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Radiation Physics for Medical Physiscists - E.B. Podgorsak

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8.3 Radioactive Series Decay

269

The rate of change dND/dt in the number of daughter nuclei D is equal to the supply of new daughter nuclei D through the decay of P given as λPNP(t) and the loss of daughter nuclei D from the decay of D to G given as [−λDND(t)], i.e.,

dND/dt = λPNP(t) − λDND(t) = λPNP(0) e−λPt − λDND(t) ,(8.21)

where NP(0) is the initial number of parent nuclei at time t = 0.

The parent P follows a straightforward radioactive decay process with the

initial condition NP(t = 0) = NP(0), as described by (8.7)

 

NP(t) = NP(0) e−λPt .

(8.22)

We are now interested in obtaining the functional relationship for the number of daughter nuclei ND(t) assuming an initial condition that at t = 0 there are no daughter nuclei D present. The initial condition for the number of daughter nuclei ND is thus as follows:

ND(t = 0) = ND(0) = 0 .

(8.23)

The general solution of the di erential equation given by (8.21) will be of the form

ND(t) = NP(0)

peλP t + deλD t ,

(8.24)

where p and d are constants to be determined using the following four steps:

1. Di erentiate (8.24) with respect to time t to obtain

 

dN

−pλPeλPt − dλDeλDt .

 

dtD = NP(0)

(8.25)

2. Insert (8.24) and (8.25) into (8.21) and rearrange the terms to get

e−λPt {−pλP − λP + D} = 0 .

(8.26)

3.The factor in curly brackets of (8.26) must be equal to zero to satisfy the equation for all values of t, yielding the following expression for the constant p:

p =

λP

(8.27)

λD − λP .

4.The coe cient d depends on the initial condition for ND at time t = 0, i.e., ND(t = 0) = 0 and may now be determined from (8.24) as

p + d = 0

 

 

(8.28)

or after inserting (8.27)

 

d = −p =

λP

(8.29)

 

.

λD − λP

270 8 Radioactivity

The number of daughter nuclei ND(t) of (8.24) may now be written as follows:

ND(t) = NP(0)

λP

eλPt − eλDt .

(8.30)

λD − λP

Recognizing that the activity of the daughter AD(t) is λDND(t) we now write AD(t) as

AD(t) =

NP(0)λPλD

eλPt − eλDt

 

 

 

λD − λP

 

 

= AP(0)

λD

 

 

 

eλPt − eλDt =

 

λD − λP

 

=

 

 

P(0)

1

 

 

 

 

 

 

 

 

 

A

 

 

 

 

 

 

eλPt

eλDt

 

1 λD

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

λP

 

 

 

 

 

 

= AP(t)

 

λD

 

 

 

1 − e(λD−λP)t ,

(8.31)

λD − λP

 

where

AD(t) AP(0) AP(t)

is the activity at time t of the daughter nuclei equal to λDND(t), is the initial activity of the parent nuclei present at time t = 0, is the activity at time t of the parent nuclei equal to λPNP(t).

8.3.2 Characteristic Time

Equation (8.31) represents several general expressions for the activity AD(t) of the daughter nuclei D and predicts a value of zero for AD(t) at t = 0 (initial condition) and at t = (when all nuclei of the parent P and daughter D have decayed). This suggests that AD(t) will pass through a maximum at a specified characteristic time (tmax)D for λP =λD. The characteristic time (tmax)D is determined by setting dAD/dt = 0 at t = (tmax)D and solving for (tmax)D to get

λPeλP(tmax)D = λDeλD(tmax)D

(8.32)

and

 

 

ln λP

 

(tmax)D =

λD

(8.33)

 

.

