Diffusion aerosol spectrometer

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.     

Particle size dependent response of aerosol counters

During an international workshop at the Institute for Experimental Physics of the University of Vienna, Austria, which was coordinated within the Committee on Nucleation and Atmospheric Aerosols (IAMAS-IUGG), 10 instruments for aerosol number concentration measurement were studied, covering a wide range of methods based on various different measuring principles. In order to investigate the detection limits of the instruments considered with respect to particle size, simultaneous number concentration measurements were performed for monodispersed aerosols with particle sizes ranging from 1.5 to 50 nm diameter and various compositions.The instruments considered show quite different response characteristics, apparently related to the different vapors used in the various counters to enlarge the particles to an optically detectable size. A strong dependence of the 50% cutoff diameter on the particle composition in correlation with the type of vapor used in the specific instrument was found. An enhanced detection efficiency for ultrafine hygroscopic sodium chloride aerosols was observed with water operated systems, an analogous trend was found for n-butanol operated systems with nonhygroscopic silver and tungsten oxide particles.     

Nolan–Pollak type CN counters in the Vienna aerosol workshop

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.     

Aerosol concentration measurement with multiple light scattering system and laser aerosol spectrometer

The performance of two different optical concentration-measuring techniques was investigated over a concentration range starting with about 10² cm⁻³ and extending over more than four decades. Both instruments are capable of real-time counting, however due to their particular design-single particle counter and ensemble particle-measuring system—they operate in overlapping, but different concentration ranges. The upper, coincidence-free counting limit for the single particle counter used in this study was established to be in the order of 10⁴ cm⁻³. The ensemble technique was found to be functional and stable for concentrations of about 10³ cm⁻³ and limited by the onset of multiple scattering at concentrations nearby 2×10⁶ cm⁻³. Within the determined boundaries, both techniques proved to provide reliable aerosol concentration data.     

On the effect of the chemical composition of atmospheric aerosol particles on nucleation scavenging and the formation of a cloud interstitial aerosol

Nucleation scavenging and the formation of a cloud interstitial aerosol (CIA) were theoretically studied in terms of the chemical composition of atmospheric aerosol particles. For this study, we used our air-parcel cloud model, which includes the entrainment of air and detailed microphysics, for determining the growth and interaction of aerosol particles and drops. Maritime and remote continental aerosol particle spectrums were used whose size distributions were superpositions of three log-normal distributions, each of a prescribed chemical composition. Our results show (1) that the CIA exhibits a size distribution with a distinctive cut-off at a specific radius of the dry as well as of the wet particle size distribution. All particles above this limiting size become activated to cloud drops and, thus, are not present in the CIA spectrum. This limiting size was found to be independent of the chemical composition of the particles and only dependent on the prevailing supersaturation. Below this specific size, the CIA spectrum becomes depleted of dry aerosol particles in a manner which does depend on their chemical composition and on the supersaturation in the air. (2) The number of aerosol particles nucleated to cloud drops depends critically on the chemical composition of the particles and on the prevailing supersaturation.     

An aerosol climatology of Samoa

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.     

On the growth of nitric and sulfuric acid aerosol particles under stratospheric conditions

We present a theory for the formation of frozen aerosol particles in the Antarctic stratosphere, the coldest region of the Earth's stratosphere. The theory is applied specifically to the formation of polar stratospheric clouds. We suggest that the condensed ices are composed primarily of nitric acid and water with small admixtures of other compounds such as H₂SO₄ and HCl in solid solution. Our assumed particle formation mechanism is in agreement with the magnitude and seasonal behavior of the optical extinctions observed in the winter polar stratosphere. Physical chemistry and thermodynamic considerations suggest that at temperatures between about 200 and 185 K, stratospheric particulates are composed primarily of frozen nitric acid solutions with a composition near that of the trihydrate. Available data suggest the particles are amorphous solid solutions and not in the crystalline hydrate form. At lower temperatures (i.e., below the forst point of pure water) cirrus-like ice clouds can form.     

Early stage of critical clusters growth in phenomenological and molecular dynamics simulation models

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.     

Charging state of atmospheric nanoparticles during the nucleation burst events

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.     

南京地区冬季大气冰核特征及其与气溶胶关系的研究

2011年11月15日～12月2日期间对南京地区近地面大气气溶胶和冰核进行了同步观测,综合分析了 冰核浓度的特征及其与气溶胶粒子浓度的关系。结果表明:活化温度T_a为-20℃,水面过饱和度为1%时,南京地区冰核浓度N_IN为0.352 L-1,与0.01～10 μm气溶胶数浓度比值仅为4×10-8。冰核活化温度越低,湿度越大,冰核浓度越高。雾和降雨对冰核都有明显的清除作用。对比不同气团对南京地区冰核的影响发现,偏东方向的污染气团中冰核以及气溶胶的浓度最高,但是来自西北地区的气团中冰核占气溶胶的比例最高,这可能是由于冰相核化能力较强的沙尘气溶胶导致的。分析冰核与不同粒径段气溶胶的相关性发现,较大粒径气溶胶的表面积浓度与冰核相关性更高,本文也得到了由活化温度T_a和粒径大于0.5 μm气溶胶数浓度N_{0.5～10 μm}共同计算冰核浓度的经验公式。     

A history and state-of-the-art of accommodation coefficients

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.     

