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Beard samples were collected every day from a single person (55 [at start] to 66- [at end] years old) over a 12-year period. Beard hair samples were analyzed by particle induced X-ray emission (PIXE) to determine variations in concentrations of aluminum, chromium, arsenic, mercury and lead over the sampling period. Only mercury showed a gentle upward trend with age, and a significant increase of 20–30% was observed. This fact was consistent with the results of our previous studies on more than 1250 hairs collected from healthy people. It was also found that concentrations of many toxic elements tended to be higher in summer than in winter, except for chromium. In particular, arsenic and mercury concentrations significantly increased in summer. Their concentrations in the winter dropped to less than 50% and 86% of those in the summer, respectively. These seasonal changes can be attributed to changes in the ingestion of season-specific foods, such as marine products. These findings indicate that beard analyses are a powerful tool for evaluating the exposure to toxic-element.

The aim of study was to investigate the relationships among serum diamine oxidase (DAO) activity, postnatal days and the plasma copper (Cu) concentration, using calves with or without diarrhea. In healthy calves, the serum DAO activity was significantly higher at 2 postnatal days than at ≥7 postnatal days, and no significant changes were observed after 7 postnatal days. In addition, no significant correlation was found between serum DAO activity and plasma Cu concentration at all postnatal days in healthy calves. Although, the serum DAO activity in 14 diarrheic calves (66.78 ± 14.37 IU/ml) was lower than that in 19 healthy calves (170.33 ± 97.83 IU/ml, P

More than 4000 beard samples were collected from a single person every morning over a 12-year period and analyzed using a standard-free method. We detected significant annual variations in the concentrations of magnesium and calcium in the study period, although significant monthly and seasonal variations were not noted. Calcium tends not to be obtained from season-specific foods or drinks, so its variations may be affected by changes in the metabolism of the body. In contrast, however, potassium showed marked long-term variations with significant seasonal differences. As our previous studies confirmed that green vegetables contain large quantities of potassium and that their supply and consumption increase from May to July, the seasonal variations in potassium concentration were attributed to the ingestion of green vegetables. Although magnesium is also contained in green vegetables in large quantities, its principle supply sources are diverse and its concentration did not show any clear seasonal changes.

A total of 4269 beard samples were collected from the same person every day over a 12-year period and analyzed by PIXE using a standard-free method. It was found that the concentrations of copper and zinc showed certain short-term changes but did not show a noticeable long-term trend over the study period, with only iron showing a slightly decreasing tendency with age. All of these elements showed clear yearly variations with a cycle of a few years possibly due to periodic metabolic changes in the subject’s body or long-term changes in eating habits. In contrast, however, selenium showed clear seasonal variations. Its concentration significantly increased in the summer and decreased in the winter, just as was observed with arsenic and mercury. This suggests that most of the subject’s selenium intake was from marine products, whose supply and consumption were increased in the summer. These findings confirmed that beard analyses are useful not only for evaluating essential-element intake but also for estimating the relationship between the body-element concentrations and ingestion of certain foods.

We performed a particle-induced X-ray emission (PIXE) analysis of tea leaf samples (Camellia sinensis (L.) Kuntze) to evaluate the possibility of internal radiation exposure due to the intake of green tea contaminated with [Formula: see text]Cs and [Formula: see text]Sr. The tea leaf samples were obtained from tea trees (Camellia sinensis cv. ‘Yabukita’) cultivated with stable Cs and Sr added to the soil. We prepared the used leaf samples which were placed in distilled hot water (90[Formula: see text] for 1 min) as well as the unused leaf samples. The results of PIXE analysis combined with the internal standard method using Indium as a standard element showed little elution of Ca and Sr from the leaves to green tea, while the concentration of alkali elements, including Cs in the leaf, decreased by 30–40% after the tea was extracted.

We investigated the relationships between the element concentrations in blood and hair to clarify the sex-specific differences in elemental movement from blood to hair, as we confirmed the presence of large sex-specific differences in the concentrations of certain elements in hair in our previous study. First, we compared the elemental concentrations in serum/plasma taken from healthy people ([Formula: see text] females, 142 males) and found that there were significant differences (up to 20%) between females and males in levels of phosphorus, sulfur, calcium, bromine, and lead. We then examined the sex-specific differences in the elemental transfer factors from blood to hair by analyzing plasma and hair samples that had been simultaneously collected from the same people (20 females, 21 males). Calcium and selenium showed significant differences in transfer factors from plasma to hair. Particularly, large sex-specific differences in the calcium concentration were explained by the difference in the transfer factors from blood to hair. We also examined the sex-specific differences among teenaged subjects alone ([Formula: see text] females, 9 males; average age was approximately 17 years old) and noted no significant difference in the transfer factors between sexes. Taken together, these findings indicate that the transfer factors themselves are influenced by the excretion of sex hormones.

