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CHAPTER 1

INTRODUCTION

THE TRACER CONCEPT A brief historical view

Big Bang

THE TRACER CONCEPT A brief historical view Big Bang All matter in the universe has its

All matter in the universe has its origin in an event called the “Big Bang”, a cosmic explosion releasing an enormous amount of energy about 14 billion years ago. Particles like protons and neutrons, the building stones of the nucleus, were condensed as free particles during the first seconds. However, it took several minutes until the decreasing temperature of the expanding universe reached a level that allowed the formation of particle combinations like deuterium (heavy hydrogen) as well as helium (see figure below).

32 16 S Heavy ion fusion in red super giants 31 15 P 30 14
32
16
S
Heavy ion
fusion in red super giants
31
15
P
30
14
28 Si
29 Si
Si
12
C-fusion
13
27 Al
24
12
n
Mg
25 Mg 26 Mg
23
11
Na
22
10
20 Ne
21 Ne
Ne
19
9
F
16
17 O
18
n
8
O
O
He-fusion in
14
15
7
N
N
red giants
n
12
13
6
C
C
10 B
11
5
B
8
4
Be
9 Be
7
3
6 Li
Li
2
4 He
p+n
d (deuterium),
d+d
He
n
1
p
d
H-fusion in gas clouds
and stars
0
n
0
1
2
3
4
5
6
7
8
9
10
11
12
13 14
15
16
Number of protons
16
O-fusion

Number of neutrons

For several 100 million years the universe was a large plasma composed by hydrogen, deuterium

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and helium ions and free electrons. With time the temperature decreased and after 700 million years the electrons were able to attach to the ions forming neutral atoms and the plasma was transformed to a large cloud of hydrogen and helium gas. In the neutral gas gravity was able to locally condense the gas, a process that again increased the temperature, and the first stars, the red giants were born. The temperature and the density in the stars increased the probability of other nuclear reactions like the formation of beryllium-8 by two helium nuclides. This nucleus could then pick up another helium ion (or -particle) to form carbon-12. In steps of four mass units (2 protons and 2 neutrons) light elements were formed, oxygen-16, neon-20, manganese-24, sulphur-32 etc in a process called fusion. Other reactions such as neutron capture, splitting of the target nucleus in nuclear reactions and radioactive decay contributed to create other combinations of proton and neutrons.

The fusion process worked for elements up to iron but for more heavy elements other mechanisms took over. The iron nucleus picked up neutrons creating instable proton and neutron combinations that decayed emitting a negative

charge in the form of a beta particle ( - ). A new element (cobalt) with an extra proton in the nucleus was then created. The cobalt nucleus captured new neutrons and formed nickel nuclei via radioactive decay. In such a way, step by

step, all the heavy elements we know were

created.

When the red giants grow old they exploded.

All their content of heavy material was spread

around in universe. By gravity other stars

picked it up and formed planets. Actually, all

matter around us, including our-selves, was

once created in one of these red stars.

Billion years have passed since our planet Tellus was formed. Most of the unstable proton- neutron combinations once created has

undergone transformations (radioactive decay) into stable combinations. However, some with very long half-lives remain: potassium-40, lead- 204, thorium-232 and the natural occurring isotopes of uranium.

The pioneers

These “glowing” pieces after the cosmic cookery event were discovered by Henri Becquerel 1896 and were further investigated by Marie Curie and her husband Pierre Curie. It was the scientific sensation of that time, which still has great implications in our lives.

Suddenly several new elements were discovered that emitted radiation of several types. First was polonium named after Poland, Marie Curie’s country of birth. The second was radium, which was soon found to have properties useful in medicine (cancer treatment). However, some elements were chemically identical with already known elements, such as lead, but emitted this strange new radiation. This was puzzling for the scientists at that time. They had only vague knowledge about the structure of the atom, and the neutron was still to be discovered. Soddy, in 1913, introduced the concept of isotopes (Greek: iso= same, tope= place). Isotopes occupied the same place in the periodical system, were chemically identical, but differed from each other in atomic weight and emission of radioactivity. When Chadwick in 1932 discovered the neutron this concept was given a rational explanation.

the neutron this concept was given a rational explanation. Antoine Henri Becquerel Frederick Soddy Marie Curie

Antoine Henri Becquerel

was given a rational explanation. Antoine Henri Becquerel Frederick Soddy Marie Curie George de Hevesy 2

Frederick Soddy

explanation. Antoine Henri Becquerel Frederick Soddy Marie Curie George de Hevesy 2 Almost at the same

Marie Curie

Antoine Henri Becquerel Frederick Soddy Marie Curie George de Hevesy 2 Almost at the same time

George de Hevesy

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Almost at the same time (1913), George de Hevesy demonstrated the practical implication of the isotopic theory. He and his colleagues used a radioactive isotope of lead, 210 Pb, as a tracer (or indicator) when they studied the solubility of sparingly soluble lead salts. Hevesy was also the first to apply the radioactive tracer technique in biology when he investigated lead uptake in plants (1923) using 212 Pb. Only one year later, Blumengarten and Weiss carried out the first clinical study. They injected 212 Bi into one arm of a patient and measured the arrival time in the other arm. From this study, they concluded that the arrival time was prolonged in patients with heart disease.

Induced radioactivity

So far, nature was the supplier of the radioactive nuclides that were used. Isotopes of uranium and thorium generated a variety of radioactive heavy elements such as lead, but radioactive isotopes of light elements were not known. Marie Curie’s daughter Irène, together with her husband Frédéric Joliot took the next step. Alpha-emitting sources had for long been used to bombard different elements. Rutherford studied e.g. the deflection of alpha particles in gold foils and discovered the small, charged nucleus of the atom. But Joliot-Curie also showed that the alpha particles induced radioactivity in the bombarded foil (in their case aluminum foil). The induced radioactivity had a half-life of about 3 minutes.

induced radioactivity had a half-life of about 3 minutes. Frédéric Joliot Irène Joliot-Curie Correctly, they

Frédéric Joliot

had a half-life of about 3 minutes. Frédéric Joliot Irène Joliot-Curie Correctly, they identified the radiation

Irène Joliot-Curie

Correctly, they identified the radiation to be emitted from 30 P created in the nuclear reaction.

27 Al ( , n) 30 P

They also concluded that “These elements and similar ones may possibly be formed in different nuclear reactions with other bombarding particles: protons, deuterons and neutrons. For example, 13 N could perhaps be formed by capture of a deuteron in 12 C, followed by the emission of a neutron.”

in 1 2 C, followed by the emission of a neutron.” Ernest Orlando Lawrence Enrico Fermi

Ernest Orlando Lawrence

by the emission of a neutron.” Ernest Orlando Lawrence Enrico Fermi The same year this was

Enrico Fermi

The same year this was proved to be true by Ernest Lawrence in Berkeley, California and Enrico Fermi, Rome. Lawrence had built a cyclotron capable of accelerating deuterons up to about 3 MeV and it was by pure chance that this group had not yet discovered induced radioactivity. He soon reported the production of 13 N with a half-life of 10 minutes. After this the cyclotron was used to produce several other biologically important radionuclides such as 11 C, 32 P and 22 Na.

Fermi realized that the neutron was advantageous for radionuclide production. Since it has no charge, it could easily enter into the nucleus and induce a nuclear reaction. He immediately made a strong neutron source by sealing up 232 Ra-gas with beryllium powder in a glass vial. The alpha particle emitted from 232 Ra caused a nuclear reaction in beryllium and a neutron was emitted.

9 Be ( , n) 12 C

Fermi started a systematical search by irradiating all available elements in the periodic system with fast and slow neutrons to study the creation of induced radioactivity. From hydrogen to oxygen, no radioactivity was observed in their targets, but in the ninth element, fluorine, their hopes were fulfilled. In

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the following weeks, they bombarded some 60 elements and found induced radioactivity in 40 of them. They also observed that the lighter elements were usually transmuted into radionuclides of a different chemical element, whereas heavier elements appeared to yield radioisotopes of the same element as the target.

These new discoveries excited the scientific community. From having been a rather limited technique, the radioactivity tracer principle could suddenly be applied in a variety of fields and especially in life sciences. De Hevesy immediately started to study the uptake and elimination of 32 P-phosphate in various tissues of rats and demonstrated, for the first time, the kinetics of vital elements in living creatures. 128 I was applied in the diagnosis of thyroid disease. This was the start of the radiotracer technology in biology and medicine, as we know it today.

One early cyclotron-produced nuclide was 11 C. It is of special importance since carbon is fundamental in life science. 11 C has a half-life of only 20 minutes but by setting up a chemical laboratory close to the cyclotron, organic compound labeled with 11 C can be obtained in large amounts. Photosynthesis was studied using 11 CO 2 and the fixation of carbon monoxide in humans by the use of inhalation of 11 CO. However, 20 minutes was short and the use of 11 C was limited to the most rapid biochemical reactions. One must remember that the radio-detectors used at that time were primitive and that the chemical synthetic and analytic tools were not adapted to such short times. A search to find a more long-lived isotope of carbon resulted 1939 in the discovery of 14 C produced in the nuclear reaction

13 C (d, p) 14 C

However, 14 C produced this way was of limited use since the radionuclide could not be separated from the target.

During the bombardments, a bottle of ammonium nitrate solution had been standing close to the target. By pure chance, it was discovered that this bottle also contained 14 C, which had been produced in the reaction

14 N (n, p) 14 C

The deuterons used in the bombardment consist of one proton and one neutron with a binding energy of about 2 MeV. When high-energy deuterons hit a target, it is likely that the binding between the particles breaks and that a free neutron is created in what is called a “stripping reaction”. The bottle with ammonium nitrate had thus unintentionally been neutron irradiated. Since no carbon was present in the bottle (except small amounts from solved air- borne carbon dioxide) the 14 C produced this way was of high specific radioactivity. It was also very easy to separate from the target. In the nuclear reaction, a “hot” carbon atom was created, which formed 14 CO 2 in the solution. By simply bubbling air through the bottle, the 14 C was released from the target.

The same year, and in the same place, tritium was discovered by deuteron irradiation of water. One of the pioneers Martin Kamen stated:

“Within a few months, after the scientific world had somewhat ruefully concluded that development of tracer techniques would be seriously handicapped because useful radioactive tracers for carbon, hydrogen, oxygen and nitrogen did not exist, 14 C and 3 H were discovered, and the situation greatly improved”. This is indeed true. The role of 3 H- and 14 C- labeled tracers in biochemical research is a story in itself.

Before the Second World War, the cyclotron was the main producer of radionuclides since the neutron sources at that time were very weak. But with the development of the nuclear reactor, the situation changed. Suddenly, a tremendously strong neutron source was available, which easily could produce almost unlimited amounts of radioactive nuclides including such biological important elements as 3 H, 14 C, 32 P, 35 S and clinically interesting radionuclides as 60 Co (for external radiotherapy) and 131 I for nuclear medicine. After the war, a new industry was born which could deliver a variety of radiolabeled compounds at a reasonable price.

