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1.
The HO x (OH and HO2) production rate in indoor air caused by radon decay was measured by the chemical amplification technique. The average HO x production rate was found to be (4.31±0.07)×105 HO x per Rn decay per second (Bq) within the range of relative humidity from 3.4 to 55.0 percent at 22 °C. This work providedG(HO x )-value, 7.86±0.13 #/100 eV in air by directly measuring [HO x ] from radiolysis of water vapor. It is also found that there is no obvious relationship between the HO x production rate and the relative humidity in this range. Therefore, this work provides both the basic data for the evaluation of radioactive pollution in indoor air as well as a potentially useful way to produce HO x concentrations in air.  相似文献   

2.
To characterize atmospheric particulate matter equal or less than 2.5 μm in diameter (PM2.5) over the Tropical Atlantic Ocean, aerosol sampling was carried out in Puerto Rico during August and September, 2006. Aerosols were analyzed by ion chromatography for water-soluble inorganic and organic ions (including Na+, NH4 +, Mg2+, Ca2+, K+, Cl?, SO4 2?, NH4 +, F?, methanesulfonate (MSA), and oxalate), by inductive coupled plasma mass spectrometry (ICPMS) for trace elements (Al, Fe, Zn, Mn, Cu, Ni, V, Pb, Cr, Sb, Co, Sc, Cd), and by scanning electron microscopy for individual aerosol particle composition and morphology. The results show that the dominant cations in aerosols were Na+, (mean: 631 ng m?3), accounting for 63.8 % of the total cation and NH4 + (mean: 164 ng m?3), accounting for 13.8 % of the total cation measured in this study. The main inorganic anions were Cl? (576 ng m?3, 54.1 %) and SO4 2? (596 ng m?3, 38.0 %). The main organic anion was oxalate (18 ng m?3). Crustal enrichment factor calculations identified 62 % of the trace elements measured (Cu, Ni, V, Co, Al, Mn, Fe, Sc, and Cr) with crustal origin. Single particle analysis demonstrated that 40 % of the aerosol particles examined were Cl? rich particles as sodium chloride from seawater and 34 % of the total particles were Si-rich particles, mainly in the form of aluminosilicates from dust material. Based on the combination of air-mass trajectories, cluster analysis and principal component analysis, the major sources of these PM2.5 particles include marine, Saharan dust and biomass burning from West Africa; however, volcanic emissions from the Soufriere Hills in Montserrat had significant impact on aerosol composition in this region at the time of sample collection.  相似文献   

3.
During the summer (8 June through 3 September) of 2008, 9 ozone profiles are examined from Dakar, Senegal (14.75°N, 17.49°W) to investigate ozone (O3) variability in the lower/middle troposphere during the pre-monsoon and monsoon periods. Results during June 2008 (pre-monsoon period) show a reduction in O3 concentrations, especially in the 850–700 hPa layer with Saharan Air Layer (SAL) events. However, O3 concentrations are increased in the 950–900 hPa layer where the peak of the inversion is found and presumably the highest dust concentrations. We also use the WRF-CHEM model to gain greater insights for observations of reduced O3 concentrations during the monsoon periods. In the transition period between 26 June and 2 July in the lower troposphere (925–600 hPa), a significant increase in O3 concentrations (10–20 ppb) occur which we suggest is caused by enhanced biogenic NOX emissions from Sahelian soils following rain events on 28 June and 1 July. The results suggest that during the pre-monsoon period ozone concentrations in the lower troposphere are controlled by the SAL, reducing ozone concentrations through heterogeneous chemical processes. At the base of the SAL we also find elevated levels of ozone, which we attribute to biogenic sources of NOX from Saharan dust that are released in the presence of moist conditions. Once the monsoon period commences, lower ozone concentrations are observed and modeled which we attribute to the dry deposition of ozone and episodes of ozone poor air that is horizontally transported into the Sahel from low latitudes by African Easterly Waves (AEWs).  相似文献   

