Particle Hygroscopic Growth Research Articles

Evaluation of a low-cost dryer for a low-cost optical particle counter

Abstract. The use of low-cost sensors for air quality measurements has become very popular in the last few decades. Due to the detrimental effects of particulate matter (PM) on human health, PM sensors like photometers and optical particle counters (OPCs) are widespread and have been widely investigated. The negative effects of high relative humidity (RH) and fog events in the mass concentration readings of these types of sensors are well documented. In the literature, different solutions to these problems – like correction models based on the Köhler theory or machine learning algorithms – have been applied. In this work, an air pre-conditioning method based on a low-cost thermal dryer for a low-cost OPC is presented. This study was done in two parts. The first part of the study was conducted in the laboratory to test the low-cost dryer under two different scenarios. In one scenario, the drying efficiency of the low-cost dryer was investigated in the presence of fog. In the second scenario, experiments with hygroscopic aerosols were done to determine to which extent the low-cost dryer reverts the growth of hygroscopic particles. In the second part of the study, the PM10 and PM2.5 mass concentrations of an OPC with dryer were compared with the gravimetric measurements and a continuous federal equivalent method (FEM) instrument in the field. The feasibility of using univariate linear regression (ULR) to correct the PM data of an OPC with dryer during field measurement was also evaluated. Finally, comparison measurements between an OPC with dryer, an OPC without dryer, and a FEM instrument during a real fog event are also presented. The laboratory results show that the sensor with the low-cost dryer at its inlet measured an average of 64 % and 59 % less PM2.5 concentration compared with a sensor without the low-cost dryer during the experiments with fog and with hygroscopic particles, respectively. The outcomes of the PM2.5 concentrations of the low-cost sensor with dryer in laboratory conditions reveal, however, an excess of heating compared with the FEM instrument. This excess of heating is also demonstrated in a more in-depth study on the temperature profile inside the dryer. The correction of the PM10 concentrations of the sensor with dryer during field measurements by using ULR showed a reduction of the maximum absolute error (MAE) from 4.3 µg m−3 (raw data) to 2.4 µg m−3 (after correction). The results for PM2.5 make evident an increase in the MAE after correction: from 1.9 µg m−3 in the raw data to 3.2 µg m−3. In light of these results, a low-cost thermal dryer could be a cost-effective add-on that could revert the effect of the hygroscopic growth and the fog in the PM readings. However, special care is needed when designing a low-cost dryer for a PM sensor to produce FEM similar PM readings, as high temperatures may irreversibly change the sampled air by evaporating the most volatile particulate species and thus deliver underestimated PM readings. New versions of a low-cost dryer aiming at FEM measurements should focus on maintaining the RH at the sensor inlet at 50 % and avoid reaching temperatures higher than 40 ∘C in the drying system. Finally, we believe that low-cost dryers have a very promising future for the application of sensors in citizen science, sensor networks for supplemental monitoring, and epidemiological studies.

Influence of selected cationic, anionic, and nonionic surfactants on hygroscopic growth of individual aqueous coarse mode aerosol particles

Influence of selected cationic, anionic, and nonionic surfactants on hygroscopic growth of individual aqueous coarse mode aerosol particles

Impacts of snow cover on micrometeorological conditions and rural air quality in Northeast China