However, accelerator-produced nuclides have a special character, which makes them differ from reactor-produced nuclides. Today, their popularity is increasing again. Generally, one

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may say that reactor-produced radionuclides are most suitable for laboratory work, whereas accelerator-produced radionuclides are more clinically useful. Some of the most used radionuclides in nuclear medicine, such as 111 In and 201 Tl, are accelerator produced. When using very short-lived radionuclides ( 11 C, 13 N, 15 O and 18 F) for positron emission tomography (PET) the need for an in-house accelerator is obvious.

Radioactive nuclides with short half-life may play an important role in the future laboratory use of the tracer technique. We know that biological systems, such as pheromones, may work at extremely low concentrations. The radiotracer technique, as we know it today, is often not useful to study such systems since it is not sensitive enough. The drawback with 14 C is its very long half-life of 5370 years. If we have one million 14 C-labeled molecules, in the mean only one will decay in an experiment lasting a few days. Usually, the practical detection limits are in the pico-mole area. When using the more short-lived 11 C, almost all labeled molecules contribute to the signal during an experiment lasting one hour. The sensitivity increases considerably to the femto-mole or even atto- mole level.

DEFINITION OF IONIZING RADIATION

Ionizing radiation is high-energy particles or photons that can cause ionization, in other words, cause the emission of electrons from atoms or molecules. Subatomic particles with a mass (such as electrons, protons and neutrons) transfer their kinetic energy, in different processes, to the orbit electrons of the atom. Photons (electromagnetic radiation) with wavelength of atomic dimensions or less behave as discrete ”packets” of energy (quanta). These quanta, in different processes, also transfer their energy to matter creating ionization.

In 1895, Wilhelm Conrad Roentgen discovered X-rays, the first man made ionization radiation. When fast electrons are slowed down in dense material, they create radiation of electro- magnetic nature similar to that of ordinary visible light. However, these quanta, roentgen or X-rays, have considerably higher energy than

light. This type of continuous radiation is also called bremsstrahlung.

type of continuous radiation is also called bremsstrahlung. Figure 1 A collimated radium source in a

Figure 1 A collimated radium source in a magnetic field.

The direction of the field is perpendicular to the plane of the page. The heavy,

positive

deflected slightly to the left whereas the light negative - particle is deflected markedly to the right. The uncharged - photons being insensitive to the magnetic field carry straight on.

particle is

In 1896, Henri Becquerel demonstrated that uranium mineral emits penetrating radiation with properties similar to X-rays. The couple, Marie and Pierre Curie, showed in 1898 that certain uranium minerals contained a previously unknown element, radium, which emits intense ionizing radiation of different types. A magnetic field can separate the radium radiation into three components (Figure 1).

On closer analysis, it became apparent that radiation was identical with helium nuclei, -radiation consisted of electrons, and -radiation was of electromagnetic nature.

Shortly afterwards, ionizing radiation was used in medicine for diagnostic radiology and the irradiation of tumors. However, at that time there were little knowledge about the effects of radiation on matter, how radiation transferred energy to the region irradiated and how to quantify radiation. Ionizing radiation is of course invisible and humans have no sensory organ that can detect it. Consequently, a series of tragic events occurred in the early decades of the use of ionization radiation. The need for measuring techniques (dosimetry) and protective procedures for those working with ionizing radiation was soon perceived.

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Subsequent development was rapid. The technology to accelerate charged particles to high energy was developed. In the 1930’s, a new ionizing particle, the neutron, was discovered. Like roentgen and gamma radiation, it had no charge. It was soon demonstrated that the neutron caused nuclear reactions including nuclear fission in heavy elements.

During the1940’s, physicists learnt to control the fission process, which in nuclear weapons can liberate instantaneously enormous amounts of energy in the form of ionizing radiation. In nuclear reactors, nuclear fission can be controlled and used to produce energy and large amounts of radioactive material. The explosion of nuclear weapons, especially in the biosphere, disperses enormous amounts of radioactive material, which resulted in many people being exposed to radiation. Nuclear power plants also contributed to an increase in radioactive nuclides in the environment even if during normal operation the increase is small.

HISTORICAL SUMMARY

1895

1896

1900 -

1920 amongst radiologists due to lack of knowledge.

1920 National and international radiation protection standards begin to be instituted.

1930 The neutron and induced radioactivity discovered. Construction of particle accelerators begins.

1939 Nuclear fission discovered

1945 Nuclear bombs used (Hiroshima and Nagasaki).

1950- Development of nuclear reactors

1960- Use of reactors for production of energy, development of trace element techniques, increased use of radiation in medicine, research and industry

Discovery of X-rays Discovery of natural radioactivity Period of serious personal injuries

Energy of ionizing radiation

When ionizing radiation (in the form of high- energy photons, neutrons or charged particles) collides with matter, the full energy or part of it can be transferred to the matter in various types of interaction. It is by such energy transfer that radiation exerts its damaging effect on living creatures. Part of the transmitted energy causes ionization or excitation in the material (Figure 2). Ionization means that electrons in the matter receive so much additional energy that they are liberated completely from the atom or molecule to which they are bound. By excitation, the additional energy is insufficient for the electrons to be liberated from the molecule.

for the electrons to be liberated from the molecule. Figure 2 Ionizing radiation transfer energy to

Figure 2 Ionizing radiation transfer energy to the atom's orbital electrons. They can either be displaced to a distal orbit (excitation) or they can be free electrons (ionization).

The electron is displaced only to an orbit with a lower binding energy. The atom or molecule does not change its charge number but the process may change its chemical properties.

+1 volt e - , electron E e = 1 eV v e = 600
+1 volt
e - , electron
E e = 1 eV
v e = 600 km/s
e + , proton
E p =1 eV
v p =14 km/s
0

Figure 3 An electron is accelerated from the negative towards the positive electrode. At arrival, the electron has acquired a kinetic energy of 1 eV. A particle with positive charge, e.g. a proton, undergoes a similar event from the positive to the negative electrode. However, since the proton mass is about 2000 times the mass of the electron, the proton velocity is considerably lower.

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To cause ionization or excitation, it is essential that the incoming radiation has certain energy. This is expressed as electron volt eV. One eV is the kinetic energy an electron or a proton receives after acceleration in a potential drop of 1 volt (Figure 3).

Generally, charged and non-charged particles can be allotted a certain kinetic energy expressed in eV or keV (kiloelectron volt = 10 3 eV), MeV (megaelectron volt = 10 6 eV) and GeV (gigaelectron volt = 10 9 eV).

X-ray and gamma radiation does not have mass or kinetic energy in the real sense. However, when their wavelength diminishes and begins to approximate the dimensions of the atom and the nucleus, the electromagnetic radiation can be regarded as particles (photons or radiation quanta). Each photon has certain energy (E)

E = h where

oscillations of the radiation, h is "Planck's

is the frequency of the electromagnetic

constant", and E is energy in eV.

On average, about 30 eV are needed to cause one ionization in most materials. We define ionizing radiation to have energy higher than 100 eV. Radiation with lower energy is called non-ionizing radiation.

PRODUCTION OF IONIZING RADIATION

In electromagnetic fields, charged particles can be accelerated to such energies that they can penetrate matter. Important types of accelerators are:

a for acceleration of electrons

1 X-ray tubes (0 - 300 keV)

2 Linear accelerators (2 - 100 MeV)

3 Betatrons (15 - 100 MeV)

4 Microtrons (5 - 50 MeV)

b for acceleration of heavy, charged particles (protons, heavier ions)

1 Van de Graaff accelerator (1-25 MeV)

2 Linear accelerator (1 - 800 MeV)

3 Cyclotron (1 - 1,000 MeV)

4 Synchrotron (1 - 300 GeV)

Secondary ionizing radiation arises when the accelerated particles meet a radiation target.

a X-ray photons, when for example

electrons are decelerated in an X-ray tube. Radiation protection when working with X- ray equipment is dealt with in Chapter 5.

b Protons, neutrons, photons or other

radiation particles when protons, heavier particles or photons cause nuclear reactions.

heavier particles or photons cause nuclear reactions. Figure 4 Cyclotron that accelerates protons to 17 MeV.

Figure 4 Cyclotron that accelerates protons to 17 MeV. Generally used for radionuclide production.

to 17 MeV. Generally used for radionuclide production . Figure 5 Modern diagnostic X-ray laboratory for

Figure 5 Modern diagnostic X-ray laboratory for tomographic information.

Important parameters specifying an accelerator's performance are the type of accelerated particles (electrons, protons etc.), maximum particle energy (most often given in keV, MeV or GeV)

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and beam current (number of particles per unit of time or in microamperes). From the radiation protection point of view, an essential feature of accelerators is that radiation production can be turned off easily. The only risk involved is the possible occurrence of induced radioactivity. Radioactive sources, which are the commonest source of radiation in the laboratory, do not have this convenient attribute.

Other examples are neutron and gamma radiation, which arise as a result of nuclear fission processes in a fission reactor.

CHAPTER 2

NUCLEAR STABILITY AND INSTABILITY

Number of protons

ORGANIZATION OF MATTER

Chemists learnt during the late 19 th century to organize chemical knowledge into the periodic system. Radioactivity, when it was discovered, conflicted with that system. Suddenly various samples, apparently with the same chemical behavior, were found to have different physical qualities such as half-life, emitted type of radiation and energy. The concept of isotopes or elements occupying the same place in the periodic system (from the Greek: iso- = same and topos = place) was introduced by Soddy 1913, but a complete explanation had to wait for the discovery of the neutron (Chadwick

1932).

The periodic system was organized according to the number of protons in the nucleus. This related to the number of surrounding electrons that determined the chemistry of the element. Since the number of neutrons in the nucleus is

of importance as well, the physicist’s way to

organize matter, the nuclide chart, is somewhat different. Each proton-neutron combination is identified in this chart.

A

X

Z

N

A

proton-neutron combination is identified by

Z X

= element name (e. g. C for carbon)

A

= number of protons in the nucleus

= number of neutrons in the nucleus

= mass number (A=Z+N)

The expression above is over-determined. If the element name X is known, so is the number of protons in the nucleus, Z. Usually, the following simplified expression is used.

A

X

Some relations of the numbers of protons and neutrons have special names such as Isotopes = number of proton is constant

(Z = constant)

Isotones = number of neutrons is constant

(N = constant)

Isobars = mass number is constant

(A = constant)

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Of these expressions only the isotope concept is generally used. It is important to understand that whenever we use the expression isotope, we must always relate it to a specific element or a group of elements, e.g. isotopes of carbon (e.g. 11 C, 12 C, 13 C and 14 C) or isotopes of the halogens.

NUCLIDE CHART

protons = neutrons 100 On this side neutron deficient 80 nuclides which decay by +
protons
= neutrons
100
On this side
neutron deficient
80
nuclides which
decay by +
60
and EC
40
On this side
neutron excess
20
nuclides which
decay by -
0
0
50
100
150
Number of protons

Number of neutrons

Figure 1 Chart of nuclides. The black dots represent 279 naturally existing combinations of protons and neutrons (stable or almost stable nuclides). Around this stable line are about 2300 proton/neutron-combinations that are radioactive.

