during residence within the high Arctic.  相似文献   

19.
Ground-based FTIR measurements have been performed in the Arctic summer in July 1993 and June 1994 at 79° N to study the zenith column densities of several trace gases in the undisturbed Arctic summer atmosphere. Zenith column densities of H2O, N2O, HNO3, NO2, NO, ClONO2, ClO, HCl, HF, COF2, OCS, SF6, HCN, CH4, C2H6, C2H2, CO, O3, CFC-12, CFC-22, and CO2 were retrieved by line-by-line calculations. The results are compared with winter and springtime observations measured at the same site, with column densities obtained in the Antarctic summer atmosphere, and with measurements at midlatitudes. For HCl the spectra give lower total zenith columns than expected, but the ratio HF/HCl agrees well with midlatitude literature data. Measurements of ClONO2 give low total columns in agreement with observations at midlatitudes. In the undisturbed atmosphere HCl was found to be in excess of ClONO2. The total columns of HNO3, N2O and the sum of NO and NO2 agree with summer observations in Antarctica. Results for the tropospheric trace gas C2H6 are higher by 250% when compared with Antarctic observations. Contrary to N2O and CH4 the seasonal cycle of C2H6 and C2H2 give much higher total columns in winter/spring compared to the summer observations. This is assigned to transport of polluted airmasses from mid-latitudes into the Arctic.  相似文献   

20.
Carbon dioxide (CO2) has been measured at Alert by grab flask sampling since 1975 as part of the World Meteorological Organization's Background Air Pollution Monitoring Program. Deviations of CO2 concentration from the mean annual cycle have previously been attributed to air masses arriving at Alert from the source regions of the industrialized parts of Europe and the Soviet Union. In situ measurements of ambient CO2 and methane (CH4) were made at Alert using an automated gas chromatograph, as part of the Arctic Haze Study during April 1986. The temporal behaviour of CO2 and CH4 during this period was found to be highly correlated with measurements of particulate sulphate and other atmospheric trace species of anthropogenic origin. Examination of calculated air mass back-trajectories provided further evidence that the observed short-term increases in CO2 and CH4 mixing ratios were due to long-range transport from anthropogenic source regions.  相似文献   

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