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1.
Analyses of cloud condensation nuclei (CCN) number concentrations (cm− 3) measured at the Mace Head Atmospheric Research Station, near Carna, County Galway, Ireland, using a DH Associates Model M1 static thermal diffusion cloud chamber over the period from March 1994 to September 2002 are presented in this work. Air masses are defined as being ‘marine’ if they originate from a wind direction of 180–300° and ‘continental’ air masses are defined as originating from a wind direction of 45–135°. Air masses without such filtering were classified as ‘undefined’ air masses. Air masses were found to be dominated by marine sector air, re-affirming Mace Head as a baseline atmospheric research station. CCN levels for specific air masses at Mace Head were found to be comparable with earlier studies both at Mace Head and elsewhere. Monthly averaged clean marine (wind direction of 180–300° and black carbon absorption coefficient < 1.425 Mm− 1) CCN and marine CCN varied between 15–247 cm− 3 and 54–670 cm− 3, respectively. As expected, significant increases in number concentration were found in continentally sourced CCN over that of marine CCN and were found to follow a log-normal distribution significantly tighter than that of clean marine air masses. No significant trend was found for CCN over the 9-year period. While polluted continental air masses showed a slight increase in CCN concentrations over the winter months, most likely due to increased fuel usage and a lower mixed boundary layer, the dominance of marine sector air arriving at Mace Head, which generally consists of background CCN concentrations, reduced seasonal differences for polluted air. Marine air showed a distinct seasonal pattern, with elevated values occurring over the spring and summer seasons. This is thought to be due to enhanced biogenic aerosol production as a result of phytoplankton bloom activity in the North Atlantic.  相似文献   

2.
The chemistry of glycolaldehyde (hydroxyacetaldehyde) relevant to the troposphere has been investigated using UV absorption spectrometry and FTIR absorption spectrometry in an environmental chamber. Quantitative UV absorption spectra have been obtained for the first time. The UV spectrum peaks at 277 nm with a maximum cross section of (5.5± 0.7)×10–20 cm2 molecule–1. Studies of the ultraviolet photolysis of glycolaldehyde ( = 285 ± 25 nm) indicated that the overall quantum yield is > 0.5 in one bar of air, with the major products being CH2OH and HCO radicals. Rate coefficients for the reactions of Cl atoms and OH radicals with glycolaldehyde have been determined to be (7.6± 1.5)×10–11 and (1.1± 0.3)×10–11 cm3 molecule–1 s–1, respectively, in good agreement with the only previous study. The lifetime of glycolaldehyde in the atmosphere is about 1.0 day for reaction with OH, and > 2.5 days for photolysis, although both wet and dry deposition should also be considered in future modeling studies.  相似文献   

3.
Barnes  I.  Bastian  V.  Becker  K. H.  Fink  E. H.  Nelsen  W. 《Journal of Atmospheric Chemistry》1986,4(4):445-466
The reactions of OH radicals with SO2, H2S, thiophenol, and a series of aliphatic thiols (1–5 C-atoms) have been investigated in 201 and 381 reaction chambers at 1 atm total pressure and 300 K using a competitive kinetic technique. Initially, OH radicals were produced by photolysis of CH3ONO/NO mixtures in air. Applying this OH source rate constants for OH with SO2, H2S, and thiophenol in synthetic air were determined to be (1.1±0.2)×10-12, (5.5±0.8)×10-12 and (1.1±0.2)×10-11 cm3 s-1, respectively. However, when this method was applied to the aliphatic thiols the rate constants obtained were found to be dependent on the partial pressures of O2 and NO. These effects have been attributed to the built-up of a radical species, not yet identified, which leads to uncontrolled chain reactions in the system. Using the photolysis of H2O2 at wavelengths greater than 260 nm as the OH source in 1 atm N2, rate constants for the 1–5 aliphatic thiols in the range 2.9 to 5.6×10-11 cm3 s-1 were obtained. The rate constants obtained in the present study are compared with recent literature values.  相似文献   

