Mathematical derivation and physical interpretation of particle size-resolved activation ratio based on particle hygroscopicity distribution: Application on global characterization of CCN activity

Jiang, Xuejuan; Tao, Jiangchuan; Kuang, Ye; Hong, Juan; Ma, Nan

doi:10.1016/j.atmosenv.2020.118137

Cited by 5 publications

(5 citation statements)

References 42 publications

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“…As can be seen in Fig. 6a, N CCN_meas at 0.05 % SS was strongly underestimated by N CCN_Chem , especially at lower N CCN_meas (∼ 10 2 cm −3 ), which is similar to the results of studies that encountered high fractions of organics (Chang et al, 2010;Kawana et al, 2016). This deviation between N CCN_meas and N CCN_Chem may have resulted from the hypothesis of internal mixing state and the difference of particle hygroscopicity derived by particle chemical composition measurements and CCN activity.…”

Section: The Influence Of Diurnal Variation Of Ccn Activity On N Ccn Predictionsupporting

confidence: 80%

Secondary aerosol formation alters CCN activity in the North China Plain

Tao

Kuang

et al. 2021

Atmos. Chem. Phys.

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Abstract. 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), PM2.5 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.

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Section: The Influence Of Diurnal Variation Of Ccn Activity On N Ccn Predictionsupporting

confidence: 80%

Secondary aerosol formation alters CCN activity in the North China Plain

Tao

Kuang

et al. 2021

Atmos. Chem. Phys.

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“…Studies have shown that in the TP, the PNSD is characterized by a peak value less than 1,000 at approximately 200 nm and can be presented by one lognormal distribution (Shang et al., 2018; Tang et al., 2023). Moreover, studies have shown that the size‐resolved CCN activity at a particular SS can be parameterized using one or two sigmoidal functions (Jiang et al., 2021; Rose et al., 2010; Tao, Kuang, et al., 2020). To maintain simplicity while preserving generality, when analyzing the influence of the AAC transfer function on the measured size‐resolved CCN activity in the following, we assume that the preset PNSD is parameterized with a single lognormal distribution, and the size‐resolved CCN activity is represented by a single error function.…”

Section: Aac‐ccnc Systemmentioning

confidence: 99%

“…In addition, for σ values between 0.02 and 0.05, a linear correction scheme is proposed to ensure that the absolute deviation of the parametric scheme does not exceed 0.003. Jiang et al (2021) reviewed the measurements of sizeresolved CCN activity worldwide and reported that the measured σ is primarily no smaller than 0.1, suggesting that the correction of σ is not necessary in the majority of atmospheric observations.…”

Section: Journal Of Geophysical Research: Atmospheresmentioning

confidence: 99%

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A New Method for Size‐Resolved Aerosol CCN Activity Measurement at Low Supersaturation in Pristine Atmosphere

Tao,

Luo,

Meng

et al. 2024

JGR Atmospheres

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Understanding aerosol‐cloud interactions under pristine atmospheric conditions is crucial for meaningful global climate change predictions. However, ability of aerosol particles to act as cloud condensation nuclei (CCN) activity of aerosols in pristine atmosphere remains limited, mainly because of the difficulty of measuring it in pristine environments. Given the extremely low CCN number concentration under low supersaturations (SSs) and the complex impact of the kinetic limitation in CCN measurements, size‐resolved CCN activity measurements at low SSs cannot be achieved with traditional methods using differential mobility analyzers and a CCN counter (CCNC) because of the low sample efficiency and the impact of particles with multiple charges. To overcome this difficulty, we propose a new method for measuring size‐resolved CCN activity at low aerosol number concentrations. The new method is based on a combined system comprising an aerodynamic aerosol classifier (AAC) and a CCNC (AAC‐CCNC system). A control program was developed to achieve high‐resolution scans of the SS and particle size within a reasonable time frame. A data inversion scheme, including corrections for the transfer function and kinetic limitation, was developed to obtain accurate size‐resolved CCN activity. In July‐August 2022, the new method was used to measure the size‐resolved CCN activity on the Tibetan Plateau. This new method can advance the size‐resolved CCN measurements, thereby enhancing our understanding of aerosol‐cloud interactions in pristine atmosphere.

