ABSTRACT
Pyrocumulonimbus (pyroCb) firestorm systems have been shown to inject significant amounts of black carbon (BC) to the stratosphere with a residence time of several months. Injected BC warms the local stratospheric air, consequently perturbing transport and hence spatial distributions of ozone and water vapor. A distinguishing feature of BC-containing particles residing within pyroCb smoke is their thick surface coatings made of condensed organic matter. When coated with non-refractory materials, BC's absorption is enhanced, yet the absorption enhancement factor (Eabs) for pyroCb BC is not well constrained. Here, we perform particle-scale measurements of BC mass, morphology, and coating thickness from inside a pyroCb cloud and quantify Eabs using an established particle-resolved BC optics model. We find that the population-averaged Eabs for BC asymptotes to 2.0 with increasing coating thickness. This value denotes the upper limit of Eabs for thickly coated BC in the atmosphere. Our results provide observationally constrained parameterizations of BC absorption for improved radiative transfer calculations of pyroCb events.
ABSTRACT
Primary biological aerosol particles (PBAP) play an important role in the climate system, facilitating the formation of ice within clouds, consequently PBAP may be important in understanding the rapidly changing Arctic. Within this work, we use single-particle fluorescence spectroscopy to identify and quantify PBAP at an Arctic mountain site, with transmission electronic microscopy analysis supporting the presence of PBAP. We find that PBAP concentrations range between 10-3-10-1 L-1 and peak in summer. Evidences suggest that the terrestrial Arctic biosphere is an important regional source of PBAP, given the high correlation to air temperature, surface albedo, surface vegetation and PBAP tracers. PBAP clearly correlate with high-temperature ice nucleating particles (INP) (>-15 °C), of which a high a fraction (>90%) are proteinaceous in summer, implying biological origin. These findings will contribute to an improved understanding of sources and characteristics of Arctic PBAP and their links to INP.
ABSTRACT
Wildfires emit large amounts of black carbon and light-absorbing organic carbon, known as brown carbon, into the atmosphere. These particles perturb Earth's radiation budget through absorption of incoming shortwave radiation. It is generally thought that brown carbon loses its absorptivity after emission in the atmosphere due to sunlight-driven photochemical bleaching. Consequently, the atmospheric warming effect exerted by brown carbon remains highly variable and poorly represented in climate models compared with that of the relatively nonreactive black carbon. Given that wildfires are predicted to increase globally in the coming decades, it is increasingly important to quantify these radiative impacts. Here we present measurements of ensemble-scale and particle-scale shortwave absorption in smoke plumes from wildfires in the western United States. We find that a type of dark brown carbon contributes three-quarters of the short visible light absorption and half of the long visible light absorption. This strongly absorbing organic aerosol species is water insoluble, resists daytime photobleaching and increases in absorptivity with night-time atmospheric processing. Our findings suggest that parameterizations of brown carbon in climate models need to be revised to improve the estimation of smoke aerosol radiative forcing and associated warming.
ABSTRACT
We have measured artificial radionuclides, such as 90Sr and 137Cs, in atmospheric depositions since 1957 in Japan. We observed the variations in 90Sr and 137Cs, which were emitted from atmospheric nuclear tests and nuclear power plant accidents, due to their diffusion, deposition, and resuspension. In March 2011, the Fukushima Daiichi Nuclear Power Plant accident occurred in Japan, and significant increases in 90Sr and 137Cs were detected at our main site in Tsukuba, Ibaraki. Our continual observations revealed that the 137Cs monthly deposition rate in 2018 declined to ~ 1/8100 of the peak level, but it remained more than ~ 400 times higher than that before the accident. Chemical analysis suggested that dust particles were the major carriers of 90Sr and 137Cs during the resuspension period at our main site. Presently, the effective half-life for 137Cs deposition due to radioactive decay and other environmental factors is 4.7 years. The estimation suggests that approximately 42 years from 2011 are required to reduce the atmospheric 137Cs deposition to a state similar to that before the accident. The current 90Sr deposition, on the other hand, shows the preaccident seasonal variation, and it has returned to the same radioactive level as that before the accident.
