Observation of regional new particle formation in the urban atmosphere

Long-term measurements of fine particle number-size distributions were carried out over 9.5 yr (May 1997–December 2006), in the urban background atmosphere of Helsinki. The total number of days was 3528 with about 91.9% valid data. A new particle formation event (NPF) is defined if a distinct nucleation mode of aerosol particles is observed below 25 nm for several hours, and it shows a growth pattern. We observed 185 NPF events, 111 d were clear non-events and most of the days (around 83.5%) were undefined. The observed events were regional because they were observed at Hyytiälä (250 km north of Helsinki). The events occurred most frequently during spring and autumn. The observed formation rate was maximum during the spring and summer (monthly median 2.87 cm⁻³ s⁻¹) and the modal growth rate was maximum during late summer and Autumn (monthly median 6.55 nm h⁻¹). The events were observed around noon, and the growth pattern often continued on the following day. The observation of weak NPF events was hindered due to pre-existing particles from both local sources. It is clear that regional NPF events have a clear influence on the dynamic behaviour of aerosol particles in the urban atmosphere.     

Development of particle size and composition distributions with a novel aerosol dynamics model

An aerosol dynamics model, AEROFOR2, is developed in the context of the BIOFOR project focussing on boreal forest aerosol. It is the second version of a Lagrangian type box model AEROFOR for investigating the formation and growth of particles under clear sky atmospheric conditions. Particles can consist of soluble and insoluble material and the particle population can be externally or internally mixed. AEROFOR2 includes gas phase chemistry and aerosol dynamics, and calculates the number and composition distributions of particles as functions of time. Observed growth rates of the nucleation mode particles after a typical nucleation event are 2–3 nm/h. The model simulations predict that 3·10⁷ molecules cm⁻³ of insoluble organic vapour and less than 6·10⁶ molecules cm⁻³ of soluble vapour condensing onto particles are enough to make them grow in good agreement with the observed growth rates. Then the source rate of the organic vapour must be an order of 10⁵ molecules cm⁻³ s⁻¹, and its saturation vapour density should be below 10⁶ molecules cm⁻³. If the aerosol was initially an internal mixture of soluble (70%) and insoluble (30%) constituents it transformed to an externally mixed aerosol during the simulation. By applying the externally‐mixed aerosol based on measured soluble volume fractions, it was concluded that the modelled soluble fraction of the nucleation mode was too low in comparison with the measurements, and thus, a part of the condensable organic vapour must be water soluble.     

Seasonal variation of the molecular hydrogen uptake by soils inferred from continuous atmospheric observations in Heidelberg, southwest Germany

The dominant sink of atmospheric molecular hydrogen (H₂) is its enzymatic destruction in soils. Quantitative estimates of the global sink strength, as derived from bottom-up process studies, are, however, still associated to large uncertainties. Here we present an alternative way to estimate atmosphere-to-soil flux densities, respectively deposition velocities of H₂, based on atmospheric H₂ and ²²²Rn observations in the boundary layer. Two and a half years of continuous measurements from a polluted site in the Rhine-Neckar area have been evaluated and night-time flux densities were calculated for situations of strong nocturnal boundary layer inversions using the Radon-Tracer Method. The influences from local anthropogenic combustion sources could be detected and successfully separated by parallel measurements of carbon monoxide. Inferred daily uptake fluxes in the Heidelberg catchment area range from 0.5 to 3 × 10⁻⁸ g H₂ m⁻² s⁻¹ with a mean value of (1.28 ± 0.31) × 10⁻⁸ g H₂ m⁻² s⁻¹. Uptake rates are about 25% larger during summer than during winter, when soil moisture is high, and diffusive transport of H₂ into the soil is inhibited. The mean deposition velocity is 3.0 ± 0.7 × 10⁻² cm s⁻¹_, which is very well in line with direct measurements on similar soil types in Europe and elsewhere.     

Spectral absorption coefficients and imaginary parts of refractive indices of Saharan dust during SAMUM-1

