Publication Date: 8/1/75
    Pages: 6
    Date Entered: 1/5/93
    Title: Qualification, Calibration, and Error Estimation Methods for Nondestructive Assay
    August 1975
    U.S. NUCLEAR REGULATORY COMMISSION
    REGULATORY GUIDE
    OFFICE OF STANDARDS DEVELOPMENT
    REGULATORY GUIDE 5.53
    QUALIFICATION, CALIBRATION, AND ERROR
    ESTIMATION METHODS FOR NONDESTRUCTIVE ASSAY
A. INTRODUCTION
    Section 70.58, "Fundamental Nuclear Material Controls," of 10 CFR
    Part 70, "Special Nuclear Material," requires certain licensees to
    establish a measurement quality assurance program for material control
    and accounting. Specifically, paragraph 70.58(f) requires that a
    program be established, maintained, and followed for the maintenance of
    acceptable measurement quality in terms of measurement bias and random
    and systematic errors and for the evaluation and control of the quality
    of the measurement system.
    Nondestructive assay (NDA) constitutes a unique measurement
    technology. When applied under appropriate rigorous controls, it can
    enhance the ability of the material control and accounting system to
    detect diversion of special nuclear material to unauthorized uses. This
    guide describes methods and procedures acceptable to the NRC staff for
    meeting the provisions of paragraph 70.58(f) of 10 CFR Part 70 as it
    relates to the use of nondestructive assay.
B. DISCUSSION
    Nondestructive assay has been applied to virtually every variety
    of chemical or physical form of special nuclear material encountered in
    contemporary reactor fuel processing. Special considerations are
    required to achieve high-accuracy assay results and to properly estimate
    the errors associated with nondestructive assay applications.
    Recognizing these considerations, the American National Standards
    Institute has developed Standard N15.20-1975, entitled "Guide to
    Calibrating Nondestructive Assay Systems."(1) This guide endorses the
    standard as augmented in the regulatory position.
C. REGULATORY POSITION
    The methods, procedures, and guidance relating to the application
    of nondestructive assay, as detailed in the American National Standards
    Institute Standard N15.20-1975, "Guide to Calibrating Nondestructive
    Assay Systems," are acceptable to the NRC staff for material protection
    programs as supplemented by the following.
1. Nondestructive Assay Method Selection
    Prior to selection of an assay method, a study should be made to
    determine the required performance for that application. The specific
    nondestructive assay method should be selected to provide precise and
    accurate results which are compatible with plant material balance
    requirements. Methods to enhance attainable performance should be
    considered (e.g., container selection and packaging procedures for bulk
    materials). (See also Ref. 1.)2. Instrument Specifications
    An evaluation of each new nondestructive assay application,
    including the proposed placement of the instrument, should be conducted
    prior to procurement. A study of each existing nondestructive assay
    application should be conducted to substantiate the basis for its
    further use. The impact of each of the measurement-to-measurement and
    item-to-item sources of error encountered in practice or anticipated
    should be established as a part of each of these efforts.
    ----------
    (1) Copies may be obtained from the American National Standards
    Institute, 1430 Broadway, New York, New York 10018.
    ----------
    A decision should be made to reduce each potentially significant
    source of error through (1) appropriate instrument design
    considerations, (2) operational controls, or (3) supplementary
    measurements made to establish bias corrections (see also Ref. 2).
    Instrument procurement specifications and operational instructions
    should be developed and followed to reflect each error reduction
    decision.
    To minimize operator-related errors and to promote uniform
    measurement practices, nondestructive assay instruments used for
    fixed-station operations should be automated to control (1) data
    acquisition and analysis, (2) diagnostic testing of instrument
    performance stability and calibration validity, and (3) calculation of
    associated error estimates.
    Instruments should be tested to ensure meeting procurement
    specifications prior to calibration.
3. Operators
    Operators should be selected, trained, and tested to be qualified
    before routine use of the instrument. Only qualified operators should be
    permitted to make special nuclear material assays.
4. Stability Testing
    A preventive maintenance program should be devised and implemented
    to ensure the long-term stability and reliability of each instrument.
