scholarly journals Hygroscopic properties and mixing state of aerosol measured at the high-altitude site Puy de Dôme (1465 m a.s.l.), France

2014 ◽  
Vol 14 (18) ◽  
pp. 9537-9554 ◽  
Author(s):  
H. Holmgren ◽  
K. Sellegri ◽  
M. Hervo ◽  
C. Rose ◽  
E. Freney ◽  
...  

Abstract. A Hygroscopicity Tandem Differential Mobility Analyser (HTDMA) was used to evaluate the hygroscopic properties of aerosol particles measured at the Puy de Dôme research station in central France, periodically from September 2008 to January 2010, and almost continuously from October 2010 to December 2012. This high-altitude site is ideally situated to allow for both the upper part of the planetary boundary layer and the lower free troposphere to be sampled. The aim of the study is to investigate both the influence of year-to-year, seasonal and diurnal cycles, as well as the influence of air mass type on particle hygroscopicity and mixing state. Results show that particle hygroscopicity increases with particle size and depends both on air mass type and on season. Average growth factor values, GFs, are lowest in winter (1.21 ± 0.13, 1.23 ± 0.18 and 1.38 ± 0.25 for 25, 50 and 165 nm particles, respectively) and highest in autumn (1.27 ± 0.11, 1.32 ± 0.12 and 1.49 ± 0.15 for 25, 50 and 165 nm particles, respectively). Particles are generally more hygroscopic at night than during the day. The seasonal and diurnal variations are likely to be strongly influenced by boundary layer dynamics. Furthermore, particles originating from oceanic and continental regions tend to be more hygroscopic than those measured in African and local air masses. The high hygroscopicity of oceanic aerosol can be explained by large proportions of inorganic aerosol and sea salts. Aerosols measured at the Puy de Dôme display a high degree of external mixing, and hygroscopic growth spectra can be divided into three different hygroscopic modes: a less-hygroscopic mode (GF < 1.3), a hygroscopic mode (GF~1.3–1.7) and a more-hygroscopic mode (GF > 1.7). The majority of particles measured can be classified as being in either the less-hygroscopic mode or the hygroscopic mode, and only few of them have more-hygroscopic properties. The degree of external mixing, evaluated as the fraction of time when the aerosol is found with two or more aerosol populations with different hygroscopic properties, increases with particle size (average yearly values are 20, 28 and 45 {%} for 25, 50, and 165 nm particles, respectively). The degree of external mixing is more sensitive to season than to air mass type, and it is higher in the cold seasons than in the warm seasons. With more than two years of nearly continuous measurements, this study gathers the results from one of the longest data sets of hygroscopic growth factor measurements to date, allowing a statistically relevant hygroscopic growth parameterization to be determined as a function of both air mass type and season.

2014 ◽  
Vol 14 (5) ◽  
pp. 6759-6802
Author(s):  
H. Holmgren ◽  
K. Sellegri ◽  
M. Hervo ◽  
C. Rose ◽  
E. Freney ◽  
...  

Abstract. A Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) was used to evaluate the hygroscopic properties of aerosol particles measured at the Puy de Dôme research station in central France from September 2008 to December 2012. This high-altitude site is ideally situated to allow for both the upper part of the planetary boundary layer and the lower free troposphere to be sampled. The aim of the study is to investigate both the influence of year-to-year, seasonal, and diurnal cycles, as well as the influence of air mass type on particle hygroscopicity and mixing state. Results show that particle hygroscopicity increases with particle size and depends both on air mass type and on season. Average growth factor values are lowest in winter (1.21 ± 0.13, 1.23 ± 0.18 and 1.38 ± 0.25 for 25, 50 and 165 nm particles, respectively) and highest in autumn (1.27 ± 0.11, 1.32 ± 0.12 and 1.49 ± 0.15 for 25, 50 and 165 nm particles, respectively). Particles are generally more hygroscopic at night than during the day. The seasonal and diurnal variations are likely to be strongly influenced by boundary layer dynamics. Furthermore, particles originating from oceanic and continental regions tend to be more hygroscopic than those measured in African and local air masses. The high hygroscopicity of marine aerosol may be explained by large proportions of inorganic aerosol and sea salts, and it is speculated that continental particles are more hygroscopic than local and African ones due to ageing of fresh combustion aerosol. Aerosol measured at the Puy de Dôme display a high degree of external mixing, and hygroscopic growth spectra can be divided into three different hygroscopic modes: a less hygroscopic mode (GF < 1.3), a hygroscopic mode (GF 1.3–1.7) and a more hygroscopic mode (GF > 1.7). The majority of particles measured can be classified as being in either the less hygroscopic mode or the hygroscopic mode, and only few of them have more hygroscopic properties. The degree of external mixing, evaluated as the fraction of time when the aerosol is found with two or more populations with different hygroscopic properties, is found to increase with particle size (average yearly values are 22, 33 and 49% for 25, 50, and 165 nm particles, respectively). The degree of external mixing is more sensitive to season than to air mass type, and it is higher in the cold seasons than in the warm seasons. This study gathers the results from one of the longest data sets of hygroscopic growth factor measurements to date, allowing a statistically relevant hygroscopic growth parameterization to be determined as a function of both air mass type and season.