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17

F

18

F

19

F

20

F

21

F

22

F

23

F

24

F

25

F

8

         

13

O

14

O

15

O

16

O

17

O

18

O

19

O

20

O

21

O

22

O

23

O

24

O

7

         

12

N

13

N

14

N

15

N

16

N

17

N

18

N

19

N

20

N

21

N

22

N

23

N

6

     

9

C

10

C

11

C

12

C

13

C

14

C

15

C

16

C

17

C

18

C

19

C

20

C

   

5

     

8

B

 

10

B

11

B

12

B

13

B

14

B

15

B

 

17

B

       

4

     

7 Be

8 Be

9 Be

10 Be

11 Be

12 Be

 

14 Be

           

3

     

6

Li

7

Li

8

Li

9

Li

 

11

Li

               

2

 

3

He

4

He

 

6

He

 

8

He

                   

1

1

H

2

H

3

H

                           

0

   

n

                             
   

0

 

1

 

2

 

3

4

5

6

7

8

9

10

11

12

13

14

15

16

Number of neutrons

Figure 2 A part of the nuclide chart where the lightest elements are shown. The dark squares represent stable nuclides that are important for our existence. Nuclides to the left of the stable ones are radionuclides deficient in neutrons and those to the right, rich in neutrons.

The force that keeps the nucleons (protons and neutrons) together in the nucleus is called the “strong force” or the “nuclear force”. Other

forces, e.g. the Coulomb force, tend to separate the charged particles in the nucleus. In the stable and in the radioactive nucleus, there is a balance between binding and separating forces. The interplay between the forces is illustrated in Figure 4. A proton and a neutron are held together by the strong force and create a stable isotope of hydrogen, deuterium. Two protons do not create a stable system since the Coulomb force exceeds the nuclear force.

system since the Coulomb force exceeds the nuclear force. electron proton neutron Figure 3 Here, three

electron

proton

neutron

Figure 3 Here, three isotopes of the element hydrogen are illustrated using a simple atomic model. 1 H has only one proton, deuterium 2 H has a proton and a neutron in its nucleus, and tritium 3 H has a proton and two neutrons. Isotopes behave in the same way chemically since it is the electron shell that determines what happens in chemical reactions. Physically they are completely different.

Between two neutrons, no Coulomb force is

present and one should expect this system to be stable. However, this is not the case since besides the strong force and the Coulomb force a symmetry rule exist saying that a higher nuclear stability is achieved when there are about the same number of protons and neutrons

in the nucleus. This symmetry rule prevents two

neutrons from sticking together, but allows two neutrons and a proton to form a radioactive nucleus, 3 H.

A useful measure is the binding energy that

keeps the nucleons together. If the energy of 2.2 MeV is added to a deuterium nucleus, the two nucleons are parted as a free proton and a free neutron. Another way to express this is to measure the differences in weight. The deuterium nucleus is somewhat lighter than the sum weight of the free neutron and proton. This mass difference can be converted into energy using the Einstein formula E = mc 2 and is found

to be 2.2 MeV.

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proton neutron proton proton
proton
neutron
proton
proton

Liquid drop model

Figure 4 Binding and separating forces in the nucleus. A proton and a neutron can form a stable nucleus whereas two protons can not.

It is far beyond the ambition of this book to give

a comprehensive understanding of these

processes. However, some penetration of the topic is necessary to get a general feeling of the fundamental aspects of stability and nuclear decay. We use a model describing the exchange of nuclear forces that is referred to as the “liquid drop model”. This model gives an empirical formula of the binding energy B of the nucleus.

an empirical formula of the binding energy B of the nucleus. Figure 5 The range of

Figure 5 The range of the nuclear force is short. Only neighbors are interacting.

We explain the model step by step.

B

The binding energy is in the first approximation proportional to the number of nucleons in the nucleus. This is because the nuclear force has a very short range. Only neighbors are affected and can bind to each other. The nucleons in the central part of the nucleus all have the same

number of neighbors. In a large nucleus the total binding energy, B, is then approximately equal

to a constant*A where A is the number of

nucleons. The same is true between molecules

in a liquid, thus the model’s name.

a 1 *A

B

a 1 *A - a 2 *A 2/3

Nucleons at the surface have fewer neighbors and binding sites and are more loosely bound. The total binding energy is decreased by a factor that is proportional to the surface of the nucleus. The number of nucleons, A, is proportional to the volume of the nucleus. Thus, the nucleus radius is proportional to A 1/3 and the surface to

A 2/3 .

B a 1 *A - a 2 *A 2/3 - a 3 *Z 2 /A 1/3

When the numbers of protons start to increase, the Coulomb repulsing force starts to become more important. The Coulomb force is the sum

of all proton combinations, F = (Zi*Zj)/(rij) 2. If we integrate this function as a function of distance, we obtain a measure of the energy related to the force. It can then be shown that the negative contribution to the binding energy

is

proportional to Z 2 /A 1/3

B

a 1 *A - a 2 *A 2/3 - a 3 *Z 2 /A 1/3 - a 4 *(A/2-Z) 2 /A

Nature seems to prefer to have about the same number of protons and neutrons in the nucleus. This is seen in Figure 1 where for light nuclides the nuclide chart is very close to a straight line (equal number of protons and neutrons). For heavier elements there seems to be a tendency towards an excess of neutrons. This is understandable if one considers the Coulomb force contribution. Adding neutrons will increase the distances between the protons, which will lower the Coulomb force and total binding energy in the nucleus increases. The expression a 4 *(A/2-Z) 2 /A is only empirically found but gives the wanted relations. If Z=A/2 i.e. the number of protons and neutrons is equal the binding energy is at a maximum. The contribution of this term is also less important for heavier nuclides, which agrees with experimental findings.

B

a 1 *A - a 2 *A 2/3 - a 3 *Z 2 /A 1/3 - a 4 *(A/2-

Z)

2 /A+a 5

Paired electrons in the outer electron shell give chemically stable compounds, whereas unpaired electrons give radicals. The most chemically inert atoms are the noble gases (He, Ne, Ar, Kr, Xe, Ra), which have closed electron shells. The same phenomenon is found in the nucleus as

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well. A nucleus with an odd number of protons or neutrons is less stable than a nucleus with an even number of both protons and neutrons. The most unstable nuclei have an odd number of both protons and neutrons, e.g. 14 N (Z=7, N=7). In fact, only seven odd-odd stable nuclides exist, all of them among the light elements. This last factor a 5 takes care of this effect in the following way

a 5

=

a pair A -3/4

0

for even-even nuclei for even-odd nuclei

-a pair A -3/4 for odd-odd nuclei

When this model is fitted to experimental data the following parameters are obtained

a 1 =15.76 MeV a 2 =17.81 MeV a 3 =0.7105 MeV a 4 =94.81 MeV a pair = 34 MeV

An interesting parameter is the mean binding per nucleon, B/A.

interesting parameter is the mean binding per nucleon, B/A. Figure 6 Mean binding energy per nucleon

Figure 6 Mean binding energy per nucleon as a function of mass number A. The liquid drop model is fitted to measured data. The area from 0<A<50 is enlarged in the lower part of the figure. As seen, the crude empirical model fits the data well except for the light elements.

This value, which gives the mean energy needed to separate one nucleon from the nucleus, varies from a few MeV to about 9 MeV as illustrated in Figure 6. The mean binding energy per nucleon is a smoothly varying curve that has a maximum around the iron part (A 60). If two light elements are fused together they gain energy. This effect is used in the fusion principle to obtain nuclear power. If one heavy element is split in two, the total binding energy increases as well. The excess in energy is then released and used in the fission principle to obtain nuclear power.

As seen in Figure 6, the liquid drop model fits experimental data quite well. However, at a closer look, especially for the light elements there are some disagreements. This is because the nucleus can have closed proton and neutron shells that are especially stable structures. Critical numbers are 2, 8, 20, 28, 50, 82 and 126. This should be interpreted as if the nucleus has eight protons (oxygen) there is a closed proton shell and 20 neutrons will give a closed neutron shell, etc. Of special interest are nuclei with both a closed proton shell and a closed neutron shell e.g. 16 O (Z=8, N=8) or 40 Ca (Z=20, N=20). It has long been known that some nuclides (so called magic nuclides) were especially stable, but not the reason why. In the close-up of Figure 6, these nuclides seem to have extra high binding energy in comparison with the surrounding nuclides.

RADIATION FROM RADIOACTIVE NUCLIDES

Since radioactive material is the source of radiation commonly encountered in a laboratory (labeled compounds, calibration preparations), radioactive decay is reviewed fairly thoroughly in this section.

The concepts of nuclide and isotope are not related with whether the nucleus is stable or unstable. There are stable (non-radioactive) nuclides and isotopes, just as there are unstable (radioactive) nuclides and isotopes.

The number of neutrons and protons in the stable nucleus obeys certain laws of symmetry.

11

The carbon isotope 12 C is stable. The element carbon has six protons (Z = 6) and the same

number of neutrons (N = Z = 6). If one neutron

is

removed, the carbon isotope 11 C (Z=6, N= 5)

is

obtained. This nuclide is not stable and will

sooner or later undergo restructuring. If a neutron is added, 13 C (Z=6, N = 7) is obtained, which is stable. However, its natural abundance (1.1 %) is low compared with 12 C.

Further addition of one neutron gives 14 C(Z=6, N=8), which also is radioactive. It is a general rule (with a lot of exceptions) that the further you move from the stable combination of neutrons and protons, the more unstable the nucleus becomes, which means that restructuring to a stable condition occurs more quickly (shorter half-life).

Radioactivity and decay time

The radioactive process, i. e. the decay of a nucleus, is a statistical process. This means that the decay time of an individual radioactive nucleus can vary. But, for a large number of radioactive atoms (N) the same fraction (dN) always decays during the same time (dt). We can write this mathematically as

dN =

where is called the decay constant and is the probability for a nucleus to decay per time unit. We can integrate this equation to obtain

N = No e - t

where No is the number of radioactive atoms at

t=0.

N dt

-

The number of decay per time unit (A = - dN/dt)

is called radioactivity. The relation between the

radioactivity and the number of radioactive

atoms is then A = N. Replacing this in the formula above gives

A = Ao e - t

where Ao is the radioactivity at t=0. Ao is also equal to No.

Every radioactive decay is associated with a characteristic decay time. A common way to

express this is to use the half-life (T½) i.e. the time it takes to half the number of radioactive atoms. If we insert this time in the decay formula, we get the following relation between the half-life and the decay constant

Ao/2 = Ao e - T½ or

T½ = ln(2)/

We can also write the decay formula as

A = Ao 2 -t/T½

After one half-life the radioactivity is reduced to a half, after two half-lives to a quarter, after three half-lives to an eight, and after four half- lives to a sixteenth. Since

( 1/2 ) 10 =

1/1024 ~

10 -3

one may use as a rule of thumb that ten half- lives reduces the radioactivity by a factor thousand and 20 half-lives by a factor million of its initial value.

The half-life varies considerably for the various radioactive nuclides. It can be fractions of seconds, to hundreds of years or more. We usually express the half-life in seconds (s), minutes (m), hours (h), days (d) and years (a). Note that a is the SI-unit for the mean year = 365.24220 days.

The unit of radioactivity in the SI-system is the Becquerel, after the French physicist who in 1896 discovered natural radioactivity. The unit

is abbreviated to Bq.

1 Bq

=

1 decay / s

Decay per second is also written as dps, after the initial letters of the English words. An alternative way to express radioactivity is dpm, decays per minute.

