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1.
Organic compounds in the atmosphere can influence the activation, growth and lifetimes of haze, fog and cloud droplets by changing the condensation and evaporation rates of liquid water by these aqueous aerosol particles. Depending on the nature and properties of the organic compounds, the change can be to enhance or reduce these rates. In this paper we used a tandem differential mobility analyzer (TDMA) to examine the effect of tetracosane, octanoic acid, and lauric acid on the hygroscopic properties of NaCl aerosol particles at relative humidities (RH) between 30 and 95%. These organic compounds have been identified in ambient aerosol particle samples. A slight lowering of the deliquescence relative humidity (DRH) and suppression of hygroscopic growth for the NaCl-organic compound mixtures were observed when compared to pure NaCl particles. The growth of pure NaCl particles was 2.25 in diameter at 85% RH while the growth of the mixed particles was 1.3 to 1.7 in particle diameter at 85% RH with organic mass fraction of 30–50%. This shows that these organic compounds have to be present in rather large mass fractions to effect the hygroscopic behavior to a similar degree observed for ambient aerosol during field measurements. Despite the mixing of the organic material with NaCl, hysteresis was observed for decreasing RH histories, suggesting the formation of metastable droplets. These laboratory results are strikingly similar to ambient field results. For example, if the total organic mass fraction of the particles is between 0.30 and 0.50, the particle growth at 85% RH is about a factor of 1.4 for the laboratory and field measurements. Such reduction in growth compared to the pure inorganic salt is in contradiction to speculations concerning significant effects by organic compounds on cloud condensation nuclei and thus formation on clouds.  相似文献   

2.
A multifunctional HTDMA system with a robust temperature control   总被引:3,自引:0,他引:3  
The hygroscopicity of atmospheric aerosols significantly influences their size distribution, cloud condensation nuclei ability, atmospheric residence time, and climate forcing. In order to investigate the hygroscopic behavior of aerosol particles and serious haze in China, a Hygroscopic Tandem Differential Mobility Analyzers (HTDMA) system was designed and constructed at Fudan University. It can function as a scanning mobility particle sizing system to measure particle size distribution in the range of 20--1000 nm in diameter, as well as a hygroscopicity analyzer for aerosol particles with diameters between 20--400 nm in the range of 20%--90% RH (relative humidity). It can also measure the effect of uptake of inorganic acids or semi-VOCs on the hygroscopic behavior of aerosols, such as typical inorganic salts in atmospheric dust or their mixtures. The performance tests show that the system measured particle size of the standard polystyrene latex spheres (PSLs) is 197 nm, which is in excellent agreement with the certified diameter D=199±6 nm, as well as a standard deviation of the repeated runs SD=8.9x10-4. In addition, the measured hygroscopic growth factors of the model compounds, (NH4)2SO4 and NaNO3, agree with the Kohler theoretical curves. The results indicate that the HTDMA system is an excellent and powerful tool for studying the hygroscopic behavior of submicron aerosols and meets the demand required for laboratory research and fieldwork on atmospheric aerosols in China.  相似文献   

3.
Mass size distribution of the crustal elements (Al, Ca, Fe, Mg, Si, Ti), anthropogenic elements (Zn, Mn, Cr, Cu, K, P, Pb) and sea elements (Na, Cl) were obtained from measurements carried out with an inertial cascade impactor in Sfax. A fitting procedure by data inversion was applied to those data. This procedure yields accurate size distributions of aerosols in the diameter range 0.1–25 μm in two different sites. In a coastal industrial site, the mass distribution of the aerosol showed a bimodal structure; and in urban area, the lower particle mode cannot be observed. The elemental dry deposition flux was calculated as a function of particle size. The element flux size distribution increased rapidly with particle size. The modelling results indicate that the majority of the crustal and anthropogenic elements flux (>90%) was due to particles larger than 3 μm in diameter.  相似文献   

