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In Vivo Measurement Sensitivity and Occurrence of Radionuclides
in Residents of the Carlsbad, New Mexico Area

Introduction

    Citizen volunteers from the Carlsbad, New Mexico area were monitored for internally deposited radionuclides through a project entitled "Lie Down and Be Counted" (LDBC). This project is provided as an outreach service to the public to support education about naturally occurring and man-made radioactivity present in people and the environment prior to the opening of the Waste Isolation Pilot Plant (WIPP). The data collected prior to the opening of the WIPP facility will provide information for future studies and serve as a baseline for operational monitoring. In addition, information obtained from these measurements will be used to evaluate and reduce the uncertainties associated with bioassay methodologies. It is important to note that these data represent an interim summary of an ongoing study.

Methods

    Following the commissioning of the Center's in vivo monitoring facility, 272 citizen volunteers were assayed during July 1997 to September 1998. These volunteers were recruited through presentations to local community groups and businesses. When a citizen volunteer arrived at the Center for a bioassay, he or she viewed a short video explaining the measurement protocol, and completed a lifestyle questionnaire which included questions regarding age, sex, ethnicity, occupation, foreign travel, wild game consumption, smoking habit and any nuclear medicine procedures (Table 12). In addition, the subject's height and weight were recorded.

Measurement System     Lung and whole body counts were simultaneously performed with the subject positioned horizontally using two arrays of hyper-pure Ge detectors. Each array consisted of four detectors and represented a specific detector design, low energy (LEGe) and coaxial (COAX). The primary function of the LEGe detector array was lung counting (7 to 250 keV). Each LEGe detector was fitted with a 0.6 mm thick carbon composite entrance window. The active diameter, area, and thickness of each LEGe detectors as 70 mm, 3800 mm2, and 20 mm, respectively. The function of the second detector array (COAX detectors) was to measure higher energy photons (100 to 2000 keV) emitted from radionuclides deposited in the whole body. The active diameter, length, and relative efficiency of the COAX detectors were 75 mm, 76 mm, and 80%, respectively. The high energy (1333 keV) resolution performance of the LEGe detectors was matched to that of the COAX and was added, using additional signal processing electronics, to the signal from the COAX detectors to increase the sensitivity of the whole body count.

    The counting shield consists of a large shielded room measuring 2.7 m wide, 3.0 m long, and 2.7 m high. It is constructed from 25 cm-thick cast iron obtained from pre-World War II iron. A graded-Z liner (Z represents the charge of the liner element) consisting of 64 mm of lead, 32 mm of tin, and 32 mm of stainless steel was added to the inside of the iron walls of the shield to attenuate photons produced within the shield walls.

    Radionuclides analyzed for in lungs included 232Th, 144Ce, natural U, 235U, 226Ra, 233U, 155Eu, 210Pb, 237Np, Pu isotopes, 241Am, 244Cm, and 252Cf. Radionuclides analyzed for in the whole body included 40K, 51Cr, 54Mn, 58Co, 59Fe, 60Co, 65Zn, 88Y, 95Zr, 103Ru, 106Ru, 125Sb, 131I, 133Ba, 133I, 134Cs, 137Cs, 140Ba, 141Ce, 152Eu, 154Eu and 192Ir (Table 13). A 30-min count time was used for each subject.

Data Analysis     The proprietary software package ABACOS Plus from Canberra Industries was used for routine calibration, operation, data analysis, and data archival. This software was specially developed for in vivo applications and is currently employed at in vivo facilities located at General Electric Nuclear, Wilmington, North Carolina; Savannah River Plant, Aiken, South Carolina; Rocky Flats Environmental Technology Site, Golden, Colorado; Oak Ridge National Laboratory, Oak Ridge, Tennessee; Mound Site, Mound, Ohio; Fernald Site, Fernald, Ohio; and Lawrence Livermore National Laboratory, Livermore, California.

    The identification of radionuclides of interest was accomplished using a library-driven peak search and a library-driven region of interest (ROI) analysis. The concept of 'library driven' means that only the portions of the spectrum that would contain the photons of interest (usually listed in a library) are examined.