Curie (Ci) is an old unit for radioactivity that is still used. From the beginning it was defined as the radioactivity of 1 g radium, but was later standardized to 3.7 * 10 10 decays per second.

12

The conversion factor from the old unit to the new unit is

1 Ci

= 3.7 * 10 10

Bq = 37 GBq (G = giga)

Table 3 Conversion from Curie (Ci) to Becquerel (Bq) and the prefixes in the SI-system

 

Prefix

   

Ci

Bq

 

Prefix

M=mega

MCi

10

6

3.7*10 16

37

PBq

P=peta

k

= kilo

kCi

10

3

3.7*10 13

37

TBq

T=tera

 

Ci

1

3.7*10 10

37

GBq

G=giga

m = milli

mCi

10

-3

3.7*10 7

37

MBq

M=mega

=micro

Ci

10

-6

3.7*10 4

37

kBq

k

= kilo

n

= nano

nCi

10

-9

3.7*10 1

37

Bq

 

p

= pico

pCi

10

-12

3.7*10 -2

37

mBq

m = milli

f

= femto

fCi

10

-15

3.7*10 -5

37

Bq

=micro

a

= atto

aCi

10

-18

3.7*10 -8

37

nBq

n

= nano

Surface radioactivity is given in Bq /m 2 , radioactivity concentration in Bq /m 3 and specific radioactivity in Bq /kg.

Radioactive decay

Unstable nuclides have a surplus of energy compared with the surrounding nuclides. By making a transformation within the nucleus, this surplus energy decreases and the remaining nucleus will be more stable (the binding energy increases). There are many ways to rearrange the nucleus to obtain a more stable nucleus. As an example, if we remove one neutron from e.g. 14 C we obtain the stable 13 C. However, this is usually not a spontaneous process. As seen in Figure 6, one needs 5-8 MeV to remove one nucleon. Even if the nucleus gains energy in the end it does not have access to the primary energy needed to run this process. For very heavy nuclides the binding energy of the neutrons decreases and here we can find spontaneous neutron emission. However, in general this process is rare.

The - decay

A process that can occur spontaneously is the

beta-decay. The number of nucleons is kept constant in the decay but a neutron is changed into a proton, or vice versa. A particle of

positive (positron or + ) or negative charge (negatron or ) is removed from the nucleus along with energy (the particle's rest mass + kinetic energy).

The particle has the same weight and the same particle properties as an electron. In fact, it can not, when it has lost its kinetic energy, be distinguished from an electron. Still, we name it a beta particle to mark that it was created in a nuclear process in the nucleus. We will below see that also electrons can be emitted in radioactive decays but they all will come from the electron shells around the nucleus.

In a radioactive nucleus rich in neutrons, the

decay occurs as if a neutron (n) were converted

to a proton (p):

n -->

p

+

+ energy

(1a)

This reaction formula fulfils some criteria. On both sides

1. the mass is about equal since the neutron weight is the sum of the proton and the electron weight

2. the charge is the same

3. the numbers of nucleons are the same

However, although the energy released per decay is a constant it was found that the kinetic energy of the beta particles varied between zero and the decay energy. To explain the missing energy the physicist Wolfgang Pauli 1930

suggested an additional particle now known as the neutrino. This uncharged particle with little

or no mass was also emitted in the decay and

shared the decay energy with the beta particle. 25 years later the neutrino was experimentally verified. The complete reaction formula for the beta decay can then be written as

n -->

 

+

+

+ energy

(1b)

p

 

13

where is the neutrino. The bar above the indicates that the neutrino is an antiparticle (antineutrino).

Symmetry is an important feature of nature. For most particles, there is an associated antiparticle which has the same mass. Other properties like charge will be the opposite. Charged particle- antiparticle pairs can annihilate, i.e. the masses will disappear and the released energy will be converted to photons.

Formula 1b also fulfils another rule in particle physics that you can not create particles out of nothing. The number of heavy particles (the nucleons) is the same on both sides. The same is true for light particles like the electron and the neutrino. Since particles and antiparticle cancel out the number of light particle is then also the same on both sides (zero).

The decay of 14 C is an example of beta minus decay.

14 C(Z=6, N=8) --> 14 N(Z=7, N=7)+ + +energy (2}

N=8) --> 1 4 N (Z=7, N=7) + + + energy (2} Figure 7 Decay scheme

Figure 7 Decay scheme for 14 C. The x-axis gives the number of protons in the nucleus and the y-axis its energy content. By converting a neutron to a proton, the number of protons in the nucleus increases and at the same time it becomes more stable. In the process, a negatively charged beta particle is emitted.

The + decay can be regarded as a proton that is converted to a neutron.

p --> n + + + + energy

(3)

The + is now the antiparticle and cancel out the “real” neutrino to sum up light particles on the right side to be zero.

An example of the positron decay is:

11 C(Z=6, N=5) --> 11 B(Z=5, N=6) + + + +energy (4}

11 C Z=6, N=5 E=2 MeV 11 B Z=5, N=6 5 6 Binding energy
11
C
Z=6, N=5
E=2 MeV
11
B
Z=5, N=6
5
6
Binding energy

Number of protons in the nucleus

Figure 8 Decay scheme for 11 C. The x-axis gives the number of protons in the nucleus and the y-axis its energy content. By converting a proton to a neutron, the number of protons in the nucleus decreases and at the same time it becomes more stable. In the process, a positively charged beta particle is emitted.

The radioactive nuclides used in laboratory work usually have an excess of neutrons and consequently emit their energy in the form a - particle, which is ejected from the nucleus with a specific kinetic energy and decelerates in the surrounding material.

The kinetic energy of the emitted particles is determined by the energy released in transformation of the nucleus. This may be illustrated in an energy diagram or a decay scheme. Figure 7 shows such a diagram for 14 C and Figure 8 for 11 C.

The 14 C-decay releases energy of 156 keV and the beta particle has a maximum kinetic energy of 156 keV. The 11 C decay releases 2 MeV but the maximum energy of the + is only about 1 MeV. This is because two new electron masses are created in the + decay, which corresponds to 1 MeV. We can understand this by looking

14

at the mass balance in equations (1b) and (3). The mass of the neutrino can be neglected.

The mass of a neutron (Mn) is approximately equal to the mass of a proton (Mp) and a beta particle (M ). Equation (1b) is then in a mass balance

Mn

Mp

+

M

In equation (3) we have the mass of a proton on the left side and the mass of a neutron and a beta particle on the right side. The only way to get the equation in balance is to add two beta masses on the left side.

2* M +

Mp = Mn + M

According to the Einstein formula E = Mc 2 . The mass of two beta particles corresponds to 1,022 MeV. In the 11 C decay, a total energy release of 2 MeV is available. Of this energy about 1 MeV is taken to account for the extra mass created in the decay, leaving 1 MeV to be shared by the positron and the neutrino. In the decay scheme in Figure 8, this is indicated by the broken arrow from 11 C to 11 B. The first vertical part indicates the energy needed within the 11 C nucleus to create the two electron masses. The diagonal part of arrow indicates the part of the decay energy that is converted into kinetic energy of emitted particles.

The decay energy

The decay of 14 C always releases 156 keV. Other beta decays, i.e. 3 H and 32 P (see Table 1), are also associated with a unique energy release.

Table 1 Decay parameters of some common radionuclides.

Nuclide

Half -life

Residual

Decay energy, Eo KeV

3

H

12.26 a

3

He

18

14

C

5 760 a

14

N

156

32

P

14.3 days

32

S

1710

The -particles share this energy with the neutrino randomly. The sum of the particle

and the neutrino kinetic energies are then equal to the decay energy, Eo:

E

+

E

=

Eo

In most beta decay the relative energy distribution of the -particles has the same shape (Figure 9).

Relative number of -particles

the same shape (Figure 9). Relative number of -particles Figure 9 Energy spectrum of particles at

Figure 9 Energy spectrum of particles at radioactive -decay. The energy is given on the x-axis and the number of particles per energy bin on the y-axis.

The distribution of energy to the particles is determined statistics. The neutrino is an uncharged particle of unknown, but very small, mass. It seldom interacts with matter and its energy can in practice be ignored. Only the energy, E , can be transferred to the surrounding material. The maximal beta energy and the mean beta energy can be written as:

(E ) max = E o

E

E o /3

When calculating the maximum range of the

particles, ( ) max is used.

Table 2 Maximum range of -particles in air and water.

Nuclide

(E ) max

Range (mm)

 

(keV)

Air

Water

3

H

18

6.5

0.007

14

C

159

300

0.3

32

P

1710

7700

7.9

15

Q-value

Each nuclear transition is characterized by a fixed energy release or a Q-value. If the Q-value is positive, surplus energy is emitted in the transformation. If the Q-value is negative, additional energy is needed to enable the transformation. A spontaneous radioactive decay has always a positive Q-value, whereas a nuclear reaction in e.g. a nuclear reactor often is associated with a negative Q-value. The energy released in a nuclear decay can be used to create new mass or to give emitted particles kinetic energy.

Pure beta decays go from the ground level of the radioactive nucleus to the ground level in the daughter nuclide. Three bodies share the decay energy, the beta particle, the neutrino and the recoiling rest nucleus. However, since the mass of the recoiling nucleus is much larger than for the other particles, the energy of the recoil nucleus is virtually zero. The total reaction energy is then statistically distributed between the beta and the neutrino, and the Q-value is numerically close to (E ) max .

More generally, the decay may produce excited states in the daughter nuclide. The nucleons, i.e. the protons and the neutrons, create quantified states of the nucleus. In the ground state, movements and energy contents are at a minimum. In an excited or deformed state, the energy content is higher. The nucleus can suddenly change its state, from a more excited state to a less excited or deformed state. In this process electromagnetic photons, i.e. gamma rays, are emitted. The gamma rays carry away parts of the total decay energy. For each photon (gamma quantum) emitted, the excitation energy of the nucleus diminishes until it finally reaches the ground energy state.

An example is the decay of 60 Co what can be illustrated in the decay scheme below (Figure 10). It is a beta minus decay emitting a beta particle with a maximal energy of 2.824 – 2.506=0.318 MeV. The decay created an excited daughter nucleus 60 Ni. This excited levels emits a gamma of 2.506-1.332=1.173 MeV. A new excited level is created which also

emits a gamma of 1,332 Mev. If we ad up the total energy emitted 0.318+1.173+1.332 we end up with the Q-value of the decay (2.824 MeV).

Energy (M eV ) 2.824 2.506 1.173 M eV gam m a em itted 1.332
Energy
(M eV )
2.824
2.506
1.173 M eV
gam m a
em itted
1.332
1.332 M eV
gam m a
em itted
0

Figure 10 A simplified decay scheme for 60 Co. Only dominant radiation is included.

Electron capture

The total energy release (the Q-value) in a positron decay has to be more than 1 MeV to compensate for the increase in mass (see above). An alternative route of decay that does not need this extra energy is electron capture. Instead of converting a proton to a neutron and a positron, the nucleus can attract an electron from the surrounding electron shells and join it with a proton to create a neutron.

e -

The effect is the same as in the positron decay; a proton is converted to a neutron. However, since no beta particle is emitted the full excess energy in the decay of the nucleus has to be given to the neutrino. Accordingly, in this type of decay monoenergetic neutrino particles are emitted. The decay of 125 I is a typical example of this process (Figure 11 and 12).