During the SAMUM-1 experiment, absorption coefficients and imaginary parts of refractive indices of mineral dust particles were investigated in southern Morocco. Main absorbing constituents of airborne samples were identified to be iron oxide and soot. Spectral absorption coefficients were measured using a spectral optical absorption photometer (SOAP) in the wavelength range from 300 to 800 nm with a resolution of 50 nm. A new method that accounts for a loading-dependent correction of fibre filter based absorption photometers, was developed. The imaginary part of the refractive index was determined using Mie calculations from 350 to 800 nm. The spectral absorption coefficient allowed a separation between dust and soot absorption. A correlation analysis showed that the dust absorption coefficient is correlated ( R ² up to 0.55) with the particle number concentration for particle diameters larger than 0.5 μm, whereas the coefficient of determination R ² for smaller particles is below 0.1. Refractive indices were derived for both the total aerosol and a dust aerosol that was corrected for soot absorption. Average imaginary parts of refractive indices of the entire aerosol are 7.4 × 10⁻³, 3.4 × 10⁻³ and 2.0 × 10⁻³ at wavelengths of 450, 550 and 650 nm. After a correction for the soot absorption, imaginary parts of refractive indices are 5.1 × 10⁻³, 1.6 × 10⁻³ and 4.5 × 10⁻⁴.     

Observations of the evolution of the aerosol, cloud and boundary‐layer characteristics during the 1st ACE‐2 Lagrangian experiment

During the 1st Lagrangian experiment of the North Atlantic Regional Aerosol Characterisation Experiment (ACE‐2), a parcel of air was tagged by releasing a smart, constant level balloon into it from the Research Vessel Vodyanitskiy . The Meteorological Research Flight's C‐130 aircraft then followed this parcel over a period of 30 h characterising the marine boundary layer (MBL), the cloud and the physical and chemical aerosol evolution. The air mass had originated over the northern North Atlantic and thus was clean and had low aerosol concentrations. At the beginning of the experiment the MBL was over 1500 m deep and made up of a surface mixed layer (SML) underlying a layer containing cloud beneath a subsidence inversion. Subsidence in the free troposphere caused the depth of the MBL to almost halve during the experiment and, after 26 h, the MBL became well mixed throughout its whole depth. Salt particle mass in the MBL increased as the surface wind speed increased from 8 m s⁻¹ to 16 m s⁻¹ and the accumulation mode (0.1μm to 3.0 μm) aerosol concentrations quadrupled from 50 cm⁻³ to 200 cm⁻³. However, at the same time the total condensation nuclei (>3 nm) decreased from over 1000 cm⁻³ to 750 cm⁻³. The changes in the accumulation mode aerosol concentrations had a significant effect on the observed cloud microphysics. Observational evidence suggests that the important processes in controlling the Aitken mode concentration which, dominated the total CN concentration, included, scavenging of interstitial aerosol by cloud droplets, enhanced coagulation of Aitken mode aerosol and accumulation mode aerosol due to the increased sea salt aerosol surface area, and dilution of the MBL by free tropospheric air.     

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.     

Properties of dust aerosol particles transported to Portugal from the Sahara desert

Aerosol properties of mineral particles in the far field of an African desert dust outbreak were investigated that brought Saharan dust over the Mediterranean in different layers to Portugal. The measurements were performed inside the project Desert Aerosols over Portugal (DARPO) which was linked to the Saharan Mineral Dust Experiment (SAMUM). The maximum particle mass concentration was about 150 μg m⁻³ and the corresponding scattering coefficient was 130 M m⁻¹ which results in a mass scattering efficiency of 0.87 m² g⁻¹. The aerosol optical depth reached values up to 0.53 and the lidar ratio was between 45 and 50 in the whole dust loaded column. A comparison between particle size distributions and refractive indices derived from different instruments and models showed a general good agreement but some minor differences could also be observed. Measurements as well as calculations with a particle transport model suggest that there is a relatively higher concentration of very large particles in the upper region of the dust layer than on the surface which is likely connected with meteorological conditions at the observational site (Évora, Portugal).     

Vertical fluxes and micrometeorology during aerosol particle formation events

Fluxes of aerosol particles with sizes larger than 10 nm together with fluxes of momentum, sensible and latent heat and CO₂ were measured 10 m above a Scots pine forest with the eddy covariance method. During days when nucleation events were observed particle size distribution measurements showed particle growth from 3 nm sizes to the Aitken mode. Analysis of the experimental data showed systematic differences in fluxes during the days when new particle production was observed compared to other days. During the nucleation events the particle flux measurements showed downward aerosol particle transport, i.e., indicating an elevated source, with respect to the measurement level, of particles larger than 10 nm. Furthermore the turbulence intensity and the heat fluxes were observed to be significantly higher. Evidences of mesoscale circulation were observed in wind speed records as well as in turbulent fluxes on nucleation days. The measurement results show that micrometeorology, the synoptic scale conditions and the particle formation are closely related.     

