共查询到20条相似文献，搜索用时 31 毫秒
1.
《Atmospheric Research》2007,83(3-4):489-502
We compare two molecular Monte Carlo simulation methods, the discrete summation method and the growth/decay method, which calculate the vapor-liquid nucleation free energy barrier by simulating isolated clusters of fixed size without the surrounding vapor. The methods are applied to calculations of nucleation barriers of Lennard–Jones argon at 60 K and 80 K. Both of these methods are computationally efficient, as only isolated clusters without the surrounding vapor are simulated, and the methods can be applied with any given cluster definition. They give equivalent results to other methods where the vapor phase is also included. The discrete summation method is based on the calculation of the difference in free energies between two systems containing an n-cluster and an (n − 1)-cluster plus one non-interacting (free) molecule. We show that the configurational space is not equivalent in the two systems. Hence, there has to be an additional term in the free energy calculation that accounts for several kT in magnitude. In contrast to previous studies we also show that it is not correct to prevent the overlap of the non-interacting molecule and another molecule by a zero or an arbitrarily small repulsive potential, but with a small excluded space around the free molecule. 相似文献
2.
A.-K. Viitanen T. Mattila J.M. Mkel M. Marjamki O. Anttalainen J. Keskinen 《Atmospheric Research》2008,90(2-4):115-ICNAA07
Ion mobility spectrometry offers a robust and effective technique to study ion clusters in ambient conditions. Here, we have experimentally studied the influence of temperature on the positive ion cluster formation of 2-propanol vapor in air, along with parallel measurements for n-butyl acetate vapor in air. For both of these low proton affinity compounds in the ppm concentration range, temperatures below 0 °C tend to favor formation of dimers and trimers. The measurements indicate that approximate estimations for the fractions of these n-mers (n > 1) in the ion spectra, can be obtained by classical theory for ion induced nucleation. Presence of natural background vapors however slightly blurs the data, especially for the fraction of monomers, so that accurate prediction of the fractions of n-mers in the spectra would require more accurate information on the gas composition. The findings concerning thermal behavior of ions help to understand better ion phenomena also in field conditions. 相似文献
3.
《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
4.
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
5.
Study of tropical cyclogenesis using satellite data 总被引：1，自引：1，他引：0
Summary Satellite data are used to study the cloud development and water vapor supply during the genesis of Typhoon Nina (November 1987). Using satellite microwave and infrared data, the following physical parameters are retrieved and analyzed: water vapor path, surface wind, sea surface evaporation, precipitation, and cloud type.During the week prior to the genesis of Nina, several cloud clusters were observed in the region of the subsequent genesis (near 5° N, 170° E). Cloud type studies showed that several clusters had similar structures. By examining the sea surface evaporation and precipitation in the cloud clusters, we found that the precipitation exceeded evaporation by several times in the precipitating areas of the cluster that evolved into a tropical storm, indicating that local evaporation alone could not supply enough water vapor, and that horizontal transfer of water vapor from surrounding areas is required for the tropical cyclogenesis. Surface wind fields indicated that there was a constant increase of cyclonic wind in the area of the cloud cluster that finally led to the tropical storm, while no apparent increase of wind was found in the other cloud clusters. In addition, water vapor amount did not decrease for several days until the disturbance was upgraded to a tropical storm, while it was found to decrease after the mature stage for the other cloud clusters that did not evolve into tropical storms.From consideration of the water vapor balance, the cyclogenesis can be interpreted as a transition from an unbalanced cluster to a balanced cluster. Horizontal transfer of water vapor in a water vapor-unbalanced cloud cluster is not large enough to overcome the deficit caused by precipitation over evaporation. The shortage of water vapor in the unbalanced cluster results in a short-lived cloud cluster. When the sum of evaporation and horizontal transfer can provide enough water vapor supply to balance the removal by precipitation (balanced cluster), the precipitation does not dry up the atmosphere. This is the necessary condition for the cyclogenesis. The increase in horizontal transfer of water vapor is found in this study to be associated with the increase of the surface cyclonic wind.With 5 Figures 相似文献
6.
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
7.
