Ar-37 IN ATMOSPHERIC AND SUB-SOIL GASES
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1 2014 Safeguards Symposium, Vienna Ar- IN ATMOSPHERIC AND SUB-SOIL GASES Roland Purtschert Robin Riedmann Lauren Raghoo
2 Ar as a Neutron Flux Monitor Atmosphere 40 Ar + n Ar + 4n Natural or Level? Artificial Background Underground 40 Ca + n Ar + Background Level?
3 Indicators and Sources Xe-135 Xe-133m Xe-133 Xe-131m Ar- Kr h 2.19 d d 10.8 y 5.24 d Nuclear power plant 35 d? reprocessing facility Isotope production (e.g. for medicine) Nuclear explosions After Schlosser 2005 Release rate high medium low Test explosions Xe Isotopes Ar- Plutonium production Kr-85 (Xe Isotopes)
4 Ar- yield (NR+UNE) Sedan Plowshare Crater (Wikipedia) P C N ( E ) ( E )de E 1 GWth Bq/year [Ca] 4% Fission Fusion BWR ~ 1011 P Ar- (Bq/kT) ~ ~ PWR ~ 1011 HTGR ~ 1014 Matuszek et al, (1973) Fay & Biegalski (2012 Teller, (1968) Studer, (1973) Takano, (2003)
5 Atmospheric Background Activity 8 3 Ar mbq/m Air Caribic Mean observed Caribic background 1-2 mbq/m3air Minimal values and theoretically expected tropospheric background ~0.4 mbq/m3air (Lal and Peters, 1973
6 Isotopic properties and decay mode of Ar- Ar- (τ1/2=35.04 d) decays by electron capture (EC) with a decay energy of 2.8 kev. Isotope ratio Ar/Ar at natural levels in the atmosphere: Detection method: Low level counting LLC
7 Ar Laboratories University of Bern, Switzerland 70 mwe PNNL, USA (Seifert et al, 2013) 30 mwe Sample volume: Lair DL 1 mbq/m3air Lead shield and guard counters 100 cc counter
8 Atmospheric Measurements around Bern to Bern 10 km 500 m 90% < 3 mbq/m3air 3 Values > 3 mbq/m3air 1 Value > 5 mbq/m3air Wind Mühleberg BWR MWel 3 Univ. of Bern Near Reactor Ar mbq/m Air
9 Oak Ridge High Flux Isotope Reaktor (85 MW) (Fay & Biegalski, 2012) >0.1 mbq/m3air >0.01 mbq/m3air >0.001 mbq/m3air ((From Fay & Biegalski, 2012) Estimated yearly emissions (2010): Bq Releases after 26 days operation cycle Dilution to 0.1 mbq/m3air air after tens of kilometres
10 Ar activities in tropospheric air (Bern) mbq/m3 mbq/m3air mbq/m km from Bern Observations after 1970 Expected natural background level (Lal and Peters 1969) (Loosli et al. 1986) Start Operation of Swiss Power Plants Possibly slightly elevated Ar background in the vicinity of nuclear power plants (1-3 mbq/m3air)
11 Atmospheric Background Activity? 8 3 Ar mbq/m Air Caribic Caribic
12 Comparison with results from high-volume samplers in Geneva, Switzerland ArmBq/m Luft Cs-1 Cs-134 I-131 /5 1 0 Bq/m air Bq/m3air Ar mbq/m air 7 8 Cs-1 Cs I-131/ Mar Apr May J un J ul Aug The increase of Ar coincidence with the increase of Cs134, Cs-1 and I-131 two weeks after the Fukushima event
13 Hypotheses Reactor Block 4 "It is no exaggeration to say that the fate of Japan and the whole world depends on No. 4 reactor." -Former Japanese Ambassador to Switzerland Mitsuhei Murata to UN Secretary-General Ban Ki-moon (CTV News, Monday, 21 May 2012)
14 Ar activities in tropospheric air (Bern) mbq/m3 mbq/m3air Maximal values after NTE mbq/m3 0. Observations after 1970 Expected natural background level (Lal and Peters 1969) (Loosli et al. 1986) Elevated Values after Nuclear Test Explosions (NTE)
15 Measurements in Bern atmospheric air t: 2 weeks 3 Ar (mbq/m ) 1 Assumptions Ar- Production/MT 1018 Bq (Takano, 2003) Total yield: 7 MT (Lawson, 1994) Homogeneous mixing in northern troposphere (10 km -> V= m3) Measured value in Bern: 70 mbq/m3air atmospheric mixing + decay [Loosli et al. 1970,1973, 1986, ] decay (t1/2: 35 d) Jun Sep Dec Mar Jun Sep Dec Mar Date Novia Semlya, Semipalatinsk (UDSSR), 7 MT, underground 2% Typical release rate after UNE ~1-10 %
16 DPRK Test: 2006: Ar- results measured in Bern Detection probability Ar- Produktion/kT 1014 Bq (Takano, 2003) Yield 1 kt Decay time 1 month (factor 2) Mixing in northern hemisphere (V= m3) Release rate 10% (Saey et al, 2007) Expected signal: mbq/m3 No Ar anomalies detectable in Bern because of large distance dilution
17 Ar sampling in Tokyo after the 2013 DPNK nuclear test SPEEDI simulations (System for Prediction of Environmental Emergency Dose Information) 2/14 9:00(JST) temp:3.2c wind:nnw 1.1m/s Ar- 3±2 mbq/m3air 2/15 9:00(JST) temp:3.6c wind:nnw 1.4m/s Ar- <5 mbq/m3air No Ar anomalies detected in plume over Japan because of missing release vent (Xe-131m and Xe-133 detected 55 days after the event; CTBTO 2013)
18 From IMS to OSI OSI: On-Site Inspection
19 OSI: Soil gas sampling Soil gas sampling 2-10 m
20 Ar in the shallow alluvium From Riedmann & Purtschert 2011 Sun and Carrigan, 2012 Ar concentrations in soils depend on Sampling depth Geology (Ca concentration, soil permeability) Geographical location (altitude and latitude) Ranges mbq/m3air over most of the Earths surface
21 Global scaling of Ar production at 70 cm depth in relation to a reference site (120 mbq/m 3 air) 1000 mbq/m3air 100 mbq/m3air 20 mbq/m3air Ca content from harmonized world soil database Production scaled to latitude and altitude 5' x 5' resolution From Riedmann & Purtschert 2011
22 OSI Ar detection system Movable Ar Rapid Detection System (MARDS) Institute of Nuclear Physics and Chemistry, Mianyang, China Sample volume: >200 L Preparation and counting time: 3-4 h DL > 20 Bq/m3air,
23 Mards System Detection Limit H. Miley, PNNL, 2011
24 Conclusions High precision Ar measurement provide a sensitive tool for the detection of elevated n-fluxes On a regional scale in the atmosphere (IMS) On a local scale In the underground (OSI) Background activities are low and likely < 3 mbq/m3 in the atmosphere air <100 mbq/m3soil-air in the underground Completing Ar samples taken in the frame of XeIMS would be a valuable and non-ambiguous indicator for clandestine high n-flux activities More investigations are needed about activation source terms in the environment (power plants, deep lithosphere, stratosphere)
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