After the 2011 Off the Pacific Coast of Tohoku Earthquake on 11 March, 2011, volcanic activity in Japan was observed to increase. In this study, we use the PIXE method to analyze elemental concentrations in stream water flowing directly from the fumarolic area on Mount Hakone, which erupted on 30 June 2015. Throughout a two-year monitoring period following the eruption, concentrations of 12 dissolved elements were measured. We found that the stream water was strongly acidic. For one year after the eruption, the concentrations of magma-derived elements (S, Cl) and rock-derived elements (Al, Ca, Fe, K, Mg, Mn, and Na), except for Si, showed a clear decreasing trend. These measurements suggest that magmatic activity and fumarolic activity reduced gradually over one year. After this year-long period, elemental concentrations stopped decreasing and instead showed broadly flat levels with sporadic increases and decreases. However, throughout the year immediately following the eruption, the number of volcanic earthquakes was consistently at zero or close to zero. These different indications of volcanic activity suggest that the elemental concentrations in stream water may be more sensitive indicators of small changes in subterranean behavior than of the number of volcanic earthquakes.

In recent years, the contamination of marine products with heavy toxic elements has become a problem in Japan, as the Japanese coastal sea water is confirmed to be highly contaminated with heavy elements. In this study, parts of scallops and ascidians, which are the main foods of the people living in the Sanriku District, including hijiki and the fatty meal of whale, were analyzed. We also analyzed some parts that are not commonly eaten in general but are often consumed by some local populations, such as the mantle, mid-gut gland, ovary and spermary of scallops, and the internal organs and pharyngeal basket of ascidians. Dangerous quantities were detected for mercury in fatty meal of whale and for arsenic in hijiki, the mid-gut gland and mantle of scallops and the internal organs and pharyngeal basket of ascidians. In addition, concentrations of cadmium in the mid-gut gland and mantle of scallops as well as in the internal organs and pharyngeal basket of ascidians also showed high values. These results suggested that, even in the daily diet, it is possible to consume arsenic and cadmium in greater-than-tolerable quantities.

At Nishina Memorial Cyclotron Center (NMCC), a large number of studies in various research fields have been pursued under nation-wide common usage since 1993. One of the features of NMCC’s PIXE is the performance of many problem-based studies in order to determine effective measures against a range of issues. Various samples must be quantitatively analyzed quickly and accurately to cope with environmental issues. We have developed several original methods for analyzing a variety of samples with good sensitivity. Specially designed absorbers were developed for sensitive analyses of samples composed of heavy elements. In addition, a powdered-internal-standard method was established for the accurate quantitative analyses of powdered samples whose matrixes are heavy elements. The standard-free method for bio-samples allowed us to quantitatively analyze untreated samples, micro samples of nearly 1 [Formula: see text]g, and live bio-samples. We have been tackling a number of environmental problems in many countries in Southeast and East Asia using these original methods. We also wrestled with environmental problems caused by the massive tsunami that struck the Sanriku district of Japan in March 2011.

The objective of this study is to examine the ability of PIXE to distinguish the country of origin of duvets. The stable isotope method that is currently used is not recognized as reliable. Mineral concentrations of down feathers from France, Poland and Taiwan were measured by PIXE. The measurements were statistically analyzed. The results show even a scatter plot of appropriately chosen minerals distinguished between those countries at 95% accuracy.

Recent rise of social attention towards ethical jewelry has led scientists to a challenge of how to construct analytical systems that can deliver in line with social and supply chain expectations. Of the various kinds of methods, “Proton/Particle-Induced X-ray Emission” (PIXE) seems to be robust and promising in characterizing gemstones because of its capability of trace element analysis without destruction. The authors established a non-standard method to analyze cultured pearls and applied it to test specimens from different places. The results showed that PIXE could detect important elements for pearl study with good accuracy and sensitivity and that pearl chemistry can be useful to differentiate freshwater and marine pearl products.

Levels of trace element pollution in surface soil have been estimated using soil analyses and leaching tests. These methods may reveal different results due to the effect of soil properties on the elemental availability. Therefore, this study advocates an alternative method for monitoring and assessment of trace element pollution in surface soil using terricolous fruticose lichens. Lichens and their substrata were analyzed using particle induced X-ray emission (PIXE), inductively coupled plasma-mass spectrometry (ICP-MS) and XRF to clarify the relationships between Cu, Zn, As and Pb concentrations in lichens and soils, including their absorption properties. Concentrations of these elements in the lichens were positively correlated with those in the soils regardless of lichen species, location, habitat, or conditions of soils. The analyzed lichens had neither competitive nor antagonistic properties in their elemental absorption, which made them good bioindicators of trace element pollution in surface soil. The distribution maps of average Cu, Zn, As and Pb concentrations at each sampling region was detected at almost all of the Cu, Zn and As pollution of the soils. Therefore, lichens could be used in practical applications to monitor Cu, Zn and As pollution in surface soils.

Recently, atmospheric particles, including Asian dust, have attracted considerable attention because of their potential effects on the environment and human health. From March to May, a huge volume of Asian dust is whipped up over China and carried to Japan by the westerly winds. In this study, we analyzed the elemental compositions of 72 aerosol samples collected biweekly in Kumamoto City from March 2004 to March 2007, to investigate the characteristics of Asian dust. The mass concentrations of the aerosol in Asian dust events were 1.5 times higher than non-Asian dust events. The concentrations of elements were determined by the Proton Induced X-ray Emission (PIXE) method. Concentrations of Si, Al, Fe, Ca, Ti, Mg and K in Asian dust events were 2.3, 2.0, 2.0, 1.6, 1.6, 1.5 and 1.4 times higher than those in non-Asian dust events, respectively. These elements are considered indicators of a soil-derived fraction. The concentrations of the soil-derived fraction were calculated, assuming that the Al concentration in the soils is 7%. The predicted mean concentration of the soil-derived fraction in Asian dust events (16.92 μg·m−3) was twice that in non-Asian dust events (8.39 μg·m−3). Moreover, in Asian dust events, the soil-derived fraction was the main component in aerosols and accounted for 43% of the total aerosol mass.