+

p

-->

n +

Although no beta particle is emitted the electron capture is a variant of the beta decay since the same physics is involved. There is then three branches of the beta decay, the beta minus, the beta plus and the electron capture.

Conversion electrons

The decay of 125 I gives a new example of a decay process ending in an excited state of the daughter nuclide (Figure 11). As said above, the

16

common way to emit the energy in the excited state is by emitting a gamma ray. This is also done in the 125 I decay, but only in 7 % per decay. The excited state, 35.5 keV, is very close to the binding energy of the K-shell electrons (33 keV). There is a probability that a K-shell electron is inside the nucleus due to the quantum mechanical nature of the electron. There is also a probability that the excited state interacts with and transfers its energy to the K- shell electron. The transferred energy is higher than the binding energy, and we obtain a monoenergetic electron, a conversion electron, in 93 % of all decays.

The excited state does not only interact with the K-shell but also with the L-shells and the M- shells although the probability is less (the electrons are further away from the nucleus and thus the probability of being inside the nucleus is smaller). The energy of the conversion electrons varies according with the formula below

E = 35.5 keV - E shell

where E shell is the binding energy of the shell from which the electron is emitted.

In the 60 Co decay a small amount of conversion electrons is found as well. In fact, an excited state in a nucleus always has two ways to de- excite, either by emitting a gamma or by converting the excited energy to a shell electron. The heavier the nuclide is, the higher the percentage of conversion electrons. A heavy nucleus has many protons in the nucleus and a strong attractive force on the shell electrons that are close to the nucleus. Thus, the probability that the excited state will interact with the electrons increases.

Another important factor that affects the probability of emitting conversion electrons is the energy of the excited level. Energies close to the binding energy of the shell electrons give the highest probabilities.

The electron capture and the conversion electrons both create holes in the electron shell. The process to fill these holes created a cascade

of events and the emission of electrons called Auger electrons and characteristic X-rays. These processes are exemplified and explained in more details in the decay of 125 I.

Decay of 125 I

125 I is a neutron deficient nucleus (the stable isotope of iodine is 127 I). It decays to 100% by electron capture since its Q-value of 186 keV is far to low for positron decay. The decay scheme is seen in figure 11 and shows that the decay in 100% yields an excited level in the daughter nuclide Tellurium-125. This excited level of 35.5 keV is just above the binding energy of the k-shell electrons (33 keV). This excited level is de-excited by gamma emission but only in 7% per decay. More likely (93% per decay) is that a conversion electron (energy 35.5-33=2.5 keV) is emitted.

149

35.5

125 I (Z = 53, N = 72)

keV EC (Electron capture) 125 Te in an excited stage keV emitted gamma (7 %)
keV
EC (Electron capture)
125 Te in an excited stage
keV
emitted gamma (7 %) or
conversion electron (93 %)

125 Te (Z = 52, N = 73)

Figure 11 Decay scheme of 125 I. The number of protons in the nucleus is on the x-axis and the energy content of the nucleus on the y-axis. By capturing an orbital electron, a proton is converted to a neutron and at the same time, the nucleus becomes more stable. In the process, a neutrino is emitted and carries away the energy which is formed. The new nucleus is formed in a excited state, but after a time it is de-excited to a more stable state. In this process, either a gamma ray or a conversion electron is emitted.

Both at the electron capture, when an electron is drawn into the nucleus, and at the forming of conversion electrons, holes appear in the electron shell around the nucleus. These holes become filled by electrons from the outer shell. In this process, the disparity in the binding

17

energy is transmitted as X-rays or free electrons that are dislodged from the atom (Auger electrons). This process is seen in more detail in Figure 12.

Electron

capture, EC

Cascade of

characteristic

X-rays

and Auger

125 Te in an excited state

X-rays and Auger 1 2 5 Te in an excited state Step 1 Step 2 Step

Step 1

X-rays and Auger 1 2 5 Te in an excited state Step 1 Step 2 Step

Step 2

and Auger 1 2 5 Te in an excited state Step 1 Step 2 Step 3

Step 3

Auger 1 2 5 Te in an excited state Step 1 Step 2 Step 3 Step

Step 4

2 5 Te in an excited state Step 1 Step 2 Step 3 Step 4 Step

Step 5

Decay of excited 125 Te to ground state by internal conversion

Conversion

electron

state by internal conversion Conversion electron Step 6 1 2 5 Te in ground state Figure

Step 6

125 Te in ground state

Figure 12 Details of the 125 I-decay

Hence, the main radiation from 125 I are K shell X-rays of 27 keV and Auger electrons of low energy. The range of the electrons is

comparable to that of

Generally, the photon radiation is brought to a standstill practically by two millimeters of

brass, whereas several decimeters of water are required.

particles from 3 H.

Alpha decay

Alpha emitting radionuclides are not commonly used in the laboratory and will only briefly be treated here. The physics involved is different from the beta decay and can actually be described as a tunneling effect through the potential barrier around the nucleus. The following description is just to get an idea of what this potential barrier is and the main features of the decay.

Consider a free He ++ ion outside a heavy nucleus (see Figure 13). If you try to move the He ++ ion closer, an increasing Coulomb force

in-between occurs. This force tries to repel the He ++ ion until it is so close to the nucleus that the strong force starts to act. The He ++ ion is then trapped inside the so-called nuclear potential, which is created in a balance between the nuclear force and the Coulomb force. The barrier the He ++ ion has to climb before it reaches the attracting nuclear force is called the coulomb barrier. Its height depends on the number of protons in the nucleus, but is in the order of 5-7 MeV for heavy nuclei.

When particles are trapped in the nucleus they loose their identity. However, the He ++ ions consist of two protons and two neutrons. Both the proton shell and the neutron shell are closed and the He ++ ion is a very stable combination of nucleons. One might consider that this stable combination can exist in the nuclear “soup” in the form of a virtual -particle. Also, these virtual particles may populate different energy levels in the nucleus. In the nucleus, the energy content is quantified and different quantified energy levels exist.

In Figure 13, two such levels are indicated. In the bound level 1, the virtual particle cannot escape the nucleus since it is bouncing against an infinitely thick potential wall. In the bound level 2, however, a potential wall exists that keeps the virtual particle trapped but it is not infinitely thick. The -particle may penetrate the wall by, what is known in quantum mechanics as, tunneling. Suddenly, the - particle appears in a materialized form outside the Coulomb barrier with energy corresponding to the excited level.

He ++ repulsive + coulomb + force
He ++ repulsive
+ coulomb
+ force
 
He ++ repulsive + coulomb + force  

bound level 2

 

bound level 1

 

Nucleus Z>80

heavy positivly

charged

18

Figure 13 Schematic view of the alpha decay The probability of decay is highly determined

by the thickness of the barrier, and the half-life of useful radioactive sources varies from hours

to many thousands of years. Alpha particles

appear in one or more energy groups that are, for all practical purposes, monoenergetic. For each distinct transition between initial and final nucleus, a fixed energy difference or Q-value characterizes the decay. This energy is shared between the alpha particle and the recoil nucleus.

The alpha particle energy correlates strongly with the half-life of the parent nuclide; the highest energies have the shortest half-lives. Above 7 MeV, the half-life can be expected to be less a few hours and. On the other hand, if the energy drops below 4 MeV, the barrier penetration probability becomes very small and the half-life of the isotope will be very large. Probably the most commonly used source for alpha particles is 241 Am (T½=433 a) with an - energy of 5.5 MeV.

Because alpha particles lose energy rapidly in materials, alpha particle sources must be prepared in very thin layers. To contain the radioactive material, typical sources are covered with a metallic foil or other material that must also be kept very thin if the original energy and monoenergetic nature of the alpha emission is to be preserved.

Almost all naturally occurring alpha emitters are heavy elements with Z >83. The principle features of alpha decay can be learned from the example of 226 Ra:

226

88

Ra

222

86

Rn +

4

2

He

The energy released (Q-value = 4.88 MeV) in the decay arises from a net loss in the masses

M Ra , M Rn and M He of the radium, radon, and

helium nuclei:

Q = M Ra - M Rn - M He

The general equation for the energy release in the alpha decay is then

Q =M parent -M daughter -M He Spontaneous fission

The fission process splits the nucleus into two parts of almost equal size. In the process free neutrons are also emitted. Fission fragments are used to calibrate and test detectors intended for general application in heavy ion measurements.

The most widely used example is 252 Cf, which undergoes spontaneous fission (3% per decay) and alpha decay (97% per decay) with a half-life of 2.65.

Each fission gives rise to two fission fragments, which, by the conservation of momentum, are emitted in opposite directions. Because the normal physical form for a spontaneous fission source is a thin deposit on a flat backing, only one fragment per fission can escape from the surface, whereas the other is lost by absorption within the backing. The spontaneous fission of 252 Cf also liberates a number of fast neutrons.

Natural radioactivity

Some heavy elements ( 232 Th, 235 U and 238 U) has such long half-lives (10 9 -10 10 a) that they have survived the time since the where created in the Big Bang and are still to be found in appreciable amounts. In there decays they produce a series of more short-lived radioactive daughters. Some of these daughters we are very much aware of e.g. the alpha emitter Radon-222, which is a noble gas and that can penetrate into our house

40 K EC (11 %) 1461 keV (T½=1.28 10 9 a)
40 K
EC (11 %)
1461 keV
(T½=1.28 10 9 a)
into our house 40 K EC (11 %) 1461 keV (T½=1.28 10 9 a) + (0.001

+ (0.001 %) 482 keV

- (89 %) 1312 keV
- (89 %)
1312 keV

40 Ca

40 Ar

Figure 14 Decay scheme for 40 K

19

Few lighter elements have naturally occurring radioisotopes with that long half-live. The most important from the standpoint of human exposure is 40 K, which is about 0.01% abundant and has a half-life of 1.26 x 10 9 years (Figure 14). The nuclide can decay by - emission (89%), EC (11%), or + emission (0.001%). The maximum - energy is 1.314 MeV. This isotope is an important source of human internal radiation exposure, because potassium is a natural constituent of plants and animals.

Another important, naturally occurring radioisotope is 14 C, used in carbon dating. It is produced by the bombardment of nitrogen in the atmosphere by cosmic rays, causing the reaction 14 N(n, p) 14 C. Its half-life is 5730 yr. The radioisotope, existing as CO 2 in the atmosphere, is used by e.g. trees and becomes fixed in their structure through photosynthesis. When an tree dies the incorporation of new 14 C atoms stop and the number will start to decrease due to the radioactive decay. By, in a sample, comparing the number of 14 C with the number of stable 12 C one can then calculate the time that has passed since the tree was cut and used for e.g. building a house. Thus, the age of such objects can be determined. The atmospheric testing of nuclear weapons has significantly added to the world's inventory of 14 C.

DATA ON RADIOACTIVE NUCLIDES

There are several books available, with all relevant information on decay-time, type and number of particles emitted per decay, energy per particle, etc. However, the fastest and cheapest way to obtain information today is by the Internet. One good site is

http://www.nndc.bnl.gov/nudat2/indx_dec.jsp

Below there is an example of the 125 I decay and with some explanations.