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.


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.


2020 ◽  
Vol 22 (20) ◽  
pp. 11327-11336
Author(s):  
C. P. F. Day ◽  
A. Miloserdov ◽  
K. Wildish-Jones ◽  
E. Pearson ◽  
A. E. Carruthers

The hygroscopic growth factor for individual aqueous 2-hydroxypropyl β-cyclodextrin droplets has been measured and compared with dynamic vapour sorption measurements.


2020 ◽  
Author(s):  
Chang Hoon Jung ◽  
JiYi Lee ◽  
Junshik Um ◽  
Yong Pyo Kim

&lt;p&gt;In this study, simplified analytic type of expression for size dependent MEs (Mass efficiencies) are developed. The entire size was considered assuming lognormal size distribution for sulfate, nitrate and NaCl aerosol species and the MEE of each aerosol chemical composition was estimated by fitting Mie&amp;#8217;s calculation. The obtained results are compared with the results from the Mie-theory-based calculations and showed comparable results.&lt;/p&gt;&lt;p&gt;The mass efficiencies of all aerosol components for each size range are compared with Mie&amp;#8217;s results and approximated as a function of geometric mean diameter in the form of a power law formula. Finally, harmonic mean type approximation was used to cover entire particle size range.&lt;/p&gt;&lt;p&gt;Also, analytic expression of approximated scattering enhancement factor which stands for the effect of hygroscopic growth factor for polydispersed aerosol on aerosol optical properties are obtained.&lt;/p&gt;&lt;p&gt;Based on aerosol thermodynamic models, mass growth factor can be obtained and their optical properties can be obtained by using Mie theory with different aerosol properties and size distribution. Finally, scattering enhancement factor was approximated fRH for polydispersed aerosol as a function of RH.&lt;/p&gt;&lt;p&gt;Finally, we also compared the simple forcing efficiency (SFE, W/g) of polydisperse aerosols between the developed simple approach and by the method using the Mie theory. The results show that current obtained approximated methods are comparable with existing numercal calculation based results for polydipersed particle size.&lt;/p&gt;


2021 ◽  
Author(s):  
Diego Aliaga ◽  
Victoria A. Sinclair ◽  
Marcos Andrade ◽  
Paulo Artaxo ◽  
Samara Carbone ◽  
...  

Abstract. Observations of aerosol and trace gases in the remote troposphere are vital to quantify background concentrations and identify long term trends in atmospheric composition on large spatial scales. Measurements made at high altitude are often used to study free tropospheric air however such high-altitude sites can be influenced by boundary layer air masses. Thus, accurate information on air mass origin and transport pathways to high altitude sites is required. Here we present a new method, based on the source-receptor relationship (SRR) obtained from backwards WRF-FLEXPART simulations and a k-means clustering approach, to identify source regions of air masses arriving at measurement sites. Our method is tailored to areas of complex terrain and to stations influenced by both local and long-range sources. We have applied this method to the Chacaltaya (CHC) GAW station (5240 m a.s.l.,16.35° S, 68.13° W) for the 6-month duration of the “Southern hemisphere high altitude experiment on particle nucleation and growth” (SALTENA) to identify where sampled air masses originate and to quantify the influence of the boundary layer and the free troposphere. A key aspect of our method is that it is probabilistic and for each observation time, more than one air mass (cluster) can influence the station and the percentage influence of each air mass can be quantified. This is in contrast to binary methods, which label each observation time as influenced either by boundary layer or free troposphere air masses. We find that on average, 9% of the air sampled at CHC, at any given observation time, has been in contact with the surface within 4 days prior to arriving at CHC, 24% of the air was located below 1.5 km above ground level and consequently, 76% of the measured air masses at CHC represent free tropospheric air. However, pure free-tropospheric influences are rare and often samples are concurrently influenced by both boundary-layer and free-tropospheric air masses. A clear diurnal cycle is present with very few air masses that have been in contact with the surface being detected at night. The 6-month analysis also shows that the most dominant air mass (cluster) originates in the Amazon and is responsible for 29% of the sampled air. Furthermore, short-range clusters (origins within 100 km of CHC) have high temporal frequency modulated by local meteorology driven by the diurnal cycle whereas the mid- and long-range clusters’ (>200 km) variability occurs on timescales governed by synoptic-scale dynamics. To verify the reliability of our method, in-situ sulfate observations from CHC are combined with the SRR clusters to correctly identify the (pre-known) source of the sulfate: the Sabancaya volcano located 400 km northwest from the station.