Snow cover is one of the most typical underlying surface types in Northeast China in winter. Snow cover can affect air quality potentially through changing atmospheric diffusion capacity, with the underlying physics awaiting a further exploration for Northeast China. Therefore, the impacts of snow cover on micrometeorological conditions and air quality were investigated using surface and tower meteorological observations from October 2019 to March 2020 in Fujin, a typical rural area in the Sanjiang Plain in Northeast China. Low atmospheric visibility and poor air quality were observed to occur more frequently on snow-cover days than on snow-free days, with visibility exhibiting a decreasing trend with increasing snow depth (< 8 cm). Compared with snow-free days, the presence of snow cover was found to produce weakened unstable stratification in the near-surface layer and lower daily surface sensible heat flux (reduced by 54.8%), mainly related to higher snow surface albedo (0.5–0.8), which can suppress the development of daytime atmospheric boundary layer height and vertical dispersion of air pollutants. Moreover, moister ambient conditions on snow-cover days presumably favored secondary aerosol formation and particle hygroscopic growth. Stronger wind speeds and shears, friction velocity, and turbulence kinetic energy were observed on snow-cover days than on snow-free days when the air was clean, probably due to smaller aerodynamic roughness length on snow cover. However, when air pollution occurred on snow cover, winds and mechanic turbulence decreased significantly, favoring aerosols' accumulation near the surface. These findings can facilitate a comprehensive understanding of the physical mechanism of air pollution occurring over a large portion of the snow-cover region in wintertime Northeast China and helpful for the pollution controls.

Constraining the Effect of Surfactants on the Hygroscopic Growth of Model Sea Spray Aerosol Particles

The cloud condensation nuclei activation of sea spray aerosol (SSA) is tightly linked to the hygroscopic properties of these particles and is defined by their physical and chemical properties. While hygroscopic sea salt in SSA strongly influences particle water uptake, the marine-derived components that make up the organic fraction of SSA constitute a complex mixture, and their effect on hygroscopic growth is unknown. To constrain the effect of organic compounds and specifically surface-active compounds that adsorb on particle interfaces, particle hygroscopic growth studies were performed on laboratory-generated model sea salt/sugar particles. For sea salt/glucose particles, ionic surfactants facilitated water uptake at low relative humidity (RH), increasing the particle growth factor (GF) by up to 7.61%, and caused a reduction in the deliquescence relative humidity (DRH), while nonionic surfactants had a minimal effect. Replacing glucose with polysaccharide laminarin in sea salt/sugar/surfactant particles caused a reduction in GF at low RHs and minimized the effect of ionic surfactants on the DRH. At RHs above the DRH, the addition of anionic or nonionic surfactants caused a decrease in GF for both sea salt/glucose and sea salt/laminarin particles. The addition of cationic surfactants, however, did not have a dampening effect on water uptake of sea salt/sugar particles and even showed a GF increase of up to 3.7% at 90% RH. An increase in the complexity of the sugar dampens the water uptake for particles containing nonionic surfactants but increases the water uptake for cationic surfactants. The cloud activation potential for 100 nm particles analyzed in this study is higher for ionic surfactants and decreases with an increase in surfactant molecular size when particle interfacial tension is considered. The surfactant effect on the hygroscopic growth and cloud activation potential of the particles containing sea salt/sugar is dependent on the surfactant ionicity and molecular size, the particle size and interfacial tension, and the interactions between inorganic salt and organic species under different RH conditions.

Insight into the interaction between water and surfactant aerosol particles based on molecular dynamics simulations

The ubiquitous surfactant significantly influences the hygroscopic growth of atmospheric aerosol particles. However, knowledge on the morphology of surfactant particles after the adsorption of water is insufficient. In this study, the interaction between water and particles composed of surface active malonic acid (MA) or adipic acid (AA) are simulated based on the molecular dynamics method. The key point is the combined effect of temperature and water content on the structural properties of particles and the surface propensity of surfactants at the equilibrium state. Results show that demixed structure 1 with the adsorption of water clusters on acid grain, mixed structure and demixed structure 2 with acids coating on water droplet can be observed. With temperature increasing from 160 K to 330 K the surface propensity of MA and AA increases first and then weakens. Near the standard atmospheric temperature (280–330 K), the surface propensity of MA and AA increases with increasing water content and alkyl group, and its sensitivity to temperature and water content varies regularly. Moreover, all surfactants at the particle surface orient their hydrophobic groups toward the gas. These findings improve our insight into the surfactant partitioning and further assist in more accurate prediction of the particle hygroscopic growth.

