Radiochemistry

NE 560

Nuclear Radiation
Dr. Ghadeer Malkawi

Fall 2018
 General Properties of Nuclear
Radiation
Knowledge of the properties of nuclear radiation is needed for the
measurement and identification of radionuclides and in the field of
radiation protection.
Charged high-energy particles or photons, such as a-particles, protons,
electrons, positrons, y-ray or X-ray photons, set off ionization processes in
gases, liquids or solids:
M>Mt+e

where M is an atom or a molecule. Any kind of radiation that is able to

produce ions is called ionizing radiation. The arrow > indicates a reaction
induced by ionizing radiation.
Excited atoms or molecules M° may also be produced
 Radiation Primary Reactions
* The minimum energy needed for ionization or
excitation of atoms or molecules Is of the order of
several eV, depending on the nature of the atoms or
molecules.
¢ Particles with energies of the order of (0.1 to IO) MeV,
however, produce a great number of ions and electrons
and of excited atoms or molecules.
* Heavy particles, such as a particles or protons, lead to
a high density of the reaction products in the track,
whereas the density of ionization reaction products Is
low in the track of electrons or gamma photons.
 Radiation secondary reactions
* The ions M* and the excited atoms or molecules M* produced in the
primary reactions with radiation give rise to further (secondary)
reactions:

M*>ReR. (dissociation)
O Mtt+e 3M (recombination)
UY Mt+xoyY (chemical reaction)
LU M*+XDOM+xX* (charge transfer)
L) M+ > M™+(n-i1)e (emission of Auger electrons)
YO MOM+hv (fluorescence)
CL) M'> Rtt+R (dissociation into ions)
O M +x 3Y (chemical reaction)
WU M'+XOM+X* (transfer of excitation energy)

« Many of these secondary reactions are very fast and occur within |O”
to 107s.
 Interaction density

¢ The concentration of the reaction products in the

track is proportional to the energy lost by the
ionizing particles per unit distance travelled along
their path, which is called linear energy transfer
(LET).
¢ For example, in water the LET value of 1 MeVa
particles is 190 eV/nm and for 1 MeV electrons it
is 0.2 eV/nm.
¢ This means that the concentration of reaction
products in the track is higher by a factor of
about I0? for alpha particles.
 Alpha Radiation
¢ The limited range of a
radiation can be seen in the
figure to the right
¢ The range depends on the
energy of the a particles
and it has amount of
several centimetres in air.
¢ Rarely an a particle collides
with a nucleus and is
strongly deflected, or it is
captured by a nucleus and
induces a nuclear reaction.
 a-lonization
The specific ionization of a
particles in air is shown in the uuu ,
figure. The number of ion pairs
produced per millimetre of air 6000 |__| -____
increases strongly with the
distance and falls off rather | 5000 . _
sharply near the end of the

[ion pairs per mm air

range of the a particles.

apecitic ionization

co
Co
~
o
The increase is due to the
decreasing velocity of the a

|
ad
oo

=]
l
co
particles.
As the energy decreases by

=)
-
i
o
2

|
about 35 eV per ion pair
extrapolated
generated, an a particle with 1000 |. ignization range 3.870om | |
an initial energy of 3.5 MeV | ~ |
produces about |0° ion pairs. 0G — 5 3 ,
At the end of its path it forms Distance [cm] ——»
a neutral He atom.
 Range of a-particles
The relative number of a
particles is plotted in the | \ | D
figure asa function of | | fs

the distance from the

0,8 | Ht a —

} j 1
I | \ Gifferentiated
source. H\ | (curve |
= on} — _ A A
The variation of the z= \
5s po. iL po A)
range is caused by the = j extrapdated \ | j
statistical variation of the = 047————_ range 3,897 cm —Fy +— — +

number of collisions.
= | ~\ ! | \ |

=a Thean yt t 1
. t

Exact values of the range © 92| —__rangeseezom AI Ne |

in air are obtained by | LAN NA
DUP OR PSA
2 PS
extrapolating or by 0 et

35 3.6 3.7 3,8 3,5 40

differentiating the curve Distance in air [cm] ——*
 Simple device for range
measurements
A simple device for the
determination of the range of
a particles in air is shown in
Fig. 6.5: ZnS emits light as
long as it is being hit bya ZnS screen

/
particles.
sample
At a certain distance between
the ZnS screen and the a
source the emission of light
decreases very fast, indicating

!
the range of the a particles in
air.
4 5 6 7 8 9
By application of this method,
curves of the kind shown in
[em]
the previous figure can be eg a la al ala a a al al al al

obtained.
 a-Ranges in various media
¢ The range of a particles in various substances is listed in the
following table. Multiplication of the range in cm by the density of
the substance (g/cm?) gives the range in g/cm7?.
* Table shows that the ranges in mg/cm? are similar for very different
substances; they increase markedly at higher atomic numbers.

Substance Extrapolated range Density Range in

in [cm] [g/cm] [mg/eom?|

Air 6.95 0.001226 8.5

Mica 0.0036 2.8 10.1
Lithium 0.01291 0.534 6.9
Aluminium 0.00406 2.702 11.0
Zinc 0.00228 7.14 16.3
Tron 0.00187 7.86 14.7
Capper 0.00183 $.92 16.3
Silver 0.00192 10.50 20.2
Gold 0.00140 19.32 27.0
Lead 0.00241 11.34 27.3
 Beta Radiation
¢ The interaction of B radiation with matter is much weaker
than that of a radiation.

¢ A3 MeV a particle has a range of about 1.7 cm in air and

produces several thousand ion pairs per millimeter, while a B
particle of the same energy covers a distance of about 10m
in air and produces only about 4 ion pairs per millimeter.

¢ On the other hand, the electrons are markedly deflected by

collisions with other electrons, in contrast to the heavy a
particles, and they therefore exhibit a zigzag course.
 R... max VSE max

Maximum range in Al [mg/crn?] ——-»

1000

Absorption curves of B and Bt

radiation are very similar.

By use of the calibration curve

in the Figure to the right the
maximum energy E,,., of B
particles can be determined

oO
So
from their maximum range
R max

10
0,1 1 10
Maximum energy of the f particles [MeV] —— 12
 Conversion electrons absorption
5000°
| |
Conversion electrons are
monoenergetic and exhibit a
nearly linear absorption 4000 \
curve, if their energy is >0.2
MeV.

§ ——-»
e At energies <0.2 MeV the 3000

Relative intensity
absorption curve deviates

¢
more or less from linearity.
To obtain the effective range
2000 + \
of conversion electrons, the
linear part of the absorption
curve is extrapolated to the
1000 5 \
intensity | = 0. extrapolated range*

-,
(225 mg/cm?) >. \
‘\.

0 | = ae

0 100 200 300

Thickness of the aluminium absorber [mg/cm*] ——»
 B interaction with matter
¢ Interaction of Beta radiation with target atoms has a
three different consequences:

A. Interaction with electrons leads to excitation of the electron

shell and ionization

B. Interaction with atomic nuclei causing a Bremsstrahlung

radiation emission

C. Backscattering of B particles
 A. Interaction with target electrons
¢ The important parameter for this interaction is the electron density in the
absorber, i.e. the number of electrons per mass unit given by Z/A .

¢ This is shown in Table 6.2 for three different energies E,.., of particles and
different absorbers.

Maximum energy Substance Z/A Maximum range

[MeV] [mg/cem?]

0.156 (4C) Water 8/18 = 0.44 34

Aluminium 13/27 = 0.48 28
1.71 (2P) Water 0.44 810
Aluminium 0.48 800
1.0 Aluminium 0.48 400
Gold 79/197 = 0.40 500
B. Interaction with atomic nuclei
¢ Inthe electric field of a nucleus high-energy electrons emit X-rays of continuous
energy distribution (bremsstrahlung).

¢ The ratio of energy loss by emission of bremsstrahlung and energy loss by

ionization is approximately given by

E( Bremsstr.) Emax: Z
(6.16)
E{Ionis.) — 800

¢ where E_., is the maximum energy of the B radiation in MeV and Z the atomic
number of the absorber.
C. Backscattering

Lat
1

hy
NM
4
SR

~~
A
Geiger—Muller counter

SS
¢ Backscattering can be

SS
SSS
measured by the method é

~~ s
shown in the figure on the 4
right

¢ It also depends on the energy S SSS

E ax Of the B radiation and the radioactive
atomic numberZ of the sambre
absorber.
backscattering
/ material
ESS SEENON};
 B* (positron) Radiation

¢ positrons (B*) are the antiparticles of electrons.

¢ After having given off their energy by the interactions (A) to

(C), they react with electrons by annihilation and emission
of predominantly two y-ray photons with an energy of 0.51
MeV each in opposite directions (conservation of
momentum).

¢ The energy of 2 x 0.51 =1.02 MeV is equivalent to the rest

mass energy the electron and the positron.
 Gamma Radiation
Gamma rays and X rays have similar properties and are
distinguished by their origins:

X rays are emitted from the electron shell of atoms, if electrons

are passing from states of higher energy to those of lower energy
(characteristic X rays) or if electrons are slowed down in the field
of nuclei (bremsstrahlung)

y rays are emitted from nuclei, if these pass from excited states to
states of lower energy.

In contrast to the y rays emitted from nuclei, the Bremsstrahlung

shows a continuous energy distribution.
 Attenuation equation
The absorption ofy rays and X rays is, in principle, different from that of a or B rays. While the latter
lose their energy by a succession of collisions, y-ray photons give off their energy mostly in one process.