CHAPTER 3

INTERACTION WITH MATTER

Matter is composed by a number of different atoms in chemical combinations. A piece of iron is in a macroscopic sense solid and difficult to penetrate. However, at the dimensions of ionization radiation, matter is rather empty and without any major mechanical obstructions to prevent radiation to pass.

Consider a neutron entering a piece of iron. The iron atom has a dimension of 10 -10 meters but the iron nucleus is only 10 -15 meters, and the neutron itself is even smaller. The electrons have no known extension and since the neutron has no charge it will not feel any electric forces. The neutron will probably pass through a thin iron foil without noticing the material. However, if the foil grows thicker it will increase the likelihood that the neutron will hit one of the atom nuclei, cause a nuclear reaction and transfer its energy to the matter.

If we exchange the neutron for a proton, a dramatic change occurs. The proton will experience that matter is full of charge. Each orbit electron in the vicinity of the proton will feel a force of attraction, the Coulomb force (Figure 1).

electron mass m charge -q distance r closest distance d F = q*q/r 2 proton
electron
mass m
charge -q
distance r
closest
distance d
F = q*q/r 2
proton
mass M

velocity v

charge +q

Figure 1 A proton that enters into matter experiences an attractive force from all the orbit electrons in the vicinity.

We can say that we have a collision between two electrical fields and in which energy is transferred to the orbit electron. Sometimes the

21

energy exceeds the binding energy and we obtain a free electron, ionization. The same thing is true for an electron or a beta particle that will experience a force of the same strength but repulsive.

will experience a force of the same strength but repulsive. Figure 2 An -particle transfers so

Figure 2 An -particle transfers so much energy that an ionization occurs. Since the - particle and the orbital electron have opposite polarity, there is an attractive in-between.

have opposite polarity, there is an attractive in-between. Figure 3 The electrical field of a beta

Figure 3 The electrical field of a beta particle collides with that of an outer orbit electron. So much energy is transferred that the orbital electron is dislodged (ionization). Since the incoming electron and the orbital electron have same polarity, a repulsive force is created.

However, the electron and the proton differ considerably; they have different masses and different speeds. An electron with the energy of 1 MeV has a speed close to the speed of light (3*10 8 m/s). The time it will spend in the vicinity of an atom and an orbit electron will be 10 -18 - 10 -19 seconds. The force will act during a very short time and the impulse F*dt transferred from the incoming electron to the orbit electron will be small. A proton of the same energy (1 MeV) will have a speed 20 times lower than the electron. The time spent in the vicinity of the orbit electrons will be correspondingly longer and the transferred impulse larger. From this simple consideration we can draw two important conclusions that are true for charged particles:

1. The heavier the particle is, the more energy is transferred per collision.

2. The lower the kinetic energy of the particle is, the more energy is transferred.

The expression "ionizing radiation" includes many types of "radiation". The most important kinds of radiation are classified according to how they transfer energy to matter in the diagram below (Figure 4).

IONIZING RADIATION

Electro-magnetic Particles radiation, photons (X-rays and gamma) (protons, electrons, alpha and neutrons) Uncharged
Electro-magnetic
Particles
radiation, photons
(X-rays and gamma)
(protons, electrons,
alpha and neutrons)
Uncharged particles
Charged particles
(neutrons)
(protons, electrones
and alpha)
Light, charged
Heavy, charged
particles
particles
(electrones)
(protons and alpha)

Figure 4 Schematic subdivision of the different types of ionizing radiation.

The direction of heavy, charged particles is scarcely affected by collisions with orbital electrons. They continue to travel mainly

22

straightforward to the end of their range, deviating only slightly from a straight line. Thus, heavy, charged particles have a well- defined range and monoenergetic particles travel about the same distance in a given material.

When heavy, charged particles are obstructed their speed diminishes. Consequently, they spend a longer time close to the next orbital electron and transfer more energy to it. Then, the number of ion pairs formed per unit of length increases (see Figure 5).

pairs formed per unit of length increases (see Figure 5). Figure 5 Deceleration of an particle

Figure 5 Deceleration of an

particle in air.

The -particle at high energy has high speed. The time it spends near each orbit electron is short; hence, the transferred energy is small and the probability for ionization is relatively small. When the energy diminishes so does the velocity. The probability of ionization increases and a typical ionization peak at the end of the particle track (the Bragg peak) occurs.

If the incoming charged particle is an electron, the rest mass of this particle is the same as for the orbital electron. When two particles with the same mass collide, a great deal of energy (almost all) can be transferred in a direct impact and the incoming particle will come to a complete stop. For two electrons we have a problem; they are identical. We cannot with any means know which one is the incoming particle and which one is the orbital electron. For practical reasons, therefore, we define the electron with the highest energy after the collision to be the incoming particle.

At each collision, light charged particles can change direction very markedly and by repeated large directional changes can even be scattered backwards to the direction of their origin (Figure 6). Hence, the range of electrons differs considerably. However, a maximum range can be given (Figure 7).

At these collisions, the energy that is transferred is frequently sufficient to ionize an orbital electron. The energy might even be so high that the free electron, in turn, can cause new ionization. Hence, part of the energy of the primary charged particles is deposited at some distance from the original track of the particle. Secondarily formed electrons, particles, can give rise to further ionization tracks.

Back-scattered electron Bremsstrahlung S 2 0 4 0 6 0 8 0 1 0 0
Back-scattered
electron
Bremsstrahlung
S
2
0
4
0
6
0
8
0
1
0
0

Figure 6 Electrons, which penetrate material, collide with orbit electrons of the same mass as the incoming particles. They can effect marked directional changes including scattering in the direction opposite to the original course.

scattering in the direction opposite to the original course. Figure 7 A schematic figure illustrating the

Figure 7 A schematic figure illustrating the range of monoenergetic electrons. Most of the electrons are absorbed within a distance shorter than the maximal range.

23

Bremsstrahlung

When electrical charges are accelerated or decelerated, they can emit electromagnetic radiation. We call this roentgen, continuous X- rays or bremsstrahlung. Synchrotron light is of the same nature.

or bremsstrahlung. Synchrotron light is of the same nature. Figure 8a An incoming electron feels the

Figure 8a An incoming electron feels the Coulomb force from the nucleus and is deflected. The electron speed and kinetic energy decreases in the process - the electron decelerates. The difference in kinetic energy between in-going and out-going electron is emitted as an X-ray photon.

10 Coulomb collision 1.0 Water Lead 0.1 Bremsstrahlung 0.01 0.1 1.0 10 100 Energy loss
10
Coulomb collision
1.0
Water
Lead
0.1
Bremsstrahlung
0.01
0.1
1.0
10
100
Energy loss (MeV/g*cm 2 )

Electron energy (MeV)

Figure 8b Loss of energy by electrons per track length (expressed in mass per unit area) as a function of electron energy. A heavy and a light material show how the atomic number of the material influences the two ways by which electrons transfer energy to material.

Heavy particles lose only little energy per collision and are only decelerated in small steps.

Thus, for heavy particles the loss by bremsstrahlung is of little importance. Electrons, on the other hand, often lose a great deal of their energy by deceleration in the strong fields of heavy atoms; hence, the loss by bremsstrahlung is of more importance. The result of continuous radiation increases with the electron energy and atomic number of the absorber. For high electron energies and heavy elements (e.g. lead), the highest X-rays yield is obtained (Figure 8b).

Stopping power

Charged particles gradually lose their energy (they are decelerated) by many close "collisions" with orbital electrons in the irradiated material. The ability of different materials to decelerate charged particles varies considerably depending on the charge and energy of the charged particles, and the density and atomic number of the irradiated material. The deceleration capacity attributed to a given

material is denoted by how much energy (

expended in a given length ( l) of the charged particle’s track.

) is

Stopping power = (

) / ( l)

STOPPING POWER AS A FUNCTION OF PARTICLE ENERGY

10000 1000 electron 100 proton alfa 10 1 0.01 0.1 1 10 Stopping power (MeV/cm)
10000
1000
electron
100
proton
alfa
10
1
0.01
0.1
1
10
Stopping power (MeV/cm)

Particle energy (MeV)

Figure 9 Stopping power in water for electrons, protons and alpha particles as a function of energy.

Stopping power is a parameter that describes the material’s ability to stop charged radiation. For different combinations of particles and material, the ability to stop the radiation can be calculated

24

and tabulated. Stopping power data for electrons in lead and water are given in Figure 8. Stopping power for water is given for electrons, protons and - particles in Figure 9.

Linear energy transfer, LET

The energy that charged particles lose by deceleration is transferred to the irradiated material in different ways. The energy can be deposited more or less concentrated around the primary particles' track. Direct ionization results in energy deposition in the vicinity of the particles' track. However, secondary particles, such as bremsstrahlung and neutrons (in nuclear reactions) with no charge, may deposit their energy far away from the particle track. To understand the effect of radiation on living material, it is also important to have a measure of how densely the radiation's energy is deposited around the particles' track. Hence, the concept Linear Energy Transfer (LET) was introduced. It denotes the amount of energy the specified particle emits per unit track length and that is distributed near it.

DNA double helix

cylinder diameter 2r
cylinder
diameter 2r

5.3 MeV - track

DNA double helix cylinder diameter 2r 5.3 MeV - track Figure 10 Illustration of the ionization

Figure 10 Illustration of the ionization pattern around an -particle track. Each black spot represent one ionization. Around the track, the ionization density is highest. The limited stopping power or the linear energy transfer, LET r , is given as the energy per track length deposited inside a cylinder with the radius r. The radius r can vary, which gives different LET-values. Often, the radius r is set to be the diameter of the DNA double helix. Instead of giving the radius length in nanometers, it is given as the energy of an electron with the range r.

When living tissue is irradiated, LET usually denotes the energy absorbed per unit length around the particles' track within a cylinder. The diameter of this cylinder is chosen to be in the

same order as a biological critical structure, e.g. the cell nucleus or the DNA-molecule.

High LET and low LET

It is of interest to understand how many ionization are created in the DNA molecule of different types of radiation. A rough estimate is made in the following.

The stopping power for electrons, protons and alphas (see Figure 9) is recalculated and expressed in number of ionization/nm (Figure 11). It is seen that for electrons of all energies the number is below 0.1 ionization per nm. The more correct use of LET, not stopping power, gives an even lower number. Since the DNA molecule has a diameter of 2 nm, this indicates that it is very unlikely that electrons of any energy will cause two ionizations so close that a double strand break occurs.

High energy protons (E > 10 MeV) have the same pattern but low energy protons with energies <1 MeV yield more than 1 ionization/nm. Alpha particles over a wide range of energies also yield more than 1 ionization/nm. If the probability of causing a double strand break is low, we have low LET radiation whereas if the probability is high, high LET.

IONIZATION DENSITY

10 1 0.01 0.1 1 10 electron 0.1 proton alfa 0.01 0.001 0.01 0.1 1
10
1
0.01
0.1
1
10
electron
0.1
proton
alfa
0.01
0.001
0.01
0.1
1
10
Ions/nm

Particle energy MeV

Figure 11 Stopping power in water given as number of ionizations per nanometer for electrons, protons and alpha particles and as a function of particle energy.

