New aerosol particle formation via certain ion driven processes

Ions can speed up the formation of aerosol particles. The former studies have mainly concerned on the role of the ion charge itself. We have studied the possible (additional) role of the actual small air ion spectrum shape, and the quantitative role of ion–ion recombination pathway. By means of our ion evolution model, formation of new species (H₂SO₄)_n(NH₃)_m(HNO₃)_k via ion–ion recombination was investigated. The model shows how the generation rate of the new species depends on the concentrations of H₂SO₄ and NH₃, and how it depends on the tropospheric background aerosol situation. The rate can be up to a few new neutral complexes per cubic centimeter and per second. New particle generation via ion–ion recombination provides an extra channel, especially for the clean atmosphere. Former results have shown that such situations are often present in Antarctica. Our aerosol spectrum measurements reveal a number of similar non-Antarctic results. Sometimes, such situations are followed by aerosol bursts, which may be (partly) due to an ion–ion recombination channel.     

New aerosol particle formation via certain ion driven processes

Ions can speed up the formation of aerosol particles. The former studies have mainly concerned on the role of the ion charge itself. We have studied the possible (additional) role of the actual small air ion spectrum shape, and the quantitative role of ion–ion recombination pathway. By means of our ion evolution model, formation of new species (H₂SO₄)_n(NH₃)_m(HNO₃)_k via ion–ion recombination was investigated. The model shows how the generation rate of the new species depends on the concentrations of H₂SO₄ and NH₃, and how it depends on the tropospheric background aerosol situation. The rate can be up to a few new neutral complexes per cubic centimeter and per second. New particle generation via ion–ion recombination provides an extra channel, especially for the clean atmosphere. Former results have shown that such situations are often present in Antarctica. Our aerosol spectrum measurements reveal a number of similar non-Antarctic results. Sometimes, such situations are followed by aerosol bursts, which may be (partly) due to an ion–ion recombination channel.     

Physical characterization of aerosol particles during nucleation events

Particle concentrations and size distributions have been measured from different heights inside and above a boreal forest during three BIOFOR campaigns (14 April–22 May 1998, 27 July–21 August 1998 and 20 March–24 April 1999) in Hyytiälä, Finland. Typically, the shape of the background distribution inside the forest exhibited 2 dominant modes: a fine or Aitken mode with a geometric number mean diameter of 44 nm and a mean concentration of 1160 cm⁻³ and an accumulation mode with mean diameter of 154 nm and a mean concentration of 830 cm⁻³. A coarse mode was also present, extending up to sizes of 20 μm having a number concentration of 1.2 cm⁻³, volume mean diameter of 2.0 μm and a geometric standard deviation of 1.9. Aerosol humidity was lower than 50% during the measurements. Particle production was observed on many days, typically occurring in the late morning. Under these periods of new particle production, a nucleation mode was observed to form at diameter of the order of 3 nm and, on most occasions, this mode was observed to grow into Aitken mode sizes over the course of a day. Total concentrations ranged from 410–45 000 cm⁻³, the highest concentrations occurring on particle production days. A clear gradient was observed between particle concentrations encountered below the forest canopy and those above, with significantly lower concentrations occurring within the canopy. Above the canopy, a slight gradient was observed between 18 m and 67 m, with at maximum 5% higher concentration observed at 67 m during the strongest concentration increases.     

The influence of aerosol particle composition on cloud droplet formation

A difference in partitioning between cloud droplets and interstitial air for two chemical species (elemental carbon and sulphur) with different expected behaviour in nucleation scavenging was observed in clouds at Mt. Kleiner Feldberg (825 m asl), near Frankfurt, Germany. The fraction of sulphur incorporated in cloud droplets was always higher than the fraction of elemental carbon. This difference in partitioning has also been observed in fog but under different pollution conditions in the Po Valley, Italy. Both these studies were based on bulk samples. In the present study at Kleiner Feldberg, impactor samples of the particles in the interstitial air and the cloud droplet residuals were taken and a single particle analysis was done on the samples. It was found that, for a given particle size, the majority of particles forming cloud droplets were soluble and that insoluble particles preferentially remained in the interstitial air.     

Studying the aerosol fluxes by using the floating aerosol trap

In this paper, a functional scheme and basic principles of the floating aerosol trap, which has been developed by the authors, are presented. The first experimental results of the vertical aerosol fluxes coming on the Visla Bay surface (the Baltic Sea) and measured with the trap are demonstrated.     

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.     

Vertical fluxes in katabatic flows

Katabatic flow is a dynamical process occurring on relatively calm, clear nights above sloping terrain. Its existence is dependent on long-wave radiative transfer, particularly radiative flux divergence within the air itself, for both its generation and (it is concluded here), along with advective warming, for much of its retardation.Utilising sounding data closely spaced in time, a discussion is presented of the importance of surface shear, interfacial shear, advective warming and radiative divergence in a strong katabatic flow. It is concluded that radiative divergence is important in generating static and dynamic instabilities in the flow. The role of radiative cooling in mixing of momentum has largely been ignored so far, and might explain why higher-order models tend to overestimate katabatic speeds on smooth slopes.     