4.
Simultaneous measurements of ozone and ozoneprecursors were made during a field campaign atSchauinsland in the Black Forest and in the valleynorth of Schauinsland that channels the flow ofpolluted air from the city of Freiburg to the site.From the decay of hydrocarbons and NOx between the twomeasuring sites and the known rate coefficients, theconcentration of OH radicals was calculated. From abudget analysis of OH and HOx it is concluded that therelatively high OH concentrations (5–8 ×106cm-3) in the presence of high NO2concentrations cannot be explained by the knownprimary sources. The budget can be closed if efficientrecycling of OH via HO2 is assumed to occur andthat, based on the measured hydrocarbons, 2 HO2molecules are formed for each OH radical that reactswith a hydrocarbon molecule. This assumption is inaccordance with the budget of Ox obtained from ourmeasurements and with results from earliermeasurements of alkylnitrates and peroxy radicals atSchauinsland. A possible conclusion is that the decayof precursors and production of photooxidants in urbanplumes proceeds at a faster rate than is currentlyassumed. The potential role of biogenichydrocarbons for the radical budget is alsodiscussed.  相似文献   

5.
The photochemical activation of chlorine by dissolved iron in artificial sea-salt aerosol droplets and by highly dispersed iron oxide (Fe2O3) aerosol particles (mainly hematite, specific surface ~150 m2 g?1) exposed to gaseous HCl, was investigated in humidified air in a Teflon simulation chamber. Employing the radical-clock technique, we quantified the production of gaseous atomic chlorine (Cl) from the irradiated aerosol. When the salt aerosol contained Fe2O3 at pH 6, no significant Cl production was observed, even if the dissolution of iron was forced by “weathering” (repeatedly freezing and thawing for five times). Adjusting the pH in the stock suspension to 2.6, 2.2, and 1.9 and equilibrating for one week resulted in a quantifiable amount of dissolved iron (0.03, 0.2, and 0.6 mmol L?1, respectively) and in gaseous Cl production rates of ~1.6, 6, and 8?×?1021 atoms cm?2 h?1, respectively. In a further series of experiments, the pure Fe2O3 aerosol was exposed to various levels of gaseous hydrogen chloride (HCl). The resulting Cl production rates ranged from 8?×?1020 Cl atoms cm?2 h?1 (at ~4 ppb HCl) to 5?×?1022 Cl atoms cm?2 h?1 (at ~350 ppb HCl) and confirmed the uptake and conversion of HCl to atomic Cl (at HCl to Cl conversion yields of 2–5 %, depending on the relative humidity). The Fe2O3 experiments indicate that iron-induced Cl formation may be important for highly soluble combustion-aerosol particles in marine environments in the presence of gaseous HCl.  相似文献   

6.
An investigation of the influence of mineral dust ontrace gas cycles in the troposphere is carried out inthis study. A 3D regional scale atmospheric chemistrymodel (STEM-III) which includes aerosol processes isused for the numerical simulations for May 1987.Heterogeneous interactions between gaseous species(SO2, N2O5, HNO3, HO2andH2O2) and the dust particles are considered.Emissions of dust behind convective cold fronts aremodeled. The transport and distribution of mineraldust predicted from the model is compared withsatellite measurements (aerosol index from TOMS). Themodel is shown to capture the synoptic variability inthe observed aerosol index. Calculations show twomajor dust events in May 1987, during which thedust levels close to the source reach more than500 g/m3. The transport of dust is mostlyrestricted towards the north, with the net continentaloutflow of 6 Tg for the entire month. Results showthat the presence of mineral aerosol can greatlyimpact sulfate and nitrate distributions. Averagedover the month of May, the presence of dust isestimated to increase particulate sulfate and nitratelevels in east Asia by 40%. Furthermore, the sulfateand nitrate on the dust particles are predicted to beassociated with the coarse mode (3–5 m particlediameter), consistent with observations over Japan.The influence of mineral dust on the photochemicaloxidant cycle is also investigated. For the entiremonth, a5–10% decrease in boundary layer ozone ispredicted by the model closer to regions of higherdust levels. The ratio of nitric acid to NOx overmarine regions is reduced by a factor between 1 and 2in the boundary layer to more than 2 in the freetroposphere as a result of aerosol processes.  相似文献   

