8. V. A. Shevchenko et al., Radiobiologiyi, 21, No. 5, 780 (1981).

9. D. Grahn et al., in: Biological Implications of Radionuclides Released from Nuclear

Industries, volume I, IAEA, Vienna (1979).
i0. Yu. I. Moskalev et al., The Concept of BiologicalRisk from the Action of Ionizing Ra-
diation [in Russian], Atomizdat, Moscow (1973).
ii. V. A. Knizhnikov, Gigiena Sanitariya, No. 3, 96 (1975).
12. E. E. Pochin, IAEA Bull., 2-1, No. 4, 44 (1979).
13. Radiation Safety Standards (NRB-76) [in Russian], Energoizdat, Moscow (1981).
14. Z. Jaworskii, IAEA Bull., 24, No. 2, 38 (1982).

A COMPARISON OF METHODS OF DETERMINING THE CONCENTRATIONS

OF 222Rn DECAY PRODUCTS IN AIR

M. V. Terent'ev and E. M. Krisyuk UDC 614.876:543.27:546.296

Natural environmental radioactivity is the main source of background irradiation for the
population. The largest contribution to the effective equivalent dose from this source is
produced by the daughter decay products (DDP) from 222Rn [i]. To determine this contribution,
one examines the contents of the DDP in the air of buildings and underground structures (pits,
tunnels, caves, etc.) together with the factors influencing the concentrations.
The most common methods of determining the DDP concentrations are those due to Kusnetz
[2] and Thomas [3] and modifications of these, as well as the rapid methods due to Rolle [4]
and Markov [5]. Here instead of the original methods due to Kusnetz and Thomas we consider
a modification of the method of [2] proposed by Nazaroff [6] and the method of [3] as modified
by Groer [7]. All these methods enable one to determine the concentration of the equivalent
equilibrium radon (EER)* responsible for the radiation dose to human lung tissue. Also,
Markov's and Thomas's methods enable one to determine the concentrations of the individual
DDP and as a result to estimate the ventilation rate. These methods differ in laboriousness
and in systematic errors, as well as in sensitivity and in statistical error.
SYSTEMATIC ERROR IN DETERMINING EER CONCENTRATIONS
The systematic error in determining EER concentrations arises from the unknown shift in
the equilibria between the DDP and it occurs in Kusnetz's, Rolle's, and Markov's methods.
In Thomms's method, in which one determines three values for the DDP concentration from three
measurements on the activity of a filter, there is no systematic error. In the other methods,
the systematic error is dependent on the duration of the air sampling and on the times at
which the measurements on the filter activity start and end. Kusnetz's method is also
affected by the numerical value of the Kusnetz factor: the coefficient for converting from
the number of counts recorded in the measurement on the filter activity to the EER concen-
tration in the sample of air passing with a known speed through the filter.
To estimate the systematic error, we selected at random i0 values for the shift in equi-
librium b e t w e e n t h e DDP, each of which was uniquely determined by two numbers R~ and R=:

Rt = CjC,; R2 = CJCt, (t)

where C~, C2, and C3 are the concentrations of the DDP 2XSPo(RaA), 2x~Pb(RaB), and =~4Bi(RaC)
correspondingly.

*The EER concentration is the radon concentration such that the short-lived DDP in equilib-
rium with it have the same level of latent energy as is characteristic of the atmosphere with
the measured radon concentration.

Translated from Atomnaya ~nergiya, Vol. 55, No. 5, pp. 310-313, November, 1983. Original
article submitted ~ r c h 9, 1983.

0038-531X/83]5505-0763507.50 9 1984 Plenum Publishing Corporation 763

 TABLE l. Calculation of ~ for i0 Values
of the Equilibrium Shift between DDP and
A in the Determination of EER Concentra-
tion by the Methods Considered

8,%

-method
- - _ of
_ [2] [m et h- ] meth-
RI R2 second!third o .of od of
[51
mrm form form ( ~ ; ]
I I 12) ] (~;o~;
(10;40; (t0;40;(t0.~0.]

