Radioactive decay and the Bateman equation

Introduction to Nuclear Science

Simon Fraser University

Spring 2011

NUCS 342 — January 19, 2011

NUCS 342 (Lecture 4) January 19, 2011 1 / 34

Outline

1 Natural radioactivity

NUCS 342 (Lecture 4) January 19, 2011 2 / 34

Outline

1 Natural radioactivity

2 Nuclear decay

NUCS 342 (Lecture 4) January 19, 2011 2 / 34

Outline

1 Natural radioactivity

2 Nuclear decay

3 Independent decay of radioactive mixture

NUCS 342 (Lecture 4) January 19, 2011 2 / 34

Outline

1 Natural radioactivity

2 Nuclear decay

3 Independent decay of radioactive mixture

4 The Bateman equation

NUCS 342 (Lecture 4) January 19, 2011 2 / 34

Outline

1 Natural radioactivity

2 Nuclear decay

3 Independent decay of radioactive mixture

4 The Bateman equation

5 Decay branches

NUCS 342 (Lecture 4) January 19, 2011 2 / 34

 Natural radioactivity

Natural radioactivity

Natural radioactivity has been discovered by Henri Becquerel and

Marie Sklodowska-Curie in late 1890s.
Radioactive polonium and radium elements were isolated by Marie
and Pierre Curie in 1898.
The process involves spontaneous disintegration of the parent element
and a formation of a daughter element.
A number of long-lifetime processes were identified since then:
α-decay : emission of 4 He
β − -decay: emission of an electron and electron anti neutrino
electron capture: capture of an electron from an atomic orbit by a
proton
β + -decay: emission of a positron and electron neutrino
heavy fragment emission: for example 12 C or 16 O
fission: split of a nucleus into two fragments of comparable mass and
charge

NUCS 342 (Lecture 4) January 19, 2011 3 / 34

 Natural radioactivity

Natural radioactivity

To quantify the decay process several measures can be introduced:

Activity A: number of disintegration per second

half-life T 12 : time after which the number of radioactive nuclei in a

sample is reduced to half of its initial value

lifetime τ : time after which the number of radioactive nuclei in a

sample is reduced by a factor of e ≈ 2.718 of its initial value.

NUCS 342 (Lecture 4) January 19, 2011 4 / 34

 Natural radioactivity

Units
Lifetimes and half-lives are measured in units of time.
Nuclear lifetimes span broad range from 10−20 s up to infinity (for
stable nuclei).
The SI unit for activity is 1 Becquerel, abbreviated as [Bq],
1 [Bq] = 1 [dps] (decay/disintegration per second). (1)
An often used non-SI unit is 1 Curie, abbreviated [Ci].
1 [Ci] = 3.7 × 1010 [Bq] (2)
1 [Ci] corresponds to activity of 1 g of Radium and is a sizable unit.
Typical environmental levels of radioactivity are pico-nano Curie
(0.01-10 [Bq]), research calibration sources are typically of micro
Curie (10 [kBq]) activity, a reactor upon a shutdown have activity in
the range of giga Curie ( 109 Ci or 1019 [Bq]).
NUCS 342 (Lecture 4) January 19, 2011 5 / 34
 Natural radioactivity

Natural radioactivity

Some naturally occurring long-lived radioactive isotopes

Nuclide Half-life [years] Natural abundance
40 K 1.28×109 0.01%
19
87 Rb 4.8×10 10 27.8%
37
113 Cd 9×10 15 12.2%
48
115 In 5.5×10 14 95.7%
49
128 Te 7.7×10 24 31.7%
52
130 Te 2.7×10 21 33.8%
52
138 La 1.1×10 11 0.09%
57
144 Nd 2.3×10 15 23.8%
60
147 Sm 1.1×10 11 15%
62
148 Sm 7×10 15 11.3%
62

NUCS 342 (Lecture 4) January 19, 2011 6 / 34

 Nuclear decay

Nuclear decay
One can show experimentally that the sample activity A is
proportional to the number N of nuclei in the sample
(decay is the first-order reaction).
Denoting the proportionality constant by λ and calling it the decay
rate one obtains
A = λN
Activity is the number of disintegration per second,
A∆t = N(t) − N(t + ∆t) = −(N(t + ∆t) − N(t))
N(t + ∆t) − N(t) dN
A=− =−
∆t dt
Above equations when combined give
dN
− = λN
dt
N(t) = N(0) exp(−λt)
NUCS 342 (Lecture 4) January 19, 2011 7 / 34
 Nuclear decay

