Stratospheric air intrusions promote global-scale new particle formation.

New particle formation in the free troposphere is a major source of cloud condensation nuclei globally. The prevailing view is that in the free troposphere, new particles are formed predominantly in convective cloud outflows. We present another mechanism using global observations. We find that during stratospheric air intrusion events, the mixing of descending ozone-rich stratospheric air with more moist free tropospheric background results in elevated hydroxyl radical (OH) concentrations. Such mixing is most prevalent near the tropopause where the sulfur dioxide (SO2) mixing ratios are high. The combination of elevated SO2 and OH levels leads to enhanced sulfuric acid concentrations, promoting particle formation. Such new particle formation occurs frequently and over large geographic regions, representing an important particle source in the midlatitude free troposphere.

Development of a multi-stage fog droplet screening system based on the virtual impact principle.

Accurately measuring fog droplet spectra is essential for understanding fog's formation, dissipation, and composition, which makes a challenge to the performance of droplet sampling and measurement systems. Standard particles such as glass beads are widely used to characterize their performance. However, the disparities between glass beads and fog droplets, including refractivity, size distribution, and composition, may lead to calibration errors. In this context, we developed a three-stage fog droplet screening system based on the virtual impact principle. We determined the Stokes number and the diameter of the acceleration nozzle through theoretical analysis. Subsequently, we utilized the computational fluid dynamics software Fluent to explore the influence of key system parameters on screening efficiency, including the diameter of the collection nozzle (D1) and the distance between the acceleration nozzle and the collection nozzle (S). The simulation results indicated that the screening efficiency improved with S. The best performance was achieved when D1 = 1.35 D0 and S = 1.90 D0 (where D0 represents the diameter of the acceleration nozzle), resulting in an average screening efficiency of 75.4%. Finally, we conducted experiments to validate the effectiveness of the screening system. The screening efficiency of each outlet was estimated at 42.2%, 66.1%, 84.0%, and 95.3%, with differences of 2.0%, 3.3%, 4.1%, and 4.7% compared to the simulations. The average screening efficiency was 71.9%, with a deviation of 3.5% from the simulation. These findings demonstrated that the screening system could provide an alternative technical apparatus for characterizing droplet sampling and measurement systems.

Investigating the effect of volatility on the hygroscopicities of acetate nanoparticle aerosols by surface plasmon resonance microscopy.

Under high relative humidity (RH) conditions, the release of volatile components (such as acetate) has a significant impact on the aerosol hygroscopicity. In this work, one surface plasmon resonance microscopy (SPRM) measurement system was introduced to determine the hygroscopic growth factors (GFs) of three acetate aerosols separately or mixed with glucose at different RHs. For Ca(CH3COO)2 or Mg(CH3COO)2 aerosols, the hygroscopic growth trend of each time was lower than that of the previous time in three cyclic humidification from 70% RH to 90% RH, which may be due to the volatility of acetic acid leading to the formation of insoluble hydroxide (Ca(OH)2 or Mg(OH)2) under high RH conditions. Then the third calculated GF (using the Zdanovskii-Stokes-Robinson method) for Ca(CH3COO)2 or Mg(CH3COO)2 in bicomponent aerosols with 1:1 mass ratio were 3.20% or 5.33% lower than that of the first calculated GF at 90% RH. The calculated results also showed that the hygroscopicity change of bicomponent aerosol was negatively correlated with glucose content, especially when the mass ratio of Mg(CH3COO)2 to glucose was 1:2, the GF at 90% RH only decreased by 4.67% after three cyclic humidification. Inductively coupled plasma atomic emission spectrum (ICP-AES) based measurements also indicated that the changes of Mg2+concentration in bicomponent was lower than that of the single-component. The results of this study reveal thatduring the efflorescence transitions of atmospheric nanoparticles, the organic acids diffusion rate may be inhibited by the coating effect of neutral organic components, and the particles aging cycle will be prolonged.

Arctic warming by abundant fine sea salt aerosols from blowing snow.