4.
Rate constants for the gas-phase reactions of OH radicals with nopinone (6,6-dimethylbicyclo[3.1.1]heptan-2-one) and camphenilone (3,3-dimethylbicyclo[2.2.1]heptan-2-one) and for the reactions of 4-acetyl-1-methylcyclohexene with OH and NO3 radicals and O3 have been measured at 296±2 K. The rate constants (cm3 molecule–1 s–1 units) obtained were, for reaction with the OH radical: nopinone, (1.43±0.37)×10–11; camphenilone, (5.15±1.44)×10–12; and 4-acetyl-1-methylcyclohexene, (1.29±0.33)×10–10; for reaction with the NO3 radical: 4-acetyl-1-methylcyclohexene, (1.05±0.38)×10–11; and for reaction with O3: 4-acetyl-1-methylcyclohexene, (1.50±0.53)×10–16. These data are used to calculate the tropospheric lifetimes of these monoterpene atmospheric reaction products.  相似文献   

5.
The reaction of Cl with cyclohexanone (1) was investigated, for the first time, as a function of temperature (273–333 K) and at a low total pressure (1 Torr) with helium as a carrier gas using a discharge flow-mass spectrometry technique (DF-MS). The resulting Arrhenius expression is proposed, k 1= (7.7 ± 4.1) × 10–10 exp[–(540 ± 169)/T]. We also report a mechanistic study with the quantitative determination of the products of the reaction of Cl with cyclohexanone. The absolute rate constant derived from this study at 1 Torr of total pressure and room temperature is (1.3 ± 0.2) × 10–10 cm3 molecule–1 s–1. A yield of 0.94 ± 0.10 was found for the H-abstraction channel giving HCl. In relative studies, using a newly constructed relative rate system, the decay of cyclohexanone was followed by gas chromatography coupled with flame-ionisation detection. These relative measurements were performed at atmospheric pressure with synthetic air and room temperature. Rate constant measured using the relative method for reaction (1) is: (1.7 ± 0.3) × 10–10 cm3 molecule–1 s–1. Finally, results and atmospheric implications are discussed and compared with the reactivity with OH radicals.  相似文献   

6.
A novel method has been examined for monitoring tropospheric hydroxyl radicals (OH), the most important oxidant in tropospheric chemistry. Aqueous phase salicylic acid reacts with atmospheric OH to produce 2,5-dihydroxy benzoic acid (2,5-DHBA) and other products. High Performance Liquid Chromatography (HPLC) is used to separate the post-reaction solution and the products are quantified using fluorescence detection. Unlike other methods, it has been reported to be inexpensive, portable and relatively simple. Although the sensitivity was sufficient to measure typical daytime OH concentrations of 0.04–0.4 ppt., the method was hindered by numerous interferences. Successive identification and elimination of these still resulted in a signal that was much larger than expected. Tests showed that this was not likely to be due to ozone, HO2, NOx, H2O2, aerosols, light or bacteria. Experimental and numerical studies suggest that the interference could be due to methyl peroxy radicals. The effect of many other components in the atmosphere, both individual and combined, must also be tested before the method can be used reliably in the field. The validity of previous reports of ambient hydroxyl measurements using this technique is therefore brought into question.  相似文献   

7.
A new version of an atmospheric pressure chemical ionisation mass spectrometer has been developed for ground based in situ atmospheric measurements of OH and total peroxy (HO2 + organic peroxy) radicals. Based on the previously developed principle of chemical conversion of OH radicals to H2SO4 in reaction with SO2 and detection of H2SO4 using an ion molecule reaction with NO3─, the new instrument is equipped with a turbulent chemical conversion reactor allowing for measurements in moderately polluted atmosphere at NO concentrations up to several ppb. Unlike other similar devices, where the primary NO3─ ions are produced using radioactive ion sources, the new instrument is equipped with a specially developed corona discharge ion source. According to laboratory measurements, the overall accuracy and detection limits are estimated to be, respectively, 25% and 2 × 105 molecule cm-3 for OH and 30% and 1 × 105 molecule cm-3 for HO2 at 10 min integration times. The detection limit for measurements of OH radicals under polluted conditions is 5 × 105 molecules cm-3 at 10 min integration times. Examples of ambient air measurements during a field campaign near Paris in July 2007 are presented demonstrating the capability of the new instrument, although with reduced performance due to the employment of non isotopic SO2.  相似文献   