    As part of an on-going program, a minimum of two working
    standards(2) should be fabricated to periodically test the performance
    stability of the instrument. Each working standard should contain a
    different amount of the species of the special nuclear material to be
    assayed. Working standards should be nominally representative of the
    items to be assayed, as described in ANSI N15.20-1975.
    ----------
    (2) Working standards are used to check the performance of an NDA
    instrument. They should be nominally representative of the items to be
    assayed. They should be fabricated and handled to ensure their internal
    integrity so that deviations in the measured response of the assay
    system can be attributed to the instrument. As stated in ANSI
    N15.20-1975, working standards built to meet these requirements are not
    acceptable as calibration standards. Calibration standards are defined
    in ANSI N15.20-1975 as "physically and chemically similar to the items
    to be assayed, for which the mass of the nuclide(s) of interest and all
    properties to which the measurement technique is sensitive are known."
    Calibration standards can be used as working standards, but working
    standards cannot be used as calibration standards. When calibration
    standards meet the requirements for working standards, licensees may
    elect to maintain only calibration standards. In many cases, however,
    calibration standards may deteriorate through extensive use, or may be
    prohibitively expensive for stability monitoring purposes.
    ----------
    A study should be made to determine the frequency with which the
    working standards are to be measured. In cases of extreme instability,
    a working standard should be measured before and after each unknown item
    assay, and the calibration should be normalized to reflect the average
    of the before-assay and after-assay tests. In any case, a working
    standard should be measured a minimum of twice per shift, once at the
    beginning of the shift and again at some random time during the shift.
    Each response to a working standard should be compared to the mean
    value of all previous measurements of that working standard that were
    accumulated during the preceding material balance period; the difference
    should be plotted on a working chart. Control chart limits should be
    established at 0.05 and 0.001 levels of significance. Whenever control
    data exceed the 0.05 control limits, the test should be repeated.
    Whenever the control data exceed the 0.001 control limits, normal assay
    operations should cease. Normal operations should not resume until the
    out-of-control performance has been remedied and the instrument
    recalibrated.
    The control chart of the working standard responses should be
    examined at frequent intervals to detect indications of drift, which
    should be compensated. The frequency for such examinations should be
    determined by the operating characteristics of each instrument. A
    minimum frequency for examining the control chart for indications of
    drift should be once per week.
5. Calibration
    Nondestructive assay should be employed as a relative indicator of
    special nuclear material content. Thus, calibration should be
    accomplished by measuring the response to calibration standards whose
    contents are characterized through chemical assay procedures, as
    described in ANSI N15.20-1975. The chemical assay procedures should be
    calibrated relative to national standards or nationally accepted
    measurement systems. The calibration standards should represent the
    unknown items in both physical and chemical characteristics.
    Calibration data should be obtained by averaging the responses
    from repeated measurements of the calibration standards. Calibration
    data should be corrected to remove measured nonrandom variations.
    Recalibration should be performed following any repair or parts
    replacement or whenever the characteristics of the items being assayed
    shift so that previous calibration standards no longer adequately
    represent the unknown items. The calibration should be checked
    following a power outage or any unusual mechanical or electrical shock
    to the system.
    Criteria for segregating and packaging different forms of special
    nuclear material should be developed and implemented. Each material
    category should be established to enhance assay performance, consistent
    with safety requirements and subsequent processing needs. (Guidance for
    material categorization is provided in Regulatory Guides 5.2,
    "Classification of Unirradiated Plutonium and Uranium Scrap;" 5.11,
    "Nondestructive Assay of Special Nuclear Material Contained in Scrap and
    Waste;" and 5.34, "Nondestructive Assay for Plutonium in Scrap Material
    by Spontaneous Fission Detection.") For all categories of materials to be assayed, with the exception
    of small content miscellaneous categories (e.g., furnace liner bricks,
    contaminated tools or machine parts), the calibration relationship
    should be a least-squares fit to an appropriate function. The graphical
    calibration method is acceptable for miscellaneous categories of
    material which contain a total of no more than 0.1 effective kilogram(3)
    of special nuclear material in each category during a material balance
    period. The combined contribution from all assays calibrated through
    the graphical method should be less than 10% of the total plant limit of
    error of material unaccounted for (LEMUF).
