Publication Date: 5/1/74
    Pages: 16
    Date Entered: 1/5/93
    Title: In Situ Assay of Plutonium Residual Holdup
    May 1974
    U.S. ATOMIC ENERGY COMMISSION
    REGULATORY GUIDE
    DIRECTORATE OF REGULATORY STANDARDS
    REGULATORY GUIDE 5.23
    IN SITU ASSAY OF PLUTONIUM RESIDUAL HOLDUP
A. INTRODUCTION
    Part 70, "Special Nuclear Material," of Title 10 of the Code of
    Federal Regulations requires licensees authorized to possess more than
    one kilogram of plutonium to calculate a material balance based on a
    measured physical inventory at intervals not to exceed two months.
    Further, these licensees are required to conduct their nuclear material
    physical inventories in compliance with specific requirements set forth
    in Part 70. Inventory procedures acceptable to the Regulatory staff are
    detailed in Regulatory Guide 5.13, "Conduct of Nuclear Material Physical
    Inventories."
    Plutonium residual holdup is defined as the plutonium inventory
    component remaining in and about process equipment and handling areas
    after those collection areas have been prepared for inventory. Whenever
    possible, process equipment should be designed(*) and operated so as to
    minimize the amount of holdup. In this guide, procedures are detailed
    for the in situ assay of the residual plutonium holdup.
    Assay information can be used in one of two ways:
1. When the limit of error of plutonium holdup is compatible with
    constraints on the overall limit of error on the facility MUF (LEMUF),
    the material balance can be computed using the measured contents of Pu
    holdup. Additional cleanout and recovery for accountability will then
    not be necessary.
    ----------
    (*) Design features to minimize holdup in process equipment are
    the subject of a series of regulatory guides.
    ----------
2. When the limit of error of Pu holdup is not compatible with
    constraints on the overall LEMUF, the information obtained in the holdup
    survey can be used to locate principal Pu accumulations and to assure
    that other areas of the process contain less than the detectable amount
    of plutonium. Once located, substantial accumulations can be recovered,
    transforming the plutonium to a more accurately measurable inventory
    component. Having reduced the amount of plutonium holdup, the limit of
    error on the remeasurement of the remaining holdup may be sufficiently
    reduced to be compatible with overall LEMUF requirements.
B. DISCUSSION
    Plutonium accumulates in cracks, pores, and zones of poor
    circulation within process equipment. The walls of process vessels and
    associated plumbing often become coated with plutonium during solution
    processing. Surfaces internal and adjacent to process equipment,
    especially glove box walls and floors, accumulate deposits of plutonium
    which can become appreciable. Plutonium also accumulates in air filters
    and associated ductwork. The absolute amounts of plutonium holdup is
    must be small for efficient processing and proper hazards control.
    However, the total amount of plutonium holdup may be significant in the
    context of the tolerable facility MUF.
    The measurement procedures detailed in this guide are based on the
    controlled observation of gamma rays and neutrons which are
    spontaneously emitted by the plutonium isotopes. Because the gamma rays
    of interest are emitted by Pu-239, gamma ray assay is the preferred
    assay method whenever its acceptance criteria are satisfied. To
    accomplish either gamma ray or neutron assay, it is essential to
    consider the facility in terms of a series of zones which can be
    independently assayed. Such zones are designated as "collection zones."
1. Delineation of Collection Zones
    Typical plutonium process facilities comprise a number of
    interconnected glove boxes which contain work areas and most process
    equipment, in-process storage areas, and self-contained process
    equipment. Also, solution processing requires tanks, plumbing, and
    pumping equipment, which are often located in close proximity to the
    glove box lines. Finally, storage areas for feed, scrap and waste, and
    final product are also often located in close proximity to the plutonium
    process area.
    Each facility can be divided into a series of collection zones on
    the basis of a logical understanding of process activities. Individual
    glove boxes can be subzoned to improve assay performance, but for most
    applications, individual glove boxes are examples of suitable size areas
    for discrete collection zones.
    Gamma ray assay for plutonium holdup measurement is practical when
    a collection zone consists of a single structure of relatively uniform
    cross section. When a collection zone contains an item of equipment
    having significant shielding properties and capable of contributing to
    the holdup, the uncertainty in the holdup prediction based on the
    observed response may become primarily due to attenuating the radiations
    in the internal structure. In such cases, neutron assay is applicable.
2. Applicable Methods and Instruments
    Two considerations are critical to the selection of methods and
    instruments. First, to perform an assay, the plutonium radiations must
    reach the detector and be detected. Second, the observed response must
    be attributable to the collection zone being assayed. Therefore, the
    assay scheme is developed around penetrating radiations and the detector
    is collimated to provide for sufficient directionality in the response
    to resolve a collection zone from its neighbor zones and from the
    background.
    2.1 Gamma Ray Assay
    Under closely controlled conditions, the measured plutonium gamma
    ray spectrum can be interpreted in terms of the abundance of each gamma
    ray emitter present in the sample. Because of the large number of gamma
    rays(1,2) present, many regions of the observed spectrum are
    characterized by overlapping lines. To accomplish the assay, it is
    necessary to select an appropriate spectral region and provide a
    detection system with sufficient resolution to measure the activity from
    one or two isotopes of interest.
    Gamma ray assay has an advantage over neutron assay in that the
    emissions are primarily from the principal isotopes of interest.
    Because of the higl emission rate of gamma rays, a detection sensitivity
    of less than one gram is generally attainable.
    The most useful portion of the spectrum for holdup assay is the
    Pu-239 gamma ray complex in the 375-440 keV range. The yields of these
    lines are given in Table B.1.
    (Due to database constraints, Table B.1 is not included. Please contact
    LIS to obtain a copy.) 2.1.1Gamma Ray Detection Instruments
    Gamma ray detection systems consist of a scintillation or
    semiconductor detector sensitive to gamma rays and appropriate
    electronics.(3) Required electronics include at least a single channel
    analyzer and a timer-scaler unit. A second single channel analyzer used
    to determine the background radiation correction is a time-saving
    feature. Battery powered systems are commercially available and can
    provide operational convenience, particularly in this application.