4.
In this work, the charging state of atmospheric nanoparticles was estimated through simultaneous measurements of aerosol size distribution and air ions mobility distribution with the aim to elucidate the formation mechanisms of atmospheric aerosols. The measurements were performed as a part of the QUEST 2 campaign at a boreal forest station in Finland. The overlapping part of the measurement ranges of the particle size spectrometers and air ion mobility spectrometers in the mass diameter interval of 2.6–40 nm was used to assess the percentage of charged particles (charging probability). This parameter was obtained as the slope of the linear regression line on the scatterplot of the measured concentrations of total (neutral + charged) and charged particles for the same diameter interval. Charging probabilities as a function of particle diameter were calculated for different days and were compared with the steady state charging probabilities of the particles in the bipolar ion atmosphere. For the smallest particles detectable by the particle size spectrometers (2.6–5 nm), the high percentages of negatively charged particles were found during the nanometer particle concentration bursts. These values considerably exceeded the values for the steady charging state and it was concluded that negative cluster ions preferably act as condensation nuclei. This effect was found to be the highest in the case of comparatively weak nucleation bursts of nanoparticles, when the rate of the homogeneous nucleation and the concentration of freshly nucleated particles were low. The nucleation burst days were classified according to the concentration of the generated smallest detectable new particles (weak and strong bursts). Approximately the same classification was obtained based on the charge asymmetry on particles with respect to the charge sign (polarity). The probabilities of negative and positive charge on the particles with the diameter of 5–20 nm were found to be nearly equal and they approximately agree with the values corresponding to the steady state charge distribution for negative particles known from lab experiments. It means that the steady charging state was reached during the growing time of particles up to 5 nm. The natural charging state of particles with a diameter between 2.5 and 4.5 nm was estimated by means of a special DMPS setup. Results were found to be in good correlation with the data by the particle size spectrometers and air ion mobility spectrometers.  相似文献   

5.
In this work we propose and test a method to calculate cloud condensation nuclei (CCN) spectra based on aerosol number size distributions and hygroscopic growth factors. Sensitivity studies show that this method can be used in a wide variety of conditions except when the aerosol consist mainly of organic compounds. One crucial step in the calculations, estimating soluble ions in an aerosol particle based on hygroscopic growth factors, is tested in an internal hygroscopic consistency study. The results show that during the second Aerosol Characterization Experiment (ACE-2) the number concentration of inorganic ions analyzed in impactor samples could be reproduced from measured growth factors within the measurement uncertainties at the measurement site in Sagres, Portugal.
CCN spectra were calculated based on data from the ACE-2 field experiment at the Sagres site. The calculations overestimate measured CCN spectra on average by approximately 30%, which is comparable to the uncertainties in measurements and calculations at supersaturations below 0.5%. The calculated CCN spectra were averaged over time periods when Sagres received clean air masses and air masses influenced by aged and recent pollution. Pollution outbreaks enhance the CCN concentrations at supersaturations near 0.2% by a factor of 3 (aged pollution) to 5 (recent pollution) compared to the clean marine background concentrations. In polluted air masses, the shape of the CCN spectra changes. The clean spectra can be approximated by a power function, whereas the polluted spectra are better approximated by an error function.  相似文献   

6.
The hygroscopic growth of individual aerosol particles has been measured with a Tandem Differential Mobility Analyser. The hygroscopic growth spectra were analysed in terms of diameter change with increasing RH from 20% to 85%. The measurements were carried out during the GCE cloud experiment at Kleiner Feldberg, Taunus, Germany in October and November 1990.Two groups of particles with different hygroscopic growth were observed. The less-hygroscopic group had average growth factors of 1.11, 1.04 and 1.02 for particle diameters of 50, 150 and 300 nm, respectively. The more-hygroscopic group had average growth factors of 1.34, 1.34, and 1.37 for the same particle diameters. The average fraction of less-hygroscopic particles was about 50%. Estimates of the soluble fractions of the particles belonging to the two groups are reported.Hygroscopic growth spectra for total aerosol, interstitial aerosol and cloud drop residuals were measured. A comparison of these hygroscopic growths of individual aerosol particles provides clear evidence for the importance of hygroscopic growth in nucleation scavenging. The measured scavenged fraction of particles as a function of diameter can be explained by the hygroscopic growth spectra.  相似文献   

