Interstellar

Earth is constantly bombarded with extraterrestrial dust containing invaluable information about extraterrestrial processes, such as structure formation by stellar explosions or nucleosynthesis, which could be traced back by long-lived radionuclides. Here, we report the very first detection of a recent ^{60}Fe influx onto Earth by analyzing 500 kg of snow from Antarctica by accelerator mass spectrometry. By the measurement of the cosmogenically produced radionuclide ^{53}Mn, an atomic ratio of ^{60}Fe/^{53}Mn=0.017 was found, significantly above cosmogenic production. After elimination of possible terrestrial sources, such as global fallout, the excess of ^{60}Fe could only be attributed to interstellar ^{60}Fe which might originate from the solar neighborhood.

Ultratrace Determination of 99Tc in Small Natural Water Samples by Accelerator Mass Spectrometry with the Gas-Filled Analyzing Magnet System.

In the frame of studies on the safe disposal of nuclear waste, there is a great interest for understanding the migration behavior of 99Tc. 99Tc originating from nuclear energy production and global fallout shows environmental levels down to 107 atoms/g of soil (∼2 fg/g). Extremely low concentrations are also expected in groundwater after diffusion of 99Tc through the bentonite constituting the technical barrier for nuclear waste disposal. The main limitation to the sensitivity of the mass spectrometric analysis of 99Tc is the background of its stable isobar 99Ru. For ultratrace analysis, the Accelerator Mass Spectrometry (AMS) setup of the Technical University of Munich using a Gas-Filled Analyzing Magnet System (GAMS) and a 14 MV Tandem accelerator is greatly effective in suppressing this interference. In the present study, the GAMS setup is used for the analysis of 99Tc in samples of the seawater reference material IAEA-443, a peat bog lake, and groundwater from an experiment of in situ diffusion through bentonite in the controlled zone of the Grimsel Test Site (GTS) within the Colloid Formation and Migration (CFM) project. With an adapted chemical preparation procedure, measurements of 99Tc concentrations at the fg/g levels with a sensitivity down to 0.5 fg are accomplished in notably small natural water samples. The access to these low concentration levels allows for the long-term monitoring of in situ tracer tests over several years and for the determination of environmental levels of 99Tc in small samples.

Assessment of 53Mn deposition on Earth via accelerator mass spectrometry.

The 53Mn flux onto Earth is a quantity relevant for different extraterrestrial and astrophysical questions. It is a proxy for related fluxes, such as supernova-produced material or interplanetary dust particles. In this work, we performed a first attempt to assess the 53Mn flux by measuring the 53Mn/10Be isotopic ratio in a 1400 L sample of molten Antarctic snow by AMS (Accelerator Mass Spectrometry). Using the 10Be production rate in the atmosphere, an upper limit of 5.5 × 103 atoms cm-2 yr-1 was estimated for the deposition of extraterrestrial 53Mn. This result is compatible with one of the two discrepant values existing in the literature.

Plutonium Isotopes (239-241Pu) Dissolved in Pacific Ocean Waters Detected by Accelerator Mass Spectrometry: No Effects of the Fukushima Accident Observed.

The concentration of plutonium (Pu) and the isotopic ratios of 240Pu to 239Pu and 241Pu to 239Pu were determined by accelerator mass spectrometry (AMS) in Pacific Ocean water samples (20 L each) collected in late 2012. The isotopic Pu ratios are important indicators of different contamination sources and were used to identify a possible release of Pu into the ocean by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. In particular, 241Pu is a well-suited indicator for a recent entry of Pu because 241Pu from fallout of nuclear weapon testings has already significantly decayed. A total of 10 ocean water samples were prepared at the Radiochemie München of the TUM and analyzed at the Vienna Environmental Research Laboratory (VERA). Several samples showed a slightly elevated 240Pu/239Pu ratio of up to 0.22 ± 0.02 compared to global fallout (240Pu/239Pu = 0.180 ± 0.007), whereas all measured 241Pu-to-239Pu ratios were consistent with nuclear weapon fallout (241Pu/239Pu < 2.4 × 10-3), which means that no impact from the Fukushima accident was detected. From the average 241Pu-to-239Pu ratio of 8-2+3 ×10-4 at a sampling station located at a distance of 39.6 km to FDNPP, the 1-σ upper limit for the FDNPP contribution to the 239Pu inventory in the water column was estimated to be 0.2%. Pu, with the signature of weapon-grade Pu was found in a single sample collected around 770 km off the west coast of the United States.