    The detection efficiency and resolution of good NaI(TI)
    detectors is generally adequate for this application. CdTe, Ge(Li), and
    intrinsic Ge detectors have better resolution than NaI(TI) but cost
    more, are generally less available, and are more difficult to operate.
    The 332.3 keV gamma ray from U-237, a short-lived (6.75 d)
    daughter of Pu-241, is usually the principal interference for Pu-239
    assay by NaI detection of the 375-440 keV complex. If the U-237 is in
    equilibrium with Pu-241, the intensity of this gamma ray is 1.15 x 10(6)
    gamma/sec-g Pu-241.
    Since this gamma ray is also emitted in the decay of Am-241,
    the interference from this decay branch may also be important in case of
    preferential americium holdups. To avoid this interference when using
    NaI detectors, the assay energy window is adjusted to span the range
    from 390 to 440 keV.
    Detector dimensions are selected to provide a high
    probability for detecting the appropriate gamma rays. The geometric
    detection efficiency increases as the square of the detector radius;
    however, the weight of the gamma ray shielding material required to
    collimate the detector also increases when larger detectors are used.
    The crystal depth is chosen such that most of the gamma rays of interest
    will lose all their energy within the crystal.
    To reduce the pile-up of low energy radiations, the crystal
    face can be covered with an appropriate shield (e.g., 0.075 cm cadmium).
    This procedure will reduce counter dead time effects without
    significantly affecting assay results.
    2.1.2Collimators for Gamma Rays
    A shaped shield constructed of any dense material is
    appropriate for gamma ray collimation. For cost, availability, and ease
    of fabrication, lead is recommended. Less than 2% of all 400 keV gamma
    rays striking a 1.5-cm-thick sheet of lead will pass through without
    having suffered an energy loss.
    The collimator will be most effective when it is concentric
    about the crystal and photomultiplier and completely covers the
    photomultiplier base. Extending the collimator forward of the crystal at
    least a distance equal to half the diameter of the crystal, and
    preferably the full diameter, is recommended.(4) Making this distance
    variable to reproductible settings will permit adjustment over a range
    of collection zone sizes.
    2.1.3Check Source for Gamma Ray Assay
    It is important to check the operation of the detection
    system prior to each inventory sequence. Either recalibrating one or
    more collection zones and comparing the results to previous analyses or
    testing the instrument with an appropriate check source is appropriate.
    When the performance remains within the expected value, the previous
    calibration data are assumed to be valid. If not, the energy window may
    have shifted, or the unit may be in need of repair and recalibration.
    An appropriate check source enables the stability of the
    assay instrument to be tested at any location. Such a source can be
    prepared by implanting a small encapsulated plutonium source
    (containing~0.5 g Pu) in the face of a plug of shielding material. The
    plug is shaped to fit and close the collimator channel, and the source
    is positioned to be adjacent to the crystal when the plug is in place.
    The check source is fabricated in a manner to ensure its
    internal stability. Other than radiations increasing from the ingrowth
    of Am-241, the emission rate of the check source should remain constant.
    2.1.4Calibration Source for Gamma Ray Assay
    To calibrate a collection zone, the observed assay response
    is compared to the response obtained when the zone contains a known
    amount of plutonium.
    Because of the complexity of the assay, the response is
    assumed to be linear. To be representative of typical holdup
    situations, the calibration standard is prepared as an encapsulated disk
    with a bed thickness of less than 0.2 cm. Care must be exercised in the
    preparation of the calibration standard to ensure that the amount
    encapsulated of total plutonium, Pu-239, and the amount of Am-241, is
    known. It is important to measure the gamma ray attenuation through the
    encapsulating material and correct the calibration standard response to
    compensate for that attenuation. The amount of plutonium encapsulated in
    the gamma ray calibration standard is selected to be representative of
    typical accumulations.
    2.2 Neutron Assay
    Neutrons are emitted in the spontaneous fission of Pu-238,
    Pu-240, and Pu-242 and through the interaction of emitted alpha
    particles with certain light nuclei. These neutrons suffer little
    attenuation in passing through uranium or plutonium or through most
    structural and containment materials. Glove box windows may reduce the
    energy of emerging neutrons, but because of their regular and constant
    shape, their effect can generally be factored into the assay
    calibration.
    To be useful for the assay of plutonium holdup, the neutron
    production rate per gram of plutonium must be known. The spontaneous
    fission contribution to the total neutron production can be computed
    from basic nuclear data, once the isotopic composition of the contained
    plutonium has been determined. Computing the (alpha,n) contribution
    requires a knowledge of the chemical form of the plutonium and the
    amount and distribution of certain high (alpha,n) yield target
    materials.
    The background count rate from neutron detectors may be a
    substantial part of the observed activity, often corresponding to as
    much as 20 g of plutonium in typical holdup assays. Thus, neutron assay
    is primarily applicable to the measurement of significant accumulations
    of plutonium.
    The measured neutron yield from prepared calibration
    standards is used to calibrate each neutron assay collection zone. In
    the Appendix, a method is given to calculate the anticipated neutron
    yield. This method provides the ability to calculate the neutron yield
    when the isotopic or impurity composition of the plutonium holdup is
    different from that of the calibration standards. The method can be
    used to calculate a ratio of the neutron production rate of the unknown
    material to the standard material neutron production rate. The yield
    from the holdup material is then determined by multiplying the measured
    "known" material yield by the computed ratio.
    2.2.1Neutron Detection Instruments
    To effectively employ the spontaneous neutron yield as a
    measure of plutonium holdup, it is necessary to detect the neutrons in
    the presence of a more intense gamma ray background and to collimate the
    detector so that the only neutrons being counted are emanating from the
    collection zone under assay.
    Holdup assay is performed under in-plant conditions where
    ruggedness, high detection efficiency, and high (gamma,n) rejection
    performance in the detectors is important. He-3 has one advantage over
    BF(3) detector tubes in that the operating voltage for He-3 tubes does
    not increase as rapidly with increased gas pressure.
    To increase the efficiency of the system, detector gas
    pressure in the tubes may be increased or multiple detectors can be
    connected in parallel to feed a common preamplifier.