Nuclear decay

Defining lifetime as
1
τ=
λ
the nuclear decay law can be written as
 t
N(t) = N(0) exp −
τ
It is easy to note that after time t = τ the number of radioactive
nuclei in the samples is reduced by the factor of e
 τ 1
N(τ ) = N(0) exp − = N(0) exp−1 = N(0)
τ e

NUCS 342 (Lecture 4) January 19, 2011 8 / 34

 Nuclear decay

Nuclear decay

The half-life is
  1
N(t = T 1 ) = N(0) exp −λT 1 = N(0)
2 2 2
  1
exp −λT 1 =
2
 2
1
−λT 1 = ln = − ln(2)
2 2
ln(2)
T1 = = ln(2)τ = 0.693τ
2 λ

NUCS 342 (Lecture 4) January 19, 2011 9 / 34

 Nuclear decay

Nuclear decay

T1/2 = 1.5, τ = T1/2 / ln(2) = 2.16

100
Number of atoms [%]

80

60 T1/2

τ
40
2T1/2

20 3T1/2

0
0 2 4 6 8 10
Time [arb.]

NUCS 342 (Lecture 4) January 19, 2011 10 / 34

 Nuclear decay

Nuclear decay

T1/2 = 1.5, τ = T1/2 / ln(2) = 2.16

100
T1/2
τ
2T1/2
Number of atoms [%]

3T1/2

10

0 2 4 6 8 10
Time [arb.]

NUCS 342 (Lecture 4) January 19, 2011 11 / 34

 Nuclear decay

Decay rate measurements

For large range of lifetimes measurements of the decay curves shown
on the graphs above can be carried out and lifetimes/decay rates can
be fitted.
However, for lifetimes comparable or longer than the span of a human
life there are no measurable changes in the activity of a sample which
prohibits direct decay curve measurements.
In these cases the decay rates are deduce from the ratio of observed
activity A to the absolute number of radioactive atoms N in a sample.
1 N
A = λN =⇒ τ = = (3)
λ A
The absolute number of atoms can be established based on the total
mass of the sample and its isotopic composition.
Isotopic composition can be established using mass spectroscopy.
NUCS 342 (Lecture 4) January 19, 2011 12 / 34
 Nuclear decay

Activity

It should be stressed that the activity of a sample depends on its mass

m (number of radioactive atoms) and the decay rate. Denoting the
molar mass by µ and the Avogadro number by NA one gets
m 1m
A = λN = λ NA = NA (4)
µ τ µ
This implies that small mass of short-lived isotopes may have the
same activity as a large mass of long-lived isotopes.

For example 1 MBq of tritium (T1/2 =12.33 y) corresponds to

5.59 × 1014 or 1.1 [nmole] of atoms or 2.78 [ng] of mass

1 MBq of 14 C (T1/2 =5730 [y]) corresponds to 2.6×1017 or

0.43 [µmole] of atoms or mass of 6 [µg].

NUCS 342 (Lecture 4) January 19, 2011 13 / 34

 Nuclear decay

Detection efficiency

Radiation detectors are built to detect decay products.

As such detectors respond to activity.

In a typical experiments number of counts NC corresponding to

detection of radiation of interest in a detector is recorded per unit of
time. The units of NC are counts per second.

This number of counts is related to the activity by the response

function of a detector  called efficiency

NC = A (5)

Efficiency depends on the type and geometry of the detector, as well

as type and energy of detected radiation.

NUCS 342 (Lecture 4) January 19, 2011 14 / 34

 Nuclear decay

Activation analysis

Tritium is produced in atmosphere by reaction of fast neutrons

generated by cosmic rays with 14 N

n +14 N →12 C +3 H (6)

Tritium is then incorporated into water and remove from atmosphere

as rain and snow.

A 50 ml sample of water typically show 1 [dpm] (disintegration per

minute) associated with the β − decay of tritium to 3 He. Based on
that let us estimate number ratio of tritium to hydrogen in water.