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.     

Evolution of aerosol vertical distribution during particulate pollution events in Shanghai

A set of micro pulse lidar(MPL)systems operating at 532 nm was used for ground-based observation of aerosols in Shanghai in 2011.Three typical particulate pollution events(e.g.,haze)were examined to determine the evolution of aerosol vertical distribution and the planetary boundary layer(PBL)during these pollution episodes.The aerosol vertical extinction coefficient(VEC)at any given measured altitude was prominently larger during haze periods than that before or after the associated event.Aerosols originating from various source regions exerted forcing to some extent on aerosol loading and vertical layering,leading to different aerosol vertical distribution structures.Aerosol VECs were always maximized near the surface owing to the potential influence of local pollutant emissions.Several peaks in aerosol VECs were found at altitudes above 1 km during the dust-and bioburning-influenced haze events.Aerosol VECs decreased with increasing altitude during the local-polluted haze event,with a single maximum in the surface atmosphere.PM2.5 increased slowly while PBL and visibility decreased gradually in the early stages of haze events;subsequently,PM2.5 accumulated and was exacerbated until serious pollution bursts occurred in the middle and later stages.The results reveal that aerosols from different sources impact aerosol vertical distributions in the atmosphere and that the relationship between PBL and pollutant loadings may play an important role in the formation of pollution.     

Vertical distributions of aerosol optical properties during haze and floating dust weather in Shanghai

A comparative study on the vertical distributions of aerosol optical properties during haze and floating dust weather in Shanghai was conducted based on the data obtained from a micro pulse lidar.There was a distinct difference in layer thickness and extinction coefficient under the two types of weather conditions.Aerosols were concentrated below 1 km and the aerosol extinction coefficients ranged from 0.25 to 1.50km^-1 on haze days.In contrast,aerosols with smaller extinction coefficients(0.20 0.35 km^-1) accumulated mainly from the surface to 2 km on floating dust days.The seasonal variations of extinction and aerosol optical depth（AOD） for both haze and floating dust cases were similar greatest in winter,smaller in spring,and smallest in autumn.More than 85%of the aerosols appeared in the atmosphere below 1 km during severe haze and floating dust weather.The diurnal variation of the extinction coefficient of haze exhibited a bimodal shape with two peaks in the morning or at noon,and at nightfall,respectively.The aerosol extinction coefficient gradually increased throughout the day during floating dust weather.Case studies showed that haze aerosols were generated from the surface and then lifted up,but floating dust aerosols were transported vertically from higher altitude to the surface.The AOD during floating dust weather was higher than that during haze.The boundary layer was more stable during haze than during floating dust weather.     

New aerosol particle formation in different synoptic situations at Hyytiälä, Southern Finland

We examine the meteorological conditions favourable for new particle formation as a contribution to clarifying the responsible processes. Synoptic weather maps and satellite images over Southern Finland for 2003–2005 were examined, focusing mainly on air mass types, atmospheric frontal passages, and cloudiness. Arctic air masses are most favourable for new aerosol particle formation in the boreal forest. New particle formation tends to occur on days after passage of a cold front and on days without frontal passages. Cloudiness, often associated with frontal passages, decreases the amount of solar radiation, reducing the growth of new particles. When cloud cover exceeds 3–4 octas, particle formation proceeds at a slower rate or does not occur at all. During 2003–2005, the conditions that favour particle formation at Hyytiälä (Arctic air mass, post-cold-frontal passage or no frontal passage and cloudiness less than 3–4 octas) occur on 198 d. On 105 (57%) of those days, new particle formation occurred, indicating that these meteorological conditions alone can favour, but are not sufficient for, new particle formation and growth. In contrast, 53 d (28%) were classified as undefined days; 30 d (15%) were non-event days, where no evidence of increasing particle concentration and growth has been noticed.     

Vertical divergence of fogwater fluxes above a spruce forest

Two almost identical eddy covariance measurement setups were used to measure the fogwater fluxes to a forest ecosystem in the “Fichtelgebirge” mountains (Waldstein research site, 786 m a.s.l.) in Germany. During the first experiment, an intercomparison was carried out with both setups running simultaneously at the same measuring height on a meteorological tower, 12.5 m above the forest canopy. The results confirmed a close agreement of the turbulent fluxes between the two setups, and allowed to intercalibrate liquid water content (LWC) and gravitational fluxes. During the second experiment, the setups were mounted at a height of 12.5 and 3 m above the canopy, respectively. For the 22 fog events, a persistent negative flux divergence was observed with a greater downward flux at the upper level. To extrapolate the turbulent liquid water fluxes measured at height z to the canopy of height h_c, a conversion factor 1/[1+0.116(z−h_c)] was determined. For the fluxes of nonvolatile ions, no such correction is necessary since the net evaporation of the fog droplets appears to be the primary cause of the vertical flux divergence. Although the net evaporation reduces the liquid water flux reaching the canopy, it is not expected to change the absolute amount of ions dissolved in fogwater.     