Peak Search Analysis     A peak search was the first analysis performed on the spectral data. In simplified terms, a peak was identified by approximating, through a correlation function, the second derivative of each channel in the spectrum (Canberra, 1991, Nuclide Identification Algorithms and Software Verification and Validation Manual, 07-0464). When the algorithm is sampling a portion of the spectrum that contains no peaks, the second derivative should approach zero. When a peak is encountered, the second derivative will become positive and remain so until an inflection point is reached. At the inflection point, the second derivative will become negative and increase to a very large negative value just past the apex or centroid of the peak. When these conditions occurred within the spectrum, a peak was considered identified. The peak ROI, background and net counts were determined for identified peaks as described below. Region of Interest Analysis     A region of interest, centered at a given photon energy, was established for all radionuclides regardless of whether or not a peak was identified as described above. For radionclides that were not identified by the peak search, the width of the ROI was determined by multiplying a constant by the calibrated resolution of the spectrometer at the photon energies of interest. Constants of 2 and 3 were empirically determined and verified for radionuclides deposited in lungs and whole body, respectively. Typical ROI widths for radionuclides in lungs were 25 channels and for radionuclides in whole body were 13. For radionuclides identified by the peak search, the ROI width was determined as the channels on both sides of the centroid, where the second derivative returned to zero.

    Background and net counts for each ROI were calculated using a step-background computation. This computation calculates the background counts for each channel (i) in the ROI of interest (Bi) using the following equation:


equation 1

where Yj is the total counts in channel j, L is the left starting channel of the ROI, R is the right ending channel of the ROI, Lavg is the average value of the Compton continuum on the left side of the ROI determined from the sum of four channels to the left of L, and Ravg is the average value of the Compton continuum on the right side of the ROI determined from the sum of four channels to the right of R.Next,the total background counts for the region of interest (BT) were calculated by summing Bi from channels R to L. Finally, the net count rate in the ROI was calculated by subtracting BT from the observed gross counts and dividing by the count time.

Decision Level (Lc) and Minimum Detectable Amount (MDA)     To determine whether or not activity has been detected in a particular person, the parameter, Decision Level (LC) was used. The LC represents the 95th percentile of a null distribution that results from the differences of repeated, pair-wise background measurements. An individual result (net count rate) was assumed to be statistically greater than background if it was greater than LC. It is important to recognize that the use of this criterion (LC) will result in a statistically inherent 5% false positive error rate per pair-wise comparison (5% of all measurements will be determined to be positive when there is actually no activity in the person). Decision levels were calculated using the following equation based on the recommendations of HPS N13.30 (Performance Criteria for Radiobioassay, May 1996):

equation 2

where Cgross is the total gross counts in the region of interest and t is the count time in seconds.

    The value of MDA indicates the ability of a facility to detect a radionuclide in a person. The MDA represents the amount of a radionuclide that, if present, would be detected 95% of the time under routine operation of a facility. The MDA is used to measure the efficacy of a facility, but it should not be used to decide if a specific radiobioassay has or has not detected activity within a person. MDA was calculated using the following equation (HPS N13.30, Performance Criteria for Radiobioassay, May 1996):

equation 3

where K0.05 is the calibration factor, taking into consideration counting efficiency and self absorption, that represents the 5th percentile in distribution of individual specific calibration factors; U is a conversion factor taking into account photon yield, radioactive decay during the counting interval and unit conversion; t is the count time in seconds; SB1 is the standard deviation, including Poisson and other random error components in the count of a subject, determined by the routine measurement procedure, where the subject contains no actual analyte activity above that of the appropriate blank; and SB0 is the standard deviation, including Poisson and other random error components, in the unadjusted count of an appropriate blank. The term SB1 was determined from the measurement of 272 and 271 individuals for radionuclides deposited in lungs and whole body, respectively (a single whole body count was invalidated due to instrument malfunction). The term SB0 was determined from 20 measurements of a bottle manikin absorption (BOMAB) phantom filled with de-ionized water.

    It is important to note that the use of K0.05 applies to lung counting where individual-specific calibration factors vary with subject chest wall thickness. For example, in this study individual-specific calibration factors for 238Pu ranged from 4E-5 to 4E-7. For radionclides deposited in the whole body, a single calibration factor per photon energy is applied to all individuals regardless of anthropomorphic characteristics. Historically, the variability associated with K in lung counting has been ignored, resulting in unrealistically low estimates of MDA for radionuclides deposited in lungs.

    Calibration factors for lung counting were determined as a function of photon energy and muscle equivalent chest wall thickness (MCWT) using the humanoid torso phantom developed by Lawrence Livermore National Laboratory, 100% muscle equivalent chest plates, and 238Pu and 241Am/152Eu lung sets. Calibration factors for whole body counting were determined using a BOMAB phantom filled with a muscle equivalent epoxy containing 152Eu and 40K.

