scholarly journals Hygroscopic growth of urban aerosol particles in Beijing (China) during wintertime: a comparison of three experimental methods

2009 ◽  
Vol 9 (18) ◽  
pp. 6865-6880 ◽  
Author(s):  
J. Meier ◽  
B. Wehner ◽  
A. Massling ◽  
W. Birmili ◽  
A. Nowak ◽  
...  

Abstract. The hygroscopic properties of atmospheric aerosols are highly relevant for the quantification of radiative effects in the atmosphere, but also of interest for the assessment of particle health effects upon inhalation. This article reports measurements of aerosol particle hygroscopicity in the highly polluted urban atmosphere of Beijing, China in January 2005. The meteorological conditions corresponded to a relatively cold and dry atmosphere. Three different methods were used: 1) A combination of Humidifying Differential Mobility Particle Sizer (H-DMPS) and Twin Differential Mobility Particle Sizer (TDMPS) measurements, 2) A Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA), and 3) A simplistic solubility model fed by chemical particle composition determined from Micro Orifice Uniform Deposit Impactor (MOUDI) samples. From the H-DMPS and TDMPS particle number size distributions, a size-resolved descriptive hygroscopic growth factor (DHGF) was determined for the relative humidities (RH) 55%, 77% and 90%, and particle diameters between 30 and 400 nm. In Beijing, the highest DHGFs were observed for accumulation mode particles, 1.40 (±0.03) at 90% RH. DHGF decreased significantly with particle size, reaching 1.04 (±0.15) at 30 nm. H-TDMA data also suggest a decrease in growth factor towards the biggest particles investigated (350 nm), associated with an increasing fraction of nearly hydrophobic particles. The agreement between the H-DMPS/TDMPS and H-TDMA methods was satisfactory in the accumulation mode size range (100–400 nm). In the Aitken mode range (<100 nm), the H-DMPS/TDMPS method yielded growth factors lower by up to 0.1 at 90% RH. The application of the solubility model based on measured chemical composition clearly reproduced the size-dependent trend in hygroscopic particle growth observed by the other methods. In the case of aerosol dominated by inorganic ions, the composition-derived growth factors tended to agree (± 0.05) or underestimate (up to 0.1) the values measured by the other two methods. In the case of aerosol dominated by organics, the reverse was true, with an overestimation of up to 0.2. The results shed light on the experimental and methodological uncertainties that are still connected with the determination of hygroscopic growth factors.

2009 ◽  
Vol 9 (2) ◽  
pp. 6889-6927 ◽  
Author(s):  
J. Meier ◽  
B. Wehner ◽  
A. Massling ◽  
W. Birmili ◽  
A. Nowak ◽  
...  

Abstract. This paper presents hygroscopicity measurements of aerosol particles in the urban atmosphere of Beijing carried out in January 2005. Therefore, three different methods were used: 1) Combining Humidifying Differential Mobility Particle Sizer (H-DMPS) and Twin Differential Mobility Particle Sizer (TDMPS) measurements; 2) Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) technique; 3) Calculating hygroscopic growth factors on the basis of a solubility model quantified by Micro Orifice Uniform Deposit Impactor (MOUDI) samples. Particle number size distributions from H-DMPS and TDMPS were evaluated to derive size-resolved descriptive hygroscopic growth factors (DHGF) of 30–400 nm particles at relative humidities (RH) of 55%, 77% and 90%. The atmospheric particles in Beijing were rather hydrophobic, with a maximum growth factor in the accumulation mode around 1.40 (±0.03) at 90% RH. The descriptive hygroscopic growth factors decreased significantly towards the lower measurement limit (1.04 (±0.15) at Dp=30 nm). A good agreement was found between the DHGFs and the H-TDMA-derived hygroscopic growth factors in the accumulation mode (100–400 nm), the DHGFs underestimated the values from the H-TDMA in the Aitken mode (<100 nm) by up to 0.1 at 90% RH. The calculation of hygroscopic growth factors based on the measured chemical composition showed that different modes of combining the inorganic ions caused a variation in growth factor of 0.1 at 90% RH. The solubility model was able to reproduce the size-dependent trend in the growth factor found by the other methods. In two cases of ion-dominated aerosol, the composition-derived growth factors tended to agree (±0.05) or underestimate (up to 0.1) the values measured by the other two methods. In the case of the organic-dominated aerosol, the reverse was true, with an overestimation of up to 0.2. The results shed light on the real experimental and methodological uncertainties that are still connected with the determination of hygroscopic growth factors.