1 t 1 0 0 0 0 --9,t
2 0,9 0,75 --I,0 --1,2 --1,9 -4-4,5 --4,1
3 0,8 0,6 --1,3 --1,6 --2,8 -4-6,9 - - t , 4
4 0,7 o,5 --1,0 --1,4 --2,8 +7,9 --0,3
5 0,6 0,4 --0,6 --1,t --2,8 -4-9,2 .4.1,0
6 0,5 0,3 --0,4 --0,7 --2,8 -4-tt,1 -4-2,9
7 0,4 0,2 +0,8 --0,t --2,8 ,4,13,8 +5,8
8 0,3 0,t5 +3,2 .4.2,t --0,7 -[-t3,0 -4-4,7
9 0,2 0,t -4-6,9 -4-5,8 -4-2,7 ,+tt,8 +2,9
10 0,i 0,05 +13,8 t-i2,5 -,~8,9 -4-9,5 --O,t
A % 5,3 4,8 3,8 t0,2 4,4

*The first number is the sampling time,

while the second and third are the times
for the start and end of the activity
measurement, with recording started at the
end of the sampling in min.

Table I gives results on the relative systematic error $ for the I0 values of the equi-
librium shift together with the relative standard deviation A for each method. In calculating
the systematic error, the Kusnetz factor was determined from the equilibrium condition for the
DDP for the three forms of the method (selected out of 40 forms considered by Nazaroff).
The minus sign indicates that the true value of the EER concentration is overestimated by that
method, while plus indicates an underestimation. The systematic error is least in the third
form, but it increases with the equilibrium shift; approximately the same systematic error oc-
curs in Markov's method, while Rolle's method has a relatively large systematic error. A
similar picture is evidently to be expected for any other choice of values for the equilibrium
shift between the DDP.
SENSITIVITY IN METHODS OF DETERMINING EER CONCENTRATIONS
The minimal EER concentration [(CoF)min] is determined by the throughput of the air-
sampling device, the background in the measuring equipment, and the method used, where Co is
the 222Rn concentration, while F is the factor for the equilibrium shift between 22iRn and
the DDP. We derive (CoF)mi n for equilibria between the DDP on the basis of the known value
for the statistical error gc (note that here CoF = C, where C is the concentration in pCi/
liter). Then for Kusnetz's method

Cmln = (t + V ~ + 8nbaZAT)12a2eBKv; (2)

for Rolle's method

Cm,~= (t + V t + 48nbO~)/140eno~v; (3)

for Markov's method

Cml n = (t -~-V t + 24n bO2)/7to~e~lv; (4)

and for Thomas's method

Cm~ = (1 + 1/1 + 0.45nba2)/t5o2~lv. (5)

764
 TABLE 2. Relative Standard Deviations in
Determining the EER Concentrations by the
Methods Considered as Calculated for Var-
ious Equilibrium DDP Concentrations

method of [2] ] method meth-Imeth-

od of od of:
p(~i / first second thud [5] [3]
liter form form form

t(D 0,02 0,014 0,009 0,02 0,028 O,t)6

t0 0,063 0,046 0,029 0,063 0,089 ] 0,19
t 0,2 0,t44 0,09 0,2 0,28 0,6
0,1 0,63 0,455 0,286 0,628 0,885 t ,9

TABLE 3. Relative Standard Deviations Gci/C

in Determining the Concentrations of Individ-
ual DDP Calculated for Various Equilibrium
Concentrations

method of [5] method of [31

(5; i--~; 7--I0)* (5; I--5;6--20;21--30)*
Deviation.
C, pCi/liter
t06 1 ,o I , 1 ~ I '0~ I '0 I ' I ~

