Highlights:1. Morphological transformation occurs via two key complementary and sequential processes, i.e., void filling in the particle and its diameter growth 15 2. A framework was developed for quantifying the state of morphological transformation of soot, i.e., the utilization of material for filling and growth during the condensation processes 3. A method was developed for (i) quantifying the fraction of internal voids and open voids in the soot agglomerate, (ii) deriving the volume equivalent diameter (inclusive of internal voids), and (iii) estimating the in-situ dynamic shape factor 20
Abstract.The morphological transformation of soot particles via condensation of low-volatility materials constitutes a dominant atmospheric process with serious implications for the optical and hygroscopic properties, and atmospheric lifetime of the soot. We consider the morphological transformation of soot agglomerates under the influence of condensation of vapors of sulfuric acid, and/or limonene ozonolysis products. This influence was systematically investigated using a Differential 25Mobility Analyzer-Aerosol Particle Mass Analyzer (DMA-APM) and the Tandem DMA techniques integrated with a laminar flow-tube system. We discovered that the morphology transformation of soot results (in general) from a two-step process, i.e., (i) filling of void space within the agglomerate; (ii) growth of the particle diameter. Initially, the transformation was dominated by the filling process followed by growth, which led to the accumulation of sufficient material that exerted surface forces, which eventually facilitating further filling. The filling of void space was constrained by the initial 30 morphology of the fresh soot as well as the nature and the amount of condensed material. This process continued in several sequential steps until all void space within the soot agglomerate was filled. And then "Growth" of a spherical particle continued as long as vapors condensed on it. We developed a framework for quantifying the microphysical transformation of Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-769 Manuscript under review for journal Atmos. Chem. Phys. Discussion started: 27 October 2017 c Author(s) 2017. CC BY 4.0 License. 2 soot upon the condensation of various materials. This framework used experimental data and the hypothesis of 'ideal sphere growth' and void filling to quantify the distribution of condensed materials in the complementary filling and growth processes. Using this framework, we quantified the percentage of material consumed by these processes at each step of the transformation. We also used the framework to estimate the fraction of internal voids and open voids. This information was then used to derive the volume equivalent diameter of the soot agglomerate containing internal voids and to calculate the in-5 situ dynamic shape factor. The dynamic shape factor estimated based on the traditional assumption (of no internal voids) differed significantly from the value obtained in this study. Internal vo...