Atmosphere ◽  
2018 ◽  
Vol 9 (8) ◽  
pp. 293 ◽  
Author(s):  
Eric Kelsey ◽  
Adriana Bailey ◽  
Georgia Murray

Discrimination of the type of air mass along mountain slopes can be a challenge and is not commonly performed, but is critical for identifying factors responsible for influencing montane weather, climate, and air quality. A field campaign to measure air mass type and transitions on the summit of Mount Washington, New Hampshire, USA was performed on 19 August 2016. Meteorological observations were taken at the summit and at several sites along the east and west slopes. Ozone concentrations were measured at the summit and on the valley floor. Additionally, water vapor stable isotopes were measured from a truck that drove up and down the Mount Washington Auto Road concurrent with radiosonde launches that profiled the free atmosphere. This multivariate perspective revealed thermal, moisture, and air mass height differences among the free atmosphere, leeward, and windward mountain slopes. Both thermally and mechanically forced upslope flows helped shape these differences by altering the height of the boundary layer with respect to the mountain surface. Recommendations for measurement strategies hoping to develop accurate observational climatologies of air mass exposure in complex terrain are discussed and will be important for evaluating elevation-dependent warming and improving forecasting for weather and air quality.


2014 ◽  
Vol 14 (14) ◽  
pp. 7519-7531 ◽  
Author(s):  
J. Jung ◽  
K. Kawamura

Abstract. To investigate the hygroscopic properties of ultrafine particles during new particle formation events, the hygroscopic growth factors of size-segregated atmospheric particles were measured at an urban site in Sapporo, northern Japan, during the summer of 2011. The hygroscopic growth factor at 85 % relative humidity [g(85%)] of freshly formed nucleation mode particles was 1.11 to 1.28 (average: 1.16 ± 0.06) at a dry particle diameter (Dp) centered on 20 nm, which is equivalent to 1.17 to 1.35 (1.23 ± 0.06) at a dry Dp centered on 100 nm after considering the Kelvin effect. These values are comparable with those of secondary organic aerosols, suggesting that low-volatility organic vapors are important to the burst of nucleation mode particles. The equivalent g(85%) at a dry Dp of 100 nm for nucleated particles that have grown to Aitken mode sizes (1.24 to 1.34; average: 1.30 ± 0.04) were slightly higher than those of newly formed nucleation mode particles, suggesting that the growth of freshly formed nucleation mode particles to the Aitken mode size can be subjected to condensation of not only low-volatility organic vapors, but also water-soluble inorganic species. Based on this result, and previous measurement of radiocarbon in aerosols, we suggest that the burst of nucleation mode particles and their subsequent growth were highly affected by biogenic organic emissions at this measurement site, which is surrounded by deciduous forest. Gradual increases in mode diameter after the burst of nucleation mode particles were observed under southerly wind conditions, with a dominant contribution of intermediately hygroscopic particles. However, sharp increases in mode diameter were observed when the wind direction shifted to northwesterly or northeasterly, with a sharp increase in the highly hygroscopic particle fraction of the Aitken mode particles, indicating that the hygroscopic growth factor of newly formed particles is perturbed by the local winds that deliver different air masses to the measurement site.


2018 ◽  
Vol 18 (16) ◽  
pp. 11739-11752 ◽  
Author(s):  
Yuying Wang ◽  
Zhanqing Li ◽  
Yingjie Zhang ◽  
Wei Du ◽  
Fang Zhang ◽  
...  

