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1.
Ocean emissions of inorganic and organic iodine compounds drive the biogeochemical cycle of iodine and produce reactive ozone-destroying iodine radicals that influence the oxidizing capacity of the atmosphere. Di-iodomethane (CH2I2) and chloro-iodomethane (CH2ICl) are the two most important organic iodine precursors in the marine boundary layer. Ship-borne measurements made during the TORERO (Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated VOC) field campaign in the east tropical Pacific Ocean in January/February 2012 revealed strong diurnal cycles of CH2I2 and CH2ICl in air and of CH2I2 in seawater. Both compounds are known to undergo rapid photolysis during the day, but models assume no night-time atmospheric losses. Surprisingly, the diurnal cycle of CH2I2 was lower in amplitude than that of CH2ICl, despite its faster photolysis rate. We speculate that night-time loss of CH2I2 occurs due to reaction with NO3 radicals. Indirect results from a laboratory study under ambient atmospheric boundary layer conditions indicate a k CH2I2+NO3 of ≤4 × 10?13 cm3 molecule?1 s?1; a previous kinetic study carried out at ≤100 Torr found k CH2I2+NO3 of 4 × 10?13 cm3 molecule?1 s?1. Using the 1-dimensional atmospheric THAMO model driven by sea-air fluxes calculated from the seawater and air measurements (averaging 1.8 +/? 0.8 nmol m?2 d?1 for CH2I2 and 3.7 +/? 0.8 nmol m?2 d?1 for CH2ICl), we show that the model overestimates night-time CH2I2 by >60 % but reaches good agreement with the measurements when the CH2I2 + NO3 reaction is included at 2–4 × 10?13 cm3 molecule?1 s?1. We conclude that the reaction has a significant effect on CH2I2 and helps reconcile observed and modeled concentrations. We recommend further direct measurements of this reaction under atmospheric conditions, including of product branching ratios.  相似文献   

2.
During the POPCORN campaign between 3 and 24 August 1994 we measured peroxyacetyl nitrate (PAN) in a rural area of Mecklenburg-Vorpommern (North-Eastern Germany) above a corn field. A total of about 5000 PAN measurements were carried out within the three weeks of the campaign. Measured PAN mixing ratios ranged from below the detection limit of 10 ppt up to an afternoon maximum of 1 ppb. The mean value of all data was 140 ppt. The daily mean PAN mixing ratios were typically in the range of 50 to 250 ppt, but during a clean air episode PAN mixing ratios of well below 40 ppt were observed. The characteristic relative diurnal variation of the PAN mixing ratios with a late night/early morning minimum and an afternoon maximum persisted during these episodes. The daily averages of the PAN mixing ratios showed clear episodic variations which coincided with the duration of typical synoptic episodes of two to six days duration. Based on the measurements of the various parameters determining the PAN formation and destruction rates, the local budget for PAN was calculated. During daytime the calculated net photochemical formation rate of PAN was nearly always significantly higher than the observed change of the PAN concentration. This demonstrates that substantial amounts of PAN (often in the range of several hundred ppt/h) were exported from the corn field. The resulting removal of NOx to some extent effects the budget of nitrogen oxides (NOx), but the export of odd oxygen radicals in the form of PAN during daytime often amounted up to 30–50% of the OH-radical formation by ozone photolysis. Thus the importance of PAN as reservoir and transport medium for odd oxygen radicals can be very substantial and may have a significant impact on the budget and distribution of odd oxygen radicals.  相似文献   