For the absorption ofy rays an exponential law is valid:

f= Ipe~¥4 (6.18)

(uu. = absorption coefficient and d = thickness of the absorber).

The relation between the energy of y radiation and its absorption is characterized by the half-thickness
dj, i.e. the thickness of the absorber by which the intensity of the y radiation is reduced to half of it.
Introducing | = |,/2 in eq. (6.18) gives:

dip ==UIn2
(6.19)
Instead of the linear absorption coefficient, the mass absorption coefficient u/p (cm2/g) is often used:

T = Ipe7*4/? (6.20)
In this equation, d is in units of g/cm?
 Absorption
¢ The absorption of the y radiation of
137Cs as a function of d in g/cm? is
plotted in Fig. 6.12.

——-»
Relative intensity.
¢ By 7d,,, the initial intensity is
reduced to about 1%, and by 10d,/,
to about 0.1%,.

3S mo
¢ For the purpose of radiation
protection, it is useful to know that
the intensity of 1 MeV y radiation is
reduced to about 1% by 5 cm of
lead or 25 cm concrete.
10
0 ie 20 30 40 50
Thickness of the lead absorber [g/om?] ——»
 Absorption in Various Materials
e Inthe first place, the absorption of y radiation depends on the
density of the absorber, similarly to the absorption of a or B
radiation.
¢ In Table 6.3 the mass absorption coefficients for various absorbers
and various energies of y radiation are listed.

E,{[MeV] Nitrogen Water Carbon Sodium Aluminium _ Iron Copper Lead

0.1022 0.1498 0.165 0.1487 0.1532 0.1643 0.3589 0.4427 5.30

0.2554 0.1128 0.1255 0.1127 0.1086 0.1099 G.1186 0.1226 0.558
0.5108 0.0862 0.096 0.0862 0.0827 0.0833 0.0824 0.0814 0.149
1.022 0.0629 0.0697 0.0629 0.0603 0.0607 0.0590 0.0580 0.0682
2.043 0.0439 0.0488 0.0438 0.0422 0.0427 0.0420 0.0414 0.0442
5.108 0.0270 0.0298 0.0266 0.0271 0.0286 0.0312 0.0315 0.0434
10.22 0.0216 — - 0.0226 — ~ 0.0537

22
 Effect of y energy

The half-thickness ofy radiation in lead

_
can be used as a measure of the energy

Haif-thickness in lead [g/cm?]

(Fig. 6.13). The fact that at higher
energies two values are found for the
same half thickness

is due to the overlap of three different

main absorption mechanisms:
Photoelectric
Compton scattering
Pair production

“O4 1 40
Energy [MeV] --— =
23
The total absorption coefficient pi is given approximately by the sum of the
partial absorption coefficients due to the photoeffect (p1,,), the Compton
effect (U,) and pair formation (p,):

= Upp tHe tH, seesseesees (6.24)

wn
_—
Absorption coefficient [cm='] ——»

1,0

0,5

01 1 10 10 24
Eneray of » radiation [MeV] ———
 Effect of Zonwu
¢ In this figure; the total absorption coefficient of y radiation in various materials is
plotted as a function of the energy of the y radiation.
¢ The strong influence of the atomic number is evident from this figure.

uw
—
——-»
Absorption coefficient in cm-'!
Oo
—
ion
Oo

0,1 1 10 10
Energy of » radiation [MeV] ———»
25
 Neutrons
Neutrons are emitted by spontaneously fissioning heavy nuclei.
High fluxes of neutrons are available in nuclear reactors.

Neutrons are not stable in the free state, but undergo B decay:

1. B (0.782) , bon
on .6 Min
iP Tok Tov

The interaction of neutrons with matter is practically confined to

the nuclei and comprises elastic and inelastic scattering and nuclear
reactions.

In elastic collisions the total kinetic energy remains constant,

whereas in inelastic collisions part of the kinetic energy is given off
as excitation energy.
 Neutron Absorption
In contrast to protons, deuterons, alpha particles and other particles carrying
positive charges, neutrons do not experience Coulomb repulsion by nuclei.

Low-energy (thermal and slow) neutrons are very effectively absorbed by a great
number of nuclei, giving rise to nuclear reactions.

Fast neutrons lose their energy mainly in elastic and inelastic collisions.

The energy given off in one elastic collision depends on the angle of collision and is at
maximum 4AE,/(A + 1)? in the case of central collisions, where E, is the energy of the
neutron before the collision and A is the mass number of the target nucleus.

The lighter the nucleus, the higher the energy loss of the neutron.
End of Chapter 6
Radiochemistry
NE 560

Chapter 2
Dr. Ghadeer Malkawi

Fall 2018
 What is Radiochemistry
¢ Defined as the chemical study of radioactive elements, the types of
radioactive decay, radiation-matter interactions and the detection
techniques, and also the study to use of this radiation and radioactive
materials in some applications in medicine, industry, geology... etc.
based on nuclear science and the analytical chemistry.

¢ Historically, radiochemistry appears to have been the first in line, When

Madame Curie was carrying through her laborious chemical procedures
to isolate and identify the radioactive elements and to establish their
transformations, she was doing “radiochemistry”.
 Comparison of chemical and nuclear reaction

Chemical Reactions Nuclear Reactions

One substance is converted into another, Atoms of one element typically are
but atoms never change identity. converted into atoms of another element.

Electrons in orbitals are involved as bonds Protons, neutrons, and other nuclear
break and form; nuclear particles do not particles are involved; electrons in
take part. orbitals take part much less often.

Reactions are accompanied by relatively Reactions are accompanied by relatively

small charges in energy and no large charges in energy and measurable
measurable changes in mass. changes in mass.

Reaction rates are influenced by Reaction rates depend on number of

temperature, concentration, catalyst, and nuclei, but are not affected by
the compound in which an element occurs. temperature, catalysts, or, except on rare
occasions, the compound in which an
element occurs.
 The Nucleus
The atomic nucleus consists of protons and neutrons
Protons and neutrons are generally called nucleons
A nucleus is characterized by:
¢ A: Mass Number = number of nucleons A=Z+N
¢ Z: Charge Number = number of protons Determines the Element
¢ N: Neutron Number Determines the Isotope

Chemical symbol
for the element.
Mass number = =
4- f+ A

Atomic number = C
e.g. EC has an atomic number of6 and a mass number of 12.
number of protons

N = neutron number Particle Symbol Charge Mass (a.m.u.)

proton p +1 1.007276
neutron n 0 1.008665
electron e -1 0.000549
1 a.m.u. = 1.66 x 10-2’ kg.
 The Nuclear Radius
Nucleus is very small tim V = 4ar° (fm’)
r (im

¢ fm: femtometer ~ 250

* nucleus ~ 1—10fm 44 ris proportional to A'. - 200
¢ atom ~ 1 A= 1 x10°!8 m= 100,000 fm 34 - 150
25 + 100

All experiments suggest that R =_ +r7,AAl al | ; 59

ry = constant 1.1-1.6 fm; A-mass number Pye ee
0 T T T T T 0

0 10 20 30
Mass number A

Copyright © 2004 Pearson Education, Inc., publishing as Addison Wesley

 Isotopes
Isotopes: same Z “Ca, 47Ca, “4Ca
often, ‘isotope’ used instead of ‘nuclide’ XY | Z isodiaphors
isotopes have same Z, so same number of electrons => same chemistry
use radioactive isotope in place of stable one — can monitor AR Atle | AW p
. Zt+1°~“N-1)) Z41°“N | Z4l°“ N41
decay for tracer studies
A-l A A+l :
Isotones: same N “Ca, “Ti,7 4Cr Zz 4 Yn) oY 741 --—» isotopes

Isobars: . same A 42 “Ca, “Ti, 42

427; 44Cr OX
A-2 val A-l1X y |X
A

:
Isodiaphors: same neutron excess 420q “Ca, 467;“Ti, 50 °°Cr LS “Ne, isobars
isotones
The atomic mass of an element is the average of the atomic masses and
abundances of each of the naturally-occurring isotopes.

Vv
e.g. The atomic mass of carbon is 12.01.

That is (12.0000x98.89 + 13.00335x1.11)/100

12 1
6C oC
 P N Nuclide Nuclide mass Natural abundance Atomic mass Remarks
[ul [] [ul

] 0 'W 1,007825 99.985 Stable

] 1 7H (D) 2.014102 0.0155 } 1.00797 Stable
¢ Proton- 1 2 3H (T) 3.016049 Unstable
2 1 3He 3.016030 <0.0001 Stable
Neutron model 2 2 *He 4.002603 100.00 } 4.00260 Stable
of the nuclides 2 3 >He Unstable
2 4 6He 6.018891 Unstable
¢ P= number of 3 2 shi Unstable
protons; 3 3 °Li 6.015123 7.42 } 6.940 Stable
3 4 PLi 7.016004 92.58 , Stable
¢ N=number of 3 5 SLi 8.022487 Unstable
neutrons. 3 6 *Li 9.026790 Unstable
4 3 "Be 7.916930 Unstable
4 4 ®Be 8.005305 Unstable
4 5 *Be 9.012183 100.00 9.01218 Stable
4 6 Be 10.013535 Unstable
4 7 Be 11.021660 Unstable
5 3 3B 8.024608 Unstable
5 4 °B Unstable
5 5 0B 10.012938 19.6 } 10.811 Stable
5 6 0} 11.009305 80.4 , Stable
5 7 RB 12.014353 Unstable
5 8 BR 13.017780 Unstable
6 4 10C 10.016858 Unstable
6 5 Ne 11.011433 Unstable
6 6 12¢ 12.000000 98.892 \ 12.0112 Stable
6 7 BC 13.003354 1.108 , Stable
6 8 4c 14.003242 Unstable
6 9 5c 15.010599 Unstable
6 10 6c 16.014700 Unstable
 Radioactive Isotopes
¢ Isotopes of certain unstable elements that spontaneously emit particles and energy
from the nucleus.