The nanoparticles, which releases anticancer drug with response to radiation, were developed. Also, two categories were tested: (i) their ability to release anticancer drug in vitro; and (ii) their kinetics in the body, when they were injected through tail vein of BALB/c mice in vivo. To prepare the particles, hyaluronic acid and protamine were mixed into carboplatin solution, and reacted for 30 min in room temperature. Those particles were exposed to a single dose of 10 Gy of 140 KeV X-ray. Their ability to release carboplatin with response to radiation was expressed as the percentage of ruptured particles, basing on images of particles, using micro PIXE camera. The amount of released carboplatin was measured by quantitative PIXE method. The kinetics of particles in body was assessed by counting the number of particles, which were trapped in lungs, using micro PIXE camera. The mean diameter of particles was 743 ± 34 nm. By irradiation, 59.3 ± 7.23% of particles ruptured, and 95.9 ± 2.3% carboplatin was released from particles. The trapped particles in lungs were significantly reduced, when compared with previous alginate-hyaluronic particles.

We aimed to image and treat the lung metastases of MM48 breast cancer cells in C3He/N mice by using microcapsules that release liposome-protamine-hyaluronic acid nanoparticles (LPH-NP) in response to two radiation sessions. In session one, computed tomography (CT)-detectable microcapsules containing P-selectin and 5% iopamiron were mixed with a 1 mL solution of 4% alginate, 3% hyaluronate, 1 mg ascorbate, and 1 μg/mL P-selectin. This was sprayed into 0.5 mmol/L FeCl2 containing 1 μg/mL VEGFR-1/2 antibodies (Abs). The mice were intravenously injected with microcapsules, which released the P-selectin, and then a CT study was performed to detect lung metastases. After the CT evaluation, the mice received 10 or 20 Gy (140 keV) of X-ray radiation to the lungs. In session two, carboplatin-LPH-NP was released into the tumor, which was treated with another dose of radiation. To do this, carboplatin LPH-NP was mixed with the cocktail used in session one and sprayed into 0.5 mmol/L FeCl2 containing 1 μg/mL anti-P-selectin Abs. Microcapsules (1 × 1010) were injected intravenously and then interacted with the P-selectin. The released carboplatin LPH-NP attacked lung metastases synergistically with radiation, which resulted in further reduction of the lung metastases.

The effects of spraying mineral water onto agricultural crops on their yields and mineral contents were examined. We sprayed a solution containing a large quantity of essential minerals onto the leaves of various agricultural crops every other week for a few months. The mineral concentrations in the agricultural crops and of the sprayed solution were measured by particle induced X-ray emission (PIXE). It was found that the effect of spraying mineral water on the crops was remarkable, especially for rice and soybeans, for which the yields became nearly three times higher and the concentrations of many essential minerals increased in their stems and leaves. However, no clear increase in the mineral contents was observed for polished rice. In addition, not all of the farm products showed positive effects. This indicates that an effective method and timing of spraying mineral water should be examined depending on the conditions of each individual agricultural crop.

The purpose of our research is to identify causative metals by using particle-induced X-ray emission (PIXE) method to directly analyze trace elements in the oral mucosa with oral lichen planus (OLP). Subjects were 72 patients with OLP, and the patients are 25 men and 47 women, with a mean age of 60.1 years (OLP group). The control is elemental analysis data by PIXE method of 100 cases of the oral mucosa of healthy persons (control group). Seventeen essential elements and 12 contaminating elements were detected from the oral mucosa of the OLP and control groups. As to appearance ratio of elements in oral mucosa, among the contaminating elements, levels of Al, Ga, Sb, Hg and Pb were significantly lower, whereas Au and Y were significantly higher in the OLP group than in the control group. About concentration of elements in oral mucosa, the contaminating elements in the oral mucosa of the OLP group had a lower appearance ratio than in the control but each of the contaminating elements was more abundant. Among 25 subjects in the OLP group and seven in the control group, serum, oral mucosa and saliva were collected from the same individual. Abundance in serum and saliva varied depending on the element, but in general, a tendency was seen for contaminating elements to be more abundant in saliva than in serum and for essential elements to be more abundant in serum than in saliva.