3.
A detailed climatology of the cyclogenesis over the Southern Atlantic Ocean (SAO) from 1990 to 1999 and how it is simulated by the RegCM3 (Regional Climate Model) is presented here. The simulation used as initial and boundary conditions the National Centers for Environmental Prediction—Department of Energy (NCEP/DOE) reanalysis. The cyclones were identified with an automatic scheme that searches for cyclonic relative vorticity (ζ10) obtained from a 10-m height wind field. All the systems with ζ10 ≤ ?1.5 × 10?5 s?1 and lifetime equal or larger than 24 h were considered in the climatology. Over SAO, in 10 years were detected 2,760 and 2,787 cyclogeneses in the simulation and NCEP, respectively, with an annual mean of 276.0 ± 11.2 and 278.7 ± 11.1. This result suggests that the RegCM3 has a good skill to simulate the cyclogenesis climatology. However, the larger model underestimations (?9.8%) are found for the initially stronger systems (ζ10 ≤ ?2.5 × 10?5 s?1). It was noted that over the SAO the annual cycle of the cyclogenesis depends of its initial intensity. Considering the systems initiate with ζ10 ≤ ?1.5 × 10?5 s?1, the annual cycle is not well defined and the higher frequency occurs in the autumn (summer) in the NCEP (RegCM3). The stronger systems (ζ10 ≤ ?2.5 × 10?5 s?1) have a well-characterized high frequency of cyclogenesis during the winter in both NCEP and RegCM3. This work confirms the existence of three cyclogenetic regions in the west sector of the SAO, near the South America east coast and shows that RegCM3 is able to reproduce the main features of these cyclogenetic areas.  相似文献   

4.
A systematic comparison of wind profiles and momentum exchange at a trade wind site outside Oahu, Hawaii and corresponding data from the Baltic Sea is presented. The trade wind data are to a very high degree swell dominated, whereas the Baltic Sea data include a more varied assortment of wave conditions, ranging from a pure growing sea to swell. In the trade wind region swell waves travel predominantly in the wind direction, while in the Baltic, significant cross-wind swells are also present. Showing the drag coefficient as a function of the 10-m wind speed demonstrates striking differences for unstable conditions with swell for the wind-speed range 2 m s?1 < U 10 < 7 m s?1, where the trade-wind site drag values are significantly larger than the corresponding Baltic Sea values. In striking contrast to this disagreement, other features studied are surprisingly similar between the two sites. Thus, exactly as found previously in Baltic Sea studies during unstable conditions and swell, the wind profile in light winds (3 m s?1) shows a wind maximum at around 7–8 m above the water, with close to constant wind speed above. Also, for slightly higher wind speeds (4 m s?1 < U 10 < 7 m s?1), the similarity between wind profiles is striking, with a strong wind-speed increase below a height of about 7–8 m followed by a layer of virtually constant wind speed above. A consequence of these wind-profile features is that Monin–Obukhov similarity is no longer valid. At the trade-wind site this was observed to be the case even for wind speeds as high as 10 m s?1. The turbulence kinetic energy budget was evaluated for four cases of 8–16 30- min periods at the trade-wind site, giving results that agree very well with corresponding figures from the Baltic Sea.  相似文献   

5.
Turbulent fluxes of sensible and latent heat and ozone were measured aboard a German Aerospace Research Establishment motorglider over the Swiss Plateau during the first field experiment of the Swiss air pollution experiment POLLUMET. In the lower part of the boundary layer, the ozone fluxes are negative (downward) throughout the day as a result of deposition and photochemical destruction at the surface. In the upper part of the boundary layer, the ozone fluxes tend to be negative until mid-afternoon and then become positive. The change in sign occurs after the ozone concentration in the boundary layer exceeds that in the reservoir above the inversion. Downdrafts bringing air parcels with ozone deficits across the inversion then become major contributors to the flux. The positive fluxes at upper levels result in an increase in flux divergence in mid-afternoon that is balanced by a relatively large source term in the ozone concentration budget.  相似文献   