气溶胶对云中水成物粒子荷电情况的影响

利用已有的二维雷暴云起电模式,加入气溶胶模块,建立一个完善的雷暴云起电模式.结合SEET个例,初步探讨了气溶胶浓度对雷暴云内各种水成物粒子荷电情况的影响.发现气溶胶的浓度与雷暴云内云滴、霰粒、冰雹以及雨滴等水成物粒子在空间所携带的最大电荷面密度值以及电荷量有很好的正相关性;同时气溶胶粒子浓度的增加使得雨滴在空间携带电荷量达到峰值的时间有一定提前.     

Vertical ozone fluxes and related deposition parameters over agricultural and forested landscapes

The spatial variability and temporal behavior of the vertical flux of ozone have been investigated from turbulence measurements collected on aircraft flight legs in the daytime period during two consecutive summer experimental field programs. The data were obtained during horizontal flight legs conducted over agricultural crops and forested land in three different regions of the eastern United States.Results from individual experimental cases and statistics derived from all cases in each region are presented. Ozone flux generally exhibited a significant height dependency. The strongest negative (downward) fluxes in the lowest-level flight legs were primarily attributed to the uptake of ozone by the surface and vegetative cover. Fluxes were near-zero in the middle of the convective boundary layer (CBL) in the afternoon period. As ozone flux was proportional to concentration, slightly stronger fluxes were found in low-level urban plume segments where ozone concentrations were 10–20 ppb higher than in the surrounding area. The derived deposition velocity showed no such bias as a function of position across the urban plume. Ozone flux differences were not apparent between the more heavily forested sections and the primarily agricultural cropland areas in these regions. During the afternoon period when no clear temporal trend was evident, means from values obtained below 0.15Z _i (Z _i being the CBL height) were -0.421 and -0.431 ppb m^-2 s^-1 for ozone flux and 0.81 and 0.82 cm s^-1 for the derived mean deposition velocity in the southeastern Pennsylvania and central Ohio areas, respectively. These experimental results for ozone provide support to a dry deposition parameterization module which computes grid-area averaged deposition velocities for use in regional-scale models.On assignment from the National Oceanic and Atmospheric Administration, U.S. Department of Commerce.     

A closure study of sub-micrometer aerosol particle hygroscopic behaviour

The hygroscopic properties of sub-micrometer aerosol particles were studied in connection with a ground-based cloud experiment at Great Dun Fell, in northern England in 1995. Hygroscopic diameter growth factors were measured with a Tandem Differential Mobility Analyser (TDMA) for dry particle diameters between 35 and 265 nm at one of the sites upwind of the orographic cloud. An external mixture consisting of three groups of particles, each with different hygroscopic properties, was observed. These particle groups were denoted less-hygroscopic, more-hygroscopic and sea spray particles and had average diameter growth factors of 1.11–1.15, 1.38–1.69 and 2.08–2.21 respectively when taken from a dry state to a relative humidity of 90%. Average growth factors increased with dry particle size. A bimodal hygroscopic behaviour was observed for 74–87% of the cases depending on particle size. Parallel measurements of dry sub-micrometer particle number size distributions were performed with a Differential Mobility Particle Sizer (DMPS). The inorganic ion aerosol composition was determined by means of ion chromatography analysis of samples collected with Berner-type low pressure cascade impactors at ambient conditions. The number of ions collected on each impactor stage was predicted from the size distribution and hygroscopic growth data by means of a model of hygroscopic behaviour assuming that only the inorganic substances interacted with the ambient water vapour. The predicted ion number concentration was compared with the actual number of all positive and negative ions collected on the various impactor stages. For the impactor stage which collected particles with aerodynamic diameters between 0.17–0.53 μm at ambient relative humidity, and for which all pertinent data was available for the hygroscopic closure study, the predicted ion concentrations agreed with the measured values within the combined measurement and model uncertainties for all cases but one. For this impactor sampling occasion, the predicted ion concentration was significantly higher than the measured. The air mass in which this sample was taken had undergone extensive photochemical activity which had probably produced hygroscopically active material other than inorganic ions, such as organic oxygenated substances.     

激光探测平流层气溶胶层后向散射系数分布

1983年2月以来,利用红宝石激光雷达对平流层气溶胶层进行了一系列探测.结果表明:因受El Chichon火山爆发的影响,平流层气溶胶层后向散射比峰值和14—23.5公里高度范围内积分后向散射系数均明显增大。本文对部分探测结果进行了分析和讨论.