8.
Rate constants for the gas-phase reactions of OH radicals, NO3 radicals and O3 with the C7-carbonyl compounds 4-methylenehex-5-enal [CH2=CHC(=CH2)CH2CH2CHO], (3Z)- and (3E)-4-methylhexa-3,5-dienal [CH2=CHC(CH3)=CHCH2CHO] and 4-methylcyclohex-3-en-1-one, which are products of the atmospheric degradations of myrcene, Z- and E-ocimene and terpinolene, respectively, have been measured at 296 ± 2 K and atmospheric pressure of air using relative rate methods. The rate constants obtained (in cm3 molecule–1 s–1 units) were: for 4-methylenehex-5-enal, (1.55 ± 0.15) × 10–10, (4.75 ± 0.35) × 10–13 and (1.46 ± 0.12) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively; for (3Z)-4-methylhexa-3,5-dienal: (1.61 ± 0.35) × 10–10, (2.17 ± 0.30) × 10–12, and (4.13 ± 0.81) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively; for (3E)-4-methylhexa-3,5-dienal: (2.52 ± 0.65) × 10–10, (1.75 ± 0.27) × 10–12, and (5.36 ± 0.28) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively; and for 4-methylcyclohex-3-en-1-one: (1.10 ± 0.19) × 10–10, (1.81 ± 0.35) × 10–12, and (6.98 ± 0.40) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively. These carbonyl compounds are all reactive in the troposphere, with daytime reaction with the OH radical and nighttime reaction with the NO3 radical being predicted to dominate as loss processes and with estimated lifetimes of about an hour or less.  相似文献   

9.
Three independent methods have been used to sort the ozone, carbonmonoxide, and other radiatively important trace gases measured at Mace Head,Ireland, and thereby distinguish clean air masses transported over the NorthAtlantic from the more polluted air masses which have recently travelledfrom the European continent. Over the period April 1987–June 1995 theNorthern Hemisphere surface ozone baseline concentrations exhibited a meanconcentration of 34.8 ppb, with a small positive trend (+0.19 ppbyr-1), while the corresponding trend in air originating fromthe polluted European areas was negative (–0.39 ppbyr-1). Carbon monoxide measurements from March 1990 toDecember 1994 showed negative trends for both the unpolluted (–0.17ppb yr-1) and polluted data (–13.6 ppbyr-1). Overall the continent of Europe was shown to be a smallnet sink of 2.6 ppb for all occasions when European air was transported tothe North Atlantic.  相似文献   

10.
The absolute rate constants for the gas-phasereactions of the NO3 radical with a series ofaldehydes such as acetaldehyde, propanal, butanal,pentanal, hexanal and, heptanal were measured overthe temperature range 298–433 K, using a dischargeflow system and monitoring the NO3 radical byLaser Induced Fluorescence (LIF).The measured rate constants at 298 K for thereaction of NO3, in units of 10–14 cm3molecule–1 s–1, were as follows:acetaldehyde 0.32 ± 0.04, propanal 0.60 ± 0.06, butanal 1.46± 0.16, pentanal 1.75 ±0.06, hexanal 1.83 ± 0.36, and heptanal 2.37 ±0.42. The proposed Arrhenius expressions arek1 = (6.2 ± 7.5) × 10–11 exp[–(2826 ± 866)/T] (cm3 molecule–1s–1),k2 = (1.7 ± 1.0) × 10–11 exp[–(2250 ± 192)/T] (cm3 molecule–1s1), k3 =(7.6 ± 9.8) × 1011 exp[–(2466 ± 505)/T] (cm3 molecule–1s–1),k4 = (2.8 ± 1.4) × 10–11 exp[–(2189 ± 156)/T] (cm3 molecule–1s–1), k5 = (7.0 ± 1.8) ×10–11 exp [–(2382 ± 998)/T](cm3 molecule–1 s–1), andk6 = (7.8 ± 1.0) × 10–11 exp[–(2406 ± 481)/T](cm3 molecule–1 s–1).Tropospheric lifetimes for these aldehydes werecalculated at night and during the day for typicalNO3 and OH average concentrations and showed thatboth radicals provide an effective tropospheric sinkfor these compounds and that the night-time reactionwith the NO3 radical can be an important, if notdominant, loss process for these emitted organics andfor NO3 radicals.  相似文献   