6.
The use of high resolution atmosphere–ocean coupled regional climate models to study possible future climate changes in the Mediterranean Sea requires an accurate simulation of the atmospheric component of the water budget (i.e., evaporation, precipitation and runoff). A specific configuration of the version 3.1 of the weather research and forecasting (WRF) regional climate model was shown to systematically overestimate the Mediterranean Sea water budget mainly due to an excess of evaporation (~1,450 mm yr?1) compared with observed estimations (~1,150 mm yr?1). In this article, a 70-member multi-physics ensemble is used to try to understand the relative importance of various sub-grid scale processes in the Mediterranean Sea water budget and to evaluate its representation by comparing simulated results with observed-based estimates. The physics ensemble was constructed by performing 70 1-year long simulations using version 3.3 of the WRF model by combining six cumulus, four surface/planetary boundary layer and three radiation schemes. Results show that evaporation variability across the multi-physics ensemble (～10 % of the mean evaporation) is dominated by the choice of the surface layer scheme that explains more than ～70 % of the total variance and that the overestimation of evaporation in WRF simulations is generally related with an overestimation of surface exchange coefficients due to too large values of the surface roughness parameter and/or the simulation of too unstable surface conditions. Although the influence of radiation schemes on evaporation variability is small (～13 % of the total variance), radiation schemes strongly influence exchange coefficients and vertical humidity gradients near the surface due to modifications of temperature lapse rates. The precipitation variability across the physics ensemble (～35 % of the mean precipitation) is dominated by the choice of both cumulus (～55 % of the total variance) and planetary boundary layer (～32 % of the total variance) schemes with a strong regional dependence. Most members of the ensemble underestimate total precipitation amounts with biases as large as 250 mm yr?1 over the whole Mediterranean Sea compared with ERA Interim reanalysis mainly due to an underestimation of the number of wet days. The larger number of dry days in simulations is associated with a deficit in the activation of cumulus schemes. Both radiation and planetary boundary layer schemes influence precipitation through modifications on the available water vapor in the boundary layer generally tied with changes in evaporation.  相似文献   

7.
The distribution of the mean oceanic oxygen concentration results from a balance between ventilation and consumption. In the eastern tropical Pacific and Atlantic, this balance creates extended oxygen minimum zones (OMZ) at intermediate depth. Here, we analyze hydrographic and velocity data from shipboard and moored observations, which were taken along the 23°W meridian cutting through the Tropical North East Atlantic (TNEA) OMZ, to study the distribution and generation of oxygen variability. By applying the extended Osborn–Cox model, the respective role of mesoscale stirring and diapycnal mixing in producing enhanced oxygen variability, found at the southern and upper boundary of the OMZ, is quantified. From the well-ventilated equatorial region toward the OMZ core a northward eddy-driven oxygen flux is observed whose divergence corresponds to an oxygen supply of about 2.4 μmol kg?1 year?1 at the OMZ core depth. Above the OMZ core, mesoscale eddies act to redistribute low- and high-oxygen waters associated with westward and eastward currents, respectively. Here, absolute values of the local oxygen supply >10 μmol kg?1 year?1 are found, likely balanced by mean zonal advection. Combining our results with recent studies, a refined oxygen budget for the TNEA OMZ is derived. Eddy-driven meridional oxygen supply contributes more than 50 % of the supply required to balance the estimated oxygen consumption. The oxygen tendency in the OMZ, as given by the multidecadal oxygen decline, is maximum slightly above the OMZ core and represents a substantial imbalance of the oxygen budget reaching about 20 % of the magnitude of the eddy-driven oxygen supply.  相似文献   

8.
The oxidation of nonmethane hydrocarbons represents a source of tropospheric ozone that is primarily confined to the boundary layers of several highly industrialized regions. (Each region has an area greater than one million km2). Using a photochemical model, the global tropospheric ozone budget is reexamined by including the in-situ production from these localized regimes. The results from these calculations suggest that the net source due to this photochemistry, which takes place on the synoptic scale, is approximately as large as the amount calculated for global scale photochemical processes which consider only the oxidation of methane and carbon monoxide. Such a finding may have a considerable impact on our understanding of the tropospheric ozone budget. The model results for ozone show reasonable agreement with the climatological summer distribution of ozone and the oxides of nitrogen at the surface and with the vertical distribution of ozone and nonmethane hydrocarbons obtained during a 1980 field program.  相似文献   