ABSTRACT
It is the conventional understanding that rain removes aerosols from the atmosphere. However, the question of whether rain plays a role in releasing aerosols to the atmosphere has recently been posed by several researchers. In the present study, we show additional evidence for rain-induced aerosol emissions in a forest environment: the occurrence of radiocaesium-bearing aerosols in a Japanese forest due to rain. We carried out general radioactive aerosol observations in a typical mountainous village area within the exclusion zone in Fukushima Prefecture to determine the impacts and major drivers of the resuspension of radiocaesium originating from the nuclear accident in March 2011. We also conducted sampling according to the weather (with and without rain conditions) in a forest to clarify the sources of atmospheric radiocaesium in the polluted forest. We found that rain induces an increase in radiocaesium in the air in forests. With further investigations, we confirmed that the fungal spore sources of resuspended radiocaesium seemed to differ between rainy weather and nonrainy weather. Larger fungal particles (possibly macroconidia) are emitted during rainy conditions than during nonrainy weather, suggesting that splash generation by rain droplets is the major mechanism of the suspension of radiocaesium-bearing mould-like fungi. The present findings indicate that radiocaesium could be used as a tracer in such research fields as forest ecology, meteorology, climatology, public health and agriculture, in which fungal spores have significance.
ABSTRACT
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 â¼3 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.
Subject(s)
Air Pollutants/chemistry , Biomass , Particulate Matter/chemistry , Smoke/analysis , Tars/chemistry , Aerosols/chemistry , Climate , Organic Chemicals/analysis , Surface Tension , ViscosityABSTRACT
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.
Subject(s)
Air Pollution, Radioactive/analysis , Cerium Radioisotopes/analysis , Spores, Fungal/chemistry , Air Pollution, Radioactive/adverse effects , Fukushima Nuclear Accident , Japan , Radiation Monitoring/methods , SeasonsABSTRACT
Combustion-induced carbonaceous aerosols, particularly black carbon (BC) and brown carbon (BrC), have been largely considered as the only significant anthropogenic contributors to shortwave atmospheric heating. Natural iron oxide (FeOx) has been recognized as an important contributor, but the potential contribution of anthropogenic FeOx is unknown. In this study, we quantify the abundance of FeOx over East Asia through aircraft measurements using a modified single-particle soot photometer. The majority of airborne FeOx particles in the continental outflows are of anthropogenic origin in the form of aggregated magnetite nanoparticles. The shortwave absorbing powers (Pabs) attributable to FeOx and to BC are calculated on the basis of their size-resolved mass concentrations and the mean Pabs(FeOx)/Pabs(BC) ratio in the continental outflows is estimated to be at least 4-7%. We demonstrate that in addition to carbonaceous aerosols the aggregate of magnetite nanoparticles is a significant anthropogenic contributor to shortwave atmospheric heating.
ABSTRACT
The mass extinction of life 66 million years ago at the Cretaceous/Paleogene boundary, marked by the extinctions of dinosaurs and shallow marine organisms, is important because it led to the macroevolution of mammals and appearance of humans. The current hypothesis for the extinction is that an asteroid impact in present-day Mexico formed condensed aerosols in the stratosphere, which caused the cessation of photosynthesis and global near-freezing conditions. Here, we show that the stratospheric aerosols did not induce darkness that resulted in milder cooling than previously thought. We propose a new hypothesis that latitude-dependent climate changes caused by massive stratospheric soot explain the known mortality and survival on land and in oceans at the Cretaceous/Paleogene boundary. The stratospheric soot was ejected from the oil-rich area by the asteroid impact and was spread globally. The soot aerosols caused sufficiently colder climates at mid-high latitudes and drought with milder cooling at low latitudes on land, in addition to causing limited cessation of photosynthesis in global oceans within a few months to two years after the impact, followed by surface-water cooling in global oceans in a few years. The rapid climate change induced terrestrial extinctions followed by marine extinctions over several years.
ABSTRACT
Microparticles containing substantial amounts of radiocesium collected from the ground in Fukushima were investigated mainly by transmission electron microscopy (TEM) and X-ray microanalysis with scanning TEM (STEM). Particles of around 2 µm in diameter are basically silicate glass containing Fe and Zn as transition metals, Cs, Rb and K as alkali ions, and Sn as substantial elements. These elements are homogeneously distributed in the glass except Cs which has a concentration gradient, increasing from center to surface. Nano-sized crystallites such as copper- zinc- and molybdenum sulfide, and silver telluride were found inside the microparticles, which probably resulted from the segregation of the silicate and sulfide (telluride) during molten-stage. An alkali-depleted layer of ca. 0.2 µm thick exists at the outer side of the particle collected from cedar leaves 8 months after the nuclear accident, suggesting gradual leaching of radiocesium from the microparticles in the natural environment.
