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1.
Three “standard” Nolan–Pollak (N–P) and a modified N–P design condensation nucleus (CN) counters were included in the Vienna Workshop on Intercomparison of Condensation Nuclei and Aerosol Particle counters. These counters came from diverse backgrounds, namely programs in USA, Europe and Australia. In this work, principles of the operation and previous history of calibration of the N–P expansion counter are briefly reviewed and comparisons between the particular counters used in the workshop are presented and discussed. Counting agreement was found to be very good between the N–P counters, typically better than ±12% for a range of aerosol sizes and compositions from a minimum diameter of 4 nm. The independently calibrated GIV CNC-440 (modified N–P type counter) also agreed well with the N–P counters. The minimum size sensitivity of the N–P counter was examined showing a lower detection limit for insoluble (Ag) particles of around 2.6±0.3 nm diameter.  相似文献   

2.
Aerosols affect precipitation by modifying cloud properties such as cloud droplet number concentration (CDNC). Aerosol effects on CDNC depend on aerosol properties such as number concentration, size spectrum, and chemical composition. This study focuses on the effects of aerosol chemical composition on CDNC and, thereby, precipitation in a mesoscale cloud ensemble (MCE) driven by deep convective clouds. The MCE was observed during the 1997 department of energy's Atmospheric Radiation Measurement (ARM) summer experiment. Double-moment microphysics with explicit nucleation parameterization, able to take into account those three properties of aerosols, is used to investigate the effects of aerosol chemical composition on CDNC and precipitation. The effects of aerosol chemical compositions are investigated for both soluble and insoluble substances in aerosol particles. The effects of soluble substances are examined by varying mass fractions of two representative soluble components of aerosols in the continental air mass: sulfate and organics. The increase in organics with decreasing sulfate lowers critical supersaturation (Sc) and leads to higher CDNC. Higher CDNC results in smaller autoconversion of cloud liquid to rain. This provides more abundant cloud liquid as a source of evaporative cooling, leading to more intense downdrafts, low-level convergence, and updrafts. The resultant stronger updrafts produce more condensation and thus precipitation, as compared to the case of 100% sulfate aerosols. The conventional assumption of sulfate aerosol as a surrogate for the whole aerosol mass can be inapplicable for the case with the strong sources of organics. The less precipitation is simulated when an insoluble substance replaces organics as compared to when it replaces sulfate. When the effects of organics on the surface tension of droplet and solution term in the Köhler curve are deactivated by the insoluble substance, Sc is raised more than when the effects of sulfate on the solution term are deactivated by the insoluble substance. This leads to lower CDNC and, thus, larger autoconversion of cloud liquid to rain, providing less abundant cloud liquid as a source of evaporative cooling. The resultant less evaporative cooling produces less intense downdrafts, weaker low-level convergence, updrafts, condensation and, thereby, less precipitation in the case where organics is replaced by the insoluble substance than in the case where sulfate is replaced by the insoluble substance. The variation of precipitation caused by the change in the mass fraction between the soluble and insoluble substances is larger than that caused by the change in the mass fraction between the soluble substances.  相似文献   

3.
During May-June of 1990 an extensive flight series to survey aerosol present in the upper-troposphere was undertaken aboard the NASA DC-8 as part of the CLObal Backscatter Experiment (GLOBE). About 50,000 km were characterized between 8–12 km altitude and between 70°N and 58°S. Aerosol with diameters greater than 3nm were counted and sized with a combination of condensation nuclei counters and optical particle counters. Aerosol number and mass concentrations were separately identified with regard to both refractory and volatile components. Regions of the free-troposphere with the lowest mass concentrations were generally found to have the highest number concentrations and appeared to be effective regions for new particle production. These new particle concentrations appear inversely related to available aerosol surface area and their volatility suggests a sulfuric acid composition. The long lifetime of these new particles aloft can result in their growth to sizes effective as CN and CCN that can be mixed throughout the troposphere.  相似文献   