In this paper, methods of quantitative elemental analysis of very small quantity of cultured cells were developed. First of all, an internal-standard method for the solution containing cells whose density is more than 1 × 106 cells/mL was established and then a standard-free method for cultured cells was developed. It was confirmed that the method allows us to quantitatively analyze more than 25 elements in the samples containing only 20,000 cells. Also, the methods for removing cultured cells from a flask were examined in order to improve accuracy and sensitivity of analysis since the use of trypsin and PBS sometimes brings a large amount of sodium, phosphorus and potassium, which have direct effect upon accuracy of analysis based on the standard-free method. It was found that the method of removing cells with a scraper without using trypsin and PBS is the best manner. Also, the effects of using thinner backing materials were examined in order to improve sensitivity of analyses. It is expected that accurate analysis of samples containing nearly two thousand cells is possible on the basis of the standard-free method when using a thinner backing material.

We report an elemental analysis of murine solid tumors treated with cisplatin-incorporated polymeric micelles (NC-6004) to evaluate the concentration of the drug in the tumor tissue using conventional particle-induced X-ray emission (PIXE) analysis, as well as the spatial distribution in the tumor section using sub-millimeter PIXE analysis. The results reveal that the platinum concentration in the tumor treated with NC-6004 was higher than in that treated with cisplatin, whereas no significant difference was found in platinum concentration between NC-6004 and cisplatin samples in the normal tissue. This suggests that NC-6004 can both provide therapeutic efficacy and reduce the side effects caused by conventional treatment using cisplatin. These results show that PIXE analysis is a powerful tool for research into drug delivery systems.

Since the Great East Japan Earthquake on 11 March 2011, we have seen a rapid increase of requests for soil analysis by PIXE. In the Nishina Memorial Cyclotron Center (NMCC), a powdered internal standard method with palladium on carbon powder has been adopted for soil sample preparation. However, the method can be heavily laborious when many samples need to be handled in a limited time. Here, we report an alternative to the method which takes a standard in the liquid form with a few drops of acetone to be homogenized with soil sample in an agate mortar. The applicability of the moist method was examined using some standard reference materials by comparing the analyzed results with those from the conventional method and with the certified values. The results were generally satisfactory, although further examination is needed to improve the accuracy and reliability of the new method.

The effects of the vascular disrupting agent AVE8062 on tumor and normal tissue samples were investigated by particle-induced X-ray emission (PIXE) analysis using quantum dots (QDs). We investigated fibrosarcoma tumors in mice, and used kidney tissue as a control. Non-targeted QDs were used to characterize the tissue regions where blood flow is interrupted by AVE8062. We found that the concentration of the QDs in the tumors and kidneys exposed to AVE8062 was lower than that of the control group. Sub-millimeter PIXE analysis (with a beam size of 0.5 [Formula: see text] 0.5 mm2) was used to investigate the spatial distribution of QDs in the tissue samples. We found that the QDs were accumulated in localized regions of the kidney section of the AVE8062-treated group whereas the QDs were uniformly distributed in the control kidney. This suggests that AVE8062 caused blood flow interruption not only in the tumor samples but also in the normal blood vessels in the kidneys.

In this paper, we used microcapsules releasing liposome-protamine-hyaluronic acid nanoparticles (LPH-NP) with/without carboplatin in response to radiation to image and treat MM48 breast cancer in C3He/N mice in two radiation sessions. The micro-particle-induced X-ray emission (PIXE) camera and quantitative PIXE were used to image and measure the release of nanoparticles from the microcapsules. In session one, iopamiron and computed tomography (CT)-detectable microcapsules containing P-selectin and LPH-NP were mixed with a solution of alginate, hyaluronate, ascorbate, and P-selectin. This solution was sprayed into an FeCl2 solution containing VEGFR-1/2 antibodies (Abs). The microcapsules obtained were injected intravenously into mice, and after 9 h, the mice were exposed to 10 or 20 Gy (140 keV) of X-ray radiation. Anti-VEGFR-1/VEGFR-2 microcapsules accumulated around tumors and released P-selectin and the iopamiron-labeled LPH-NP in response to the first radiation. The iopamiron-containing nanoparticles were detected by CT, allowing detection of MM48 tumors by CT. In the second session, the microcapsules released LPH-NH that delivered carboplatin into the tumor cells. This treatment had a significant antitumor effect [Formula: see text]. The micro-PIXE camera and quantitative PIXE successfully imaged and measured the release of contents from microcapsules. Our results indicate that targeted nanoparticles allow for accurate detection and treatment of tumors.

The concentrations of alkali elements in Japanese green tea leaves were evaluated using particle-induced X-ray emission (PIXE) analysis combined with an internal standard method to investigate the elution of radioactive cesium into green tea using potassium and rubidium. The concentrations of potassium and rubidium of used tea leaf samples were lower than those of unused samples, whereas no significant differences in the concentrations of the other elements were observed between them. In addition, we found a similarity in the relative concentrations between potassium and rubidium although the other elements showed different aspects. These results suggest that it is possible to investigate the elution of radioactive cesium into green tea using potassium and rubidium as substitutes of cesium.

The spatial distributions of potassium and rubidium in Lentinula edodes mushrooms contaminated with radioactive cesium were measured using particle-induced X-ray emission (PIXE) analysis by a beam scanning technique with a submillimeter sized proton beam to study relationships in elemental concentration in the mushrooms between radioactive cesium and other alkali elements. The results of PIXE analysis were compared with the spatial distribution of radioactive cesium in the samples measured by an autoradiographic method. Radioactive cesium was not uniformly distributed and strongly concentrated in the peripheral region of pileus of the mushroom while the elemental maps evaluated from PIXE analysis showed that potassium and rubidium are highly accumulated in the same area as radioactive cesium. The present results suggest a common mechanism of the accumulation of alkali elements including radioactive cesium in Lentinula edodes mushrooms.