7.
We used both a conventional transmission electron microscope and an environmental transmission electron microscope (ETEM) to determine morphology, composition, and water uptake of 80 individual aerosol particles collected from the young smoke of flaming and smoldering fires during SAFARI-2000, a comprehensive air quality campaign in southern Africa. Six representative carbonaceous particle types are described, including soot, tar balls, and heterogeneously internally mixed particles containing C with S-, K-, Mg- or Na-rich inorganic phases. The hygroscopic behavior of these particles over the range 0–100% relative humidity (RH) was studied in detail. Soot and tar balls did not take up water, whereas the mixed organic–inorganic particles took up water between 55 and 100% RH, the exact value depending on the composition of their water-soluble phases. The inorganic phase appeared to determine the hygroscopic properties of all mixed organic–inorganic particles. Thus, incorporation of inorganic plant material or reactions with inorganic atmospheric components can dramatically alter the hygroscopic properties of carbonaceous particles in smoke plumes. The fraction of these mixed organic–inorganic particles plausibly increases with time, which will modulate the effects of smoke on radiative budgets.  相似文献   

8.
The change of the chemical composition of the near-ground level atmospheric aerosol was studied during two summer episodes by a Lagrangian type of experimental approach. Bulk and single-particle chemical analyses of ions and elements in the particulate phase were deployed. N(-III) and N(V) components were also measured in the gas-phase. The measurements were completed by particle size distributions.Secondary inorganic aerosols (SIA) and fine particles of ≈0.2–0.4 μm size were still elevated 50 km downwind of the city. The direct comparison of transport over the city in contrast to transport over the surrounding areas showed that SIA was formed from emission from the city within less than 3 h. Relative increases, i.e., enrichment during transport were observed for primary and secondary aerosol components. The degree of mixing on the individual particle level increased significantly during transport in the area. In particular, newly emitted carbonaceous particles became internally mixed within hours with pre-existing sulphate particles. Mostly due to secondary aerosol formation the average particle size (mass median diameter) of major constituents of the aerosol was significantly decreased while being transported over 13 h. Given recent insights which link fine particles number and mass concentrations with health risks, the results suggest that rural populations in areas which frequently are located within an urban plume might run an elevated health risk relative to populations in areas not affected by urban plumes.  相似文献   

9.
黄山地区气溶胶吸湿增长特性数值模拟研究   总被引:4,自引:2,他引:2  
江琪  银燕  秦彦硕  陈魁  杨素英 《气象科学》2013,33(3):237-245
应用多种化学组分气溶胶的绝热气块分档模式,对2008年春季黄山地区气溶胶吸湿增长特性进行了模拟分析.结果表明:黄山地区气溶胶吸湿增长因子f的大小与粒子半径、相对湿度、粒子化学组分、上升速度及上升高度密切相关,且小粒子吸湿增长比大粒子显著.吸湿增长因子与相对湿度呈正相关,相对湿度越接近粒子的临界饱和比,吸湿增长因子变化越显著.可溶性有机气溶胶,通过增加溶液中溶质的百分比来影响临界饱和比,使吸湿增长因子增大.若不考虑不可溶粒子的成核作用,会高估粒子的吸湿性.随着上升速度增大,吸湿增长因子降低,降低程度与粒子初始高度的相对湿度有关.上升高度通过改变气块相对湿度的变化来影响气溶胶吸湿增长因子.  相似文献   

10.
The interpretation of the physico-chemical processes in clouds is facilitated by segregating in situ cloud elements from their carrier gas and small particles (interstitial aerosol). Thus, the present study focuses on the quantitative phase segregation of interstitial air from cloud phase by two complementary samplers with microphysical on-line analysis of the separated phases. An improved counterflow virtual impactor (CVI) was developed for the collection and subsequent evaporation of the condensed phase, releasing dissolved gaseous material and residual particles. This sampler operates in the size range of few micrometers up to 50 μm in cloud element diameter and is matched by an interstitial Round Jet Impactor sampling the gas phase with interstitial particles. Calibrations of both samplers verified the calculated cut sizes D50 of 4, 5, and 6 μm and quantified the slope of the collection efficiency curves. Until this study no direct CVI measurements of the residual particle sizes far below the diameter of 0.1 μm were available. For the first time a CVI was connected to a Differential Mobility Particle Sizer (DMPS) scanning between 25 nm and 850 nm, thus, including the entire Aitken mode in the residual size analysis. Cloud studies on the Puy de Dôme, France, revealed residual particle sizes including Aitken mode (diameter D<100 nm) and accumulation mode (D>100 nm). A major feature of the CVI data is expressed by the fact that despite incomplete incorporation of accumulation mode particles in cloud elements there are contributions of particles with diameters smaller than 0.1 μm to the number of residual particles. Cloud entrainment from height levels above the maximum supersaturation as wells as the size-dependent chemical composition of the aerosol population most likely produced the S-shaped size-dependent partitioning of residual particles. Compared to earlier studies the 50% partitioning diameters dropped significantly below 100 nm to roughly 70 nm.  相似文献   

