海盐气溶胶和硫酸盐气溶胶在云微物理过程中的作用

利用大气气溶胶和云分档模式研究海盐气溶胶和硫酸盐气溶胶在云微物理过程中的作用, 计算结果表明:云中液态水含量随高度的分布并不随海盐、硫酸盐的数目以及云团上升速度的变化而变化; 随着云滴数目的增加, 云滴的有效半径会减小; 硫酸盐对云滴数目影响起主导作用, 海盐在水汽相对充足情况下增加了云滴数目, 在水汽相对不足的情况下减少了云滴数目; 硫酸盐粒子浓度特别强的情况下 (人类活动污染比较严重时), 如果水汽相对不足, 云滴数目会明显小于硫酸盐粒子浓度; 而海盐粒子的存在, 加剧了水汽的供应不足, 从而可以在很大程度上进一步降低云滴数目。也就是说, 在有些情况下, 如果不考虑海盐气溶胶的作用, 硫酸盐气溶胶对云特性的影响会被过高估计。     

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.     

Equilibria of the marine multiphase ammonia system

A lack of empirical data has made it difficult to ascertain whether ammonia is in equilibrium between the oceanic, atmospheric gas and atmospheric particle phases in the remote marine environment. Reported here are simultaneous measurements of the saturation concentration of ammonia relative to ammonia concentrations in ocean surface waters; total seawater ammonia; atmospheric gas phase ammonia; and atmospheric particulate-phase ammonium, non-seasalt sulfate, methanesulfonate, and nitrate. Sampling was performed in May of 1987 in the northeast Pacific Ocean environment and in April and May of 1988 in the central Pacific Ocean environment.These measurements were used to determine the degree to which ammonia approached equilibrium between the oceanic and atmospheric gas and aerosol particle phases. The experimental atmospheric gas phase ammonia concentrations were compared with calculated equilibrium concentrations assuming a Henry's law type of partitioning between the gas and condensed phases. Characteristic times of the processes controlling the fate of ammonia in the marine environment also were compared.The measured atmospheric gas phase and oceanic concentrations of ammonia indicate that ammonia is not in a Henry's law equilibrium across the air/sea interface. This disequilibrium is a result of the long air/sea exchange equilibration time relative to the lifetime of ammonia in the atmosphere. Comparison of the calculated equilibrium gas phase ammonia concentrations with the measured gas phase ammonia concentrations shows that attainment of equilibrium between the atmospheric gas and particle phases is a strong function of the chemical composition of the aerosol particles. The data suggest that fully neutralized aerosol particles are not in Henry's law equilibrium with the gas phase while equilibrium is observed for particles with an average ammonium to non-seasalt sulfate molar ratio less than 1.8.     

Aerosol bacteria over the Southern Ocean during ACE-1

Individual bacterial cells occur in many samples that were collected at Cape Grim, Tasmania and during the Lagrangian “B” experiment of the Aerosol Characterization Experiment 1 (ACE-1) campaign that was conducted above the Southern Ocean. They are present in samples from altitudes as high as 5.4 km. Morphologically, almost all bacteria are rod-shaped, about 1 μm long or smaller, have one polar flagellum, and contain inclusions that are rich in P and K. Their morphological features suggest that these bacteria are motile, marine species. It seems likely that the cells became airborne by the same bubble-bursting mechanism that ejects sea-salt aerosol particles into the atmosphere; however, the bacteria and sea-salt particles are typically not aggregated with one another. The estimated number ratio of bacteria and the dominant aerosol species, sea salt, varies in the samples and averages about 1%. The aerosol bacteria seem to represent an important atmospheric reservoir of P and organic compounds; on the other hand, since they are externally mixed with sea salt, they are unlikely to be effective as cloud condensation nuclei.     