    For plutonium isotopes, 244Cm and 252Cf, the MCWT was determined from the subject's height, weight and age using Equation 4 (Sumerlin, T. J. and S. P. Quant, 1982, Radiation Protection Dosimetry, 3, 203):


equation 4

where Wa is the subject's weight (kg), Ha is the subject's height (m) and A is the subject's age. The total thickness of tissue composing the chest wall (CWT) was determined for the remaining radionuclides in lungs using Equation 5, which represents a composite of the work performed by Fry (Fry, F. A., 1980, Health Physics, 39, 89), Garg (Garg, S. P., 1977, Health Physics 32, 54) and Dean (Dean, P. N., 1973, Health Physics, 24, 439):


equation 5

where Wb is the subject's weight (lb) and Hb is the subject's height (inch). It is important to note that this predictive equation is not normalized to muscle equivalent thickness and will result in a conservative estimate of calibration factors (Vickers, L. R., 1996, Health Physics, 70, 346). The calibration factors selected for the MDA calculation for plutonium isotopes, 244Cm and 252Cf (photon energies less than 20 keV) corresponded to the 95th percentile of the MCWT (K is inversely proportional to MCWT) determined from Equation 4. The calibration factors selected in the calculation of MDA for the remaining radionuclides in lungs (photon energies greater than 20 keV) corresponded to the 95th percentile of CWT determined from Equation 5. This value of CWT was then converted into muscle equivalent chestwall thicknesses for each photon energy greater than 20 keV (MCWT>20 keV) using Equation 6 (Krammer, G. H., et. al. 1998, Health Physics, 74, 594):


equation 6

where mmsc,i is the linear attenuation coefficient at photon energy i for muscle (cm-1), madp,iis the linear attenuation coefficient at photon energy i for adipose (cm-1) and AMF is the adipose mass fraction. The AMF for male and females were assumed to be 0.34 and 0.64, respectively (Vickers, L. R., 1996, Health Physics, 70, 346). A single value of AMF, weighted by the proportion of males and females in the cohort, was used for the calculation of MCWT>20 keV.

Results and Discussion

Cohort Demographics     Demographic characteristics (Table 12) of the LDBC cohort are generally consistent with the survey published by CERMC in 1998 entitled "Survey of Factors Related to Radiation Exposure and Perception of Environmental Risks in Carlsbad, Loving, Malaga, and Hobbs" and the 1990 Census for citizens living in Carlsbad. With respect to gender, ethnicity, and lifestyle, the current LDBC cohort is reasonably representative of the citizens living in the vicinity of the WIPP. The largest deviations of the LDBC demographics from those of the 1990 census were the over-sampling of males and under-sampling of Hispanics by 12.7 and 19.4 %, respectively. Interestingly, the 1998 CEMRC survey study (cited above) also under-sampled Hispanics, to an even greater degree, relative to the 1990 Census. The LDBC project is ongoing, and future recruitment efforts will focus on enrolling additional females and Hispanics. However, the 1998 CEMRC survey and current study results suggest that the recruitment of Hispanics, in proportion to the 1990 Census, will be difficult. In addition, it is important to note that if the presence of a radionuclide is dependent on a subclass of interest (gender, ethnicity,etc.), valid population estimates can still be made by correcting for the proportion of under- or over-sampling for the particular subclass. Background Rates and Variability     The variance in background count rates generally decreased with photon energy for each count type (e.g. lung or whole body count) and source of background (e.g. human subjects or BOMAB phantom, Fig. 39 and 40). This is expected, since the counting efficiency of the instrument decreases with photon energy. Background rates of a whole body count were generally greater than that of a lung count. This also would be expected, since whole body counts were performed with eight detectors compared with four for lung counts, and the primary whole body counting detectors (COAX) are massive relative to the lung counting detectors, resulting in greater background due to increased intrinsic efficiency and photon/cosmic ray interaction cross sections.

    The difference in background rates between the human subjects and the BOMAB phantom were greater for lung counts than whole body counts, where the BOMAB phantom provided a reasonable estimate of human subject background at energies less than 700 keV. The energy response or shape of the background spectrum was well approximated by the BOMAB phantom, especially for a lung count (Fig. 39). For both lung and whole body counts, repeated measures of the BOMAB phantom underestimated the variance in human subject background (Fig 40).