Particle-induced X-ray emission (PIXE) analysis of Lentinula edodes mushrooms (Shiitake mushrooms) contaminated with radioactive cesium was performed to study relationships between concentrations of alkali elements in the shiitake mushroom samples and their radioactive cesium levels. The shiitake mushrooms were cultivated using radiocontaminated hard wood logs due to the nuclear power plant accident in Fukushima. The significant localization of radioactive cesium was found in the pileus region of the shiitake mushroom from autoradiographic observation. The concentrations of alkali elements in the shiitake sample were measured by PIXE analysis. The PIXE analysis has shown that the concentrations and transfer coefficients of potassium and rubidium in the pileus are much higher than the other parts of the shiitake sample as is the case of radioactive cesium. It is suggested that radioactive cesium is transferred into shiitake mushrooms in a manner similar to potassium and rubidium. The results of this work have shown the possibility to be able to use rubidium as an elemental tracer for radioactive cesium.

National Institute of Advanced Industrial Science and Technology is working for the Global Alliance to Eliminate Lead Paint (GAELP) of the United Nations Environment Program (UNEP), under the cooperation of Iwate Medical University Cyclotron Center and Nishina Memorial Cyclotron Center of Japan Radioisotope Association. In order to demonstrate how the PIXE is useful to monitor lead in human body, hair samples were collected from local communities and analyzed by the PIXE at the University together with the control of office workers. The analysis showed a clear anomaly of lead for factory workers. It is recommended that the PIXE be added as one of the instruments to assist UNEP's lead and other heavy metal studies.

We have been developing microcapsules that release anticancer drugs in response to radiation with an aim of targeted delivery and increasing the efficacy of anticancer drugs by a combination of these drugs with radiation. The aim of this study was to micronize microcapsules by adding carbonated water to the core material of microcapsules, which releases the anticancer drugs in response to radiation. The core material of microcapsules was prepared by mixing 0.1 g of hyaluronic acid and 0.2 g of alginate into 5 mL of carbonated water. The mixture was sprayed onto a 0.3 mmoL/L solution of calcium chloride (CaCl2) and ferrous chloride (FeCl2) using an ultrasound disintegrator. The vibration of the ultrasound disintegrator generated microbubbles in the carbonated water, which micronized the microcapsules. Intravenous injection of the micronized microcapsules to tumor-bearing mice showed that the micronized microcapsules passed more efficiently through the capillaries of lungs or kidneys, which resulted in increased delivery of microcapsules to the tumors and increased the anticancer effect.

The aim of this study was to determine whether oxygen-releasing microcapsules could be used to sensitize cancer cells to kill by radiation. The microcapsules were generated by spraying a mixture of 0.1% alginate and hyaluronic acid into a 0.3 mmol/l solution of CaCl2 and FeCl2. These were then subcutaneously injected around a MM48 tumor (a cell line derived from human breast cancer) in the left hind legs of C3H/HeN mice, and tumors were dosed with 60Co γ-ray radiation. We showed that the oxygen released from the microcapsules enhanced the anti-tumor effect of radiation treatment via the generation of oxygen radicals.

The aim of this study was to evaluate the reliability of direct determination of trace and major element concentrations in plasma samples from wild (six hawksbill, nine green, and nine loggerhead) and captive sea turtles (25 howksbill, five green, and three loggerhead) in Okinawa, Japan. The particle induced X-ray emission method allowed detection of 23 trace and major elements (Al, As, Br, Ca, Cl, Cr, Cu, Fe, Hg, K, Mg, Mn, Mo, Ni, P, Pb, S, Se, Si, Sr, Ti, Y, and Zn). The wild sea turtles were found to have high concentrations of As and Pb in plasma compared with captive, but there were no significant changes in the Al and Hg concentrations. Loggerhead sea turtles were found to have significantly higher accumulation of As and Pb in plasma in comparison to other species. These findings may be useful when adjusting environmental and species-related factors in severely polluted marine ecosystems. Our results indicate that measuring the plasma As and Pb concentrations in wild sea turtles might be of help to assess the level of pollution in marine ecosystems, keeping in mind that loggerhead sea turtles had been shown to have higher levels of As and Pb in plasma.

The aim of this study was to evaluate the reliability and effectiveness of direct determination of trace and major element concentrations in bronchoalveolar lavage fluid samples from Holstein calves with Mycoplasma bronchopneumonia (n = 21) and healthy controls (n = 20). The samples were obtained during bronchoscopy using a standard examination method. A total of 18 elements (aluminum, bromine, calcium, chlorine, chromium, copper, iron, potassium, magnesium, manganese, molybdenum, nickel, phosphorous, sulfur, silicon, strontium, titanium, and zinc) were detected by particle-induced X-ray emission. The average bromine, iron, potassium, magnesium, and phosphorous concentrations were higher in calves with bronchopneumonia than in controls (p < 0.05). They were found to have higher amounts of calcium and zinc, and a higher zinc–copper ratio than that in healthy calves (p < 0.001). Based on the receiver operating characteristics curves, we propose a diagnostic cutoff point for zinc–copper ratio for identification of Mycoplasma pneumonia of 8.676. Our results indicate that assessment of the elemental composition of broncholaveolar lavage fluid is a promising diagnostic tool for Mycoplasma bronchopneumonia.