    He-3 and BF(3) detectors have efficiencies which increase as
    the energy of the neutrons decrease. To take advantage of this
    characteristic, the detectors can be surrounded by a neutron moderating
    material (see Figure B-1). Polyethylene is recommended. The thickness
    of the moderator is important. When the moderating distance is short, a
    fraction of the higher energy neutrons pass through the gas chamber
    without being detected. Conversely, when the moderating distance is too
    long, a substantial number of low-energy neutrons are absorbed by the
    hydrogen contained in the moderator. A balance between these two
    effects is reached when the spacing between adjacent tubes is
    approximately one inch of polyethylene, and the spacing between the
    front of the unit and the detectors and the back of the unit and the
    detectors is approximately 1 1/4 inch when one-inch-diameter tubes are
    used, and approximately one inch when two-inch-diameter tubes are used.
    To shield the detector from low-energy neutrons which may
    produce a complicated response pattern, the moderator material is
    covered with a thermal neutron absorber. Cadmium sheeting approximately
    0.075 cm thick can be used for this application.
    2.2.2Collimators for Neutron Detectors
    To assay a specific collection zone in the presence of other
    distributed sources of plutonium, it is necessary to collimate the
    detector. This is accomplished by stopping neutrons coming to the
    detector from all directions except the desired one. The cadmium
    surrounding the detector will stop essentially all neutrons striking the
    detector with energies below 0.4 eV. By adding moderator material
    around the outside of the detector in all directions except for the
    collimator channel, neutrons coming from unwanted directions will lose
    energy in this shield and will be absorbed in the Cd cover. For each
    six inches of polyethylene added, the collimator assembly provides a
    factor of approximately ten in the directionality of the response. An
    example of a collimated neutron detector assembly for plutonium holdup
    assay is shown in Figure B-1.
    The weight of the combined detector and collimator assembly
    can easily exceed requirements for a hand-held detector probe.(4) For
    this reason, and to provide for reproducible positioning at each assay,
    a sturdy cart housing both the detector/collimator and the associated
    electronics is recommended. Further, as the items to be assayed will be
    at different heights, the ability to raise and lower the assembly to
    reproducible settings is recommended to expedite the assay and reduce
    the possibility of errors.
    2.2.3Check Source for Neutron Assay
    To ensure the proper operation of the neutron assay system
    prior to making an assay, it is necessary to test the response of the
    instrument. An appropriate neutron assay check source can be measured,
    or one or more collection zones can be recalibrated and compared to the
    results of previous calibrations.
    An appropriate neutron assay check source can be prepared by
    implanting a small encapsulated plutonium source (containing about 5 g
    Pu) into the face of a plug of neutron moderating material (see Figure
    B-2). The plug is fabricated to fit and close the collimator channel.
    2.2.4Calibration Source for Neutron Assay
    To calibrate a neutron assay collection zone, the observed
    response is compared to the response obtained when the zone contains an
    additional known amount of plutonium. Neutron assay is less sensitive
    to attenuation than is gamma ray assay. It is important to know how
    much plutonium is encapsulated in the neutron assay calibration
    standard, and the isotopic composition of that plutonium.
    The spontaneous neutron production rate from typical reactor
    plutonium is significantly less than the production rate of 375-440 keV
    gamma rays. To provide an adequate response for calibration, it is
    therefore necessary to encapsulate a larger amount of plutonium in the
    neutron assay calibration standard.
    (Due to database constraints, Figures B-1 through B-3 are not included.
    Please contact LIS to obtain a copy.)While the amount needed is best determined through an evaluation of
    typical accumulations, 100 g Pu is adequate for most applications.
    The neutron assay calibration standard may generate more
    neutrons than directly attributable to the spontaneous fission and
    (alpha,n) reactions. Because a relatively large quantity of PuO(2) is
    encapsulated in the neutron assay calibration standard, some of the
    spontaneous fission or (alpha,n) neutrons may be absorbed in Pu-239 or
    Pu-241 nuclei, producing additional neutrons through the induced fission
    reaction. The amount of multiplication depends in a complex manner on
    the amount and distribution of PuO(2) and on the surrounding medium.
    The potentially significant calibration error arising by having too
    large a neutron yield per gram of plutonium will be corrected in the
    long term through assay verification tests. In the initial phase of
    assaying holdup, a rough correction for this yield can be measured by
    preparing two additional PuO(2) sources containing 1/3 and 2/3 of the
    neutron assay calibration standard mass. These samples need not be
    encapsulated, as they will be measured only once and can then be
    returned to the process stream.
    The PuO(2) used in this test is taken from the same batch
    used to prepare the neutron assay calibration standard. After weighing
    out the proper quantities, the PuO(2) is put into containers having
    close to the same geometry as found in the neutron assay calibration
    standard. Each test sample is transferred to an empty glove box and
    positioned next to the window for measurement. The neutron assay probe
    is positioned as close as possible to the sample but outside the glove
    box. After the measurement is made, that sample is transferred from the
    glove box and the next sample is transferred in and positioned in the
    identical location for measurement. A plot of counts minus background
    as a function of PuO(2) mass is made and the points visually fitted
    using a French curve. If there is no multiplication, a straight line
    can be drawn through the origin connecting all points. Multiplication
    is indicated when the curve turns upward, indicating an increase in
    counts per gram as the mass of PuO(2) increases. A correction term is
    obtained by determining the increase in counts per gram at the mass
    value corresponding to the neutron assay calibration standard mass.
    This increase is readily determined by plotting the straight line
    through the origin and the lowest mass sample response and reading the
    difference in counts between the two lines at the abscissa coordinate
    corresponding to the neutron assay calibration standard mass. All
    measurements relating to this standard are thereafter reduced by the
    ratio of the difference in counts to the observed counts.
3. Isolation of Collection Zones
    To ensure that each collection zone is independently assayed, it
    is necessary to screen all radiations from the detector except those
    radiations emanating from the collection zone being assayed. This is
    principally accomplished through the use of the collimators described in
    Sections B.2.1.2 and B.2.2.2. Two additional means exist to further
    isolate a collection zone.
    3.1 Detector Positioning
    An unobstructed side view of a collection zone is preferred.
