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ii new data and directions for neutron activation analysis richard b firestone lawrence berkeley national laboratory berkeley ca 94720 usa lecture presented at the workshop on nuclear data for activation ...

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                      II.  New Data and Directions for Neutron Activation Analysis 
                                              
                                      Richard B. Firestone 
                     Lawrence Berkeley National Laboratory, Berkeley, CA 94720 USA 
                                              
                                              
                  Lecture presented at the Workshop on Nuclear Data for Activation Analysis,  
                                  7-18 March 2005, Trieste, Italy 
                                              
                                              
              I. Introduction 
               
              In recent years substantial progress has been achieved in the field of Prompt 
              Gamma-ray Activation Analysis (PGAA).  The PGAA application also incorporates 
              the use of short-lived activation analysis products.  Recently, new precise k  
                                                                     0
              measurements for PGAA were performed at the Budapest Reactor.  As part of an 
              IAEA CRP, these data were combined with data from the Evaluated Nuclear 
              Structure Data File (ENSDF) and the literature to create the Evaluated Gamma-ray 
              Activation File (EGAF).  Much of the data contained in EGAF pertains directly to the 
              k  values used in NAA, and there is an opportunity to evaluate the data from both 
               0
              communities to develop better databases for both applications.  Additional data 
              needs for Fast Neutron Activation Analysis (FNAA), will also be discussed. 
               
              II. Prompt Gamma-ray Activation Analysis (PGAA) 
               
              PGAA is a complimentary method to NAA that uses neutron beams to produce 
              prompt γ-rays, following neutron capture, which are used to identify the capturing 
              elements as described in Figure 1.   
               
                                           PGAA 
               
               
               
               
               
               
               
               
               
                                                         NAA 
               
                                    Figure 1.  PGAA and NAA 
               
                                        7
              The neutron beams are typically 10  n/s, far less than the thermal flux of a reactor, 
              and the emitted γ-ray spectra are usually complex.  These limitations are offset by 
              sensitivity to all elements, rapid analysis, and minimal induced radioactivity in the 
              samples.  PGAA also uses k  analysis techniques and includes short-lived NAA 
                                   0
              isotopes in its analysis.  The γ-rays used in PGAA come from the prompt de-
              excitation neutron capture state as shown in Figure 2. 
               
               
                                                                             
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                     
                                                                                                                                                                 24                25
                                    Figure 2.  Example of a PGAA neutron capture decay scheme for  Mg(n,γ) Mg.  
                                                                                   γ
                                    Unlike NAA, most of the  -rays are emitted immediately following the neutron 
                                    capture.  Here the primary or initial γ-rays de-excite a capture state at 7330.67 keV 
                                    producing a cascade of γ-rays to the ground state. 
                                     
                                    A typical elemental spectrum for aluminum is shown in Figure 3.  Note that the 1779-
                                             γ                                                                               28
                                    keV  -ray in this spectrum is from the decay of  Al (2.24 m).  Short-lived isotopes 
                                    produced by NAA are also used for PGAA.  The k  value in PGAA is defined similarly 
                                    to that of NAA where                                                                          0
                                     
                                                                                                  k  = M θ σ /M θ σ   
                                                                                                    0         c a γa          a c γc
                                                                                                                      
                                    M and M  are the atomic weights of the comparator and analyte respectively, θ is the 
                                        c             a
                                    isotopic abundance and σ =P σ is the partial γ-ray cross section where P  is the γ-
                                                                                     γ       γ   0                                                                              γ
                                                                                           σ  
                                    ray transition probability and  0 is the total radiative neutron capture cross section. 
                                                                                                                                                                                                       
                          Figure 3.  PGAA spectrum for Al O
                                                                 2  3 
                                                                                                                              
                   A.  Budapest Reactor Measurements 
                    
                   For many years PGAA was limited by the lack of a well-standardized k  database like 
                                                                                        0
                   the one for NAA.  Researchers at the Budapest reactor have recently measured k  
                   values for nearly all elements from H to U.  Capture gamma ray spectra were     0
                                                                                            1
                   measured with natural targets using a Compton suppression spectrometer .  All 
                   elemental targets were measured together with a chlorine target in order to achieve a 
                                                                                             35
                   consistent energy calibration.  The precise energies of two peaks from the  Cl(n, γ) 
                           2
                   reaction  were used to determine the energies of two distinct peaks, which were then 
                   used for the energy calibration of elemental spectra after non-linearity correction.  
                   The accurate new energy and intensity data were sufficient to identify over 13,000 
                   gamma rays from 79 elements.   
                    
