Radiometric Measurements of Environmental Radioactivity Beta Counting, Alpha and Gamma Spectrometry

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Downloaded from orbit.dtu.dk on: Jan 31, 2018 Radiometric Measurements of Environmental Radioactivity Beta Counting, Alpha and Gamma Spectrometry Nielsen, Sven Poul Publication date: 2013 Link back to DTU Orbit Citation (APA): Nielsen, S. P. (2013). Radiometric Measurements of Environmental Radioactivity: Beta Counting, Alpha and Gamma Spectrometry [Sound/Visual production (digital)]. NKS Workshop on Radioanalytical Chemistry, Roskilde, Denmark, 02/09/2013, http://www.nks.org/en/seminars/presentations/nksb_radioanalysis_workshop_2-6_september_2013.htm General rights Copyright and moral rights for the publications made accessible in the public portal are retained by the authors and/or other copyright owners and it is a condition of accessing publications that users recognise and abide by the legal requirements associated with these rights. Users may download and print one copy of any publication from the public portal for the purpose of private study or research. You may not further distribute the material or use it for any profit-making activity or commercial gain You may freely distribute the URL identifying the publication in the public portal If you believe that this document breaches copyright please contact us providing details, and we will remove access to the work immediately and investigate your claim.

Radiometric Measurements of Environmental Radioactivity Beta Counting, Alpha and Gamma Spectrometry Sven Nielsen

Early start at Risø Measurements of environmental radioactivity started at Risø in 1956 using Geiger-Müller equipment (e.g. Anton Electronic Laboratories, New York) Alpha/beta measurements using proportional counters from 1960 Gamma spectrometry (air filters) started in 1960 using a 4-inch NaI well detector and a 100- channel pulse height analyzer Gamma spectrometry using small Ge(Li) detectors (e.g. 2 cm 3 ) made at Risø started in 1965 with 1024 channel analyzers Alpha spectrometry using Si detectors and 256-ch MCAs from 1968 Commercial Ge(Li) detectors used from 1974, own production stopped 1966 Compton rejection setup

Risø Low-Level Beta GM Multicounter

Description Low-level gas-flow beta multicounter for simultaneous measurements of 5 samples. Incorporates 5 individual counter elements and a common guard counter Guard counter uses anticoincidence technique to reduce background from cosmic radiation by more than a factor 700 Aluminized Mylar window of thickness less than 1 mg/cm 2 Counter gas 99% Ar / 1% isobutane or propane Counter placed in 10-cm lead shield

Specifications and Applications Multicounters used for total beta counting of 90 Sr and 99 Tc Guard count rates typically about 2 cps Detector background count rates typically about 0.2 cpm Detector efficiencies checked monthly using reference sources, 36 Cl and 99 Tc Counting efficiencies about 58% for 90 Y sources mounted on steel cores and about 40% for 99 Tc sources on steel disks Detection limits for routine applications about 2 mbq for 90 Sr and 4 mbq for 99 Tc Results from spreadsheet calculations COUNTS PER MINUTE 1000 Bq/kg Ca 100 10 1 0.3 0.25 0.2 0.15 0.1 0.05 0 Multicounter 10 Background 0 0.5 1 1.5 2 2.5 3 3.5 DAYS Strontium-90 in Danes 1960 1970 1980 1990 2000 Year D1 D2 D3 D4 D5

Alpha Spectrometry

Risø Vacuum Chamber

Description 32 Si detectors Vacuum chambers made at Risø 20 mm diameter sources electrodeposited on stainless steel disks Counting times typically 3-7 days Detection limits 0.1-0.2 mbq Results from spreadsheet calculations Analyses of Po, U, Pu, Am, (Np)

Gamma Laboratory

Lead Shields

Ge Detector Specifications Risø id. Producer Year Efficiency Fwhm (kev) Other 1 Ortec 1986 38% 1.8 1.3 mm Al window 2 Ortec 1986 35% 1.8 1.3 mm Al window 3 Ortec 1986 33% 1.9 Low energy, 0.5 mm Be window 4 Ortec 1986 33% 1.9 Low energy, 0.5 mm Be window Low energy, Mg well, low 5 Canberra 1987 35%/180 cm³ 2.0 background 6 Canberra 1998 118 cm³ 1.8 Low energy, 0.5 mm carbon epoxy, low background 7 Canberra 2001 260 cm³ 2.3 Low energy, Al well, low background 414 PGT 1979 25% 1.8 Ge(Li) 423 PGT 1978 27% 2.0 Ge(Li) Low energy, 0.5 mm Be window, low 952 Ortec 1995 37% 1.8 background

Electronics

Sample Geometries 1-L Marinelli beaker (1 L) 210 ml cylindrical beaker (range 20-200 ml) 25 ml Petri dish (5, 10 and 15 ml) 10 ml vial (range 1-8 ml) 2 ml vial (range 0.2-2 ml)

