R. Pöllänen

Characterization of radioactive particles using non-destructive alpha spectrometry.

Spherical particles with known properties were used to demonstrate and test a novel software package known as AASIFIT, which is able to unfold complex alpha spectra. A unique feature of the program is that it uses simulated peak shapes in the fitting process. The experimental reference particles in the testing were artificially produced U particles of diameter 1.4microm and a nuclear bomb particle with a twenty-fold greater diameter, mainly composed of U and Pu dioxides. AASIFIT was used to determine the density of the U particles. In addition, the activities of (239+240)Pu and (241)Am were determined for the nuclear bomb particle and compared to earlier determinations in the literature. The results of this investigation demonstrated that the software can be used to estimate the properties of particles emitting alpha radiation. However, the composition and geometry of the investigated particles need to be known with good accuracy for reliable estimates. Furthermore, uncertainties in the stopping power data, especially for U and Pu, may have an influence on the results obtained from the software.

Transport of radioactive particles from the Chernobyl accident

Abstract After the Chernobyl accident large and highly radioactive particles were found in several European countries. Particles > 20 μm in aerodynamic diameter were transported hundreds of kilometres from the plant, and they were sufficiently active (> 100 kBq) to cause acute health hazards. Here, a particle trajectory model is used to identify the areas of large particle fallout. Effective release height of the particles and atmospheric phenomena related to their transport are investigated by comparing particle findings with locations given by trajectory calculations. The calculations showed that in the Chernobyl accident either the maximum effective release height must have been considerably higher than previously reported (> 2000 m) or convective warm air currents may have lifted radioactive material upwards during transport. Large particles have been transported to other areas than small particles and gaseous species. The particulate nature of the release plume must be taken into account in dispersion and transport analyses. Air parcel trajectories alone are not necessarily sufficient for identifying the fallout area of radioactive material.

Radiation surveillance using an unmanned aerial vehicle.

Radiation surveillance equipment was mounted in a small unmanned aerial vehicle. The equipment consists of a commercial CsI detector for count rate measurement and a specially designed sampling unit for airborne radioactive particles. Field and flight tests were performed for the CsI detector in the area where (137)Cs fallout from the Chernobyl accident is 23-45 kBq m(-2). A 3-GBq (137)Cs point source could be detected at the altitude of 50 m using a flight speed of 70 km h(-1) and data acquisition interval of 1s. Respective response for (192)Ir point source is 1 GBq. During the flight, the detector reacts fast to ambient external dose rate rise of 0.1 microSv h(-1), which gives for the activity concentration of (131)I less than 1 kB qm(-3). Operation of the sampler equipped with different type of filters was investigated using wind-tunnel experiments and field tests with the aid of radon progeny. Air flow rate through the sampler is 0.2-0.7 m(3)h(-1) at a flight speed of 70 km h(-1) depending on the filter type in question. The tests showed that the sampler is able to collect airborne radioactive particles. Minimum detectable concentration for transuranium nuclides, such as (239)Pu, is of the order of 0.2 Bq m(-3) or less when alpha spectrometry with no radiochemical sample processing is used for activity determination immediately after the flight. When a gamma-ray spectrometer is used, minimum detectable concentrations for several fission products such as (137)Cs and (131)I are of the order of 1 Bq m(-3).

Advanced simulation code for alpha spectrometry

A Monte Carlo code, known as advanced alpha-spectrometric simulation (AASI), is developed for simulating energy spectra in alpha spectrometry. The code documented here is a comprehensive package where all the major processes affecting the spectrum are included. A unique feature of the code is its ability to take into account coincidences between the particles emitted from the source. Simulations and measurements highlight the importance of coincidences in high-resolution alpha spectrometry. To show the validity of the simulated results, comparisons with measurements and other simulation codes are presented.