11.
The Saharan Mineral Dust Experiment (SAMUM) was conducted in May and June 2006 in Tinfou, Morocco. A H-TDMA system and a H-DMA-APS system were used to obtain hygroscopic properties of mineral dust particles at 85% RH. Dynamic shape factors of 1.11, 1.19 and 1.25 were determined for the volume equivalent diameters 720, 840 and 960 nm, respectively.
During a dust event, the hydrophobic number fraction of 250 and 350 nm particles increased significantly from 30 and 65% to 53 and 75%, respectively, indicating that mineral dust particles can be as small as 200 nm in diameter. Log-normal functions for mineral dust number size distributions were obtained from total particle number size distributions and fractions of hydrophobic particles. The geometric mean diameter for Saharan dust particles was 715 nm during the dust event and 570 nm for the Saharan background aerosol.
Measurements of hygroscopic growth showed that the Saharan aerosol consists of an anthropogenic fraction (predominantly non natural sulphate and carbonaceous particles) and of mineral dust particles. Hygroscopic growth and hysteresis curve measurements of the 'more' hygroscopic particle fraction indicated ammonium sulphate as a main component of the anthropogenic aerosol. Particles larger than 720 nm in diameter were completely hydrophobic meaning that mineral dust particles are not hygroscopic.  相似文献   

12.
Measuring of charged nanometer particles in atmospheric air is a routine task in research on atmospheric electricity, where these particles are called the atmospheric ions. An aspiration condenser is the most popular instrument for measuring atmospheric ions. Continuous scanning of a mobility distribution is possible when the aspiration condenser is connected as an arm of a balanced bridge. Transfer function of an aspiration condenser is calculated according to the measurements of geometric dimensions, air flow rate, driving voltage, and electric current. The most complicated phase of the calibration is the estimation of the inlet loss of ions due to the Brownian deposition. The available models of ion deposition on the protective inlet screen and the inlet control electrofilter have the uncertainty of about 20%. To keep the uncertainty of measurements low the adsorption should not exceed a few tens of percent. The online conversion of the mobility distribution to the size distribution and a correct reduction of inlet losses are possible when air temperature and pressure are measured simultaneously with the mobility distribution. Two instruments called the Balanced Scanning Mobility Analyzers (BSMA) were manufactured and tested in routine atmospheric measurements. The concentration of atmospheric ions of the size of about a few nanometers is very low and a high air flow rate is required to collect enough of ion current. The air flow of 52 l/s exceeds the air flow in usual aerosol instruments by 2–3 orders of magnitude. The high flow rate reduces the time of ion passage to 60 ms and the heating of air in an analyzer to 0.2 K, which suppresses a possible transformation of ions inside the instrument. The mobility range of the BSMA of 0.032–3.2 cm2 V− 1 s− 1 is logarithmically uniformly divided into 16 fractions. The size distribution is presented by 12 fractions in the diameter range of 0.4–7.5 nm. The measurement noise of a fraction concentration is typically about 5 cm− 3 and the time resolution is about 10 min when measuring simultaneously both positive and negative ions in atmospheric air.  相似文献   

13.
The growth of monodisperse particles (0.07 to 0.5 µm) exposed to SO2 (0–860 ppb), H2O2 (0–150 ppb) and sometimes NH3 (0–550 ppb) in purified air at 22 °C at relative humidities ranging from 25 to 75% were measured using the Tandem Differential Mobility Analyzer technique. The experiments were performed in a flow reactor with aqueous (NH4)2SO4 and Na2SO4 droplets. For (NH4)2SO4 droplets the fractional diameter growth was independent of size above 0.3 µm but decreased with decreasing size below that. When NH3 was added the fractional growth increased with decreasing size. Measurements were compared with predictions of a model that accounts for solubility of the reactive gases, the liquid phase oxidation of SO2 by H2O2, and ionic equilibria. Agreement between measured and predicted droplet growth is reasonable when the ionic strength effects are included. Theory and experiments suggest that NH3 evaporation is responsible for the decrease in relative growth rates for small aqueous ammonium sulfate particles. The observed droplet growth rates are too slow to explain observed growth rates of secondary atmospheric sulfate particles.  相似文献   