7.
A photochemical box model including a detailed heterogeneous chemistrymodule has been used to analyze in detail the effects of temperature andaerosol surface area on odd oxygen production/depletion in the lowerstratosphere at 30° S. Results show that for background aerosolloading, the hydrolysis of BrONO2 and N2O5are most important atall temperatures studied except when the temperature falls below about205 K, when ClONO2 hydrolysis becomes most important. Thisprocessing leads to removal of active nitrogen to form nitric acid andenhancement of HOx, BrOx, ClOx levels. Detailed O3 budgets asa function of temperature are presented showing how ozone loss andproduction terms vary with changes in stratospheric sulfate aerosol loadingfor the individual families. For (most) aerosol loading levels, thelargest ozone losses occurred at warmer temperatures due to the strongtemperature dependence of the NOx ozone-destroying reactions. Theexception to this occurred for the conditions representative of volcanicloading, which showed a strong increase in ozone destruction due toincreases in destruction from the ClOx and HOx families.The ozoneproduction term k[NO][HO2] did not show a strong dependence oneithertemperature or aerosol loading, due to the offsetting effect of reducedNOxand increased HOx concentrations.  相似文献   

8.
An instrument is developed for the measurement of peroxy radical using chemical amplification coupled with NO2-luminol chemiluminescence detection. The chain length of 147 ± 10 (1σ) is determined by an HO2 source that uses the photolysis of water vapor under 184.9 nm in air. A Nafion system equipped with a Nafion tube of ~2.2 mm external diameter and 350 mm length is employed in the PERCA instrument (Nafion-PERCA system). When flowing an air sample containing HO2 through the Nafion system, it is found that - 94.6 % of HO2 is removed. In contrast, only 17.8 % of RO2 radicals (a mixtures of CH3O2 and CH3C(O)O2 with a ratio of 1.1:0.9) are removed. The results indicate the Nafion system has a good selective removing performance of HO2 radical during the PERCA measurement. Therefore, the method could be applied to ambient and laboratory measurements of absolute concentrations of RO2 as well as the sum of HO2 and RO2.  相似文献   

9.
The dynamics and the aerosol chemistry of the air masses reaching the free troposphere of the subtropical Northeast Atlantic region during the period 1995–98 have been studied. Seven days backward trajectories were calculated daily with HYSPLIT-4 model for Izaña Global Atmospheric Watch (GAW) Observatory (28.3°N 16.5°W, 2367 m a.s.l.). These back-trajectories were classified by means of a k-means clustering strategy. The daily air masses have been coded using 16 variables to detect the aerosol load of each one of them. Four clusters were found: Cluster 1, representative of Atlantic oceanic middle troposphere air masses, (OMT), has an average frequency of occurrence of 50.6%. Cluster 2, which includes air masses originated in the African continent (AfD), has been recorded in a 19.8% of time. Cluster 3 represents a mixture at least of two of the next sources: Europe, Africa and Ocean, (EAM), with a frequency of 12.7%. Finally, Cluster 4 includes air masses with a high load of maritime aerosols, (MaA), and it has been detected in a 16.9%. An analysis of four aerosol components: NO3 ?, NH4 +, non-sea-salt-SO4 2?, and mineral dust and its relation with the origin and transport of the air masses have been done. The highest quantities of mineral dust and nss-SO4 2? are linked with African air masses with a mean value of 86.5 and 1.9 μg/m3 respectively. Whereas the highest levels of NO3 ?, 1.0 μg/m3, and NH4 +, 0.4 μg/m3, were obtained for AfD and EAM. The lowest levels were associated with OMT and MaA air masses types: 12.7, 0.6, 0.2, and 0.5 μg/m3 for dust, NO3 ?, NH4 +, and nss-SO4 2? in average for the four studied years. However, it is remarkable that the values of the median for dust are 2.2 and 3.5 μg/m3 in clusters MaA and OMT respectively. Using non-parametric statistical tests the distributions of concentrations in each cluster by year have been compared in order to detect similarities. The results show that the aerosol loads of OMT and MaA air masses are quite similar and the same occurs for AfD and EAM air masses. However, the correlation analysis between the levels of anions and ammonium evidenced important differences among the air mass types. In AfD air masses is clear a low correlation between levels of nss-SO4 2? and NH4 + (r 2 = 0.08) suggesting that the sulfate speciation was dominated by sulfate species others than ammonium sulfate, such as calcium sulfate. CaSO4 ?2H2O (gypsum) is mainly present in the coarse mode, where the radiative effects of sulfate are less important that in the accumulative mode. For OMT air masses is noticeable an important increasing on the correlation between the levels of anions and those of NH4 + for the two last years of the study period (1997–1998, r 2 = 0.61 –0.85%) with respect to the first ones (1995–1996, r 2 = 0.25–0.49%), coinciding with the second strongest ENSO (El Niño Southern Oscillation) event recorded. This behavior indicates a change in the speciation of the aerosol component.  相似文献   