Single Particle Characterisation of the Aerosol in the Marine Boundary Layer and Free Troposphere over Tenerife, NE Atlantic, during ACE-2

In the framework of the 2nd Aerosol Characterization Experiment (ACE-2), in June and July 1997, size segregated samples were collected for single particle analysis on the island of Tenerife, in both the marine boundary layer (MBL) and the free troposphere (FT), to study the characteristics of the North Atlantic aerosol. A systematic assessment was made of the aerosol under background conditions and when the environment was perturbed by European emissions and/or Saharan dust. The aerosol particles were analysed by automated and manual SEM-EDX, followed by cluster analysis to identify the different particle types and their abundance. Basing on back trajectory calculations, particle numbers and volume concentrations, different periods can be identified regarding the origin of the sampled air masses. In the FT, the air masses were classified as clean Atlantic, Saharan dust from Africa or pollution from Europe. In the MBL, air masses were classified as clean, polluted or perturbed by emissions from Europe. For both the FT and MBL samples, the main changes in chemical composition were observed between the fine and coarse mode aerosol. The FT fine mode aerosol is dominated by S-poor aluminosilicates (62%) in the event of the dust samples or sulphates, carbonaceous particles (20%) and S-rich aluminosilicates (46%) in the polluted samples. For the larger fractions, a strong decreasing trend was observed for the sulphates (less than 20%) and carbonaceous particles (10%) in the polluted samples. The MBL fine mode was completely dominated by S-rich particles (polluted 55% and perturbed 59%), and to a lesser extent, carbonaceous and aged sea salt particles. In the coarse mode, the polluted air mass is dominated by sea salt particles (62%). Contrary to the fine fraction, the polluted air mass in the coarse fraction contained 5.3% of S-rich particles. The combined interpretation of the data from the analysis of size-fractioned particles and the calculated backward trajectories for air masses coming from Europe, Africa and the Atlantic, results in better insights on aerosol chemistry, especially for the comparison of the particle composition in the FT and the MBL.     

Continental impact on marine boundary layer coarse particles over the Atlantic Ocean between Europe and Antarctica

Aerosol samples were collected in the Atlantic marine boundary layer between the English Channel and Antarctica during November–December 1999. The composition of coarse (aerodynamic diameter 1–3 μm) individual aerosol particles was studied using the SEM/EDX method. The major particle types observed were fresh sea salt, sea-salt particles reacted partly or totally with sulphuric acid or nitric acid, Mg-sulphate, Ca-sulphate, mixed aluminosilicates and sea salt, aluminosilicates, Ca-rich particles and Fe-rich particles. The relative fractions of sea-salt particles with moderate or strong Cl depletion were high near the coasts of Europe (65–74%) and Northern Africa (44–87%), low far from the coast of Western Africa (10–20%) and very low in remote sea areas between Africa and Antarctica (1%). The Cl depletion was strongest when air masses arrived from the direction of anthropogenic pollution sources. The fractions of Mg-sulphate particles were high (18–25%) in 2 samples near Europe. The Mg-sulphate particles were probably formed as a result of fractional recrystallization of sea-salt particles in which Cl was substituted by sulphate. It remained unclear whether these particles were formed in the atmosphere or during and after sampling. The relative fractions of particles from continental sources were quite low (10–15%) near Europe, very high (25–78%) near the coast of Northwestern Africa and very low in the remote sea areas (0–2%). Most of the continental particles were aluminosilicates and some of them were internally mixed with sea salt. Near the coast of Northwestern Africa, the main source of aluminosilicates was Saharan dust, and near the Gulf of Guinea, emissions from biomass burning were also mixed with aluminosilicates and sea salt.     

利用GRAPES模式研究气溶胶对云和降水过程的影响

在GRAPES中尺度模式的双参数微物理方案中加入了气溶胶活化参数化过程,实现了对云滴数浓度的预报。选取不同季节两个降水过程进行模拟,并分别开展了不同气溶胶背景下的两个试验进行对比分析,研究气溶胶对云和降水可能的影响。结果表明:气溶胶浓度增加后,因为活化产生了更多尺度较小的云滴,抑制了云雨的自动转化,使大气中滞留了更多的云水,暖云降水减小;另一方面,云水的增加会使冰相粒子,尤其是雪和霰通过碰并云水等过程而增大,最后融化成雨增加冷云降水,同时冰相粒子增加会释放更多的潜热,促进上升气流的发展,进一步增加冷云降水。气溶胶对降水的影响存在空间不一致性,暖云较厚的地方暖雨过程受到的抑制明显,使地面降水减小,冷云厚度相对较厚时,冷云降水的增加会大于暖云降水的抑制,使地面降水增加。同时由于在云降水发展的不同阶段冷暖云的变化,气溶胶对降水的影响也存在着时间不一致性。     