λP − λD

Equation (8.33), governed by the initial conditions at t = 0

 

AP(t = 0) = AP(0) and AD(t = 0) = 0

(8.34)

may also be expressed in terms of half-lives (t1/2)P and (t1/2)D as well as in terms of mean-lives τP and τD for the parent P nuclei and daughter D nuclei,

8.3 Radioactive Series Decay

271

respectively, as

 

 

 

 

 

 

 

 

ln

(t1/2)D

 

 

 

 

 

 

 

 

 

 

 

 

 

(tmax)D =

 

 

 

 

 

 

 

(t1/2)P

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

1

 

 

 

 

 

 

 

 

1

 

 

 

 

 

 

 

 

 

ln2

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

(t

 

 

 

)

 

 

(t

 

 

 

)D

 

 

 

 

 

 

 

 

 

 

1/2

 

P

 

 

 

1/2

 

(t1/2)D

 

 

 

 

 

(t1/2)P(t1/2)D

 

 

ln

 

 

 

 

 

 

=

 

(t1/2)P

 

(8.35)

(t1/2)D (t1/2)P

 

 

 

 

ln2

 

and

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

τD

 

 

 

 

 

 

 

 

τPτD

 

 

 

 

τP

 

 

 

(tmax)D =

 

ln τP

 

 

 

=

 

 

 

 

ln

.

(8.36)

1

 

 

 

 

1

 

 

τP − τD

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

τD

 

 

 

 

τD

τP

 

 

 

 

 

 

 

 

8.3.3 General Form of Daughter Activity

Equations (8.33), (8.35) and (8.36) show that (tmax)D is positive and real, irrespective of the relative values of λP and λD, except for the case of λP = λD for which AD(t) in (8.31) is not defined.

At t = (tmax)D, we get from (8.31) that AP[(tmax)D] = AD[(tmax)D], i.e., the activities of the parent and daughter nuclei are equal and the condition referred to as the ideal equilibrium is met. The term ideal equilibrium was introduced by Robley Evans to distinguish this instantaneous condition from other types of equilibrium (transient and secular) that are defined below for the relationship between the parent and daughter activity under certain special conditions.

For 0 < t < (tmax)D, the activity of parent nuclei AP(t) always exceeds the activity of the daughter nuclei AD(t), i.e., AD(t) < AP(t).

For (tmax)D < t < ∞, the activity of the daughter nuclei AD(t) always exceeds, or is equal to, the activity of the parent nuclei AP(t), i.e., AD(t) AP(t).

Equation (8.31), describing the daughter activity AD(t), can be written in a general form covering all possible physical situations. This is achieved by introducing variables x, yP, and yD as well as a decay factor m defined as

1. x: time t normalized to half-life of parent nuclei (t1/2)P

 

x =

t

,

(8.37)

(t1/2)P

2.yP: parent activity AP(t) normalized to AP(0), the parent activity at t = 0

yP =

AP(t)

= eλPt

[see (8.8) and (8.22)] ,

(8.38)

 

AP(0)

 

 

 

272 8 Radioactivity

3.yD: daughter activity AD(t) normalized to AP(0), the parent activity at t = 0

yD =

AD(t)

,

(8.39)

 

AP(0)

 

 

4.m: decay factor defined as the ratio of the two decay constants, i.e.,

λPD

m =

λP

=

(t1/2)D

,

(8.40)

λD

 

(t1/2)P

 

 

 

 

 

Insertion of x, yD, and m into (8.31) results in the following expression for yD, the daughter activity AD(t) normalized to the initial parent activity AP(0)

yD = 1 − m e

 

− e

 

 

= 1 − m

 

2x

2 m

. (8.41)

1

 

x ln 2

 

x

ln 2

1

 

1

 

1

 

 

 

 

 

 

 

m

 

 

 

 

 

 

x

 

Equation (8.41) for yD as a function of x has physical meaning for all positive values of m except for m = 1 for which yD is not defined. However, since (8.41) gives yD = 0/0 for m = 1, we can apply the L’Hˆopital’s rule and determine the appropriate function for yD as follows:

 

 

d

 

1

 

 

 

1

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

yD(m = 1) = lim

dm

 

2x −

2x/m

 

 

 

 

 

 

d

 

 

 

 

 

 

 

 

m→1

 

 

(1

 

m)

 

 

 

 

 

 

dm

 

 

 

 

 

 

 

 

 

x

 

 

 

 

x

 

 

 

 

 

2m ln 2

 

 

x

 

 

lim

 

 

m2

 

 

 

 

 

 

 

 

= (ln 2)

2x .