The number of tritium atoms in the sample is

1
N3 H = A = τ A = 12.33 [y]∗1 [1/min] = 6.5×106 = 1.08×10−17 [mole]
λ
(7)
NUCS 342 (Lecture 4) January 19, 2011 15 / 34
 Nuclear decay

Activation analysis

The number of tritium atoms in the sample is

1
N3 H = A = τ A = 12.33 [y]∗1 [1/min] = 6.5×106 = 1.08×10−17 [mole]
λ
The mass of the 50 ml sample is 50 g.

The number of water molecules in the sample is

m 50
NH2 O = = = 2.77 [mole] = 16.7 × 1023 (8)
µ 18.02
There are two hydrogen atoms per molecule, thus the tritium to
hydrogen number ratio is

N3 H 1.08 × 10−17
= = 2 × 10−18 (9)
N1 H 5.54

NUCS 342 (Lecture 4) January 19, 2011 16 / 34

 Independent decay of radioactive mixture

Independent decay of radioactive mixture

Quite often radioactive samples are mixtures of radioactivities

decaying at different rates.

If the decay products from both samples are the same (for example
electrons from β − decay) a detector will see the combined decay of
the mixture.

In such cases a special care has to be taken if lifetimes are extracted.

A common procedure is to extract parameters for the longest-lived
activity first, subtract it from the data, analyze the next longest lived,
etc.

Currently this is done using computer fits.

An example for a two-component mixture is analyzed below.

NUCS 342 (Lecture 4) January 19, 2011 17 / 34

 Independent decay of radioactive mixture

Independent decay of two radioactivities

   
t t
N(t)=70 × exp − +30 × exp −
ln(2)1.5 ln(2)15

100
Number of atoms [%]

80

60

40

20

0
0 5 10 15 20 25 30 35 40
Time [arb.]

NUCS 342 (Lecture 4) January 19, 2011 18 / 34

 Independent decay of radioactive mixture

Independent decay of two radioactivities

   
t t
N(t)=70 × exp − +30 × exp −
ln(2)1.5 ln(2)15

100
Number of atoms [%]

10

0 5 10 15 20 25 30 35 40
Time [arb.]

NUCS 342 (Lecture 4) January 19, 2011 19 / 34

 The Bateman equation

Decay chains
Decay chains in which radioactive decay of an unstable isotope feeds
radioactive decay of another unstable isotope are commonly
encountered in nature and experimental nuclear science.
For example, there are three naturally occurring, long-lived chains of
α and β decays originating in the long-lived isotopes of 232 Th
(T1/2 =14.1 Gy), 235 U (T1/2 =0.7 Gy) and 238 U (T1/2 =4.5 Gy).
Another example is a sequence of β decay of unstable isotopes along
the mass parabolas for a fixed mass number until the most stable
isotope is reached.
In case of the decay chain activities and abundances of radioactive
isotopes are not independent. Rather, they are determined by the
history of the decay: the decay rates and abundances in the preceding
part of the chain.
Thus the chain decay is different then independent decay of a mixture
considered so far.
NUCS 342 (Lecture 4) January 19, 2011 20 / 34
 The Bateman equation

235 238
U and U chains

NUCS 342 (Lecture 4) January 19, 2011 21 / 34

 The Bateman equation

The Bateman equation

The Bateman equation is a mathematical model describing

abundances and activities in a decay chain as a function of time,
based on the decay rates and initial abundances.

The Bateman equation is not a single equation, rather it is a method

of setting up differential equations describing the chain of interest
based on its known properties.

We are going to consider the simplest case with a parent feeding

single daughter.

Then by varying the parameters such as the decay rates and relative
initial abundances we will investigate the chain evolution as a function
of time.

NUCS 342 (Lecture 4) January 19, 2011 22 / 34

 The Bateman equation

Two-decay chain

Let us denote
Initial number of parent and daughter atoms as N1 (0) and N2 (0)
Number of parent and daughter atoms in time as N1 (t) and N2 (t)
Parent and daughter activities in time as A1 (t) and A2 (t)
Parent and daughter decay rates by λ1 and λ2
The equation for the time evolution of the parent is the same as for a
single step decay
dN1 (t)
= −λ1 N1 (t) (10)
dt
The equation for the time evolution of the daughter, however,
includes a term describing daughter decay but also daughter feeding
by the parent
dN2 (t)
= −λ2 N2 (t) + λ1 N1 (t) (11)
dt

NUCS 342 (Lecture 4) January 19, 2011 23 / 34

 The Bateman equation

Two-decay chain

The solution of Eq. 10 is

N1 (t) = N1 (0) exp (−λ1 t) (12)

Taking this into account Eq. 11 become

dN2 (t)
= −λ2 N2 (t) + N1 (0) exp (−λ1 t) (13)
dt
The solution for N2 (t) is

N2 (t) = N2 (0) exp (−λ2 t) +

λ1
− N1 (0) (exp (−λ2 t) − exp (−λ1 t)) (14)
λ2 − λ1

NUCS 342 (Lecture 4) January 19, 2011 24 / 34

 The Bateman equation

Two-decay chain: abundance for a special case

Blue: parent T1/2 =1.5, N1 (0) = 100%

Red: daughter T1/2 =3, N2 (0) = 0%

100
Number of atoms [%]

80

60

40

20

0 2 4 6 8 10 12 14
Time [arb.]