10.
In situ measurements of [OH], [HO2] (square brackets denote species concentrations), and other chemical species were made in the tropical upper troposphere (TUT). [OH] showed a robust correlation with solar zenith angle. Beyond this dependence, however, [OH] did not correlate to its primary source, the product of [O3] and [H2O] ([O3]?[H2O]), or its sink [NOy]. This suggests that [OH] is heavily buffered in the TUT. One important exception to this result is found in regions with very low [O3], [NO], and [NOy]. Under these conditions, [OH] is highly suppressed, pointing to the critical role of NO in sustaining OH in the TUT and the possibility of low [OH] over the western Pacific warm pool due to strong marine convections bringing NO-poor air to the TUT. In contrast to [OH], [HOx] ([OH] + [HO2]) correlated reasonably well with [O3]?[H2O]/[NOy], suggesting that [O3]?[H2O] and [NOy] are the significant source and sink, respectively, of [HOx].  相似文献   

11.
Reported are the results from a comparison of OH,H2O2CH3OOH, and O3 observationswithmodel predictions based on current HOx–CH4reaction mechanisms. The field observations are thoserecorded during the NASA GTE field program, PEM-Tropics A. The major focus ofthis paper is on thosedata generated on the NASA P-3B aircraft during a mission flown in the marineboundary layer (MBL) nearChristmas Island, a site located in the central equatorial Pacific (i.e.,2° N, 157° W). Taking advantage of thestability of the southeastern trade-winds, an air parcel was sampled in aLagrangian mode over a significantfraction of a solar day. Analyses of these data revealed excellent agreementbetween model simulated andobserved OH. In addition, the model simulations reproduced the major featuresin the observed diurnalprofiles of H2O2 and CH3OOH. In the case ofO3, the model captured the key observational feature whichinvolved an early morning maximum. An examination of the MBL HOxbudget indicated that the O(1D) + H2Oreaction is the major source of HOx while the major sinks involveboth physical and chemical processes involving the peroxide species,H2O2 and CH3OOH. Overall, the generally goodagreement between modeland observations suggests that our current understanding ofHOx–CH4 chemistry in the tropical MBL isquite good; however, there remains a need to critically examine this chemistrywhen both CH2O and HO2are added to the species measured.  相似文献   

12.
An extensive aerosol sampling program was conducted during January-December 2006 over Kolkata (22o33?? N and 88o20?? E), a mega-city in eastern India in order to understand the sources, distributions and properties of atmospheric fine mode aerosol (PM2.5). The primary focus of this study is to determine the relative contribution of natural and anthropogenic as well as local and transported components to the total fine mode aerosol loading and their seasonal distributions over the metropolis. The average concentrations of fine mode aerosol was found to be 71.2?±?25.2???gm-3 varying between 34.5???gm-3 in monsoon and 112.6???gm-3 in winter. The formation pathways of major secondary aerosol components like nitrate and sulphate in different seasons are discussed. A long range transport of dust aerosol from arid and semi-arid regions of western India and beyond was observed during pre-monsoon which significantly enriched the total aerosol concentration. Vehicular emissions, biomass burning and transported dust particles were the major sources of PM2.5 from local and continental regions whereas sea-salt aerosol was the major source of PM2.5 from marine source regions.  相似文献   