14.
This study is devoted to the performance of the CLIMET CI-8060, a white-light optical particle counter (OPC). Designed for clean-room monitoring, the off-the-shelf performance of this instrument is rather poor for outdoor studies. Modifications of this instrument are described turning this low-cost instrument into an OPC with excellent performance. The modifications include a reduction of the flow rate to 1.4 l/min, an altered design of the inlet nozzle, a buffer chamber to assure continuous flow, and a 16-channel pulse height analyzer.The modified version has been checked thouroughly. The counting efficiency is very close to 100% for particle sizes between 0.295 and 0.801 μm. The loss of giant particles is also marginal, as comparative tests with a cascade impactor show. The sizing calibration has been redetermined experimentally, using latex spheres, and theoretically, applying a software package by Jüngert [1988] using the Mie theory. With the help of the established relationship between experimental and theoretical response for latex, calibration tables for any other particle material are obtained (in particular for ambient aerosols and H2O for fog and cloud condensation studies).The modified counter has been used for monitoring the growth of hygroscopic aerosols in humid conditions, using two different inlet lines, one of them drying the aerosol before entering the OPC, the other one preserving ambient conditions. This system allows to observe haze and fog formation and cloud condensation processes in situ at a one-minute time resolution.  相似文献   

15.
The results presented are the first complete analysis of inorganic soluble ions in a tropical savannah region. Atmospheric particles were collected in six rural Venezuelan savannah sites. Concentrations and size distribution of NO3 , SO4 2-, CI, PO4 3-, NH4 +, Na+, K+, Ca2+ and Mg2+ were determined in samples collected with Hi Vol samplers equipped with five-stage cascade impactors. Concentrations were higher in the dry season, with a maximum during the burning periods. Using Na+ as a reference, the results show a deficit of Cl and, with the exception of Mg2+, an enrichment of all other ions with respect to marine aerosols. Significant variations were observed in particle-size distribution between different periods. Various pairs of ions present similar size distributions: SO4 2- and NH4 +; Cl and Na+; PO4 3- and K+; Ca2+, Mg2+ and NO3 ; indicating that the ions were produced by the same source and/or were involved in similar atmospheric processes. Possible primary sources, the gas-to-particle atmospheric process, environmental implication of long-range transport of nutrients during dry seasons, etc., are discussed.  相似文献   

16.
Chemical characteristics of haze during summer and winter in Guangzhou   总被引:33,自引:0,他引:33  
Airborne particles were collected with a 10-stage MOUDI and a PM10 sampler in Guangzhou, China, during both haze and normal days in the summer of 2002 and 2003, and winter 2002. The characteristics of PAHs, organic carbon, elemental carbon and water-soluble inorganic ions were studied under four periods (summer normal, summer haze, winter normal and winter haze). In this study, secondary pollutants (OC, SO42−, NO3 and NH4+) were the major chemical components and appeared to show a remarkably rapid increase from normal to haze days. The particle mass size distributions were bimodal and dominated by fine particles in haze days. A significantly higher OC/EC ratio was found in haze days (3.2–4.7) compared to normal days (1.8–2.8), indicating secondary organic aerosol formation might be significant during haze days. Correlation analysis between visibility and chemical species showed that the major scattering species were TC (total carbon) and sulfate in normal days and nitrate and TC in haze days, respectively. Simultaneously, correlation analysis between visibility and meteorological factors demonstrated that visibility increased with both temperature and wind speed, while it decreased with relative humidity. Furthermore, the relatively higher value of IcdP/(BghiP + IcdP) and the low value of Cmax, CPI, and BghiP/BeP in winter haze could be due to the growth of motor vehicle usage and energy consumption in winter.  相似文献   