                   Measurements with composite targets (stoichiometric compounds, mixtures, or 
                                                                                          γ
                   solutions) yielded accurate normalizing factors, with respect to the H(n,  ) cross 
                                                                  3
                   section, by means of internal k standardization .  Thus, very accurate determinations 
                                                 0 
                   of the partial gamma-ray production cross-sections and related k -factors became 
                                                                                   0
                   possible.  Energies and k -factors for the most important gamma lines have been 
                             4,5            0                          6,7,8
                   published  and the data library has been discussed     .  Partial cross sections for 
                                                                   9                                γ
                   the best lines for each element were remeasured , often with several targets, and  -
                                                       10
                   rays from short-lived decay products  were included, as summarized in Table I. 
                    
                   B.  Evaluated Gamma-ray Activation File (EGAF) 
                   An IAEA CRP was established to evaluate the Budapest data, and other data from 
                   the Evaluated Nuclear Structure Data File (ENSDF) and the literature to create a 
                                                      σ 
                   comprehensive database of k  and     values.  An IAEA TECDOC containing data for 
                                                0      γ            11
                          γ
                   35,000  -ray from 80 elements has been prepared  is available on the Internet at 
                   http://www-nds.iaea.org/pgaa/.  These data are included in the Evaluated Gamma-
                   ray Activation File (EGAF) which is distributed by the IAEA, and is provided through 
                   an interactive data viewer at http://www-nds.iaea.org/pgaa/pgaa7/index.html.  
                    
                   1.  EGAF Evaluation Methodology 
                   The procedure for evaluation of the EGAF file proceeded as follows. 
                                                               γ
                          a.   Create literature and Budapest (n, ) datasets for each isotope
                                i)  Literature dataset from ENSDF, Reedy and Frankel, and the more 
                                recent literature (NSR):  E , I (per 100 neutron captures) 
                                                          γ  γ
                                                        γ                            σ
                                ii)  Match the Budapest  -rays by energy and relative  γ to the literature 
                                                       σ
                                dataset: Eγ, elemental  γ(barns) 
                          b.   Combine literature and Budapest datasets into EGAF dataset 
                                                      γ
                                i)  Least-squares fit of  -ray energies to level scheme with GAMUT. 
                                ii)  Least-squares fit of γ-ray intensities and cross sections with GAMUT. 
                                iii)  Evaluate discrepancies and statistical outliers. 
                                iv) Create EGAF data file:  E , elemental σ , normalization to isotopic σ  
                                                             γ            γ                           γ
                                                      γ
                          c.  Test EGAF level scheme  -ray intensity balance. 
                                i)  Check the level scheme intensity balance 
                                ii) Compare the total GS γ-ray feedings with BNL-325. 
                                                                                                        
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...Ii new data and directions for neutron activation analysis richard b firestone lawrence berkeley national laboratory ca usa lecture presented at the workshop on nuclear march trieste italy i introduction in recent years substantial progress has been achieved field of prompt gamma ray pgaa application also incorporates use short lived products recently precise k measurements were performed budapest reactor as part an iaea crp these combined with from evaluated structure file ensdf literature to create egaf much contained pertains directly values used naa there is opportunity evaluate both communities develop better databases applications additional needs fast fnaa will be discussed a complimentary method that uses beams produce rays following capture which are identify capturing elements described figure typically n s far less than thermal flux emitted spectra usually complex limitations offset by sensitivity all rapid minimal induced radioactivity samples techniques includes isotopes i...

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