9.
Summary The boundary-layer structure of the Elqui Valley is investigated, which is situated in the arid north of Chile and extends from the Pacific Ocean in the west to the Andes in the east. The climate is dominated by the south-eastern Pacific subtropical anticyclone and the cold Humboldt Current. This combination leads to considerable temperature and moisture gradients between the coast and the valley and results in the evolution of sea and valley wind systems. The contribution of these mesoscale wind systems to the heat and moisture budget of the valley atmosphere is estimated, based on radiosoundings performed near the coast and in the valley. Near the coast, a well-mixed cloud-topped boundary layer exists. Both, the temperature and the specific humidity do not change considerably during the day. In the stratus layer the potential temperature increases, while the specific humidity decreases slightly with height. The top of the thin stratus layer, about 300 m in depth, is marked by an inversion. Moderate sea breeze winds of 3–4 m s−1 prevail in the sub-cloud and cloud layer during daytime, but no land breeze develops during the night. The nocturnal valley atmosphere is characterized by a strong and 900 m deep stably stratified boundary layer. During the day, no pronounced well-mixed layer with a capping inversion develops in the valley. Above a super-adiabatic surface layer of about 150 m depth, a stably stratified layer prevails throughout the day. However, heating can be observed within a layer above the surface 800 m deep. Heat and moisture budget estimations show that sensible heat flux convergence exceeds cold air advection in the morning, while both processes compensate each other around noon, such that the temperature evolution stagnates. In the afternoon, cold air advection predominates and leads to net cooling of the boundary layer. Furthermore, the advection of moist air results in the accumulation of moisture during the noon and afternoon period, while latent heat flux convergence is of minor relevance to the moisture budget of the boundary layer. Correspondence: Norbert Kalthoff, Institut für Meteorologie und Klimaforschung, Universit?t Karlsruhe/Forschungszentrum Karlsruhe, Postfach 3640, 76021 Karlsruhe, Germany  相似文献   

10.
This study examines the processes controlling the diurnal variability of ozone (O3) in the marine boundary layer of the Kwajalein Atoll, Republic of the Marshall Islands (latitude 8° 43′ N, longitude 167° 44′ E), during July to September 1999. At the study site, situated in the equatorial Pacific Ocean, O3 mixing ratios remained low, with an overall average of 9–10 parts per billion on a volume basis (ppbv) and a standard deviation of 2.5 ppbv. In the absence of convective storms, daily O3 mixing ratios decreased after sunrise and reached minimum during the afternoon in response to photochemical reactions. The peak-to-peak amplitude of O3 diurnal variation was approximately 1–3 ppbv. During the daytime, O3 photolysis, hydroperoxyl radicals, hydroxyl radicals, and bromine atoms contributed to the destruction of O3, which explained the observed minimum O3 levels observed in the afternoon. The entrainment of O3-richer air from the free troposphere to the local marine boundary layer provided a recovery mechanism of surface O3 mixing ratio with a transport rate of 0.04 to 0.2 ppbv per hour during nighttime. In the presence of convection, downward transport of O3-richer tropospheric air increased surface O3 mixing ratios by 3–12 ppbv. The magnitude of O3 increase due to moist convection was lower than that observed over the continent (as high as 20–30 ppbv). Differences were ascribed to the higher O3 levels in the continental troposphere and weaker convection over the ocean. Present results suggest that moist convection plays a role in surface-level O3 dynamics in the tropical marine boundary layer.  相似文献   