《Atmospheric Research》2009,91(2-4):187-194
Heterogeneous nucleation of supersaturated n-nonane vapour on seed particles of different size and composition has been investigated using a fast expansion chamber. Monodisperse seed particle sizes were ranging from about 4 nm up to about 24 nm in diameter. By using different types of particle generators WOx, Ag and (NH4)2SO4 particles were generated. For direct comparison between different particle compositions overlapping sizes have been generated for WOx and Ag at about 7 nm particle diameter as well as for Ag and (NH4)2SO4 at about 15 nm. Nucleation temperature was kept constant at about 278 K. Experimental data were compared to Kelvin equation and Fletcher theory including the effect of line tension. It was found that heterogeneous nucleation of n-nonane seems to be independent of seed particle composition and starts well below the Kelvin curve. Good agreement was achieved with Fletcher theory including the effect of line tension. 相似文献
8.
Jiabin Zhou Tieguan Wang Yanping Zhang Ningning Zhong Patricia M. Medeiros Bernd R.T. Simoneit 《Atmospheric Research》2009,93(4):849-861
The solvent-extractable organic compounds of atmospheric PM10 samples, collected over two years beginning in 2003 at urban and suburban sites of Beijing, were characterized using gas chromatography–mass spectrometry (GC–MS). The elemental carbon (EC) contents were determined and ranged from 4.3 to 42 μg m− 3. Organic compounds in total extracts were identified and included unresolved complex mixture (UCM) and series of n-alkanes, n-alkanols, n-alkanoic acids, polycyclic aromatic hydrocarbons (PAHs); saccharides, alkanedioic acids, steroids, and other biomarkers and source tracers. The seasonal variations of their relative abundances are discussed. The abundance order for the major molecular classes in the particulate organic matter (POM) was the following: UCM > saccharides > n-alkanoic acids >n-alkanes > n-alkanols > PAHs > hydroxy-PAHs > other biomarker tracers. Based on the genetic significance of the molecular tracers, the dominant sources of POM are proposed for the two sampling sites. The emissions from fossil fuel use (both coal and petroleum products), biomass combustion, other pyrolysis sources, higher plant wax, and secondary products contribute > 98.0% of the POM mass. The fossil fuel use (average = 65% of POM) is the largest contributor and derives mainly from vehicular traffic. 相似文献
9.
Heterogeneous nucleation and condensation of dibutylphthalate, octadecane, octadecanol, and octadecanoic acid vapors at various pressures on insoluble AgCl and Ag nanoparticles in a turbulent mixing condensation nuclei counter (TMCNC) have been studied theoretically. A method to interpret the particle size distributions measured with a DMA and estimate the parameters for nucleation on single particles is proposed. Based on this semi-empirical method, the Gibbs free energy is calculated and a rate of heterogeneous nucleation on single particles is estimated directly from the experimental “condensation spectra” of inactive and active CN using the DMA data. In some cases, the dependence of the Gibbs nucleation energy on the vapor supersaturation had two maximums and one minimum, instead of one maximum as described by Gibbs' classical thermodynamics of phase transitions. This phenomenon, called “double barrier nucleation” (DBN) is caused by the surface heterogeneity of nano-CN; this is first experimental verification of DBN that had been previously predicted theoretically. Two types of heterogeneity may be present: topographic or energetic. Focusing on energetic heterogeneity, a theoretical model of DBN for spherical geometry is developed. The surface heterogeneity for insoluble nano-sized CN is shown to be critical to explaining the unusual transformation of a monomodal size distribution of inactive CN into a bimodal distribution of activated CN when coagulation is excluded. Future studies will be directed toward more data for further refining the theory and developing a model that simultaneously accounts for both types of surface heterogeneity of nano-CN. 相似文献
10.
11.
