Abstract

Effective density is one of the most important physical properties of atmospheric particles. It is closely linked to particle chemical composition and morphology, and could provide special information on particle emissions and aging processes. In this study, size-resolved particle effective density was measured with a combined DMA-CPMA-CPC system in Multiphase chemistry experiment in Fogs and Aerosols in the North China Plain (McFAN) in autumn 2019. With a new developed flexible Gaussian fit algorithm, frequent (77–87 %) bimodal distribution of particle effective density is identified, with a low-density mode (named sub-density mode) accounting for 22–27 % of total observed particles. The prevalence of the sub-density mode is closely related to fresh black carbon (BC) emissions. The geometric mean for the main-density mode (eff,main) increases from 1.18 g cm−3 (50 nm) to 1.37 g cm−3 (300 nm) due to larger fraction of high-density components and more significant restructuring effect at large particle sizes, but decreases from 0.89 g cm−3 (50 nm) to 0.62 g cm−3 (300 nm) for the sub-density mode (eff,sub) ascribed to the agglomerate effect. eff,main and eff,sub show similar diurnal cycles with peaks in the early afternoon, mainly attributed to the increasing mass fraction of high material density components associated with secondary aerosol production, especially of secondary inorganic aerosol (SIA). To investigate the impact of chemical composition, bulk particle effective density was calculated based on measured chemical composition (ρeff,ACSM) and compared with the average effective density at 300 nm (eff,tot,300 nm). The best agreement between the two densities is achieved when assuming a BC effective density of 0.60 g cm−3. The particle effective density is highly dependent on SIA and BC mass fractions. The influence of BC on the effective density is even stronger than SIA, implying the importance and necessity of including BC in the estimate of effective density for ambient particles.

Highlights

  • It is generally observed within the range of 1.06–1.81 g cm−3 in the ambient atmosphere (Cha and Olofsson, 2018; Geller et al, 2006; Hu et al, 2012; Levy et al, 2014; Lin et al, 2018; Rissler et al, 2014; Zamora et al, 2019), and these high values are attributed to the dominant of ammonium sulfate ((NH4)2SO4), ammonium nitrate (NH4NO3), and metals

  • Based on the flexible Gaussian fit, a considerable amount (77 %–87 %) of bimodal distribution condition occurred for all size particles

  • The results suggest insignificant influence associated with the variation of organic aerosol (OA) density, and the selection of OA density of 1.30 g cm−3 is appropriate for the effective density calculation of ambient particles

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Summary

Introduction

Atmospheric aerosol has a significant impact on air quality, climate change and public health (Dockery and Pope, 1994; IPCC, 2007; Laden et al, 2000; Su et al, 2020) This is determined by a combination of various particle physical and chemical properties. As one of important physical properties of aerosol particles, is intimately associated with optical, chemical and dynamic properties of particles (Ditas et al, 2018; Nosko and Olofsson, 2017; Park et al, 2003) It serves as a link between particle mass and mobility size (McMurry et al, 2002; Schmid et al, 2007) and is usually used to infer particle morphology, chemical composition, and associated atmospheric processes such as emission and aging (Abegglen et al, 2015; Levy et al, 2013; Olfert et al, 2007, 2017; Park et al, 2003; Wang et al, 2018; Wu et al, 2019; Zhang et al, 2018). While the effective densities of inorganic components are well recognized, there exists large uncertainties in the effective densities of both BC and OA (Li et al, 2016; Malloy et al, 2009; Zhang et al, 2008), leading to significant variations in the effective densities of ambient bulk particles

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