    When plutonium is located behind the zone under assay in another
    collection zone or a storage facility, either consider positioning the
    detector above or below the collection zone, or consider the use of
    shadow shielding.
    3.2 Shadow Shielding
    It may not be possible to avoid interfering radiations through the
    collimator design or through choosing the detector position for assay.
    In such cases, it may be possible to move a shield panel between the
    source of interfering radiations and the collimator zone under assay.
    If the shield panel is very thick and its dimensions match or exceed the
    back side of the collection zone under assay, no interfering radiations
    will penetrate through the shadow shield to the detector. While such
    characteristics are desirable, the size of such a shield would limit its
    transportability. A rectangular panel containing ~5 cm of neutron
    moderator (e.g., benelex, WEP, or polyethylene) and ~0.5 cm lead sheet
    is recommended, mounted on wheels as an upright panel. To use such a
    panel, two measurements are required.(*)(Due to database constraints, this equation is not included. Please
    contact LIS to obtain a copy.)To correct for the interference, subtract R(2) from R(1), and solve for
    R(Interference):
    (Due to database constraints, this equation is not included. Please
    contact LIS to obtain a copy.
    To ensure that this correction is sufficiently accurate, it may be
    necessary to extend the length of the normal counting period to
    accumulate sufficient counting statistics (1% statistics are generally
    adequate for this application).
4. Calibration of Collection Zones
    Each collection zone is independently calibrated, as background
    factors and the composition of each zone vary widely from zone to zone.
    A collection zone is best calibrated through the in situ measurement of
    known calibration standards. When such a program is not possible, the
    calibration can be based on the calculation of the anticipated response
    or through measuring a mockup of the collection zone of interest.(5)----------
    (*) Response terms refer to neutron or gamma response, as
    appropriate.
    ----------
    The calibration obtained through this procedure is recommended
    until a history of comparisons between predicted and recovered holdup
    quantities is developed, as described in Section B.5 of this guide.
    4.1 Detector Positioning
    To calibrate each collection zone, the best position or
    series of positions is selected to observe the collection zone with the
    least amount of interference from principal structural components. It
    is important to view the collection zone with the detector located
    between the collection zone and all areas used for Pu storage during
    inventory. A three-dimensional approach can be investigated,
    positioning the detector on top of or below the collection zone if it is
    not possible to have an unobstructed, interference-free side view of the
    collection zone. The use of shadow shielding can be explored if it is
    not possible to get a clear view of each collection zone for assay.
    On the basis of a detailed examination of the physical
    layout of the facility, some preliminary measurements are made to
    determine optimum detector positions for holdup assay. Once the assay
    positions for the detector and shadow shields are established,
    permanently marking the assay positions will facilitate subsequent
    measurements.
    4.2 Calibration Sources
    Since this assay is to measure the amount of plutonium
    holdup, it is appropriate to use plutonium as the calibration standard
    material. Further, as the plutonium holdup will generally be
    distributed over a large surface area, it is recommended that the gamma
    ray calibration standard be fabricated to resemble this characteristic,
    as described in Section B.2 of this guide.
    4.3 Calibration Procedures
    Once the principal items containing plutonium have been
    removed and the detector located in its assay position, the response
    from a calibration standard combined with the plutonium already held up
    is obtained. When the collection zone is appropriately isolated, two
    factors influence the observed response from the calibration standard:
1. the location of the calibration standard within the collection
    zone, and
2. the shielding of radiations from the calibration standard caused
    by the items comprising the collection zone.
    The geometric response variation is measured by observing
    the response from one calibration standard with the other standard
    removed from the collection zone under investigation. The calibration
    standard response is measured with the standard positioned in various
    parts of the collection zone, avoiding internal items which may
    attenuate the radiation emanating from the standard.
    When neutron assay is employed or when the collection zone
    consists of a hollow box, pipe, or duct, attenuation is either
    relatively uniform or negligibly small. The calibration of each
    collection zone then becomes a matter of appropriately averaging the
    geometric response variations. The average response of the entire
    collection zone is assumed to properly represent that zone. If,
    however, it is known that plutonium accumulates in one particular
    location within a collection zone, the response of the standard is
    emphasized when located near the principal collection site.
    If the item to be assayed consists of a large unit, assay
    performance may be enhanced by subdividing the unit into smaller
    contiguous measurement zones. The repeat dimensions of the subzones are
    determined by measuring the response while moving the standard along an
    axis perpendicular to the detector centerline. By studying the response
    curve, the distance D is selected as the point beyond which sufficient
    activity is detected to flatten the response within the subzone. Each
    subzone will measure 2D across its face. An example is illustrated in
    Figure B-3. As the response about the centerline is assumed to be
    symmetrical, only half of the traverse is indicated. In Figure B-3, D
    is selected such that the area under the curve to the right of D is
    approximately equal to the area above the curve to the left of D (Area
    A(1) approx Area A(2)). Note: the distance from the collection zone to
    the detector or the distance from the crystal face to the end of the
    collimator, or both, can be varied to divide the collection zone into an
    integral number of subzones.
    To use this relationship, the detector is first positioned
    at point d and a reading is taken. Point d is the center of the first
    subzone, selected to coincide with the physical edge of the calibration
    zone. The detector is then moved a distance 2D along the traverse to
    the center point of the second subzone, and the second measurement
    taken. The cycle is repeated to include all of the larger collection
    zone. The value interpreted for calibration for each subzone
    corresponds to the maximum of the traverse across each subzone because
    the response has been flattened. The content of the entire collection
    zone is the sum of the contributions from the subzones.
5. Estimation of the Holdup Error
    The overall uncertainty associated with the measured plutonium
    holdup is due to (1) the uncertainty in the observed response and (2)
    the uncertainty in the interpretation of that response. The random
    uncertainty components in this application are frequently negligible in
    comparison with the geometric uncertainty and the uncertainty in the
    isotopic composition. In this assay application, it is appropriate to
    estimate the assay error components by assuming the measured range
    (R(i)) of the ith fluctuation constitutes an interval four standard
    deviations wide. The midpoint of the range estimates the mean effect,
    and the distance from the midpoint to each extreme comprises an
    estimated 95% confidence interval. The error attributable to this
    effect is then approximately
    (Due to database constraints, this equation is not included. Please
    contact LIS to obtain a copy.) If a severe effect is noted, the response can often be corrected
    for the variation in the corresponding parameter by measuring the value
    of that particular parameter at the time of the assay. Using a measured
    relationship between the response and the value of that parameter, the
    observed response is corrected.