    The variance to mean ratio (Fig. 41) in human subject background for a lung and whole body count was consistently greater than one. This has important implications to whole body and nuclear counting, since it is often assumed that background is characterized by a Poisson distribution. With a Poisson distribution, the variance to mean ratio is one, and the best estimate of the mean response is that observed (Knoll, G. F., 1989, Radiation Detection and Measurement, John Wiley & Sons Inc., New York). If there are no other sources of variability, then the mean, variance and standard deviation of a count result (e.g. background) can be estimated from a single measurement. For these data, if the Poisson assumption is applied and the human background was estimated from the measurement of single subject or phantom (often the case), the variability in background would have been underestimated by as much as a factor of 10, but in all cases at least a factor of 2. Underestimating the variability of background will result in an unrealistically low estimate of measurement sensitivity.

Minimum Detectable Amount     The range, mean and 95th percentile of MCWT (Equation 4) for plutonium isotopes, 244Cm and 252Cf were 1.7 to 4.9, 2.7 and 3.6 cm, respectively. The range, mean and 95th percentile of CWT  (Equation 5) were 1.0 to 6.8, 3.1 and 5.0 cm, respectively. The 95th percentile of CWT when converted to MCWT>20 keV (Equation 6) ranged from 3.6 cm at 47 keV to 4.7 cm at 440 keV (Table 13).

    MDAs calculated as described herein for radionuclides in lungs ranged from 6.2E+00 Bq for 235U to 3.1E+04 Bq for 239Pu (Table 13). MDAs for radionuclides in the whole body ranged from 1.4E+01 Bq for 88Y to 1.9E+02 for 40K. Values of MDA reported herein are a factor of 2 to 12 greater than those reported in the CEMRC 1997 Report. The reasons for the increases are threefold. First, values of MDA reported in 1997 were based on repeated measures of a BOMAB phantom filled with 140 g of K (reference man level). Although this is standard practice in bioassay programs throughout the U.S., the data reported herein demonstrated that such methodology underestimates the variability in human background (Fig. 40 and 41). Based on a priori assumptions, a CWT value of 2.4 was used for calculations in the CEMRC 1997 Report to determine K0.05for MDA calculation of radionuclides in lungs. Finally, the previous calibration for radionuclides in lungs was based on phantom overlays consisting of 50% muscle and 50% adipose equivalent materials. A calibration based on 50% muscle/50% fat overlays has less photon attenuation because of the adipose content than that used for the current data (100% muscle overlays).

    Values of MDA reported herein are more realistic than the MDAs as typically calculated, because the variability and magnitude of human subject background and population based calibration factors (K0.05) have been considered. It is important to note that most facilities, especially those for lung counting, do not calculate MDA in this manner. Typically, an average or more ideal value of CWT (corresponding to K) is selected for the MDA calculation. However, such methodology can be quite misleading when applied to a population of individuals whose body shapes and sizes are unknown a priori. For example, the reported MDA applies only to those individuals with a CWT less than or equal to that assumed in the MDA calculation. If the assumed value of CWT was the average of a population, then 50% of the individuals in the population would have a CWT greater than the assumed value, resulting in a non-detect lung count for a lung burden equal to the reported MDA. In contrast, for this study only 5% of the population would be expected to have a CWT thickness greater than that assumed for the MDA calculation (in this case MCWT). Thus, the MDA reported herein would result in only 5% of the population having a non-detect lung count for a lung burden equal to the reported MDA at the 95% confidence level.

Results Greater Than LC     As previously discussed, the criterion, LC, was used to evaluate whether a result was in excess of background, and the use of this criterion will result in statistically inherent 5% false positive error rate per pair-wise comparison (5% of all measurements will be determined to be positive when there is no activity present in the person). For a particular radionuclide, to evaluate whether the frequency of results greater than LC was consistent with a false positive error rate, a binomial statistical approach was applied. For example, if a radionuclide was not present in the sample population, the frequency of results greater than LC should fall within the distribution-free confidence interval for a proportion equal to the error rate. The width of the confidence interval is dependent on the sample size (in this case, 272 and 271 for lung and whole body counts, respectively), the proportion of interest (5%) and level of confidence (95%). A frequency of results greater than the distribution-free confidence interval, for a radionuclide not present in the shielded room background (defined as a 24-hour count of the BOMAB phantom), would suggest a low frequency baseline of occurrence in the local population. The term ‘distribution-free’ refers to the idea that the derived statistical interval does not require any distributional assumptions with regards to the data being evaluated (Hahn, J. and W.Q. Meeker, 1991, Statistical Intervals A Guide for Practitioners, John Wiley & Sons, Inc. New York).