2006 ◽  
Vol 6 (2) ◽  
pp. 471-491 ◽  
Author(s):  
J. Rissler ◽  
A. Vestin ◽  
E. Swietlicki ◽  
G. Fisch ◽  
J. Zhou ◽  
...  

Abstract. Aerosol particle number size distributions and hygroscopic properties were measured at a pasture site in the southwestern Amazon region (Rondonia). The measurements were performed 11 September-14 November 2002 as part of LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia - SMOke aerosols, Clouds, rainfall and Climate), and cover the later part of the dry season (with heavy biomass burning), a transition period, and the onset of the wet period. Particle number size distributions were measured with a DMPS (Differential Mobility Particle Sizer, 3-850nm) and an APS (Aerodynamic Particle Sizer), extending the distributions up to 3.3 µm in diameter. An H-TDMA (Hygroscopic Tandem Differential Mobility Analyzer) measured the hygroscopic diameter growth factors (Gf) at 90% relative humidity (RH), for particles with dry diameters (dp) between 20-440 nm, and at several occasions RH scans (30-90% RH) were performed for 165nm particles. These data provide the most extensive characterization of Amazonian biomass burning aerosol, with respect to particle number size distributions and hygroscopic properties, presented until now. The evolution of the convective boundary layer over the course of the day causes a distinct diel variation in the aerosol physical properties, which was used to get information about the properties of the aerosol at higher altitudes. The number size distributions averaged over the three defined time periods showed three modes; a nucleation mode with geometrical median diameters (GMD) of ~12 nm, an Aitken mode (GMD=61-92 nm) and an accumulation mode (GMD=128-190 nm). The two larger modes were shifted towards larger GMD with increasing influence from biomass burning. The hygroscopic growth at 90% RH revealed a somewhat external mixture with two groups of particles; here denoted nearly hydrophobic (Gf~1.09 for 100 nm particles) and moderately hygroscopic (Gf~1.26). While the hygroscopic growth factors were surprisingly similar over the periods, the number fraction of particles belonging to each hygroscopic group varied more, with the dry period aerosol being more dominated by nearly hydrophobic particles. As a result the total particle water uptake rose going into the cleaner period. The fraction of moderately hygroscopic particles was consistently larger for particles in the accumulation mode compared to the Aitken mode for all periods. Scanning the H-TDMA over RH (30-90% RH) showed no deliquescence behavior. A parameterization of both Gf(RH) and Gf(dp), is given.


2014 ◽  
Vol 14 (2) ◽  
pp. 737-749 ◽  
Author(s):  
K. A. Kamilli ◽  
L. Poulain ◽  
A. Held ◽  
A. Nowak ◽  
W. Birmili ◽  
...  

Abstract. Aerosol hygroscopic growth factors and chemical properties were measured as part of the MEGAPOLI "Megacities Plume Case Study" at the urban site Laboratoire d'Hygiène de la Ville de Paris (LHVP) in the city center of Paris from June to August 2009, and from January to February 2010. Descriptive hygroscopic growth factors (DGF) were derived in the diameter range from 25 to 350 nm at relative humidities of 30, 55, 75, and 90% by applying the summation method on humidified and dry aerosol size distributions measured simultaneously with a humidified differential mobility particle sizer (HDMPS) and a twin differential mobility particle sizer (TDMPS). For 90% relative humidity, the DGF varied from 1.06 to 1.46 in summer, and from 1.06 to 1.66 in winter. Temporal variations in the observed mean DGF could be well explained with a simple growth model based on the aerosol chemical composition measured by aerosol mass spectrometry (AMS) and black carbon photometry (MAAP). In particular, good agreement was observed when sulfate was the predominant inorganic factor. A clear overestimation of the predicted growth factor was found when the nitrate mass concentration exceeded values of 10 μg m−3, e.g., during winter.


2011 ◽  
Vol 11 (2) ◽  
pp. 6601-6650
Author(s):  
E. O. Fors ◽  
E. Swietlicki ◽  
B. Svenningsson ◽  
A. Kristensson ◽  
G. P. Frank ◽  
...  

