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。     

Balloon-Borne Optical Counter for in Situ Aerosol Measurements

A new balloon-borne optical particle counter has been developed to make in situ measurements of stratospheric aerosols. The intensity of light scattered at 60° from the forward direction by individual particles is measured. Aerosol number concentrations in seven size channels can be inferred. The counter has been calibrated using polystyrene and polyvinyl toluene latex spheres. There is good agreement between measured and calculated individual pulse intensities for aerosol with radii from 0.16 to 2.6 µm. The size resolution is limited by broadening of the pulse count/pulse height spectrum, arising mainly from the photoelectron statistics of photomultipliers. Stratospheric aerosol measurements have been made using this instrument at Kiruna (68°N, 21°E), Sweden, in February 1995, and at Aire sur l'Adour (44°N, 0°W), France, in 1992, 1993, and 1994. The uncertainties in the measurements are discussed. The retrieved aerosol concentrations and size distributions are presented, and shown to be broadly consistent with measurements made by the University of Wyoming optical particle counter.     

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.     

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.     

Surface aerosol measurements at Barrow during AGASP-II

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).     

Highly Biased Hygroscopicity Derived from Size-Resolved Cloud Condensation Nuclei Activation Ratios without Data Inversion

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.     

Airborne and lidar measurements of aerosol and cloud particles in the troposphere over Alert Canada in April 1986

As a component of the Canadian Arctic Haze Study, held coincident with the second Arctic Gas and Aerosol Sampling Program (AGASP II), vertical profiles of aerosol size distribution (0.17 m), light scattering parameters and cloud particle concentrations were obtained with an instrumented aircraft and ground-based lidar system during April 1986 at Alert. Northwest Territories. Average aerosol number concentrations range from about 200 cm^–3 over the Arctic ice cap to about 100 cm^–3 at 6 km. The aerosol size spectrum is virtually free of giant or coarse aerosol particles, and does not vary significantly with altitude. Most of the aerosol volume is concentrated in the 0.17–0.50 m size range, and the aerosol number concentration is found to be a good surrogate for the SO₄ ⁼ concentration of the Arctic haze aerosol. Comparison of the aircraft and lidar data show that, when iced crystal scattering is excluded, the aerosol light scattering coefficient and the lidar backscattering coefficient are proportional to the Arctic haze aerosol concentration. Ratios of scattering to backscattering, scattering to aerosol number concentration, and backscattering to aerosol number concentration are 15.3 steradians, 1.1×10^–13 m², and 4.8×10^–15 m² sr^–1, respectively. Aerosol scattering coefficients calculated from the measured size distributions using Mie scattering agree well with measured values. The calculations indicate the aerosol absorption optical depth over 6 km to range between 0.011 and 0.018. The presence of small numbers of ice crystals (10–20 crystals 1^–1 measured) increased light scattering by over a factor of ten.     

Modeling Marine Stratocumulus with a Detailed Microphysical Scheme

A one-dimensional 3rd-order turbulence closure model with size-resolved microphysics and radiative transfer has been developed for investigating aerosol and cloud interactions of the stratocumulus-topped marine boundary layer. A new method is presented for coupling between the dynamical model and the mierophysical model. This scheme allows the liquid water related correlations to be directly calculated rather than parameterized. On 21 April 2001, a marine stratocumulus was observed by the Caesar aircraft over the west Pacific Rim south of Japan during the 2001 APEX/ACE-Asia field measurements. This cloud is simulated by the model we present here. The model results show that the general features of the stratocumulus-topped marine boundary layer predicted by the model are in agreement with the measurements. A new onboard cloud condensation nuclei (CCN) counter provides not only total CCN number concentration (as the traditional CCN counters do at a certain supersaturation) but also the CCN size distribution information. Using these CCN data, model responses to different CCN initial concentrations are examined. The model results are consistent with both observations and expectations.The numerical results show that the cloud microphysieal properties are changed fundamentally by different initial CCN concentrations but the cloud liquid water content does not differ significantly. Different initial CCN loadings have large impacts on the evolution of cloud microstructure and radiation transfer while they have a modest effect on thermodynamics. Increased CCN concentration leads to significant decrease of cloud effective radius.     

