EPA 520/5-73-006
    A COMPARISON  OF CaF2:Mn AND LiF
      THERMOLUMINESCENT DOSIMETERS
FOR  ENVIRONMENTAL  RADIATION  MONITORING
                    J. E. Partridge
                    S. T. Windham
          Eastern Environmental  Radiation Facility
                    P. 0. Box 3009
                Montgomery, Alabama 36109

                       J. Eakins
             Florida State Health Department
                    P. 0. Box 6635
                 Orlando, Florida 32803

                      J. Lochamy
          Department of Environmental Engineering
                  University of Florida
                  Gainesville, Florida
             ENVIRONMENTAL PROTECTION AGENCY
              Office of Radiation Programs
                  Waterside Mall East
                  401 M Street, S.W.
                Washington, D.C. 20460

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                                  PREFACE
      The Eastern Environmental Radiation Facility participates in the identification
of solutions to problem areas as defined by the Office of Radiation Programs. The
Facility provides analytical capability for evaluation  and assessment of radiation
sources through environmental  studies and surveillance and analysis.  The EERF
provides  technical assistance to the State and local health  departments in their
radiological health programs and provides special analytical support for EPA Regional
Offices and other federal government agenciesjs requested.
                                         Charles R. Porter
                                          Acting Director
                          Eastern  Environmental  Radiation  Facility

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    A  Comparison  of Calcium  Fluoride:Manganese  and
      Lithium  Fluoride  Thermoluminescent  Dosimeters
           for Environmental  Radiation  Monitoring
Introduction

      Several chemical and physical forms of thermoluminescent dosimeters (TLD's)
are commercially available, and each type  has its special advantages and special
applications. Two commonly used types of  TLD's for environmental monitoring are
calcium fluoride:manganese activated and lithium fluoride Each of the two types has
several advantages and some disadvantages.

      The primary advantages of lithium fluoride are negligible fading (five percent
per year at twenty degrees centigrade) and energy independence from the keV to MeV
energy ranges (1).

      The major advantage  of calcium fluoride:manganese over lithium fluoride is
sensitivity. The calcium fluoride:manganese is approximately 3 times more sensitive
to 60Co gammas than lithium fluoride (2).

      This report gives the results of a study conducted by the Eastern Environmental
Radiation Facility (EERF), the University of Florida (U of F), and the Florida Division of
Health (FDH). The study  was  designed tc  compare and evaluate  environmental
ambient  radiation  monitoring programs   using lithium  fluoride  and   calcium
fluoride:manganese TLD's.

      The study was conducted in conjunction with a  preoperational radiological
survey at the Crystal River Unit 3  Power Plant site, Crystal River, Florida. The pre-
operational survey is being conducted by the FDH and the U of F.

      As part of the Pre-Operational Radiological Survey at the Crystal River site, the
University of Florida  conducts  an extensive TLD monitoring program using lithium
fluoride TLD's. The University of Florida has sixteen TLD  stations on or near the site.

      The Florida Division of Health is also conducting  a pre-operational survey at
the Crystal River site. Their survey includes a network of five TLD stations (all off-site)
to  monitor  the ambient  gamma  radiation levels.  The  State  uses   calcium
fluoride:manganese, glass encapsulated TLD's.

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      The EERF is currently involved in ambient radiation monitoring at several
nuclear  plants.  This ambient monitoring is in conjunction with several short-term
strategic studies which  are  designed to meet specific objectives. The EERF uses
calcium fluoride:manganese, glass-encapsulated  TLD's in the ambient monitoring
program.
Objectives

      The objectives'of this study were to answer any questions concerning the
validity of reported ambient gamma radiation  levels at the Crystal River site and to
compare the results of TLD monitoring programs using the two types of TLD's. The
second objective is especially important  to the Office of Radiation Programs of EPA
which routinely relies on ambient radiation levels reported by various agencies using
different types of TLD's.
Study Design

      A total of eight sites in the vicinity of the Crystal River plant were selected for
"cross-check" purposes. Each of the sites was previously used by either the U of F
or the FDH as a TLD monitoring station. Five of the sites were located inside thin
aluminum storage buildings. The remaining three sites were located on wooden
stakes approximately one meter above ground. A total of eight TLD's were positioned
at each  site - - four lithium fluoride and four calcium fluoridermanganese.