    5.1 Response Uncertainties
    5.1.1Counting Statistics
    The magnitude of the uncertainties attributable to
    variations in the geometric distribution and in the attenuation of the
    radiations are expected to dominate the total response uncertainty. The
    relative standard deviation due to counting statistics can usually be
    made as small as desired through (1) using more efficient detectors or
    (2) extending the counting period. Having 1000 to 10,000 net counts is
    generally sufficient for most holdup assay applications.
    5.1.2Instrument Instabilities
    Fluctuations in ambient temperature, humidity,
    electronic noise, and line voltage (for non-battery-powered electronic
    units) generally affect the stability of electronic systems. The
    magnitude of this uncertainty can be estimated by monitoring the check
    standard response and determining the range of variability as described
    in Section B.5 of this guide.
    5.1.3Geometric Uncertainty
    The geometrical variation in the observed response is
    measured by moving the calibration source within the bounds of each
    collection zone. Two cases are described below.
    5.1.3.1 Isolated Collection Zones
    When a single unit comprises a collection zone,
    the standard is moved to all sites within the zone at which an
    accumulation of plutonium might occur. With sufficient collimation, the
    response for the collection zone under investigation is independent of
    its neighbor zones. The average of the response, weighted to reflect
    prejudgments on the likelihood of accumulation sites, is then used as
    the calibration point. As shown in Section B.5, the range of values can
    be assumed to comprise an expectation interval four standard deviations
    wide. The geometric error is then estimated using Equation 6.
    5.1.3.2 Overlapping Collection Zones
    When a collection zone is subdivided to
    overlapping subzones, the geometric uncertainly due to the dimension
    perpendicular to the detector collection zone centerline is eliminated
    through the area-averaging calibration method described in Section 4.3.
    The uncertainty in the depth dimension in each
    subzone can be determined through the procedure outlined for isolated
    collection zones. Judgment can be used to weight the calibration data to
    emphasize principal accumulation sites.
    5.1.4 Attenuation Uncertainty
    If the attenuation is not extreme, it can be measured
    in situ, mocked up, or computed for the different conditions
    encountered. The worst and best cases can be assumed to determine the
    range of permissible effects. Using Equation 6, the magnitude of this
    uncertainty component can then be estimated. Again, judgment is
    appropriate to weight the correction factor.
    5.2 Interpretation Uncertainties
    Two factors are central to the issue here, assuming that the
    calibration standard material is similar to the held-up material.
    5.2.1Interfering Radiations
    5.2.1.1 Gamma Ray Assay
    An uncertainty in the observed gamma ray
    response may arise due to the presence of extraneous gamma ray emitters
    or due to fluctuations in the background from the Compton scattering of
    higher-energy gamma rays. The shape of the background gamma ray
    spectrum may change in such cases to such an extent that even with the
    energy windows stabilized, the background correction is irregular and
    uncertain. The magnitude of this effect is generally small. It can be
    monitored by observing the spectrum with a multichannel analyzer, but
    unless the data on periodically recovered holdup accumulations are in
    error, this contribution can be ignored.
    5.2.1.2 Neutron Assay
    A change in the neutron yield for a plutonium
    sample of fixed isotopic content is primarily attributable to the
    fluctuation in the concentration of high (alpha,n) yield impurities.(*)
    Judgment can be used to determine the range of permissible impurity
    concentrations. The variation in a typical neutron yield can then be
    predicted using the methods discussed in the Appendix of this guide.
    Again, the range of permissible variations is assumed to constitute an
    acceptance interval from which the component error is computed using
    Equation 6.
    5.2.2Isotopic Uncertainties
    If the process equipment is cleaned each time the
    isotopic composition of the plutonium feed is varied, the holdup will
    consist primarily of the current material. New calibration standards
    can be prepared or the previous yield data can be normalized using the
    methods presented in the Appendix to correct for this effect. When
    mixing occurs, use of the stream-averaged isotopic composition is
    appropriate. The uncertainty bounds are estimated by considering the
    highest and lowest fissile isotopic batches and computing the
    corresponding range.
    5.3 Holdup and Its Associated Error
    The amount of Pu holdup can be measured through the
    systematic application of the program developed in conjunction with the
    principles and pitfalls discussed herein. For each collection zone,
    measured holdup and its error can be determined.
    ----------
    (*) Over a long period of time the alpha-particle production rate
    increases due to the ingrowth of Am-241.
    ----------
    5.3.1Initial Operations
    During the initial phase of operations, the error
    associated with the in situ assay of plutonium holdup is estimated by
    combining the component errors determined in the preceding sections of
    this guide (B.5.1 and B.5.2).
    5.3.2Routine Operations
    To ensure the validity of assay predictions and to
    more realistically estimate the uncertainty in those predictions, it is
    necessary to establish a program to measure the amount of plutonium
    recovered when a collection zone is cleaned out. By comparing the
    amount of plutonium recovered to the recovery amount predicted, the
    collection zone calibration can be updated and the assay error can be
    based on relevant verification tests.
    The update data is computed as the difference in the
    assays before and after cleanout:
    (Due to database constraints, this equation is not included. Please
    contact LIS to obtian a copy.) The standard deviation in the Delta values (s(Delta))
    is computed separately for each collection zone, including no more than
    the twelve preceding measurement tests:
    (Due to database constraints, this equation is not included. Please
    contact LIS to obtain a copy.) When a value of Delta is determined, it is used to
    update the estimate s(Delta). The standard deviation estimate s(Delta)
    can be used to estimate the error in the assay prediction for the
    collection zone for which it has been established.
    The amount of plutonium collected during the cleanout
    of a specific collection zone can be assayed through sampling and
    chemical analysis, through calorimetry, or through other applicable
    nondestructive assay methods (e.g., spontaneous fission coincidence
    detection or gamma ray assay). Each of these topics is the subject of a
    Regulatory Guide.