(8.42)

= m→1

 

 

 

 

1

 

 

 

Similarly, (8.15) for the parent activity AP(t) can be written in terms of variables x and yP as follows:

yP = eλPt = ex ln 2 =

1

,

(8.43)

2x

 

 

 

where x was given in (8.37) as x = t/(t1/2)P and yP = AP(t)/AP(0) is the parent activity AP(t) normalized to the parent activity AP(0) at time t = 0.

The characteristic time (tmax)D can now be generalized to xmax by using

(8.37) to get the following expression:

 

(xmax)D =

(tmax)D

.

(8.44)

 

 

(t

1/2

)

 

 

 

 

P

 

Three di erent approaches can now be used to determine (xmax)D for yD in (8.41)

1. Set (dyD/dx) = 0 at x = (xmax)D and solve for (xmax)D to get

(8.45)

 

dx x=xmax = 1

 

 

 

m 2−x + m 2m x=xmax = 0 .

 

dyD

 

 

 

ln 2

1

 

x

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

max

D

 

we finally get

 

 

 

Solving (8.45) for (x

)

 

 

 

 

 

 

(xmax)D =

m

 

 

 

log m

=

m ln m

.

 

(8.46)

 

 

 

 

 

 

 

m − 1

log 2

m − 1

ln 2

 

8.3 Radioactive Series Decay

273

Fig. 8.2. Variable yD of (8.41) against variable x for various values of decay parameter m. The dashed curve is for yP of (8.43) against x. The parameter (xmax)D shown by dots on the yP curve is calculated from (8.46). Values for (yD)max are obtained with (8.49)

For m = 1 (8.46) is not defined; however, since it gives xmax = 0/0, we can apply the L’Hopital’s rule to get (xmax)D|m→1 as follows:

 

 

 

 

 

 

d(m ln m)

 

 

 

 

 

 

 

(x

max)D|m→1

lim

 

 

dm

 

 

 

 

 

 

 

 

 

d(m−1)

 

 

 

 

 

= m

1

ln 2

 

 

 

 

 

 

 

 

dm

 

 

 

 

 

 

 

 

 

= lim

1 + ln m

 

=

1

 

= 1.44 ,

(8.47)

 

 

 

ln 2

ln 2

 

 

m→1

 

 

 

 

 

 

Thus, (xmax)D is calculated from (8.46) for any positive m except for m = 1. For m = 1, (8.47) gives xmax = 1.44.

2.Insert (8.37) and (8.40) into (8.33) for (tmax)D and solve for (xmax)D to get the result given in (8.46).

3.Recognize that when x = (xmax)D the condition of ideal equilibrium applies for (8.41), i.e., yP[(xmax)D] = yD[(xmax)D]. Insert x = (xmax)D into (8.41) and (8.43), set yP[(xmax)D] = yD[(xmax)D], and solve for (xmax)D to get the result of (8.46).

In Fig. 8.2 we plot (8.41) for yD against x using various values of the decay factor m in the range from 0.1 to 10.0. For comparison we also plot yP of (8.43) against x (dotted curve).

The function plotted as a dashed curve for m = 1 in Fig. 8.2 is the function given in (8.42). The point of ideal equilibrium for this curve occurs at xmax given as (1/ ln 2) = 1.44 in (8.47) and at yD(xmax) = 1/e = 0.368.

274 8 Radioactivity

All yD curves of Fig. 8.2 start at the origin at (0,0), rise with x, reach a peak at (xmax)D, as given in (8.46), and then decay with an increasing x. The smaller is m, the steeper is the initial rise of yD, i.e., the larger is the initial slope of yD. The initial slope and its dependence on m can be determined from the derivative dyP/dx of (8.45) by setting x = 0 to get

dx

x=0 =

1 m

2−x + m

2m x=0 =

m .

(8.48)

dyD

ln 2

1

 

x

 

ln 2

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

Noting that x = t/(t1/2)P, m = λPD, and yD = AD(t)/AP(0), we can link the data of Fig. 8.2 with physical situations that occur in nature in the range

0.1 < m < 10. Of course, the m region can be expanded easily to smaller and larger values outside the range shown in Fig. 8.2 as long as a di erent scale for the variable x is used.