¢ Henri Becquerel 1896 accidentally observed radioactivity of uranium salts that were
fogging photographic film. His associates were Marie and Pierre Curie.

¢ For identification, the symbol (or the atomic number) and the mass number are used.

¢ The atomic number can be omitted ('4C), because it is known by the symbol. 4C can
also be written as C-14.

¢ For complete information, the kind and the energy of transmutation and the half-life
may also be indicated: B- (0.156 MeV)
l4c l4ny
 Radioactive Substances In Nature
¢ Some Radioactive substances are found in the atmosphere, but the major
part is present in the lithosphere. The most important ones are the ores of
uranium and thorium, and potassium salts, including the radioactive decay
products of uranium and thorium.

¢ Uranium and thorium are common elements in nature. Their

concentrations in granite are about 4 and 13mg/kg, respectively, and the
concentration of uranium in seawater is about 3 pg/L.

¢ The most important uranium mineral is pitchblende ( U,0,). While the

most important thorium mineral is monazite, which contains between
about 0.1 and 15% Th.

¢ The measurement of natural radioactivity is an important tool for dating,

e.g. for the determination of the age of minerals
 Uranium and thorium minerals

Mineral Composition Conc of U Conc of Th Deposits

[>] [%]
Pitchblende U,08 60-90 Bohemia, Congo,
Colorado (USA)
Becquerelite 2U0;-3H2,O 74 Bavaria, Congo
Uraninite 65-75 0.5—10 Japan, USA, Canada
Broeggerite UO, - U0; 48—75 6-12 Norway
Cleveite 48—66 3.5-4.5 Norway, Japan, Texas
Carnotite K(UO2)(VO«4) -nH2O 45 USA, Congo, Russia,
Australia
Casolite PbO - UO; - SiO, -H,O 40 Congo
Liebigite Carbonates of UandCa 30 Austria, Russia
Thorianite (Th, UjO, 4-28 60-90 Ceylon, Madagascar
Thorite ThSiO, -H2,O 1-19 40-70 Norway, USA
Monazite Phosphates of Th and 0.1-15 Brazil, India, Russia,
Rare Earths Norway, Madagascar
 Nuclides, Nucleons and Isotopes
It is evident that the Periodic Table of the elements does not have room to
include information about all the isotopes of the elements. For example tin has
10 stable and 18 unstable isotopes.

For that purpose the chart of the nuclides has been designed, which is based on
the proton-neutron model of atomic nuclei.

Stable nuclei result from the combination of about equal numbers of protons and
neutrons.

The transfer of this information into a diagram in which the number of neutrons
is plotted as ordinate and the number of protons as abscissa gives the chart of
the nuclides, the first part of which is shown (Next slide)
Chart of the nuclides for low Z elements
"7 oe | or] Mor PPeup cr Pu Ber es |i | cr | Per

—=Z7—»
16 EX aa Ms 326 Be He By ey ae 38 8 40,

15 28 sed #7, 5 34, a #e a aan aan "e | a5

1é Be eo 7 PF ae oe Noi Re, Be Me, Be at 24

Number of protons, P
13 7a, Far Pan [Bafa] acl aula Pat Pac [aL 23
12 20 Mag 22 Mg 24 25 Sg 27 q ae Mg Mg "Mg

" 8a "Na |2Nall hia | “No [No | “Nal “”Nal Ne | “Na Na Na | ha Ne

10 “We | "Ne| “Ne|“Nel Ne] “Nel Nel “Ne| Ne} “Ne
9 me [ee [ee [me he lm 1, 18 19 20 21 22
3 % |¥o "o [of 5 1% 1% 10 | [2 [#01 17
7 Ny Sy My By ey ™N ye, *y 20) 7 16

6 ve % Ne %s Be Me Be ®e "c Bo * 15

5 ap 95 "5 ", i) 38 4p *a "a 14

o "Be "ae [eel “Bel "Be|"Be| | “Be 13

3 ui Pupu pfu} |" " stable nuclides
2 “Hef ‘He | He |°He]” He) He "
+ fap . , "0 unstable nuclides
o;1{,2 3 4 5 6 7 8

Number of neutrons, V= A-2—>

 Chart of the Nuclides
¢ The following groups of nuclides can
be distinguished: lsotones
Isobars 4 Isodiaspheres

——
Lilsotopes: Z=P equal
Lilsotones: N=A-Z equal

Number of protons, P
— —r lsotopes
Llsobars: A=N+Z equal
Llsodiaspheres: A-2Z= N-Z equal

¢ The positions of these groups of

nuclides in the chart of the nuclides is
shown in this Figure
Number of neutrons, N= A—- 2 ——1»
 Chart of the Nuclides
¢ By comparison of the number of
protons P and the number of - " we
neutrons N in stable nuclei, itis =z =o
found that for light elements 60
(small Z) N=P. With increasing
atomic number Z, however, an Lat
increasing excess of neutrons is 40
necessary in order to give stable ee
nuclei. Le
20

eal 0 20 40 60 80 100 120

e A-2Z is a measure of the neutron excess. Naa Z——

¢ Thus, if in the chart of the nuclides the stable nuclides are

connected by a mean line, this line starts from the origin with
a Slope of | and is bent smoothly towards the abscissa.
 Chart of the Nuclides
* plot of nuclei as a function of Zand N glk.
¢ “Not just one box per element”

proton number

Mi stable
pec decay
GF decay
C] a decay
B pemission
0 spontaneous fission
[] predicted
#2 magle number
Radioactive Decay
¢ Unstable nuclei decay through a range of mechanisms involving the
release of particles with high kinetic energy or of gamma radiation.

¢ Statistical process
¢ Spontaneous emission of particle or electromagnetic radiation from the
atom
¢ Unaffected by temperature, pressure, physical state, etc.
¢ Exoergic process
¢ Conserves total energy, linear and angular momentum, charge, mass
number, etc.
Thorium decay series (thorium family): A = 4n

Nuclide Half-life Decay Maximum energy of

mode the radiation [MeV]

a 1405-10" y a 4.01
“8 Ra (MsTh)) 5.75 y a 0.04
228 Ac (MsTh2) 6.13h i 2.11
“8Th (RdTh) LOL y oF 5.42
24 Ra (Thx) 3.66d “t 5.69
Rn (Tn) 55.63 of 6.29
“16 Po (ThA) 0.158 a 6.78
“I? bb (ThB) 10.64 h fin 0.57
712Bi (ThC) 60.6 min a, 4: 6.09; 6: 2.25
"2 By (THO) 3.0-107's at 8.79
| The) 3.05 min i 1.80
48 Pb (ThD) Stable
nem nemeetasnneeenasnee
Uranium-radium decay series (uranium family): A
=4n+2
Nuclide Half-life Decay Maximum energy of
mode the radiation [Mev]

=8U UT) 4.47-10? y at 4,20

— 4TH UX) 24.1d & 0.199
24m Pal UX) 1.17 min gf 2,28
Le 24pa(UZ) | 6.7h i 1.24
SUI) + 245-10 y a 4.78
20TH To) 7.54-104 y ot 4.69
“OR a 1600 y a 4,78
22R yn 382d ce 5.49
— !®Po{RaA) 3.11 min at, Bl a: 6.00
+ ‘4ph(RaB) - 26.8 min gf 1.02
i, 1B At 1.68 a, fp #:6.745
i Rn 0.0355 ee 7.13
i+ ‘FRY RaC) + 19.9 min eS ft @: 5.51, 6 :3.27
+ *4PocRac'y - 1.64-10-* s ot 7.69
+ MTV Rac") _] 1.3 min i 2.34
29ph(RaD) + 22.3y cel”, 8 4:23.72 6 : 0.061
+ Hy 8.15 min B 1.31
— "Ri(RaF) 4 s0id ol) Bp 2: 4.6% fF : 1.16
4 WT) RaE") 4.2 min B- 1.53
LL 710Po(RaF) _] 138.4d ct 5.31
*6Pb( RaG) Stable
Actinium decay series (actinium family): A = 4n + 3
Nuclide Half-life Decay Maximum energy of
mode the radiation [MeV]

51 (AcL) 7.04. 108 y a 4.60

SITHCUY) 25.5h i 0.31
Apa 3.28- 104y x 5.06
— #227 Ac 21.77 y¥ a) B #: 4.95; fF : 0.046
: 22 Th(RdAc} 18.72d tf 6.04
25Fr(AcK) 21.8 min a B #: 5.34; : 1.15
“SRa(AcX) d 11.434 of 5.87
—- 21 At J 545 a, p #: 6.28
+ Ratan) 7 3.96 5 oe 6.82
+ Bi = 7.4mio ie 2.2
—- SPo(AcA) « 1.78-10°73 a, 6 ™ 4: 7.39
> Ph AcB) — 36.1 min A 1.38
+ 715 At — «10's eo 8.02
— TN BifAcCy — 2.14 min a, o a: 6.62;8 > 0.29
+» “Im Pig — 25.55 of 8.87
H+ Pal AcC’) — 0.5165 ot 745
Ke OT ACC") — 4.77 min Bb 1.44
“7 Ph(AcD)
Neptunium decay series (neptunium family): A = 4n + 1
—— —— =

Nuclide Half-life Decay Maximum energy of

mode the radiation [MeV]
27Np 2.14- 10% y A 47
“Py 27.0d ‘is 0.57
231] 1.59. 10° y oe 482
22Th 734-10y 2 5.05
“Ra 14.8d B 0.32
a Ac 10.0d a 5.83
221 F Pr 4.9 min 2 6,34
217 At 0.0328 a 7.07
2S Bi 45.6min al”! A #: 5.87; Ff : 1.42
L.23p, 4.2-107%s a 8.38
L, eT] 22min if |.83
Ph 3.25h 0.64
ae Ri Stable

¢ Members of this family have been produced artificially by nuclear

reactions.
¢ Parent/daughter, branching
 Law and Energy of Radioactive Decay

Where,
oe
N : the number of atoms of a certain radionuclide
-dN/dt : the disintegration rate
A. the disintegration or decay constant (dimension s‘!), It is a measure of the probability of
radioactive decay.