Impact of water uptake and mixing state on submicron particle deposition in the human respiratory tract (HRT) based on explicit hygroscopicity measurements at HRT-like conditions

Abstract. Particle hygroscopicity plays a key role in determining the particle deposition in the human respiratory tract (HRT). In this study, the effects of hygroscopicity and mixing state on regional and total deposition doses on the basis of the particle number concentration for children, adults, and the elderly were quantified using the Multiple-Path Particle Dosimetry model, based on the size-resolved particle hygroscopicity measurements at HRT-like conditions (relative humidity = 98 %) performed in the North China Plain. The measured particle population with an external mixing state was dominated by hygroscopic particles (number fraction = (91.5 ± 5.7) %, mean ± standard deviation (SD); the same below). Particle hygroscopic growth in the HRT led to a reduction by around 24 % in the total doses of submicron particles for all age groups. Such a reduction was mainly caused by the growth of hygroscopic particles and was more pronounced in the pulmonary and tracheobronchial regions. Regardless of hygroscopicity, the elderly group of people had the highest total dose among three age groups, while children received the maximum total deposition rate. With 270 nm in diameter as the boundary, the total deposition doses of particles smaller than this diameter were overestimated, and those of larger particles were underestimated, assuming no particle hygroscopic growth in the HRT. From the perspective of the daily variation, the deposition rates of hygroscopic particles with an average of (2.88 ± 0.81) × 109 particles h−1 during the daytime were larger than those at night ((2.32 ± 0.24) × 109 particles h−1). On the contrary, hydrophobic particles interpreted as freshly emitted soot and primary organic aerosols exhibited higher deposition rates at nighttime ((3.39 ± 1.34) × 108 particles h−1) than those in the day ((2.58 ± 0.76) × 108 particles h−1). The traffic emissions during the rush hours enhanced the deposition rate of hydrophobic particles. This work provides a more explicit assessment of the impact of hygroscopicity and mixing state on the deposition pattern of submicron particles in the HRT.

Deposition potential of 0.003–10 µm ambient particles in the humidified human respiratory tract: Contribution of new particle formation events in Beijing

Ultrafine particles (UFPs) usually explosive growth during new particle formation (NPF) events. However, the risk of exposure to UFPs on NPF days has been ignored due to the prevalence of mass-based air quality standards. In this study, the daily deposited doses, i.e., the daily deposited particle number dose (DPNd), mass dose (DPMd), and surface area dose (DPSd), of ambient particles in the human respiratory tract in Beijing were evaluated based on the particle number size distribution (3 nm-10 µm) from June 2018 to May 2019 utilizing a Multiple-Path Particle Dosimetry Model (MPPD) after the hygroscopic growth of particles in the respiratory tract had been accounted for. Our observations showed a high frequency (72.6%) of NPF on excellent air quality days, with daily mean PM2.5 concentrations less than 35 μg m−3. The daily DPNd on excellent air quality days was comparable with that on polluted days, although the DPMd on excellent air quality days was as low as 15.6% of that on polluted days. The DPNd on NPF days was ~1.3 times that on non-NPF days. The DPNd in respiratory tract regions decreased in the order: tracheobronchial (TB) > pulmonary (PUL) > extrathoracic (ET) on NPF days, while it was PUL > TB > ET on non-NPF days. The number of deposited nucleation mode particles, which were deposited mainly in the TB region (45%), was 2 times higher on NPF days than that on non-NPF days. Our results demonstrated that the deposition potential due to UFPs in terms of particle number concentrations is high in Beijing regardless of the aerosol mass concentration. More toxicological studies related to UFPs on NPF days, especially those targeting tracheobronchial and pulmonary impairment, are required in the future.