NABESHIMA-DANTSU is the name of the first Japanese-made carpets which have been produced in the Nabeshima domain (Saga Prefecture) since the later Edo period. The NABESHIMA-DANTSU carpets have been woven from one kind of cotton, and have been dyed with various dyes and color fixatives. We analyzed pieces of the NABESHIMA-DANTSU carpets stored in the Saga Prefectural Museum and the Saga Prefectural Art Museum, by using PIXE method in order to detect dyeing methods used in them. We also analyzed dyes, color fixatives and cotton used in the traditional Japanese dyeing method. From the NABESHIMA-DANTSU carpets, small amounts of dyed and non-dyed samples were picked up and were analyzed by in-air PIXE system at Tohoku University. It was found that Fe and Cu are related to the parts dyed orange, and Al is related to the parts dyed green. The analysis of cotton dyed by the traditional Japanese method shows the similar results. It means that both colors in the NABESHIMA-DANTSU carpets were dyed by the traditional Japanese method which uses natural dyes. From literature documentation, it is considered that synthetic dyes were mainly used during the Taisho era. The present result shows that natural dyes might have been used in the Taisho era. In this research the PIXE method has proved to be very effective for the analysis of dyeing methods.

The tidelands (tidal flats) of the seaside district of Tohoku, Japan, which play an important role in maintaining the diversity of the marine ecosystem, were almost completely destroyed by the massive tsunami that occurred on March 11, 2011. The tsunami also brought large quantities of contaminated sludge from the bottom of the sea to the coastal lands including the tidelands. In this study, we collected sludge samples from three tidelands: the Tsugaruishi estuary tideland (Iwate pref.), the Orikasa estuary tideland (Iwate pref.), and the Gamou tideland (Miyagi pref.). We then analyzed the samples using PIXE in accordance with a powdered-internal-standard method that we developed. In order to investigate the effects of the contaminated sludge on the ecosystem, we gathered and analyzed various kinds of wild plants and seaweed. We found that the tidelands are contaminated with heavy elements, such as arsenic, lead, zirconium, and barium, although the contamination is less serious in the vicinity of the beach.

A gigantic tsunami following Tohoku-Earthquake Disaster brought a large amount of sludge, which originated from the sediments pilling upon the bottom of the sea to the residential areas. As it is anticipated that the sludge contains a large amount of heavy toxic elements, its influence on the health of the suffered people will become a problem. In the present study, 72 sludge samples were taken from the stricken areas by the tsunami over the wide area; (Aomori, Iwate and Miyagi prefectures). These samples were treated on the basis of a powdered-internal-standard method and analyzed by means of PIXE with a specially-designed absorber. It was found that the sludge contains much amount of heavy elements such as arsenic, lead, zirconium, barium etc. in comparison with those in soils collected in the inland district of Iwate prefecture. Furthermore, 16 plant samples were gathered in the estuary area, on which the sludge deposited, and analyzed in order to evaluate the effect of the sludge on the ecosystem. These results were compared with those for 45 plant samples collected in the inland district of Iwate, Miyagi and Fukushima prefectures. It was found that these plants contain lager amount of heavy elements in comparison with those in the inland plants.

The aim of this study was to evaluate the relationships between carapace parameters as indicators of age and plasma elements in 25 captive hawksbill sea turtles. Particle-induced X-ray emission allowed detection of 23 trace and major elements. There were significant but weak correlations between the virtual carapace surface area and plasma bromide (r = -0.552, P

Platinum concentration in a murine solid tumor treated with proton therapy combined with the platinum-based chemotherapeutic agent cisplatin [cis-diamminedichloro-platinum(II) (CDDP)] was investigated with conventional and submilli-PIXE (particle-induced X-ray emission) analyses. An enhanced therapeutic effect on tumor growth was observed in NFSa fibrosarcoma tumors in mice when proton therapy with a single dose of 30 Gy and CDDP treatment (10 mg/kg) were combined. The conventional PIXE analysis based on an internal standard method showed that the platinum concentration was 2.6 ± 0.3 µg/g for the tumor samples excised from the mice 6 h after the CDDP administration. The submilli-PIXE analysis of the tumor sections showed that spatial distribution of CDDP may be more or less uniform in the tumor. Copyright © 2011 John Wiley & Sons, Ltd.

Particle-induced X-ray emission (PIXE) analysis of Lentinula edodes (Shiitake) mushrooms contaminated with radioactive cesium was performed to study relationships between concentrations of principal elements of shiitake mushrooms and their radioactive cesium levels. After the Fukushima nuclear disaster caused by the huge tsunami on March 11, 2011, we collected five shiitake samples in Marumori town, Miyagi Prefecture, on April 21, 2011. The mean radioactive level of the samples was 228 Bq/kg (the sum of 134 Cs and 137 Cs ). The preliminary result of PIXE analysis using an internal standard method has demonstrated that shiitake mushrooms significantly collect rubidium as well as potassium. It is suggested that radioactive cesium is accumulated in shiitake just like rubidium during the course of potassium uptake.