      The study was continued for approximately four months, (two 1 -month and one
2-month monitoring periods). At the end of each monitoring period the TLD's were
read out and repositioned at their respective location.
Procedures

       During the study each group performed their ambient monitoring programs
using their normal operating procedures in order to obtain typical results.

       A brief description of each procedure follows:
                    University of  Florida  (Lithium fluoride)

       The University of Florida uses the Eberline TLR-5 integrating reader for readout
of lithium fluoride ribbons. The reader is set for a 6-second pre-heat to 150 degrees

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centigrade  with a  12-second readout to 250 degrees centigrade. A set of 200
dosimeters (TL-100) was divided into two pools of 100 for routine background
measurements. The pools are alternated each month so that each pool is  in the
laboratory every other month where quality control measures are taken to remove
ribbons which exhibit any anomalous behavior. The dosimeters used by the University
for this present study were drawn from these pools and handled in the routine manner
established at the University and described below.

       Before being placed in the field, the dosimeters are "zeroed" by cycling them
through the reader once or twice. No formal pre-irradiation batch annealing procedure
is used. High temperature annealing is necessary only when the TLD is to be exposed
to low levels following a high level exposure history. Four ribbons are zeroed at once,
allowed to cool, and placed in a TLD shipping vial with polystyrene packing (see figure
1). The vials are wrapped in aluminum foil to make them light-tight and sealed in thick
polyethylene bags along with identification tags.

       After the desired'exposure time, the TLD's are recovered and post-annealed
for  10 minutes  in boiling water to remove the low  temperature components.  The
dosimeters are  read out one  at  a time in  a nitrogen  atmosphere. The  reader
background is determined by recycling several TLD's just after they have been read.
The  recycled response  is taken as  background. All responses are  recorded  and
computer analyzed for quantitative exposure.

       A calibration factor is determined by exposing field packaged TLD's to one of
two NBS tre.ceable sources (226Ra or s°Co). The  sources have been cross-checked and
given the same calibration factor. Calibrations are performed at least once every three
months and as often as monthly.
                   Eastern  Environmental  Radiation Facility
                        (Calcium fluoride:manganese)
      The dosimeter used by the EERF is the EG&G model TL-15 (figure  2). This
dosimeter consists of two hot- pressed calcium fluoride:manganese activated chips
which are held on  either side of a flat heating element. The chips and the  heating
element are enclosed in a glass envelope which is filled with carbon dioxide. When
in use the glass envelope is placed in an energy-compensating shield which reduces
the over-response of calcium fluoride:manganese to low energy radiation. The reader
used was the EG&G model TL-3 equipped with a low noise photomultiplier  tube.

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   SEALED VIAL
LIGHT/WATER TIGHT
                  PACKING
                  PACKING
                                                   VIAL
                                                                    ALUMINIUM
                                                                        FOll
                        Figure  1.   Details of Shipping Vial
                 :- ».•••• -... s'v'-• .•.;,-!.•. S'•"•'

                  ; v  • ' • . • , "•! _.

                  '   . .  '--'  :
                                            v^,-   I
                                               ~ '
                         Figure  2.   EG&G TL-15 Dosimeter

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      Prior to  this study the  EERF and  the Tennessee Valley  Authority (TVA)
concluded  a joint project to evaluate the suitability of this type dosimeter for
environmental radiation monitoring purposes (3). The results of this project showed
that each individual dosimeter should be calibrated. This calibration was performed
using an NBS calibrated 226Ra source. The joint EERF-TVA project also indicated the
importance of knowing the self-dosing characteristics of this type dosimeter. As a
result of this study, individual determinations of self-dosing characteristics for each
dosimeter were performed.