25

Photon interactions

Non-charged particles such as photons and neutrons do not feel the Coulomb force and cannot transfer their energy to matter this way. However, in occasional interactions they may transfer all or much of their energy to charged particles in the irradiated material. Thus, these secondary charged particles (photons give rise to secondary electrons and neutrons chiefly to secondary protons) can continue to ionize through the charge interaction. Since the ionization of the primary interactions is small compared with the ionization of the secondary radiation, we sometimes refer to photons and neutrons as indirect ionization radiation. Only the interaction of photons is described here.

Regarding the interaction of photons with matter, three processes can be distinguished. The photoelectric effect implies that a bound electron, mainly a K-shell electron, absorbs the photon in one of the innermost atom shells. This electron, the photoelectron, obtains a kinetic energy that corresponds to the photon energy minus the electron's binding energy in the shell. An electron from one of the outer shells then fills the “hole” in the electron shell, and characteristic X-rays (or Auger electrons) are emitted. The energy balance in the transfer is

Auger electron Incoming photon Energy h*
Auger electron
Incoming photon
Energy h*

Characteristic

X-ray

Photo electron

Figure 12 The photoelectric effect. A photon interacts with a K-shell electron. All the photon's energy is used to displace the electron and give it kinetic energy. When the "hole" of the electron is filled with an electron from an outer shell, energy is liberated as a photon (characteristic X-radiation) or is transferred to another orbit electron (Auger electron) that leaves the atom.

h

=

el

+

e

where h

electron's kinetic energy and Be is the binding energy.

is the photon energy, Eel is the

The photoelectric effect is not significant in air and soft tissue (which includes material of low atomic number) for photon energies over 200 keV.

In the Compton effect, the electron binding energy is always insignificant in relation to the photon energy (Figure 13). The Compton effect can be interpreted as an impact process in which the photons collide with a free electron.

process in which the photons collide with a free electron. Figure 13 Compton effect. A photon

Figure 13 Compton effect. A photon interacts with an electron in an outer orbit. Only part of the photon's energy is used to dislodge the electron and deliver kinetic energy. The remaining energy is transmitted to a new photon that has a different direction and less energy than the incoming photon.

Hence, in this process the main electrons involved are the outer, loosely bound electrons. The physical laws of impact apply, since the system's total energy and momentum are the same before as after impact. This results in a photon with lower energy and indeed greater wavelength. The energy and the angle between the scattered photons and electrons can be calculated by using the laws on conservation of energy and impulse.

The probability of “Compton scattering" per electron of per unit mass is about the same for all material, but it decreases somewhat with increasing photon energy. The Compton effect is significant for photon energies between 100 keV and 10 MeV. Part of the incoming photon

26

energy, which is transmitted to the Compton electrons, is absorbed within a tiny volume around the region where the process occurs. The amount of energy transmitted to the scattered photons, however, is usually not absorbed in the immediate vicinity. The photon can cover a considerable distance before being absorbed.

The pair production effect (Figure 14) signifies

that the photon interacts with the electrical field

in the neighborhood of an atom's nucleus. The

photon disappears and its energy is converted to an electron and a positron (see Figure 15). The electron mass is equivalent to 0.511 MeV. Since two electron masses are created the incoming photon must have energy of at least 1.02 MeV. Surplus energy is given as kinetic energy to the electrons.

- e Incoming photon Energy h* + e
-
e
Incoming photon
Energy h*
+
e

Figure 14 Pair production. The incoming photon energy is so great that it can create two new particles, an electron and a proton. The entire energy of the incoming photon is required to create the mass of these particles (2*511 keV) and give these particles their kinetic energy.

A

positron can be said to be a positive electron.

It

has the same mass as an electron but a

positive, not a negative unit charge. On decelerating in matter, the positron behaves in the same way as the electron except that the positron at the end of the track attracts an electron and is "annihilated" by it. This means that the energy that is equivalent to two electron rest masses (2*511 keV) is converted to two 511 keV photons which are emitted in two directly opposite directions. This radiation is called annihilation radiation.

Recoil

Pair production and annihilation are thus two diametrically opposite processes. In pair production, a photon is lost and two light particles are formed, a negatron (ordinary electron) and a positron. Both of these particles are decelerated whereupon the positron is annihilated by an orbital electron during the emission of two 511 keV photons.

100 Photoelectric Pair 80 effect production 60 40 Compton effect 20 0 0.01 0.1 1
100
Photoelectric
Pair
80
effect
production
60
40
Compton
effect
20
0
0.01
0.1
1
10
100
Atomic number

Photon energy (MeV)

Figure 15 Dependent on the energy of the photons and the atomic number, the probability of different photon interactions varies. In the figure is shown a special case when the probability for the Compton effect is equal to the probability of the photo-effect (the curve to the left) and when the probability for the Compton effect is equal to the probability of pair production (curve to the right).

The relative significance of the different processes can be denoted as functions of photon energy and absorbing material. The combinations of energy and atomic number by which the probability of obtaining the photoelectric or the Compton effect are equally large (Figure 15).

For water and soft tissue with "effective atomic numbers" lower than 10, the photo-electric effect dominates for photon energies < 100 keV, the Compton effect for > 100 keV and < 10 MeV, and pair production for photon energies > 10 MeV.

For low photon energies and for high Z material where the photoelectric effect dominates, absorption discontinuities occur (Figure 16) at photon energies equivalent to the binding

27

energies of the inner shell electron. Just below, the photon energy is too low to interact and the electrons in this shell do not contribute at all to the attenuation processes. Just above, the probability of photon absorption is very high.

10 5 10 4 10 3 10 2 0 100 200 300 400 Probability of
10
5
10
4
10
3
10
2
0
100
200
300
400
Probability of the
photo effect (m -1 )

Photon energy (keV)

Figure 16 The probability for the photo effect in lead as a function of photon energy. Some discreet jumps in the curve are seen at energies corresponding to binding energies of the orbit electrons.

Heavy elements, where the binding energy of the K-shell electrons is high, are therefore likely to interact with high-energy photons. For example: In lead (atomic number = 82) the photoelectric effect dominates for photons with energies of < 0.5 MeV, the Compton effect at photon energies > 0.5 MeV and < 5 MeV, and pair conversion for photons with energies >

5MeV.

Attenuation of photons

For photons, as for neutrons, matter looks empty. Photons can pass a long way through a piece of material before they interact. They may even penetrate a piece of matter without any interaction. However, when the photons interact they lose all or most of their energy, which is transferred to charged particles.

The formula for the attenuation (damping) of photon radiation in material is:

N

where

=

No e - x

N is the number of non-scattered photons that leave the absorber No the number of photons incident on the absorber and is the linear attenuating coefficient (m -1 ), which is a measure of probability per unit length for a photon to interact x is the thickness of the absorber.

a photon to interact x is the thickness of the absorber. Figure 17 A narrow beam

Figure 17 A narrow beam of photons, No, hit a piece of material with thickness x. Some photons are absorbed or attenuated out of the beam. The number of photons hitting the detector is then N.

10 4 10 3 10 2 ==== ++++ ++++ 10 1 0.1 0.1 1 10
10
4
10
3
10
2
====
++++
++++
10
1
0.1
0.1
1
10
100
1000
Probability for different photon
interaction effects (m -1 )

Photon energy (MeV)

Figure 18 The probability in aluminum for the three main ways in which photons interact as a function of photon energy. The different effects are denoted. = photo effect = the Compton effect = the pair production effect = the sum of the three separate effects gives the total attenuation coefficient.

Unlike charged particles, photon radiation has no fixed range or maximum range. The interaction of photon radiation leads to an

28

exponential attenuation and there is always a certain finite probability that some photons will penetrate even thick material. What we can calculate is the fraction of photons that will interact in a certain thickness of irradiated material.

The linear attenuation coefficient ( ) is the sum of the photoelectric effect ( ), the Compton effect ( ) and pair conversion effect ( ). The photoelectric effect dominates at low photon energies, the Compton effect for moderate energies and the pair conversion effect for high photon energies. The contributions of different attenuating coefficients in aluminum are shown in Figure 18.

The thickness of the absorber that decreases the number of incoming photons by a factor of two is of special interest and has a special name, the half layer value (HLV). It is defined as

1/2 No

=

No e

HLV

It is related to the attenuation coefficient in the following way

HLV =

ln 2/

=

0.693/

So far, only the linear attenuating coefficient has been mentioned. It is often more convenient to deal with attenuation coefficient per unit mass, which is given by divided by , the density of the material. This gives the mass attenuation coefficient, which is also denoted by .

/

When using the mass attenuation coefficient per unit mass, it is necessary to multiply by both the thickness of the material and its density to obtain a non-dimensional exponent in the expression.

N

=

No

e - /

· x

where

dimension m 2 /kg and x m, hence it follows that

) has the

has the dimension m -1 , kg/m 3 . ( /

the exponent has no dimension. Variations of

the mass attenuation coefficient for lead,

copper, water and air are illustrated in Figure

19.

1 lead 10 -1 copper water air 10 -2 10 -3 0.01 0.1 1 10
1
lead
10
-1
copper
water
air
10
-2
10
-3
0.01
0.1
1
10
Mass attenuation coefficient (m 2 /kg)

Photon energy (MeV)

Figure 19 Mass attenuation coefficients for different materials.

There are other types of attenuation coefficients besides the mass and linear coefficients. An example is the mass energy absorption

coefficient, en / .

Compton and annihilation photons) can travel some distance from their production site before donating their energy in the form of secondary electrons. They may even escape the absorbing material completely. Secondary electrons (photo-, Auger-, Compton-, and pair-electrons), however, expend their energy in the immediate vicinity of the primary interaction and contribute to the dose absorbed in this region (absorbed dose is defined in the next section). To calculate the dose absorbed by these charged particles, the mass energy absorption coefficient, en / can be used. It is the product

of the mass attenuation coefficient /

fraction of the photons' energy f, which is converted to secondary electrons that lose their energy locally.

Scattered photons (X-ray,

and the

en /

= ( / )

f

It is evident by definition that en / is less than

/

( en /

< /

).

CHAPTER 4

Dosimetry

Absorbed dose

Ionization radiation carries energy. In different processes this energy is transferred to matter. Some of this energy is deposited locally; some travels away and might even escape the irradiated mass volume. Since some ionizing radiation can participate in nuclear reactions, energy may also be created (or lost) inside the irradiated volume.

E in m Figure 1 Absorbed energy E in a mass element m
E in
m
Figure 1 Absorbed energy E in a mass
element m

Generally we may write

Ei = E i,in -E i,out +Qi

where

(1)

E out

E i,in = energy of an incoming ionizing particle

(excluding rest mass)

E i,out = sum of energies of all ionizing particles,

created by incoming particle, leaving the place

of interaction (excluding rest mass)

Q i = accounts for changes in the rest mass

energy of the nucleus and of all elementary

particles involved in the interaction.

The energy, E imparted to a volume of matter with weight m (this volume is regarded as the place of interaction) is then

E =

E i

(2)

and the specific energy imparted, which is also called absorbed dose, is

D = E/m

(3)

30

The absorbed dose D has the unit gray (Gy) equal to 1 J per kg. An old unit is

1 rad = 0.01 Gy

One may reflect on the size of the unit Gy. A whole body absorbed dose of 4 Gy to man is a lethal dose, but raises the body temperature by only 0.001 o C. Obviously, 1 Gy is a rather large unit. Local absorbed doses of several Gy are given in radiation therapy whereas in laboratory work and in radiation protection, mGy and Gy are more commonly used.