4.
Particle detection by condensation particle counters (CPCs) is ultimately limited by the onset of homogeneous nucleation. At vapour supersaturations around the homogeneous nucleation limit the diameter of critical clusters is typically about 2 nm. It is widely assumed that only particles larger than critical clusters can be activated by vapour condensation and the general detection limit of CPCs is therefore currently accepted to be around 2 nm particle diameter. Using an expansion type CPC with n-propanol as working fluid we investigated the transition from heterogeneous to homogeneous nucleation, clearly showing that particles are activated much before the onset of homogeneous nucleation, even at particle diameters as small as 1.4 nm. For particle diameters below 2 nm we have usually found condensation particle counting to be influenced by the simultaneous presence of ions as generated in a bipolar diffusion charger. In this paper we illustrate how the presence of ions influences particle number concentration measurement and how ions can be removed in order to obtain accurate seed particle number concentrations for particle diameters down to 1 nm.  相似文献   

5.
The impact of aerosols on the climate and atmospheric environment depends on the water uptake ability of particles; namely, hygroscopic growth and acti- vation into cloud condensation nuclei （CCN）. The size-resolved activation ratios （SRAR）, characterizing the fraction of aerosol particles that act as CCN at different particle sizes and supersaturations, can be measured using a combination of differential mobility analyzers （DMA） and particle counters. DMA-based measurements are in- fluenced by the multiply charged particles and the quasi-mono-dispersed particles （effect of DMA transfer function） selected for each prescribed particle size. A theoretical study, assuming different particle number size distributions and hygroscopicity of aerosols, is performed to study the effects of the DMA transfer function and multiple charging on the measured SRAR and the derived hygroscopicity. Results show that the raw SRAR can be significantly skewed and hygroscopicity may be highly biased from the true value if the data are not corrected. The effect of the transfer function is relatively small and depends on the sample to sheath flow ratio. Multiply charged particles, however, can lead to large biases of the SRAR. These results emphasize that the inversion algo- rithm, which is used to correct the effects of the DMA transfer function and multiple charging, is necessary for accurate measurement of the SRAR.  相似文献   

6.
Measurements at Barrow during the second Arctic Gas and Aerosol Sampling Program (AGASP-II), conducted in April 1986, showed no rapid long-range transport from lower-latitude source regions to Barrow, and only limited vertical transport from above the boundary layer to the surface. New aerosol size distribution measurements in the 0.005–0.1 m diameter size range using a Nuclepore-filter diffusion battery apparatus showed a median diameter of about 0.01 m during times of high condensation nucleus (CN) concentrations. Aerosol black carbon concentrations exceeding 400 ng m–3 were detected at the surface and were more strongly correlated with CN concentrations than with aerosol scattering extinction (sp), suggesting that aerosol carbon was generally associated with small particles rather than large particles. Measurements at Barrow during AGASP-I, conducted in March–April 1983, showed a series of aerosol events detected at the ground that were caused by rapid long-range transport paths to the vicinity of Barrow from Eurasia. These events were strongly correlated with aerosol loading in the vertical column (optical depth).  相似文献   

7.
In a first attempt to assess a proposed climatic change feedback process involving cloud condensation nuclei (CCN) and cloud albedo, CCN concentrations N as a function of supersaturation S were measured on a voyage from latitude 43 to 65°S in October–November 1988. The usual relationship N=CSk, with k=0.5 and C a constant was a fair apprraximation for S in the range 0.3–0.7% implying that CCN concentrations should largely determine cloud drop concentrations and hence albedo for clouds with S in that range. South of latitude 50°S and at smaller S,k was 1 or larger on average, which would lead to reduced dependence of albedo on CCN for the relevant clouds. N varied very widely for separations of the order of 100 km or 6 hours in time, particularly when the sea was partly ice-covered, suggesting strong local influences. During a large increase in N 60°S, unaccompanied by an increase in condensation nuclei (CN), cloud drops grew more rapidly than usual. In a subsidiary experiment particles were collected and examined by transmission electron microscopy. For particles less than 0.2 μm diameter, 80–90% appeared to consist of ammonium sulfate, the remainder being sea salt or an unknown substance which was more liquid and heat-resistant. Dialysis showed that the sulfate particles contained a few percent of insoluble material. Particles which formed cloud drops in vapours other water, were also studied. Comparison of these and water CCN and the rates of droplet suggested that the water insoluble portion of the particles was ethanol-soluble and surface-active. CN concentrations decreased by a factor of about 2 between 43 and 65°S, a change closely paralleled by ethanol CCN concentrations.  相似文献   

