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The high concentration of fine particles and gaseous pollutants makes polluted areas, such as the urban setting of North China Plain (NCP) of China, a different environment for new particle formation (NPF) compared to many clean regions. Such conditions also hold for other polluted environments in this region (for instance, the rural area of NCP), yet the underlying mechanisms for NPF remain less understood, owing to the limited observations of particles in the sub -3 nm range. Comprehensive measurements, particularly covering the particle number size distribution down to 1.3 nm, were conducted at a rural background site of Gucheng (GC) in the North China Plain (NCP) from 12 November to 24 December 2018. In total, five NPF events during the 39 effective days of measurements for the campaign were identified, with the mean particle nucleation rate (J1.3) and growth rate (GR 1.3–2.4) being 22.0 cm -3 s -1 and 3.9 nm h -1 , respectively. During these 5 d, NPF concurrently occurred at an urban site in Beijing. Sharing similar sources and transport paths of air masses arriving at our site to that of urban Beijing, we hypothesize that NPF events during these days in this region might be a regional phenomenon. The simultaneous occurrence of NPF in both places implies that H 2 SO 4 -amine nucleation, concluded for urban Beijing there, could probably be the dominating mechanism for NPF at our rural site. The higher concentration of sulfuric acid during many non-event days compared to that of event days indicates that the content of sulfuric acid may not necessarily lead to NPF events under current atmosphere. Only when the condensation sink or coagulation sink was significantly lowered, atmospheric NPF occurred, implying that condensation sinks (CSs) and coagulation sinks (CoagSs) are the dominating factors controlling the occurrence of NPF for the present rural environment of the NCP, which is quite similar to the feature seen in urban Beijing. [ABSTRACT FROM AUTHOR]

Secondary aerosols (SAs, including secondary organic and inorganic aerosols, SOAs and SIAs) are predominant components of aerosol particles in the North China Plain (NCP), and their formation has significant impacts on the evolution of particle size distribution (PNSD) and hygroscopicity. Previous studies have shown that distinct SA formation mechanisms can dominate under different relative humidity (RH). This would lead to different influences of SA formation on the aerosol hygroscopicity and PNSD under different RH conditions. Based on the measurements of size-resolved particle activation ratio (SPAR), hygroscopicity distribution (GF-PDF), PM 2.5 chemical composition, PNSD, meteorology and gaseous pollutants in a recent field campaign, McFAN (Multiphase chemistry experiment in Fogs and Aerosols in the North China Plain), conducted during the autumn–winter transition period in 2018 at a polluted rural site in the NCP, the influences of SA formation on cloud condensation nuclei (CCN) activity and CCN number concentration (NCCN) calculation under different RH conditions were studied. Results suggest that during daytime, SA formation could lead to a significant increase in NCCN and a strong diurnal variation in SPAR at supersaturations lower than 0.07 %. During periods with daytime minimum RH exceeding 50 % (high RH conditions), SA formation significantly contributed to the particle mass and size changes in a broad size range of 150 to 1000 nm, leading to NCCN (0.05 %) increases within the size range of 200 to 500 nm and mass concentration growth mainly for particles larger than 300 nm. During periods with daytime minimum RH below 30 % (low RH conditions), SA formation mainly contributed to the particle mass and size and NCCN changes for particles smaller than 300 nm. As a result, under the same amount of mass increase induced by SA formation, the increase of NCCN (0.05 %) was stronger under low RH conditions and weaker under high RH conditions. Moreover, the diurnal variations of the SPAR parameter (inferred from CCN measurements) due to SA formation varied with RH conditions, which was one of the largest uncertainties within NCCN predictions. After considering the SPAR parameter (estimated through the number fraction of hygroscopic particles or mass fraction of SA), the relative deviation of NCCN (0.05 %) predictions was reduced to within 30 %. This study highlights the impact of SA formation on CCN activity and NCCN calculation and provides guidance for future improvements of CCN predictions in chemical-transport models and climate models. [ABSTRACT FROM AUTHOR]