The Arctic warms nearly four times faster than the global average, and aerosols play an increasingly important role in Arctic climate change. In the Arctic, sea salt is a major aerosol component in terms of mass concentration during winter and spring. However, the mechanisms of sea salt aerosol production remain unclear. Sea salt aerosols are typically thought to be relatively large in size but low in number concentration, implying that their influence on cloud condensation nuclei population and cloud properties is generally minor. Here we present observational evidence of abundant sea salt aerosol production from blowing snow in the central Arctic. Blowing snow was observed more than 20% of the time from November to April. The sublimation of blowing snow generates high concentrations of fine-mode sea salt aerosol (diameter below 300 nm), enhancing cloud condensation nuclei concentrations up to tenfold above background levels. Using a global chemical transport model, we estimate that from November to April north of 70° N, sea salt aerosol produced from blowing snow accounts for about 27.6% of the total particle number, and the sea salt aerosol increases the longwave emissivity of clouds, leading to a calculated surface warming of +2.30 W m-2 under cloudy sky conditions.

Characterization of the vertical evolution of urban nocturnal boundary layer by UAV measurements: Insights into relations to cloud radiative effect.

The complex structure of the nocturnal boundary layer (NBL) and its impact on air pollution remain poorly understood. In this study, we present in-situ nocturnal flight measurements onboard an unmanned aerial vehicle (UAV) during the wintertime of 2022 at an urban site in Hefei, China. Besides, co-located measurements of radiation intensity and total amount of cloud were conducted. The vertical distribution of temperature, particle number concentration, and relative humidity were obtained to study the structure of NBL and the key factors driving the evolution of the NBL. A multi-layer inversion boundary layer was observed during haze and fog episodes, which affects the vertical diffusion of particles near the surface and leads to a vertical gradient of particle number concentrations. The particle size distribution demonstrates a drastic vertical variation over different sections of the nocturnal boundary layer: homogeneously mixed in the SBL and the RL layer, sharply reduced in the IL. It is found that the temperature and particle number concentration differences between near-surface and at 500 m are highly related to variations of the radiation intensity and the amount of cloud. The decreased cloud cover enhances the surface cooling, creating a shallow NBL with multiple inversion layers, which reinforces the suppression of vertical diffusions and consequently promotes the accumulation of aerosols within the NBL. This reveals an important mechanism for the impact of NBL evolution modulated by cloud radiative effect on the formation of urban haze.

Investigating the hygroscopicities of calcium and magnesium salt particles aged with SO2 using surface plasmon resonance microscopy.

The hygroscopicities of calcium and magnesium salts strongly affect the environment and climate, but the aging products of these salts at high relative humidities (RHs) are still poorly understood. In this study, surface plasmon resonance microscopy (SPRM) was used to determine the hygroscopic growth factors (GFs) of Ca(NO3)2 and Mg(NO3)2 separately or mixed with galactose at different mass ratios at different RHs before and after aging. For all particles, the measured GFs showed no indication of deliquescence across the range of RHs tested, and overall hygroscopicity was clearly lower after than before aging. The Ca(NO3)2 and Mg(NO3)2 GFs at 90 % RH were 1.80 and 1.66, respectively, before aging and 1.33 and 1.42, respectively, after 4 h aging, meaning aging decreased the GFs by 26.11 % and 14.46 %, respectively. Aging decreased the hygroscopicity because insoluble or sparingly soluble substances (CaSO3, CaSO4, MgSO3) formed and strongly changed the overall hygroscopicity. For bicomponent aerosols with different mass ratios, the GFs (calculated using the Zdanovskii-Stokes-Robinson method) of the other components except galactose at 90 % RH after 1 h aging were all lower, respectively, than the measured GFs of pure Ca(NO3)2 and Mg(NO3)2 after aging for 1 h, especially with the mass ratio of 1:2, their GFs have decreased by 14.63 % and 7.50 %, respectively. Subsequently, Ion chromatograms indicated that the peak area ratio of SO42- to NO3- ratios were higher for the aged bicomponent particles than aged single-component particles, possibly because adding galactose improved the gas-liquid state stability during drying after the aging process and therefore promoted nitrate consumption and sulfate formation. The results indicated that organic components may play important roles in heterogeneous reactions between trace gases and multicomponent aerosols and should be considered in evaluating the impacts on submicron aerosol composition of high atmospheric SO2 concentrations at high humidities.

Retrieval of refractive index of ultrafine single particle using hygroscopic growth factor obtained by high sensitive surface plasmon resonance microscopy.

