Bimodal distribution of size-resolved particle effective density: Results from a short campaign in a rural environment over the North China Plain

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 differential mobility analyzer-centrifugal particle mass analyzer-condensation particle counter (DMA-CPMA-CPC) system in autumn 2019 as part of the Multiphase chemistry experiment in Fogs and Aerosols in the North China Plain (McFAN). With a newly 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 the total number of 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 (ρ3/4eff,main) increases from 1.18±0.10gcm-3 (50nm) to 1.37±0.12gcm-3 (300nm) due to a larger fraction of high-density components and a more significant restructuring effect at large particle sizes but decreases from 0.89±0.08gcm-3 (50nm) to 0.62±0.12gcm-3 (300nm) for the sub-density mode (ρ3/4eff,sub), which could be mainly ascribed to the agglomerate effect of BC. ρ3/4eff,main and ρ3/4eff,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 to the average effective density at 300nm (ρ3/4eff,tot,300nm). The best agreement between the two densities is achieved when assuming a BC effective density of 0.60gcm-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.