13.
We show that photochemical processes in the lower half of the troposphere are strongly affected by the presence of liquid water clouds. Especially CH2O, an important intermediate of CH4 (and of other hydrocarbon) oxidation, is subject to enhanced breakdown in the aqueous phase. This reduces the formation of HO x -radicals via photodissociation of CH2O in the gas phase. In the droplets, the hydrated form of CH2O, its oxidation product HCO2 –, and H2O2 recycle O2 – radicals which, in turn, react with ozone. We show that the latter reaction is a significant sink for O3. Further O3 concentrations are reduced as a result of decreased formation of O3 during periods with clouds. Additionally, NO x , which acts as a catalyst in the photochemical formation of O3, is depleted by clouds during the night via scavenging of N2O5. This significantly reduces NO x -concentrations during subsequent daylight hours, so that less NO x is available for O3 production. Clouds thus directly reduce the concentrations of O3, CH2O, NO x , and HO x . Indirectly, this also affects the budgets of other trace gases, such as H2O2, CO, and H2.  相似文献   

14.
Ground-based aerosol instrumentation covering particle size diameters from 25 nm to 32 µm was deployed to determine aerosol concentration and cloud condensation nuclei (CCN)-activation properties at water vapor supersaturations in the range of S = 0.20–1.50 % in the remote Brazilian northeast semi-arid region (NEB) in coastal (maritime) and continental (inland) regimes. The instruments measured aerosol number concentration and activation spectra for CCN and revealed that aerosol properties are sensitive with respect to the sources as a function of the local wind circulation system. The observations show that coastal aerosol total number concentrations are above 3,000 cm?3 on average, exhibiting concentration peaks depending on the time of the day in a consistent daily pattern. The variation on aerosol concentration has also influences on the fraction of particles active as CCN. At 1.0 % water vapor supersaturation, the fraction can reach as high as 80 %. Inland aerosol total concentrations were about 1,800–1,900 cm?3 and did not show much diurnal variation. The fraction of particles active as CCN observed inland depend on the history of the air masses, and was much higher when air masses were originated over the sea. It was found that (NH4)2SO4 and NaCl are the major soluble inorganic fraction of the aerosols at the coast. The major fraction of NaCl was present in the coarse mode, while ammonium sulfate dominates the inorganic fraction at the submicron range, with about 10 % of the total aerosol mass at 0.32 µm. Inorganic compounds are almost absent in particles with sizes around 0.1 μm. The study suggests that the air masses with high concentration of CCN originate at the sea. The feasible explanation lies in the fact that the NEB’s beaches have a particular morphology that produces a wide surf zone and creates a large load of aerosols when combined with strong and permanent winds of the region.  相似文献   

15.
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   

16.
Using long path UV absorption spectroscopy we have measured OH concentrations close to the earth's surface. The OH values observed at two locations in Germany during 1980 through 1983 range from 0.7×106 to 3.2×106 cm-3. Simultaneously we measured the concentrations of O3, H2O, NO, NO2, CH4, CO, and the light non methane hydrocarbons. We also determined the photolysis rates of O3 and NO2. This allows calculations of OH using a zero dimensional time depdendent model. The modelled OH concentrations significantly exceed the measured values for low NO x concentrations. It is argued that additional, so far unidentified. HO x loss reactions must be responsible for that discrepancy.  相似文献   

17.
Reactive halogen species (RHS = X, XO, HOX, OXO; X = Cl, Br, I) are known to have an important influence on the chemistry in the polar boundary layer (BL), where they are responsible for ozone depletion events in spring. Recent field campaigns at Mace Head, Ireland, and the Dead Sea, Israel, identified for the first time iodine oxide (IO) at mixing ratios of up to 6.6 ppt and 90 ppt bromine oxide (BrO), respectively, by DOAS also at lower latitudes. These results intensified the discussion about the role of the RHS in the mid-latitude BL.Photochemical box model calculations show that the observed IO mixing ratios can destroy ~0.45 ppb ozone per hour. This is comparable to the rates of the known O3-loss processes in the boundary layer. The model studies also reveal that IO, at these levels, has a strong influence on the BL photochemistry, increasing the OH/HO2- and the NO2/NO - ratios. In combination these changes lead to a reduction of the photochemical ozone formation, which - in addition - reduces ozone mixing ratios by up to 0.15 ppb/h.The studies for the Dead Sea case give no information on the heterogeneous process responsible for the bromine release, but they show that a total of 2 – 4 ppb of total bromine have to be released to explain the observed complete depletion of 60 ppb ozone in 2 – 3 hours.  相似文献   