Vertical profiling of Saharan dust with Raman lidars and airborne HSRL in southern Morocco during SAMUM

Three ground-based Raman lidars and an airborne high-spectral-resolution lidar (HSRL) were operated during SAMUM 2006 in southern Morocco to measure height profiles of the volume extinction coefficient, the extinction-to-backscatter ratio and the depolarization ratio of dust particles in the Saharan dust layer at several wavelengths. Aerosol Robotic Network (AERONET) Sun photometer observations and radiosoundings of meteorological parameters complemented the ground-based activities at the SAMUM station of Ouarzazate. Four case studies are presented. Two case studies deal with the comparison of observations of the three ground-based lidars during a heavy dust outbreak and of the ground-based lidars with the airborne lidar. Two further cases show profile observations during satellite overpasses on 19 May and 4 June 2006. The height resolved statistical analysis reveals that the dust layer top typically reaches 4–6 km height above sea level (a.s.l.), sometimes even 7 km a.s.l.. Usually, a vertically inhomogeneous dust plume with internal dust layers was observed in the morning before the evolution of the boundary layer started. The Saharan dust layer was well mixed in the early evening. The 500 nm dust optical depth ranged from 0.2–0.8 at the field site south of the High Atlas mountains, Ångström exponents derived from photometer and lidar data were between 0–0.4. The volume extinction coefficients (355, 532 nm) varied from 30–300 Mm⁻¹ with a mean value of 100 Mm⁻¹ in the lowest 4 km a.s.l.. On average, extinction-to-backscatter ratios of 53–55 sr (±7–13 sr) were obtained at 355, 532 and 1064 nm.     

Is the recent build-up of atmospheric CO2 over Europe reproduced by models. Part 2: an overview with the atmospheric mesoscale transport model CHIMERE

In this issue, Ramonet et al. revealed a positive trend in European, atmospheric CO₂ concentrations relative to a marine, North Atlantic reference baseline, for the years 2001–2006. The observed build up mainly occurred during the cold season where it reaches a 0.8 ppm yr⁻¹ at low-altitude stations to a 0.3 ppm yr⁻¹ at mid-altitude stations. We explore the cause of this build-up using the mesoscale model CHIMERE. We first model the observed trends, using interannually varying fluxes and transport, then suppress the interannual variability in fluxes or aspects of transport to elucidate the cause. The run with no interannual variability in fluxes still matches observed trends suggesting that transport is the major cause. Separate runs varying either boundary layer height or winds show that changes in boundary layer height explain the trends at low-altitude stations within the continents while changes in wind regimes drive changes elsewhere.     

In situ measurements of optical properties at Tinfou (Morocco) during the Saharan Mineral Dust Experiment SAMUM 2006

In situ measurements of optical and physical properties of mineral dust were performed at the outskirts of the Saharan Desert in the framework of the Saharan Mineral Dust Experiment part 1 (SAMUM-1). Goals of the field study were to achieve information on the extent and composition of the dust particle size distribution and the optical properties of dust at the ground. For the particle number size distribution, measured with a DMPS/APS, a size dependent dynamic shape factor was considered. The mean refractive index of the particles in this field study is  1.53–4.1 × 10⁻³ i   at 537 nm wavelength and  1.53–3.1 × 10⁻³ i   at 637 nm wavelength derived from measurements of scattering and absorption coefficients, as well as the particle size distribution. Whereas the real part of the refractive index is rather constant, the imaginary part varies depending on the mineral dust concentrations. For high dust concentration the single scattering albedo is primarily influenced by iron oxide and is  0.96 ± 0.02  and  0.98 ± 0.01  at 537 nm and 637 nm wavelength, respectively. During low dust concentration the single scattering albedo is more influenced by a soot-type absorber and is  0.89 ± 0.02  and  0.93 ± 0.01  for the same wavelengths.     

南京霾天颗粒物数浓度特征及其受气象条件影响分析

2013年12月,我国中东部地区爆发持续性霾污染过程。本研究利用空气动力学粒径谱仪和气溶胶粒径谱仪在线观测这次霾污染过程中13.6~20 000 nm颗粒物数浓度,结合气象参数和颗粒物化学组分对南京霾天颗粒物数浓度分布特征,及其与气象条件相关性进行分析。结果表明,霾天颗粒物主要分布在积聚模态,且500~1 000 nm和1 000~2 500 nm粒径段颗粒物数浓度的增多是造成霾天能见度低的主要原因;随着相对湿度的增大,13.6~100 nm粒径段颗粒物数浓度逐渐降低,而大于100 nm颗粒物数浓度升高;500~1 000 nm和1 000~2 500 nm粒径段颗粒物数浓度受相对湿度的影响尤为明显,并且这2个粒径段颗粒物受气态污染物(SO2,NOX)的二次转化影响较大。霾污染期间南京大气颗粒物主要来自南京东南和西北方向的污染源排放,颗粒物数浓度总体上与风速呈负相关关系;温度对颗粒物数浓度的影响主要集中在13.6~100 nm粒径段;边界层的高度与粒径100 nm颗粒物呈负相关性,边界层的抬升反而利于超细粒子的生成和增长;逆温层的强度对超细粒子的作用更为明显。     