Aerosol surface area concentration ( S A ) is crucial for studying atmospheric chemical reactions happened in aerosol water or on aerosol surface. However, there is no commercial instrument that can provide direct measurements of ambient S A . In this paper, we propose a method to calculate ambient S A based only on measurements of a three-wavelength humidified nephelometer system, which measures aerosol optical properties at three wavelengths under dry state and different relative humidity (RH) conditions. Two critical steps are required in this method: (1) Calculating surface area concentration of ambient aerosols in dry state, S A (dry) , using a trained random forest machine learning model based only on optical properties measured by the "dry" nephelometer. The proposed machine learning method is evaluated with particle number size distributions (PNSD) datasets from eight field campaigns conducted on the North China Plain during different seasons. The square of correlation coefficients between predicted and calculated S A (dry) for PNSD is about 0.99, the average ratio between predicted and calculated S A (dry) is 1.01 and 70% of data points has a relative difference less than 10%. (2) Calculating the surface area growth factor f S (RH) of ambient aerosol particles due to water uptake using the proposed f S (RH) parameterization scheme f S (RH) = (1 + κ S R H 100 − R H) 2 3 , and the hygroscopicity parameter κ S can be calculated using measured aerosol light scattering enhancement factor and Å ngstr o ¨ m exponent. The ambient S A values during two field campaigns which are conducted on the North China Plain (Wangdu campaign and Gucheng campaign, in summer and winter respectively) are calculated using the proposed method. The ambient S A ranges from 42 to 1871 μ m 2 / c m 3 with an average of 319 μ m 2 / c m 3 during Wangdu campaign, and ranges from 19 to 4156 μ m 2 / c m 3 with an average of 788 μ m 2 / c m 3 during Gucheng campaign. Drastic daily variations of ambient S A are observed during these two campaigns. The results demonstrate that aerosol hygroscopic growth impacts significantly on variations in ambient S A especially under high RH conditions. The f S (RH) ranges from near 1 to 4 with an average of 1.4 during Wangdu campaign, and ranges from near 1 to 2.7 with an average of 1.3 during Gucheng campaign. The results indicate that the larger RH, the more sensitive f S (RH) becomes to variations in κ S which highlights that real-time measurements of aerosol hygroscopicity are required for accurate calculations of ambient S A . The advantage of the proposed method is that the ambient S A can be obtained solely based on measurements of a three-wavelength humidified nephelometer system, facilitating real-time measurements of ambient S A and promoting studies in aerosol heterogeneous reactions. • Humidified nephelometer system performs great in predicting aerosol surface area. • Proposed method can be used in different regions. • Aerosol hygroscopic growth impacts significantly on aerosol surface area. [ABSTRACT FROM AUTHOR]

Abstract The light scattering enhancement factor f (RH), defined as the ratio of the light scattering coefficient (σ S P ) observed under an elevated relative humidity (RH) conditions to that under dry conditions, is a crucial parameter for estimating aerosol direct radiative effects and atmospheric visibility. In this paper, a new f (RH) parameterization scheme considering both the influence of aerosol chemical compositions and that of particle number size distribution (PNSD) is proposed based on in situ measurements in the North China Plain. The development of this parameterization scheme includes three steps. First, aerosol hygroscopicity parameter κ is parameterized with aerosol chemical compositions. Then, the ratio between f (RH) fitted parameter κ s c a (f (R H) = 1 + κ s c a R H 100 − R H ) and κ is introduced to correlate f (RH) with κ. The ratio, influenced mostly by PNSD, is described as a function of scattering Ångström exponent (SAE) because the SAE can represent the predominant size of aerosol particles to some extent. Finally, f (RH) cycle is parameterized with κ s c a . Validation results show that a good consistency between the parameterized and measured f (RH = 80%) is achieved and the correlation coefficient is 0.80. This parameterization scheme between aerosol chemistry and f (RH) can be used in chemical transport models for reducing uncertainties in estimations of direct aerosol radiative forcing and air quality assessments. Highlights • A relationship between the f (RH) fitted parameter (κ sca) and the aerosol hygroscopicity parameter (κ f(RH)) is found. • The ratio of κ sca and κ f(RH) increases linearly with the increase of the scattering Ångström exponent. • A new parameterization of f (RH) considering the aerosol chemical compositions is developed. [ABSTRACT FROM AUTHOR]