C. REGULATORY POSITION
    To develop a program for the periodic in situ assay of plutonium
    residual holdup as an acceptable measurement method for this inventory
    component, it is necessary to consider the factors in the following
    sections.
    Note: Care must be exercised during the fabrication and use of check
    sources and calibration standards to ensure their continued integrity
    and to prevent contamination.
1. Delineation of Assay Collection Zones
    A plan of each plutonium processing facility should be examined to
    establish independent collection zones. Individual glove boxes and
    similar containment structures should be so identified. Using the
    layout and touring the facility, an assay site(s) for each collection
    zone should be selected:
1. Assay site(s) should afford a clear, unobstructed view of the
    collection zone with no other collection or storage areas in the line of
    sight of the collimator assembly. Location of the detector probe above
    or below the collection zone should be considered if an unobstructed
    side view is not possible. If an unobstructed view is not possible,
    shadow shielding should be used to isolate the collection zone for
    assay.
2. The assay site should be set back as far as possible from each
    collection zone to reach a compromise between interference from neighbor
    zones and efficient counting.
3. Gamma ray assay should be applied to measure the plutonium held up
    in all collection zones containing less than the neutron detection limit
    and for single containment structures which do not contain irregularly
    shaped structural components capable of significantly attenuating the
    emerging gamma rays. Neutron assay should be applied to measure the
    accumulation of plutonium holdup in all structures not suitable for
    gamma ray assay.
4. Each collection zone should be uniquely numbered. (Neutron
    collection zones could be preceded by an "N", gamma ray collection zones
    by a "G". Subzones should be identified by an alphabetic suffix to the
    collection zone identification.)5. Each assay site should be marked with paint or colored tape on the
    floor. (To be consistent, blue tape should be used for neutron assay
    sites, orange for gamma ray sites.) The height setting for midpoint
    assay should be recorded in the measurement log corresponding to each
    assay site.
2. Assay Instruments
    Neutron and gamma ray assay capability should be provided using
    separate or compatible electronics with interchangeable detector probes.
    Compatible electronic should provide for both He-3 or BF(3) neutron
    detection and NaI(TI) gamma ray detection. The electronics unit should
    have a temperature coefficient of less than 0.1% per degree C.
    Battery-powered electronics should be provided to expedite assays.
    2.1 Gamma Ray Assay
    Gamma ray assay should be based on the activity observed in
    the energy range from 375 keV to 440 keV, excluding the composite gamma
    ray complex centered at 333 keV. Yield data for appropriate gamma rays
    are presented in Section B.2.1 of this guide.
    2.1.1Detector Selection
    Gamma ray detectors should have FWHM resolution equal
    to or better than 7.5% at 662 keV (Cs-137 gamma ray). NaI(TI) can meet
    such specifications and is suitable for this application. The crystal
    depth should be sufficient to detect a significant percentage of 400-keV
    gamma rays. For NaI(TI), the minimum depth should be one inch. A
    two-inch depth is recommended.
    The crystal should be stabilized with a suitable
    radioactive source. An internal CsI seed containing Am-241 is
    recommended for this application. The electronics should be capable of
    stabilizing on the reference radiation emitted by the seed. The crystal
    face (external to the cover) should be covered with 0.075 to 0.150 cm
    cadmium sheet to filter low-energy radiations.
    Two single-channel analyzers should be provided with
    lock-set energy windows. One channel should be set to admit gamma rays
    from 390 keV to 440 keV unless equilibrium of the U-237 and Pu-241 can
    be assured. The 333-keV region of the gamma ray spectrum should be
    excluded. With NaI detectors, it is necessary to exclude the 375 keV
    gamma ray to ensure that the tail from the 333 keV complex is not added.
    The second channel should be set above the first window to provide a
    background correction for the assay window. This second window should
    be set from approximately 450 keV to 600 keV.
    2.1.2Gamma Ray Collimator
    A cylinder of shielding material such as lead should
    be made concentric with the gamma ray detector. The end of the cylinder
    opposite the crystal should be blocked with the shielding material. The
    thickness of the collimator should be chosen to provide sufficient
    directionality for the specific facility (1.5 cm of lead thickness
    should be sufficient for most applications). The collimator sleeve
    should be extendible over the end of the crystal to reproducible
    settings to vary the degree of collimation for different collection
    zones.
    2.1.3Gamma Ray Check Source
    To ensure the continued normal operation of each
    system, an encapsulated plutonium check source should be provided. The
    source should be small enough to be implanted in a section of shielding
    material so shaped as to close off the collimator opening. The check
    source should be positioned adjacent to the detector. The source should
    contain an amount of plutonium sufficient to provide a gross count rate
    of 1000 to 10,000 counts per second.
    2.1.4Gamma Ray Calibration Source
    To permit the calibration of gamma ray assay
    collection zones, a calibration standard should be fabricated by
    encapsulating plutonium oxide in a disk. The isotopic composition of the
    plutonium and the abundance of Am-241 should be measured and be chosen
    to be nominally representative of the plutonium being processed. The
    total amount of plutonium encapsulated should be closely monitored.
    Attenuation losses within the bed of PuO(2) and through the
    encapsulating material should be measured and the calibration standard
    response normalized to counts per gram incorporating these corrections.
    2.2 Neutron Assay
    2.2.1Neutron Detector Selection
    Neutron detectors should have high detection
    efficiency and be capable of operating in the presence of gamma
    radiation. He-3 and BF(3) neutron detectors are recommended for this
    application. Multiple detector tubes with matched operating performance
    should be connected in parallel to a single preamplifier to increase the
    overall detection efficiency obtainable from a single detector tube.
    Neutron detectors should be surrounded by a layer of neutron moderator
    material to enhance their detection efficiency. The neutron moderator
    layer should be covered with a low-energy neutron absorber to filter out
    extraneous neutrons from the desired signal. A recommended
    configuration is diagrammed in Figure B-1.
    2.2.2Neutron Collimator
    A slab collimator or concentric cylinder collimator of
    a suitable neutron moderator material (e.g., polyethylene) should be
    constructed to completely surround the detector with its associated
    moderator and filter assembly, leaving open only the collimator channel.