6. Calibration Standards
    A minimum of four calibration standards should be obtained to
    serve as the basis for the initial calibration of each instrument for
    each separate category of material. The calibration standards should be
    completely characterized, including the mass and isotopic composition of
    the species of special nuclear material to be assayed, plus all physical
    or chemical variables to which the response of the instrument is
    sensitive. The mass of special nuclear material contained in the
    standards should span the range of loadings to be encountered in routine
    assays.
    The isotopic composition of the material used in all calibration
    standards should be identical with the isotopic composition of the
    material being assayed. When the isotopic composition changes so that
    the response per gram of special nuclear material differs by 10% or more
    from the value of the calibration standards, the material should be
    identified as a new material category. The nondestructive assay system
    should be recalibrated for that category, using new calibration
    standards made up using the new isotopic composition. When the change
    in response per gram is less than 10%, a bias correction should be
    determined and applied to the assay data.
    ----------
    (3) The term "effective kilogram" is defined in 10 CFR Section
    70.4(t).
    ----------
    The uncertainty in the bias correction should be determined and
    used in estimating the total assay uncertainty. (Appropriate error
    propagation procedures are described in Regulatory Guide 5.18, "Limit of
    Error Concepts and Principles of Calculation in Nuclear Materials
    Control.") When the response is sensitive to ingrowth or decay of a daughter
    product, the procedures described in the preceding paragraphs are
    appropriate and should be applied.
    Once fabricated, the calibration standards should be handled with
    extreme care to ensure that the distribution of contents remains fixed.
    Calibration standards should be used only when developing the initial
    calibration or when recalibrating the instrument following a repair or
    power outage. (Working standards should be used to test the continued
    stability of the instrument, see footnote 2.) The degree of effort which should be expended in fabricating the
    calibration standards depends on the method used to estimate the assay
    uncertainty, as described in the next section.
7. Assay Uncertainty Estimation Methods
    Random errors associated with nondestructive assay should be
    estimated through a replicate assay program during each material balance
    period.(4) The second assay of each replicate pair should be performed
    a minimum of 4 hours after the first assay.
    Three methods are acceptable to estimate the uncertainties
    associated with calibrations and bias corrections for nondestructive
    assay. The first two procedures, graphical estimation and analytical
    estimation through the calibration relationship, are detailed in the
    standard. The third procedure, comparative evaluation, is not described
    in ANSI N15.20-1975.
    ----------
    (4) A regulatory guide related to random error evaluation is in
    preparation (to be entitled "Considerations for Determining the Random
    Error of Special Nuclear Material Accounting Measurements").
    ----------
    7.1 Graphical Estimation
    Use of the graphical error estimation technique should result in a
    conservative error estimate that is acceptable for miscellaneous unusual
    assay categories, as described in Regulatory Position 5 of this guide.
    7.2 Analytical Estimation Through the Calibration Relationship
    When the calibration standards can be shown to adequately
    represent the unknown items, the combined systematic error associated
    with the nondestructive assay of an inventory of items can be estimated
    through the calibration relationship, as demonstrated in ANSI
    N15.20-1975. The calibration standards should be fabricated from
    different batches of material. The uncertainty associated with the
    content of special nuclear material elements and response-related
    isotopes contained in each calibration standard should be based on an
    extensive characterization as described in N15.20. The uncertainty
    associated with the contained mass of the response-related isotopes
    should be included in the calibration, as described in N15.20. Further,
    the element uncertainty should be factored into the estimated total
    assay uncertainty.
    Using this procedure, it is necessary to periodically ensure that
    the calibration standards adequately represent the unknown items. This
    can be accomplished by isolating and characterizing the extraneous
    interference factors that affect the response of the instrument.
    Typically, this separation and characterization is most easily
    accomplished when the items are either finished fuel items or uniform
    containers of feed or intermediate product material.
    To ensure that the calibration standards continue to adequately
    represent the unknown items, key parameters(5) that affect the observed
    response (i.e., item-to-item variations) should be monitored through
    separate tests. Measurements of the key parameters should be compiled
    and analyzed at the close of each material balance period. When the
    mean value of a parameter shifts from its previously established value,
    the impact of the shift on the response of the assay instrument should
    be measured through an appropriate experiment or calculation (Ref. 3).