11.
Sixteen years (1994 – 2009) of ozone profiling by ozonesondes at Valentia Meteorological and Geophysical Observatory, Ireland (51.94° N, 10.23° W) along with a co-located MkIV Brewer spectrophotometer for the period 1993–2009 are analyzed. Simple and multiple linear regression methods are used to infer the recent trend, if any, in stratospheric column ozone over the station. The decadal trend from 1994 to 2010 is also calculated from the monthly mean data of Brewer and column ozone data derived from satellite observations. Both of these show a 1.5 % increase per decade during this period with an uncertainty of about ±0.25 %. Monthly mean data for March show a much stronger trend of?~?4.8 % increase per decade for both ozonesonde and Brewer data. The ozone profile is divided between three vertical slots of 0–15 km, 15–26 km, and 26 km to the top of the atmosphere and a 11-year running average is calculated. Ozone values for the month of March only are observed to increase at each level with a maximum change of +9.2?±?3.2 % per decade (between years 1994 and 2009) being observed in the vertical region from 15 to 26 km. In the tropospheric region from 0 to 15 km, the trend is positive but with a poor statistical significance. However, for the top level of above 26 km the trend is significantly positive at about 4 % per decade. The March integrated ozonesonde column ozone during this period is found to increase at a rate of ~6.6 % per decade compared with the Brewer and satellite positive trends of ~5 % per decade.  相似文献   

12.
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13.
The spatial variability and temporal behavior of the vertical flux of ozone have been investigated from turbulence measurements collected on aircraft flight legs in the daytime period during two consecutive summer experimental field programs. The data were obtained during horizontal flight legs conducted over agricultural crops and forested land in three different regions of the eastern United States.Results from individual experimental cases and statistics derived from all cases in each region are presented. Ozone flux generally exhibited a significant height dependency. The strongest negative (downward) fluxes in the lowest-level flight legs were primarily attributed to the uptake of ozone by the surface and vegetative cover. Fluxes were near-zero in the middle of the convective boundary layer (CBL) in the afternoon period. As ozone flux was proportional to concentration, slightly stronger fluxes were found in low-level urban plume segments where ozone concentrations were 10–20 ppb higher than in the surrounding area. The derived deposition velocity showed no such bias as a function of position across the urban plume. Ozone flux differences were not apparent between the more heavily forested sections and the primarily agricultural cropland areas in these regions. During the afternoon period when no clear temporal trend was evident, means from values obtained below 0.15Z i (Z i being the CBL height) were -0.421 and -0.431 ppb m-2 s-1 for ozone flux and 0.81 and 0.82 cm s-1 for the derived mean deposition velocity in the southeastern Pennsylvania and central Ohio areas, respectively. These experimental results for ozone provide support to a dry deposition parameterization module which computes grid-area averaged deposition velocities for use in regional-scale models.On assignment from the National Oceanic and Atmospheric Administration, U.S. Department of Commerce.  相似文献   

14.
Atmospheric surface layer meteorological observations obtained from 20-m-high meteorological tower at Mangalore, situated along the west coast of India are used to estimate the surface layer scaling parameters of roughness length (z o) and drag coefficient (C D), surface layer fluxes of sensible heat and momentum. These parameters are computed using the simple flux–profile relationships under the framework of Monin–Obukhov (M–O) similarity theory. The estimated values of z o are higher (1.35–1.54 m) than the values reported in the literature (>0.4–0.9 m) probably due to the undulating topography surrounding the location. The magnitude of C D is high for low wind speed (<1.5 m s?1) and found to be in the range 0.005–0.03. The variations of sensible heat fluxes (SHF) and momentum fluxes are also discussed. Relatively high fluxes of heat and momentum are observed during typical days on 26–27 February 2004 and 10–11 April 2004 due to the daytime unstable atmospheric conditions. Stable or near neutral conditions prevail after 1700 h IST with negative SHF. A mesoscale model PSU/NCAR MM5 is run using a high-resolution (1 km) grid over the study region to examine the influence of complex topography on the surface layer parameters and the simulated fluxes are compared with estimated values. Spatial variations of the frictional velocity (u *), C D, surface fluxes, planetary boundary layer (PBL) height and surface winds are noticed according to the topographic variations in the simulation.  相似文献   