《Atmospheric Research》2009,91(2-4):151-158
The relevance of ion-induced nucleation of sulfuric acid and water (IINSW) in the troposphere over the boreal forest at northern latitudes is investigated by combining two existing and previously published models (MALTE — model to predict new aerosol formation in the lower troposphere; PARNUC — a parameterized steady-state model of neutral and ion-induced nucleation of sulfuric acid and water for atmospheric conditions). Simulations were performed for 4 days with observed new particle formation at ground level by using input data from the SMEAR II station in Hyytiälä, Finland. The selected days were chosen to cover a wide range of values of the parameters most relevant for IINSW. The results showed that ion-induced nucleation of sulfuric acid and water can contribute up to 15% to the total amount of newly formed particles in the size range of 3–10 nm inside the mixed layer at the Hyytiälä site. The importance of IINSW seemed to increase in the free troposphere above the boundary layer, however, lack of measurements in the vertical structure of the input parameters suggest that the model results are burdened with high uncertainties. 相似文献
12.
This paper presents the development of a simple and precise analytical method for the determination of nitrogen dioxide in ambient air. In this method nitrogen dioxide is determined in the form of nitrite. The determination of nitrogen dioxide needs no reagents except for a solution of sodium hydroxide mixed with sodium arsenite (NaOH–Na2As2O3) which is used as an absorbing reagent for trapping the nitrogen dioxide from the atmosphere in the form of nitrite, i.e., a prior analysis step. The determination of submicrogram levels of nitrogen dioxide is based on the selection of a strong and sharp quantitative analytical peak at 1380 cm− 1 using diffuse reflectance infrared spectroscopy (DRS-FTIR). The limit of detection (LOD) and the limit of quantification of the method are found to be 0.008 μg g− 1 NO2− and 0.05 μg g− 1 NO2−, respectively. The precision in terms of standard deviation and relative standard deviation value at a level of 2 μg NO2− / 0.1 g KBr for n = 10 is found to be 0.036 μg NO2− and 1.8%, respectively. The relative standard deviation (n = 10) for the determination of nitrogen dioxide in ambient air was observed to be in the range 2.6–3.8%. The method proposed is time-saving and eliminates the slow and cumbersome steps of pH maintenance of the reaction mixture and color formation of the EPA recommended spectrophotometric and other methods for quantitative determination of nitrogen dioxide. 相似文献
13.
Growth of homogeneously nucleated water droplets: a quantitative comparison of experiment and theory
The formation of aerosols proceeds through nucleation, growth and aging stages. The understanding of nucleation and droplet growth is essential for handling the more complex atmospheric condensation processes. To achieve this goal, measurements of the nucleation rate of various systems are performed in an expansion chamber. In this manner nucleation and growth are decoupled by applying a short nucleation pulse of about 1 ms during which the nuclei are formed. The subsequent droplet growth is quantitatively monitored by Mie-scattering. To this end, the Mie-maxima and -minima are detected as a function of time and compared to theoretical Mie-scattering calculations for increasing radii. In this fashion, a wealth of growth curves for pure water depending on supersaturations, number densities of droplets, and temperatures were obtained. Following the approach of Fuchs and Sutugin [Fuchs, N.A., Sutugin, A.G., 1970. Highly Dispersed Aerosols. Ann Arbor Science Publishers, Ann Arbor; Fuchs, N.A., Sutugin, A.G., 1971. In: Hidy, G.M., Brock, J.R. (Eds.), International Reviews in Aerosol Physics and Chemistry: Topics in Current Aerosol Research (Part 2), Pergamon, New York, p. 1], we calculated theoretical growth curves taking into account the depletion of water vapor, the increase of droplet- and system-temperature, temperature-dependent functions of the diffusion coefficient, surface tension, liquid density and latent heat of condensation. The calculated growth curves and experimental data for 230, 240 and 250 K with number densities of droplets between 5×102 and 2×106 droplets/cm3 yield quantitative agreement between theory and experiment. This is remarkable in so far as the theory contains no adjustable parameters and assumes the sticking probability of the vapor molecules to be unity. Using a sticking probability smaller than 0.8 in the calculation leads to growth functions already outside the experimental error. 相似文献
14.
从周边建筑物对所考虑建筑物的扩大宽度影响的角度,分析了周边有等高、更低或更高的其他建筑物3种情况下,周边建筑物对所考虑的建筑物截收面积的实际影响.在此基础上提出了周边建筑物的高度、相对位置、环绕程度等均对建筑物截收面积有较大影响,并不能将其乘以一个恒定的位置因子作为考虑了周边建筑物的影响,应根据建筑物所处环境的实际情况的不同做更为精确的计算,以提高风险评估的准确性. 相似文献
15.