NUCS 342 (Lecture 4) January 19, 2011 25 / 34

 The Bateman equation

Two-decay chain: abundances for a special case

Blue: parent T1/2 =1.5, N1 (0) = 100%

Red: daughter T1/2 =3, N2 (0) = 0%
100
Number of atoms [%]

10

1
0 2 4 6 8 10 12 14
Time [arb.]

NUCS 342 (Lecture 4) January 19, 2011 26 / 34

 The Bateman equation

Two-decay chain: activities

Eqs 12 and 14 define abundances

Activities of the parent and the daughter can be calculated from

A1 (t) = λ1 N1 (t) = λ1 N1 (0) exp (−λ1 t)

A2 (t) = λ2 N2 (t) = λ2 N2 (0) exp (−λ2 t) + (15)
λ1 λ2
− N1 (0) (exp (−λ2 t) − exp (−λ1 t))
λ2 − λ1

NUCS 342 (Lecture 4) January 19, 2011 27 / 34

 The Bateman equation

Two-decay chain: activities for a special case

Blue: parent T1/2 =1.5, N1 (0) = 100%

Red: daughter T1/2 =3, N2 (0) = 0%
70

60
Decay per unit time

50

40

30

20

10

0 2 4 6 8 10 12 14
Time [arb.]

NUCS 342 (Lecture 4) January 19, 2011 28 / 34

 The Bateman equation

Two-decay chain: activities for a special case

Blue: parent T1/2 =1.5, N1 (0) = 100%

Red: daughter T1/2 =3, N2 (0) = 0%
100
Decay per unit time

10

1
0 2 4 6 8 10 12 14
Time [arb.]

NUCS 342 (Lecture 4) January 19, 2011 29 / 34

 Decay branches

Decay branches

Decay branches are observed when there is more than a single process
for disintegration of the parent nucleus.

For example, in the decay chain of 238 U 218 Po can α-decay to 214 Pb

or β − decay to 218 At.

Another example is in the decay chain of 235 U with 227 Ac having an α

branch to 223 Fr and a β − decay branch to 227 Th.

Yet another example are decays of 235 U and 238 U by spontaneous

fission which is a tiny, however, existing branch as compared to the
dominating α decay.

NUCS 342 (Lecture 4) January 19, 2011 30 / 34

 Decay branches

235 238
U and U chains

NUCS 342 (Lecture 4) January 19, 2011 31 / 34

 Decay branches

Total decay rate and branching ratios

For clarity, let us consider two competing branches in the decaying

parent: an α and a β branch.

The decay rates λα and λβ define probability per unit time for
disintegration by the respective process. The total probability for
disintegration is
λ = λα + λβ (16)
Relative probability for each branch decay, called the branching ratio,
is the ratio of the respective decay rate to the total decay rate
λα λα
brα = =
λ λα + λβ
λβ λβ
brβ = = (17)
λ λα + λβ

NUCS 342 (Lecture 4) January 19, 2011 32 / 34

 Decay branches

Lifetime and partial lifetimes

The decay (without feeding) is defined by the total rate

dN(t)
= −λN(t) = −(λα + λβ )N(t) =⇒
dt
N(t) = N(0) exp (−λt)) = N(0) exp (−(λα + λβ )t) =
N(0) exp (−λα t) exp (−λβ t) (18)

Lifetime of the parent is defined by the total rate

1
τ= (19)
λ
Partial lifetimes for the decays are defined as
1 1
τα = , τβ = (20)
λα λβ

NUCS 342 (Lecture 4) January 19, 2011 33 / 34

 Decay branches

Lifetime and partial lifetimes

Note that while
λ = λα + λβ (21)
and the total rate is dominated by the larger of λα , λβ partial rates.
For the lifetime and partial lifetimes this implies
1 1 1
= + (22)
τ τα τβ
and the lifetime of the parent is dominated by the shorter partial
lifetime.
It should be stressed that
τ 6= τα + τβ
and that there is only one lifetime τ defining decay of the parent.
Partial lifetimes can be extracted from measured branching ratios.
NUCS 342 (Lecture 4) January 19, 2011 34 / 34