Measurement report: Hygroscopic growth of ambient fine particles measured at five sites in China

Abstract. The aerosol hygroscopic growth describes the interaction between aerosols and water vapor, which varies largely, depending on the chemical composition, types, and emissions of gas precursors under diverse environments. In this study, we analyzed size-resolved hygroscopic growth measured at five field sites of China by a hygroscopic tandem differential mobility analyzer (H-TDMA). Results show that the probability density function of hygroscopic growth factor (GF-PDF) at the megacity sites of Guangzhou (GZ), Shanghai (SH), and Beijing (BG) was generally with bimodal hydrophobic and hydrophilic modes, while a unimodal hydrophilic mode was dominated at the suburb sites of Xinzhou (XZ) and Xingtai (XT) throughout the measured particle size of 40–200 nm. As a result, the more hygroscopic (MH) mode accounts for a number fraction of &gt;80 % at the suburb sites, compared to only 20 %–40 % for 40 nm particles at the megacity sites. Further analysis shows that the GF value increases with the aggravated PM2.5 pollution at the sites (BG, XZ, and XT) in northern China, but that is not the case for GZ and SH, which are located in the southern regions. The distinct dependence of GF on the variations in PM2.5 concentrations among the sites suggests the spatial variability in particle composition with the evolution of pollution events in different regions of China. Moreover, different particle hygroscopic behaviors during new particle formation (NPF) events were observed at the five sites, reflecting the distinct mechanisms of NPF in diverse atmospheric environments. By including results from more sites, we find that the aerosol particles observed at those suburb sites are basically more hygroscopic than those in megacities. However, a large variability in the hygroscopic parameter κ at a given particle size among different sites is also observed, suggesting a complex impact from local sources and atmospheric processes. The measured dataset is helpful for improving the understanding of the formation of fine particles and the regional environmental and climate change.

Physical-Optical Properties of Marine Aerosols over the South China Sea: Shipboard Measurements and MERRA-2 Reanalysis

Aerosols play an important role in the Earth–atmosphere system. Their impacts on the weather and climate are highly dependent on spatiotemporal distributions as well as physical-optical properties. Physical-optical properties of the aerosols over the Asian continent have been widely investigated, but there are relatively few observations in maritime locations, especially the South China Sea (SCS). Here, with the combination of in situ ship-based observations from June and July 2019 as well as long-term MERRA-2 reanalysis datasets from January 2012 to December 2021, the physical and optical properties of marine aerosols in the SCS are explored. The impacts of meteorological factors, particularly frontal systems, on the aerosol properties are further analyzed based on detailed observations. The observed results show that aerosols are vertically concentrated below 3 km and the extinction coefficient reaches the maximum value of 0.055 km−1 near 480 m. Moreover, the particles are composed of an accumulation and a coarse particle mode, and they conform to the lognormal distribution. The synoptic-scale case study demonstrates that both the cold front and stationary front lead to an increase in aerosol optical thickness (AOD), which is due to the enhanced wind speed and the hygroscopic growth of fine particles, respectively. The long-term analysis indicates that AOD decreases from northwest to southeast with the increasing distance away from the continent, and it reflects higher values in spring and winter than in summer and autumn. Sulfate and sea salt dominate AOD in this region when compared with other components. The overall AOD shows a significant negative trend of −0.0027 year−1. This work will help us further understand the physical and optical properties of marine aerosols over the SCS and then contribute to quantifying the aerosol radiative forcing in the future.

Indoor air particles in research vessel from Shanghai to Antarctic: Characteristics, influencing factors, and potential controlling pathway

Despite millions of seafarers and passengers staying on ships each year, few studies have been conducted on the indoor air quality inside ship hulls. In this study, we investigated the levels and size distribution of indoor particulate matter during two cruises of the research vessel “Xuelong” from Shanghai to Antarctica. The results showed that the particle size less than 2.5 µm (PM2.5), and particle size less than 10 µm (PM10) concentrations in different rooms of the ship widely varied. We observed high particulate matter (PM) levels in some of the rooms. The mass concentration distribution was dominated by 1–4 µm particles, which may have been caused by the hygroscopic growth of fine particles. The dominant factors influencing PM concentrations were indoor temperature, relative humidity, and human activity. We quantified contributions of these factors to the levels of indoor particles using a generalized additive model. In clean rooms, the levels of indoor particles were controlled by temperature and relative humidity, whereas in polluted rooms, the levels of indoor particles were mainly influenced by temperature and human activity, which implied that controlling temperature and human activity would efficiently reduce the levels of indoor particles.