The law of ractfoactive decay describes the kinetics of the reaction

A B+x+AkE
where A denotes the radioactive mother nuclide, B is the daughter nuclide, x the particle
emitted and AE the energy set free by the decay process, which is also called the daughter
nuclide, Q-value.
 Law and Energy of Radioactive Decay

¢ Radioactive decay is only possible if AE > 0.

¢ AE can be determined by comparison of the masses. According to the
relation found by Einstein,

AE = AM c? =(Ma — (Mp — Mx)|2

¢ By calculation of AE it can be decided whether a decay process is

possible or not.
 Law and Energy of Radioactive Decay
N= Neen”!

¢ where Nop is the number of radioactive atoms at the time t = 0.

* the half-life t ,,. is frequently used. This is the time after which half the
radioactive atoms have decayed: N = N,/2.

In? 0.693 pine

h2= == 7 N = No( )
A A 2
 Law and Energy of Radioactive Decay
¢ The activity A of a radionuclide is given by its disintegration rate:
cL In?
A= ——-=JN=——N
di thy
A=Ae“%t

¢ The dimension is s! , and the unit is called becquerel (Bq)

1Bq=1s'!

¢ An older unit is the curie (C1)

1 Ci = 3.700. 10°!° s:'!= 37 GBa.
 Law and Energy of Radioactive Decay
* The mass m of the radioactive atoms can be calculated from their number N and their activity A:

m NM AM ACM
Nay Naya Nayln2 1?

* In laboratory experiments with radionuclides, knowledge of the mass of the radioactive substances
is very important. For example, the mass of 1 MBq of *?P (t,,. = 14.3d ) is only about 10°!° g, and
that of 1 MBq of ?’Tc (t,,. = 6.0 h) is only about 5 x10 g.

* If there is no carrier present in the form of a large excess of inactive atoms of the same element in
the same chemical state, these small amounts of radionuclides may easily be lost, for instance by
adsorption on the walls.
 Law and Energy of Radioactive Decay
¢ The ratio of the activity to the total mass m of the element (the sum of radioactive
and stable isotopes) 1s called the specific activity

A
_——_— |
A, m [Ba / 2)

¢ Sometimes high or well-defined specific activities are required, for instance in the
case of the application of radionuclides or labelled compounds in medicine, or as
tracers in other fields of research.
 Radioactive Equilibria
¢ Decay Series
nuclide 1 — nuclide 2 — nuclide 3
¢ At any instant, the rate of production of nuclide 2 is given by the decay rate
of nuclide | diminished by the decay rate of nuclide 2:

dN dN;
— = — — — Ad Ng = AYN, — AN
dt do ;
cLN
—=44, ly — Ay Nye ~at — ()
dr
N;=-
hi yo
|
etl!_ at 4at
| 1 N° Ant
25 — A) i| eC ) 2&

* If nuclides | and 2 are separated quantitatively at t = 0,

N; = NI (e 4 — ena") Nz = Al
Ni[l— eo bain
Aa - ~ At As — Ay | I
 Radioactive Equilibria
— Api). yaaa)
= l2)/tpll(iy
~ 1 fp [ - (5) |

pot 1a t
ty 2l2) aay [3 (1) fiya(2)

* After a sufficiently long time

Al ro thy2(2)/tral I)
hea) 1 92)/npll)
Ny == ——— Vj,

* The time necessary to attain radioactive equilibrium depends on the half-life of the daughter
nuclide as well as on the ratio of the half-lives.
 Radioactive Equilibria
¢ In the radioactive equilibrium, the ratio N2/N1, the ratio of the
masses and the ratio of the activities are constant.

¢ This is not an equilibrium in the sense used in thermodynamics and

chemical kinetics, because it is not reversible
 Radioactive Equilibria
¢ Four cases can be distinguished:

(a) The half-life of the mother nuclide is much longer than that of the daughter nuclide, t
tj. (1) >> t,,(2).

(b) The half-life of the mother nuclide is longer than that of the daughter nuclide, but the
decay of the mother nuclide cannot be neglected, t ,, (1) > t,(2)

i) tye of the mother nuclide is shorter than that of the daughter nuclide: t ,,. (1)
Sti

(d) The half-lives of the mother nuclide and the daughter nuclide are similar:
tin (1) =t,(2).
 Radioactive Equilibria
wn byel Mhyel2) =10
t ! —tyeftitiyel2) =2
a " ~~tyol TMA yel2) =1.5
|
= O8
=
i,

= O6
aay
Po

2 3 4 5 6 7 8 8 W
. Oo 1 tity ale] —
~
Secular Radioactive Equilibrium
tio(1)>>t,,(2).

A
Na = 5 Mille No _ Ai _ Hp(2)
Noa. ffl)
M=GM(-e*) AA

Decay
i
0 I ? 3 & 5 6 7 6
hele) ———
Secular Radioactive Equilibrium

Total activity A = A, + A;

wt ea
As growing ln (1)

Activity, 4 ——te

10
As separated from (1)

1
Q ] Z 3 & 5 6 7 a $ 0
ttyl? -
 Transient Radioactive Equilibrium
tip C1 )/ typ(2)=5

Total activity 4 = A, + Ae
10°

es a,
Activity, A

ee

As saparated from (7)

S

As growing in (7)
I

tya(2) ——
 Transient Radioactive Equilibrium
In transient radioactive equilibrium the daughter activity is always higher:

No fale)
Ny tyye{l) = tya(2)

Ar AM |) 4 _ nl?)
Ar Ag N> Ap tyyall)

M, A>
my fyyo(l) ~ fy2(2)]
 Half-life of Mother Nuclide Shorter than Half-life of
Daughter Nuclide

¢ In this case the mother nuclide decays faster than the daughter
nuclide, and the ratio between the two changes continuously, until
the mother nuclide has disappeared and only the daughter nuclide is
left
 Half-life of Mother Nuclide Shorter than Half-life
of Daughter Nuclide
Ratio=0.1

Az separated Total activity A = A, + Ap

2h frorn {1}
0

-_
Activity, A

A> growing in (1)

0

o 1 2 3 & 5&5 & FT 8 8

ftsya(1) ——
 Similar Half-lives

¢ As the difference between the half-lives of mother nuclide and

daughter nuclide becomes smaller and smaller, the attainment of
radioactive equilibrium is more and more delayed
 Branching Decay
A

-_
¢ e.g. “°K, which is responsible for the natural radioactivity of potassium, decays
into *°Ca with a probability of 89.3% by emission of beta particles and into *°Ar
with a probability of 10.7% by electron capture.
¢ As these two probabilities are independent of each other, the
* decay constant of the radionuclide A is given by the sum of A, and A,

dN4
= AyNa +dcNa = AaNa
di
 Branching Decay
Integration of this equation gives

Na = Noe (or iel

The rates of production of the nuclides B and C are

dNp dNe a
——di Ap
= ApvA dn d ——=4
dy ,.N
AelW A

and the decay rates of these nuclides are

dNvas, dNe , ,
de An-VR and — Gp = 4eNe
 Branching Decay
The net rate of production of B is

di
a= = ApNa — ABN

dNp
= + ApNa — dpNie Vetae]t — ()

Integration of this equation with Vg = Oat t= 0 gives

Np _ Ab N'le (Agbag
le e “Ht
Ap — (Ab + Ac)
 Branching Decay
¢ Secular equilibrium (Ay + de & An)
Np ab Ne _ A
Na apy and Ny ac
In? In?
A 6 eCreYS = =
i
1/2 ) An Ant de
In? In?
ty o(A}, = i and t(A),=—
b Ae

Np _ ty2(B) Ne _ fj2(C)
= and
Na tyolAd, Na tyy(A),
 Branching Decay
* For longer lived daughters

Ne =
dy
———~—
,
Nalelot*e!!
— 4
eT dy+ Ae al 2
Ne Ag
=——— Na +i
(Apbacdtyp]
c dh ob de le

Np
_ 4»
No de
 Radiochemistry
NE 560

Radiation Detection/ 1
Dr. Ghadeer Malkawi

Fall 2018
 Activity and Counting Rate
¢ The activity (disintegration rate) A is a property of radioactive matter
and can be measured by various devices which give a certain
counting rate |’, which depends on the activity A:

r l+h=—9yA+ hy

Where,
n: the overall counting efficiency.
|: net counting rate caused by the radioactive sample to be measured.
|: background counting rate, It is due to the radiation emitted by the
surrounding material and cosmic radiation.
 Activity and Counting Rate
a
¢ In Fig. 7.1 the logarithm of the net counting eo SE I
rate | is plotted as a function of time t. -" T |