As indicated with dots on the yP curve in Fig. 8.2, (ymax)D, the maxima in yD for a given m, occur at points (xmax)D where the yD curves cross over the yP curve. The xmax values for a given m can be calculated from (8.46) and (yD)max for a given m can be calculated simply by determining yP(x) at x = xmax with yP(x) given in (8.43). We thus obtain the following expression for (ymax)D:

(y ) = y (x

) = 2( 1−m ) ln 2

=

1

 

e 1−m ln m

 

 

m ln m

 

 

m

max D P

max D

 

 

 

 

 

 

2(xmax)D

 

 

 

= e(ln 2)(xmax)D ,

 

 

 

(8.49)

where (xmax)D was given by (8.46). Equation (8.49) is valid for all positive m with the exception of m = 1. We determine (yD)max for m = 1 by applying the L’Hˆopital’s rule to (8.49) to get

 

 

 

 

 

 

d

 

 

(m ln m)

 

 

 

 

(y

 

 

 

 

 

dm

ln m+1

1

 

 

 

 

 

 

 

 

 

 

 

 

 

 

d

 

 

 

 

 

)

D|m=1

= lim 2

 

 

 

(1−m) ln 2

= lim 2 ln 2

= 2

ln 2

 

dm

 

max

m→1

 

 

 

 

m→1

 

 

 

 

 

 

= e1 = 0.368 .

 

(8.50)

As shown in (8.49), (ymax)D and (xmax)D are related through a simple exponential expression plotted in Fig. 8.3 and also given by (8.43) with x = (xmax)D and yP = (ymax)D. As shown in (8.49) the ideal equilibrium value (ymax)D exhibits an exponential decay behavior starting at (ymax)D = 1 at (xmax)D = 0 through (ymax)D = 0.5 at (xmax)D = 1 to approach 0 at

(xmax)D → ∞.

Figures 8.4 and 8.5 show plots of (ymax)D and (xmax)D, respectively, against m as given by (8.49) and (8.46), respectively, for positive m except for m = 1. The m = 1 values of (xmax)D and (ymax)D, equal to 1/ ln 2 and 1/e, respectively, were calculated from (8.47) and (8.50), respectively. With increasing m, the parameter (xmax)D starts at zero for m = 0, goes through 1/ ln 2 = 1.44 at m = 1, and then increases as ln m for very large m. Parameter (ymax)D, on the other hand, starts at 1 for m = 0, goes through 1/e = 0.368 at m = 1, and then decreases exponentially for very large m.

8.3 Radioactive Series Decay

275

Fig. 8.3. Parameter (ymax)D against parameter (xmax)D as given in (8.49)

Fig. 8.4. Parameter (ymax)D against decay factor m calculated from (8.49) for all m > 0 except for m = 1. The value of (ymax)D for m = 1 is calculated from (8.50)

276 8 Radioactivity

Fig. 8.5. Parameter xmax against decay factor m calculated from (8.46) for all m > 0 except for m = 1. The value of (xmax)D for m = 1 is calculated from (8.47)

8.3.4 Equilibria in Parent-Daughter Activities

In many parent →daughter →granddaughter relationships after a certain time t the parent and daughter activities reach a constant ratio independent of a further increase in time t. This condition is referred to as radioactive equilibrium and can be analyzed further by examining the behavior of the activity ratio AD(t)/AP(t) obtained from (8.31) as

AP(t)

λD − λP

 

 

 

AD(t)

=

λD

1

 

e(λDλP)t

1

 

 

=

 

 

1 − e(λD−λP)t

 

 

1 − λPD

 

for the two initial conditions:

1.AP(t = 0) = AP(0) = λPNP(0),

2.AD(t = 0) = AD(0) = 0.

(8.51)

(8.52)

(8.53)

Inserting the decay factor m of (8.40) and variable x of (8.37) into (8.51) and defining parameter ξ as ξ = AD(t)/AP(t) = yD/yP, we write (8.51) as follows:

 

 

D(t)

1

 

 

1−m

 

1

 

 

 

m−1

 

 

AP(t)

 

 

 

 

 

 

 

 

1 − m

1 − m

 

 

ξ =

A

 

=

 

1

 

e(ln 2) m x

 

 

 

1

 

2 m x .