Experimental estimates of hygroscopic growth of particulate fission product species (mixed CsI–CsOH) with implications in reactor accident safety research

Studies on severe nuclear reactor accidents consider CsI and CsOH as the two predominant forms of cesium expected to be released following a reactor accident; 137Cs, 134Cs and 131I being their dominant radioactive forms. Recent studies have measured the hygroscopic growth factors (HGF) and activation fractions for laboratory generated CsI and CsOH particles in sub-saturation and super-saturation relative humidity environments. This work measures and compares the HGF of mixed CsI–CsOH particles with those of individual components. The experiments have been performed with hygroscopic tandem differential mobility analyser for varying mass ratios (w/w) of CsI: CsOH and the results have been compared with the theoretical estimates made using Brechtel and Kredneweis (2000) theory in conjugation of ZSR (Zdanovskii–Stokes–Robinson) mixing rule. The study shows different behavioural pattern of hygroscopic growth of mixed particles in comparison to individual components. A clear transitional change in the growth factor patterns was observed for the ratio below 1:1. Additionally, the experiments to study the effect of different dry diameters (50, 100, 150 and 200 nm) for 1:1 ratio revealed that hygroscopic growth was independent of initial dry diameter. Effect of dehydration for 3 mixing ratios viz., 1:02, 1:1 and 1:10 showed continuous pattern indicating the dominance of CsOH. Terminal settling velocities for the mixed and individual particles are compared for highlighting the probable impact on surface deposition flux calculations. The aerosol hygroscopic growth of mixed CsI–CsOH particles has direct implications in improving source term estimates for a severe reactor accident safety analysis.

Vertical profile of aerosol number size distribution during a haze pollution episode in Hefei, China

The vertical distribution of aerosols has important implications on haze formation as development, which is manifested to some extent by the planetary boundary layer (PBL)–aerosol interactions. Information on the number concentration and size of particles is essential to understand these processes, but studies on vertical profiles of particle number-size distribution are limited. Herein, an unmanned aerial vehicle (UAV) equipped with a custom-built optical particle counter (0.4–10 μm) was used to investigate the vertical profiles of particle number-size distribution in Hefei (China) during January 20–30, 2021. Combining ground-based scanning mobility particle sizer and meteorological data, the pollution accumulation and diffusion mechanisms were analyzed in depth. Results showed that as the pollution episode developed, the vertical distribution of the particle number concentration changed from a flat profile to a sharp vertical gradient. Under polluted conditions, a three-layer structure was clearly evident: uniform distribution in a mixed layer near the ground, a sharply reduced transition layer, and a low number concentration layer in the free atmosphere. Analysis revealed that fundamental to this conversion is that aerosols are highly affected by the PBL dynamics. Concurrent on-UAV and ground-based observations revealed that the ratio of particle numbers in the accumulation mode to that in the Aitken mode was 0.92 ± 0.05 in polluted days, which was almost three times that of clean days. This difference in the ratio of large to small particles suggests that hygroscopic growth of aerosol particles under high humidity conditions played an important role in haze development. Moreover, the sharp vertical gradient of the particle number concentration in the transition layer was identified as an important parameter for characterizing PBL height. The findings in this study highlight the importance of PBL dynamics on the under-studied vertical profiles of particle number-size distribution, especially during heavy pollution episodes.