播撒盐粉局部消除暖雾的数值模拟

本文使用二维暖雾数值模式来研究人工播撒盐粉局部消除暖雾的物理过程以及盐粉粒子半径、盐粉播撒量、雾层厚度和雾中液水含量对消雾效果的影响。结果表明,使用盐粉局部消除暖雾以增大播撒区的能见度是完全可能的。一般来讲,较大的盐粉粒子和较大的播撒量更有利于提高消雾的效果,但消雾的成本以及对环境的污染也随之加大。文章最后对使用大水滴代替盐滴进行消雾的可能性提出初步的看法。      

Role of the volatile fraction of submicron marine aerosol on its hygroscopic properties

The hygroscopic growth factor (HGF) of 85 nm and 20 nm marine aerosol particles was measured during January 2006 for a three-week period within the frame of the EU FP6 project MAP (Marine Aerosol Production) winter campaign at the coastal site of Mace Head, using the TDMA technique. The results are compared to aerosol particles produced in a simulation tank by bubbling air through sea water sampled near the station, and through synthetic sea water (inorganic salts). This simulation is assimilated to primary production. Aitken and mode particles (20 nm) and accumulation mode particles (85 nm) both show HGF of 1.92 and 2.01 for particles generated through bubbling in natural and artificial sea water respectively. In the Aitken mode, the marine particles sampled in the atmosphere shows a monomodal HGF slightly lower than the one measured for sea salt particles artificially produced by bubble bursting in natural sea water (HGF = 1.83). This is also the case for the more hygroscopic mode of accumulation mode particles. In addition, the HGF of 85 nm particles observed in the atmosphere during clean marine sectors exhibits half of its population with a 1.4 HGF. An external mixture of the accumulation mode marine particles indicates a secondary source of this size of particles, a partial processing during transport, or an inhomogeneity of the sea water composition. A gentle 90 °C thermo-desorption results in a significant decrease of the number fraction of moderately hygroscopic (HGF = 1.4) particles in the accumulation mode to the benefit of the seasalt mode, pointing to the presence of semi-volatile compounds with pronounced hydrophobic properties. The thermo-desorption has no effect on the HGF of bubble generated aerosols, neither for synthetic or natural sea water, nor on the atmospheric Aitken mode, indicating that these hydrophobic compounds are secondarily integrated in the particulate phase. No difference between night and day samples is observed on the natural marine aerosols regarding hygroscopicity, but a more pronounced sensitivity to volatilization of the 1.4 HGF mode in the accumulation mode is observed during the day.     

Temporal and spatial variations of marine aerosols over the Atlantic Ocean

Aerosol samples, collected daily were analyzed with electron microscopy for particle concentration and size distribution. The chemical compositions of individual particles were determined with X-ray energy spectrometry and specific morphological tests. The results demonstrated clear and significant dependencies of aerosol properties on air trajectories computed from a backtrack model. Air parcels, such as American air pollution and Sahara dust, were identified. Their physical mixing and chemical reactions with marine aerosols as well as aerosol wet deposition are discussed.     

Biogenic and anthropogenic organic matter in aerosol over continental Europe: source characterization in the east Baltic region

An Aerodyne quadruple aerosol mass spectrometer (Q-AMS) has been used to provide on-line measurements of size dependent chemical composition of fine aerosol particles (PM₁) at the Air Pollution Research Station in Preila, Lithuania, representing the east Baltic region. The size dependent chemical composition measurements by AMS have revealed that in marine air masses 118?nm mode organics-containing particles were fresher compared to sulfate-containing particles (295?nm), likely originated as secondary aerosol from forest emissions or produced by primary sea spray over the Baltic Sea. In polluted continental air masses sulfate and organics were highly internally mixed and aged. The mass spectral results indicated that the major components of organic compounds were oxygenated organic species with strong signals at m/z 18, 43, 44 with several specific features. Positive matrix factorization (PMF) of AMS organic mass spectral data has identified three factors: aged oxygenated low-volatility organic aerosol (LV-OOA), less oxygenated semi-volatile organic aerosol (SV-OOA), and biogenic organic aerosol (BGOA) of either terrestrial or marine origin. The measurements were compared with a real-time particulate matter Beta Absorption Monitor (Thermo ESM Andersen) and Micro Orifice Uniform Deposit Impactor (MOUDI) data. The intercomparison showed a good correlation and a stable ratio between PM₁ and PM_2.5 concentrations. A comparison of the on-line Q-AMS data and the off-line MOUDI fine particle (<1???m) data yielded a reasonable agreement in size distributions but not the absolute mass concentrations due to sampling conditions, evaporation of acidic species from sampling substrates and bounce of the particles in the MOUDI.     