SSS
OP ype SS eg SS

Counting rate [|] ———~

¢ The curve obtained is called the decay curve
and is used for determination of half-lives. pea ot

he
pT {.—{| —{ [fy

¢ The counting rate | of a radioactive sample | fd NO |

which contains several radionuclides is given . i
by the sum of the counting rates of the Pp —_e
individual radionuclides: [ | fly) 4
0 Time
{| ——

P=f+bhroc= Al + Hy Az ree Figure 7.1. Counting rate as a function of time (determination of half-lives).
Activity and Counting Rate;

¢ If the number of radionuclides

present in the sample is low, the

Counting rate [| ———»

decay curve can be separated by
subtraction into the individual

a
decay curves of the
radionuclides, either graphically
or arithmetically, as shown in
Fig. 7.2. -

0 tye(t) tyjal2) rime! |

ime tf ——s
Figure 7.2. Counting rate of a mixture of two radionuclides.
Contamination by A Short- a -
lived Impurity

=
oo
—
¢ The analysis of decay curves

.
is of practical importance for

Counting rate [cpm] ——»

Os
the investigation of

ee
radionuclide purity. As
N\ |

——
examples, contamination of
a sample by a short-lived \
impurity is shown in Fig. 7.3 0? ; | \
1 T(t,)9 = 20,8h) NOt
2 = 804 d)

10 2 - | NO
o 0 20 30 40 50 60 70 4&0
Time [d] ———+

Figure 7.3. Short-lived impurity (1°71 in °!1).

Contamination by A Long-lived
Impurity
10

‘€oO
Z
DB
oO
pa 43
1
2" Pa
5 (luge LT mn)
o
©

D 5 10 5
Time [min} ——*

Figure 7.4. Long-lived impurity @*Th in 74" Pa).

 Activity and Counting Rate
¢ The overall counting efficiency n depends on:
The frequency H of the decay mode measured in relation to the activity.
The self-absorption S$ of the radiation in the radioactive sample.
The contribution B of backscattered radiation.
The geometrical arrangement G of the sample with respect to the counter.
The absorption W of the radiation in the air and in the window of the counter.
The internal counting efficiency n, of the counter.
The correction D for the dead time of the counter:

y= H-(1-—S)-(14+ 8)-G:(l- W)-9,-(l- dD) (7.3)

By self-absorption, absorption in the air and the window, and dead time of the
counter, n is reduced, whereas it increases by the influence of backscattering.
The overall counting efficiency n may vary between about 0.01 and 1, depending
on the kind of radiation and its energy and the type of counter used.
 Activity and Counting Rate
¢ Self-absorption S in the sample is high for a and low-energy 6
radiation, but negligible for y radiation.
ld ——>—

A
08 _—

| |
oy5 08 — |, a
€
3 |

Bu
9
< +}
3
oy |
|

02 bP

0 + |;
0 1G 20 30 40 50 60
Thickness of the CaCOs sample [mafem®]_ ——»

Figure 7.5. Self-absorption S of the 8 radiation of #°Ca in CaCO, as a function of the thickness of
the sample.

¢ Backscattering may contribute appreciably to the counting rate in the case of

6 radiation, if the sample is placed on materials of high atomic number.
 Activity and Counting Rate
¢ The influence of the geometrical arrangement G is given
by the solid angle 0/4n. |

¢ Absorption in the air and the window of the counter is | + — detector

very high for a and low-energy 6 radiation, like self-
absorption S in the samples, and thin windows are needed 4 7
for the measurement of these kinds of radiation. \ |

¢ The internal counting efficiency ni varies appreciably \ i

between about 0.01 and 1.0 with the kind of radiation and \ /
the type of counter. rf
47
1}
Val ;
* The dead time of the counters is due to the fact that they SWZ — radioactive sample
need some time for recovery with the result that during a
certain period, the dead time, registration of a following
event is not possible.
 anode anodes radioactive sample
‘ Jona thin foil

radioactive sample

2m counter 4a cqunter
Gas-filled Detectors
Ionizing radiation passing through a gas creates a trail of ion pairs (positive ions and free
electrons).
¢ If an electric field is applied, the ions and the electrons move in opposite directions.
¢ The motion of the charged particles gives rise to a current that can be measured in an external
circuit.
* Commonly the detector has the form of a cylinder, the outer wall serves as the cathode and a wire
along the axis of the cylinder acts as the anode.
* At typical distances of several cm, it takes a few ps for the electrons to reach the anode and a few
ms for the slower-moving positive ions to reach the cathode.
Gas-filled Detectors
* The total number of ion pairs arriving at the electrodes and hence the height of the pulse
observed in the circuit depend on the electric field strength or the voltage, respectively,
applied to the detector.

¢ At low voltages, the electrons recombine with the ions (region of partial recombination).

¢ With increasing voltage nearly all the electrons are collected at the cathode and a
saturation value is observed. This is the range of operation of ionization chambers.

* Because the specific ionization is appreciably higher in the case of @ particles than in the
case of 6 particles, an a particle produces a much higher pulse in a ionization chamber
 10
| {region of Geiger-Muller!
}—_1+—_1— counters le
= | | _
c i | I
GD | i ib j= :
£ 0 region of limited |]
oe proportionality J
wD i

Ss ft |
2 saturation —{- Proportional region— 1
2 ‘ fionization {proportional counters);
° + chambers) — rp
2l11
i T
3 1 —
1 T
| t
i
+
|
L 1 1
I 1| _—- | Ji !
o o i
ata particles |
B ti | | |) |
er
— oe I

yi i. ij.

pt
3
4

PTT eer |1 |
ft yo | a i |4

pa § particles —

14H a}e ,
i
! 1
};
0 200 400) 600 800 1000 T2000 1400 1600
Field strength [V/crn] ——m-

Figure 7.9. Pulse height as a function of the field strength.

 Gas-filled Detectors
¢ Further increase of the voltage in the device leads also to an
increase of the pulse height . The electrons are accelerated on
their way to the cathode and gain so much energy that they are
able to produce secondary free electrons by collisions with the gas
molecules (gas amplification).

,ee
Ww
e

-@ ®@
e ©.

¥
e.

“@

‘ee’
®
E-field

¢ Over a wide voltage range the output pulse increases with the
voltage applied. This is the range of operation of proportional
counters.
Gas-filled Detectors
¢ If the voltage applied in the device further increased, the number of
electrons collected at the cathode becomes independent of the number of
initial ion pairs produced by the incident radiation.

¢ This is the operation range of Geiger-Muller counters, a single ionization

produced in the gas by any kind of radiation leads to a discharge spreading
out over the whole counter by a sequence of secondary ionization
processes and giving a relatively high pulse of several volts that can be
measured directly without amplification.

¢ At still higher voltages, continuous discharge takes place without the

influence of radiation.
 Scintillation Detector

photocathode
scintillator

* In the transparent crystal or liquid the radiation is absorbed and photons are emitted. At the
photocathode of the photomultiplier tube the photons release electrons which are
multiplied by the dynodes of the multiplier to give pulses of several mV.
 Semiconductoe detector
¢ An energetic incident radiation collides with electrons of the
semiconductor and lifts them from the valence to the conduction
band. Electrons appear in normally empty bands and holes appear . y
in normally fully occupied bands “9 Eg

¢ This configuration does not last long, in times of the order of 10°
s, the interaction between electrons and holes makes the
electrons concentrate at the bottom of the conduction band and
the holes concentrate near the top of the valence band

* The average energy necessary for the creation of one electron-

hole pair is much larger than the energy gap E,. For silicon at room
temperature, E,= 1.106 eV, and the average energy for the
production of one electron-hole pair is 3.66 eV
Semiconductoe detector

¢ In the application of semiconductor detectors two influences have to

be considered,
- Temperature > thermal noise
- Impurities > (doping) charge carriers
 The p-n Junction
¢ Semiconductor detectors operate like ionization counters:
In ionization counters, the charges produced by the incident radiation
are collected with the help of an electric field from an external voltage
In semiconductor detectors, the electric field is established by a process
more complicated than in gas counters. It is a process that depends on
the properties of n- and p-type semiconductors (p-n junction)

¢ Radiation incident upon the junction produces electron-hole pairs as it

passes through it.
¢ Electrons and holes are swept away under the influence of the electric
field and, with proper electronics, the charge collected produces a pulse
that can be recorded ——

(-) | (+)
a
Za" 1
1
1
ea 1
.ae |
wo ne ane of rm —— Electrici field 4
oo t 1
‘
 662 key
30004
Counting rate

2000+

1000

Compton continuum —|

q ; eS s*Figuire 7.15. y-ray spectrum of '°’Cs

0 1 0620 HD 60g = 700 taken with a Gre (Li} detector (the » rays
Energy [kev] — are emitted by the metastable '?"" Ba).
 Choice of Detector Type
Table 7.2. Suitabality of detectors for the mensurement of various kinds of radiation,
— —<—<———=

Kind of radiation lonixation Proportional! Geoiper—hluller Scntillavon Second achor

chambers counters couniens. detectors detectors

@ radiation Favourable Flow counters Unfavourable Liquid scant. Si barrier detectors

very fevourable favourable favorable
High-energy ff radiation Unsuitable Suitable Favourable Organic cryst. Si barrier detectors
f>1 MeV] favourable auitable
Low-energy ff radiation Uneuitable Favourable Unfsvourable Liquid scant. very Sa barrier detectors
(20.5 MeV) favourable faverorable
High-energy 7 radiation Unsuitable Unsuitable Unfavourable Nal( Th, CslfTh) i-Ge, Ge(Li)
(hl MeV) crystals wery detectors very
favourable favourable
Low-energy } radiation Unsuitable Suitable K-ray counters Wal( TT), Cst(11) Sal La) detectors
(0.1 Mev and favourabbe crystals very Favourable
A-rays favourable
 O00
Viva Mev

6000f-—— ——.
Phatopeaks | 4 a9 May
5000}-———} ++ py + —~——

“TTLi\
Caunting rate [epm|

fA \
ee a ee
2000

cof Compton continuum

A LL aie NS .
ro F0 11 2 13 1a 15
Energy [MeV] ——=

Figure 7.16. y-ray spectra of “Co taken with a Nal (Tl) scintillation detector and a Ge (Li) semi-
conductor detector.
 Low Level Counting
¢ If samples of very low activity are to be measured, the contribution of the
background to the counting rate and hence the error of the measurement
are relatively high.