Quantifying the impacts of PM2.5 constituents and relative humidity on visibility impairment in a suburban area of eastern Asia using long-term in-situ measurements

The deterioration of visibility due to air pollutants and relative humidity has been a serious environmental problem in eastern Asia. In most previous studies, chemical compositions of atmospheric particles were provided using filter-based offline analyses, which were unable to provide long-term and in-situ measurements that resolve sufficient temporal variations of air pollution and meteorology, hindering the resolution of the relationship between air quality and visibility. Here, we present a year-long continuously measured data from a comprehensive suite of online instruments to investigate diurnal and seasonal impacts of the aerosol chemical compositions in PM2.5 on visibility seasonally and diurnally. The measured dry aerosol extinction at λ = 550 nm reached a closure with that predicted by aerosol compositions within 12%. However, the hygroscopic growth of particles under ambient RH could enhance the aerosol extinction by a factor of 2–6, matching the perceptive visibility of the public. Particulate ammonium nitrate was most sensitive to reducing visibility, while ammonium sulfate contributed the most to the light extinction. In spring and winter, the monsoon and stagnant air masses reduced the visibility and increased PM2.5 (>35 μg m−3). The moisture was found to substantially enhance the light extinction under RH = 60–90%, reducing visibility by approximately 15 km, largely attributed to hygroscopic inorganic salts. This study serves as a metric to highlight the need to consider the influence of RH, and aqueous reactions in producing secondary inorganic aerosols on atmospheric visibility, underpinning the more accurate mitigation strategies of air pollution.

Indirect Measurements of the Composition of Ultrafine Particles in the Arctic Late‐Winter

AbstractWe present indirect measurements of size‐resolved ultrafine particle composition conducted during the Ocean‐Atmosphere‐Sea Ice‐Snowpack (OASIS) Campaign in Utqiagvik, Alaska, during March 2009. This study focuses on measurements of size‐resolved particle hygroscopicity and volatility measured over two periods of the campaign. During a period that represents background conditions in this location, particle hygroscopic growth factors (HGF) at 90% relative humidity ranged from 1.45 to 1.51, which combined with volatility measurements suggest a mixture of ∼30% ammoniated sulfates and ∼70% oxidized organics. Two separate regional ultrafine particle growth events were also observed during this campaign. Event 1 coincided with elevated levels of H2SO4 and solar radiation. These particles were highly hygroscopic (HGF = 2.1 for 35 nm particles), but were almost fully volatilized at 160 °C. The air masses associated with both events originated over the Arctic Ocean. Event 1 was influenced by the upper marine boundary layer (200–350 m AGL), while Event 2 spent more time closer to the surface (50–150 m AGL) and over open ocean leads, suggesting marine influence in growth processes. Event 2 particles were slightly less hygroscopic (HGF = 1.94 for 35 nm and 1.67 for 15 nm particles), and similarly volatile. We hypothesize that particles formed during both events contained 60–70% hygroscopic salts by volume, with the balance for Event 1 being sulfates and oxidized organics for Event 2. These observations suggest that primary sea spray may be an important initiator of ultrafine particle formation events in the Arctic late‐winter, but a variety of processes may be responsible for condensational growth.

Effects of hygroscopic growth of ambient urban aerosol particles on their modelled regional and local deposition in healthy and COPD-compromised human respiratory system

Total, regional and local deposition fractions of urban-type aerosol particles with diameters of 50, 75, 110 and 145 nm were modelled and studied in their dry state and after their hygroscopic growth using a Stochastic Lung Model and a Computational Fluid and Particle Dynamics method. Healthy subjects and patients with severe chronic obstructive pulmonary disease (COPD) were considered. The hygroscopic growth factors (HGFs) adopted were determined experimentally and represent a real urban-type environment. The hygroscopic growth of particles resulted in decrease of the deposition fractions in all major parts of the healthy respiratory system and the extent of the deposited fractions was rising monotonically with particle size. In the extrathoracic (ET) region, the relative decrease was between 7% and 13%. In the lungs the deposition decreased by 11–16%. The decrease of deposition fraction due to hygroscopic growth was more accentuated in the conductive airways (up to 25%) and less pronounced towards the terminal airways. The spatial distribution of the deposited particles remained highly inhomogeneous with some areas containing thousands times more particles than the average number of particles per unit surface area. For COPD patients, the hygroscopic growth produced similar deposition alterations in the ET region than for healthy subjects. In the conductive airways, however, the particle growth caused a substantial relative decrease in the deposition fractions. In contrast, the relative depositions of hygroscopic particles increased in the acinar region.