When exposed to different relative humidities (RHs), the optical properties of atmospheric aerosols will change because of changes in the aerosol particle size and complex refractive index (RI), which will affect haze formation and global climate change. The potential contributions of ultrafine particles to the atmospheric optical characteristics and to haze spreading cannot be ignored because of their high particle number concentrations and strong diffusibility; measurement of the optical properties of wet ultrafine particles is thus highly important for environmental assessment. Therefore, a surface plasmon resonance microscopy with azimuthal rotation illumination (SPRM-ARI) system is designed to determine the RIs of single particle aerosols with diameters of less than 100 nm in the hygroscopic growth process. Measurements are taken using mixed single particles with different mass ratios. The RIs of mixed single aerosols at different RHs are retrieved by measuring the scattering light intensity using the SPRM-ARI system and almost all the RIs of the bicomponent particles with different mass ratios decrease with increasing water content under high RH conditions. Finally, for each of the bicomponent particles, the maximum standard deviations for the retrieved RI values are only 2.06×10-3, 3.08×10-3 and 3.83×10-3, corresponding to the NaCl and NaNO3 bicomponent particles with a 3:1 mass ratio at 76.0% RH, the NaCl and glucose particles with a 1:3 mass ratio at 89.0% RH, and the NaCl and OA particles with a 1:1 mass ratio at 78.0% RH, respectively; these results indicate that the high-sensitivity SPRM-ARI system can measure the RI effectively and accurately.

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.

In Situ Quantitative Observation of Hygroscopic Growth of Single Nanoparticle Aerosol by Surface Plasmon Resonance Microscopy.

Aerosol particle hygroscopicity is an important factor in visibility reduction, cloud formation, radiation forcing, and the global climate. The high number concentration of nanoparticles (defined as particles with diameters below 100 nm) means that their hygroscopic growth abilities and potential contributions to the climate and environment are significant. Therefore, a rapid and accurate in situ analysis method for single nanoparticle hygroscopic growth in an atmospheric environment is important to characterize the effects of the particle's physical and chemical properties in this process. In this work, surface plasmon resonance microscopy with azimuthal rotation illumination (SPRM-ARI) is used to observe the hygroscopic growth and water content of single nanoparticles in situ. The hygroscopic growth results of a single-component nanoparticle are well matched with the extended aerosol inorganic model (E-AIM) results, and the proposed method remains reliable even when the relative humidity (RH) exceeds 90%. For a bicomponent nanoparticle (with NaCl as the primary content), the presence of a component without deliquescence phase transitions under increasing humidity conditions causes the measured data to differ from both the Zdanovskii-Stokes-Robinson (ZSR) model and E-AIM predictions in the low RH range. However, because of their complete liquefaction, the growth factor (GF) variation of the bicomponent nanoparticle is close to the model predictions in the high RH range. Finally, based on the positive correlation between particle volume and the gray intensity of SPRM-ARI, GF values can be obtained from the cube root of the gray intensity and the actual water content of single nanoparticles can then be derived.

Development of a static test apparatus for evaluating the performance of three PM2.5 separators commonly used in China.

PM2.5 separator directly affects the accuracy of PM2.5 sampling. The specification testing and evaluation for PM2.5 separator is particularly important, especially under China's wide variation of terrain and climate. In this study, first a static test apparatus based on polydisperse aerosol was established and calibrated to evaluate the performance of the PM2.5 separators. A uniform mixing chamber was developed to make particles mix completely. The aerosol concentration relative standard deviations of three test points at the same horizontal chamber position were less than 0.57%, and the particle size distribution obeyed logarithmic normal distribution with an R2 of 0.996. The flow rate deviation between the measurement and the set point flow rate agreed to within ±1.0% in the range of -40 to 50°C. Secondly, the separation, flow and loading characteristics of three cyclone separators (VSCC-A, SCC-A and SCC112) were evaluated using this system. The results showed that the 50% cutoff sizes (D50) of the three cyclones were 2.48, 2.47 and 2.44 µm when worked at the manufacturer's recommended flow rates, respectively. The geometric standard deviation (GSD) of the capture efficiency of VSCC-A was 1.23, showed a slightly sharper than SCC-A (GSD =1.27), while the SCC112 did not meet the relevant indicator (GSD = 1.2 ±â€¯0.1) with a GSD = 1.44. The flow rate and loading test had a great effect on D50, while the GSD remained almost the same as before. In addition, the maintenance frequency under different air pollution conditions of the cyclones was summarized according to the loading test.

On the Performance of an Aerosol Electrometer with Enhanced Detection Limit.