¢ The influence of the background can be reduced by intensification of the

detector shielding. Usually, detectors are shielded by housings of lead or of
lead outside and steel inside.

¢ Steel is used to absorb the radiation from radioactive impurities in lead.

¢ Low counting rates may be measured in underground locations to reduce
the contribution of high-energy cosmic radiation.
Neutron Detection and Measurement

¢ Neutron detection and measurement are based largely on the

production of secondary ionizing radiation by the neutrons.

¢ Thermal neutrons, are measured with high efficiency by means of the

charged particles emitted in neutron-induced reactions, such as (n,p)
or (n,a) reactions or nuclear fission.

¢ The charged particles (e.g. protons or a particles) can be measured in

gas-filled detectors, scintillation detectors or semiconductor detector
Neutron Detection and Measurement

¢ Thermal neutrons are most frequently detected by means of the

nuclear reactions !°B(n, a )’/Li or *He (n,P ) 3H. For this purpose,
ionization chambers are covered on the inner surface with a thin layer
of material containing *°B , or with proportional counters filled with
1OBF, or He.
Neutron Detection and Measurement

¢ Slow neutrons may be detected via the ®Li(n,a)?H or the 1°B(n, a )/Li
reactions. °Li or 1°B is incorporated in a ZnS scintillator or in liquid or
glass scintillators.

¢ Semiconductor detectors are used as neutron counters by deposition

of a suitable “converter” material on the surface of a semiconductor.
For instance, a compound containing °Li may be deposited by
evaporation
To be continued
 Radiochemistry
NE 560

Radiation Detection/ 2
Dr. Ghadeer Malkawi
Track Detectors

¢ Another detection technology in which the radiation can be visualized

by seeing a path of ionization that an energetic particle can leave
behind during its interaction with a certain medium.

LIPhotographic Emulsions and Autoradiography

LI Dielectric Track Detectors
LICloud Chambers
LIBubble Chambers
LISpark Chambers
Photographic Emulsions and Autoradiography
¢ The oldest track detectors are photographic plates. They led to the
detection of radioactivity by Becquerel in 1896.

¢ Photographic emulsions on plates or films indicate the position of

radionuclides (autoradiography).

¢ The main advantage of autoradiography is the possibility of exact

localization of radionuclides emitting a or B rays.

¢ Smooth surfaces are required for autoradiography. The samples can be

metals, polished surfaces of minerals or thin sections of tissues of
biological or medical origin.
* As an example, the autoradiograph of an iron surface is shown
in Fi 7.18, indicating the deposition, by corrosion, of extremely
small amounts of iron hydroxide labeled with >?Fe in a drop of
water.

Figure 7.18. Autoradiograph of a sheet of iron showing the very early stage of corrosion at the edge
ofa drop of water by labelling with *’ Fe.
 Autoradiography
¢ The local resolution of an autoradiograph depends on the thickness
of the layer containing the radionuclide, the distance between that
layer and the photographic emulsion, the thickness of the
photographic emulsion and the radiation emitted by the
radionuclide.
¢ The influence of the distance between the radioactive layer and the
photographic emulsion is illustrated in Fig. 7.19.
I region of
| olackening |
| |
region of
| |
{
; OO "|
- + ae
AES ys
-
ASSES
eo.
‘olackening!
_ photographic emulsion ,

air
” FT Ae

_ LA : Lage: UL, Cp 7
< ~~~ radioactive sampie- O LEE LE LE EL EE
Autoradiography
¢ Short-range radiation such as a or low-energy B radiation gives good
contrast.
° The influence of the energy of B radiation is shown in Fig. 7.20. At lower
energy of the B particles the autoradiograph is appreciably sharper.

a) b)

Figure 7,20, Autoradiograph of two f emitters of different energies: a} 3§ (Emax = 0.167 MeV),
b) 3?P (Emax = 1.71 MeV).
 Autoradiography

e After exposure and developing, sample and photographic

emulsion can be investigated by means of a microscope
(microautoradiography).

¢ The time of exposure depends on the activity and the energy

of the radionuclide, and on the sensitivity of the
photographic emulsion.
Dielectric track detector
¢ Heavy ionizing particles produce tracks of radiation damage in insulators.
The tracks have the shape of a cylindrical channel with dimensions of about
1 to 10 nm. Without further treatment, they can only be observed in an
electron microscope, but after etching (e.g. by HF) they are visible under a
normal microscope.

¢ Various etching procedures have been developed and tracks of heavy

particles have been studied in many materials, such as minerals, glasses,
inorganic crystals and plastics.

¢ Each material can be characterized by a certain value of linear energy

transfer (LET, given by dE/dx), below which tracks are not observed.
Dielectric track detector

¢ An application of track detectors is dosimetry of a particles and

neutrons. For neutron dosimetry the track detectors may be covered
with uranium foils in which the neutrons induce fission. Alternatively,
the detectors may be covered with a foil containing B or Li, and the a
particles produced by (n, a) reactions are recorded.

¢ Since tracks caused by radiation damage are very stable, they can be
investigated after very long periods of time. Many minerals contain a
record of damage by fission products or cosmic rays that has been
conserved over millions of years. This makes track detectors very
valuable for geochemistry and space science.
Cloud Chambers
In cloud chambers (Wilson chambers) the tracks of ionizing particles are
visible by condensation of droplets on the ions produced.

The gas in the chamber is saturated with the vapor of water, alcohol or
other volatile liquids.

By sudden expansion supersaturation is obtained and condensation occurs

along the ion tracks.

Dust or other condensation centers must be eliminated, to avoid

interferences.
https://www.youtube.com/watch ?v=ZiscokCGOhs
 Bubble Chambers
¢ The bubble chamber makes use of the fact that liquids can be heated
for short times above their boiling points without actually boiling.

¢ Charged particles passing through such a superheated liquid induce

the formation of vapor bubbles along their tracks.

¢ Because superheated liquids are not stable for long periods of time,
bubble chambers are operated intermittently by variation of the
pressure.

e At normal pressure the liquid is just below the boiling point, and by
reducing the pressure super-saturation is obtained.
httos://www.youtube.com/watch ?v=teDejUPjdIM
 Spark Chambers
¢ Spark chambers contain a system of parallel plates or wires that are
alternately at a positive high voltage and at earth potential. The
chamber is filled with a noble gas.

¢ An ionizing particle crossing the gap between two plates or wires

causes the production of a spark near its trajectory.

¢ The detection efficiency of spark chambers is very high and the

resolution is very good.

¢ Wire spark chambers with dimensions of many meters containing of

the order of |0° wires have been constructed.
https://www.youtube.com/watch ev=-8G|zUjYazs
 Radiochemistry
NE 560

Production of Radionuclides and

Labeled Compounds/ 1
 Production in Nuclear Reactors
Most radionuclides used in science and technology are produced in nuclear reactors (high
flux densities of neutrons @ = 10!° to 10!®cm* s"! and high cross sections of (n, y) reactions).

In general, research reactors are applied for production of radionuclides, because they are
mostly equipped with special installations for that purpose.

Power reactors may also be used for the production of greater amounts of long-lived
radionuclides, such as ©°Co as a radiation source.

Larger reactors offer more space for introducing a greater number of samples without
affecting the neutron flux too much.

High neutron flux densities are required for the production of high activities.
 Production in Nuclear Reactors
The samples used for irradiation must withstand the temperature
and the radiation in the reactor without decomposition.

In general, they are encapsulated in aluminum cans or in quartz

ampoules which are introduced in irradiation tubes or directly into
special positions within the reactor.

Some research reactors are equipped with a so-called thermal

column of about 1m x 1mx1mM, consisting of blocks of graphite and
installed near the reactor core.

Due to the moderator properties of graphite, only thermal neutrons

are present in such a column.
 Production in Nuclear Reactors

¢ Fast pneumatic transport systems are needed for the

investigation of short-lived radionuclides.
¢ They can be operated over distances of several meters and the
samples can be brought, within 0.1 to 1s, directly from the
place of irradiation to the counter.
 Production in Nuclear Reactors

¢ Asurvey of neutron-induced reactions used for the production of radionuclides:

Table 12.1. Neutron-induced reactions in nuclear reactors (survey).