    An appropriate bias correction should be determined and applied to all
    items that were assayed after the best estimate of when the parameter
    changed. The uncertainty in that bias estimate should be combined with
    the uncertainty in the assay values as predicted through the calibration
    function to estimate the total assay uncertainty.
    ----------
    (5) See Section 5.4 of ANSI N15.20-1975. See Regulatory Position
    6 of this guide for provisions to include the effects of changing
    isotopic compositions.
    ----------
    The uncertainty due to a bias correction may significantly
    increase the limit of error of the assay. In severe cases, the increase
    may increase the LEMUF above the level acceptable for the total plant.
    In such cases, new calibration standards should be obtained and the
    assay system should be recalibrated.
    As a further check on the continued validity of the calibration
    standards, a program to periodically introduce new calibration standards
    should be implemented. A minimum of one new calibration standard. for
    each category of materials should be introduced during each 6-month
    period.
    7.3 Comparative Evaluation
    The procedure described in this section is not included in ANSI
    N15.20-1975.
    When two measurement methods are used for each of a series of
    items and one of the methods is considerably more accurate than the
    other, corresponding measurements can be usefully compared. The
    comparison can be used to establish an estimate of bias between the
    measurement methods. The comparison can also be used to estimate the
    total uncertainty associated with the less accurate measurement method.
    To determine the uncertainty associated with the nondestructive
    assay of an inventory of items using this method, unknown items should
    be randomly selected for comparative measurements. The special nuclear
    material content of the items selected should span the range of contents
    normally encountered. Random error should be estimated through
    replicate analyses. To estimate the remaining contributions to the
    total assay uncertainty, each item should be repeatedly assayed to
    reduce the random assay error to less than 10% of the estimated or
    previously established total uncertainty. Then, to determine the
    special nuclear material content of each item selected for comparative
    evaluation, one of the following procedures should be employed:
    a. Each item should be completely dissolved, independently, and
    the resulting solution should be analyzed by high-accuracy elemental and
    isotopic assay procedures, which in turn are calibrated relative to
    national standards or nationally accepted measurement systems.
    Items composed of an aggregate of similar units, e.g., fuel
    rods containing discrete pellets, should be opened and the contained
    units should be weighed, pulverized, blended, and sampled for assay
    through appropriate high-accuracy elemental and isotopic assay
    procedures. The emptied container should be examined for indications of
    residual accumulations and cleaned, leached, or assayed nondestructively
    to determine the residual special nuclear material content.
    b. Plutonium-bearing items only: Each item should be assayed
    through calorimetric procedures (Ref. 4). Large items should be
    subdivided into smaller containers. Each small container should be
    assayed calorimetrically. Samples should be taken from at least three
    of the smaller containers. The samples should be micro-calorimetered and
    then assayed through highly accurate elemental and isotopic procedures
    which in turn are calibrated relative to national standards or
    nationally accepted measurement systems (Ref. 5). The istotopic
    measurement data should be examined for evidence of nonhomogeneous
    isotopic content. Isotopically nonhomogeneous materials should be
    blended and reanalyzed.
    On the basis of the average grams of plutonium per watt of
    the micro-calorimetered samples, the total amount of plutonium in each
    of the subcontainers should be determined. The total plutonium content
    of the items selected for comparison is then estimated as the combined
    contents of the subcontainers.
    For the first full material balance period during the
    initial implementation of this guide, two items from each category of
    assay items should be randomly selected each week for an accuracy
    verification measurement. Following this initial implementation period,
    licensees may reduce the verification measurement frequency to two items
    per month per category. When fewer than one hundred new items of a
    given category are created per week, at least two item comparative
    verification measurements should be made per material balance period per
    category, through the procedures described above. In such cases, to
    provide an adequate data base to update the uncertainty estimates for
    nondestructive assay, licensees may pool the verification data provided
    the measurements are in statistical control; i.e., when repeated samples
    from the portion of the measurement system under test behave as random
    samples from a stable probability distribution. Under such conditions,
    data sets may be combined provided the parameters based on the current
    set of data and the previous set of data are not significantly different
    on the basis of acceptable statistical tests.