Abstract. This study investigates aerosol hygroscopicity, mixing state, and cloud condensation nucleation as part of the Atmosphere–Aerosol–Boundary Layer–Cloud Interaction Joint Experiment performed in the summer of 2016 at Xingtai (XT), a suburban site located in the center of the North China Plain (NCP). In general, the probability density function (PDF) of the hygroscopicity parameter (κ) for 40–200 nm particles had a unimodal distribution, and mean κ-PDF patterns for different sizes were similar, suggesting that the particles were highly aged and internally mixed because of strong photochemical reactions. The κ calculated from the hygroscopic growth factor in the daytime and at night suggests that photochemical reactions largely enhanced the aerosol hygroscopicity. This effect became weaker as the particle size increased. In addition, the aerosol hygroscopicity was much larger at XT than at other sites in the NCP. This is because new particle formation takes place much more frequently in the central NCP, which is heavily polluted from industrial activities, than elsewhere in the region. The evolution of the planetary boundary layer played a dominant role in dictating aerosol mass concentration. Particle size was the most important factor influencing the ability of aerosols to activate, whereas the effect of chemical composition was secondary, especially when supersaturation was high. Using a fixed value of κ=0.31 to calculate the cloud condensation nuclei number concentration in this region suffices.


2005 ◽  
Vol 5 (8) ◽  
pp. 2203-2226 ◽  
Author(s):  
R. Van Dingenen ◽  
J.-P. Putaud ◽  
S. Martins-Dos Santos ◽  
F. Raes

Abstract. Aerosol physical properties were measured at the Monte Cimone Observatory (Italy) from 1 June till 6 July 2000. The measurement site is located in the transition zone between the continental boundary layer and the free troposphere (FT), at the border between the Mediterranean area and Central Europe, and is exposed to a variety of air masses. Sub-μm number size distributions, aerosol hygroscopicity near 90% RH, refractory size distribution at 270°C and equivalent black carbon mass were continuously measured. Number size distributions and hygroscopic properties indicate that the site is exposed to aged continental air masses, however during daytime it is also affected by upslope winds. The mixing of this transported polluted boundary layer air masses with relatively clean FT air leads to frequent nucleation events around local noon. Night-time size distributions, including fine and coarse fractions for each air mass episode, have been parameterized by a 3-modal lognormal distribution. Number and volume concentrations in the sub-μm modes are strongly affected by the air mass origin, with highest levels in NW-European air masses, versus very clean, free tropospheric air coming from the N-European sector. During a brief but distinct dust episode, the coarse mode is clearly enhanced. The observed hygroscopic behavior of the aerosol is consistent with the chemical composition described by Putaud et al. (2004), but no closure between known chemical composition and measured hygroscopicity could be made because the hygroscopic properties of the water-soluble organic matter (WSOM) are not known. The data suggest that WSOM is slightly-to-moderately hygroscopic (hygroscopic growth factor GF at 90% relative humidity between 1.05 and 1.51), and that this property may well depend on the air mass origin and history. External mixing of aerosol particles is observed in all air masses through the occurrence of two hygroscopicity modes (average GF of 1.22 and 1.37, respectively). However, the presence of "less" hygroscopic particles has mostly such a low occurrence rate that the average growth factor distribution for each air mass sector actually appears as a single mode. This is not the case for the dust episode, where the external mixing between less hygroscopic and more hygroscopic particles is very prominent, and indicating clearly the occurrence of a dust accumulation mode, extending down to 50 nm particles, along with an anthropogenic pollution mode. The presented physical measurements finally allow us to provide a partitioning of the sub-μm aerosol in four non-overlapping fractions (soluble/volatile, non-soluble/volatile, refractory/non-black carbon, black carbon) which can be associated with separate groups of chemical compounds determined with chemical-analytical techniques (ions, non-water soluble organic matter, dust, elemental carbon). All air masses except the free-tropospheric N-European and Dust episodes show a similar composition within the uncertainty of the data (53%, 37%, 5% and 5% respectively for the four defined fractions). Compared to these sectors, the dust episode shows a clearly enhanced refractory-non-BC fraction (17%), attributed to dust in the accumulation mode, whereas for the very clean N-EUR sector, the total refractory fraction is 25%, of which 13% non-BC and 12% BC.


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