Biomass burning (BB) emits enormous amounts of aerosol particles and gases into the atmosphere and thereby significantly influences regional air quality and global climate. A dominant particle type from BB is spherical organic aerosol particles commonly referred to as tarballs. Currently, tarballs can only be identified, using microscopy, from their uniquely spherical shapes following impaction onto a grid. Despite their abundance and potential significance for climate, many unanswered questions related to their formation, emission inventory, removal processes, and optical properties still remain. Here, we report analysis that supports tarball formation in which primary organic particles undergo chemical and physical processing within ∼3 h of emission. Transmission electron microscopy analysis reveals that the number fractions of tarballs and the ratios of N and O relative to K, the latter a conserved tracer, increase with particle age and that the more-spherical particles on the substrates had higher ratios of N and O relative to K. Scanning transmission X-ray spectrometry and electron energy loss spectrometry analyses show that these chemical changes are accompanied by the formation of organic compounds that contain nitrogen and carboxylic acid. The results imply that the chemical changes increase the particle sphericity on the substrates, which correlates with particle surface tension and viscosity, and contribute to tarball formation during aging in BB smoke. These findings will enable models to better partition tarball contributions to BB radiative forcing and, in so doing, better help constrain radiative forcing models of BB events.

A large quantity of radionuclides was released by the Fukushima Daiichi Nuclear Power Plant accident in March 2011, and those deposited on ground and vegetation could return to the atmosphere through resuspension processes. Although the resuspension has been proposed to occur with wind blow, biomass burning, ecosystem activities, etc., the dominant process in contaminated areas of Fukushima is not fully understood. We have examined the resuspension process of radiocesium ( 134,137 Cs) based on long-term measurements of the atmospheric concentration of radiocesium activity (the radiocesium concentration) at four sites in the contaminated areas of Fukushima as well as the aerosol characteristic observations by scanning electron microscopy (SEM) and the measurement of the biomass burning tracer, levoglucosan. The radiocesium concentrations at all sites showed a similar seasonal variation: low from winter to early spring and high from late spring to early autumn. In late spring, they showed positive peaks that coincided with the wind speed peaks. However, in summer and autumn, they were correlated positively with atmospheric temperature but negatively with wind speed. These results differed from previous studies based on data at urban sites. The difference of radiocesium concentrations at two sites, which are located within a 1 km range but have different degrees of surface contamination, was large from winter to late spring and small in summer and autumn, indicating that resuspension occurs locally and/or that atmospheric radiocesium was not well mixed in winter/spring, and it was opposite in summer/autumn. These results suggest that the resuspension processes and the host particles of the radiocesium resuspension changed seasonally. The SEM analyses showed that the dominant coarse particles in summer and autumn were organic ones, such as pollen, spores, and microorganisms. Biological activities in forest ecosystems can contribute considerably to the radiocesium resuspension in these seasons. During winter and spring, soil, mineral, and vegetation debris were predominant coarse particles in the atmosphere, and the radiocesium resuspension in these seasons can be attributed to the wind blow of these particles. Any proofs that biomass (Continued on next page)

No abstract

We observed the atmospheric resuspension of radiocaesium, derived from the Fukushima Dai-ichi Nuclear Power Plant accident, at Namie, a heavily contaminated area of Fukushima, since 2012. During the survey periods from 2012 to 2015, the activity concentrations of radiocaesium in air ranged from approximately 10−5 to 10−2 Bq per m3 and were higher in the warm season than in the cold season. Electron microscopy showed that the particles collected on filters in summer were predominantly of biological origin (bioaerosols), with which the observed radiocaesium activity concentration varied. We conducted an additional aerosol analysis based on fluorescent optical microscopic observation and high-throughput DNA sequencing technique to identify bioaerosols at Namie in 2015 summer. The concentrations of bioaerosols fluctuated the order of 106 particles per m3, and the phyla Basidiomycota and Ascomycota (true Fungi) accounted for approximately two-thirds of the bioaerosols. Moreover, the fungal spore concentration in air was positively correlated with the radiocaesium concentration at Namie in summer 2016. The bioaerosol emissions from Japanese mixed forests in the temperate zone predominately included fungal cells, which are known to accumulate radiocaesium, and should be considered an important scientific issue that must be addressed.