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A novel nondestructive light element analysis method for bulk materials using muon beams was demonstrated. This method is based on the lifetime measurement of muons in a material and performed by measuring muon-decay electrons and identifying elements using the atomic number based on muon lifetimes. Muon irradiation on pure iron and two steel samples with known carbon contents was conducted to prepare a calibration curve for the quantitative analysis. We also performed a muon lifetime measurement for a Japanese sword and successfully determined its carbon content as 0.51 wt% using the calibration curve, without sample destruction. [ABSTRACT FROM AUTHOR]

The amount of C in steel, which is critical in determining its properties, is strongly influenced by steel production technology. We propose a novel method of quantifying the bulk C content in steel non-destructively using muons. This revolutionary method may be used not only in the quality control of steel in production, but also in analyzing precious steel archaeological artifacts. A negatively charged muon forms an atomic system owing to its negative charge, and is finally absorbed into the nucleus or decays to an electron. The lifetimes of muons differ significantly, depending on whether they are trapped by Fe or C atoms, and identifying the elemental content at the muon stoppage position is possible via muon lifetime measurements. The relationship between the muon capture probabilities of C/Fe and the elemental content of C exhibits a good linearity, and the C content in the steel may be quantitatively determined via muon lifetime measurements. Furthermore, by controlling the incident energies of the muons, they may be stopped in each layer of a stacked sample consisting of three types of steel plates with thicknesses of 0.5 mm, and we successfully determined the C contents in the range 0.20–1.03 wt% depth-selectively, without sample destruction. [ABSTRACT FROM AUTHOR]

A knob bow fibula (Bügelknopffibel) of the Leutkirch type, which typologically belongs to the second half of the 4th and early 5th century CE, was excavated in 2018 in the Roman city of Augusta Raurica, present-day Kaiseraugst (AG, Switzerland). This was analyzed for the first time for its elemental composition by using the non-destructive technique of Muon Induced X-ray Emission (MIXE) in the continuous muon beam facility at the Paul Scherrer Institute (PSI). In the present work, the detection limit is 0.4 wt% with ∼ 1.5 hours of measurement time. The fibula was measured at six different positions, at a depth of 0.3–0.4 mm inside the material. The experimental results show that the fibula is made of bronze, containing the main elements copper (Cu), zinc (Zn), tin (Sn) and lead (Pb). The compositional similarities/differences between different parts of the fibula reveal that it was manufactured as two "workpieces". One workpiece consists of the knob (13.0±0.6 wt% Pb), bow (11.9±0.4 wt% Pb) and foot (12.5 ± 0.9 wt% Pb). These show a higher Pb content, suggesting a cast bronze. The spiral (3.2 ± 0.2 wt% Pb), which is part of the other workpiece, has a comparatively lower Pb content, suggesting a forged bronze. [ABSTRACT FROM AUTHOR]

Elemental analysis based on muonic X-rays resulting from muon irradiation provides information about bulk material composition without causing damage, which is essential in the case of precious or otherwise unreachable samples, such as in archeology and planetary science. We developed a three-dimensional (3D) elemental analysis technique by combining the elemental analysis method based on negative muons with an imaging cadmium telluride double-sided strip detector (CdTe-DSD) designed for the hard X-ray and soft γ -ray observation. A muon irradiation experiment using spherical plastic samples was conducted at the Japan Proton Accelerator Research Complex (J-PARC); a set of projection images was taken by the CdTe-DSD, equipped with a pinhole collimator, for different sample rotation angles. The projection images measured by the CdTe-DSD were utilized to obtain a 3D volumetric phantom by using the maximum likelihood expectation maximization algorithm. The reconstructed phantom successfully revealed the 3D distribution of carbon in the bulk samples and the stopping depth of the muons. This result demonstrated the feasibility of the proposed non-destructive 3D elemental analysis method for bulk material analysis based on muonic X-rays. [ABSTRACT FROM AUTHOR]

The deposition of insoluble radiocesium-bearing microparticles (CsMPs), which were released from the Fukushima Daiichi Nuclear Power Plant (F1NPP) accident in March 2011, has resulted in the widespread contamination of eastern Japan. Obviously, these deposited insoluble CsMPs may become the secondary contamination sources by atmospheric migration or other environmental transferring process; however, the understanding of the transport mechanism remains non-elucidation, and the relevant evidence has not been directly provided. This study, for the first time, provides the direct evidence for the resuspension of these insoluble CsMPs to the atmosphere from (1) proximity of 137Cs radioactivity and resemblance of the morphology and the elemental compositions of CsMPs in the samples of soil and aerosol derived from the same sampling site, (2) the special characteristics of the resuspended CsMPs of which the ratios of Na/Si, K/Si and/or Cs/Si were smaller than those from the initially released CsMPs collected at either long distance or near F1NPP, which can be ascribed to the slowly natural corrosion of CsMPs by the loss of the small amount of soluble contents in CsMPs, and (3) high CsMPs concentration of 10 granules/g in the surface soil of our sampling site and high resuspension frequency of CsMPs in spring when predominant suspended particles were soil dust. Specifically, 15 single CsMPs were successfully isolated from the aerosol filters collected by unmanned high-volume air samplers at a severely polluted area in Fukushima Prefecture, about 25 km away from F1NPP, from January 2015 to September 2019. The mean diameter of these CsMPs was 1.8 ± 0.5 μm, and the average 137Cs radioactivity was 0.35 ± 0.23 Bq/granule. The contribution rate of the resuspended CsMPs to the atmospheric radiocesium was estimated from the ratio of 137Cs radioactivity of a single CsMP to that of the aerosol filter to be of 23.9 ± 15.3%. There has been no considerable decreasing trend in the annual CsMP resuspension frequency. [ABSTRACT FROM AUTHOR]