      The dosimeters are annealed or "zeroed" just prior to being positioned on
location. This annealing process is performed using either the TL-3 reader or an EERF
designed and constructed  portable electronic annealer (4). This annealer duplicates
the heating function of the EG&G TL-3 reader and  further annealing is not required
when working with environmental  levels (3,4).  After annealing, the dosimeters are
divided  into groups of three.and placed in  zip-lock plastic bags for protection from
moisture. The dosimeters are now ready to be positioned at the desired field locations.

      Following the desired exposure period the dosimeters are collected and read
out. These raw  readout values are computer analyzed to calculate the average
exposure rate in microroentgens/hour at each  site. The computer program  applies
the appropriate correction  factor and self-dosing correction for each dosimeter.
                         Florida Division  of  Health
                        (Calcium fluoride:manganese)
      The Florida  Division  of  Health uses  the EG&G  model TL-15  calcium
fluoridermanganese activated TLD in its ambient radiation monitoring program. A
Victoreen 2600B TLD reader is used for reading and annealing of the dosimeters.

      A total of five FDH TLD sites surround the Crystal River Nuclear Power Facility.
The TLD monitoring program at Crystal  River was begun  in  April,  1971.  These
dosimeters are collected and read on a monthly schedule. One TLD is located at each
site.

      The Division of Health TLD program is set up to look for trends in the ambient
radiation levels and has made no attempt to report the actual  background values.
Hence,  the internal  background of  the TLD's arising from the 40K  in the  glass
encapsulation has not been subtracted from reported values in the past. The self-
dosing values are available for some dosimeters,  however.

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6

Results

       The results of the three monitoring periods are given in table 1. Only the results
of the EERF and the U of F dosimeters are shown. Since the FDH looks only for trends
in the ambient radiation levels and not actual background levels, their results are not
shown for this comparison.

       An indication  of the precision or reproducibility of  both (EERF and U of  F)
systems can be determined  by calculating the mean of the one sig'ma error terms
given in table 1. The results of this calculation show a  precision of 2.6% for the
calcium fluoride:manganese  system and 3.3% for the lithium fluoride system.

       Table 2  shows the average  reading in microroentgens/hour at each site for
the entire  study period.  Also shown  in table  2  is  the  ratio  of  the  calcium
fluoride:manganese average  to the lithium fluoride average at each site.

       The dosimeters at sites  1-5  were located inside aluminum storage buildings
and sites 6-8 were on wooden  stakes one meter above ground. Analysis of the ratios
(column 4, table 2) shows that the calciu.vi fluoride:manganese results are 16% lower
than the lithium fluoride results at sites 1-5. A similar analysis for sites 6-8 shows
the calcium fluoride:manganese results 30% lower than the lithium fluoride.
Discussion and Conclusions

      The precision or reproducibility of the two systems, approximately 3%, is very
good.

      The difference in the average microroentgens/hour values for the two systems,
approximately 16% in one group and 30% in the other, is significant. This percentage
is approximately 2 microroentgens/hour at these levels. At higher exposure rates the
percentage difference would probably decrease. Several factors such as calibration
procedures, energy response or sensitivities might account for this difference.