8.
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   

9.
The meaning of baseline as applied to measurements of CN, at atmospheric monitoring sites such as Cape Grim, is discussed and the idea that a baseline exists only in a statistical sense advocated. Use of the concentration frequency-distribution geometric-mean is proposed as the best measure of CN concentrations. Variations in CN concentrations at Cape Grim for periods greater than 12 months are derived by Kalman filtering the monthly estimates of geometric mean concentration obtained from 1977 to 1987. Significant variations are shown to be present on this timescale with quasi-periodic oscillations in concentration. Some association between major fluctuations and El-Nino Southern Oscillation perturbations in the regional circulation is suggested.  相似文献   

10.
The construction and operating principles of the Turbulent Mixing Condensation Nucleus Counter (TM CNC) are described. Estimations based on the semiempirical theory of turbulent jets and the classical theory of nucleation and growth show the possibility of detecting particles as small as 2.5 nm without the interference of homogeneous nucleation. This conclusion was confirmed experimentally during the International Workshop on Intercomparison of Condensation Nuclei and Aerosol Particle Counters (Vienna, Austria). Number concentration, measured by the Turbulent Mixing CNC and other participating instruments, is found to be essentially equal.  相似文献   

11.
Although it is believed that organic aerosols play a key role in cloud nucleation and make an important contribution to the cloud condensation nuclei (CCN) population, their specific species remain poorly characterized. This paper reviews the current knowledge of organic acids (mainly formic, acetic, pyruvic and oxalic acids). Without specification, organic acids in this paper refer to these four organic acids in the gas and aerosol phases. This paper analyzes the extent to which organic acids act as CCN and compares the physical and chemical properties of organic acids with those of CCN. The results show that aerosol formate and acetate concentrations range from 0.02 to 5.3 nmol m−3 and from 0.03 to 12.4 nmol m−3, respectively, and that between 34 to 77% of formate and between 21 to 66% of acetate are present in the fine fraction of aerosols. It was found that although most (98–99%) of these volatile organic acids are present in the gas phase, their concentrations in the aerosol particles are sufficient to make them a good candidate for CCN. The results also show that organic acids may make an important contribution to the formation of CCN in some special sources such as vegetation emissions and biomass-burning. Organic acids are expected to contribute significantly to the estimates of indirect (cloud-mediated) forcing due to aerosols.  相似文献   

12.
A traditional mulching technique used in Lanzarote, Canary Islands, allows dry farming as well as pronounced water savings in irrigation. It is known to reduce evaporational losses, but is also supposed to enhance the nocturnal condensation of water vapour from the atmosphere. The mulch layer consists of porous volcanic rock fragments abundantly available on the island. The mulched surface is believed to cool rapidly and to be more hygroscopic than a bare soil surface. This was investigated during a field experiment conducted over 68 nights during different seasons in 2001 and 2002, as well as some simple laboratory measurements. It was found that nocturnal condensation on the mulch surface (max 0.33 mm) was lower than on the bare soil surface (max 0.57 mm) or any one of three alternative mulch substrates. However, a slightly stronger nocturnal cooling of the mulched as compared to the bare surface was present. It is shown that these contrary findings can be explained by the higher hygroscopicity of the dry loam soil, resulting in condensation gains beyond the strict definition of dew. Differences in plant-availability of non-hygroscopic dew water and hygroscopic water uptakes are discussed, and conditions under which mulching would show positive condensation effects are defined. This includes a theoretical section demonstrating that non-hygroscopic mulch layers of a proper thickness can provide small amounts of dew to plant roots at the mulch–soil interface. This condensation could also happen during the day and would be favoured by a high amplitude of the diurnal atmospheric moisture cycle.  相似文献   