15.
Methyl Chloride (CH3Cl) is a chlorine-containing trace gas in the atmosphere contributing significantly to stratospheric ozone depletion (Carpenter et al. 2014). In the global CH3Cl budget, the atmospheric CH3Cl emissions is predominantly maintained by natural sources, of which magnitudes have been relatively well-constrained. However, significant uncertainties still remain in the CH3Cl emission strengths from anthropogenic sources. High-frequency and high-precision in situ measurements of atmospheric CH3Cl concentrations obtained since 2008 at Gosan station (a remote background site in the East Asia) reveal significant pollution events superimposed on the seasonally varying regional background levels. Back trajectory statistics showed that air masses corresponding to the observed CH3Cl enhancement largely originated from regions of intensive industrial activities in China. Based on an inter-species correlation method, estimates of CH3Cl emissions from manufacturing industries including coal combustion, use of feedstocks, or process agents in chemical production for China (2008–2012) are 297 ± 71 Gg yr.?1 in 2008 to 480 ± 99 Gg yr.?1 in 2009, followed by a gradual decrease of about 25% between 2009 and 2012 (398 ± 92 Gg yr.?1 for 2010; 286 ± 68 Gg yr.?1 for 2011; 358 ± 92 Gg yr.?1 for 2012). The annual average of industrial CH3Cl emissions for 2008–2012 (363 ± 85 Gg yr.?1) in China is comparable to the known total global anthropogenic CH3Cl emissions accounting only for coal combustion and indoor biofuel use. This may suggest that unless emissions from the chemical industry are accounted for, global anthropogenic emissions of CH3Cl have been substantially underestimated. In particular, since industrial production and use of CH3Cl have not been regulated under the Montreal Protocol (MP) or its successor amendments, continuous monitoring of Chinese CH3Cl outflow is important to properly evaluate its anthropogenic emissions.  相似文献   

16.
Observations from aircraft, an island station, and tworesearch vessels are used to investigate the development of an elevated mixed layeror land plume over the Arabian sea during the Indian Ocean Experiment Intensive FieldPhase 1999 (INDOEX) through air mass modification. Much of the transport of aerosolsand gases occurs in this plume located above a well-mixed convective marine boundary layerwith a depth of 800–1000 m. The depth of the land plume isapproximately 2000 m with the peak ozone concentrations occurring near the centre of this land plume.Significant latitudinal variations in the concentration of ozone occur in the marineboundary layer and in the plume. Mean ozone concentrations in the land plume decreasedwith distance from the Indian coastline.  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.
Wind-Turbine Wakes in a Convective Boundary Layer: A Wind-Tunnel Study   总被引：1，自引：1，他引：0  
Thermal stability changes the properties of the turbulent atmospheric boundary layer, and in turn affects the behaviour of wind-turbine wakes. To better understand the effects of thermal stability on the wind-turbine wake structure, wind-tunnel experiments were carried out with a simulated convective boundary layer (CBL) and a neutral boundary layer. The CBL was generated by cooling the airflow to 12–15 °C and heating up the test section floor to 73–75 °C. The freestream wind speed was set at about 2.5 m s?1, resulting in a bulk Richardson number of ?0.13. The wake of a horizontal-axis 3-blade wind-turbine model, whose height was within the lowest one third of the boundary layer, was studied using stereoscopic particle image velocimetry (S-PIV) and triple-wire (x-wire/cold-wire) anemometry. Data acquired with the S-PIV were analyzed to characterize the highly three-dimensional turbulent flow in the near wake (0.2–3.2 rotor diameters) as well as to visualize the shedding of tip vortices. Profiles of the mean flow, turbulence intensity, and turbulent momentum and heat fluxes were measured with the triple-wire anemometer at downwind locations from 2–20 rotor diameters in the centre plane of the wake. In comparison with the wake of the same wind turbine in a neutral boundary layer, a smaller velocity deficit (about 15 % at the wake centre) is observed in the CBL, where an enhanced radial momentum transport leads to a more rapid momentum recovery, particularly in the lower part of the wake. The velocity deficit at the wake centre decays following a power law regardless of the thermal stability. While the peak turbulence intensity (and the maximum added turbulence) occurs at the top-tip height at a downwind distance of about three rotor diameters in both cases, the magnitude is about 20 % higher in the CBL than in the neutral boundary layer. Correspondingly, the turbulent heat flux is also enhanced by approximately 25 % in the lower part of the wake, compared to that in the undisturbed CBL inflow. This study represents the first controlled wind-tunnel experiment to study the effects of the CBL on wind-turbine wakes. The results on decreased velocity deficit and increased turbulence in wind-turbine wakes associated with atmospheric thermal stability are important to be taken into account in the design of wind farms, in order to reduce the impact of wakes on power output and fatigue loads on downwind wind turbines.  相似文献   

