Abstract

Abstract. Mixing states of soot-containing aerosol particles constitute important information for the simulation of climatic effects of black carbon in the atmosphere. To elucidate the mixing states and morphological features of soot-containing particles over remote oceans, we conducted on-board observations over the southern Indian Ocean and the Southern Ocean during the TR/V Umitaka-maru UM-08-09 cruise, which started from Benoa, Indonesia, on 1 December 2008 via Cape Town, South Africa, and which terminated in Fremantle, Australia, on 6 February 2009. The light absorption coefficients of size-segregated particles (< 0.5 and < 1.0 µm diameter) and aerosol number concentrations (0.1–0.5 µm diameter) were measured to assist direct aerosol sampling. Size-segregated aerosol particles were collected for chemical analysis using ion chromatography. For transmission electron microscopy (TEM) analyses using water-dialysis methods, dried submicrometer aerosol particles were collected using a cascade impactor. We analyzed 13 TEM samples. Results of water-dialysis analysis demonstrate that most particles were water-soluble. However, for all TEM samples, particles were rarely found (2.1 % of particles on a TEM sample at a maximum) containing insoluble residuals with the characteristic soot shape. For samples collected over the Indian and Southern oceans at latitudes less than 62∘ S, some (20–35 %) soot-containing particles were found as bare soot. For samples collected near the Antarctic coast (65–68∘ S, 38–68∘ E), all soot-containing particles were mixed with water-soluble materials. Furthermore, 56 % of soot-containing particles had a satellite structure formed by the impact of droplets such as sulfuric acid. Chemical analysis of submicrometer particles near the Antarctic coast revealed high concentrations of non-sea-salt (nss) SO42- and CH3SO3-, suggesting that aged soot-containing particles were transformed by soluble materials derived from dimethyl sulfide (DMS) oxidation. The obtained information of soot at various remote ocean areas is expected to be useful to understand long-range transport processes and to improve simulations of global soot concentration.

Highlights

  • Soot in the atmospheric aerosol is a by-product of fossil fuel combustion and open biomass burning

  • After transmission electron microscopy (TEM) samples for individual particle analysis using water dialysis were obtained, 13 samples were chosen for detailed analysis by sampling location and babs

  • Water-dialysis examination revealed that many particles in the 13 TEM samples contained water-soluble materials

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Summary

Introduction

Soot in the atmospheric aerosol is a by-product of fossil fuel (diesel and coal) combustion and open biomass burning It is a carbonaceous material with a deep black appearance to visible solar radiation in the atmosphere (Ramanathan and Carmichael, 2008). Water dialysis to detect insoluble soot selectively under a microscope is a powerful technique to investigate the mixing states of well-aged soot-containing particles (Okada, 1983; Ueda et al, 2011a, b) This method comprises morphological observation and comparison before and after water dialysis of aerosols. Elucidating the mixing states of soot-containing particles for low-BC concentration areas will be helpful for elucidating the long-range transport of soot in remote areas, and eventually for understanding the global diffusion processes of BC through the atmosphere. This study was conducted mainly to ascertain the mixing states of soot-containing particles with water-soluble materials and to assess their relationship to the morphological features of the mixing materials

Aerosol number–size distribution
Size-segregated light absorption coefficient
Data screening of aerosol number concentration and light absorption
Ionic constituents of size-segregated aerosol particles
Samples of morphological particle analyses using an electron microscope
Air mass backward trajectories
Temporal variation of aerosol parameters
Samples
Morphological features and mixing states
Features of soot-containing particles
Conclusions
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