    As an alternative to this selection criteria, licensees may
    elect the latter frequency for a specific category when it can be
    demonstrated that the contribution to the LEMUF from that category is
    less than 100 grams in any material balance period.
    At the close of the reporting period, the assay value for
    each item selected for verification should be plotted against the
    verified quantity. The verification data plot should be examined for
    indications of nonlinearity or obvious outlier data. Anomalous
    indications should be investigated and remedied.
    A linear regression analysis to a non-zero-intercept
    straight line should be performed on the nondestructive assay versus
    verification assay data. The intercept should be tested against zero
    with a "t" test at a 5% level of significance for an indication of a
    constant bias. In addition, the slope should be tested against unity
    for an indication of proportional bias. When bias is indicated (i.e.,
    the bias exceeds 10% of its estimated uncertainty), assays performed
    during the preceding operating period should be compensated. The
    uncertainty associated with bias corrections should be estimated with
    the standard error of estimate associated with the verification line.
    The total assay uncertainty should be estimated by combining the random
    error estimate for the collection of items assayed with the estimated
    bias uncertainty.
    When all items contain essentially the same special nuclear
    material content, the difference in the mean content values should be
    tested against zero as an indication of bias. The total assay
    uncertainty associated with an inventory of items should be estimated as
    the standard deviation of the mean difference, combined with the random
    assay error. For individual items, the assay uncertainty should be
    estimated as the standard deviation of the difference distribution,
    combined with the estimated single measurement random error. Again,
    bias corrections should be applied when the indicated bias exceeds 10%
    of the standard deviation of the mean difference.
    Whenever a bias exceeding 50% of its estimated uncertainty
    is indicated, its cause should be investigated. This investigation
    should include a review of the assumptions factored into the
    nondestructive assay system's calibration. In particular, instrument
    stability and the stability of parameters that may influence the
    response of the assay system should be investigated. The investigation
    should also address the comparative measurement method, including
    sampling, sample handling, analytical procedures, interference
    compensation, and calibration validity. Results from the investigation,
    if they show the nondestructive assay system to have been incorrectly
    calibrated, should be employed to recalibrate the instrument for the
    forthcoming material balance period. Conversely, when the source of
    bias can be attributed to errors in the comparative measurements, bias
    corrections should not be made to the nondestructively assayed items.
    Results from such investigations should be documented, and the documents
    maintained in accordance with Regulatory Position 8 of this guide.
8. Records Retention
    All records generated in accordance with this guide, including
    control charts, should be retained for a period of 5 years, as specified
    in 10 CFR Section 70.51 (e)(4)(iii).
D. IMPLEMENTATION
    This section provides information to applicants and licensees
    regarding the NRC staff's plans for using this regulatory guide. Except
    in those cases in which the applicant or licensee proposes an
    alternative method, the NRC staff will use the methods described herein
    in evaluating an applicant's or licensee's capability for and
    performance in complying with specified portions of the Commission's
    regulations for submittals docketed after October 1, 1975, in connection
    with a current license or an application for a license, or amendment of
    a current license.
    An applicant or licensee may use this regulatory guide in
    developing submittals docketed on or before October 1, 1975. The
    pertinent portions of these submittals will be evaluated on the basis of
    this guide.
    REFERENCES
1. Regulatory Guide 5.11, "Nondestructive Assay of Special Nuclear
    Material Contained in Scrap and Waste," U.S. Atomic Energy
    Commission (1973).
2. T. E. Shea, "Reduction, Control, and Estimation of Nondestructive
    Assay Errors," Nucl. Mat. Mgmt., Vol. III, No. 3 (1974).
3. R. A. Forster, D. B. Smith, and H. O. Menlove, "Error Analysis of
    a Cf-252 Fuel-Rod-Assay System," LASL Reports LA-5317 (1974).
4. Regulatory Guide 5.35, "Calorimetric Assay of Plutonium," U.S.
    Atomic Energy Commission (1974).
5. F. S. Stephens, R. G. Gutmacher, K. Ernst, S. P. Turel, and T. E.
    Shea, "Methods for the Accountability of Plutonium Dioxide,"
    WASH-1335 (1975).
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