The effect of aerosol on downward diffuse radiation during winter haze in Wuhan, China

The effect of aerosol on diffuse radiation (DR) are examined using ground-based observation and radiative transfer simulation at Wuhan during the winter haze periods of 2015 and 2016. The results show that the DR values change with the severity of the pollution, from 156.51 W/m2 under clean air conditions to 157.52 W/m2 during severe pollution periods, while the ratio of DR to global radiation increases from 57% to 73% accordingly. Both DR and the ratio of DR to global radiation are significantly correlated with aerosol optical depth (AOD), with determination coefficient being 0.67 and 0.92, respectively. In addition, the aerosol forward scattering increased along with clean air to serious pollution, showing a logarithmic growth relationship with the effective radius of the fine-mode particles. The aerosol diffuse radiative effect (ADRE) was introduced to quantify aerosol's effect on DR, which increased from 122.83 W/m2 under clean air condition to 152.84 W/m2 during common pollution period and 180.99 W/m2 during severe pollution period. The sensitivity test of ADRE to aerosol optical properties show that the increase of ADRE is dominated by increase in AOD, and also related to increase in asymmetry factor (ASY) due to hygroscopic growth of fine mode particles under pollution conditions. The above findings enhance our understanding of the mechanisms governing ADRE variation during haze periods and favor the accurate evaluation of both the diffuse radiative effect of aerosols on the climate.

Hygroscopicity of secondary marine organic aerosols: Mixtures of alkylammonium salts and inorganic components

Field studies have identified alkylammonium salts as important components of secondary marine organic aerosols. In this work, we study the hygroscopic behavior of laboratory-generated alkylammonium aerosol particles, including monomethylammonium chloride (MMACl), dimethylammonium chloride (DMACl), trimethylammonium chloride (TMACl), diethylammonium chloride (DEACl), and their mixtures with inorganic salts containing ammonium sulfate (NH4)2SO4, sodium chloride NaCl, calcium nitrate Ca(NO3)2 and sodium sulfate Na2SO4 at different dry mass ratios with a hygroscopicity tandem differential mobility analyzer (HTDMA). The hygroscopic growth of pure alkylammonium salt particles (except for DEACl) reveals gradual water uptake over the whole studied range of relative humidities (RHs). In general, the impact of the presence of alkylammonium chloride on the phase behavior and hygroscopic growth of mixtures depends on the chemical composition of particles and volume fraction of the alkylammonium chloride in the mixtures. For alkylammonium/(NH4)2SO4 mixed particles (except for TMACl/(NH4)2SO4), the hygroscopic growth shows a smooth growth tendency when the organic content is high, while the deliquescence transition is observed for alkylammonium salt/NaCl mixtures at all mass ratios. Regarding the different mixtures of alkylammonium/Ca(NO3)2 particles, continuous water uptake without phase transition is observed over the studied RH range, indicating that alkylammonium salts impose no effect on the liquid-like state of calcium nitrate. The alkylammonium/Na2SO4 mixtures show obvious particle shrinkage prior to the deliquescence point. A similar behavior is also observed for alkylammonium salt/NaCl mixtures. The observed diameter reduction can be attributed to the transformation of porous or irregularly shaped solid particles into more compact near-spherical particles. In the following, measured growth factors (GFs) are compared with values predicted with the Zdanovskii–Stokes–Robinson (ZSR) mixing rule and ideal solution model. The ZSR predictions for different alkylammonium/inorganic mixtures are similar to the measured GFs as long as the mixed particles are in a liquid-like state.