Studies of ice nucleation by Arctic aerosol on AGASP-II

Aerosol particles were collected on filters for studies of their ability to nucleate ice during the second Arctic Gas and Aerosol Sampling Program (AGASP-II) in April, 1986. The ice nuclei (IN) samples were collected from an aircraft at altitudes ranging from the surface to the vicinity of the tropopause in Arctic locations over Alaska, northern Canada and Greenland. Samples of other components of the aerosol were collected and measurements were made of other properties of the aerosol coincident in time with the IN samples. The IN filters were exposed to water saturation in a dynamic developing chamber at –15° C and –25° C. Ice crystals grew on the IN and were counted on the filters at discrete time intervals during the exposure period to determine the rate of ice nucleation and the final concentration of (IN). Results show that Arctic haze aerosol, identified by pollutant signatures, had lower IN concentrations, a lower IN to total aerosol fraction and slower ice nucleation rates than aerosol which had a chemical signature more indicative of the remote unpolluted troposphere. These observations suggest that the Arctic haze aerosol does not efficiently form ice in the arctic troposphere. This may be a factor contributing to the long-range transport of Arctic haze.     

Stratospheric aerosol sulfuric acid: First direct in situ measurements using a novel balloon-based mass spectrometer apparatus

The first direct in situ measurements of the sulfuric acid contained in stratospheric aerosol particles were made using a novel balloon-based Ion Molecule Reaction Mass Spectrometer instrument (IMRMS) equipped with an aerosol vaporizer. The IMRMS method employed offers direct aerosol sulfuric acid measurements with high spatial resolution. The balloon flight took place on 23 October 1995 in middle latitudes (44°N) and reached a maximum altitude of 24 km. Measured molecular number densities of aerosol sulfuric acid decreased with increasing altitude from about 2.9 × 109 cm-3 at 15km altitude to about 2.4 × 108 cm-3 at 21 km. Corresponding mass mixing ratios are 2.5 and 0.6 ppbm, respectively. Calculated sulfuric acid mixing ratios from aerosol volumes inferred from aerosol size distribution measurements on the same balloon agree well with the IMRMS data using standard assumption aerosol composition.     

Characterization of aerosol optical depth, aerosol mass concentration, UV irradiance and black carbon aerosols over Indo-Gangetic plains, India, during fog period

Every year during winter months (December?CJanuary) fog formation over Indo-Gangetic plains (IGP) of Indian region is believed to create numerous hazards. The present study addresses variations in aerosol optical properties, aerosol mass concentration and their impact on solar irradiance for pre-during-post fog conditions of December 2004 over IGP, India. Continuous measurements on aerosol optical depth (AOD), total aerosol mass concentration, black carbon (BC) aerosols, UV_ery and UVA were carried out for pre, during and post fog periods over study site of Allahabad, India, during December 2004 as a part of Aerosol Land Campaign-II conducted by Indian Space Research Organization (ISRO). High aerosol mass concentrations were observed during fog and post-fog periods. Accumulation mode particle loading was found to be high during pre-fog period and coarse mode particle loading was observed to be high during fog and post-fog periods. Considerable reduction in UV_ery and UVA irradiance was observed during fog period compared with pre and post-fog periods. Analysis of NOAA-HYSPLIT model runs suggested that enhanced biomass burning episodes down-wind to the study area increased the concentration of AOD and BC.     

辽宁地区大气气溶胶粒子的垂直分布特征

详细分析了１９９６、１９９７年春末夏初在辽宁省进行的大气气深胶飞机观测的０～５ｋｍ气深胶粒子数深度和尺度谱分布的垂直、水平变化,初步讨论了它们与温度和相对温度的关系。结果表明,混合层顶上下粒子数深度具有不同的垂直分布特征;粒子谱受不同形成机制影响,表现为多峰分布;水平方向上气溶胶粒子数浓度存在显著变化;温度层结和相对温度对气溶胶粒子的浓度和谱分布有明显影响。     