An aerosol electrometer with enhanced detection limit was developed for measuring the collected particles electrical current ranging from -50 pA to 50 pA with no range switching necessary. The detection limit was enhanced by suppressing the electric current measurement noise and improving the detection efficiency. A theoretical model for the aerosol electrometer has been established to investigate the noise effect factors and verified experimentally. The model showed that the noise was a function of ambient temperature, and it was affected by the characteristics of feedback resistor and operational amplifier simultaneously. The Faraday cup structure of the aerosol electrometer was optimized by adopting a newly designed cup-shaped metal filter which increased the surface area of the cup; thus the particle interception efficiency was improved. The aerosol electrometer performance-linearity, noise and the particle detection efficiency, were evaluated experimentally. When compared with TSI-3068B, a 99.4% ( R 2 ) statistical correlation was achieved. The results also showed that the root mean square noise and the peak-to-peak noise were 0.31 fA and 1.55 fA, respectively. The particle detection efficiency was greater than 99.3% when measuring particle diameter larger than 7.0 nm.

Design and Evaluation of an Aerosol Electrometer with Low Noise and a Wide Dynamic Range.

A low-noise aerosol electrometer with a wide dynamic range has been designed for measuring the total net charge on high concentration aerosol particles within the range of -500 pA to +500 pA. The performance of the aerosol electrometer was evaluated by a series of experiments to determine linearity, sensitivity and noise. The relative errors were controlled within 5.0%, 1.0% and 0.3% at the range of -40 pA to +40 pA, ±40 pA to ±100 pA, and ±100 pA to ±500 pA respectively. The stability of the designed aerosol electrometer was found to be highly sensitive to temperature variations, but under temperature control, the root mean square noise and the peak-to-peak noise were 1.040 fA and 5.2 fA respectively, which are very close to the calculated theoretical limit of the current noise. The excellent correlation and the advantage of a wide dynamic range have been demonstrated by comparing with the designed aerosol electrometer to a commercial aerosol electrometer. A 99.7% (R²) statistical correlation was obtained; meanwhile, the designed aerosol electrometer operated well even when an overrange phenomenon appeared in the commercial aerosol electrometer.

Comparative study of cylindrical and parallel-plate electrophoretic separations for the removal of ions and sub-23 nm particles.

Cylindrical and parallel-plate electrophoretic separations for the removal of ions and sub-23 nm particles were compared in this study. First, COMSOL Multiphysics® software was utilized to simulate the ion and particle trajectories inside both electrophoretic separations. The results show that ions and sub-23 nm particles are removed simultaneously and that all particles can pass through both electrophoretic separations smoothly at a trap voltage of 25 V. The experimental results show that ion losses become smaller with increasing ion flow rates, and ion losses of the cylindrical and parallel-plate electrophoretic separations range from 56.2 to 71.6% and from 43.8 to 59.6%, respectively, at ion flow rates ranging from 1-3 L/min. For the removal of ions and sub-23 nm particles, the collection efficiency of both electrophoretic separations can reach 100%, but the parallel-plate electrophoretic separation requires a lower trap voltage. The particle loss of the parallel-plate electrophoretic separation is under approximately 10%, which is lower than that of the cylindrical electrophoretic separation. In particular, for large particles (800-2500 nm), the particle losses inside the cylindrical electrophoretic separation are approximately two times higher than those inside the parallel-plate electrophoretic separation. The parallel-plate electrophoretic separation is beneficial for the removal of ions and sub-23 nm particles.

Identification of long-range transport pathways and potential sources of PM2.5 and PM10 in Beijing from 2014 to 2015.

Trajectory clustering, potential source contribution function (PSCF) and concentration-weighted trajectory (CWT) methods were applied to investigate the transport pathways and identify potential sources of PM2.5 and PM10 in different seasons from June 2014 to May 2015 in Beijing. The cluster analyses showed that Beijing was affected by trajectories from the south and southeast in summer and autumn. In winter and spring, Beijing was not only affected by the trajectories from the south and southeast, but was also affected by trajectories from the north and northwest. In addition, the analyses of the pressure profile of backward trajectories showed that backward trajectories, which have important influence on Beijing, were mainly distributed above 970hPa in summer and autumn and below 950hPa in spring and winter. This indicates that PM2.5 and PM10 were strongly affected by the near surface air masses in summer and autumn and by high altitude air masses in winter and spring. Results of PSCF and CWT analyses showed that the largest potential source areas were identified in spring, followed by winter and autumn, then summer. In addition, potential source regions of PM10 were similar to those of PM2.5. There were a clear seasonal and spatial variation of the potential source areas of Beijing and the airflow in the horizontal and vertical directions. Therefore, more effective regional emission reduction measures in Beijing's surrounding provinces should be implemented to reduce emissions of regional sources in different seasons.