      The differences  in energy response of the two systems probably account for
the variation in results  between  sites 1-5  and sites  6-8.  Due to  the  energy-
compensating shield the calcium fluoride:manganese dosimeter has a low energy
threshold of approximately 80 keV (5). The lithium lower energies. Since the  storage
building acts as an effective shield against the very low energy radiation (80 keV) the
lithium fluoride  dosimeter would record an increased exposure rate outside the
building. However, due to its  low energy cut-off the calcium fluoride:manganese
dosimeter would record little or no difference in the two locations. Due to this fact

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                      Table  1.  Ambient Radiation Levels - Crystal  River, Florida
                                   (microroentgens/hour  ±  sigma')
4/17-5/22
Site No.
Calcium
Fluoride:
Lithium
Fluoride
Manganese
1
2
3
4
5
6
7
8
44
4.9
6.2
4.4
5.0
4.3
6.3
4.4
±
±
±
±
±
±
±
±
.1
.1
.1
.1
.4
.1
.2
.1
5.2
6.2
8.5
5.4
6.4
7.4
9.2
7.3
±
±
±
±
±
±
±
±-
.1
.1
.5
5
.2
.4
.3
2
5/22-6/26
Calcium
Fluoride:
Lithium
Fluoride
Manganese
4 6
49
6 1
4.5
53
43
5.8
4.5
±
±
±
±
±
±
±
±
1
.1
.1
.1
.1
.1
.1
.1
5.3
5.4
7.5
5.5
6.2
5.4
8.1
5.8
±
±
±
±
±
±
±
±
.5
2
.1
.2
.1
.1
2
1
6/26-8/31
Calcium
Fluoride:
Lithium
Fluoride
Manganese
4.4
5.1
5.9
4.3
4.9
4.1
5.0
4.2
±
±
±
±
±
±
±
±
.1
.3
.1
.1
.2
.1
.1
.1
5.2
5.5
7.3
9.1
5.2
5.0
7.3
5.7
±
±
±
±
±
±
±
±
.1
.3
.1
.1
.1
.1
.1
.2
     Error  bounds  are  one standard  deviation of the  mean
Note: calcium fluoride  manganese  results  are an average of three dosimeters per
site  and lithium  fluoride results are  an average of  four  dosimeters  per site.

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8

great care should be  taken to position the TLD's  at sites with similar shielding
characteristics for routine monitoring.

       Regardless of any errors in determining the true or actual exposure levels, the
precision of either system is adequate for environmental monitoring purposes.
However, even with this degree of precision it would be difficult to detect an increase
of 5 mR  per year in the  ambient radiation levels due to the  variations in  natural
background during the year.
                      Table  2   Average Exposure  Rates at Each Site
        Site
Calcium  Fluoride:
Manganese  micro-
roentgens/hour
^  sigma"
Lithium Fluoride
microroentgens/
hour  -j- sigma*
Ratio + Sigma*
Calcium  Fluoride:
Manganese/Lithium
Fluoride
1
2
3
4
5
6
7
8
4
5
6
4
5
4
5
4
5
0
1
4
1
2
7
4
±
±
±
±
±
±
±
±
14
26
16
13
43
.14
57
.16
5
5.
7
5.
5.
5
8.
6
2
7
8
3
9
9
2
3
±
±
±
±
±
±
±
±
55
50
76
58
.58
.14
.86
.78
85
87
.78
83
85
.71
.70
.70
±
±
±
±
±
±
±
±
.03
09
.08
09
11
.14
.10
.03
        '  Standard Deviation of a Single Reading

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                                                                        9

                               REFERENCES

1.     Cox, F. M.: New Solid UF TLD. Harshaw Chemical Company.

2.     Cameron,  Suntharalingam, and  Kenny:   Thermoluminescent Dosimetry.
      University of Wisconsin Press, Madison, T968.

3.     Partridge, Windham, Lobdell, and Oppold: Suitability of Glass-Encapsulated
      CalciunrManganese  Thermo- luminescent Dosimeters for Environmental
      Radiation Monitoring.  ORP/EERF 73-1, U. S. Environmental Protection Agency,
      1973.

4.     Windham,  Kelley, and Plant:  Portable Annealer far Thermoluminescent
      Dosimeters. ORP/EERF 73-3, U. S. Environmental Protection Agency, 1973.

5.     Edgerton Germeshausen and Grier, Laboratory Products Division, Data Sheet
      No. 36, Goleta, California.

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