Abstract. The hygroscopic growth of the atmospheric aerosol is a critical parameter for quantifying the anthropogenic radiative forcing. Until now, there has been a lack of long term measurements due to limitations in instrumental techniques. In this work, for the first time the seasonal variation of the hygroscopic properties of a continental background aerosol has been described, based on more than two years of continuous measurements. In addition to this, the diurnal variation of the hygroscopic growth has been investigated, as well as the seasonal variation in CCN concentration. These physical properties of the aerosol have been measured with a Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA), a Differential Mobility Particle Sizer (DMPS), and a Cloud Condensation Nuclei Counter (CCNC). The results show that smaller particles are generally less hygroscopic than larger ones, and that there is a clear difference in the hygroscopic properties between the Aitken and the accumulation mode. A seasonal cycle was found for all particle sizes. In general, the average hygroscopic growth is lower during wintertime, due to an increase in the relative abundance of less hygroscopic or hydrophobic particles. Monthly averages showed that the hygroscopic growth factors of the two dominating hygroscopic modes (one barely hygroscopic and one more hygroscopic) were relatively stable. The hygroscopic growth additionally showed a diurnal cycle, with higher growth factors during day time. CCN predictions based on H-TDMA data underpredicted the activated CCN concentration with 7% for 1% water supersaturation (s). The underprediction increases with decreasing $s$, most likely due to a combination of measurement and modeling uncertainties. It was found that although the aerosol is often externally mixed, recalculating to an internal mixture with respect to hygroscopicity did not change CCN parameterizations significantly.


2011 ◽  
Vol 11 (16) ◽  
pp. 8343-8361 ◽  
Author(s):  
E. O. Fors ◽  
E. Swietlicki ◽  
B. Svenningsson ◽  
A. Kristensson ◽  
G. P. Frank ◽  
...  

Abstract. The hygroscopic growth of the atmospheric aerosol is a critical parameter for quantifying the anthropogenic radiative forcing. Until now, there has been a lack of long term measurements due to limitations in instrumental techniques. In this work, for the first time the seasonal variation of the hygroscopic properties of a continental background aerosol has been described, based on more than two years of continuous measurements. In addition to this, the diurnal variation of the hygroscopic growth has been investigated, as well as the seasonal variation in CCN concentration. These physical properties of the aerosol have been measured with a Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA), a Differential Mobility Particle Sizer (DMPS), and a Cloud Condensation Nuclei Counter (CCNC). The results show that smaller particles are generally less hygroscopic than larger ones, and that there is a clear difference in the hygroscopic properties between the Aitken and the accumulation mode. A seasonal cycle was found for all particle sizes. In general, the average hygroscopic growth is lower during wintertime, due to an increase in the relative abundance of less hygroscopic or barely hygroscopic particles. Monthly averages showed that the hygroscopic growth factors of the two dominating hygroscopic modes (one barely hygroscopic and one more hygroscopic) were relatively stable. The hygroscopic growth additionally showed a diurnal cycle, with higher growth factors during day time. CCN predictions based on H-TDMA data underpredicted the activated CCN number concentration with 7 % for a 1 % water supersaturation ratio. The underprediction increases with decreasing s, most likely due to a combination of measurement and modeling uncertainties. It was found that although the aerosol is often externally mixed, recalculating to an internal mixture with respect to hygroscopicity did not change the CCN concentration as a function of supersaturation significantly.


2013 ◽  
Vol 13 (5) ◽  
pp. 14297-14330
Author(s):  
K. A. Kamilli ◽  
L. Poulain ◽  
A. Held ◽  
A. Nowak ◽  
W. Birmili ◽  
...  

Abstract. Aerosol hygroscopic growth factors and chemical properties were measured as part of the MEGAPOLI "Megacities Plume Case Study" at the urban site LHVP in the city center of Paris from June to August 2009, and from January to February 2010. Descriptive hygroscopic growth factors (DGF) were derived in the diameter range from 25 to 350 nm at relative humidities of 30, 55, 75, and 90% by applying the summation method on humidified and dry aerosol size distributions measured simultaneously with a humidified differential mobility particle sizer (HDMPS) and a twin differential mobility particle sizer (TDMPS). For 90% relative humidity, the DGF varied from 1.06 to 1.46 in summer, and from 1.06 to 1.66 in winter. Temporal variations in the observed mean DGF could be well explained with a simple growth model based on the aerosol chemical composition measured by aerosol mass spectrometry (AMS) and black carbon photometry (MAAP). In particular, good agreement was observed when sulfate was the predominant inorganic factor. A clear overestimation of the predicted growth factor was found when the nitrate mass concentration exceeded values of 10 μg m3, e.g. during winter.