11.
Absolute rate coefficient measurements have been carried out for the reactions of Cl atoms with propene and a series of 3-halopropenes, at room temperature (298 ± 2) K using a newly constructed laser photolysis-resonance fluorescence (PLP-RF) system. The rate coefficients obtained (in units of cm3 molecule–1 s–1) are: propene (1.40± 0.24) ×10–10, 3-fluoropropene (4.92 ± 0.42) ×10–11, 3-chloropropene (7.47 ± 1.50) × 10–11, 3-bromopropene (1.23± 0.14) ×10–10 and 3-iodopropene (1.29± 0.15) ×10–10. In order to test this new system, the reactions of Cl atoms with acetone and isoprene have also been studied and compared with data previously reported. The rate coefficients determined at room temperature for these last two reactions are (2.93 ± 0.20) ×10–12 cm3 molecule–1 s– 1 and (3.64± 0.20)×10–10 cm3 molecule–1 s–1, respectively. The measured values were independent of pressure over the range 20–200 Torr. The influence of the different halogen atoms substituents on the reactivity of these alkenes with Cl atoms as well as the atmospheric implications of these measurements are studied and discussed for the first time in this work and compared with the reactivity with NO3 and OH radicals.  相似文献   

12.
A global three-dimensional model of the tropospheric sulfur cycle   总被引：9，自引：0，他引：9  
The tropospheric part of the atmospheric sulfur cycle has been simulated in a global three-dimensional model. The model treats the emission, transport, chemistry, and removal processes for three sulfur components; DMS (dimethyl sulfide), SO2 and SO4 2– (sulfate). These processes are resolved using an Eulerian transport model, the MOGUNTIA model, with a horizontal resolution of 10° longitude by 10° latitude and with 10 layers in the vertical between the surface and 100 hPa. Advection takes place by climatological monthly mean winds. Transport processes occurring on smaller space and time scales are parameterized as eddy diffusion except for transport in deep convective clouds which is treated separately. The simulations are broadly consistent with observations of concentrations in air and precipitation in and over polluted regions in Europe and North America. Oxidation of DMS by OH radicals together with a global emission of 16 Tg DMS-S yr–1 from the oceans result in DMS concentrations consistent with observations in the marine boundary layer. The average turn-over times were estimated to be 3, 1.2–1.8, and 3.2–6.1 days for DMS, SO2, and SO4 2– respectively.  相似文献   

13.
The 1,4-hydroxycarbonyl 5-hydroxy-2-pentanone is an important product of the gas-phase reaction of OH radicals with n-pentane in the presence of NO. We have used a relative rate method with 4-methyl-2-pentanone as the reference compound to measure the rate constant for the reaction of OH radicals with 5-hydroxy-2-pentanone at 296 ± 2 K. The carbonyls were sampled by on-fiber derivatization using a Solid Phase Micro Extraction (SPME) fiber coated with O> -(2,3,4,5,6-pentafluorobenzyl)hydroxylamine hydrochloride with subsequent thermal desorption of the oxime derivatives and quantification by gas chromatography with flame ionization detection. For comparison, the reference compound was also analyzed following sample collection onto a Tenax adsorbent cartridge. Products of the reaction were investigated using coated-fiber SPME sampling with gas chromatography-mass spectrometry analysis as well as by using in situ atmospheric pressure ionization mass spectrometry. A rate constant for the reaction of OH radicals with 5-hydroxy-2-pentanone of (1.6 ± 0.4) × 10–11 cm3 molecule–1 s–1 was obtained at 296 ± 2 K. Two dicarbonyl products, of molecular weight 86 and 100, were observed and are attributed to CH3C(O)CH2CHO and CH3C(O)CH2CH2CHO, respectively. Reaction schemes leading to these products are presented.  相似文献   

14.
Surface measurements of cloud condensation nuclei (CCN) number concentration (cm−3) are presented for unmodified marine air and for polluted air at Mace Head, for the years 1994 and 1995. The CCN number concentration active at 0.5% supersaturation is found to be approximately log-normal for marine and polluted air at the site. Values of geometric mean, median and arithmetic mean of CCN number concentration (cm−3) for marine air are in the range 124–135, 140–150 and 130–157 for the two years of data. Analysis of CCN number concentration for high wind speed, U, up to 20 m s−1 show enhanced CCN production for U in excess of about 10–12 m s−1. Approximately 7% increase in CCN per 1 m s−1 increase in wind speed is found, up to 17 m s−1. A relationship of the form log10CCN=a+bU is obtained for the periods March 1994 and January, February 1995 for marine air yielding values a of 1.70; 1.90 and b of 0.035 for both periods.  相似文献   