    A recommended configuration is shown in Figure B-1.
    The moderator thickness should be selected to provide
    the directionality required for each facility. A directionality profile
    providing a 10:1 response ratio (six inches of polyethylene) should be
    adequate for most applications; however, each situation should be
    evaluated as discussed in Part B of this guide.
    2.2.3Neutron Check Source
    Any neutron source which emits approximately
    100-10,000 neutrons/second is acceptable for this application. The
    source should be small enough to be contained within a section of
    neutron moderator material so shaped as to completely fill the
    collimator channel of the detector assembly. The source should be
    implanted directly adjacent to the neutron detectors, outside the
    cadmium thermal neutron filter. A recommended configuration for this
    assembly is diagrammed in Figure B.2.
    2.2.4Neutron Assay Calibration Standard
    To permit the calibration of neutron assay collection
    zones, a calibration standard should be fabricated by encapsulating
    PuO(2). The PuO(2) should be nominally representative of the plutonium
    being processed in isotopic composition, in Am-241 content, and in the
    content of high (alpha,n) yield target materials. The amount of
    plutonium to be encapsulated should be chosen to be representative of
    the amounts of plutonium estimated to be held up in typical neutron
    assay collection zones.
    The neutron yield of the calibration standard should
    be measured and also computed using the method described in the
    Appendix. The observed neutron count rate should be normalized.(6) If
    the predicted response differs by more than 10%, the response should be
    normalized as discussed in Section B.2.2.4.
    2.3 Service Cart
    A cart carrying electronics and both detector probes should
    be provided. The capability to raise or lower the probes to
    reproducible settings should be included.
    2.4 Notation of Operating Parameters
    When compatible electronics are used to facilitate neutron
    and gamma ray assay, a notation of the respective settings should be
    affixed to the electronics unit. To decrease the likelihood of
    incorrect settings, the neutron probe and the appropriate electronics
    settings should be color-coded blue; the gamma ray probe and
    corresponding electronics settings should be coded orange.
3. Calibration
    Each collection zone should be independently calibrated when all
    in-process material has been located so that the response from the
    calibration standards will not be influenced by the in-process material.
    3.1 Instrument Check
    The stability of the neutron and gamma ray detection systems
    should be tested prior to each inventory by comparing the observed
    counts obtained from the check source, minus the counts with the shaped
    shield in place but without the check source, to the readings obtained
    prior to previous inventories. If the measurement is consistent with
    previous data (i.e., is within plus or minus two single-measurement
    standard deviations of the mean value of previous data), all previously
    established calibrations using this detection system should be
    considered valid. If the measurement is not consistent, the operation
    of the unit should be checked against the manufacturer's recommendations
    and repaired or recalibrated, as required.
    3.2 Zone Calibration
    The geometric response profile for each collection zone
    should be determined by measuring the variation in the response as a
    calibration standard is moved within the defined limits of the
    collection zone. The response variation should then be averaged to
    determine the response per gram of plutonium for that collection zone.
    The averaging should be weighted to reflect known local accumulation
    sites within each collection zone. The response per gram should be used
    to directly translate the observed response to grams of plutonium, after
    the response is corrected for background.
    3.2.1Subzone Calibration
    When a collection zone is too large to be accurately
    measured in a single assay, the collection zone should be divided into
    overlapping subzones. The repeat dimensions of each subzone
    perpendicular to the detector-to-collection-zone line should be
    determined so that the response variation across that distance is
    nulled. Using this procedure, the residual geometric uncertainty should
    be determined by measuring the response as a calibration standard is
    moved along the depth coordinate. The calibrated response should then
    reflect the average of the depth response, weighted to reflect known
    accumulation sites.
4. Assay Procedures
    4.1 Assay Log
    An assay log should be maintained. Each collection zone or
    subzone should have a separate page in the assay log, with the
    corresponding calibration derived on the page facing the assay data
    sheet. Recording space should be provided for the date of measurement,
    gross counts, corrected counts, and the corresponding grams plutonium
    from the calibration in addition to position and instrument electronic
    setting verification.
    4.2 Preassay Procedures
    Prior to inventory, the isotopic composition of the
    plutonium processed during the current operational period should be
    determined. Variations in the neutron and gamma ray yield data from the
    calibration standard should be calculated. Either the calibration data
    or the predicted holdup should then be corrected to reflect this
    difference.
    Prior to each inventory, the operation of the neutron and
    gamma ray assay detection systems should be checked.
    Prior to any assay measurements, feed into the process line
    should be stopped. All in-process material should be processed through
    to forms amenable to accurate accountability. All process, scrap, and
    waste items containing plutonium should be removed from the process
    areas to approved storage areas to minimize background radiations.
    4.3 Measurements
    The assay cart should be moved in sequence to the assay
    site(s) corresponding to each collection zone. Assaying all gamma ray
    sites before assaying neutron sites (or vice versa) is recommended.
    Before assaying each collection zone, the operator should
    verify the floor location, probe selection, probe height, and
    electronics settings. All check and calibration sources should be
    sufficiently removed so as not to interfere with the measurement. Prior
    to taking a measurement, a visual check of the zone and the line of
    sight of the detector probe should be made to assure that no obvious
    changes have been made to the process area and that no unintended
    accumulations of plutonium remain within the collection zone. The
    operator should initial the measurement log to assure compliance for
    each collection zone.
    Having met all preceding requirements, the measurement at
    each site should be taken, recorded, and converted to grams plutonium.
    If each value is within an expected or permissible range, the cart
    should be moved to the next site and the cycle repeated. If a high
    response is noted, the cause should be investigated. If the collection
    zone contains an unexpectedly large content of plutonium, that
    collection zone should be cleaned to remove the accumulation for
    conversion to a more accurately accountable material category. After
    the cleanout has been completed, the zone should be reassayed and the
    recovered material quantity used to test the validity of the zone
    calibration.
5. Estimation of the Holdup Error
    During the initial implementation of this program, the error
    quoted for the holdup assay should be computed on the basis of
    estimating the error components, as described in Sections B.5.1 and
    B.5.2.