Reaction Decay modes of the products Remarks

(ny) Predominantly §~; rarely 87 or ¢ Generally applicable; high yields with

thermal neutrons
{n, 2m) Predominantly #7; sometimes ff Strongly endoergic; high-energy neutrons
(> 10 MeV) required
in, p) Nearly always @ Mostly endoergic (exceptions:
4Ni(n, py4N, 2Chn, p) °S and some
others); frequently at small mass num-
bers (4 < 40)
(n, 2) Predominanily ff Mostly endoergic (exceptions °Lifn, «)°H
and 'B(n, «)’ Li}; predominantly at
small mass numbers
(n,f) Fission with thermal! neutrons: Nuclides with atomic numbers 4 > 90;
always P"; fission with high- fission of “4 U, °U and “Pu with
energy neutrons: also 6” or thermal neutrons
 Production in Nuclear Reactors

¢ Asan example, irradiation of 1 g NaCl at a thermal neutron flux density 9 =10'3cm-

*s-! may be considered:

3Na(n,y)"Na ( co 0.53; t/9 = 15.0h)

Clin, y)*Cl T= 0.43 b: ty)2 = 3.0: 10°y)
SCln,y)?S (a ().49 b; hi2> 87.5 d)
7clin,y)"Cl T= -0.43b; tf). = 37.2 min)
 Production in Nuclear Reactors
¢ The activities as well as the specific activities increase with the neutron flux
density and the irradiation time.

¢ Whether the specific activity is sufficient or not depends on the purpose for
which the radionuclides are used. For medical applications, high specific
activities are mostly required.

¢ With respect to high specific activity, (n, y) reactions followed by relatively

quick B- decay are favorable. This is illustrated by the production of !°!I by
neutron irradiation of Te (Tellurium).
 Production in Nuclear Reactors

¢ Some radionuclides can be produced by (n, p) and (n, a)

reactions with thermal neutrons, for example

3He(n,p)H = (¢ = 5327b; 4) = 12.323 y)

4N(n,p)"C — (¢ = 1.81; hy2 = 97309)
®Li(n,a)°H (o = 940b; ft). = 12.323 y)
“Ca(n,a)Ar (¢ =0.0025b; t)). = 35.0d)
 Production in Nuclear Reactors

¢ As the product nuclides are non-isotopic, their separation from the

target nuclides does not cause problems.

¢ Production of “4C is of great practical interest. The long half-life of

4C requires a long irradiation time (> 1 y) to obtain sufficient yield.
Therefore, the nitrogen compound used as target must be heat-
and radiation-resistant. Nitrides, such as AIN or Be,N,, are most
suitable.

¢ After irradiation, they are heated in a stream of oxygen; *4C escapes

as "CO, and is bound by Ba(OH), as Ba*4C0,.
 Production in Nuclear Reactors

Tritium is produced on a large scale by irradiation of Li or lithium

compounds in nuclear reactors. Due to the high cross section of
this reaction of T compared with that of *4C, the yield is relatively
high and the costs of tritium production are relatively low.

T is obtained as a gas containing about 90% T and can be oxidized

to tritiated water (T,O) for further use.

Tritium is used for application in nuclear weapons.

 Production in Nuclear Reactors

¢ Pulsed research reactors, such as reactors of the Triga type, are especially
designed for production and investigation of short-lived radionuclides.

e In these reactors the neutron flux is increased by taking out the control
rods. Due to the negative temperature coefficient of the zirconium hydride
moderator, the outburst of power causes a sudden decrease of the
moderator properties and shutting off of the reactor. After several minutes
the effects have vanished and a new pulse can be started.

¢ The table shows that pulsed reactors are useful for production and
investigation of radionuclides with half-lives < 10 s.
 Production in Nuclear Reactors

Table 12.2. Activities of radionuclides of various half-lives obtained in pulsed reactors of the Triga
type compared with those obtained at constant flux densities (activities in MBg/g for a,,, = | barn,
He= land M = 100)

Half-life Pulsed reactor Activities at constant neutron flux (saturation activity)

(Pao.
= 10! emg; ——— —
10 ms) @=1em es! @= 10" em @s! S= 104 cm*s7!

O01 s 3.0. 10°

O.1s 4.0. 10°
ls 42.10 6.0- 1 6.0- 10° 6.0. LOF
ls 4.2-107
| min 70-108
ee es
 Production in Nuclear Reactors
A great number of radionuclides are produced in nuclear reactors by fission.
Some of these fission products may be separated for practical applications.

For this purpose, special separation procedures may be included in the course of
reprocessing with the aim of isolating the desired radionuclides.

The main problems with fission products are the high activities to be handled,
and the fact that their application requires careful purification procedures to
reach acceptable radionuclide purity.

Long-lived radioactive impurities have to be separated effectively. Radionuclide

purity is of special importance in the case of medical applications .
 Production by Accelerators
Radionuclide Production Cyclotrons produce radionuclides by bombarding nuclei with high
energy charged particles.

The various types of accelerators offer the possibility of applying a great variety of
projectiles of different energies.

The most frequently used projectiles are protons, deuterons and a particles.

Neutrons may be produced indirectly by nuclear reactions, y rays are generated as

bremsstrahlung in electron accelerators, and heavy ions are available in heavy-ion
accelerators.

The exact nuclear reaction and the chemical form of the target material is one of the
choices that have to be made in designing a cyclotron target.
Table 12.4, Production of radionuclides by accelerators (survey).
i tg PA ———

Reaction Decay modes of the products Remarks

(p.7) f° ore, rarely 87 Sharp resonances with ght nuclei; (p,m) reactions
may compete
(p,m) B or c, sometimes 6 Mostly endoergic: threshold energy 2-4 MeV
(p, a - Very seldom
(d, mi) f° or e, sometimes 2” Exoergic; high yields
(d, 2n) B or «, rarely f~ Threshold energy 5—10 MeV; at higher energies
(d, 3n) and (d, 4n) reactions
(d,p) mostly 6” Generally relatively high yields; with 14 MeV
deuterons practically applicable for all elements
(d, z) B or po Mostly exoergic; frequently observed with light
nuclei, e.g. °Li(d, xe
(a, n) & ore, rarely Bf Applied for production of neutrons; yields
decrease with mecreasing atomic number; at
higher energies (2, 2n) and (x, 3n) reactions
(a, p) mostly #~, sometimes #7 or 6 Relatively high threshold energies (like other re-
actions with # particles): reactions with nuclides
of high atomic number require high energy of
the » particles
(v,n) Bt, sometimes B~ High-energy y rays available as bremsstrahlung;
always endoergic: threshold energy given by
the binding energy of the neutron; at higher
energies increasing contributions of (y,2n) and
(¥, an) reactions
tp —— 8 S$
 Production by Accelerators
¢ Deuterons are often preferred as projectiles, because of the relatively high cross
sections obtained with them.
Table 12.5. Reactions with deuterons applicable to production of radionuclides

Target Nuclear reaction Yield ae | (thick targets)

uA

8 MeV l4MeV 19 MeV

Li, LiF, LiBO: §1 fd, nn)’ Be Low 74

B20, Be(d, nyc 1.85. 107 1.79. 108 _
Mg, MgO 4Ma(d,a)2Na 39-67 -
Cr Crd, a)*V . Low .
Cr Crd, 20)? Mn - 2.96- 10° -
Fe SPa(d, Mn 37 -
Mn alloy *Min(d, 2n)" Fe - 26 0.74
Fe *Fe(d, 2n)"Co - High -
Fe S$ Fe(d, ap’ Co - High 185
Fe 'Fe(d, nF'Co High
Cu SCu(d, 20)" 70 - 130 -
Ge alloy “Ge(d, In)" As 74 370
As alloy "3 As(d, 2n)"*Se = High ~
NaBr “ard, 20)" Kr - High -
$rCO, *Sr(d, Injy ~ 141-103 -
Pd Ppa(d,n)'"Ag - Average -
Te MT e(d, 20) - 3.3. 108 -
Nal Td, 2n)!?"Ke ~ Average -
Au ' Aud, 2n}! Hg - 3.0. 107 -
 Production by Accelerators
Separation After the radioactive product is formed, it must be isolated from the residual
target material and then chemically reacted with appropriate molecules to form the desired
radiolabeled end- product.

Other considerations that affect the decision as to the physical state of the target include
the following:

The atom density of the target species in the target material—e.g., a solid or liquid might
provide higher atom densities than a gas and thus produce greater amounts of the desired
product.
the cross section of the intended target atoms for the specific nuclear reaction of interest.
The preponderance of interfering species in the irradiated target—some target materials
may contain nuclear species that produce undesired radioactive products that might be
difficult to separate from the desired species
 Production by Accelerators
¢ One of the most challenging problems in the design of
accelerator targets is finding methods to remove this heat from
the target during irradiation.