15.
A combined study of the OH gas phase reaction and uptake on aqueous surfacesof two carbonates, dimethyl and diethyl carbonate has been carried out todetermine the atmospheric lifetimes of these compounds. Rate coefficients havebeen measured for gas phase reactions of OH radicals with dimethyl and diethylcarbonate. The experiments were carried out using pulsed laser photolysis– laser induced fluorescence over the temperature range 263–372K and the kinetic data were used to derive the following Arrhenius expressions(in units of cm3 molecule–1 s–1):for dimethyl carbonate, k1 = (0.83±0.27)×10–12 exp [–(247± 98)/T] and fordiethyl carbonate, k2 = (0.46±0.15)×10–12 exp [(503± 203)/T]. At 298 K, therate coefficients obtained (in units of 10–12 cm3molecule–1 s–1) are: k1 =(0.35± 0.04) and k2 = (2.31± 0.29). The results arediscussed in terms of structure-activity relationships.The uptake coefficients of both carbonates on aqueous surfaces were measuredas a function of temperature and composition of the liquid phase, using thedroplet train technique coupled to a mass spectrometric detection. Dimethyland diethyl carbonate show very similar results. For both carbonates, themeasured uptake kinetics were found to be independent of the aqueous phasecomposition (pure water, NaOH solutions) but dependent on gas-liquid contacttime which characterises a surface saturation effect. The uptake coefficientvalues show a slight negative temperature dependence for both carbonates.These values vary from 1.4×10–2 to0.6×10–2 in the temperature range of 265–279 Kfor dimethyl carbonate, from 2.4×10–2 to0.9×10–2 in the temperature range of 270–279 Kfor diethyl carbonate. From the kinetic data, the following Henry's lawconstants were derived between 279 and 265 K: dimethyl carbonate,H1 = 20–106 M atm–1; and diethyl carbonate,H2 = 30–98 M atm–1. The reported data showthat the OH reaction is the major atmospheric loss process of these twocarbonates with lifetimes of 33 and 5 days, respectively, while the wetdeposition is a negligible process.  相似文献   

16.
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   

17.
The following temperature-dependent rate coefficients (k/cm3 molecule–1 s–1) of the reactions of hydroxyl radicals with aliphatic ethers have been determined over the temperature range 247–373 K by a competitive flow technique: diethyl ether,k OH=5.2×10–12 exp[(262±150)/T]; methyln-butyl ether,k OH=5.4×10–12 exp[(309±150)/T]; ethyln-butyl ether,k OH=7.3×10–12 exp[(335±150)/T]; di-n-butyl ether,k OH=5.5×10–12 exp[(502±150)/T] and di-n-pentyl ether,k OH=8.5×10–12 exp[(417±150)/T]. The data have been measured relative to the rate coefficientk(OH + 2,3-dimethylbutane)=6.2×10–12 cm3 molecule–1 s–1 independent of temperature.Previous discrepancies in the room-temperature rate coefficients for the OH reactions with ethyln-butyl ether and di-n-butyl ether, obtained in the flow and static experiments of Bennett and Kerr (J. Atmos. Chem. 8, 87–94, 1989;10, 29–38, 1990) compared with those of Wallingtonet al. (Int. J. Chem. Kinet. 20, 541–547, 1988;21, 993–1001, 1989) and of Nelsonet al. (Int. J. Chem. Kinet. 22, 1111–1126, 1990) have been resolved. The results are considered in relation to the available literature data and evaluated rate expressions are deduced where possible. The data are also discussed in terms of structure-activity relationships.  相似文献   