13.
This paper reviews theory and measurements of transport processes between small particles and the surrounding gas. Evaporation and condensation coefficients and gas uptake coefficients are of particular interest. There has long been a great difference in coefficients reported by different experimentalists, and much of this disagreement is considered in this overview. A brief review of the kinetic theory of gases is provided to describe molecular transport to or from a surface when the mean free path of molecules, ℓ, is large compared with the particle dimensions, that is, when the Knudsen number is large. For a sphere of radius a the Knudsen number, Kn = ℓ / a. The condition Kn >> 1 is called the free molecule regime, and for Kn << 1 continuum theory applies. It is shown that accommodation coefficients cannot be determined by experiments operating in the continuum regime. At intermediate Knudsen numbers (the Knudsen regime) transport theory is more difficult, but results based on solution of the Boltzmann equation describing the evolution of the molecular velocity distribution are reviewed. With the advent of high-speed computers transport theory has been supplemented by molecular dynamics calculations, and these calculations are often at odds with experimental measurements of accommodation coefficients. Examples are provided.Experimental methods surveyed include Knudsen cell methods, jet tensimetry, electrodynamic levitation experiments, expansion cloud chamber measurements, and vibrating orifice aerosol generator (VOAG) techniques. VOAG measurements are particularly useful for studying processes over small times, and theory and results related to VOAG experiments are presented. More recent experimental measurements of condensation coefficients involving the use of molecular beams are reported. There is a growing body of evidence that accommodation coefficients are of order unity in many cases, but coefficients smaller than 0.01 are still reported, particularly for uptake coefficients.  相似文献   

14.
The diffusion aerosol spectrometer for the measurements of particle size spectra and concentration levels is described. It includes three principal parts: (i) a block of diffusion batteries for measuring the particles, whose size does not exceed 0.15 μm, (ii) the particle amplifier for growing the particles passing through the diffusion batteries up to optically distinguishable sizes and (iii) the laser aerosol spectrometer, which counts the amplified particles and may also serve for independent measurements of particle size spectra within submicron size range. The tandem including: diffusion batteries+laser aerosol spectrometer allows for detecting particles of radius >3 nm at maximal concentration up to 2×104 particles/cm3. The tandem is managed either by PC or manually. The instrument is designed for studying aerosols in the atmosphere and for ecological measurements.  相似文献   

15.
气溶胶影响混合相对流云降水的数值模拟研究   总被引：2，自引：0，他引：2  
利用一种新的异质冰相核化参数化方案,研究了当气溶胶同时作为云凝结核和冰核时,在不同高度输送对混合相对流云和降水的影响。结果发现,对于本文研究的理想混合相对流云,气溶胶在边界层的输送导致液滴数浓度明显增加,有效半径减小,霰粒的生长受到抑制,引起霰粒质量浓度降低;而气溶胶在对流层中层4～6km输送时,导致冰晶和霰粒数浓度明显增加。由于较多的冰晶引起更加快速的贝吉隆过程,使霰粒的质量浓度增加;气溶胶在对流层中层2～4km高度输送时冰相形成作用相对较弱,并引起霰粒的数浓度略微增加,由于霰粒的有效半径减小导致其质量浓度下降。气溶胶在不同高度的输送都导致液态和固态降水率降低,随着背景气溶胶数浓度的增加,气溶胶在0～2km、2～4km以及4～6km的输送分别导致累积降水量减少28％～64％、4％～44％和3％～46％,并且对降水的抑制效应及所在高度不同引起的降水差异随着背景气溶胶数浓度的增加而减小。  相似文献   