Uranium and plutonium containing particles in a sea sediment sample from Thule, Greenland

Particles composed of radioactive materials and probably originating from US nuclear weapons were identified in sea sediment samples collected from Thule, Greenland, in 1997. The weapons were destroyed close to the Thule Air Base in 1968 in an aeroplane crash, which dispersed radioactive materials in the environment. The presence of particulate radioactive materials in the sediment samples was revealed by combining gamma-spectrometry and autoradiography. Isolation and separation of a radioactive particle from a bulk sample were performed using autoradiography, phosphor plate imaging and scanning electron microscopy. Using X-ray microanalysis as well as alpha and beta activity analysis, U and weapons-grade Pu were detected in the granular, brittle particle.

Determination of 239Pu/240Pu isotopic ratio by high-resolution alpha-particle spectrometry using the ADAM program

A novel analysis program to unfold alpha-particle energy spectra was introduced, demonstrated and validated using radiochemically processed test sources, which contained different amounts of (239)Pu and (240)Pu. A high-resolution alpha spectrometer was used for data acquisition. The software known as ADAM unfolds the spectra using nuclide-specific decay data as a constraint. The peaks can have different shapes and the software can also cope with the coincidences between alpha particles and electrons/photons. In the present paper, the (239)Pu/(240)Pu activity ratios from alpha spectrometry agreed, within the stated uncertainties, with the reference values. Number of counts in the (239,240)Pu peak group must be larger than 100 to obtain reliable values when using semiconductor detector of energy resolution FWHM=10.6 keV.

Design of an air sampler for a small unmanned aerial vehicle

In the aftermath of a nuclear accident or malevolent act, it is of paramount importance to have the capability to monitor airborne radioactive substances by collecting air samples. For potentially dangerous missions, the Radiation and Nuclear Safety Authority of Finland (STUK) has developed an air sampler to be used on a small unmanned aerial vehicle. When a Petrianov or Fluoropore filter is used in the sampler and the air velocity is 71 km h(-1), the air flow rate through the filter is 0.73 m(3) h(-1) or 0.23 m(3) h(-1), respectively. The present article introduces the developed air sampler using fluid dynamic simulations and wind tunnel data. The operation of the system was validated by collecting airborne radioactive aerosols from air.

Determination of 235 U, 239 Pu, 240 Pu, and 241 Am in a nuclear bomb particle using a position-sensitive α-γ coincidence technique

A nuclear bomb particle containing 1.6 ng of Pu was investigated nondestructively with a position-sensitive α detector and a broad-energy HPGe γ-ray detector. An event-mode data acquisition system was used to record the data. α-γ coincidence counting was shown to be well suited to nondestructive isotope ratio determination. Because of the very small background, the 51.6 keV γ rays of (239)Pu and the 45.2 keV γ rays of (240)Pu were identified, which enabled isotopic ratio calculations. In the present work, the (239)Pu/((239)Pu+(240)Pu) atom ratio was determined to be 0.950 ± 0.010. The uncertainties were much smaller than in the previous more conventional nondestructive studies on this particle. Obtained results are also in good agreement with the data from the destructive mass spectrometric studies obtained previously by other investigators.

Detection of fast neutrons from shielded nuclear materials using a semiconductor alpha detector.

The response of a semiconductor alpha detector to fast (>1 MeV) neutrons was investigated by using measurements and simulations. A polyethylene converter was placed in front of the detector to register recoil protons generated by elastic collisions between neutrons and hydrogen nuclei of the converter. The developed prototype equipment was tested with shielded radiation sources. The low background of the detector and insensitivity to high-energy gamma rays above 1 MeV are advantages when the detection of neutron-emitting nuclear materials is of importance. In the case of a (252)Cf neutron spectrum, the intrinsic efficiency of fast neutron detection was determined to be 2.5×10(-4), whereas three-fold greater efficiency was obtained for a (241)AmBe neutron spectrum.

Deconvolution of alpha spectra from hot particles

A computer code known as AASIFIT is developed to unfold complex alpha spectra. Peak shapes used in the fitting are obtained from the simulations. In addition to activities of the nuclides present in the sample, the code can provide source characterization. AASIFIT is applied for a nuclear bomb particle collected in Thule, Greenland. It is shown that direct alpha spectrometry provides more accurate activity estimate for 239+240Pu than gamma-ray spectrometry.