Size-resolved particle activation ratio (SPAR), the size-dependent ability of aerosol particles to form cloud condensation nuclei (CCN), is generally parameterized by a formula with sigmoidal shape with three key parameters. However, our understanding about the intrinsic relationship between the sigmoidal shape function and aerosol hygroscopicity distribution remains incomplete. In this study, the relationship between SPAR and particle hygroscopicity distribution is mathematically derived and relationships between key parameters for SPAR and particle hygroscopicity distribution are manifested, making it clear for the physical understanding of key CCN spectral characteristics. On the basis of the mathematically derived SPAR parameterization, a simplified method to calculate SPAR parameters (including maximum activation fraction (MAF), critical diameter and its heterogeneity of CCN-active particles) based on hygroscopicity distribution data is proposed. This simplified method is applied to Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) field measurement datasets around the world for the meta-analysis of regional and seasonal characteristics of CCN activity. It was found that, for CCN-active particles in polluted regions, the MAF can reach lower values, and the variations of both hygroscopicity and its heterogeneity can be larger, compared with those in clean regions. In summer, the MAF and the hygroscopicity of CCN can reach higher values than those in winter. In addition, the variations of SPAR parameters among different campaigns are large and thus measurements of CCN Counter or HTDMA are needed to specify the SPAR parameters at a specific site during a specific period. The bulk CCN activity at different SSs are also calculated based on the calculated SPAR by considering the measured particle number size distribution. The mathematical derivation and physical interpretation of SPAR parameterization in this study can further the understanding of CCN activity based on particle hygroscopicity distribution. The proposed simplified method to calculate SPAR parameters based on HTDMA measurements allows meta-analysis of SPAR parameters and helps expand the CCN activity datasets around the world. • Relationship between Size-resolved particle activation ratio and hygroscopicity distribution is mathematically derived. • A simplified method to calculate SPAR parameters based on hygroscopicity distribution data is proposed. • Meta-analysis of CCN activity is conducted based on HTDMA field measurement datasets in references. [ABSTRACT FROM AUTHOR]

Particle microphysical and chemical properties, including particle number size distribution (PNSD) and chemical composition of both ambient PM 1 and PM 10 particles were measured in the North China Plain (NCP) during the Multiphase chemistry experiment in Fogs and Aerosols in the North China Plain (McFAN) campaign in November 2018. Focused on the differences of measured PNSD between PM 1 and PM 10 , the variations of aerosol microphysical and chemical properties in fog were analyzed and their corresponding influence on fog droplets evolution was evaluated. Two nighttime fog events were observed on the 12th and 13th November, respectively. During fog events, PNSDs of particles with diameter larger than ∼200 nm sampled from the PM 10 inlet were similar to those after fogs. But in particle size range larger than 200 nm, particles number concentration sampled from the PM 1 inlet were very few and much lower than those after fogs, indicating that some particles larger than 200 nm have grown into droplets with diameter larger than 1 μm and thus were not detected under the PM 1 inlet. No significant decrease in particle number concentration larger than ∼200 nm was detected under the PM 10 inlet after the dissipation of these fog events, suggesting that fog droplets were generally smaller than 10 μm and could be sampled by the PM 10 inlet. The additional particles sampled in PM 10 in fogs demonstrated a normal distribution, which indicates that they belonged to an individual particle group externally mixed with those sampled under the PM 1 impactor and could outgrow 1 μm either through hygroscopic growth or through activation. This can lead to uncertainties in droplet number concentration estimations within fog from microphysical and chemical properties measurements of the aerosol with assumption of fully internal mixture. We find that PM 1 hygroscopicity derived from particle chemical composition measurements was overestimated, which may result in significant bias in the estimated droplets number concentration in the North China Plain. These results and approaches in this study can improve the understanding of aerosol microphysical properties in fogs and the corresponding influence of aerosol particles on fog microphysics. [Display omitted] • Simultaneous measurements of PM1 and PM10 during fog events in the North China Plain. • Differences between PNSDs of PM1 and PM10 suggest additional particles in PM10 different from PM1. • Ignoring external mixing state of PM10 leads to an overestimated droplet number concentration. [ABSTRACT FROM AUTHOR]