17.
Coastal nucleation events and behavior of cluster ions were characterized through the measurements of air ion mobility distributions at the Mace Head research station on the west coast of Ireland in 2006. We measured concentrations of cluster ions and charged aerosol particles in the size range of 0.34–40 nm. These measurements allow us to characterize freshly nucleated charged particles with diameters smaller than 3 nm. The analysis shows that bursts of intermediate ions (1.6–7 nm) are a frequent phenomenon in the marine coastal environment. Intermediate ion concentrations were generally close to zero, but during some nucleation episodes the concentrations increased to several hundreds per cm3. Nucleation events occurred during most of the measurement days. We classified all days into one of seven classes according to the occurrence and type of new particle formation. Nucleation events were observed during 207 days in 2006, most prominently in the spring and summer months. Rain-induced events, in turn, were observed during 132 days. Particle formation and growth events mostly coincided with the presence of low tide. Also small cluster ions (0.34–1.6 nm) were characterized. Average concentrations of small ions were 440 cm− 3 for the negative ions and 423 cm− 3 for the positive ions. Average mean mobilities of small ions were 1.86 cm2V− 1s− 1 and 1.49 cm2V− 1s− 1 for the negative and positive polarities, respectively. Concentrations of small ions were observed to be strongly dependent on the variations of meteorological parameters including wind speed and direction.  相似文献   

18.
On the formation and growth of atmospheric nanoparticles   总被引:2,自引:0,他引:2  
In this paper we summarize recent experimental, theoretical and observational results on the formation and growth of atmospheric nanoparticles. During the last years significant progress has occurred to explain atmospheric nucleation and initial steps of the growth. Due to climatic and health effects of fine and ultrafine particles the formation and growth of new aerosol particles is of growing interest. The question “How and under which conditions does the formation of new atmospheric aerosol particles take place?” has exercised the minds of scientists since the time of John Aitken, who in the late 1880s built the first apparatus to measure the number of dust and fog particles. However, only during the last 15–20 years has the measurement technology developed to such a level that size distributions of nanometer-size particles and concentrations of gases participating in particle formation can be measured in the atmosphere. Also from a theoretical point of view atmospheric nucleation mechanisms have not been resolved: several mechanisms such as ion-induced (or ion mediated) nucleation, ternary and kinetic (barrier-less) nucleation have been suggested. In the most recent theory, the activation of existing neutral and/or ion clusters has been suggested.  相似文献   

19.
An electrically based ion spectrometer is described, capable of measuring particle sizes and mobilities from molecular ions (small ions) to aerosol particles across a size range of 0.4 to 30 nm in diameter. It consists of a single cylindrical capacitor divided into three electrically insulated sections. The current arriving at the central section is measured by an electrometer and represents the ion flux over a known range of mobilities determined by the applied voltage. The applied voltage is scanned in steps to measure the ion fluxes over a large number of overlapping mobility ranges. The recorded signal and the response function of the instrument are unfolded using a maximum entropy procedure to give a high-resolution measured mobility spectrum. The maximum entropy approach offers a considerable improvement over traditional aspiration collectors and can approach the resolution of a drift tube system. In this way, the spectrometer successfully overcomes the diffusion limit to small ion resolution. Illustrative spectra are shown, demonstrating for the first time the presence of some resolved structure within the small ion spectrum at the highest mobilities. It is demonstrated that the actual mobility spectrum of small ions falls in the range 0.8–2.0 × 10−4 m2 V−1 s−1. This represents a narrower range than that previously measured which is attributed to improved spectral resolution in the present work.  相似文献   

20.
In November 2004–January 2005, a micro orifice uniform deposit impactor (MOUDI) and a Nanometer (nanometer)-MOUDI were used in the center of Taiwan to measure particle size (18 nm particle size 18 μm) distributions of atmospheric aerosols at a traffic site during the winter period. The average Mass in Media Aerodynamic Diameter (MMAD) of suspended particles is 0.99 μm this study. As for the ultra fine and nanometer (nanometer) particle mode, the composition order for these major ions species was SO42− NH4+ NO3 Mg2+ Ca2+ Na+ K+ Cl. An ion Chromatography (DIONEX-100) was used to analyze major anion species, Cl, NO3, SO42− and cation species, NH4+Na+, K+, Ca2+Mg2+. Their concentrations were also extracted from various particles size modes (nanometer (nanometer), ultra fine, fine and coarse). The results obtained in this study also indicated that the average portions for the major ionic species (SO42−, NH4+ and Mg2+) in the nanometer (nanometer), ultra fine, fine and coarse particulate modes are about 34%, 37%, 63% and 30%, respectively at this traffic sampling site during the winter period.  相似文献   

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