ABSTRACT
Synchrotron radiation (SR) X-ray microbeam analyses revealed the detailed chemical nature of radioactive aerosol microparticles emitted during the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, resulting in better understanding of what occurred in the plant during the early stages of the accident. Three spherical microparticles (â¼2 µm, diameter) containing radioactive Cs were found in aerosol samples collected on March 14th and 15th, 2011, in Tsukuba, 172 km southwest of the FDNPP. SR-µ-X-ray fluorescence analysis detected the following 10 heavy elements in all three particles: Fe, Zn, Rb, Zr, Mo, Sn, Sb, Te, Cs, and Ba. In addition, U was found for the first time in two of the particles, further confirmed by U L-edge X-ray absorption near-edge structure (XANES) spectra, implying that U fuel and its fission products were contained in these particles along with radioactive Cs. These results strongly suggest that the FDNPP was damaged sufficiently to emit U fuel and fission products outside the containment vessel as aerosol particles. SR-µ-XANES spectra of Fe, Zn, Mo, and Sn K-edges for the individual particles revealed that they were present at high oxidation states, i.e., Fe(3+), Zn(2+), Mo(6+), and Sn(4+) in the glass matrix, confirmed by SR-µ-X-ray diffraction analysis. These radioactive materials in a glassy state may remain in the environment longer than those emitted as water-soluble radioactive Cs aerosol particles.
ABSTRACT
The Fukushima nuclear accident released radioactive materials into the environment over the entire Northern Hemisphere in March 2011, and the Japanese government is spending large amounts of money to clean up the contaminated residential areas and agricultural fields. However, we still do not know the exact physical and chemical properties of the radioactive materials. This study directly observed spherical Cs-bearing particles emitted during a relatively early stage (March 14-15) of the accident. In contrast to the Cs-bearing radioactive materials that are currently assumed, these particles are larger, contain Fe, Zn, and Cs, and are water insoluble. Our simulation indicates that the spherical Cs-bearing particles mainly fell onto the ground by dry deposition. The finding of the spherical Cs particles will be a key to understand the processes of the accident and to accurately evaluate the health impacts and the residence time in the environment.
Subject(s)
Cesium/analysis , Cesium/chemistry , Fukushima Nuclear Accident , Models, Chemical , Radioactive Fallout/analysis , Computer Simulation , Japan , Microspheres , Radiation Monitoring/methodsABSTRACT
Following the "Guidelines for reporting TBL" by Haidet et al, we report on a team-based learning (TBL) course we adopted for our 4th-year students in 2011. Our TBL course is a modified version of the one suggested in the guidelines, but its structure generally follows the core elements described therein. Using an audience response system (ARS), we were able to obtain individual and group readiness assurance test scores immediately and give instant feedback to the students. Instructors were thus able to monitor students' understanding in real time and so appreciated the system, which supports interactive classes even in large classrooms. However, TBL is teacher-oriented, and students were less appreciative of ARS, because they recognized that it could be easily used for grading. Nevertheless, we believe that a combination of TBL, and problem-based learning in a mature design can improve both motivation and understanding among learners.
Subject(s)
Cooperative Behavior , Education, Medical, Undergraduate/methods , Group Processes , Problem-Based Learning/methods , Comprehension , Education, Medical, Undergraduate/standards , Humans , Motivation , Problem-Based Learning/standards , Reproducibility of Results , Surveys and Questionnaires , Teaching/methods , Teaching/standardsABSTRACT
Nanoparticles (NPs) are ubiquitous in the atmosphere. Because of their small sizes, they can travel deeply into the lungs and other parts of the body. Many are highly reactive which, combined with their large surface areas, means they can seriously affect human health. Their occurrences in the atmosphere and their biological effects are not well-understood. We focus on NPs that were either free-floating or hosted within large aerosol particles (aerodynamic diameter 50-300 nm) and consist of or contain transition or post-transition metals (m-NPs). The samples were collected from ambient air above Mexico City (MC). We used transmission electron microscopy to measure their sizes and compositions. More than half of the 572 m-NPs that we analyzed contain two or more metals, and Fe, Pb, or Zn occurs in more than 60%. Hg occurs in 21% and is especially abundant in free-floating m-NPs. We find that m-NPs are common in polluted air such as in the MC area and, by inference, presumably other megacities. The range and variety of compositions of m-NPs that we encountered, whether free-floating or hosted within larger aerosol particles, indicate the complicated occurrences that should be considered when evaluating the health effects of m-NPs in complex urban areas.