Aircraft study of aerosol vertical distributions over Beijing and their optical properties

A set of 152 vertical profiles of aerosol number concentration and size distribution with diameter ranging from 0.12 to 3.0 μm observed by the airborne optical spectrometer probe in Beijing, China, between February 2005 and September 2006 is analysed and discussed. The statistic of aerosol number concentration ( N _a) reveals a high aerosol number density in this region with average surface level number concentration ( N ₀) of about 6600 cm⁻³ (0.12–3.0 μm). The average vertical profile of N _a approximately satisfies an exponential decline function with a scale height of 1419 m. The N _a profiles are influenced by the structures of planetary boundary layer (PBL) significantly and two typical types of N _a profile under different conditions of PBL are presented and parametrized in this study. The observations of aerosol size distribution show that, in most cases the aerosol size distributions are not very sensitive to altitude, with effective radii ranging from 0.16 to 0.28 μm. Comparison between aircraft-derived aerosol optical depth (AOD) and Moderate Resolution Imaging Spectroradiometer-derived AOD shows good agreement. The Mie model calculations suggest that the surface level number concentration, the PBL height and the structure of PBL can influence the AOD significantly.     

Saharan dust absorption and refractive index from aircraft-based observations during SAMUM 2006

During the Saharan Mineral Dust Experiment (SAMUM) conducted in summer 2006 in southeast Morocco, the complex refractive index of desert dust was determined from airborne measurements of particle size distributions and aerosol absorption coefficients at three different wavelengths in the blue (467 nm), green (530 nm) and red (660 nm) spectral regions. The vertical structure of the dust layers was analysed by an airborne high spectral resolution lidar (HSRL). The origin of the investigated dust layers was estimated from trajectory analyses, combined with Meteosat 2nd Generation (MSG) scenes and wind field data analyses. The real part n of the dust refractive index was found almost constant with values between 1.55 and 1.56, independent of the wavelength. The values of the imaginary part k varied between the blue and red spectral regions by a factor of three to ten depending on the dust source region. Absolute values of k ranged from 3.1 × 10⁻³ to 5.2 × 10⁻³ at 450 nm and from 0.3 × 10⁻³ to 2.5 × 10⁻³ at 700 nm. Groupings of k values could be attributed to different source regions.     

河南省层状云降水雨滴谱特征分析

利用2015-2017年河南省层状云降水过程的Parsivel(Partical Size and Velocity)激光雨滴谱观测资料,对层状云降水的雨滴数浓度、含水量、雨滴直径等微物理参量特征及不同尺度的降水粒子对雨强的贡献进行了统计分析,并采用2种拟合方法对层状云降水雨滴谱进行了拟合。结果表明:河南省层状云降水的空间结构不均匀,各微物理参量的变化存在着起伏,雨滴数浓度为10²个/m³量级,个别达到10³个/m³,含水量在10^-2~10^-1 g/m³,粒子平均直径<0.5 mm左右,统计的不同台站平均最大粒子直径为1~2 mm,雨强平均值不超过1 mm/h。直径为<2 mm的雨滴对雨强的贡献占96.23%,直径小于1 mm的雨滴对数浓度的贡献最大。雨强是由雨滴最大直径、平均直径和数浓度3者共同决定。层状云降水雨滴的谱分布较窄,滴谱曲线比较平滑。降水开始时,谱型为单峰结构;降水处于稳定阶段时,谱型为双峰和单峰相结合的结构。层状云拟合M-P分布和Г分布偏差均出现在直径<1 mm的小雨滴端,对于微小粒子随直径增大而增多导致的曲线弯曲没能表现出来,相对而言Г分布拟合效果明显略优于M-P分布的拟合效果。河南省层状云降水的2种分布形式分别为N(D)=7373.9exp(-3.67D)和N(D)=10492.05D1.62exp(-5.11D)。     

Estimating the Asian radon flux density and its latitudinal gradient in winter using ground-based radon observations at Sado Island