18.
Airborne measurements of volatile organic compounds (VOC) were performed overthe tropical rainforest in Surinam (0–12 km altitude,2°–7° N, 54°–58° W) using the proton transferreaction mass spectrometry (PTR-MS) technique, which allows online monitoringof compounds like isoprene, its oxidation products methyl vinyl ketone,methacrolein, tentatively identified hydroxy-isoprene-hydroperoxides, andseveral other organic compounds. Isoprene volume mixing ratios (VMR) variedfrom below the detection limit at the highest altitudes to about 7 nmol/molin the planetary boundary layer shortly before sunset. Correlations betweenisoprene and its product compounds were made for different times of day andaltitudes, with the isoprene-hydroperoxides showing the highest correlation.Model calculated mixing ratios of the isoprene oxidation products using adetailed hydrocarbon oxidation mechanism, as well as the intercomparisonmeasurement with air samples collected during the flights in canisters andlater analysed with a GC-FID, showed good agreement with the PTR-MSmeasurements, in particular at the higher mixing ratios.Low OH concentrations in the range of 1–3 × 105molecules cm-3 averaged over 24 hours were calculated due to lossof OH and HO2 in the isoprene oxidation chain, thereby stronglyenhancing the lifetime of gases in the forest boundary layer.  相似文献   

19.
Rate constants for the reaction of OH radicals with some branched alkyl nitrates have been measured applying a competitive technique. Methyl nitrite photolysis in synthetic air was used as OH radical source at 295±2 K and 1000 mbar total pressure. Using a rate constant of 2.53×10-12 cm3 s-1 for the reaction of OH radicals with n-butane as reference, the following rate constants were obtained (units: 10-12 cm3 s-1): isopropyl nitrate, 0.59±0.22; isobutyl nitrate, 1.63±0.20; 3-methyl-2-butyl nitrate, 1.95±0.15; 2-methyl-1-butyl nitrate, 2.50±0.15; 3-methyl-1-butyl nitrate, 2.55±0.35. These values have been combined with the literature data to recalculate the substituent factors F(X) for the different nitrate groups which can be used to predict OH rate constants for organic nitrates for which experimental data are not available.Preliminary measurements of the photolysis frequency of isopropyl nitrate have shown that for this nitrate as a model substance, OH reactions and direct photolysis are of equal importance under tropospheric conditions.  相似文献   

20.
Aerosol chemical composition and trace gas measurements were made at twolocations on the northeastern peninsula of Tenerife during the ACE-2HILLCLOUD experiment, between 28 June and 23 July 1997. Measurementswere made of coarse (#gt;2.5 m aerodynamic diameter) and fine (#lt; 2.5m) aerosol Cl–, NO3 –,SO4 2–, non-sea saltSO4 2– (NSSS),CH3SO3 – (MSA) andNH4 +, and gas phase dimethylsulphide (DMS), HCl,HNO3, SO2, CH3COOH, HCOOH andNH3. Size distributions were measured using a cascadeimpactor. Results show that in marine air masses NSSS and MSA wereformed via DMS oxidation, with additional NSSS present in air massescontaining a continental component. Using a Eulerian box model approachfor aerosols transported between upwind and downwind sites, a mean NSSSproduction rate of 4.36 × 10–4 gm–3 s–1 was calculated for daytimeclear sky periods (highest insolation), with values for cloudy periodsduring daytime and nighttime of 3.55 × 10–4 and2.40 × 10–4 g m–3s–1, respectively. The corresponding rates for MSA were6.23 × 10–6, 8.49 × 10–6and 6.95 × 10–6 g m–3s–1, respectively. Molar concentration ratios forMSA/NSSS were 8.7% (1.8–18.2%) and 1.9%(1.3–3.5%) in clean and polluted air masses, respectively.Reactions occurring within clouds appeared to have a greater influenceon rates of MSA production, than of NSSS, while conversely daytime gasphase reactions were more important for NSSS. For MSA, nighttimein-cloud oxidation rates exceeded rates of daytime gas phase productionvia OH oxidation of DMS. NSSS, MSA and ammonium had trimodal sizedistributions, with modes at 0.3, 4.0 and >10.0 m (NSSS andNH4 +), and 0.3, 1.5 and 4.0 m (MSA). Nosignificant production of other aerosol species was observed, with theexception of ammonium, which was formed at variable rates dependent onneutralisation of the aerosol with ammonia released from spatiallynon-uniform surface sources. Seasalt components were mainly present incoarse particles, although sub-micrometre chloride was also measured.Losses by deposition exceeded calculated expectations for all species,and were highest for the seasalt fraction and nitrate.  相似文献   

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