(e~cllC)l/vlO,t62[0,51211,62[5,12]0,22610,71612,26517,16
(acJC) 1/v[0,028 0,08910,28 ]0,885[0,086[0,272[0,86 [2,72
((JcnlC)1/~'[0,06S 0,2O [0,63 ]2,00 [0,088[0,279 0,88 2,79
*The first number is the sampling time,
while the second and third are the times
for the start and end of the activity mea-
surement, with recording started at the
end of the sampling in min~

Here n b is the background count rate in count/min, e is the efficiency in a-ray record-
ing, ~ is the performance of the filter with allowance for a-ray self absorption, AT is the
time used in measuring the filter activity in min, v is the air-sampling device throughput in
liter/min, and K is the Kusnetz factor, which was taken as 69, 134, and 339 correspondingly
for the first, second, and third forms of the method in count.min/pCi (i Ci = 3.700• i0 *~ Bq).
With ~ = 0.25, gn = 0.36, and n b = 0.15 count/min, from (2)-(5) we get Cmi n = 0.69/~;
0.38/~; 0.18/~ correspondingly for the first, second, and third forms of Kusnetz's method,
while Cml n = 0.90/~, 1.32/~, and 5.8/~ correspondingly for Rolle's, Markov's, and Thomas's
methods. This shows that Thomas's method has the worst sensitivity, while the best occurs
in the third form of Kusnetz's method, which Nazaroff recommended for use when low DDP con-
centrations are expected.
STATISTICAL ERROR IN DETERMINING EER AND DDP CONCENTRATIONS
A statistical error inevitably arises in determining EER and DDP concentrations in the
measurement of the filter activity, which is dependent on the throughput of the air-sampling
device, the DDP concentration, the background, and the method used.
If the filter activity is measured not more than three times, then the EER concentration
(CoF) and the DDP concentrations (C,, C2, Ca) are found in general form from the following
expression (in pCi/liter):

Ci= J 9 a~N~, i = t , 2 , 3 for ] m a ~ = 2 , 3; (6)

CoF----aN, for jmax ----i.

765
 TABLE 4. Comparison of Methods of Deter-
mining EER in Air

Method
A ((~cIc)l/~' Time
(pCi/min)t/2 OminV' required,
(~in/)
min

[2] (first form) 0,053 0,2 0,69 55

[2] (second form) 0,048 O,144 0,385 6O
[2] (third second) 0,038 0,09 0,t84 8O
[4] O,t02 0,2 0,696 17
[51, 0,04~ 0,28 t,32 t5
[31 None 0,6 5,846 35

Here Nj is the number of pulses recorded (with background subtracted) in measurement j on the
filter activity, while a- i and a in pCi/liter,min are numerical coefficients dependent on the
feed and throughput in t~e sampler, the times at which the filter activity measurement starts
and stops, the a-ray recording efficiency, the filter efficiency, and the decay constants of
the DDP, while Jmax is the number of filter activity measurements (Jmax = i for Kusnetz's and
Rollers methods, 3max = i, 2 for Markov's method, and Jmax = 3 for Thomas's method). We use
a Poisson distribution to describe the decay of the DDP on the filter in order to calculate
the relative standard deviations (coefficients of variation) Oci/C i in determining the DDP con-
centrations and ~cof/CoF in determining the EER on the basis of the following general formulas:

%'max "Tmax
l GcJC'= V ,=IEa],Njl"j~,= a,'Ni, (7)
J i=t, 2, 3 for ]max--'~2, 3;
I. ocoFICoF= for ]o,,,x = 1.

