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A Comparison of Activation Products in Different Types of Urban Nuclear Melt Glass

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A Comparison of Activation Products in Different Types of Urban Nuclear Melt Glass 530 Nuclear Nonproliferation Policy: General A Comparison of Activation Products in Different Types of Urban Nuclear Melt Glass Joshua J. Molgaard1, John D. Auxier II2,3, Howard L. Hall2,3,4 1United States Military Academy, Science Building 753, West Point, NY, 10996, [email protected] 2Department of Nuclear Engineering, University of Tennessee, Knoxville, TN, 37996, [email protected] and [email protected] 3Radiochemistry Center of Excellence (RCOE), University of Tennessee, Knoxville, TN, 37996 4Institute for Nuclear Security, 1640 Cumberland Avenue, Knoxville, TN, 37996, [email protected] metropolitan area. The details of the emplacement INTRODUCTION scenario are not specified. In each case the device is assumed to produce a yield equivalent to 1 kiloton of Countering nuclear proliferation is one of the primary TNT explosives. Both 235U and 239Pu are considered as challenges facing our nation and the world today. fuels. Other device components (e.g. tamper, initiator, Scientists and engineers working in the nuclear industry wiring) are not included. All constituents are assumed to have a vested interest in this issue, as do politicians, mix equally within the fireball and be distributed government officials, and members of the armed forces. uniformly within the debris. This may seem to be an over- The academic community can also contribute to nuclear simplification, however, if the same assumptions are used non-proliferation efforts by conducting research and for each modeling prediction the comparisons should training experts in the fields of radiochemistry, nuclear remain valid. forensics, and nuclear security. The Radiochemistry The fuel quantities are calculated in accordance with Center of Excellence (RCOE), established at the the method developed by Giminaro et al [2]. For uranium University of Tennessee (UT) and funded by the National fueled devices the mass of fuel in a 1-gram melt glass Nuclear Security Administration (NNSA), is training sample is estimated at 66.7 micrograms. For plutonium students and developing new analysis techniques to the fuel mass is set at 21.3 micrograms. These improve the timeliness of nuclear forensics results. To calculations are based on significant quantities reported support these efforts UT has developed and patented by the International Atomic Energy Agency [4]. It is methods for creating surrogate nuclear melt glass for assumed that the fuel mass is a fixed quantity and the forensic analysis [1]. Most recently, researchers at UT efficiency of the weapon determines the yield. It is also have designed an analytical method for developing urban assumed that the mass of melt glass produced is directly matrix formulations to be used in the synthesis of urban proportional to the yield of the device [5]. nuclear melt glass surrogates [2]. The work presented here focuses on modeling efforts designed to predict and Irradiation compare activation products found in urban nuclear melt glass produced by notional events in two different For each sample FAT is used to initiate a very short metropolitan areas within the United States. reactor run in SCALE 6.1 and the output is analyzed using the f71 file analyzer in FAT. For a 1-gram sample a MODELING scaled yield of 2.67x10-9 kilotons is desired [2]. This is obtained by running the reactor for 1 microsecond at For this study the methods developed by Giminaro et. 1.24x104 megawatts. For each model a 27 group neutron al. [2] were employed to predict the elemental spectrum (27GrpSCALE6) is used and the usable energy composition of nuclear debris produced by events in New per fission is set at 180 MeV. York, NY (NYC) and Houston, TX. For each city, the Two cities (NYC and Houston) are modeled. For composition of a notional 1-gram sample was entered into each city both fuels are considered, and for each fuel two the Fallout Analysis Tool (FAT) which is run in concert ORIGEN libraries (fast and thermal) are used. This results with SCALE 6.1 [3] to generate fission and activation in a total of eight distinct models. The thermal reactor products in the sample. Only the activation products are runs are included for comparison to synthetic nuclear melt analyzed in this study. Differences in the compositions of glass samples which will be irradiated at the High Flux debris matrices developed for NYC and Houston are Isotope Reactor (HFIR) using the pneumatic tube system. expected to lead to different radioactive signatures. The fast library is