气溶胶浓度对暖云不同生长阶段物理特征影响的模拟研究

基于云微物理过程完善的TAU2D分档云模式,模拟研究了用热泡扰动生成的暖云在不同气溶胶数浓度(Na)背景条件下各演变阶段云微物理量的变化特征。结果表明:在暖云的发展过程中Na越高,云滴尺度变小,云滴间的碰并增长发动较晚,云滴谱因碰并增长而实现的滴谱拓宽变弱,云滴谱相对较窄,云滴谱标准差较小,因此云体发展越缓慢,云体生命周期越长,形成降水就越晚;反之,云滴尺度越大,碰并增长发动越早,云滴谱拓宽更明显,云滴谱标准差越大,云体生命周期相对更短,降水开始时刻越早。高Na背景下,碰并阶段云滴谱较凝结阶段更宽,沉降阶段因云体下沉蒸发导致小尺度云滴减少,使其滴谱较碰并阶段略有拓宽。在凝结阶段,低气溶胶背景下云滴数浓度(N)和离散度(ε)间呈现正相关关系,而高气溶胶背景下两者为负相关关系。在碰并阶段,N与ε的相关性关系为负相关,且随着气溶胶数浓度的增加,负相关程度降低。在沉降阶段,N和ε间为负相关关系。     

Condensation particle counting below 2 nm seed particle diameter and the transition from heterogeneous to homogeneous nucleation

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.     

Incorporation of aerosol particles between 25 and 850 nm into cloud elements: measurements with a new complementary sampling system

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.     

气溶胶影响混合相对流云降水的数值模拟研究

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。     

中国东部气溶胶在天气尺度上的辐射强迫和对地面气温的影响

本文应用WRF-Chem(Weather Research and Forecasting—Chemistry)模式研究中国东部地区气溶胶及其部分组分(硫酸盐、硝酸盐和黑碳气溶胶)在天气尺度下的辐射强迫和对地面气温的影响。5个无明显降水时间段(2006年8月23～25日、2008年11月10～12日、2008年12月16～18日、2009年1月15～17日和2009年4月27～29日)的模拟显示,气溶胶浓度呈现显著的白天低,夜间高的日变化特征,且北方区域(29.8°～42.6°N,110.2°～120.3°E)平均PM_2.5近地面浓度(40～80 μg m-3)高于南方区域(22.3°～29.9°N,109.7°～120.2°E,30～47 μg m-3)。气溶胶对地面2 m温度(地面气温)有明显的降温效果,在早上08:00(北京时,下同)和下午17:00左右最为显著,最高可降低约0.2～1 K,同时气溶胶的参与改善了模式对地面气温的模拟。本文还通过对2006年8月23～25日一次个例的模拟,定量分析了气溶胶及其部分组分(硫酸盐、硝酸盐和黑碳气溶胶)的总天气效应(直接效应+间接效应)、直接效应和间接效应分别对到达地面的短波辐射和地面气温的影响。北方区域平均气溶胶直接效应所造成的短波辐射强迫要高于南方区域,分别为-11.3 W m-2和-5.8 W m-2,导致地面气温分别降低了0.074 K和0.039 K。南方区域平均气溶胶间接效应所产的短波辐射强迫高于北方区域,分别为-14.4 W m-2和-12.4 W m-2,引起的地面气温的改变分别为-0.094 K和-0.035 K。对于气溶胶组分,硫酸盐气溶胶的直接效应和间接效应的作用相当,其总效应在北方和南方区域平均短波辐射强迫分别为-7.0 W m-2和-10.5 W m-2,对地面气温的影响为-0.062 K和-0.074 K,而硝酸盐气溶胶的作用略小。黑碳气溶胶使得北方和南方区域平均到达地表的太阳短波辐射分别减少了6.5 W m-2和5.8 W m-2,而地表气温则分别增加了0.053 K和0.017 K,相比于间接效应,黑碳气溶胶的直接效应的影响更加显著。     

Impacts of aerosol chemical composition on microphysics and precipitation in deep convection

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 (S_c) 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, S_c 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.     

冰晶核化对雷暴云闪电行为影响的数值模拟研究

为了探讨冰晶核化对雷暴云闪电行为的影响,通过已有的三维对流云起、放电模式探讨对比了3种冰晶核化方案,分别为原模式中的经验公式YS方案及与气溶胶相关的DE方案和LP方案。研究表明冰晶核化方案对雷暴云内冰晶微物理发展特征、起电及放电过程均有一定影响。模拟结果显示:(1)考虑了气溶胶的两种新参数化方案中冰晶粒子在高温区(高于-13.8℃)出现,在雷暴云发展过程中DE方案和LP方案冰晶的垂直分布均大于YS方案。(2)DE方案和LP方案中高温区出现的冰晶所带电荷极性有明显的反转现象,导致雷暴云电荷结构产生差异;雷暴云发展旺盛时刻DE方案和LP方案出现三级性电荷结构,而YS方案在整个雷暴云过程都是偶极性,并且DE方案和LP方案中电荷空间分布区域更加广泛。(3)不同核化方案下雷暴云放电特征存在差异,YS方案在偶极性电荷结构背景下没有负地闪产生,而DE方案和LP方案中次正电荷区的存在促进了负地闪的发生,并且负先导出现在较低的高度范围内;DE方案和LP方案中电荷量级较大,因此云闪发生频次以及正、负先导传播次数增加明显。     

Hygroscopic growth of aerosol particles and its influence on nucleation scavenging in cloud: Experimental results from Kleiner Feldberg

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.     

Effects of seed particle size and composition on heterogeneous nucleation of n-nonane

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 WO_x, Ag and (NH₄)₂SO₄ particles were generated. For direct comparison between different particle compositions overlapping sizes have been generated for WO_x 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.