In (7) we have not incorporated the contribution from the background to the relative standard
deviations. With ~ = 0.36, n b = 0.15 count/min and the general expression for the number of
pulses recorded Nj [8] we can neglect the contribution from the background to Oci/C i and
~cof/CoF as calculated for equilibrium between the DDP provided that ~C i = vC ~ i pCi/mln.
Here the maximum error in determining Oci/C i and on~o~~/CoF is 2-3% and will decrease as vC
increases. The inequality vC E 1 pCi/min can be met, since usually 9 ~ i0 liter/mln and
C ~ 0.i pCi/liter.
Table 2 gives values Of the relative standard deviation Oc/C in determining the EER con-
centrations as multiplied by V ~ for different equilibrium DDP concentrations. We see that
at a given sampler rate, the largest statistical error occurs in Thomas's method and the least
in the third form of Kusnetz's method. If we take 0.i pCi/liter as the minimum measurable
EER concentration for all the methods, then with a statistical error ~ = 0.25 the throughput
of the sampling device must be in the range 1.8-58 liter/min for the various methods. On
the basis of these values (each for the corresponding method), the statistical error in all
the methods is shown by Table 2 to be less than 8% for C = i pCi/liter and to fall to %2.5%
as the DDP concentration rises at C = I0 pCi/liter or to < 1% for C = i00 pCi/liter.
Markov's method (with two filter activity measurements) and Thomas's method enable one
to determine the concentrations of the individual DDP, in contrast to Kusnetz's and Rolle's
methods. Table 3 gives values of (~c./C)~Z~ for the various equilibrium DDP concentrations.
9 . i . .
We see that the statlstlcal errors in determznlng the concentrations of the individual DDP
under otherwise equal conditions are less in Markov's method relative to Thomas's one by
factors of 1.4-3.
Table 4 illustrates the accuracy and sensitivity in determining the EER concentrations by
the above methods, and it gives the required times. Thomas's method is the most accurate,
while Rolle's method has the lowest accuracy. The lowest value of Cmi n occurs in the range
0.18/v -- 5.8/v pCi/liter, ~ t h the highest sensitivity occurring in the third form of Kusnetz's
method as proposed by Nazaroff and the worst in Thomas's method. To make the sensitivities of

766
the two methods equal, Thomas's method would require an air sampler of 3 2 t i m e s the produc-
tivity (consequently more cumbersome) than that required in the third form of Kusnetz's method.
Therefore, Thomas's method is usually employed only to determine the concentrations of indi-
vidual DDP, which enables one to judge the frequency of air exchange in a building. Kusnetz~s
method has the best accuracy (leaving aside Thomas's method) and sensitivity when the throughput
of the sampler is suitably chosen along with the times for starting and ending the filter
activity measurements; an air sampler of low throughput and small size is required. There-
fore, the method is widely used in field measurements (particularly in underground structures).
The deficiency is the long time interval between the start of sampling and the end of the mea-
surement. Rolle's and Markov's rapid methods enable one to determine the EER concentrations
more rapidly. Rolle's method has a sensitivity about twice as good as Markov's method, but
it is the least accurate of all those considered. An important advantage of Markov's method
relative to Rolle's and Kusnetz's methods is that if two measurements are made on the filter
activity it enables one to determine the EER concentration and also the concentrations of the
individual DDP. However, although it is a more informative method and requires little time
(15 min) it is less sensitive.

LITERATURE CITED
i. Sources and Actions of Ionizing Radiation: Report of the UNO Scientific Committee on the
Actions of Atomic Radiation for 1977 to the General Assembly, Vol. i, UNO, New York (1978).
2. H. Kusnetz, Am. Industr. Hyg. Assoc. Q., 17, 85 (1956).
3. J. Thomas, Health Phys., 19, 691 (1970).
4. H. Rolle, ibid., 22, 233 (1972).
5. K. P. Markov, N. V. Ryabov, and K. N. Stas', Trudy SNIIP, Issue 2, Atomizdat, Moscow
(1965), p. 183.
6. W. W. Nazaroff, Health Phys., 39, 683 (1980).
7. P. Groer, Ann. Rep. ANL-7860, Part II (1972), p. 285.
8. Fu-Chia Yang and Chia-Yong Tang, Health Phys., 34, 501 (1978).

767