clearly more appropriate for simulating a nuclear weapon. Scenarios For both cities the nuclear detonation is modeled as a surface burst with ground zero located at the center of the Transactions of the American Nuclear Society, Vol. 112, San Antonio, Texas, June 7–11, 2015 Nuclear Nonproliferation Policy: General 531 RESULTS Table II. Top Five Activation Products (AP) by Activity at t=24 hours (after detonation) The elemental composition of each urban matrix is NYC Houston shown in Table I. The Houston matrix has a higher silicon Fuel Library AP Act. (bq/g) AP Act. (bq/g) and calcium content while the NYC matrix is enriched in 235 24 10 37 10 sodium, iron, and magnesium by comparison. The U Fast Na 1.76x10 Ar 8.54x10 37 24 elemental differences observed here will give rise to Ar 1.64x1010 Na 7.06x1010 unique radioactive signatures for each scenario. 42 42 K 1.88x109 K 5.50x109 32 8 32 9 Table I. Urban Matrix Compositions [2] P 6.11x10 P 2.88x10 47 47 Element NYC Houston Sc 3.52x108 Sc 1.56x109 24 24 Si 6.05E-01 6.38E-01 Therm. Na 8.19x109 Na 2.04x109 42 42 K 3.55E-02 2.20E-02 K 1.13x109 K 6.98x108 37 37 Al 1.51E-01 1.79E-01 Ar 1.36x108 Ar 1.60x108 56 31 Ca 6.35E-02 7.48E-02 Mn 9.26x107 Si 8.71x107 31 56 Na 3.23E-02 7.51E-03 Si 8.36x107 Mn 4.54x107 239 24 37 Fe 7.63E-02 6.23E-02 Pu Fast Na 3.81x1010 Ar 4.17x1010 37 24 Mg 2.65E-02 8.69E-03 Ar 3.54x1010 Na 3.45x1010 42 42 S 6.02E-04 6.58E-04 K 4.06x109 K 2.68x109 32 32 Ba 5.61E-04 8.60E-04 P 1.32x109 P 1.40x109 47 47 Mn 1.16E-03 5.61E-04 Sc 7.62x108 Sc 7.57x108 24 24 P 9.66E-04 2.85E-04 Therm. Na 1.33x1010 Na 3.32x109 42 42 Ti 6.08E-03 6.03E-03 K 1.84x109 K 1.13x109 235 37Ar 8 37Ar 8 U 6.67E-05 6.67E-05 2.22x10 2.60x10 56 31 239 Mn 8 Si 8 or Pu 2.13E-05 2.13E-05 1.52x10 1.42x10 31Si 8 56Mn 7 Total 1.00E+00 1.00E+00 1.36x10 7.38x10 24 For each of the eight distinct models the activities of Activation Product Na the top five activation products are reported at t=24 hours 24 after the detonation. The results are shown in Table II. The Na found in each notional sample may be Seven different activation products are seen here, produced in a variety of ways. The primary production route for thermal neutron irradiations is the (n, γ) reaction however, the top five and the order of precedence vary 23 24 depending on the details of each model. Table III lists the which converts stable Na to Na with a half-life of 15 likely production routes for the seven activation products hours. The comparison between NYC and Houston considered in this study. samples is thus straightforward for thermal neutron 37 irradiations (the NYC matrix contains more sodium and The Ar which appears in each model is produced by 24 neutron bombardment of 40Ca via an (n, α) reaction. The more Na as expected). This holds true for both uranium 37 40 and plutonium fueled models. However, for samples quantity of Ar produced depends on the quantity of Ca 37 produced using uranium fuel and fast neutron irradiations in the matrix, and the Houston samples have higher Ar the results may seem surprising at first glance. The cross activities then the corresponding NYC samples, as section for the (n, γ) reaction is very small for fast neutron expected. However, noble gases, such as argon, produced energies, and the higher activity of 24Na in the Houston during a surface burst are likely to be dispersed and 37 samples irradiated with fast neutrons can be explained by carried away from ground zero by winds. Thus, the Ar considering another production route for 24Na. Neutron content of nuclear melt glass is expected to be much 27 24 lower than what is reported here. Only a small fraction bombardment of Al can produce Na via an (n, α) may be trapped within vesicles formed in the melt glass. reaction and the cross section for this reaction is much For this reason 37Ar is not given further consideration in larger for fast neutron energies (see Table III). Because the Houston matrix contains more aluminum, the higher this study. The remaining activation products are 24 235 discussed individually in the following sections. Na activity in the U/Fast/Houston samples is reasonable if this second production route is assumed to Transactions of the American Nuclear Society, Vol. 112, San Antonio, Texas, June 7–11, 2015 Transactions of the American Nuclear Society, Vol. 112, San Antonio, Texas, June 7–11, 2015 532 Nuclear Nonproliferation Policy: General dominate. For plutonium fueled models a similar Once again, for models using plutonium fuel and the fast argument may explain why the 24Na activities in the NYC neutron library, the activation product quantities deviate and Houston samples are closer than expected (based on from the general trend.
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