    Using the ROI methodology, the percentage of results greater than LC were consistent with a 5% random false positive error rate, at the 95% confidence level, for all radionuclides except 232Th via 212Pb, 235U / 226Ra, 60Co, 137Cs, 40K, 54Mn, 103Ru, 232Th via 228Ac and 65Zn (Table 14). Five of these (232Th via 212Pb, 60Co, 40K, 54Mn (228Ac interference), and 232Th via 228Ac) are part of the shield-room background and positive detection would be expected at low frequency. The percentage of results greater than L for 103Ru and 65Zn were below the 95% confidence interval for the random false positive error rate and may be statistical anomalies (38 comparisons to the confidence interval were made). 40K is a naturally occurring isotope of an essential biological element, so detection in all individuals is expected. 137Cs and 235U / 226Ra are not components of the shielded room background and were observed at frequency greater than the 95% confidence interval for the false positive error rate (discussed in more detail later). In addition to false positive rates, the ROI methodology appeared to be effective with respect to false negative error rates (Table 15). For example, 24-hour measurements of the BOMAB phantom were used to determine an equivalent human body burden for shield contamination from the Th series and 60Co. Theoretically, if a subject had a body burden equal to LC, the detection of that radionuclide at LC would be missed, when actually present (false negative), 50% of the time. The false negative error rate would then increase as the body burden becomes smaller relative to LC until eventually no activity would be detected. In all cases, shield contamination was equivalent to body burdens at levels below LC and false negative error rates consistent with theory were observed.

    In contrast, the peak search methodology did not perform as well as the ROI methodology with respect to false positive and false negative error rates and low activity radionuclide detection (Table 14). While valuable to the practice of bioassay, this observation has little impact on this study because the ROI methodology was used for the detection and quantification of radionuclide activity.

    40K results were positive for all individuals, ranging from 2308 to 6513 Bq with an overall mean (±SE) of 3293 (±784) Bq. Such results are expected since K is an essential biological element contained primarily in muscle, and a constant fraction of all naturally occurring K is the radioactive isotope 40K. The mean 40K value for males (±SE), was 4730
(± 46) Bq, which was significantly greater (P < 0.0001) than that of females, which were 3507 ± 39 Bq (mean ± SE). This result was also expected since, in general, males tend to have larger body sizes and greater muscle content than females.

    In 27.8% of individual measurements, the value for 137Cs was greater than L ranging from 6 to 25 Bq. This percentage was significantly higher than the distribution-free confident interval for a 5% random false positive error rate (2.2 to 7.4%), suggesting a low frequency baseline occurrence of 137Cs in the local population. From these data, detectable 137Cs is present in 22% to 33% (95% confidence level) of citizens living in the Carlsbad area. These results are consistent with preliminary conclusions that were reported in the CEMRC 1997 Report and not unexpected, since 137Cs is an abundant, long-lived fission product. Because of its abundance, mobility, and physiological properties, 137Cs is widely distributed throughout the biosphere and has been detected previously in many organisms including humans (Whicker, F.W. and V. Schultz, 1982, Radioecology: Nuclear Energy and the Environment 1, CRC Press, Inc., Florida).

    Individual 137Cs results were then compared to two sources of demographic data to determine whether the presence of 137Cs was dependent on a particular demographic or lifestyle parameter using a Chi-square test of independence (L. Ott, 1988, An Introduction to Statistical Methods and Data Analysis, PWS-Kent Publishing Company, Boston, MA; Table 16). The presence of 137Cs was independent of gender, ethnicity, age, radiation work history, consumption of wild game, nuclear medical treatments and European travel. Occurrence of detectable 137Cs was slightly associated (p = 0.032) with smoking habit, where smokers had a higher prevalence of 137Cs relative to non-smokers (21.3 to 11.2%, respectively). These data are interesting because 137Cs is often assumed to be correlated to the consumption of wild game, but this pattern did not appear in these data. The association of 137Cs with smoking habit is also interesting, and could be related to the presence of fallout 137Cs in tobacco. However, the statistical significance of this dependence was weak, and further study is warranted.

    The percentage of results greater than L for 235U/226Ra (9.9%) was significantly (although slightly) higher than the distribution-free confidence interval for a 5% random false positive error rate (2.2 to 7.4%). These data are not nearly as suggestive, when compared to 137Cs, of low frequency baseline occurrence of 235U/226Ra. It is important to note that 235U and 226Ra are naturally occurring and these two radionuclides cannot be distinguished via gamma spectroscopy. Therefore, any positive signal could be the result of either or both radionuclides. This effect was not apparent in the initial data reported in the CEMRC 1997 Report and requires a larger sample size to support or reject the apparent pattern.