Relative Biological Effect, RBE

The absorbed dose defined in equation 3 is a

macroscopic unit representing the mean energy

to a rather large mass volume. It does not

consider the stochastic ionization pattern of the energy delivery. However, low LET and high LET ionizing radiation can for the same absorbed dose cause quite different biological effects due to their different ability to cause single and double strand breaks. Another concept, Relative Biological Effectiveness (RBE) is introduced to describe this situation.

8 6 4 2 D D 0 1 2 3 4 Number of chromosome abberations
8
6
4
2
D
D
0
1
2
3
4
Number of chromosome abberations

Absorbed dose (Gy)

Figure 2 A comparison of two different radiation qualities, and . Photon radiation is always used as the reference since all the produced electrons are low LET-radiation.

A chosen biological system is irradiated and a

biological effect is measured (in Figure 2 this is

the number of chromosomal aberrations). Two qualities of radiation are used to irradiate the system (in Figure 2, and ) so that the same

biological effect is obtained. The relative Biological Effectiveness (RBE) is then defined as a ratio between the absorbed doses delivered

RBE = D /D

(4)

Photon irradiation (X-rays > 2-3 MeV or 60 Co- gamma rays) is usually used as a reference. This is because photons produce a wide range of electrons in a reproducible way. Electrons of all energies can be considered as low-LET radiation. Hence, one should expect RBE-values close to one for all photon irradiation. This is also found to be true, maybe except for very low X-ray irradiation since low energy electrons (< 100 keV) have a somewhat higher stopping power than higher electron energies (> 100 keV).

Dose equivalent

The RBE-values vary with radiation quality and chosen biological system. In radiation therapy, where acute radiation effects are expected, the RBE value has to be carefully measured for each situation. The biological effects of neutrons, protons and heavy ions have to be compared with established photon and electron therapy not just in one biological system, but in many. In radiation protection where radiation doses are lower and mainly late effects (such as the risk for induced cancer) are expected, we may generalize somewhat more.

20 15 10 5 0 1 10 100 1000 Quality factor, W R
20
15
10
5
0
1
10
100
1000
Quality factor, W R

Stopping power in water (keV/ m)

Figure 3 The quality factor W R as a function of stopping power in water

The measured RBE-values vary from 1 to 20 as a function of the stopping power of the radiation. A weighted curve of measured RBE

31

values (W R ) that can be used for radiation protection purpose is shown in Figure 3.

If we multiply the absorbed dose, D, with W R

we obtain a new dose variable, the dose equivalent, which includes both the energy concentration of the radiation and also its capability to cause late biological effects.

H = W R * D

(5)

The unit for the dose equivalent is Sievert (Sv)

if absorbed dose is expressed in Gy.

Effective dose

The radiation sensitivity of different organs in the body varies. Tissues containing proliferating cells, such as the bone marrow and the intestine, are generally more radiation-sensitive than e.g. the liver. If the radiation dose is unevenly distributed in the body, we need to consider this when risks of biological damage are estimated. For radiation protection purposes, relative values for different organs are given below (Table 1). These weight factors mainly relate to the ability of ionizing radiation to create late effects such as radiation-induced cancer.

Table 1 Weighting factors recommended by ICRP 30 for calculation of effective dose.

Organ

Weighting Factor, W T

Gonads

0.25

Breast

0.15

Red marrow

0.12

Lung

0.12

Thyroid

0.03

Bone surface

0.03

Remaining

0.30

We can then define the effective dose as

He =

W T * W R * Dorg

(5)

where we sum over the different organs. The unit for the effective dose is also Sievert (Sv) if the absorbed dose, D, is expressed as Gy. The calculation of the effective dose is illustrated in the following example.

Example 1. We want to compare the risk of late effects of two persons exposed to radiation of different quality and distributions. One is exposed to 1 Gy of gamma rays, whole body and the other to 1 Gy of alpha particles by inhaling radon gas.

Dint (Gy) = 1.6*10 -13 *n

E

/m

(7)

where

E

is the mean energy in MeV of the

beta energy emitted per decay, and n is the total number of decays in the mass m.

Type of

 

Comments

For radioactive sources, the absorbed dose rate,

irradiation

 

not the absorbed dose is of interest. Eq 7 can

 

Absorbed

 

easily be rearranged to

 

dose (Gy)

1

1

W

R

1

20

W R for

is 20

dH/dt = 1.6*10 -13 * W R * n/h *

E

/m

(8)

W

T

1

0.12

Ra-gas gives a local

 
 

irradiation of lung

where

 

Effective

1

2.4

The Ra-exposed person has a 2.4 higher probability to express late radiation effect

dH/dt is the dose equivalent rate in Sv/h

 

dose (Sv)

 

W

R is the weight factor for radiation quality

 

n/h is the number of absorbed particles per hour

 

E

is the mean energy in MeV per particle and

m

is the mass unit in kg.

The effective dose is a theoretical concept used

to calculate risks of various types of irradiation

situations. In practical radiation protection work one need to define other measurable variables. Radiation protection instruments are calibrated

in a sphere (tissue equivalent material) of

diameter 30 cm. They are placed 10 cm or 0.07

cm

from the surface to give

Hp

(10) = individual deep dose equivalent

Hs

(0.07) = individual surface dose equivalent

Relation between dose and radioactivity

The energy emitted in radioactive decay can, of course, be expressed in units of Gy and Sv. However, since the radioactivity is usually known in Bq and the energy of emitted particles

in MeV, we need to relate the absorbed dose

from radionuclides in these units.

The relation between the two energy units Joule and eV are

1 eV = 1.6 * 10 -19 J

(6)

From this relation, we can derive a simple formula for particle irradiation, such as pure beta-emitting radionuclides

32

The weight factor W R is 1 for radioactive decays emitting only beta, electrons and photons.

A more general treatment of the radioactive

decay is given in the following.

Consider a radioactivity concentration A in an organ. The radioactive decay emits particles of different types i = 1, 2, 3 … The mean energy of particle type i emitted per decay is then

i = k n i E i

where

k

is a unit dependent constant

n

i is the mean number of particle i per decay

E i is the mean energy of particle i per decay

i has the dimension energy and can by the proper choice of k be expressed in joules (J). However, usually the dimension is given as

(kg * Gy)/(Bq * h)

or (g * rad) / ( Ci * h)

The time-integral of the radioactivity concentration in the organ, A(t)dt has the

dimension Bq/kg * h. If we multiply the time integral with i we get the absorbed dose of that organ if the absorption of the emitted particle is 100 % localized in the organ.

Sources
Sources

Figure 4 Distributed radioactivity in the body gives a rather complicated irradiation pattern.

The radioactivity gives radiation that is locally absorbed (low energy beta, electrons and X- rays) and radiation that is partly locally absorbed (gamma, high-energy beta and electrons). This radiation may irradiate other organs (Figure 4) or may completely escape the body. A complete absorbed dose calculation after the administration of radioactivity in vivo also has to consider the kinetics of the labeled compound and its metabolism and excretion.

If the emitted particle is not locally absorbed we can give a factor f i (the fraction locally absorbed) by which we multiply the i -value. In the body, the situation becomes rather complicated.

To facilitate dosimetry calculations in nuclear medicine and in radiation protection, a dosimetry concept (MIRD) has been developed. MIRD stands for Medical Internal Radiation Dose. An expert committee has agreed on certain standard ways to express and calculate data. Measured physiological and kinetic data from human studies are used as input into theoretical kinetic models, which allows a

33

detailed calculation of integrated radioactivity concentrations in different organs. Mathematical standard phantoms have been derived which allow the use of Monte Carlo calculation techniques.

which allow the use of Monte Carlo calculation techniques. Figure 5 A MIRD phantom with standardized

Figure 5 A MIRD phantom with standardized organ sizes and positions. Each organ is given a mathematical definition that makes it easy to represent it in a computer. The i-values can be calculated for each radionuclide using nuclear spectroscopic data. The fraction of absorbed energy per organ and the fraction of energy absorbed in other organs can be calculated as a function of particle type and energy using Monte Carlo techniques. From physiological models, the time integral radioactivity curves can be calculated for each organ. The dose equivalent can be calculated for each organ and the effective dose by summing over all organs.

Using such techniques, one can rather precisely estimate the effective dose corresponding to a given radioactivity of a certain radionuclide. However, one has to remember that the MIRD concept still uses a number of approximations, such as standardized organ geometry and a homogeneous distribution of the radioactivity in each organ.

Table 2 ALI values (Bq) for some common radionuclides. The ALI-values correspond to an effective dose of 50 mSv.

Nuclid

ALI

Nuclid

ALI

Nuclide

ALI

3 H

3*10

9

65 Zn

1*10

7

129

I

2*10

5

14

C

9*10

7

69m Zn

2*10

8

130

I

1*10

7

18

F

2*10

9

67

Ga

3*10

8

131

I

1*10

6

22

Na

2*10

7

68

Ga

6*10

8

132

I

1*10

8

24

Na

1*10

8

73

As

6*10

7

129

Cs

9*10

6

32

P

1*10

7

74

As

3*10

7

130

Cs

2*10

9

33

P

1*10

8

75

Se

2*10

7

131

Cs

8*10

8

35

S

8*10

7

76

Br

1*10

8

134

Cs

3*10

6

36

Cl

9*10

6

77

Br

6*10

8

134m Cs

4*10

9

38

Cl

6*10

8

82

Br

1*10

8

137

Cs

4*10

6

42

K

2*10

8

81m Rb

9*10

9

131

Ba

1*10

8

43

K

2*10

8

81

Rb

1*10

9

133m

Ba

9*10

7

45

Ca

3*10

7

86

Rb

2*10

7

135m

Ba

1*10

8

47

Ca

3*10

7

88

Rb

7*10

8

140

La

2*10

7

51

Cr

7*10

8

89

Rb

1*10

9

169

Yb

3*10

7

52

Mn

3*10

7

85m Sr

8*10

9

192

Ir

8*10

6

52m M

1*10

9

85 Sr

6*10

7

198

Au

4*10

7

54

Mn

3*10

7

87m Sr

1*10

9

197

Hg

2*10

8

56

Mn

2*10

8

89

Sr

5*10

6

203

Hg

2*10

7

52

Fe

3*10

7

90

Sr

1*10

5

201

Tl

6*10

8

55

Fe

7*10

7

90

Y

2*10

7

204

Tl

6*10

7

59

Fe

1*10

7

99

Mo

4*10

7

210

Pb

9*10

3

56

Co

7*10

6

99m Tc

3*10

9

212

Pb

1*10

6

57

Co

2*10

7

109

Cd

1*10

6

210

Po

2*10

4

58

Co

3*10

7

115

Cd

3*10

7

226

Ra

2*10

4

60

Co

1*10

6

111

In

2*10

8

232

Th

4*10

1

63

Ni

6*10

7

113m In

2*10

9

238

U

2*10

3

64

Cu

4*10

8

124

Sb

9*10

6