Time-resolved 2-million-year-old supernova activity discovered in Earth's microfossil record.

Massive stars ([Formula: see text]), which terminate their evolution as core-collapse supernovae, are theoretically predicted to eject [Formula: see text] of the radioisotope (60)Fe (half-life 2.61 Ma). If such an event occurs sufficiently close to our solar system, traces of the supernova debris could be deposited on Earth. Herein, we report a time-resolved (60)Fe signal residing, at least partially, in a biogenic reservoir. Using accelerator mass spectrometry, this signal was found through the direct detection of live (60)Fe atoms contained within secondary iron oxides, among which are magnetofossils, the fossilized chains of magnetite crystals produced by magnetotactic bacteria. The magnetofossils were chemically extracted from two Pacific Ocean sediment drill cores. Our results show that the (60)Fe signal onset occurs around 2.6 Ma to 2.8 Ma, near the lower Pleistocene boundary, terminates around 1.7 Ma, and peaks at about 2.2 Ma.

Separation of no-carrier-added 52Mn from bulk chromium: a simulation study for accelerator mass spectrometry measurement of 53Mn.

53Mn radionuclide (T(1/2) = 3.7 x 10(6) y) is produced through the interaction of cosmic rays. Measurements of concentrations of 53Mn in rocks might help to understand Earth surface processes that occurred in time periods not accessible with other cosmogenic nuclides. Only accelerator mass spectrometry (AMS) can determine such ultratrace levels of 53Mn. The main interference in the detection of 53Mn by AMS is its stable isobar 53Cr, which is roughly approximately 10(12) times more abundant in nature. A prerequisite of any AMS measurement of 53Mn in geological samples is therefore chromium separation by an efficient chemistry. Thus, we have developed a method for the separation of chromium and manganese by using a radiometric simulation. The separation procedure was monitored by 51Cr (T(1/2) = 27.70 d) and 52Mn (T(1/2) = 5.59 d) as the corresponding radiotracers for chromium and manganese, respectively. The separation studies were performed by a liquid-liquid extraction technique using trioctylamine (TOA) diluted in cyclohexane. A high separation factor (approximately 16 000) for Mn and Cr can be obtained at optimal conditions of 0.8 M TOA and 9 M HCl. The developed method has been found equally applicable for real geological samples such as manganese crusts, lava, and sediment samples. Therefore, the method offers an important tool to improve 53Mn measurements by AMS.

Separation of samarium and neodymium: a prerequisite for getting signals from nuclear synthesis.

(146)Sm (T(1/2) = 10(8) y) is a long-lived radionuclide which has been produced in significant amounts during burning in a supernova (SN). Detection of this SN produced long-lived radionuclide on Earth may be helpful for getting information on nuclear synthesis at the time of our solar system's formation. Only accelerator mass spectrometry (AMS) can determine such minute traces of (146)Sm still expected in the Earth's crust. However, the villain of (146)Sm measurement through AMS is its naturally occurring stable isobar (146)Nd which is a million times more abundant than the trace amount of (146)Sm. Therefore an efficient method for the separation of samarium and neodymium is required to measure (146)Sm through AMS. A simple liquid-liquid extraction (LLX) based method for separation of samarium and neodymium has been developed using radiometric simulation. Di-(2-ethylhexyl)phosphoric acid (HDEHP) has been used as the organic reagent. A very high separation factor ( approximately 10(6)) can be achieved when a solution containing samarium and neodymium is reduced by hydroxylamine hydrochloride followed by extraction with 0.1% HDEHP diluted in cyclohexane from 0.025 M HCl solution.

Separation of trace level hafnium from tungsten: a step toward solving an astronomical puzzle.

182Hf (T(1/2) = 9 x 10(6) y) is believed to be formed by pure r-process during a supernova explosion, and therefore, the search for minute traces of 182Hf in the earth's crust is of great interest. Only accelerator mass spectrometry (AMS) is well suited for detecting such low levels of 182Hf. But any attempt to measure 182Hf by AMS must ensure that the sample is free from its naturally occurring stable isobar 182W. A simple method for separation of tungsten and hafnium has been developed using radiometric simulation followed by checking the decontamination of tungsten from Hf in a synthetic sample by AMS. The separation studies were performed by a liquid-liquid extraction technique using tri-n-octylamine (TOA) as the organic reagent. It has been found that a very high separation factor (1.6 x 10(6)) can be achieved when 0.3 M TOA diluted in cyclohexane is used as the organic phase and 6 M HCl (in the presence of small amount of H2O2) is used as the aqueous phase.