scholarly journals Spatio-temporal variability and principal components of the particle number size distribution in an urban atmosphere

2009 ◽  
Vol 9 (9) ◽  
pp. 3163-3195 ◽  
Author(s):  
F. Costabile ◽  
W. Birmili ◽  
S. Klose ◽  
T. Tuch ◽  
B. Wehner ◽  
...  

Abstract. A correct description of fine (diameter <1 μm) and ultrafine (<0.1 μm) aerosol particles in urban areas is of interest for particle exposure assessment but also basic atmospheric research. We examined the spatio-temporal variability of atmospheric aerosol particles (size range 3–800 nm) using concurrent number size distribution measurements at a maximum of eight observation sites in and around Leipzig, a city in Central Europe. Two main experiments were conducted with different time span and number of observation sites (2 years at 3 sites; 1 month at 8 sites). A general observation was that the particle number size distribution varied in time and space in a complex fashion as a result of interaction between local and far-range sources, and the meteorological conditions. To identify statistically independent factors in the urban aerosol, different runs of principal component (PC) analysis were conducted encompassing aerosol, gas phase, and meteorological parameters from the multiple sites. Several of the resulting PCs, outstanding with respect to their temporal persistence and spatial coverage, could be associated with aerosol particle modes: a first accumulation mode ("droplet mode", 300–800 nm), considered to be the result of liquid phase processes and far-range transport; a second accumulation mode (centered around diameters 90–250 nm), considered to result from primary emissions as well as aging through condensation and coagulation; an Aitken mode (30–200 nm) linked to urban traffic emissions in addition to an urban and a rural Aitken mode; a nucleation mode (5–20 nm) linked to urban traffic emissions; nucleation modes (3–20 nm) linked to photochemically induced particle formation; an aged nucleation mode (10–50 nm). Additional PCs represented only local sources at a single site, or infrequent phenomena. In summary, the analysis of size distributions of high time and size resolution yielded a surprising wealth of statistical aerosol components occurring in the urban atmosphere over one single city. A paradigm on the behaviour of sub-μm urban aerosol particles is proposed, with recommendations how to efficiently monitor individual sub-fractions across an entire city.

2008 ◽  
Vol 8 (5) ◽  
pp. 18155-18217 ◽  
Author(s):  
F. Costabile ◽  
W. Birmili ◽  
S. Klose ◽  
T. Tuch ◽  
B. Wehner ◽  
...  

Abstract. Due to the presence of diffusive anthropogenic sources in urban areas, the spatio-temporal variability of fine (diameter <1 μm) and ultrafine (<0.1 μm) aerosol particles has been a challenging issue in particle exposure assessment as well as atmospheric research in general. We examined number size distributions of atmospheric aerosol particles (size range 3–800 nm) that were measured simultaneously at a maximum of eight observation sites in and around a city in Central Europe (Leipzig, Germany). Two main experiments were conducted with different time span and number of observation sites (2 years at 3 sites; 1 month at 8 sites). A general observation was that the particle number size distribution varied in time and space in a complex fashion as a result of interaction between local and far-range sources, and the meteorological conditions. To identify statistically independent factors in the urban aerosol, different runs of principal component analysis were conducted encompassing aerosol, gas phase, and meteorological parameters from the multiple sites. Several of the resulting principal components, outstanding with respect to their temporal persistence and spatial coverage, could be associated with aerosol particle modes: a first accumulation mode ("droplet mode", 300–800 nm), considered to be the result of liquid phase processes and far-range transport; a second accumulation mode (centered around diameters 90–250 nm), considered to result from primary emissions as well as aging through condensation and coagulation; an Aitken mode (30–200 nm) linked to urban traffic emissions in addition to an urban and a rural Aitken mode; a nucleation mode (5–20 nm) linked to urban traffic emissions; nucleation modes (3–20 nm) linked to photochemically induced particle formation; an aged nucleation mode (10–50 nm). A number of additional components were identified to represent only local sources at a single site each, or infrequent phenomena. In summary, the analysis of size distributions of high time and size resolution yielded a surprising wealth of statistical aerosol components occurring in the urban atmosphere over one single city. Meanwhile, satisfactory physical explanations could be found for the components with the greatest temporal persistence and spatial coverage. Therefore a paradigm on the behaviour of sub-μm urban aerosol particles is proposed, with recommendations how to efficiently monitor individual sub-fractions across an entire city.


2019 ◽  
Vol 9 (23) ◽  
pp. 5259
Author(s):  
Feng Wang ◽  
Qixing Zhang ◽  
Xuezhe Xu ◽  
Weixiong Zhao ◽  
Yongming Zhang ◽  
...  

Controlled laboratory combustion experiments were conducted in the fire test room to mimic freshly emitted smoldering smoke of biomass burning in China. The biomass components were determined by ultimate analysis and proximate analysis before experiments. The particle number size distribution (PNSD) between 5 and 1000 nm of smoke was measured by a high sampling frequency size spectrometer. A cavity-enhanced aerosol albedometer with wavelength of 532 nm was used to measure scattering coefficients, extinction coefficients, and single scattering albedo (SSA) of smoldering smoke. The PNSDs of smoldering smoke from the burning of agricultural straw could be fitted with a bimodal lognormal distribution as modes around 10 nm (nucleation mode) and 60 nm (Aitken mode). The PNSDs of wood sawdust could be fitted with a trimodal lognormal distribution, while the two modes were in nucleation mode, and one was in Aitken mode. The bulk optical properties (scattering and extinction coefficients) of smoldering smoke had strong correlations with particle number concentrations of sizes bigger than 100 nm. The correlation between SSA and fixed carbon (FC) was strong (the correlation coefficient is 0.89), while the correlation between SSA and volatile matter (VM) or ash was weak. The relationship between SSA and N (or S) showed a positive correlation, while that of SSA and C showed a negative correlation. The relationship between SSA and VM/FC (or N) showed a strong linear relationship (r2 > 0.8). This paper could improve understanding of the relationship between the optical and particle size distribution properties of smoke from biomass burning and the components of biomass materials under similar combustion conditions.