OGATA Koan (1810–63) was a physician and the director of Tekijuku, and he contributed to Western medicine in the late Edo period. Osaka University preserves two of his medicine chests. One of the chests, which was used in his last years (the second chest) contained 22 glass bottles and 6 wooden cylinders. These bottles and cylinders contained formulated medicines; however, about half cannot be opened because of the long-term storage. It is necessary to comprehend the physical property of both the containers and their contents for investigation of this adequate preservation method; however, destructive analysis is not allowed. To analyze the medicines sealed in the glass bottles, we focused on muonic X-ray analysis, which has high transmittance. First, we certified the analytical methods using a historical medicinal specimen preserved in Osaka University. Thereafter, we applied the method on the bottles stored in the second chest. X-ray fluorescence identified the glass of those bottles to be lead potash glass. Among these bottles, we chose the bottle with the label "甘," which contains white powdered medication, for muonic X-ray analysis. We identified the contents of the medication in the glass to be Hg2Cl2. Through this study, we first applied muonic X-ray analysis on the medical inheritances and succeeded to detect the elements contained both in the container and in the contents of the sealed bottle. This would be a new method for nondestructive analysis of such cultural properties. [ABSTRACT FROM AUTHOR]

The structural form and elemental distribution of material originating from different Fukushima Daiichi Nuclear Power Plant reactors (Units 1 and 3) is hereby examined to elucidate their contrasting release dynamics and the current in-reactor conditions to influence future decommissioning challenges. Complimentary computed X-ray absorption tomography and X-ray fluorescence data show that the two suites of Si-based material sourced from the different reactor Units have contrasting internal structure and compositional distribution. The known event and condition chronology correlate with the observed internal and external structures of the particulates examined, which suggest that Unit 1 ejecta material sustained a greater degree of melting than that likely derived from reactor Unit 3. In particular, we attribute the near-spherical shape of Unit 1 ejecta and their internal voids to there being sufficient time for surface tension to round these objects before the hot (and so relatively low viscosity) silicate melt cooled to form glass. In contrast, a more complex internal form associated with the sub-mm particulates invoked to originate from Unit 3 suggest a lower peak temperature, over a longer duration. Using volcanic analogues, we consider the structural form of this material and how it relates to its environmental particulate stability and the bulk removal of residual materials from the damaged reactors. We conclude that the brittle and angular Unit 3 particulate are more susceptible to further fragmentation and particulate generation hazard than the round, higher-strength, more homogenous Unit 1 material. [ABSTRACT FROM AUTHOR]

An elemental analysis method utilizing muons has been demonstrated to be effective for non-destructive and quantitative analysis of precious bulk materials. In muon capture process, molecular structure dependence was known, and this property has the potential to be used to identify chemical structure in addition to elemental composition. Before these potential applications, fundamental studies examining the muon capture process are necessary. In this study, muon capture ratios for two iron oxide compounds, which are both important in earth science, γ-Fe2O3 (maghemite) and Fe3O4 (magnetite), were measured. The measured muon capture ratios were A(Fe/O) = 2.34 ± 0.03 and A(Fe/O) = 2.77 ± 0.03 for γ-Fe2O3 and Fe3O4, respectively. [ABSTRACT FROM AUTHOR]

Variations in isotopic abundance provide useful information for various scientific fields. Herein we performed a feasibility study by non-destructive isotopic analysis of negative muons. We irradiated two lead plate samples, one with the natural isotopic composition and one enriched with 208Pb, with negative muons and observed the gamma rays from 208Tl with a half-life of 3 min generated via muon absorption by 208Pb during muon irradiation. The isotopic abundance of 208Pb in natPb was successfully determined without sample destruction from the gamma ray intensity to be 69%, which agreed well with the mass spectrometry results. [ABSTRACT FROM AUTHOR]

