Role of radioactive beams in stockpile stewardship science Ed Hartouni August 23, 2010 NUCL Symposium Radiochemistry at the Facility for Rare Isotope Beams (FRIB) American Chemical Society Fall National Meeting, Boston, MA * This work performed under the auspices of the U.S. Department of Energy by under Contract DE-AC52-07NA27344.
Nuclear science contributions to national security Radiochemisty nuclear forensics, stockpile stewardship, NIF nuclear diagnostics Nuclear Theory fission, fusion, nuclear reactions Nuclear Experiment cross sections, diagnostics, detectors Nuclear Data cross section evaluations, computational models And the scientists who willing and able to take on the challenges presented by a changing world 2
The last time I gave a similar talk RIA and Stockpile Stewardship August 26 th, 2003 Scientific Challenge: Determine the neutron flux in regions of enormous instantaneous neutron intensities (interior of stars, nuclear weapon tests, and NIF experiments) from remnant long lived nuclei. Accurate neutron cross sections on short lived isotopes essential for accurate flux determination Most of the neutron cross sections on the relevant shortlived states have never been measured due to production limitations. RIA changes all that. Improved physical understanding of unstable nuclei allows more accurate calculations of cross sections where measurements are not possible. 3
What has changed? The challenge of measuring reactions on short lived nuclear states remains an important goal. RIA became FRIB and has been approved by DOE. A tremendous effort has gone into exploiting indirect methods for measuring neutron reactions on relevant states. Theory is starting to become an important contributor to providing information on reactions. Nuclear Forensics has become an important notion in nuclear security. 4
An example of stock pile radiochemistry Zr 92 Zr 93 2x10 6 y 94 Zr 95 64 d 4x10 17 y 97 16.9 h 93 10.3 h 18.7 m 95 10.3 m 6.2 s 97 9.6 s 5.3 s Exp measured cs A Z stable (n,γ) (n,2n) τ 1/2 (p,n) β (n,p) β + f. frag Sr 93 7.4 m 75 s 95 25 s 1 s 97 420 ms 235,238 U, 239 Pu I(fs) > 0.5% Rb 93 5.7 s 2.7 s 95 384 ms 0.2 s 97 Count 95 Zr activity: infer ~ N atoms Expected Fraction ~ f Kr 93 0.21 s 95 0.78 s < 0.1 s 97 Total # of 95 Zr atoms produced = N/f = N tot Total # of fissions F = N tot /0.06 ~ M fissions NOTE: 0.06 is the percentage of the total fragment distribution that is assumed to decay along the A=95 mass chain into 95 Zr. IT ASSUMES NO BURN IN OR OUT OF THE CHAIN. Energy release from fission ~ F x 10 23 fissions/kt TOTAL FISSION IELD = F / Ax10 23 kt 5
Our knowledge of the reaction networks is incomplete 86m 86 48m 14.7h ttrium neutron reaction network unstable nuclei stable nuclei 87m 87 13.7h 79.8h not measured poorly measured well measured 88 106.7d 90m charged particle out reactions 89m 15.3s 90 3.19h 58.5d 89 stable Measure the ratio 88 / 89 compare to expectation 6
Unstable nuclei of interest to stockpile stewardship Loaded Element # of isotopes and isomers # with half-life > 10y # with halflife < 1d After fragment separator Ti 14 6 3 Cr 11 3 4 Fe 5 2 1 Br 6 4 1 Kr 3 2 0 11 1 6 Zr 10 3 5 Nb 5 3 1 Stockpile relevant isotopes Mo 3 1 2 Eu 20 7 5 Tm 8 1 2 Lu 24 2 14 Ta 6 2 1 Ir 21 3 12 Au 7 1 1 Lawrence Bi Livermore 7 National 3 Laboratory 1 7
Isotope harvesting 1.E+14 A=150 3 t1/2 collection time! 10 day collection time! Isotope Production Rate (atoms/sec) 1.E+13 1.E+12 100 µg! 1.E+11 10 µg! FRIB estimates 86! 1.E+10 79Kr! 1.E+09 1 µg! 194Au! 47Sc! 87 170Lu!! 146Eu!177Lu! 1.E+08 0.1 1 10 100 ng! 148Eu! 100 half-life (days) Estimated target mass as a function of isotope half-life and isotope production rates. The solid lines are calculated for an A=150 nucleus for 4 different target masses, as indicated. A further assumption limits the isotope collection time to the shorter of 10 days or 3 halflives. 8
Additional interest in fission 239 Pu(n,Fission)! (Barns) (Barns) 3.5 3.5 3 3 2.5 2.5 2 2 1.5 1.5 1 1 0.5 0.5 ENDF/B-VII "0 (2003) JEFF-3.0 (2002) 1970's ENDF/B-VI ENDL99 1960's 1950's Data (1999) release 8 (1989) ENDL99 (1999) 1960's JENDL-3.3 ENDF/B-VI 1950's Data (1987) release 8 (1989) ENDF/B-VI 1950's 1980's JENDL-3.3 release 8 (1989) Data (1987) JENDL-3.3 (1987) 1970's 1990's Data 1990's 1960's Data 1980's Data 1980's 1950's Data 1970's Data 1970's Data 1960's Data 1960's Data 1950's Data 1950's Data 0 0 0 5 5 10 10 15 15 20 20 E inc inc (MeV) 9
Proposed to develop new detector Fission TPC to push to new precision and accuracy Black Fission Fragments Green alphas Red scatters 10
Additional information from the TPC will expand fission measurements, e.g. fragment distribution 11
The NIF National Ignition Facility Hot/Dense k b T=1-20 kev 10 35 cm -2 s -1 ρ 10-1000 g/cm 3 10 36 e/cm 2 s High Neutron Flux 10 30-35 cm -2 s -1 (fluence=10 21-24 cm -2 ) Radiochemical activations are used on NIF to measure yield, and there are proposals for an expanded diagnostics program. Proposed radiochemstry diagnostics of ICF capsule mix 127 I(d,2n) 127 Xe production 12
Theory may be the only way of providing precision cross section information of interest to NIF 13
The nuclear science workforce continues to be an issue but data does not exist to track trends 120 Ph.D Production number of Ph.D.'s per year 110 100 90 80 70 60 50 40 30 20 10 Nuclear Physics average = 84/yr Nuclear- and Radio-chemistry average=11/yr 51/yr in 2010 5/yr in 2010 0 1992 1994 1996 1998 2000 2002 2004 2006 2008 2010 2012 year 14
Additional concerns regarding the fate of small facilities which produce the majority of PhDs 120 100 Ph.D.'s per year 80 60 40 20 0 Experimental Nuclear Physics Ph.D. production from Facilities 1986 1991 1996 2001 2006 DOE report total facility RHIC Jlab ANL/Atlas NSCL BATES HRIBF ORELA 88" BEVALAC Low Energy Notre Dame TAMU total experimental CENPA TUNL WNSL-ale 15
Conclusions half-way to FRIB The need for nuclear data and a skilled nuclear science workforce are increasingly important to nuclear security The development of technique, detectors, simulation and theory are necessary in preparation for FRIB experiments The nuclear science workforce pipeline continues to be a concern Small nuclear science facilities will play an essential role in all these areas before and after FRIB first beam. 16