2009 ◽  
Vol 9 (19) ◽  
pp. 7551-7575 ◽  
Author(s):  
S. S. Gunthe ◽  
S. M. King ◽  
D. Rose ◽  
Q. Chen ◽  
P. Roldin ◽  
...  

Abstract. Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. We have measured and characterized CCN at water vapor supersaturations in the range of S=0.10–0.82% in pristine tropical rainforest air during the AMAZE-08 campaign in central Amazonia. The effective hygroscopicity parameters describing the influence of chemical composition on the CCN activity of aerosol particles varied in the range of κ≈0.1–0.4 (0.16±0.06 arithmetic mean and standard deviation). The overall median value of κ≈0.15 was by a factor of two lower than the values typically observed for continental aerosols in other regions of the world. Aitken mode particles were less hygroscopic than accumulation mode particles (κ≈0.1 at D≈50 nm; κ≈0.2 at D≈200 nm), which is in agreement with earlier hygroscopicity tandem differential mobility analyzer (H-TDMA) studies. The CCN measurement results are consistent with aerosol mass spectrometry (AMS) data, showing that the organic mass fraction (forg) was on average as high as ~90% in the Aitken mode (D≤100 nm) and decreased with increasing particle diameter in the accumulation mode (~80% at D≈200 nm). The κ values exhibited a negative linear correlation with forg (R2=0.81), and extrapolation yielded the following effective hygroscopicity parameters for organic and inorganic particle components: κorg≈0.1 which can be regarded as the effective hygroscopicity of biogenic secondary organic aerosol (SOA) and κinorg≈0.6 which is characteristic for ammonium sulfate and related salts. Both the size dependence and the temporal variability of effective particle hygroscopicity could be parameterized as a function of AMS-based organic and inorganic mass fractions (κp=κorg×forg +κinorg×finorg). The CCN number concentrations predicted with κp were in fair agreement with the measurement results (~20% average deviation). The median CCN number concentrations at S=0.1–0.82% ranged from NCCN,0.10≈35 cm−3 to NCCN,0.82≈160 cm−3, the median concentration of aerosol particles larger than 30 nm was NCN,30≈200 cm−3, and the corresponding integral CCN efficiencies were in the range of NCCN,0.10/NCN,30≈0.1 to NCCN,0.82/NCN,30≈0.8. Although the number concentrations and hygroscopicity parameters were much lower in pristine rainforest air, the integral CCN efficiencies observed were similar to those in highly polluted megacity air. Moreover, model calculations of NCCN,S assuming an approximate global average value of κ≈0.3 for continental aerosols led to systematic overpredictions, but the average deviations exceeded ~50% only at low water vapor supersaturation (0.1%) and low particle number concentrations (≤100 cm−3). Model calculations assuming a constant aerosol size distribution led to higher average deviations at all investigated levels of supersaturation: ~60% for the campaign average distribution and ~1600% for a generic remote continental size distribution. These findings confirm earlier studies suggesting that aerosol particle number and size are the major predictors for the variability of the CCN concentration in continental boundary layer air, followed by particle composition and hygroscopicity as relatively minor modulators. Depending on the required and applicable level of detail, the information and parameterizations presented in this paper should enable efficient description of the CCN properties of pristine tropical rainforest aerosols of Amazonia in detailed process models as well as in large-scale atmospheric and climate models.


2008 ◽  
Vol 42 (34) ◽  
pp. 7967-7980 ◽  
Author(s):  
Zhijun Wu ◽  
Min Hu ◽  
Peng Lin ◽  
Shang Liu ◽  
Birgit Wehner ◽  
...  

2005 ◽  
Vol 5 (1) ◽  
pp. 57-66 ◽  
Author(s):  
P. Mönkkönen ◽  
I. K. Koponen ◽  
K. E. J. Lehtinen ◽  
K. Hämeri ◽  
R. Uma ◽  
...  

Abstract. Diurnal variation of number size distribution (particle size 3-800nm) and modal parameters (geometric standard deviation, geometric mean diameter and modal aerosol particle concentration) in a highly polluted urban environment was investigated during October and November 2002 in New Delhi, India. Continuous monitoring for more than two weeks with the time resolution of 10min was conducted using a Differential Mobility Particle Sizer (twin DMPS). The results indicated clear increase in Aitken mode (25-100nm) particles during traffic peak hours, but towards the evenings there were more Aitken mode particles compared to the mornings. Also high concentrations of accumulation mode particles (>100nm) were detected in the evenings only. In the evenings, biomass/refuse burning and cooking are possible sources beside the traffic. We have also shown that nucleation events are possible in this kind of atmosphere even though as clear nucleation events as observed in rural sites could not be detected. The formation rate of 3nm particles (J3) of the observed events varied from 3.3 to 13.9cm-3s-1 and the growth rate varied from 11.6 to 18.1nmh-1 showing rapid growth and high formation rate, which seems to be typical in urban areas.


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