Elemental isotopic ratios are measured in various research fields and provide useful information regarding age, origin, geological and biological activities, ancient climate, etc. Here, we report a new isotopic analysis method without sample destruction using muon-induced characteristic X-rays. We demonstrated this method by conducting muon-beam irradiation experiments on two Pb plates with different isotopic ratios: natural isotopic composition and artificially enriched 208Pb. The observed broad X-ray peaks of the Pb Kα line around 6 MeV were deconvolved with 206Pb, 207Pb, and 208Pb isotopes, giving the isotopic ratios. The resulting isotopic ratios were consistent with those obtained from mass spectrometry. [ABSTRACT FROM AUTHOR]

The role of valence electrons for the muon capture process by molecules is experimentally investigated with the aid of cascade calculations. Low-momentum muons are introduced to gas targets of CO, CO2, and COS below atmospheric pressure. The initial states of captured muons are determined from the measured muonic X-ray structure of the Lyman and Balmer series. We propose that the lone pair electrons in the carbon atom of CO significantly contribute to the capture of a muon with large angular momenta. [ABSTRACT FROM AUTHOR]

Per-atom muon capture ratios are precisely determined from characteristic muonic X-ray measurements of three nitrogen oxide samples (NO, N2O, and NO2) at pressures below 100 kPa. A higher density of covalent electrons at the N atoms relative to the O atoms is required if we explain the experimental results using the proposed muon capture models. From molecular orbit calculations, we found that the electron distributions of only the highest occupied molecular orbitals (HOMO) are dominant at the N atoms, and the electrons in the HOMO significantly contribute to the muon capture phenomena in the nitrogen oxide molecules. [ABSTRACT FROM AUTHOR]

Elemental analysis by measurement of muonic X-rays shows great potential for analyzing the elemental composition of a bulk material at a specific depth without sample destruction. For quantitative analysis, muon capture probability is the most important parameter. In this work, the muon capture ratios and muonic X-ray intensity patterns of metal oxides for geochemically and cosmochemically important compounds, MgO, CaO, MnO and Fe3O4, were determined. The muon capture ratios of Ca/Mg and Fe/Mn were proportional to the mixing ratios of CaO/MgO and Fe3O4/MnO. From this relationship, the elemental composition can be determined from the muonic X-ray intensity ratio alone. [ABSTRACT FROM AUTHOR]

To investigate the time variations of radionuclides discharged from the Fukushima Daiichi nuclear power plants accident, we started collecting aerosol samples in Osaka, Japan, using a high-volume sampler from March 15 to May 1, 2011. Atmospheric radioactivity concentrations of I-131, Cs-134 and Cs-137 were measured with germanium semi-conductor detectors. Only I-131 was detected in the early phase and two Cs-134.137 peaks were found in Osaka in April. Using the HYSPLIT model, we concluded that direct transportation of the air mass from the Fukushima area was responsible for such events. [ABSTRACT FROM AUTHOR]

Optical imaging of particle beams is a promising method for range and width estimations. However it was not clear that optical imaging was possible for muons. To clarify this, we conducted optical imaging of muons, since high-intensity muons are now available at J-PARC. We irradiated positive muons with different momenta to water or plastic scintillator block, and imaged using a charge-coupled device (CCD) camera during irradiation. The water and plastic scintillator block produced quite different images. The images of water during irradiation of muons produced elliptical shape light distribution at the end of the ranges due to Cherenkov-light from the positrons produced by positive muon decay, while, for the plastic scintillator block, we measured images similar to the dose distributions. We were able to estimate the ranges of muons as well as the measurement of the asymmetry of the direction of the positron emission by the muon decays from the optical images of the water, although the measured ranges were 4 mm to 5 mm larger than the calculated values. The ranges and widths of the beams could also be estimated from the optical images of the plastic scintillator block. We confirmed that optical imaging of muons was possible and is a promising method for the quality assessment, research of muons, and the future muon radiotherapy. [ABSTRACT FROM AUTHOR]

Radioactive particles were released into the environment during the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. Many studies have been conducted to elucidate the chemical composition of released radioactive particles in order to understand their formation process. However, whether radioactive particles contain nuclear fuel radionuclides remains to be investigated. Here, we report the first determination of Pu isotopes in radioactive particles. To determine the Pu isotopes (239Pu, 240Pu and 241Pu) in radioactive particles derived from the FDNPP accident which were free from the influence of global fallout, radiochemical analysis and inductively coupled plasma-mass spectrometry measurements were conducted. Radioactive particles derived from unit 1 and unit 2 or 3 were analyzed. For the radioactive particles derived from unit 1, activities of 239+240Pu and 241Pu were (1.70–7.06) × 10−5 Bq and (4.10–8.10) × 10−3 Bq, respectively and atom ratios of 240Pu/239Pu and 241Pu/239Pu were 0.330–0.415 and 0.162–0.178, respectively. These ratios were consistent with the simulation results from ORIGEN code and measurements from various environmental samples. In contrast, Pu was not detected in the radioactive particles derived from unit 2 or 3. The difference in Pu contents is clear evidence towards different formation processes of radioactive particles, and detailed formation processes can be investigated from Pu analysis. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]