    Prior to the cleanout of any collection zone for whatever purpose,
    that zone should be prepared for assay and measured as described in
    Section C.4 of this guide. Following this assay, the collection zone
    should be cleaned out and the collected plutonium should then be assayed
    using an appropriately accurate assay method. When the collection zone
    has been cleaned and the collected plutonium removed, the collection
    zone should be reassayed. The recovered plutonium should be used to
    update the calibration and, from the sixth test on, should serve as the
    assay error estimate. Separate records should be maintained for each
    collection zone to estimate the error in assaying the plutonium holdup.
    To ensure that error predictions remain current, only data of the
    twelve preceding independent tests should be used to estimate the assay
    error. Collection zones not cleaned for other purposes should be
    cleaned for assay verification at intervals not to exceed two months.
    REFERENCES
1. R. Gunnink and R. J. Morrow, "Gamma Ray Energies and Absolute
    Branching Intensities for (238,239,240,241)Pu and (241)Am,"
    UCRL-51087 (July 1971).
2. J. E. Cline, R. J. Gehrke, and L. D. McIsaac, "Gamma Rays Emitted
    by the Fissionable Nuclides and Associated Isotopes," ANCR-1069
    (July 1972).
3. L. A. Kull, "Catalogue of Nuclear Material Safeguards
    Instruments," BNL-17165 (August 1972).
4. An example of a collimator for uranium gamma ray assay is found in
R. B. Walton, et al, "Measurements of UF(6) Cylinders with
    Portable Instruments," Nucl. Technol., 21, 133 (1974).
5. W. D. Reed, Jr., J. P. Andrews, and H. C. Keller, "A Method for
    Surveying for Uranium-235 with Limit of Error Analysis,"
    Gulf-GA-A12641 (June 1973).
    APPENDIX
    NEUTRON YIELD COMPUTATIONS
    The following model for the calculation of the total spontaneous
    neutron yield from plutonium-bearing materials assumes that the
    plutonium is widely dispersed. With this condition, there will be no
    significant neutron production created through induced fission of Pu-239
    or Pu-241. The total neutron yield per gram of plutonium holdup will
    then be the sum of the spontaneous fission and (alpha,n) contributions:
    (Due to database constraints, this equation is not included. Please
    contact LIS to obtain a copy.)1. Spontaneous Fission Neutrons
    To determine the spontaneous neutron yield per gram of plutonium
    held up within a collection zone, the isotopic composition of the
    plutonium and uranium (if present) must be known. The contribution from
    spontaneous fission can generally be calculated by neglecting the
    contribution from U-238:
    (Due to database constraints, this equation is not included. Please
    contact LIS to obtain a copy.)2. (alpha,n) Neutrons
    The major contribution to the total neutron production from
    (alpha,n) reactions will typically be due to the O-18 (alpha,n) Ne-21
    reaction when the plutonium exists as the oxide. The yield from this
    reaction per gram of plutonium can be calculated using the isotopic
    weight fractions (W(i)) and the Y(i) yield data given in Table 1.
    (Due to database constraints, this equation is not included. Please
    contact LIS to obtain a copy.) The yield per gram of PuO(2) is calculated by multiplying the
    yield per gram of plutonium by the gravimetric dilution factor
    (Pu/PuO(2) Congruent 0.882).
    The presence of certain impurities can contribute substantially to
    the total (alpha,n) production rate. Approximate values of (alpha,n)
    impurity yields for the highest yield (alpha,n) target materials are
    given in Table 2. To compute the impurity (alpha,n) contribution, the
    total alpha particle production is determined. Production rates of
    alpha particles per gram of the principal nuclides of interest are shown
    in Table 1. This contribution to the total neutron yield can be
    computed using the relationship:
    (Due to database constraints, this equation is not included. Please
    contact LIS to obtain a copy.)(Due to database constraints, Tables 1-4 are not included. Please
    contact LIS to obtain a copy.)(Due to database constraints, this equation is not included. Please
    contact LIS to obtain a copy.)3. Sample Calculation (PuO(2)-UO(2)) Consider the case of recyle plutonium blended to 3 wt % Pu in a
    normal UO(2) matrix, where the isotopic composition is Pu-238 (.25%),
    Pu-239 (75.65%), Pu-240 (18.48%), Pu-241 (4.5%), Pu-242 (1.13%), and
    Am-241 (.28% of Pu).
    For mixed oxides, the oxygen density is approximately the same for
    the case of PuO(2). This fact, together with the atomic similarity of
    uranium and plutonium, justifies the assumption that the oxygen
    (Alpha,n) yield per gram of mixed oxide is the yield per gram of PuO(2),
    further reduced by the blending ratio, Pu/(Pu + U).
    Using the values given in Table 1, the spontaneous fission yield
    and total Alpha production per gram of plutonium can be computed.
    Results are shown in Table 3.
    The alpha particle yield of plutonium is constant in time for all
    intents. However, the Am-241 Alpha production increases at a rate which
    results in approximately a 0.3% increase per month in the total Alpha
    production, for the range of plutonium isotopic compositions intended
    for reactor fuel application.
    In the present example, the impurity levels of the principal
    (Alpha,n) target materials are shown in Table 4. The neutron yields
    attributable to (Alpha,n) interactions on those impurities are also
    shown in Table 4, calculated using the Alpha particle production rate of
    5.3 x 10E9 Alpha/sec-g Pu, computed above. In this example, the mixed
    oxides are composed of blended PuO(2) and UO(2) particles approximately
    40 microns in diameter. If the particle size were smaller or the mixed
    oxide was created through coprecipitation, the uranium impurity content
    would also contribute to the plutonium (Alpha,n) yield. This
    contribution can be ignored for large particles and estimated by
    combining the impurities for small particles and coprecipitated oxides.
    The total neutron yield in this example is 380 n/sec-g Pu. In
    this example, the percentage of plutonium to the total Pu + O is 0.8835.
    Using this gravimetric dilution factor, the neutron yield is 336 n/sec-g
    PuO(2). If the PuO(2) is blended with UO(2) to 3%, i.e., PuO(2)/PuO(2)
    + UO(2) = 0.03, the neutron yield from the blend will be 10.1 n/sec-g
    MO.
    13