基于航测的珠三角气溶胶垂直分布及活化特性

2017年9月14—27日在珠江三角洲地区开展了6个架次飞机观测试验。利用飞行获取的气溶胶、云凝结核、云滴及常规气象探头观测资料,结合天气形势、气象条件及气团后向轨迹分析,研究了珠江三角洲地区深圳气溶胶数浓度及其谱的垂直分布特征,配合不同过饱和度条件下云凝结核浓度观测,分析了气溶胶活化特性。结果表明:在不同天气条件下,深圳低层气溶胶数浓度变化范围为500~9000 cm-3;边界层内气溶胶分布相对均匀,谱型随高度变化与气象条件相关。将6个架次气溶胶观测资料根据数浓度及谱型分为3种类型:类型Ⅰ为海洋型气溶胶,数浓度小,粒子尺度大,谱型呈双峰分布;类型Ⅲ为大陆型气溶胶,数浓度高,粒子尺度小,谱宽较宽且呈三峰分布;类型Ⅱ为海洋大陆影响型气溶胶,即受海洋和大陆共同影响,数浓度低于类型Ⅲ高于类型Ⅰ,谱型为双峰分布。拟合了包含海洋型及大陆型气溶胶的3个架次近地面云凝结核活化谱,计算了气溶胶在不同过饱和度条件下的活化效率。     

2007年冬季大连市区气溶胶垂直剖面特征

选用2007年1月8—30日期间8个无云天的激光雷达资料进行分析。基于Fernald方法反演得到气溶胶消光系数廓线,结合无线电探空资料分析了边界层内气溶胶时空分布,并将反演的激光雷达最低观测高度处(180 m)的气溶胶消光系数与地面PM10、能见度资料进行对比分析。结果表明：冬季大连市区气溶胶主要分布在2 km以下区域,早晨和夜间在0.5 km以下区域经常存在一个气溶胶层;气溶胶消光系数廓线与探空资料较吻合;反演激光雷达最低观测高度处(180 m)的气溶胶消光系数与地面的PM10浓度呈正相关,与能见度呈负相关,相关性较好。     

Role of organic acids (formic, acetic, pyruvic and oxalic) in the formation of cloud condensation nuclei (CCN): a review

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.     

Aerosol black carbon measurements in the Arctic haze during AGASP-II

During the second Arctic Gas and Aerosol Sampling Program conducted in April 1986, we performed measurements of the optically absorbing carbonaceous component of the ambient aerosol from the NOAA WP-3D aircraft operating between sea level and 10 km altitude. We collected the aerosol of filters that were exposed for several hours; we also operated the aethalometer to measure the concentration of aerosol black carbon in real time. The filter analyses represent averages over the altitude range and time span during which the filter was collecting. The real-time results were sorted by altitude to calculate vertical profiles of black carbon concentration. Values typically ranged from 300 to 500 ng m^–3 at lower altitudes, decreasing gradually to 25 to 100 ng m^–3 at 8–10 km. Strong stratification at lower altitudes was frequently observed. The magnitude of these concentrations suggests that the sources are distant regions of considerable fuel consumption. The presence of this material in the tropospheric column and its probable deposition to the high-albedo surface may result in perturbations of the solar radiation balance. The concentrations measured at the highest altitudes may mean that particulate carbon and accompanying emissions for which it is a tracer are mixing into the stratosphere.     

A study of marine aerosols over the Pacific Ocean

Aerosol samples were collected on a Pacific cruise from 47°N to 55°S. Particle morphology, concentrations, and size distributions were analyzed with an electron microscope; elemental compositions of individual particles were determined with an X-ray energy spectrometer; and chemical compositions of bulk samples were measured with an ion chromatograph. Temporal and spatial variations of aerosol physico-chemical characteristics were studied in relation to ocean currents and atmospheric parameters. The results show that number and mass concentrations of primary particles depend mainly on surface wind speeds. However the ratios between the major ions, e.g., Na⁺, Cl^-, and Mg⁺⁺, are similar to the ratios in seawater regardless of location or meteorological conditions. The concentrations of secondary aerosols, e.g., non-seasalt sulfate, nitrate, and ammonium particles, show maxima at upwelling regions, such as along the California coast, at the Equator, and near the Chatham Rise where ascending motion brings nutrient-riched deep water into the surface layer. The number concentrations of small sulfate particles and large nitrate-coated particles showed diurnal variations with maxima in the early afternoon and minima at night, indicating that the particles are the products of photo-chemical reactions. Their precursor gases, e.g., CH₃SCH₃, NO, and NH₃ are known to be released from seawater in upwelling regions where biological activities thrive.     