Hygroscopic growth of aerosol particles consisted of oxalic acid and its internal mixture with ammonium sulfate for the relative humidity ranging from 80% to 99.5%

The hygroscopicity of atmospheric aerosol particles plays an important role in their effects on the environment and the public health. Oxalic acid (OA) has been recognized as the dominant dicarboxylic acid in the urban and the remote aerosol particles, so a number of studies have investigated the hygroscopicity of aerosols consisted of pure OA and its mixture with inorganic salt. However, few experimental studies have focused on the hygroscopicity of nanoscale particles at high relative humidity (RH) below saturation of water vapor (i.e., RH = 90–100%) due to the limitation of traditional measuring instruments. In this work, the hygroscopic growth factor (GF) of the aerosol particles composed of pure OA and internally mixed OA-ammonium sulfate (AS) at RH = 80–99.5% were studied using a high humidity tandem differential mobility analyzer (HHTDMA). The experimental results were used to verify the applicability of models including the ideal solution model, the extended aerosol inorganics model (E-AIM) combining with the revised universal quasi-chemical functional group activity coefficients (UNIFAC-Peng) model, the Aerosol Inorganic–Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model and the Zdanovskii–Stokes–Robinson (ZSR) model. According to the experimental results, the effect of RH, the composition and the initial dry particle diameter (D0) on the hygroscopic growth factor (GF) and the effective hygroscopicity parameter (κ) of particles at RH = 80–99.5% were analyzed in details. It has been found that for pure OA particles with D0 = 80/100 nm, the prediction of the UNIFAC-Peng model and the AIOMFAC model becomes more accurate than the ideal solution model with the increasing of RH, while all models cannot describe the GF of smaller particles at RH = 80–99.5%. For mixed OA-AS aerosol particles, the chemical reaction is an important reason for the discrepancies between the HHTDMA results and the model prediction. For the pure OA aerosol particles at RH ≤ 96% and particles containing AS at RH ≤ 99.5%, the sensitivity of GF to D0 is positively and negatively correlated with RH and D0, respectively. However, for all aerosol types in this study, the sensitivity of GF to RH is positively correlated with both D0 and RH. In addition, the κ based on the measurement is clearly dependent on D0 (at RH = 95–99.5%), RH and the particle composition (at RH = 80–99.5%). The measured hygroscopicity of aerosol particles at high RH might be useful in addressing challenges in solving the discrepancies between the κ measured under subsaturated and supersaturated conditions.

Hygroscopic growth of simulated lung fluid aerosol particles under ambient environmental conditions.

The hygroscopicity of respiratory aerosol determines their particle size distribution and regulates solute concentrations to which entrained microorganisms are exposed. Here, we report the hygroscopicity of simulated lung fluid (SLF) particles. While the response of aqueous particles follow simple mixing rules based on composition, we observe phase hysteresis with increasing and decreasing relative humidity (RH) and clear uptake of water prior to deliquescence. These results indicate that RH history may control the state of respiratory aerosol in the environment and influence the viability of microorganisms.

Haze events at different levels in winters: A comprehensive study of meteorological factors, Aerosol characteristics and direct radiative forcing in megacities of north and central China

The changes in aerosol optical and microphysical properties, and sub-band shortwave direct radiative forcing (DARF) in Beijing and Wuhan were compared at different haze levels in winters. The occurrence of haze is found to be governed by the wind circulation and boundary layer in Beijing where the ground wind speed and the height of boundary layer decreased significantly with the development of haze. Compared with the boundary layer and wind, the relative humidity has a stronger impact on haze in Wuhan. Especially, hygroscopic growth of aerosol particles is observed in Wuhan. The increase of fine-mode non-absorbing particles is the main characteristic of aerosol change during haze periods. With the development of haze, the larger increase in DARF at the top of atmosphere is found in Beijing, while the change in DARF at the atmosphere is more obvious in Wuhan. Efficiency of the DARF shows that the change of DARF depends highly on the single scattering albedo in Beijing due to the obvious enhancement of particle scattering, while it depends much more on particle radius over Wuhan. The increase in particle size can also change DARF proportion of each sub-band in shortwave that the DARF proportion in ultraviolet and visible decreased. However, the DARF proportion in near-infrared increased during haze, as the light in shorter wavelength is more sensitive to the change of the fine particle radius.