Terrestrial radon-222 flux density for the Asian continent, integrated over distances of 4500 km, is estimated in two 20° latitudinal bands centred on 48.8°N and 63.2°N. The evaluation is based on three years of wintertime radon measurements at Sado Island, Japan, together with meteorological and trajectory information. A selection of 18% of observations are suitable for evaluation of an analytical expression for the continental surface flux. Various meteorological assumptions are discussed; it is found that there is a substantial effect of increased complexity of the formulation on the flux estimates obtained. The distribution of spatially integrated radon flux over the Asian landmass is reported for the first time. Expressed as geometric means and 1σ-ranges, estimated fluxes are 14.1 mBq m⁻² s⁻¹ (1σ-range: 18 mBq m⁻² s⁻¹) and 8.4 mBq m⁻² s⁻¹ (1σ-range: 10 mBq m⁻² s⁻¹) for the lower and higher latitude bands. These results constitute an annual minimum in flux densities for these regions, and are higher than previously reported. The existence of a latitudinal gradient in the continental radon source function is confirmed; the present estimate for Asia (−0.39 mBq m⁻² s⁻¹ per degree of latitude) is in agreement with the northern hemisphere terrestrial radon flux gradient proposed previously.     

Aircraft observation of carbon dioxide at 8–13 km altitude over the western Pacific from 1993 to 1999

Abstract The spatial and temporal variations of atmospheric CO₂ at 8–13 km from April 1993 to April 1999 were observed by measuring CO₂ mixing ratios in samples collected biweekly from a commercial airliner between Australia and Japan. The CO₂ growth rate showed a considerable interannual variation, with a maximum of about 3 ppm yr⁻¹ during late 1997. This variation is related to the El Niño/Southern Oscillation (ENSO) events. A year-to-year change related to the ENSO events was also found in the latitudinal distribution pattern of the CO₂ annual mean between 30°N and 30°S. The averaged CO₂ seasonal cycle in the Northern Hemisphere gradually decayed toward the equator, and a relatively complicated variation with a double seasonal maximum appeared in the Southern Hemisphere. A significant yearly change of the seasonal cycle pattern was observed in the Southern Hemisphere. The impact of a tropical biomass-burning injection on the upper tropospheric CO₂ was estimated on the basis of the CO data from the same airliner observation.     

Ice nuclei characteristics from M-PACE and their relation to ice formation in clouds

This paper presents airborne measurements of ice nuclei (IN) number concentration and elemental composition from the mixed-phase Arctic cloud experiment (M-PACE) in northern Alaska during October 2004. Although the project average IN concentration was low, less than 1 L⁻¹ STP, there was significant spatial and temporal variability, with local maximum concentrations of nearly 60 L⁻¹ STP. Immersion and/or condensation freezing appear to be the dominant freezing mechanisms, whereas mechanisms that occur below water saturation played a smaller role. The dominant particle types identified as IN were metal oxides/dust (39%), carbonaceous particles (35%) and mixtures of metal oxides/dust with either carbonaceous components or salts/sulphates (25%), although there was significant variability in elemental composition. Trajectory analysis suggests both local and remote sources, including biomass burning and volcanic ash. Seasonal variability of IN number concentrations based on this study and data from SHEBA/FIRE-ACE indicates that fall concentrations are depleted relative to spring by about a factor of five. Average IN number concentrations from both studies compare favorably with cloud ice number concentrations of cloud particles larger than 125 μm, for temperatures less than −10 °C. Cloud ice number concentrations also were enhanced in spring, by a factor of ∼2, but only over a limited temperature range.     

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.     

A recent build-up of atmospheric CO2 over Europe. Part 1: observed signals and possible explanations

We analysed interannual and decadal changes in the atmospheric CO₂ concentration gradient (ΔCO₂) between Europe and the Atlantic Ocean over the period 1995–2007. Fourteen measurement stations are used, with Mace-Head being used to define background conditions. The variability of ΔCO₂ reflects fossil fuel emissions and natural sinks activity over Europe, as well as atmospheric transport variability. The mean ΔCO₂ increased by 1–2 ppm at Eastern European stations (∼30% growth), between 1990–1995 and 2000–2005. This built up of CO₂ over the continent is predominantly a winter signal. If the observed increase of ΔCO₂ is explained by changes in ecosystem fluxes, a loss of about 0.46 Pg C per year would be required during 2000–2005. Even if severe droughts have impacted Western Europe in 2003 and 2005, a sustained CO₂ loss of that magnitude is unlikely to be true. We sought alternative explanations for the observed CO₂ build-up into transport changes and into regional redistribution of fossil fuel CO₂ emissions. Boundary layer heights becoming shallower can only explain 32% of the variance of the signal. Regional changes of emissions may explain up to 27% of the build-up. More insights are given in the Aulagnier et al. companion paper.