2013 ◽  
Vol 30 (6) ◽  
pp. 1136-1148 ◽  
Author(s):  
Haobo Tan ◽  
Hanbing Xu ◽  
Qilin Wan ◽  
Fei Li ◽  
Xuejiao Deng ◽  
...  

Abstract The hygroscopic properties of aerosols have a significant impact on aerosol particle number size distributions (PNSD), formation of cloud condensation nuclei, climate forcing, and atmospheric visibility, as well as human health. To allow for the observation of the hygroscopic growth of aerosols with long-term accuracy, an unattended multifunctional hygroscopicity-tandem differential mobility analyzer (H-TDMA) system was designed and built by the Institute of Tropical and Marine Meteorology (ITMM), China Meteorological Administration (CMA), in Guangzhou, China. The system is capable of measuring dry and wet PNSD, hygroscopic growth factor by particle size, and mixing states. This article describes in detail the working principles, components, and calibration methods of the system. Standard polystyrene latex (PSL) spheres with five different diameters were chosen to test the system’s precision and accuracy of particle size measurement. Ammonium sulfate was used to test the hygroscopic response of the system for accurate growth factor measurement. The test results show that the deviation of the growth factor measured by the system is within a scope of −0.01 to −0.03 compared to Köhler theoretical curves. Results of temperature and humidity control performance tests indicate that the system is robust. An internal temperature gradient of less than 0.2 K for a second differential mobility analyzer (DMA2) makes it possible to reach a set-point relative humidity (RH) value of 90% and with a standard deviation of ±0.44%, sufficient for unattended field observation.


2011 ◽  
Vol 11 (9) ◽  
pp. 4251-4271 ◽  
Author(s):  
M. Stock ◽  
Y. F. Cheng ◽  
W. Birmili ◽  
A. Massling ◽  
B. Wehner ◽  
...  

Abstract. This work examines the effect of direct radiative forcing of aerosols in the eastern Mediterranean troposphere as a function of air mass composition, particle size distribution and hygroscopicity, and relative humidity (RH). During intensive field measurements on the island of Crete, Greece, the hygroscopic properties of atmospheric particles were determined using a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) and a Hygroscopicity Differential Mobility Analyzer-Aerodynamic Particle Sizer (H-DMA-APS). Similar to former studies, the H-TDMA identified three hygroscopic sub-fractions of particles in the sub-μm range: a more hygroscopic group, a less hygroscopic group and a nearly hydrophobic particle group. The average hygroscopic particle growth factors at 90 % RH were a significant function of particle mobility diameter (Dp): 1.42 (± 0.05) at 30 nm compared to 1.63 (± 0.07) at 250 nm. The H-DMA-APS identified up to three hygroscopic sub-fractions at mobility diameters of 1.0 and 1.2 μm. The data recorded between 12 August and 20 October 2005 were classified into four distinct synoptic-scale air mass types distinguishing between different regions of origin (western Mediterranean vs. the Aegean Sea) as well as the degree of continental pollution (marine vs. continentally influenced). The hygroscopic properties of particles with diameter Dp≥150 nm showed the most pronounced dependency on air mass origin, with growth factors in marine air masses exceeding those in continentally influenced air masses. Particle size distributions and hygroscopic growth factors were used to calculate aerosol light scattering coefficients at ambient RH using a Mie model. A main result was the pronounced enhancement of particle scattering over the eastern Mediterranean due to hygroscopic growth, both in the marine and continentally influenced air masses. When RH reached its summer daytime values around 70–80 %, up to 50–70 % of the calculated visibility reduction was due to the hygroscopic growth of the particles by water compared to the effect of the dry particles alone. The estimated aerosol direct radiative forcings for both, marine and continentally influenced air masses were negative indicating a net cooling of the atmosphere due to the aerosol. The radiative forcing ΔFr was nevertheless governed by the total aerosol concentration most of the time: ΔFr was typically more negative for continentally influenced aerosols (ca. −4 W m−2) compared to rather clean marine aerosols (ca. −1.5 W m−2). When RH occasionally reached 90 % in marine air masses, ΔFr even reached values down to −7 W m−2. Our results emphasize, on the basis of explicit particle hygroscopicity measurements, the relevance of ambient RH for the radiative forcing of regional atmospheres.


2010 ◽  
Vol 10 (11) ◽  
pp. 25991-26044
Author(s):  
M. Stock ◽  
Y. F. Cheng ◽  
W. Birmili ◽  
A. Massling ◽  
B. Wehner ◽  
...  