A model of ice heterogeneous nucleation is developed basing on assumption of embryo–size quasi–static distribution. When the
system becomes meta-stable (increased supersaturation or supercooling), the largest embryos become viable. The viable embryo
number and generation rate are estimated for direct sublimation of vapor onto the surface of the ice–generating nucleus and
for immersion freezing. The calculation results are compared against experimental data. 相似文献
16.
Early stage of critical clusters growth in phenomenological and molecular dynamics simulation models
Romuald Puzyrewski Jaros&#x;aw Rybicki Micha&#x; Bia&#x;oskrski 《Atmospheric Research》2006,82(3-4):465
The growth of critical clusters is discussed in the paper according to the classical and molecular dynamics (MD) approaches. A new formula for molecule numbers in critical clusters has been derived within the framework of the classical approach. A set of equations controlling the early stage of growth in a neighborhood of a critical size is presented. As far as molecular dynamics simulation is concerned, a computational technique based on the DL_POLY code is described in brief. Computation results are presented concerning cluster formation of H2O vapor, distribution of clusters versus time, cluster growth and radial density distribution of isolated clusters. A comparison with the classical results is made for a case of dense vapor, where the mechanism of strong condensation is predominant. The Hertz–Knudsen formula seems to be verified by the molecular dynamics results. 相似文献
17.
《Dynamics of Atmospheres and Oceans》2001,33(2):79-94
A wave dynamics for the super cloud clusters associated with the tropical intraseasonal oscillation is constructed. Under the present framework, the basic state of super cloud clusters is considered to be a large-scale convergence of the zonal wind. This convergence is created by a nonlinear diabatic Kelvin wave front, which moves eastward slowly without change of shape. When interacting with free equatorial waves with n=−1, 0, 1 and 2, this basic flow will suppress those waves which move eastward except for free Kelvin waves, and permit westward propagating modes such as the mixed Rossby-gravity wave, the inertio-gravity waves with n=1 and 2 to appear in the large-scale convergent region. Among these waves, only fast modes, that is, inertio-gravity waves with n=1 and 2 are regarded to be responsible for the presence of cloud clusters which move westward within a super cloud cluster, while the multiplicity of the occurrences of super cloud clusters, which move eastward within the large-scale convergent region, is due to the superposition of free Kelvin wave upon these inertio-gravity waves. 相似文献
18.
Early stage of critical clusters growth in phenomenological and molecular dynamics simulation models
《Atmospheric Research》2007,83(3-4):465-480
The growth of critical clusters is discussed in the paper according to the classical and molecular dynamics (MD) approaches. A new formula for molecule numbers in critical clusters has been derived within the framework of the classical approach. A set of equations controlling the early stage of growth in a neighborhood of a critical size is presented. As far as molecular dynamics simulation is concerned, a computational technique based on the DL_POLY code is described in brief. Computation results are presented concerning cluster formation of H2O vapor, distribution of clusters versus time, cluster growth and radial density distribution of isolated clusters. A comparison with the classical results is made for a case of dense vapor, where the mechanism of strong condensation is predominant. The Hertz–Knudsen formula seems to be verified by the molecular dynamics results. 相似文献
19.
本文利用再分析资料、GDAS等资料,引入HYSPLIT模式定性定量地分析泸州9月7～8日特大暴雨过程的水汽输送特征,并对水汽来源进行了模拟。结果表明:(1)该过程是由高空低槽、低涡切变以及低空急流共同影响导致的,强降水发生区域与850hPa低涡位置具有很好的对应关系。(2)影响此次强降水的水汽主要来源于南海、孟加拉湾和贵州、湖南等周边省份,其中周边省份的本地水汽贡献最大,850hPa(1500m)上水汽贡献率达44%,孟加拉湾和南海两者的水汽贡献率也达到了39%。(3)三维空间显示水汽主要来源于850hPa高度附近或以下区域。 相似文献
20.
《Atmospheric Research》2009,91(2-4):132-150
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