Microencapsulated anti-RLIP76 was tested in vivo using C 3 He / J mice to determine the increasing of antitumor effects by chemotherapeutic agent efflux inhibition during chemoradiotherapy. Microcapsules were produced by spraying a mixture of 3.0% hyaluronic acid, 2.0% alginate, 3.0% H 2 O 2, and 0.3 mmol carboplatin onto a mixture of 0.3 mol FeCl 2 and 0.15 mol CaCl 2. Microcapsules were subcutaneously injected into MM46 tumors previously inoculated into the left hind legs of C 3 He / J mice. Subsequent radiotherapy consisted of tumor irradiation with 10 Gy or 20 Gy 60 Co . The antitumor effects of microcapsules were tested by measuring tumor size and monitoring tumor growth. Three types of adverse effects were considered: fuzzy hair, loss of body weight, and mortality. Carboplatin levels were monitored using particle-induced X-ray emission (PIXE) and a micro-PIXE camera. Anti-RLIP76 inhibited the efflux of carboplatin from tumor tissue, which led to an increase in the concentration of carboplatin. Higher carboplatin concentration significantly increased the combined antitumor effect of radiation and chemotherapy. A significant decrease in adverse effects was also observed with microencapsulated anti-RLIP76.

Spatial distributions of principal elements in a NFSa fibrosarcoma tumor treated with a vascular disruption agent, AVE8062 (a derivative of combretastatin A-4) at a single dose of 40 mg/kg were evaluated on the basis of particle-induced X-ray emission (PIXE) analysis using a submillimeter-sized proton beam. We found not only potassium and sulfur concentrations at the periphery of the treated tumor but also a ring-shaped calcium distribution in the area between the inner necrotic region and the periphery. These observations were supported by results for quantitative evaluation of elemental concentrations in the tumor samples obtained from conventional PIXE analysis based on the internal standard method. It is suggested that the potassium and sulfur concentrations are related to residual viable cells at the tumor periphery which are commonly observed in VDA treatments whereas the ring of calcium concentration just inside the tumor periphery is possibly derived from hypoxia-induced response.

Concentrations of the chemotherapeutic agent, cis-diamminedichloro-platinum(II) (CDDP) in NFSa fibrosarcoma tumors were investigated using a conventional PIXE analysis on the basis of an internal standard method to study enhancement of antitumor effects caused by proton therapy combined with CDDP treatment. Results of the PIXE analysis showed that platinum concentration of the tumors treated with CDDP at a single dose of 10 mg/kg was 2.0±0.1 µg/g and persisted at the level at least 6 hours after the administration. The present study demonstrated that the presence of CDDP in the tumor caused an enhanced therapeutic effect on tumor growth delay when CDDP treatment was combined with post proton-irradiation in comparison with CDDP treatment alone or proton therapy alone.

We established and reported two years ago the original methods for evaluating daily changes of elemental concentration in a body by means of a standard-free method for powdered beard samples daily taken with electric shaver. It was found that the method is quite useful for investigating short- and long-term changes of elemental concentration in a body. However, the method for beard analysis is applicable only to men. In order to estimate daily changes of elemental concentration in a body for women and children, a new method which allows us to quantitatively analyze hair samples cut into 1 mm pieces has been developed and applied to three long hair samples taken from three persons. It is found that the method enables us to estimate both long- and short-term changes in elemental concentration in a body as well as beard analysis. It is found that sulfur keeps almost constant over a long period, and arsenic shows very rapid changes with a few days' period, while mercury shows only long-term changes with the period of a few months. These behaviors are almost the same as those observed in beard analyses. On the other hand, bromine shows a certain seasonal changes; its concentration shows a certain trend of increasing in summer and decreasing in winter. Lead and calcium show very long-term changes, and the behavior of strontium is quite similar to that of calcium. The method is expected to give us information about history of changes in elemental concentration in a human body over a few or more years. It is expected that the behavior of arsenic showing rapid elevation within a few days can be explained as a response to intakes of arsenic-rich foods. It is expected that the method gives us a clue to the identification of the main pathways of human exposure to certain toxic elements.

The standard-free method developed by ourselves 13 years ago has been widely applied to quantitative analyses of hairs such as head hair taken from human and body hair taken from companion and domestic animals. In the present work, the standard-free method for feather and down samples taken from wild birds such as swan, waxwing, osprey, heron and crow is developed. It is found that the standard-free method developed for human hairs can be successfully applied to feather samples without essential modification since the main constituents of feather are almost the same as those for human and animal hairs and, consequently, the shape of continuous X-rays is also the same. Accuracy and sensitivity of the present method were examined by comparing the results with those obtained by an internal-standard method combined with a chemical-ashing method. The method allows us to quantitatively analyze untreated feather samples of very small quantities and to prepare the target without complicated preparation technique. It is expected that the method will become a powerful tool for the studies not only on the mode of life of wild birds but also on environmental contamination by toxic elements.