Detector Efficiency and Energy Resolution Effeciency and energy resolution of detectors checked monthly with reference sources 241 Am, 137 Cs, 60 Co and 40 K Detector 423

Detector Gamma Background Ge detector background counts performed during prolonged holidays, i.e. Easter and Christmas Detector 423

Software for Gamma Spectrum Analysis Home made software, developed since 1970 s, implemented first in Algol programming language on main-frame computer, later in C on personal computer Peak search based on values of second derivative of smoothed spectrum Peak area calculation based on simple summation of smoothed spectrum counts over peak channels minus background, fitting of doublets Accuracy of peak-area calculation method compared with other procedures (1998) --------- Måling nr. 405486 --------- 1: Sample type: Milk 2: Date : 2009-Aug 3: Location : W-Jutland 3 6: Sample ID : 20090327 Res.el.vægt: 2.0000 kg dry 1: Detektor : 4, 4 2: Måleperiode: 20090812.1138,20090817.0847 3: Fyldning : -0.4000 4: Vægtfylde : 0.6100 5: Energikal. : 2.0606, 0.6687 6: Måletid : 421797 Spektrum: 4000 kanaler TOPAREAL fil A -> B, t = 1.5, max.eta = 40 % 41-5979 kan., delta = 2.5 kev br. fra kalib. w1: 5, w2: 13, udglat = 3 Isotoptabel indeholder 140 isotoper Milk from Videbæk august 2009 Spektrum nr. 405486, detektor 4, kalibrering 4 Kan: KeV: w:(w0) b: Bagg: Eta: cps*1000: Eta: Bq(100%) Vfk.: Bq(vf): 438761 510.6 7295.0 6( 6) 1.2 1.81 9.9-0.22 100.0 439( 7) 2.525.41 1.0 5.25 11.2 0.303 0.932 0.283 ( 3) 907 608.9 7( 7) 1.9 2.96 5.5-0.09 100.0 986 661.2 7( 7) 1.6 10.14 4.4 0.739 0.940 0.695 ( 4) 2180 1459.8 9( 9) 2.2 2.81 3.7 655.66 0.2 92.579 0.958 88.733 ( 6) 2634 1763.0 10(10) 2.9 0.87 9.6-0.13 100.0 3905 2613.4 13(13) 3.1 1.69 4.5 0.00 100.0 ----------------------- Sample output

Efficiency Calibration Calibrations based on measurements in standardized geometries of known activities of mixed radionuclide gamma-ray reference solutions and K 2 CO 3 standard, e.g. 241 Am, 109 Cd, 57 Co, 139 Ce, 51 Cr, 113 Sn, 85 Sr, 137 Cs, 88 Y and 60 Co Calibration curves fitted to measured efficiencies (photons/count) using polynomial expressions Detector 423 efficiency calibration

True Coincidence Summing Correction True coincidence summing correction factors determined experimentally as deviations between observed efficiencies and calibration curves Energy -4.8 cm -4.4 cm -3.8 cm -2.7 cm -0.8 cm Nuclide (kev) filling filling filling filling filling 57Co 122 0.98 0.99 0.99 0.99 1.00 57Co 136 0.93 0.89 0.93 0.96 0.95 60Co 1173 1.00 1.00 1.00 1.00 1.00 60Co 1332 0.99 0.99 1.00 1.00 0.99 134Cs 605 1.18 1.17 1.15 1.14 1.15 134Cs 796 1.13 1.13 1.11 1.10 1.11 134Cs 802 1.22 1.23 1.21 1.18 1.18 226Ra 186 0.47 0.47 0.49 0.48 0.46 226Ra 352 1.05 1.04 1.07 1.04 1.04 226Ra 609 1.17 1.16 1.16 1.15 1.14 226Ra 1765 0.95 0.95 1.00 0.99 0.99 Excerpt of coincidence summing correction factor table for five different fillings of the 210 ml geometry for detector 423

Density Correction Density correction based on a mathematical model of Ge detector, sample geometry and density (Lippert 1983) Correction factor CF calculated as Where ρ is sample density, xabs characteristic length for sample geometry, m 0 and m 1 constants, and E γ gamma energy. Example correction factors Gamma energy (kev) 210 ml cylinder 178 ml 100 1.33 1.13 500 1.14 1.06 1000 1.10 1.04 1500 1.08 1.03 210 ml cylinder 59 ml Furthermore, for measurements of 210 Pb at 47 kev, correction for self absorption is applied by experimental determination of attenuation using a 210 Pb point source

Commercial software for gamma analysis Using Genie2000 for single application under formal QA/QC Test of radiometric purity of eluate from 99 Mo/ 99m Tc generator Advantages of commercial software More user friendly and with better future prospects than home made software Features and documentation prepared for formal QA/QC Documentation available 21

Future Full use of Genie2000 software