Abstract. This work examines the effect of direct radiative forcing of aerosols in the eastern Mediterranean troposphere as a function of air mass composition, particle size distribution and hygroscopicity, and relative humidity (RH). During intensive field measurements on the island of Crete, Greece, the hygroscopic properties of atmospheric particles were determined using a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) and a Hygroscopicity Differential Mobility Analyzer – Aerodynamic Particle Sizer (H-DMA-APS). Like in several studies before, the H-TDMA identified three hygroscopic sub-fractions of particles in the sub-μm range: a more hygroscopic group, a less hygroscopic group and a nearly hydrophobic particle group. The hygroscopic particle growth factors at 90% RH were a significant function of particle mobility diameter (Dp): 1.42 (± 0.05) at 30 nm compared to 1.63 (± 0.07) at 250 nm. The H-DMA-APS identified up to three hygroscopic sub-fractions at mobility diameters of 1.0 and 1.2 μm. All data recorded between 12 August and 20 October, 2005 were classified into four distinct synoptic-scale air mass types distinguishing between different regions of origin (western Mediterranean vs. the Aegean Sea) as well as the degree of continental pollution (marine vs. continentally influenced). The hygroscopic properties of particles with diameter Dp ≥ 150 nm showed the most pronounced dependency on air mass origin, with growth factors in marine air masses exceeding those in more continentally influenced air masses. Particle size distributions and hygroscopic growth factors were employed to calculate aerosol light scattering coefficients at ambient RH using a Mie model. A main result was the pronounced enhancement of particle scattering over the eastern Mediterranean due to hygroscopic growth, both in the marine and continentally influenced air masses. When RH reached its daytime values around 70–80% in summer, up to 50–70% of the calculated visibility reduction was due to the hygroscopic growth of the particles by water compared to the effect of the dry particles alone. The estimated aerosol direct radiative forcings for both, marine and continentally influenced air masses were negative indicating a net cooling of the atmosphere due to the aerosol. The radiative forcing ΔFr was, nevertheless, dominated by the total aerosol concentration most of the time: ΔFr was typically more negative for continentally influenced aerosols (ca. −4 W m−2) compared to rather clean marine aerosols (ca. −1.5 W m−2). When RH occasionally reached 90% in marine air, ΔFr even reached values down to −7 W m−2. Our results emphasize, on the basis of explicit particle hygroscopicity measurements, the relevance of ambient relative humidity for the radiative forcing of regional atmospheres.


2016 ◽  
Vol 16 (2) ◽  
pp. 1123-1138 ◽  
Author(s):  
Z. J. Wu ◽  
J. Zheng ◽  
D. J. Shang ◽  
Z. F. Du ◽  
Y. S. Wu ◽  
...  

Abstract. Simultaneous measurements of particle number size distribution, particle hygroscopic properties, and size-resolved chemical composition were made during the summer of 2014 in Beijing, China. During the measurement period, the mean hygroscopicity parameters (κs) of 50, 100, 150, 200, and 250 nm particles were respectively 0.16  &amp;pm;  0.07, 0.19  &amp;pm;  0.06, 0.22  &amp;pm;  0.06, 0.26  &amp;pm;  0.07, and 0.28  &amp;pm;  0.10, showing an increasing trend with increasing particle size. Such size dependency of particle hygroscopicity was similar to that of the inorganic mass fraction in PM1. The hydrophilic mode (hygroscopic growth factor, HGF  >  1.2) was more prominent in growth factor probability density distributions and its dominance of hydrophilic mode became more pronounced with increasing particle size. When PM2.5 mass concentration was greater than 50 μg m−3, the fractions of the hydrophilic mode for 150, 250, and 350 nm particles increased towards 1 as PM2.5 mass concentration increased. This indicates that aged particles dominated during severe pollution periods in the atmosphere of Beijing. Particle hygroscopic growth can be well predicted using high-time-resolution size-resolved chemical composition derived from aerosol mass spectrometer (AMS) measurements using the Zdanovskii–Stokes–Robinson (ZSR) mixing rule. The organic hygroscopicity parameter (κorg) showed a positive correlation with the oxygen to carbon ratio. During the new particle formation event associated with strongly active photochemistry, the hygroscopic growth factor or κ of newly formed particles is greater than for particles with the same sizes not during new particle formation (NPF) periods. A quick transformation from external mixture to internal mixture for pre-existing particles (for example, 250 nm particles) was observed. Such transformations may modify the state of the mixture of pre-existing particles and thus modify properties such as the light absorption coefficient and cloud condensation nuclei activation.


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