The aim of this study was to investigate the relationships between the bronchopneumonia and mean concentrations of those trace elements in bronchoalveolar lavage fluid (BALF). Twenty-nine dogs were included this study (17 healthy dogs and 12 dogs with respiratory disease). Each BALF sample had been obtained during bronchoscope examination by use of a standardized method. The concentrations of Al, Br, Ca, Cu, Fe, K, Ni, P, Si, Sr and Zn in BALF were measured by the particle-induced X-ray emission method. We found no relationship between the bronchopneumonia and the levels of elements in the BALF, except Ca, P and Zn. The dogs with respiratory disease were found to have a large amount of Ca and Zn, and a high Ca/P and Zn/Cu ratios in BALF compared to those without respiratory disease.

Serum trace elements were analyzed by PIXE method in a patient with acute aortic dissection during the supportive process by a Nutrition support team (NST). The patient was a 53-year old male who suffered from acute aortic dissection on March 1, 2007. He received emergent Bentall operation and bow pars total displacement. Since he suffered from diarrhea as a result of hypoalbuminemia and bowel dysfunction, enteral nutrition was not sufficient to maintain adequate intake. Therefore, we also used parenteral nutrition until the 97th disease day. Afterwards, the patient managed only with enteral nutrition. We measured serum trace elements during these periods. Serum trace elements such as Fe , Zn and Se were preserved within normal ranges. On the other hand, Cu gradually decreased until the 54th disease day (44 μg/l) and stayed in the lower levels around the detection limit until the 109th disease day. Thereafter, Cu slightly increased and reached 117 μg/l on the 131st disease day (reference range of serum Cu in adult males: 700~1,300 μ g/l ). It was suggested that the serum levels of these trace elements might reflect the nutritional stages of the patient and could be useful as clinical markers for nutritional therapies.

Elemental concentrations in Chinese peanuts have been analyzed and compared with those in Japanese peanuts by means of a PIXE (Particle Induced X-ray Emission) technique with an internal standard method to investigate traces of residual agricultural chemicals or toxic elements in them because frequent detection of excessive agrochemical residues in food imported from China has posed serious health concerns to Japanese people. We prepared the samples by separating the peanut seed into two cotyledons (seed leaves) and an embryo. Significant differences in elemental concentrations between Chinese and Japanese peanuts have not been observed as far as the peanut seeds used in the present measurement are concerned. The concentrations of the several elements in the embryo are higher than those in the cotyledon.

Biomineralization has two types, biologically induced mineralization (BIM) and biologically controlled mineralization (BCM). Shark teeth is a typical representative of BCM. We have measured concentrations of fluorine and multi elements in shark teeth collected in the south of Japan. As a result, it was confirmed that the sample preparation method, which was established for the biological samples, is applicable to the shark teeth samples and the elemental concentration was obtained in good accuracy and reproducibility. Moreover, we clarified that the shark teeth is composed of Fluorapatite by the combination with X-ray Diffraction. Fluorine concentration is found to be 5500 µg/g in the shark teeth. We have 100 samples of Shark teeth and are planning on reporting the findings of a study with larger samples in the near future.

The aim of this study was to investigate the relationships between the mean concentrations of trace elements and the severity of the second-degree atrioventricular (AV) block in the mane hair of horses. Electrocardiographs of horses were continually recorded for 6 h using a holter cardiac monitor to determine dropped ventricular beats (DVBs) which can be used as an indicator of the severity of the AV block. Mane hair Ca, Cu, Mg, and Zn concentrations were measured by the particle-induced X-ray emission method. The Zn/Cu ratio and Ca concentration in mane hair were significantly and positively correlated with the hourly DVBs in horse with a second-degree AV block (p0.01, r2=0.485; p0.05, r2=0.351, respectively). Proposed diagnostic cutoff points for hair Ca concentration and Zn/Cu ratio based on receiver operating characteristics curves analysis in detecting second-degree AV block were set at 1536 microg/g and 26.0, respectively. Those results with horse hair suggest that the evaluation of the Ca, Cu, Mg, and Zn status in mane hair by this method is strongly related to the severity of second-degree AV block and might predict the susceptibility of an individual much before the development of the symptom.

A database of PIXE data, which have been accumulated at NMCC, has been constructed. In order to fill up the database, data are newly obtained as many as possible for the kind of samples whose number is small. In addition, the data for different measuring conditions are obtained for several samples. As the number of γ-ray spectrum obtained with a HPGe detector for the purpose of analyzing light elements such as fluorine, is overwhelmingly small in comparison with that of usual PIXE spectra, γ-ray spectrum and elemental concentration of fluorine are obtained as many as possible for food, environmental and hair samples. In addition, the data taken with an in-air PIXE system have been obtained for various samples. As a result, the database involving contents over various research fields is constructed, and it is expected to be useful for researches who make use of analytical techniques. It is expected that this work will give a start to many researchers to participate in the database and to make calibration with each other in order to establish reliable analytical techniques. Moreover, the final goal of the database is to establish the control concentration values for typical samples. As the first step of establishing the control values, average elemental concentration and its standard deviations in hair samples taken from 405 healthy Japanese are obtained and tabulated according to their sex and age.