Subject(s)
Atmosphere/chemistry , Metal Nanoparticles/analysis , Health , Humans , Metal Nanoparticles/ultrastructure , Mexico , Particle SizeABSTRACT
BACKGROUND: Apocrine carcinomas are rare, the immunohistochemical characterizations that are incomplete. The purpose of this study was to determine the immunohistochemical characteristics of mucin core proteins and keratins in apocrine carcinoma, extramammary Paget's disease (EMPD) and apocrine nevus. METHODS: We report four cases of apocrine carcinomas along with immunohistochemical analyses: (i) an axillary apocrine carcinoma with an apocrine nevus, (ii) an inguinal apocrine carcinoma, (iii) a vulvar apocrine carcinoma with EMPD and (iv) an axillary apocrine carcinoma with EMPD and an apocrine nevus. RESULTS: The tumor cells of apocrine carcinomas, EMPD and apocrine nevi displayed a positive reaction to MUC-1 and CK7 and a negative reaction to CK20. Apocrine carcinomas had high molecular weight (HMW) cytokeratin(+)/CK5(+)/CK14(-)/MUC5AC(-), EMPD with underlying apocrine carcinoma had HMW cytokeratin(-)/CK5(-)/CK14(-)/MUCA5AC(-) and the apocrine nevi had HMW cytokeratin(+)/CK5(+)/CK14(+)/MUCA5AC(+). CONCLUSION: The immunohistochemical findings suggest that apocrine carcinomas, apocrine nevi and EMPD with underlying apocrine carcinomas are quite different, even though they are all derived from apocrine glands.
Subject(s)
Carcinoma, Skin Appendage/metabolism , Keratins/biosynthesis , Mucins/biosynthesis , Nevus/metabolism , Paget Disease, Extramammary/metabolism , Sweat Gland Neoplasms/metabolism , Adult , Aged , Aged, 80 and over , Apocrine Glands/metabolism , Apocrine Glands/pathology , Biomarkers, Tumor/analysis , Carcinoma, Skin Appendage/complications , Carcinoma, Skin Appendage/pathology , Humans , Immunohistochemistry , Male , Nevus/complications , Nevus/pathology , Paget Disease, Extramammary/complications , Paget Disease, Extramammary/pathology , Sweat Gland Neoplasms/pathologyABSTRACT
The sources and character of individual metal and metalloid particles from atmospheric dry depositions in Kobe, Japan were investigated. Japan faces long-range pollutant transportation from northeastern Asia during winter and spring. Information regarding their properties and sources is useful for evaluating their affects on the environment and human health. Individual metal and metalloid particles that were collected for every 24 h on the plate, which was designed to reduce a local turbulence, were characterized for their composition, diameter, and deposition fluxes using a field emission scanning electron microscope with an energy dispersive X-ray spectrometer. Approximately 3,000 metal and metalloid particles were classified into 14 types based on their composition and further classified into four groups based on their distribution patterns. They are (A) Fe-O, Fe-Ba-Sb-Cu-S-Ti-O, Fe-Zn-O, Zn-O, Ni-O, and Mn-Fe-O; (B) Cu-Zn-O and Cu-Sn-O; (C) Pb-O, Sn-Sb-O, and Ag-O; (D) Pb-Zn-Cl-Si-S-O and Bi-Cl-O. From these data, this study suggests their sources as the Asian continent (Group A), local source (Group B), multiple sources (Group C), and incineration process (Group D). This study shows (1) the sources and character of individual metal and metalloid particles from short-term atmospheric depositions in Kobe, Japan and (2) application of individual particle analysis for atmospheric depositions.
Subject(s)
Air Pollutants/analysis , Environmental Monitoring , Metals/analysis , Japan , Particle Size , SeasonsABSTRACT
Tire dust is a significant pollutant, especially as a source of zinc in the urban environment. This study characterizes the morphology and chemical composition of heavy metal particles embedded in tire dust and traffic-related materials (brake dust, yellow paint, and tire tread) as measured by a field emission scanning electron microscope equipped with an energy dispersive X-ray spectrometer (FESEM/EDX). In 60 samples of tire dust, we detected 2288 heavy metal particles, which we classified into four groups using cluster analysis according to the following typical elements: cluster 1: Fe, cluster 2: Cr/Pb, cluster 3: multiple elements (Ti, Cr, Fe, Cu, Zn, Sr, Y, Zr, Sn, Sb, Ba, La, Ce, Pb), cluster 4: ZnO. According to their morphologies and chemical compositions, the possible sources of each cluster were as follows: (1) brake dust (particles rich in Fe and with trace Cu, Sb, and Ba), (2) yellow paint (CrPbO(4) particles), (3) brake dust (particulate Ti, Fe, Cu, Sb, Zr, and Ba) and heavy minerals (Y, Zr, La, and Ce), (4) tire tread (zinc oxide). When the chemical composition of tire dust was compared to that of tire tread, the tire dust was found to have greater concentrations of heavy metal elements as well as mineral or asphalt pavement material characterized by Al, Si, and Ca. We conclude that tire dust consists not only of the debris from tire wear but also of assimilated heavy metal particles emitted from road traffic materials such as brake lining and road paint.