¢ The heat generated in the target can often have several

detrimental effects. A few of these are the target density
reduction, chemical reactions occurring in the target material
or products, and the potential damage to the target foil or
body.
 Production by Accelerators
0,20 a

Cross section « [b] ——-»

|
‘

x
=

3
\ IN
a
=

l
if
a
=

0,04 Wa 7

0 i
0 é bi 6 a id i? Ma 16
Deuteron energy [MeV] ——=

Figure 12.2, Cross sections of the reactions “Mg(d, a)? Na and **Ma(d, 2)**Na as a function of the
deuteron energy. (According to J, W. Irvine, E. T. Clarke: J. chem, Physics 16, 686 (1948),)
 Production by Accelerators

|
Z “culd, za)" Zn
Cross section @ [hb] ~——* |
im]
dat

Ra

NN
01 | — f Z “cutapie
f 7

fo / |
/

D <a
0 2 b 6 a 10 12 i 6
Deuteron energy [Mev] ———

Figure 12.3, Cross sections for various nuclear reactions of deuterons with copper. (According to
J. W. Irvine, jun.: J. chem. Soc. [London] 5, 356 (1949).)
 Production by Accelerators
The samples may be irradiated inside or
outside the accelerator.
In both cases heat is generated by absorption se" pestion
mn ihe case ol
A
of radiation which must be taken away by
cooling to avoid overheating or melting of
the samples.

The thickness of the samples must also be

taken into account. Because of the strong
interaction of charged particles with matter,
their flux density decreases rapidly and their
energy distribution changes with the
penetration depth.
Only in thin foils can @ be considered to be
constant.
 Production by Accelerators
One of the most important components of any target system is the foil through which the
beam enters the target material.

This component is sometimes absent in solid targets, but is usually required in both liquid
and gaseous targets.

There are several important parameters in the choice of a foil:

The thermal conductivity
The tensile strength
The chemical reactivity (inertness)
The energy degradation properties
Radioactive activation
Melting point
To be Continued...
 Radiochemistry
NE 560

Production of Radionuclides and

Labeled Compounds/ 2
 Separation Techniques
High radionuclide purity is of great importance for application in nuclear
medicine as well as for sensitive measurements.

In this context, impurities of long-lived radionuclides are of particular

importance, because their relative activity increases with time. For
example, if the activity of °°Sr is only 0.1% of that of '*'Ba after fresh
separation, it will increase to 11.5% in three months.

The most frequently used separation techniques are:

crystallization, precipitation or co-precipitation.
Electrolysis.
Distillation.
solvent extraction.
ion exchange.
chromatography.
 Crystallization
Fractional crystallization was one of the first methods used in radiochemistry by
Marie and Pierre Curie to separate *7°RaCl, from BaCl..

Precipitation is only applicable if the solubility product is exceeded, i.e. if the

concentration of the radionuclide to be separated is high enough.

If the concentration is too low, co-precipitation may be applied by addition of a

suitable carrier, i.e. of compounds of identical or very similar chemical
properties.

Application of isotopic carriers is very effective, but it leads to a decrease in

specific activity. Therefore, non-isotopic carriers with suitable chemical
properties are preferred.
 Crystallization

¢ Hydroxides such as iron(IIl) hydroxide or other soluble

hydroxides give high co-precipitation yields, because of their
high sorption capacity .

¢ For filtration, Hahn suction filters are convenient. They allow

easy removal of the filter for further operations or subsequent
measurements.
 Crystallization

il in Buchner Filter

Vacuum cin]

po » To Vacuum

Graduated Cylinder
 Electrolysis
¢ Electrolytic deposition, as a final step of
radiochemical analysis procedure, plays an important
role in both purification and preparation of counting
sources providing an uniform and adherent source
for high resolution alpha spectrometric
measurement.

¢ The preparation of thin samples by electrolytic

deposition is of special interest for the measurement
of a emitters, such as isotopes of Pu or other
actinides.
 Distillation

Separation of radionuclides by distillation is

applicable if volatile compounds are formed
(differences in boiling points). Some examples
are:

separation of Ru (Ruthenium) as RuO, under

oxidizing conditions.
and volatilization of Tc as Tc,O, from
concentrated H,SO, at 150-250 ‘C.
32P may be purified by volatilization as PCI. ina
stream of Cl..
 Solvent Extraction
¢ Liquid—liquid extraction (LLE), also known as solvent extraction, is a method to
separate compounds, based on their relative solubility in two different
immiscible liquids, usually water (polar) and an organic solvent (non-polar).

¢ Solvent extraction is widely used for separation of radionuclides, because this

technique is simple, fast and applicable in the range of low concentrations.

¢ Solvent extraction plays an important role in reprocessing. Tributyl phosphate

(TBP), methyl isobutyl ketone (Hexon) and trilaurylamine (TLA) are preferred
complexing agents for separation and purification of U and Pu (PUREX)

https://www.youtube.com/watch?v= a2JJWcqWwm4
 lon Exchange
¢ lon Exchange chromatography is a process that separates ions based on their affinity to the
ion exchanger. It works on almost any kind of charged molecules.

e The two types of ion chromatography are anion-exchange and cation-exchange:

¢ Cation-exchange chromatography is used when the molecule of interest is positively charged.
In this type of chromatography, the stationary phase is negatively charged and positively
charged molecules are loaded to be attracted to it.
Negatively Charged Positively Charged
e Anion-exchange chromatography is when the stationary Analyte [Anion] Analyte [Cation]
tracted to Attracted to
phase is positively charged and negatively charged molecules Postve Surface Negative Surface

are loaded to be attracted to it.

 Gas Chromatography
¢ Gas chromatography (GC) is applied for separation of volatile compounds.
(mobile and stationary phases) based on preference to adsorption with
stationary phase (solid or liquid).

¢ It involves a sample being vaporized and injected onto the head of the
chromatographic column. The sample is transported through the column
by the flow of inert, gaseous mobile phase,

¢ The column itself contains a liquid stationary phase, the process is termed
gas-liquid chromatography (GLC). When the stationary phase is a solid
adsorbent, the process is termed gas-—solid chromatography (GSC)
 Gas Chromatography
Assume two components (green and orange) need to be separated using GC. Orange runs
fast in GC which shows its low relative affinity with the stationary phase and more affinity to
be in gas phase; thus it must be a low boiling point analyte however green component
prefer to stay in stationary phase thus have high relative affinity with liquid stationary phase
and thus is a high boiling point component.

ANALYTICAL GAS CHROMATOGRAPHY

 Radionuclide Generators
Application of short-lived radionuclides has the advantage that the activity
vanishes after relatively short periods of time. This aspect is of special
importance in nuclear medicine.

Short-lived radionuclides may be produced by irradiation in nuclear reactors or

by accelerators, but their supply from irradiation facilities requires matching of
production and demand, and fast transport.

These problems are avoided by application of radionuclide generators.

Radionuclide generators are devices that produce a useful short-lived medical

radionuclide (daughter) from the radioactive transformation of a non-medical
long-lived radionuclide (parent). By having a supply of parent on hand at a
facility, the daughter is continually separated on site.
 Radionuclide Generators
The mother nuclide must be present in such a chemical form that the daughter
nuclide can be separated repeatedly by a simple operation leaving the mother
nuclide quantitatively in the generator.

After each separation, the activity of the daughter nuclide increases again, and
the daughter nuclide can be separated repeatedly at certain intervals of time.

For example, after three half-lives of the daughter nuclide 87.5% of its saturation
activity is reached and separation may be repeated with a relatively high yield.

Fixation of the mother nuclide and simple separation of the daughter nuclide are
achieved by use of separation columns containing a suitable ion exchanger or
sorbent from which the daughter nuclide can be eluted.
 Example: Radiopharmaceutical Production
99Ml0°°™Tc Generator
¢ 9°Mo decays to ??™Tc
Saline Solution

¢ The daughter is then

extracted to be used in
nuclear medicine. Parent and Daughter
Lead Shielding (°°Mo and °° Tc) ~“

Glass Column
¢ The idea is to produce a Alumina (Al,O.) |

short-lived daughter from

a longer-lived parent Glass Frit Daughter (°°"Te)

— Mo T,,. = 66 hours
— ™Tc T,/) - 6.02 hours
«———__ Eluted Vial
Transient Equilibrium 99MT>
 Example: Radiopharmaceutical Production
99Mlo??™Tc Generator
Saline is initially introduced into the system
29MTc is liberated in a saline solution while ??Mo remaining in the
column
Mos SinTc Decay, Curves,
29MTc then passes through the Alumina and the glass frit (filter)
and then out to elution vial
The elution vial must be negatively pressured in order for the g
saline to move through the system. Z
&
Over time 97Mo decays to 7?™Tc
In less than 24 hours later (four 9?™Tc half-lives) from the prior a
elution ??7Mo/??™Tc reach equilibrium. Tune
te blouse
Hence according to the graph ??™Tc builds up over time, until they
both reach transient equilibrium, then they both decay at the rate
of °°Mo.
 Radionuclide Generators
Table 12.10. Examples of mother and daughter nuclides suitable for use in radionuclide generators.

Mother nuclide Daughter nuclide

Nuclide Half-life Decay mode Nuclide Half-life Decay mode

3Mip 20.9h gy 25 AI 2.25m ayy

Ar 33y Bo aK 12.36 h By
“Tj ATAy By Sc 3.92h foe y
Fe 10° y Boy Sy 10.5 m BIT. y
Se Ni 228d Bo Cu 5.1m Boy
OF n 9.26h eB, y 2Cy 9.73m Br, 8 ¥
Pn 46.5h Boy "Ga 14th By
Ge 271d é “Ga 68.3m Belay
Se g5d 2, "As 26,0h Br. 8, ¥
=Rb 86.2d é, } bom Kr 1.86 h IT
Sr 25.5d 3 Rb |.27m Boa y
“Sr IRS y B ay 64.1h Ao
Shy 80.3h ge, Bt, y sim Sr 2.81 h IT
Mo 66.0h BY Te 6.0h IT
Ru 30.35 d Boy Mme h 56,1 m IT
To be continued...