19.
The concentration of gas-phase peroxides has been measured almost continuously at the Cape Grim baseline station (41° S) over a period of 393 days (7702 h of on-line measurements) between February 1991 and March 1992. In unpolluted marine air a distinct seasonal cycle in concentration was evident, from a monthly mean value of>1.4 ppbv in summer (December) to <0.2 ppbv in winter (July). In the summer months a distinct diurnal cycle in peroxides was also observed in clean marine air, with a daytime build-up in concentration and decay overnight. Both the seasonal and diurnal cycles of peroxides concentration were anticorrelated with ozone concentration, and were largely explicable using a simple photochemical box model of the marine boundary layer in which the central processes were daytime photolytic destruction of ozone, transfer of reactive oxygen into the peroxides under the low-NOx ambient conditions that favour self-reaction between peroxy radicals, and continuous heterogeneous removal of peroxides at the ocean surface. Additional factors affecting peroxides concentrations at intermediate timescales (days to a week) were a dependence on air mass origin, with air masses arriving at Cape Grim from higher latitudes having lower peroxides concentrations, a dependence on local wind speed, with higher peroxides concentrations at lower wind speeds, and a systematic decrease in peroxides concentration during periods of rainfall. Possible physical mechanisms for these synoptic scale dependencies are discussed.  相似文献   

20.
In the present study, an attempt has been made to examine the governing photochemical processes of surface ozone (O3) formation in rural site. For this purpose, measurements of surface ozone and selected meteorological parameters have been made at Anantapur (14.62°N, 77.65°E, 331 m asl), a semi-arid zone in India from January 2002 to December 2003. The annual average diurnal variation of O3 shows maximum concentration 46 ppbv at noon and minimum 25 ppbv in the morning with 1σ standard deviation. The average seasonal variation of ozone mixing ratios are observed to be maximum (about 60 ppbv) during summer and minimum (about 22 ppbv) in the monsoon period. The monthly daytime and nighttime average surface ozone concentration shows a maximum (55 ± 7 ppbv; 37 ± 7.3 ppbv) in March and minimum (28 ± 3.4 ppbv; 22 ± 2.3 ppbv) in August during the study period. The monthly average high (low) O3 48.9 ± 7.7 ppbv (26.2 ± 3.5 ppbv) observed at noon in March (August) is due to the possible increase in precursor gas concentration by anthropogenic activity and the influence of meteorological parameters. The rate of increase of surface ozone is high (1.52 ppbv/h) in March and lower (0.40 ppbv/h) in July. The average rate of increase of O3 from midnight to midday is 1 ppbv/h. Surface temperature is highest (43–44°C) during March and April months leading to higher photochemical production. On the other hand, relative humidity, which is higher during the rainy season, shows negative correlation with temperature and ozone mixing ratio. It can be seen that among the two parameters are measured, correlation of surface ozone with wind speed is better (R 2=0.84) in compare with relative humidity (R 2=0.66).  相似文献   

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