Chloride and Bromide Loss from Sea-Salt Particles in Southern Ocean Air

Datasets on aerosol composition in Southern Ocean air at Cape Grim and Macquarie Island, and rainwater composition at Cape Grim, have been analysed for sea-salt components in order to test the validity of the multiphase autocatalytic halogen activation process proposed initially by Sander and Crutzen (1996) and developed fully for clean marine air by Vogt et al. (1996). Four distinct datasets from the two locations were analysed. All four datasets provided consistent evidence in support of three predictions of the autocatalytic model: (1) overall Cl- deficits in sea-salt aerosol were small, difficult to quantify against analytical uncertainty and at most a few percent; (2) Br- deficits were large, averaging –30% to –50% on an annual basis, with strong seasonality ranging from about –10% in some winter samples to –80% or more in some summer samples; and (3) the Br- and Cl- deficits were clearly linked to the availability of strong, S-acidity in the aerosol, confirming the importance of acid catalysis to the dehalogenation process.     

Modelling of the nighttime nitrogen and sulfur chemistry in size resolved droplets of an orographic cloud

A chemistry module has been incorporated into a Lagrangian type model that computes the dynamics and microphysics of an orographical cloud formed in moist air flowing over the summit of Great Dun Fell (GDF) in England. The cloud droplets grow on a maritime aerosol which is assumed to be an external mixture of sea-salt particles and ammonium-sulfate particles. The dry particle radii are in the range 10 nm<r<1 µm. The gas-phase chemical reaction scheme considers reactions of nitrogen compounds that are important at night. The treatment of scavenging of gases into the aqueous phase in the model takes into account the different solubilities and accommodation coefficients. The chemistry in the aqueous phase focusses on the oxidation of S(IV) via different pathways.Sensitivity analyses have been performed to investigate deviations from gas-liquid equilibria according to Henry's law and also to study the influence of iron and of nitrogen compounds on the aqueous-phase oxidation of dissolved SO₂. When addressing these questions, special attention has been given to the dependence on the droplet size distribution and on the chemical composition of the cloud condensation nuclei on which the droplets have formed. It was found that the oxidation of S(IV) via a chain reaction of sulfur radicals can be important under conditions where H₂O₂ is low. However, major uncertainties remain with respect to the interaction of iron with the radical chain. It was shown that mixing of individual cloud droplets, which are not in equilibrium according to Henry's law, can result in a bulk sample in equilibrium with the ambient air. The dependence of the aqueous-phase concentrations on the size of the cloud droplets is discussed for iron, chloride and NO₃.     

Modification of sea-salt aerosols over the coastal area in china

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Observed changes in aerosol physical and optical properties before and after precipitation events

Precipitation scavenging of aerosol particles is an important removal process in the atmosphere that can change aerosol physical and optical properties. This paper analyzes the changes in aerosol physical and optical properties before and after four rain events using in situ observations of mass concentration, number concentration, particle size distribution, scattering and absorption coefficients of aerosols in June and July 2013 at the Xianghe comprehensive atmospheric observation station in China. The results show the effect of rain scavenging is related to the rain intensity and duration, the wind speed and direction. During the rain events, the temporal variation of aerosol number concentration was consistent with the variation in mass concentration, but their size-resolved scavenging ratios were different. After the rain events, the increase in aerosol mass concentration began with an increase in particles with diameter 0.8 μm [measured using an aerodynamic particle sizer(APS)], and fine particles with diameter 0.1 μm [measured using a scanning mobility particle sizer(SMPS)]. Rainfall was most efficient at removing particles with diameter ～0.6 μm and greater than 3.5 μm. The changes in peak values of the particle number distribution(measured using the SMPS) before and after the rain events reflect the strong scavenging effect on particles within the 100–120 nm size range. The variation patterns of aerosol scattering and absorption coefficients before and after the rain events were similar, but their scavenging ratios differed, which may have been related to the aerosol particle size distribution and chemical composition.     