(8.54)

The ξ(x) expression of (8.54) is valid for all positive m except for m = 1 for which it is not defined. However, we can determine the ξ(x) functional

8.3 Radioactive Series Decay

277

Fig. 8.6. Variable ξ = AD(t)/AP(t) = yD/yP against x for several decay factors m in the range from 0.1 to 10 calculated from (8.54) except for ξ(m = 1) which gives a linear function calculated in (8.55)

relationship for m = 1 by applying the L’Hˆopital’s rule to get

 

 

d

m−1 x ln 2

 

 

 

 

 

 

 

 

 

 

 

1 − e

m

 

 

 

 

 

 

 

 

ξ(m = 1) = lim

 

dm

 

 

 

 

 

 

 

 

 

 

 

d(1 − m)/dm

 

 

 

 

 

 

 

m→1

 

 

 

 

 

 

 

 

 

 

 

e

m−1 x ln 2

x ln 2

m

1

x ln 2

lim

m

m

m

2

 

 

 

 

 

 

 

 

 

 

 

 

1

 

 

 

 

 

= (ln 2)x (8.55)

= m→1

 

 

 

 

 

 

 

 

 

 

 

Equation (8.55) shows that ξ(x) for m = 1 is a linear function of x, as shown in Fig. 8.6 in which we plot ξ(x) for various values of m in the range from 0.1 to 10. The m = 1 linear equation actually separates two distinct regions for the variable ξ: (i) region where m > 1 and (ii) region where 0 < m < 1.

1. For the m > 1 region, we write (8.54) as follows:

1

e

ξ =

 

m − 1

m−1 x ln 2 m

1 . (8.56)

Note that ξ rises exponentially with x, implying that the AD(t)/AP(t) ratio also increases with time t and thus no equilibrium between AP(t) and AD(t) will ensue with an increasing time t. The exponential behavior of ξ(x) is clearly shown in Fig. 8.6 with the dashed curves for m > 1 (in the range 1 < m < 10).

278 8 Radioactivity

2.For the 0 < m < 1 region, (8.54) suggests that the exponential term diminishes with increasing x and exponentially approaches zero. This means that at large x the parameter ξ approaches a constant value that is independent of x and is equal to 1/(1 − m). Under these conditions the parent activity AP(t) and daughter activity AD(t) are said to be in transient equilibrium, and are governed by the following relationship:

ξ =

AD(t)

=

yD

=

1

=

 

1

=

λD

 

. (8.57)

 

 

 

 

− λPD

λD

 

 

AP(t)

 

yP

1 − m 1

 

λP

After initially increasing, the daughter activity AD(t) goes through a maximum and then decreases at the same rate as the parent activity AP(t) and the two activities are related through (8.57). As m decreases, the daughter and parent activities at relatively large times t become increasingly more similar, since, as m → 0, ξ → 1. This represents a special case of transient equilibrium (λD λP, i.e., m → 0) and in this case the parent and daughter are said to be in secular equilibrium. Since in secular equilibrium ξ = 1, the parent and daughter activities are approximately equal, i.e., AP(t) AD(t) and the daughter decays with the same rate as the parent.

Equations (8.51) and (8.54) are valid in general, irrespective of the relative magnitudes of λP and λD; however, as indicated above, the ratio AD(t)/AP(t) falls into four distinct categories that are clearly defined by the relative magnitudes of λP and λD. The four categories are:

(1) Daughter Longer-Lived Than Parent:

(t1/2)D > (t1/2)P, i.e., λD < λP.

We write the ratio AD(t)/AP(t) of (8.51) as follows:

AP(t)

λP − λD

 

 

 

AD(t)

=

λD

e(λPλD)t

 

1 .

(8.58)

 

 

No equilibrium between the parent activity AP(t) and the daughter activity AD(t) will be reached for any t.

(2) Half-Lives of Parent and Daughter are Equal:

(t1/2)D = (t1/2)P, i.e., λD = λP.

The condition is mainly of theoretical interest as no such example has been observed in nature yet. The ratio AD(t)/AP(t) is given as a linear function, as shown in (8.55).