Annual and interannual variation in boreal forest aerosol particle number and volume concentration and their connection to particle formation

We investigated size-resolved submicrometre aerosol particle number and volume concentration time series as well as aerosol dynamic parameters derived from Differential Mobility Particle Sizer (DMPS) measurements at five background stations in the Nordic boreal forest area. The stations in question were Aspvreten, Hyytiälä and Utö in southern Finland and Sweden, and Värriö and Pallas in the Finnish Lapland. The objective of our investigation was to identify and quantify annual and interannual variation observable in the time series. We found that the total number and mass concentrations were much lower at the Lapland stations than at the southern stations and that the total particle number was strongly correlated to particle formation event frequency. The annual total number concentration followed the annual distribution of particle formation events at the southern stations but much less clearly at the Lapland stations. The volume concentration was highest during summer, in line with higher condensation growth rates; this is in line with the assumption that a large part of the particle volume is produced by oxidized plant emissions. The decrease of sulphate emissions in Europe was not visible in our data set. Aerosol dynamic parameters such as condensation sink, condensation sink diameter and the power law exponent linking coagulation losses and condensation sink are presented to characterize the submicron Nordic background aerosol.     

Validation of very high cloud droplet number concentrations in air masses transported thousands of kilometres over the ocean

The microstructure of orographic clouds related to the aerosol present was studied during the second Aerosol Characterisation Experiment (ACE‐2). Very high cloud droplet number concentrations (almost 3000 cm⁻³) were observed. These high concentrations occurred when clouds formed on a hill slope at Tenerife in polluted air masses originating in Europe that had transported the order of 1000 km over the Atlantic Ocean. The validity of the measured droplet number concentrations was investigated by comparing with measurements of the aerosol upstream of the cloud and cloud interstitial aerosol. Guided by distributions of the ratios between the measurements, three criteria of typically 30% in maximum deviation were applied to the measurements to test their validity. Agreement was found for 88% of the cases. The validated data set spans droplet number concentrations of 150–3000 cm⁻³. The updraught velocity during the cloud formation was estimated to 2.2 m s⁻¹ by model calculations, which is typical of cumuliform clouds. The results of the present study are discussed in relation to cloud droplet number concentrations previously reported in the literature. The importance of promoting the mechanistic understanding of the aerosol/cloud interaction and the use of validation procedures of cloud microphysical parameters is stressed in relation to the assessment of the indirect climatic effect of aerosols.     

Small-particle concentration fluctuations at a coastal site

Aerosol size spectra (d=10 nm–10 μm) were measured with an electrical aerosol spectrometer (EAS) at Mace Head on the west coast of Ireland. Several small aerosol particle (diameter 10–32 nm) concentration bursts were observed during the measurement period. Relationships between the events, air mass trajectories, tide height, and meteorological parameters are examined. Series of bursts were observed when a spectral transformation due to subsequent particle growth from 10 to 56–100 nm can be identified in an Eulerian experiment. Particle growth rates of between 1 and 3 nm/h were determined. These bursts appear in cold and comparatively clean arctic or polar air masses with temperature and relative humidity fluctuations, and do not correlate with low tide in some cases. These episodes, similar to those frequently found in the continental boundary layer, are thought to occur over a wide area and, for clear detection, require stable airflow for a few days. Elevated small-particle concentration events are more common during low tide or shortly after, and are typically associated with low wind speeds. Here, the increased shore exposure during low tide is thought to influence the nucleation and the subsequent growth of these aerosol particles. The occurrences of the bursts are found to depend on local wind direction. The highest d=10–32 nm particle concentrations appeared for wind sectors furthest from the tidal regions when the wind direction was 150–160°(south-easterly). Most of the events occurred during daytime when solar irradiation is most intense.