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“…For instance, while both CCN activity and the hygroscopic growth measurements are associated with aerosol hygroscopicity, intercomparison between CCNC and HTDMA measurements promoted investigations on aerosol hygroscopicity variations under different saturation conditions (Su et al, 2010;Juranyi et al, 2013;Lance et al, 2013;Kawana et al, 2016;Tao et al, 2020;Jiang et al, 2021). Although both SP2 and VTDMA techniques depend on the evaporation of non-refractory compositions, only the rBC remains in SP2 measurements, whereas the non-refractory composition evaporations depend on thermodenuder temperature in VTDMA measurements.…”

Section: Introductionmentioning

confidence: 99%

Markedly different impacts of primary emissions and secondary aerosol formations on aerosol mixing states revealed by simultaneous measurements of CCNC, V/HTDMA and SP2

Tao

Luo²,

Xu³

et al. 2023

Preprint

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Abstract. The aerosol mixing state is a crucial physical-chemical property that affects their optical properties and cloud condensation nuclei (CCN) activity. Multiple techniques are commonly employed to determine aerosol mixing states for various applications, and comparisons between these techniques provide insights of the variations in aerosol chemical and physical properties. These techniques include size-resolved CCN activity measurements using a system with CCN counter (CCNC) coupled with a differential mobility analyzer (DMA), a Humidified/Volatility Tandem differential mobility analyzer (H/V-TDMA) which measures aerosol hygroscopicity/volatility distributions, and a single particle soot photometer (SP2) which directly quantifies black carbon (BC) mixing states. This study provides a first time intercomparisons of aerosol mixing state parameters obtained through simultaneous measurements of a DMA-CCNC, a H/VTDMA and a DMA-SP2. The impact of primary aerosols emissions and secondary aerosol formations on the aerosol mixing states and intercomparison results were analyzed. The results showed that differences in mixing state parameters measured by different techniques varied greatly under different conditions. The V-TDMA and DMA-SP2 measurements showed that the non-volatile population identified by the V-TDMA was mainly contributed by BC-containing aerosols. The HTDMA and DMA-SP2 measurements indicated that a substantial proportion of nearly hydrophobic aerosols were not contributed from BC-containing aerosols, but likely originated from fossil fuel combustion and biomass burning emissions. Synthesized comparison results between DMA-CCNC, HTDMA and DMA-SP2 measurements revealed that some of the nearly hydrophobic BC-free particles were CCN-inactive under supersaturated conditions, likely from fossil combustion emissions, while others were CCN-active under supersaturated conditions linked to biomass burning emissions. Fossil fuel combustion-emitted BC-containing aerosols tended to be more externally mixed with other aerosol compositions compared to those emitted from biomass burning activities. These results highlight significant disparities in the mixing states as well as physiochemical properties between aerosol originated from fossil fuel combustion and biomass burning. The formation of secondary nitrate and organic aerosols exerted significant impacts on variations in aerosol mixing states, generally enhancing aerosol hygroscopicity and volatility, while reducing differences in mixing state parameters derived from different techniques, resulting in a reduction in aerosol heterogeneity. The variations in BC-free particle number fractions showed that secondary aerosols tended to form more quickly on BC-free particles than on BC-containing particles. Further comparison of mixing state parameters revealed that the two resolved SOA factors in this study exhibited remarkably different physical properties, indicating that they were likely formed through different pathways. These findings suggest that intercomparisons among aerosol mixing states derived from different techniques can provide deeper insight into aerosol physical properties and how they are impacted by secondary aerosol formation, aiding the investigation of secondary aerosol formation pathways.

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Mathematical derivation and physical interpretation of particle size-resolved activation ratio based on particle hygroscopicity distribution: Application on global characterization of CCN activity

Cited by 5 publications

References 42 publications

Secondary aerosol formation alters CCN activity in the North China Plain

Secondary aerosol formation alters CCN activity in the North China Plain

A New Method for Size‐Resolved Aerosol CCN Activity Measurement at Low Supersaturation in Pristine Atmosphere

Markedly different impacts of primary emissions and secondary aerosol formations on aerosol mixing states revealed by simultaneous measurements of CCNC, V/HTDMA and SP2

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