16.
Terry Deshler   《Atmospheric Research》2008,90(2-4):223-ICNAA07
Stratospheric aerosol, noted after large volcanic eruptions since at least the late 1800s, were first measured in the late 1950s, with the modern continuous record beginning in the 1970s. Stratospheric aerosol, both volcanic and non-volcanic are sulfuric acid droplets with radii (concentrations) on the order of 0.1–0.5 µm (0.5–0.005 cm− 3), increasing by factors of 2–4 (10–103) after large volcanic eruptions. The source of the sulfur for the aerosol is either through direct injection from sulfur-rich volcanic eruptions, or from tropical injection of tropospheric air containing OCS, SO2, and sulfate particles. The life cycle of non-volcanic stratospheric aerosol, consisting of photo-dissociation and oxidation of sulfur source gases, nucleation/condensation in the tropics, transport pole-ward and downward in the global planetary wave driven tropical pump, leads to a quasi steady state relative maximum in particle number concentration at around 20 km in the mid latitudes. Stratospheric aerosol have significant impacts on the Earth's radiation balance for several years following volcanic eruptions. Away from large eruptions, the direct radiation impact is small and well characterized; however, these particles also may play a role in the nucleation of near tropopause cirrus, and thus indirectly affect radiation. Stratospheric aerosol play a larger role in the chemical, particularly ozone, balance of the stratosphere. In the mid latitudes they interact with both nitrous oxides and chlorine reservoirs, thus indirectly affecting ozone. In the polar regions they provide condensation sites for polar stratospheric clouds which then provide the surfaces necessary to convert inactive to active chlorine leading to polar ozone loss. Until the mid 1990s the modern record has been dominated by three large sulfur-rich eruptions: Fuego (1974), El Chichón (1982) and Pinatubo (1991), thus definitive conclusions concerning the trend of non-volcanic stratospheric aerosol could only recently be made. Although anthropogenic emissions of SO2 have changed somewhat over the past 30 years, the measurements during volcanically quiescent periods indicate no long term trend in non-volcanic stratospheric aerosol.  相似文献   

17.
Considered is the process of ice nucleation in the atmosphere as a result of heterogeneous condensation of water vapor in surface inhomogeneities of aerosol particles and of subsequent heterogeneous crystallization of supercooled water accumulation. It is revealed that the size, structure, and composition of aerosol particles determine the thermal regime of crystallization.  相似文献   

18.
An atmospheric monitoring station is operated at Cape Matatula, American Samoa, by the Geophysical Monitoring for Climatic Change program under the National Oceanic and Atmospheric Administration. A nearly continuous record of condensation nucleus (CN) concentration and multiwavelength aerosol scattering extinction coefficient (sp) is available from mid-1977 to the present. This report presents the 1977–1983 data. The long-term mean of CN concentration is 274 cm-3 the long-term mean of sp (550 nm) is 1.54×10-5, and no significant long-term, annual, or diurnal trend is apparent in either data record.  相似文献   

19.
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20.
《Atmospheric Research》2009,91(2-4):125-131
Particle detection by condensation particle counters (CPCs) is ultimately limited by the onset of homogeneous nucleation. At vapour supersaturations around the homogeneous nucleation limit the diameter of critical clusters is typically about 2 nm. It is widely assumed that only particles larger than critical clusters can be activated by vapour condensation and the general detection limit of CPCs is therefore currently accepted to be around 2 nm particle diameter. Using an expansion type CPC with n-propanol as working fluid we investigated the transition from heterogeneous to homogeneous nucleation, clearly showing that particles are activated much before the onset of homogeneous nucleation, even at particle diameters as small as 1.4 nm. For particle diameters below 2 nm we have usually found condensation particle counting to be influenced by the simultaneous presence of ions as generated in a bipolar diffusion charger. In this paper we illustrate how the presence of ions influences particle number concentration measurement and how ions can be removed in order to obtain accurate seed particle number concentrations for particle diameters down to 1 nm.  相似文献   

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