Evaluation of a new aerosol model with a Brownian diffusion technique

Measurements in Alaska in sub-polar night conditions have indicated that the size distribution of atmospheric aerosols varies significantly and systematically depending upon the type of air mass. Atmospheric aerosol particles are small and numerous in warm Pacific marine air mass systems and large and sparse in cold, Arctic-derived air mass systems. In a previous paper this was hypothesized to be associated with the progressive loss of the smallest particles by attachment to cloud droplets under the driving influence of thermal Brownian motion. A theory involving two parameters, (mean particle radius), and n₀ (aerosol number concentration) was developed to describe the process. In the previous paper, the relationship where ν is the Junge power law exponent (ν 3) was derived and has recently been confirmed to acceptable accuracy with the use of a simple experiment which employed diffusive separation. The diffusion experiment has also allowed us to estimate that the fraction of time, φ, that the aerosol-laden polar air masses coexist in the presence of cloud is 0.01 < φ < 0.1. The submicron aerosol particles in Arctic-derived air masses flowing into central Alaska are deduced to have residence times on the order of 10 days.     

对流云对大气气溶胶和相对湿度变化响应的数值模拟

利用二维面对称分档云模式研究了气溶胶颗粒物浓度和尺度谱分布对混合相对流云微物理过程和降水的影响, 并重点讨论了气溶胶效应随环境相对湿度的变化。结果表明, 在初始热力和动力条件相同的情况下, 相对清洁的海洋性云在发展和成熟阶段能更有效地产生雨滴、 冰晶和霰粒, 形成更强的雷达反射率。随着气溶胶浓度增加, 比如在本文模拟的污染大陆性云中, 气溶胶粒子数浓度的增加限制云滴增长, 不利于降水粒子的形成。模拟结果也发现, 环境相对湿度对气溶胶效应有显著影响, 即当地面相对湿度从50%增大到70%时, 所模拟的云从浅对流泡发展为深对流云; 气溶胶对云微物理特性和降水的影响在干空气中较小, 但在湿空气中表现非常显著, 这与前人结果一致。随着相对湿度的增加, 冰相粒子出现的时间提前, 增长加快, 云砧范围扩大, 但相对来说, 降水起始时间对相对湿度的变化比气溶胶更敏感。     

The investigations of aerosol particle formation in urban background area of Helsinki

In this study the possible conditions for new aerosol particle formation in a background area of Helsinki have been analysed. The measurements of aerosol particle size distribution, main gaseous pollutant compounds, UV spectra and meteorological parameters were performed during April–May 1993. The main interest was concentrated on the investigations of photochemical OH radical formation, the oxidation of gas phase SO₂ to H₂SO₄ and the formation of H₂SO₄---H₂O aerosol particles. The measurements were analysed using a model for OH radical formation and aerosol dynamics. The analysis of aerosol size distributions was carried out using positive matrix factorization. The main conclusion is that based on our model analysis no evidence of new particle formation in the vicinity of the measurement station was found. However, the high concentrations of aerosol particles in the ultrafine size range indicate that some other particle formation pathways are to be considered.     

Scattering Properties of Atmospheric Aerosols over Lanzhou City and Applications Using an Integrating Nephelometer

The data, measured by a three-wavelength Integrating Nephelometer over Lanzhou City during the winters of 2001/2002 and 2002/2003 respectively, have been analyzed for investigating the scattering properties of atmospheric aerosols and exploring their relationship and the status of air pollution. The aerosol particle volume distribution is inverted with the measured spectral scattering coefficients. The results show that the daily variation of the aerosol scattering coefficients is in a tri-peak shape. The average ratio of backscattering coefficient to total scattering coefficient at 550 nm is 0.158; there exists an excellent correlation between the scattering coefficients and the concentration of PM10. The average ratio of the concentration of PM10 to the scattering coefficients is 0.37 g m-2, which is contingent on the optical parameters of aerosol particles such as the size distribution, etc.; an algorithm is developed for inverting the volume distribution of aerosol particles by using the histogram and Monte-Carlo techniques, and the test results show that the inversion is reasonable.     

南京一次重霾天气纳米气溶胶观测研究

为加深对南京地区重霾天气过程纳米尺度气溶胶物理特征的了解,对2017年12月21-25日的一次重霾天气过程进行了综合探测,利用宽范围粒径谱仪观测了此次过程中10～1000 nm颗粒物数浓度,并结合能见度等气象要素,对重霾期间纳米气溶胶谱分布进行了分析.结果 表明:此次霾重污染过程出现在低温、高湿、气压上升期间;与非重污...