18.
The size-segregated chemical composition of aerosol particles was investigated during 1?year at the puy de D?me (1,465?m?a.s.l.), France. These measurements aimed to a better understanding of the influence of the air mass origin on the size-segregated chemical composition of the aerosol at an altitude site. Mountain site measurements are important because they are representative of long range transport and useful for model validation. PM1 mass concentration exhibits a seasonal variability with a summer maximum. The composition of PM1 did not change significantly in terms of relative contribution of water soluble inorganic ions but is rather variable in term of total mass concentrations. For the PM10-1, a different seasonal behaviour was found with maxima concentrations in autumn-winter. Aerosols were classified into four different categories according to their air mass origin: marine, marine modified, continental and Mediterranean. The PM10 aerosol mass at 50?% relative humidity was close to 2.5???g?m?3 in the marine, 4.3???g?m?3 in the marine modified, 10.3???g?m?3 in the continental and 7.7???g?m?3 in the Mediterranean sectors. We noted that the influence of the air mass origin (on the chemical properties) could be seen especially on the PM10-1. A significant PM10-1 mode was found in marine, modified marine, and Mediterranean air masses, and PM1 dominated in the continental air masses samples. As a result, the aerosol chemical composition variability at the puy de D?me is a function of both the season and air mass type and we provide a chemical composition of the aerosol as a function of each of these environmental factors.  相似文献   

19.
This paper presents samples of Saharan dust outbreak affecting the Mediterranean Tunisian coasts and its impact on PM10 (Particles with an aerodynamic diameter below 10 µm) surface concentrations measured at seven monitoring stations during summer 2006. During the events, the daily PM10 levels at all stations exceeded EU and Tunisian air quality standard limits which are equal to 50 µg/m3. The maximum values ranged from 200 µg/m3 to 300 µg/m3 depending on the monitoring station. The impact is even more dramatic on PM10 hourly concentrations leading to maximum hourly peaks ranging from 400 µg/m3 to 850 µg/m3 again depending on the monitoring station (industrial or residential, traffic and commercial). Comparison between backward air masses trajectories reaching Tunisian coasts and satellite imageries vis-à-vis the PM10 hourly concentrations measured at the monitoring stations during 2006 evidenced the influence of the Saharan dust outbreaks on surface concentrations. The origin of the air masses is found to be from South-West direction under the influence of air masses from the Algerian Saharan desert.  相似文献   

20.
In situ aircraft measurements of O3, CO,HNO3, and aerosol particles are presented,performed over the North Sea region in the summerlower stratosphere during the STREAM II campaign(Stratosphere Troposphere Experiments by AircraftMeasurements) in July 1994. Occasionally, high COconcentrations of 200-300 pbbv were measured in thelowermost stratosphere, together with relatively highHNO3 concentrations up to 1.6 ppbv. The particlenumber concentration (at standard pressure andtemperature) between 0.018-1 m decreased acrossthe tropopause, from >1000 cm-3 in the uppertroposphere to <500 cm-3 in the lowermoststratosphere. Since the CO sources are found in thetroposphere, the elevated CO mixing ratios areattributed to mixing of polluted tropospheric air intothe lowermost extratropical stratosphere. Further wehave used a chemical model to illustrate that nitrogenoxide reservoir species (mainly HNO3) determinethe availability of NOx (=NO + NO2) andtherefore largely control the total net O3production in the lower kilometers of thestratosphere. Model simulations, applying additionalNOx perturbations from aircraft, show that theO3 production efficiency of NOx is smallerthan previously assumed, under conditions withrelatively high HNO3 mixing ratios, as observedduring STREAM II. The model simulations furthersuggest a relatively high O3 productionefficiency from CO oxidation, as a result of therelatively high ambient HNO3 and NOxconcentrations, implying that upward transport of COrich air enhances O3 production in the lowermoststratosphere. Analysis of the measurements and themodel calculations suggest that the lowermoststratosphere is a transition region in which thechemistry deviates from both the upper troposphere andlower stratosphere.  相似文献   

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